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# Feedback cooling of a nanomechanical resonator LAUR-03-1275

## I Introduction

Nanomechanical resonators are now being built with quality factors in the range, $`Q10^4`$, and resonance frequencies of up to several hundred MHz Experiments . The ground state energy of these devices can correspond to temperatures in the milliKelvin range. As a result, the observation of quantum behavior in these devices is becoming a real possibility Armour . To detect such behavior, the resonator must be sufficiently cold; since a quantum harmonic oscillator driven by thermal noise behaves as a classical oscillator driven by thermal noise, one must ensure that the signatures of quantum effects are not swamped by the thermal behavior. The approach taken so far to achieve low temperatures is to place the resonator in a refrigerator. However, cooling very small devices in this way is inherently inefficient in that the system becomes weakly coupled to the thermal bath. Here we explore the possibility of using feedback control to effect ‘active’ cooling of the resonator, in order to cool below the possible limits set by the ‘passive’ refrigeration technique.

To perform such feedback cooling the resonator must be monitored, and the result fed back in real time to affect the dynamics. A practical method of performing a continuous measurement of the position of the resonator is to use a Single-Electron Transistor (SET) Korotkov94 ; Hanke94 ; Shnirman . To measure the position of the resonator one locates the central island of the SET next to the resonator. When the resonator is charged, and the SET is biased so that current flows through it, changes in the resonator’s position alter the potential on the central island, which in turn changes the current. The current therefore provides a continuous measurement of the position of the resonator, and this is just what is required for implementing a linear feedback cooling algorithm Doherty99 ; Jacobs . A feedback force can be applied by applying a voltage to a gate capacitively coupled to the resonator, and adjusting the voltage so as to damp the resonator (see Fig. 1), or by passing a variable current through the oscillator in the presence of a fixed external magnetic field. We will analyze the first system, although the results should apply to the second as well. In our analysis we will use the theory of the dc-SET. While an experiment would most likely use a radio-frequency SET, the characteristic frequency of a SET is typically of the order of $`10\text{GHz}`$, so that the RF drive looks constant to the SET, and the dc-SET equations can be used.

We will use a quantum mechanical model of the measurement and feedback process, but discuss how in this case, such a description is equivalent to a classical measurement of a noisy classical system. Thus, this article is intended for both experimentalists familiar with classical descriptions of noise in systems, as well as quantum measurement theorists.

Rather than performing a microscopic analysis of the measurement process in terms of the interaction of the SET and the resonator, we start by introducing equations which describe the continuous observation of a quantum observable, and show how this includes the shot noise and back-action, these being the key sources of noise in a continuous quantum measurement. This description can then be tailored to the case of a measurement with a SET by choosing the parameters so that the noise sources match those calculated in microscopic noise analyses which have been performed for the SET Korotkov94 ; Zhang .

A treatment of the continuous quantum measurement of a two-state system using a SET has been carried out by Korotkov Korotkov01 , using what might be referred to as a partially microscopic approach. The equations we use here may be derived by replacing the two-state observable in those equations by the resonator position. A full analysis, along the lines of those performed for quantum optical systems Wiseman93 ; Milburn94 , can also be expected to produce the same equations under reasonable approximations. The form of these equations is determined by how information is obtained, and not by the specific implementation, which explains why the form of the equations is similar in optical position measurements and position measurement using SETs. If the measurement is of a physical observable, and the resulting error about the expectation value of that observable in a short time interval $`\mathrm{\Delta }t`$ is Gaussian, then the most straightforward implementation of that measurement process has the form used here.

In the next section we introduce the equations that describe a continuous measurement process, derive the form of the resulting noise, and give the equivalent classical model. We then discuss how this model can be applied to position measurement using a SET, and compare our formulae to those derived using a semi-classical treatment of the SET Korotkov94 ; Zhang  in order to express our results in terms of experimental parameters. In Section III we discuss the implementation of a feedback algorithm and calculate the minimum achievable temperature in terms of physical parameters. We then calculate estimates of realistic achievable temperatures for an an experimentally realizable sample system in Section IV, and finally conclude with a summary of the results obtained.

## II Continuous Quantum Measurement of Position

Given a quantum system whose state is specified by the density matrix $`\rho `$, and whose evolution is determined by the Hamiltonian $`H`$, then a continuous measurement of the observable $`O`$ of that system, which provides the continuous output results (measurement record),

$$dr=Odt+\frac{1}{\sqrt{8k}}dW,$$
(1)
induces the following evolution of the system Caves87 ; Jacobs98 ; Doherty99

$`d\rho `$ $`=`$ $`i[H,\rho ]dtk[O,[O,\rho ]]dt`$ (2)
$`+\sqrt{2k}(O\rho +\rho O2O)dW.`$
Here $`k`$ is proportional to the measurement strength and $`dW`$ is a Weiner process. The noise contained in the measurement record is a necessary result of the fact that only a finite amount of information is obtained regarding the observable $`O`$ in a finite time. This direct noise on the record is called the shot noise. However, this is not the only noise resulting from the measurement process. As a result of Heisenberg’s uncertainty relation, information about one observable makes other observables less certain. Due to the dynamics, the uncertainty (noise) in these observables can feed into the observable being measured. This source of noise is referred to as back-action. If the Hamiltonian is such that the increased uncertainty is not fed back into the observable being measured, then the measurement is referred to as ‘back-action evading.’

Now let us examine the case of a position measurement on a harmonic oscillator. To do this, we set $`O=x`$, and the Hamiltonian becomes

$$H=\frac{p^2}{2m}+\frac{1}{2}m\omega _0^2x^2,$$
(3)
where $`m`$ is the mass of the particle, $`\omega _0`$ is the (angular) frequency of the oscillation, and $`x`$ and $`p`$ are the position and momentum operators, respectively. To make our model sufficiently realistic, we need to include two more sources of noise: the first is the intrinsic thermal noise of the harmonic oscillator, and the second is the possibility that the oscillator may be driven by white noise over and above that required by Heisenberg’s uncertainty principle (excess ‘technical noise’).

The second of these is easily included by adding a term $`\beta [x,[x,\rho ]]`$ to the equation of motion of $`\rho `$; this describes a noise term identical to the one caused by the back-action, but without the corresponding dynamics of $`\rho `$ associated with obtaining a measurement result which causes the back-action. It is equivalent to adding a term linear in $`x`$ to the Hamiltonian (3) multiplied by white noise.

The inclusion of thermal fluctuations is only a little more involved, and can be achieved by coupling the oscillator to a thermal bath. In our case the effect of the thermal bath may be included by adding the ‘standard Brownian motion master equation’ (SBMME) QNoise  to our equation of motion for $`\rho `$:

$`d\rho `$ $`=`$ $`{\displaystyle \frac{i}{\mathrm{}}}[H,\rho ]dt{\displaystyle \frac{i\mathrm{\Gamma }}{2\mathrm{}}}[x,\{p,\rho \}_+]dt`$ (4)
$`\left(k+\beta +{\displaystyle \frac{m\omega _0\mathrm{\Gamma }}{2\mathrm{}}}\mathrm{coth}{\displaystyle \frac{\mathrm{}\omega _0}{2k_BT}}\right)\text{[}x,[x,\rho ]\text{]}dt`$
$`+\sqrt{2k}(x\rho +\rho x2x\rho )dW`$
where $`\mathrm{\Gamma }=\frac{\omega }{Q}`$, $`Q`$ being the quality factor of the resonator. The two terms proportional to $`\mathrm{\Gamma }`$ are due to the inclusion of the SBMME, the first representing dissipation due to the reservoir while the second is a diffusion term due to environmental fluctuations. Here we are using an approximate form of the SBMME appropriate for the weak coupling regime (small $`\mathrm{\Gamma }`$, large $`Q`$) but covering all ranges of temperatures CCR . Since the nanomechanical resonators we consider all have large values of $`Q`$, the weak coupling requirement is easily satisfied. The temperature dependence of the diffusion coefficient is given by $`\mathrm{coth}(\mathrm{}\omega _0/2k_BT)`$ so that the diffusion does not vanish as $`k_BT0`$: this correctly accounts for the existence of quantum vacuum fluctuations which exist even at zero temperature. In the absence of a rigorous characterization of the dissipation channels of nanomechanical systems there is as yet no need to include a more sophisticated description of SBMME environmental effects HuVit . Phenomenological corrections to the SBMME such as temperature dependence of $`\mathrm{\Gamma }`$ can be added if needed, but these are not significant effects in the high-$`Q`$ regime.

We also need to include in our model the possibility that there is noise driving the oscillator which is correlated with the noise on the measurement record (the shot noise). This can happen if the noisy behavior of the oscillator explicitly causes some of the noise in the measurement apparatus, or vice versa. In this situation, the measurement record contains more information about the oscillator position, so when it comes to adding feedback, we are able to cool the oscillator further than would otherwise be expected. In Eq. (2) the noise driving the oscillator is purely the quantum back-action. It may appear from Eqs. (1) and (2) that the quantum back-action is correlated with the shot noise due to the fact that the same noise term ($`dW`$) appears in both equations. However, this is not the case. The term proportional to $`dW`$ which appears in the equation for $`\rho `$ describes the random way in which the measurement changes the observers state of knowledge about the system. Thus, in general, this noise term decreases the entropy of $`\rho `$. The back-action noise, which is driving the oscillator and consequently increasing the entropy of $`\rho `$, is described by the term proportional to $`k`$. The quantum back-action is, in fact, completely uncorrelated with the shot noise.

To drive the oscillator with a random force, one applies the Hamiltonian $`\mathrm{}\xi (t)x`$, where $`\xi (t)`$ is the magnitude of the random force. We can choose $`\xi (t)`$ to be correlated with the shot noise, with correlation coefficient $`\kappa `$, by setting

$$d\xi =\sqrt{2\alpha }(\sqrt{\kappa }dW+\sqrt{1\kappa }dV),$$
(5)
where $`dV`$is a Wiener noise uncorrelated with $`dW`$. The resulting spectral density of $`\xi (t)`$ is $`\alpha `$, so that $`\xi (t)\xi (t^{})=\alpha \delta (tt^{})`$. The Stratonovich equation which describes the driving by $`\xi (t)`$ is

$$|\dot{\psi }=i\xi (t)x|\psi ,$$
(6)
and converting this to an Ito equation gives

$$d|\psi =i\sqrt{2\alpha }x|\psi d\xi \alpha x^2|\psi dt.$$
(7)
Converting the Ito equation further to an equation for $`\rho `$ one obtains

$$d\rho =\alpha [x,[x,\rho ]]dti\sqrt{2\alpha }[x,\rho ]d\xi .$$
(8)
Since the observer has access to $`dW`$, but not to $`dV`$, she must average over $`dV`$, and this gives

$$d\rho =\alpha [x,[x,\rho ]]dti\sqrt{2\kappa \alpha }[x,\rho ]dW.$$
(9)
If we allow part of the excess noise given by $`\beta `$ in our model to be due to driving by the shot noise $`dW`$ (that is, this noise is correlated with the shot noise $`dW`$ with correlation coefficient $`\kappa `$) then the equation of motion for the system becomes

$`d\rho `$ $`=`$ $`{\displaystyle \frac{i}{\mathrm{}}}[H,\rho ]dt{\displaystyle \frac{i\mathrm{\Gamma }}{2\mathrm{}}}[x,\{p,\rho \}_+]dt`$ (10)
$`\left(k+\beta +{\displaystyle \frac{m\omega _0\mathrm{\Gamma }}{2\mathrm{}}}\mathrm{coth}{\displaystyle \frac{\mathrm{}\omega _0}{2k_BT}}\right)[x,[x,\rho ]]dt`$
$`i\sqrt{2\kappa \beta }[x,\rho ]dW`$
$`+\sqrt{2k}(x\rho +\rho x2x\rho )dW`$
This completes our quantum mechanical description of a resonator under continuous observation.

Now that we have an equation that includes all the relevant noise terms, the noise spectrum of the measurement record can be obtained:

$`S(\omega )`$ $`=`$ $`{\displaystyle \frac{1}{8k}}+\left(k+\beta +{\displaystyle \frac{m\omega _0\mathrm{\Gamma }}{2\mathrm{}}}\mathrm{coth}{\displaystyle \frac{\mathrm{}\omega _0}{2k_BT}}\right)`$ (11)
$`\times {\displaystyle \frac{2(\mathrm{}/m)^2}{\mathrm{\Gamma }^2\omega ^2+(\omega ^2\omega _0^2)^2}}`$
The first term is the shot noise, which is white, the term proportional to $`k`$ is the quantum back-action, the term proportional to $`\mathrm{\Gamma }`$ is the effect of the noise from the resonator’s thermal environment, and the term proportional to $`\beta `$ gives any excess noise over and above the necessary quantum back-action. Note that the last three terms all have the same form as a function of $`\omega `$. This is because they are all white noises filtered through the harmonic oscillator spectral response function.

While our treatment so far has been fully quantum mechanical, it is worth noting that a completely classical model of a measured, damped oscillator will reproduce the dynamics of this measured quantum system, so long as the initial density matrix is Gaussian in $`x`$ and $`p`$ Doherty99 . Thus, one can understand the behavior of the oscillator in terms of classical noise and a classical measurement process. The equations of motion for the position, $`x_\text{c}`$, and momentum $`p_\text{c}`$ of this equivalent classical oscillator are

$`dx_\text{c}`$ $`=`$ $`{\displaystyle \frac{1}{m}}p_\text{c}dt`$ (12)
$`dp_\text{c}`$ $`=`$ $`m\omega _0^2x_\text{c}dt\mathrm{\Gamma }p_\text{c}dt+\mathrm{}\sqrt{2k}dY_\text{c}+\mathrm{}\sqrt{2\beta }dV_\text{c}`$ (13)
$`+\sqrt{m\mathrm{}\omega _0\mathrm{\Gamma }\mathrm{coth}{\displaystyle \frac{\mathrm{}\omega _0}{2k_BT}}}dU_\text{c}`$
where $`dY_\text{c}`$, $`dV_\text{c}`$ and $`dU_\text{c}`$ are each zero-mean Gaussian white noise, and mutually uncorrelated. The position of the oscillator is then observed by a continuous classical measurement, which generates the output record

$$dr_\text{c}=x_\text{c}dt+\frac{1}{8k}dZ_\text{c},$$
(14)
and where $`dZ_\text{c}`$ is zero-mean Gaussian white noise, uncorrelated with $`dY_\text{c}`$. The noise term $`dY_\text{c}`$ is what is required in the classical model to correctly include the back-action of the quantum measurement process. It is now explicit that this noise is uncorrelated with the shot noise on the measurement, $`dZ_\text{c}`$.

In the classical case, the observer’s state of knowledge about the oscillator is given by a joint probability density over $`x_\text{c}`$ and $`p_\text{c}`$. This probability density is the classical equivalent of the density matrix $`\rho `$. So long as the initial probability density is Gaussian, it remains Gaussian as time passes, and as a result the observer’s full state of knowledge may be represented by merely 5 variables: the mean position and momentum, $`x_\text{c}`$ and $`p_\text{c}`$, and the variances and covariance, given by

$`\sigma _x^2`$ $`=`$ $`x_\text{c}^2x_\text{c}^2,`$ (15)
$`\sigma _p^2`$ $`=`$ $`p_\text{c}^2p_\text{c}^2,`$ (16)
$`\sigma _{xp}^2`$ $`=`$ $`x_\text{c}p_\text{c}x_\text{c}p_\text{c}.`$ (17)
It is the means $`x_\text{c}`$ and $`p_\text{c}`$ (being the observer’s best estimates of the value of $`x_\text{c}`$ and $`p_\text{c}`$) which are the classical equivalents of the quantum expectation values $`x`$ and $`p`$. It turns out that if one writes the classical measurement record as

$$dr_\text{c}=x_\text{c}dt+\frac{1}{8k}dW_\text{c},$$
(18)
then $`dW_\text{c}`$ is zero-mean Gaussian white noise Jacobs , uncorrelated with $`dZ_\text{c}`$. The classical model is then equivalent to the quantum model if we equate $`dW_\text{c}`$ with the quantum measurement noise, $`dW`$, and correlate $`dV_\text{c}`$ with $`dW_\text{c}`$, so that $`V_\text{c}(t)dW_\text{c}(t^{})=\kappa \delta (tt^{})`$.

## III Continuous Measurement with a Single Electron Transistor

Having obtained a model which is sufficiently general to encompass the dynamics of a resonator monitored by a SET, we need to express the theoretical parameters $`k`$, $`\beta `$, and $`\kappa `$ in terms of the actual experimental parameters of the SET. Since it is by measuring current through the SET that we measure the resonator position, it is the spectral density of this current which determines the shot noise of the measurement. The back-action from the measurement is due to the action of the SET on the resonator, which is the force that the resonator feels from the charge on the SET island. As a result the back-action noise, $`\beta `$, can be calculated from the spectral density of the charge fluctuations on the SET island, and hence $`\kappa `$ is determined by the correlation between the current and the island charge fluctuations.

However, the dynamics of the SET are sufficiently complex that analytic results for these spectra have as yet only been obtained for certain parameter regimes. These calculations have been performed by Zhang and Blencowe Zhang , using previous results of Korotkov Korotkov94 . The technique used is to approximate the dynamics of the electron tunneling on and off the SET island by a classical master equation. That is, the electrons are assumed to tunnel independently across each of the junctions, with certain rates (the rates being obtained using a perturbative quantum calculation). This ignores the possibility that electrons will tunnel coherently across both junctions simultaneously, a quantum effect referred to as cotunneling.

However, it is important to note that the above “classical” method for calculating the charge fluctuations does not include the quantum back-action noise. This can be seen from the following argument HWpriv . In the classical treatment, since the fluctuating force on the resonator is due to the electrons jumping on and off the island, in principle the time history of this force can be known by detecting the electrons flowing in the circuit. In principle then, the effect of the noise can be known, and if desired, undone. As a result it cannot include the quantum back-action, since this cannot, even in principle, be undone.

The approach we will take here is to use the classical calculation of the force noise on the resonator, which determines $`\beta `$, and add to it the necessary back-action as required by quantum mechanics, which is given by $`k`$. In doing this we note that the ratio $`k/\beta `$ provides a diagnostic tool for determining when the classical calculation breaks down; if $`k/\beta 1`$ is not satisfied, then the classical calculation no longer provides a good estimate of the total force noise on the resonator. Thus it should be noted that if $`k/\beta 1`$, then the classical calculation cannot be relied upon. That is, it is possible in this case that the total noise on the resonator is significantly larger than our estimate $`k+\beta `$, due to quantum contributions not taken into account in the classical calculation.

We find that in the regions of best cooling, which we explore in the following, $`k`$ is larger than $`\beta `$ (although near-optimal cooling can be obtained with $`k\beta `$, and in particular we will give as an example results for $`k=\beta /4`$). Hence our calculations should be regarded as estimates of the performance of the feedback algorithm, rather than exact results. We note, however, that a more sophisticated analysis using the diagrammatic techniques developed by Schoeller and Schön Schoeller  might provide analytic, or semi-analytic results for the parameter regime of most interest for quantum measurement and control, and therefore may provide a method for more accurate calculations.

The spectral densities given by the classical calculation are derived in Appendix A. Approximations which are used in the derivation are detailed there, and come primarily from Zhang and Blencowe Zhang . The noise spectrum of the displacement of the resonator due to the shot noise of the SET current is

$`S_X^I`$ $`=`$ $`{\displaystyle \frac{S_\text{I}(\omega )}{(dI_{\text{ds}}/dx)^2}},`$ (19)
where $`S_I(\omega )`$ is the spectral density of the shot noise, given in Eq. (55), and $`I`$ is the current through the SET, given in Eq. (53). The dependence of the current on the displacement of the resonator comes from its dependence on the gate capacitance, which can be approximated by

$`C_\text{g}C_{g0}(1{\displaystyle \frac{x}{d}}).`$ (20)
The shot noise, $`S_I(\omega )`$ is, to a very good approximation, frequency independent, as required by our quantum measurement model. Thus

$`{\displaystyle \frac{1}{8k}}=S_X^I|_{\omega =0}={\displaystyle \frac{S_\text{I}(\omega )}{(dI_{\text{ds}}/dx)^2}}|_{\omega =0}.`$ (21)
The spectral density of the classical part of the displacement noise due to the fluctuating force on the resonator is

$`S_X^F(\omega )`$ $`=`$ $`{\displaystyle \frac{S_\text{F}(\omega )/m^2}{\mathrm{\Gamma }^2\omega ^2+(\omega ^2\omega _0^2)^2}},`$ (22)
where $`S_F(\omega )`$ is the spectral density of the fluctuating force given in Eq. (58). Since, once again, $`S_F(\omega )`$ is effectively frequency independent, we have

$$\beta =\frac{S_\text{F}}{2\mathrm{}^2}|_{\omega =0}.$$
(23)
The correlation coefficient, $`\kappa `$, between the shot noise and the excess back action is therefore simply the correlation, $`C`$, between $`S_\text{I}`$ and $`S_\text{F}`$, which is given in Eq. (56).

## IV Feedback control

We wish to cool the dynamics of the resonator by using the information obtained continuously about the state of the resonator to direct a time-dependent external force. Such a force may be applied, for example, by passing current through the resonator and immersing it in a magnetic field. It can also be applied by placing an actuating gate near the resonator, and varying the potential difference between the charged resonator and the actuating gate.

In this case the results of modern optimal control theory apply, since the dynamics of the resonator are equivalent to that of a classical oscillator driven by Gaussian noise, so long as we restrict ourselves to a linear external force Doherty99 ; Doherty00 . This allows us to obtain the optimal feedback algorithm in a straightforward manner. Choosing the minimization of the energy of the resonator as the feedback objective it turns out that as long as the force we apply is sufficiently large, this force should be chosen to be Doherty99

$$F=\gamma (m\omega _0x+p),$$
(24)
where $`\gamma `$ is a rate constant which determines the overall strength of the force. This equation gives optimal performance so long as $`\gamma \omega _0`$, which is within reach of current experiments, as detailed below.

To calculate the average energy of the controlled resonator, we first need the equations of motion for the mean values in the continually observed and controlled case, which are

$`dx`$ $`=`$ $`{\displaystyle \frac{p}{m}}dt\mathrm{\Gamma }xdt+2\sqrt{2k}\sigma _x^2dW`$ (25)
$`dp`$ $`=`$ $`m\omega ^2xdt2\mathrm{\Gamma }pdt\gamma (m\omega x+p)dt`$ (26)
$`+\sqrt{2\kappa \beta }\mathrm{}dW+2\sqrt{2k}\sigma _{xp}^2dW,`$
and for the covariances,

$`\dot{\sigma _x^2}`$ $`=`$ $`{\displaystyle \frac{2}{m}}\sigma _{xp}^28k(\sigma _x^2)^2,`$ (27)
$`\dot{\sigma _p^2}`$ $`=`$ $`2m\omega ^2\sigma _{xp}^28k(\sigma _{xp}^2)^22\mathrm{\Gamma }\sigma _p^2+2\mathrm{}^2k`$ (28)
$`+2\mathrm{}^2\left[(1\kappa )\beta +{\displaystyle \frac{m\omega _0\mathrm{\Gamma }}{2\mathrm{}}}\mathrm{coth}{\displaystyle \frac{\mathrm{}\omega _0}{2k_BT}}\right]`$
$`\dot{\sigma _{xp}^2}`$ $`=`$ $`{\displaystyle \frac{\sigma _p^2}{m}}m\omega ^2\sigma _x^2{\displaystyle \frac{\mathrm{\Gamma }}{2}}\sigma _{xp}^28k\sigma _x^2\sigma _{xp}^2`$ (29)
$`4\sqrt{\kappa \beta k}\mathrm{}\sigma _x^2.`$
In these equations, $`\sigma _x^2`$ and $`\sigma _p^2`$ are the variances in position and momentum, respectively, and

$$\sigma _{xp}^2=\frac{1}{2}xp+pxxp$$
(30)
is the symmetrized covariance. This system of equations is exactly equivalent to Eq. (10) as long as the initial state is Gaussian. In order to solve this set of equations most easily, we make what we call the truncated Gaussian approximation. We assume that the feedback rate $`\gamma `$ is much larger than the system’s small intrinsic damping $`\mathrm{\Gamma }`$, and we therefore drop all terms proportional to $`\mathrm{\Gamma }`$ from the above equations. This approximation is easily justified for current experiments.

The steady state solutions to these equations are

$`\sigma _x^2`$ $`=`$ $`{\displaystyle \frac{\sqrt{2}\omega }{8k}}\sqrt{\mathrm{\Lambda }},`$ (31)
$`\sigma _p^2`$ $`=`$ $`{\displaystyle \frac{\sqrt{2}m^2\omega ^3}{8k}}[\sqrt{\mathrm{\Lambda }}+\mathrm{\Lambda }^{3/2}]`$ (32)
$`+{\displaystyle \frac{4\sqrt{2}\mathrm{}m\omega }{k}}\sqrt{\kappa \beta k}\sqrt{\mathrm{\Lambda }},`$
$`\sigma _{xp}^2`$ $`=`$ $`{\displaystyle \frac{m\omega ^2}{8k}}\mathrm{\Lambda },`$ (33)
where

$`\mathrm{\Lambda }+1=`$
$`\left[1+16{\displaystyle \frac{k\mathrm{}^2\{k+(1\kappa )\beta +\frac{m\omega _0\mathrm{\Gamma }}{2\mathrm{}}\mathrm{coth}\frac{\mathrm{}\omega _0}{2k_BT})\}}{m^2\omega ^4}}\right]^{1/2}.`$ (34)
In the limit of both large and small values of $`k`$, $`\mathrm{\Lambda }k`$.

Using the steady state solutions for the variances $`\sigma _x^2`$ and $`\sigma _{xp}^2`$ in Eqs. (25) and (26), and calculating the variances of $`x`$ and $`p`$, we obtain

$`\sigma _x^2`$ $`=`$ $`{\displaystyle \frac{\omega (\gamma ^2+\gamma \omega +\omega ^2)}{8k\gamma (\omega +\gamma )}}\mathrm{\Lambda }+{\displaystyle \frac{\sqrt{2}\omega ^2}{8k(\omega +\gamma ))}}\mathrm{\Lambda }^{3/2}`$ (35)
$`+{\displaystyle \frac{\omega ^3}{16k\gamma (\omega +\gamma )}}\mathrm{\Lambda }^2+{\displaystyle \frac{\kappa \beta \mathrm{}^2}{m^2\omega \gamma (\omega +\gamma ))}}`$
$`+{\displaystyle \frac{\mathrm{}\sqrt{\kappa \beta k}}{2m(\omega +\gamma )}}\left[{\displaystyle \frac{\sqrt{2\mathrm{\Lambda }}}{k}}+{\displaystyle \frac{\omega \mathrm{\Lambda }}{2\gamma }}\right]`$
$`\sigma _p^2`$ $`=`$ $`{\displaystyle \frac{m^2\omega ^3(\omega +\gamma )}{8k\gamma }}\mathrm{\Lambda }+{\displaystyle \frac{m^2\omega ^4}{16k\gamma }}\mathrm{\Lambda }^2+{\displaystyle \frac{\kappa \beta \mathrm{}^2}{\gamma }}`$ (36)
$`+{\displaystyle \frac{m\omega ^2\mathrm{}\sqrt{\kappa \beta k}}{4k\gamma }}\mathrm{\Lambda }.`$
The average steady-state energy of the oscillator under observation and feedback is the sum of the intrinsic variances of the Gaussian steady state and the variances in the observer’s measurement record. Thus

$`E`$ $`=`$ $`{\displaystyle \frac{1}{2}}m\omega ^2(\sigma _x^2+\sigma _x^2)+{\displaystyle \frac{\sigma _p^2+\sigma _p^2}{2m}}`$ (38)
$`=`$ $`{\displaystyle \frac{m\omega ^3}{8k}}\left[\sqrt{2\mathrm{\Lambda }}+\mathrm{\Lambda }+{\displaystyle \frac{\sqrt{2}}{2}}\mathrm{\Lambda }^{3/2}+{\displaystyle \frac{\omega }{4\gamma }}\mathrm{\Lambda }^2\right]+{\displaystyle \frac{\kappa \beta \mathrm{}^2}{2m\gamma }}`$
$`+{\displaystyle \frac{\mathrm{}\omega \sqrt{\kappa \beta k}}{4k}}[\sqrt{2\mathrm{\Lambda }}+{\displaystyle \frac{\omega }{2\gamma }}\mathrm{\Lambda }].`$
Here we have used the simplifying assumption $`\gamma \omega `$, since this is inherent in the optimal control condition.

It is clear from Eqs. (34) and (38) that reducing the background temperature allows for lower final temperatures. Extremely low values of $`k`$ lead to heating as can be seen from the fact that $`\mathrm{\Lambda }k`$. For large $`k`$ (corresponding to large gate voltage), the increased sensitivity of the measurement cancels the increased disturbance due to the measurement, with the result that the minimal temperature levels off as $`k`$ is increased.

## V Estimates for achievable temperatures

Current refrigeration technology allows experiments on nanomechanical resonators to be performed at temperatures of about $`100\text{mK}`$. It is therefore sensible to assume that the feedback algorithm will be applied to a device which is initially at this temperature. In such experiments the resonators typically have fundamental frequencies in the range $`f_0=1100\text{MHz}`$. As our example system we take a realistic resonator with $`f_0=12\text{MHz}`$, which is $`6\mu \text{m}`$ in length, $`50\text{nm}`$ wide, and $`150\text{nm}`$ thick. We restrict ourselves to relatively low frequencies because of the limits of feedback circuitry, which we estimate can easily operate at $`50\text{MHz}`$. The effective mass of such a resonator is roughly $`10^{16}\text{kg}`$. An achievable quality factor, $`Q`$, is on the order of $`10^4`$.

Realistic values for the resistances and capacitances of the junctions of a SET which would be used to monitor the resonator are $`R_1=R_2=50\text{k}\mathrm{\Omega }`$, and $`C_1=C_2=100\text{aF}`$, and we place it $`d100\text{nm}`$ from the resonator. We estimate that the capacitance between the gate of the SET and the resonator will be roughly $`C_\text{g}=50\text{aF}`$, so that $`C_\mathrm{\Sigma }=250\text{aF}`$ ($`C_\mathrm{\Sigma }=2C_j+C_\text{g}`$). It is important to note that the analysis we use in the appendix to obtain the noise spectra is only a good approximation in certain parameter regimes. In particular, we require that $`V_{\text{ds}}`$, being the drain-source voltage across the SET, satisfies $`V_{\text{ds}}e/C_\mathrm{\Sigma }`$.

To apply the feedback force, we place the resonator $`100\text{nm}`$ from the actuating gate, and allow the controller to vary the voltage difference between the gate and the resonator between $`4\text{V}`$ to $`4\text{V}`$. The capacitance of this arrangement is about $`50\text{aF}`$, so the maximum force that can be applied to the resonator is of the order of $`10^8N`$. This corresponds to $`\gamma 1.08\times 10^{13}\text{s}^1`$, which is much larger than $`\omega `$ and $`\mathrm{\Gamma }`$, as required by the optimal control condition and truncated Gaussian approximation used in the previous section.

Before giving theoretical estimates for the achievable steady-state temperature (or equivalently, the steady-state average occupation number of the oscillator, $`N=a^{}a`$), we need to explain two subtleties which affect the presentation of our results. When one examines the dependence of the steady-state $`N`$ on the gate voltage, once finds that it oscillates very rapidly, with minima occurring in closely spaced pairs. Since $`V_\text{g}`$ is experimentally easy to tune, all else being equal it would make sense simply to plot these minima and ignore the complex structure. However, the locations of the minima are such that $`k/\beta `$ can be large, and as discussed in section III, our results are more trustworthy the smaller $`k/\beta `$. The situation is shown in detail in Figure 2, in which we display, as a function of $`V_\text{g}`$, two pairs of the $`N`$ minima, as well as $`k/\beta `$ and the current $`I_{\text{ds}}`$. When presenting results in what follows, we will plot both the minima with respect to $`V_\text{g}`$, and the temperature which results if we demand that $`k/\beta 1/4`$. For clarity these points are also displayed in Figure 2.

As an example of the relative magnitudes of the various noise sources at the minima displayed in Figure 2, if we set the drain-source voltage at $`V_{\text{ds}}=e/(4C_\mathrm{\Sigma })=0.16\text{mV}`$ and the gate voltage at $`V_\text{g}1\text{V}`$, then the noise sources are:

$`\beta =4.47\times 10^{29}\text{m}^2\text{s}^1,`$ (39)
$`k=4.2\beta ,`$ (40)
$`{\displaystyle \frac{m\omega _0\mathrm{\Gamma }}{2\mathrm{}}}\mathrm{coth}{\displaystyle \frac{\mathrm{}\omega _0}{2k_BT}}=209\beta `$ (41)
and the correlation coefficient is $`\kappa =0.633`$.

Using the above parameter values to calculate the minimum achievable temperature, we find that $`\mathrm{\Lambda }=4.95\times 10^5`$, and $`T=2.06\text{mK}`$. This corresponds to an energy of about $`E_{\text{ss}}=2.85\times 10^{26}\text{J}`$, and an average occupation number $`N=3.09`$. While this is very encouraging, ideally one wants to cool below the energy of the first excited state, and we now examine what is required to do this.

While classically an increase in measurement strength would automatically lead to improved tracking of the resonator, and therefore more efficient cooling, quantum mechanically the situation is more complex due to the fact that more precise measurement also leads to increased heating due to back-action. Nevertheless, In the present case one finds that the increased sensitivity of the measurement with increasing measurement strength effectively cancels this heating, and as a result larger $`V_\text{g}`$ corresponds to better cooling. However, after a sharp increase in cooling with increasing $`V_\text{g}`$, the minimal temperature levels off, so greater $`V_\text{g}`$ no longer provides much benefit. In addition, at some $`V_\text{g}`$ snap-in is likely to occur as the force between the SET gate and the resonator becomes too strong. This voltage, in our example system, is estimated to be roughly $`4\text{V}`$. As a result, we limit ourselves to $`V_\text{g}4\text{V}`$. At $`V_\text{g}=4\text{V}`$ the steady state energy $`E=8.37\times 10^{27}\text{J}`$, which is below the energy of the first excited state. This corresponds to $`T=0.61\text{mK}`$, and $`N=0.555`$. Thus, if the energy were to be measured directly, immediately after turning off the feedback, energy jumps as a signature of quantum behavior may well be observable. As an indication of the return from increasing the gate voltage, the steady state energy is $`E=1.48\times 10^{26}\text{J}`$ for $`V_\text{g}2\text{V}`$, which corresponds to $`N=1.36`$.

In Figure 3 we plot the theoretical estimates for the achievable steady-state temperature as a function of $`V_\text{g}`$ for a range of starting temperatures. The solid lines correspond to the absolute minima, and the dotted lines to the minima under the restriction that $`k\beta /4`$. Of particular interest is the fact that for a starting temperature of $`2\text{K}`$ (ie. with pumped liquid He), we obtain minimum temperatures in the range of $`50\text{mK}`$. Thus, even for an initial temperature of $`2\text{K}`$, feedback cooling might well be able to compete with dilution refrigerators. If the resonator is first cooled in a dilution refrigerator, and then feedback cooled, then the semi-classical theory predicts achievable temperatures below $`1\text{mK}`$. In Figure 4 we plot the dependence of the minimum temperature on $`V_\text{g}`$ for a range of quality factors, which shows that final temperatures may be increased somewhat by increasing the $`Q`$.

## VI Discussion and Conclusion

The results obtained above are consistent with heuristic arguments. The response of cooling to the measurement strength is as expected: for very weak continuous measurements, we do not learn enough about the state of the system to cool it effectively, and can in fact heat the system due to acting on our poor information. For very strong continuous measurements, we gain sensitivity, but inject more quantum back-action, and approach a minimum only asymptotically. The range of improvement is limited, however, and beyond a few volts, the benefits may not warrant the additional effort.

Higher drain-source voltages provide a larger signal-to-noise ratio, and therefore improve cooling. However, since we do not know exactly how our approximations will fail as $`V_{\text{ds}}`$ approaches $`e/C_\mathrm{\Sigma }`$, and we lack a complete theory of the SET once more than 2 island states need to be taken into account, we have chosen to stay below that limit.

We have made a few additional simplifying assumptions, as a way to indicate a goal, rather than an immediately achievable experimental realization. First, we have assumed a perfectly efficient (and infinite bandwidth) measurement – that is, that no electron passes the detector without being detected. While detection efficiency is not as much of a problem here as in optical experiments, detectors will necessarily be inefficient to some extent. Second, we have assumed perfect, noiseless feedback. In reality, the actuating gate applying the feedback voltage will not provide a perfect noiseless voltage. Also, we have assumed that the actuating gate does not affect the SET. This last assumption is realistic, however, for two reasons. First, the resonator itself acts as a shield between the gate and the SET. Second, since the observer knows the voltage on the feedback gate, she can subtract that effect off the SET signal, while adding some noise.

As mentioned previously, a quantum mechanical harmonic oscillator and a classical one are indistinguishable as long as the wave function is Gaussian, which is the case in the present analysis. Therefore, although the oscillator is near the quantum mechanical ground state, the SET measurement of position will not show any quantum behavior. In the face of these limitations, it is a pleasant result that experimentally obtainable situations today allow for the feedback cooling of an resonator to the point that quantum behavior could become distinguishable from classical behavior with an appropriate measurement scheme.

###### Acknowledgements.

The authors would like to thank Miles Blencowe, Alexander Korotkov, Daniel Steck, Howard Wiseman, Bernard Yerke, and Yong Zhang for helpful conversations and suggestions. Figure 1 is reprinted courtesy of Los Alamos Science. This research was supported in part by the Department of Energy, under contract W-7405-ENG-36.

## Appendix A The Spectra of the SET shot noise and back-action

Here we discuss briefly how the expressions for the shot noise and back-action of the position measurement via a SET are obtained. For more details the reader is referred to Zhang and Blencowe Zhang , (from which we obtain most of the following expressions) and Korotkov Korotkov94 .

The SET consists of a central island, which electrons tunnel in and out of via junctions on either side. If one requires that the spacing between the energy levels of the electron states on the island are sufficiently large compared to the voltage drop across the SET, then only two island states will be appreciably populated, these being the states in which there are $`n`$ and $`n+1`$ electrons on the island, for some $`n`$. This is because the transition rates which connect these states to the other states are suppressed. The value of $`n`$ can be set by biasing the central island. In particular, $`n`$ is determined by the condition

$$n<\left(\frac{C_\text{g}}{e}\right)\left(V_gV_{\mathrm{ds}}/2\right)<n+1.$$
(42)
As a result, we can write a master equation for the probability density for the occupation of the two states. Denoting this density by $`\stackrel{~}{\sigma }=(\sigma (n),\sigma (n+1))^T`$, we have

$$\frac{d\stackrel{~}{\sigma }}{dt}=\left(\begin{array}{cc}a(n)& b(n+1)\\ a(n)& b(n+1)\end{array}\right)\stackrel{~}{\sigma },$$
(43)
where $`a(n)`$ is the transition rate from $`n`$ to $`n+1`$, and $`b(n+1)`$ is the transition rate from $`n+1`$ to $`n`$.

If we denote the tunneling rates into the island across the source junction and the drain junction (see Fig. 1) as $`a_{}(n)`$ and $`a_+(n)`$ respectively (the plus and minus subscripts record whether the tunneling event has a positive or negative contribution to the SET current), and out of the island as $`b_+`$ and $`b_{}`$, respectively, then

$`a(n)`$ $`=`$ $`a_+(n)+a_{}(n),`$ (44)
$`b(n+1)`$ $`=`$ $`b_+(n+1)+b_{}(n+1).`$ (45)
It is also useful to define

$`f(n)`$ $`=`$ $`a_+(n)a_{}(n),`$ (46)
$`g(n+1)`$ $`=`$ $`b_+(n+1)b_{}(n+1).`$ (47)
In what follows we will repress the arguments of these functions, so that $`aa(n)`$, $`bb(n+1)`$ etc. The solution to the master equation is

$`\stackrel{~}{\sigma }(t)=\left[\left(\begin{array}{cc}\hfill b& \hfill b\\ \hfill a& \hfill a\end{array}\right)+\left(\begin{array}{cc}\hfill a& \hfill b\\ \hfill a& \hfill b\end{array}\right)e^{(a+b)t}\right]{\displaystyle \frac{\stackrel{~}{\sigma }(0)}{(a+b)}}.`$ (52)
From this it is straightforward to calculate the average steady state current flowing through the SET, the noise spectra of the current, $`S_\text{I}(\omega )`$, along with that of an arbitrary function, $`\varphi (n)`$, of the island electron number $`S_\varphi (\omega )`$, and their mutual correlation spectrum, $`C(\omega )`$. The average current is

$`I=(ag+bf)/(a+b),`$ (53)
and the spectra are

$$S_\varphi (\omega )=\frac{2ab}{(a+b)}\frac{[\varphi (n)\varphi (n+1)]^2}{(a+b)^2+\omega ^2}$$
(54)
$$S_\text{I}(\omega )=\frac{2e^2C^2}{(a+b)C_\mathrm{\Sigma }^2}\left[ab+\frac{(fg)(a^2gb^2f)}{(a+b)^2+\omega ^2}\right]$$
(55)
$$C^2(\omega )=\frac{(ag+bf)^2(ab)^2+\omega ^2(agbf)^2}{4ab\left[ab\left[(a+b)^2+\omega ^2\right]+(fg)(a^2gb^2f)\right]}$$
(56)
Since the force from the island on the resonator is given by Zhang

$$F=\frac{C_\text{g}(2CC_\text{g})}{2C_\mathrm{\Sigma }^3d}[C(V_{\text{ds}}2V_\text{g})ne]^2,$$
(57)
using Eq. (54) we have

$$S_\text{F}(\omega )=\frac{abe^2C_\text{g}^2(2CC_\text{g})^2}{2(a+b)C_\mathrm{\Sigma }^6d^2}\frac{[C(V_{\text{ds}}2V_\text{g})e(2n+1)]^2}{(a+b)^2+\omega ^2}$$
(58)
Recall that in deriving these expressions we require that the two-level approximation is valid, and this demands that

$`V_{\text{ds}}`$ $``$ $`e/C_\mathrm{\Sigma },`$ (59)
$`k_BT`$ $``$ $`eV_{\text{ds}}.`$ (60)
The tunneling rates are given by

$`a_\pm (n)`$ $`=`$ $`{\displaystyle \frac{(\mathrm{\Delta }n\pm \stackrel{~}{V}_{\mathrm{ds}})/(R_jC_\mathrm{\Sigma })}{1\mathrm{exp}\left[(\mathrm{\Delta }n\pm \stackrel{~}{V}_{\mathrm{ds}})/\stackrel{~}{T}\right]}},`$
$`b_\pm (n+1)`$ $`=`$ $`{\displaystyle \frac{(\mathrm{\Delta }n\pm \stackrel{~}{V}_{\mathrm{ds}})/(R_jC_\mathrm{\Sigma })}{1\mathrm{exp}\left[(\mathrm{\Delta }n\pm \stackrel{~}{V}_{\mathrm{ds}})/\stackrel{~}{T}\right]}},`$
where

$`\mathrm{\Delta }n`$ $`=`$ $`{\displaystyle \frac{C_gV_g}{e}}{\displaystyle \frac{C_gV_{\mathrm{ds}}}{2e}}n{\displaystyle \frac{1}{2}},`$ (61)
$`\stackrel{~}{V}_{\mathrm{ds}}`$ $`=`$ $`{\displaystyle \frac{C_\mathrm{\Sigma }V_{\mathrm{ds}}}{2e}},`$ (62)
$`\stackrel{~}{T}`$ $`=`$ $`{\displaystyle \frac{C_\mathrm{\Sigma }k_BT}{e^2}}.`$ (63)
Note that the condition which determines $`n`$ (Eq. (42)) is equivalent to $`0.5<\mathrm{\Delta }n<0.5`$.

From the expressions for the noise spectra we see that both sources of noise are effectively white (independent of $`\omega `$) so long as $`\omega ^2`$ is much less than $`[a(n)+b(n+1)]^2`$. If this is the case then the simple quantum theory of continuous position measurement presented in the main body of the paper provides a good model for the SET measurement. Note that the actual back-action noise on the position of the resonator is the force noise filtered through the resonator spectral function. This is therefore

$$S_X^F(\omega )=\frac{S_F(\omega )/m_{\mathrm{eff}}^2}{(\omega ^2\omega _0^2)^2+\omega ^2\omega _0^2/Q^2},$$
(64)
and has the same form as that predicted using the quantum mechanical model (Eq. (11)), so long as the force noise is white.

We must therefore evaluate $`[a(n)+b(n+1)]^2`$ for the range of parameters of interest, and verify that it is much larger than $`\omega ^2`$ over the relevant frequency range. First we note that the form of the spectral equations is such that they are periodic in the gate voltage. That is, the values of $`a(n)`$ and $`b(n+1)`$ depend only on $`\mathrm{\Delta }n`$, not on the particular value of $`n`$ in question. As a result we merely need evaluate $`[a(n)+b(n+1)]^2`$ for a single value of $`n`$, and check all values of $`\mathrm{\Delta }n`$ between -0.5 and 0.5.

Substituting in realistic parameter values (those that we use in our examples in the body of paper) in Eqs.(A) and (A), we find that, regardless of the value of $`\mathrm{\Delta }n`$,

$`[a(n)+b(n+1)]`$ $``$ $`2\times 10^{10}`$ (65)
for the range of initial temperatures that we consider, and this is much greater than the range of $`\omega `$ relevant for the dynamics of the resonator, as required. Thus, we can drop $`\omega `$ from the expressions for the spectra, Eqs.(55), (58) and (56), and use these to determine the parameters $`k`$, $`\beta `$ and $`\kappa `$ in the model of the quantum position measurement.


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# Study of interaction of high-power Ar+ laser beam with Ag+-doped glass

## 1 Introduction

Nonlinear optical materials, such as glasses doped with metallic clusters, are promissing ones for optical switching technology . These materials, because of their high transparency; ease of fabrication; durability and thermomechanical stability, are essential component parts of functional devices for optical communications, sensing and computing. Metal nano-cluster composites are particularly interesting because, depending on the choice of the metal and the dielectric host, they exhibit different pico-second relaxation times, range of chemical reactivities, and photo-sensitivities

Several methods have been reported on producing and manipulating of metal-cluster doped-glasses: Low-mass ion irradiation, annealinig in hydrogen atmosphere after the ion-exchange (IE) process, and induced modifications of nano-clusters by pulsed laser beam.

In this paper, we report the results of interaction of a CW high-power Ar+ laser beam with Ag+-doped glass samples, in two regimes of “slow” (SR) and “fast” (FR). In the SR, the power of the pump beam has been increased from $`0.1mW`$ to $`8W`$ in a period of $`90`$ minutes ( $`0.5W`$ increment per 5 minutes ). In the FR, the power is increased up to $`8W`$ in 1 minute. The irradiation of the samples has been performed after the IE step.

The outcome of the SR results show that a 410 nm peak is appeared in the absorption spectrum and the peak in the UV region of the spectrum has been blue-shifted relative to that of non-irradiated samples. The appearance of the 410 nm band peak implies the generation of neutral Ag clusters, and the blue-shift of the peak in the UV region implies the generation of smaller clusters. Both these features can be explained on the basis of possible fragmentation processes of the ionized nano-clusters. The evolution of these peaks are found to depend on the exposure ($`H=I.t`$, where $`I`$ is the intensity and $`t`$ is the exposure time).

In the FR, also the 410 nm peak is appeared but, in this case, the UV peak is blue-shifted relative to that in the SR results. In addition, in the FR, we have observed the generation of micro-clusters. These experimental facts are discussed in detail in the next section.

The organization of this paper is as follows. In section 2 we explain the details of the experiments and discuss the results. Section 3 is devoted to the density-functional calculations of the possible fragmentations of singly-ionized and doubly-ionized silver clusters, and finally, we conclude our work in section 4.

## 2 Experiments and discussions

In our experiments, the samples are prepared using the well-known ion-exchange (IE) method. In the IE process, some of the Ag+ ions in the molten salt and the Na+ ions in the glass matrix are exchanged by diffusion through the interfaces at both sides. The diffusion depth and the concentration of the Ag+ ions in the glass matrix depend on the temperature of the molten salt, the IE duration, and the Ag+ concentration in the molten salt. In this experiment, we insert a glass slide ($`20\times 30\times 1.8`$ mm)into the molten NaNO3/AgNO3 mixed-salt ($`98\%/2\%`$) of temperature 320 $`{}_{}{}^{}C`$ for 4 hours (Fig. 1). The glass components of our samples are specified in Table 1. The setup used to study the interaction of Ar+ laser (pump beam) with the prepared samples is sketched in Fig. 2. In this setup, the samples are subjected to the pump beam at the angle of incidence close to the normal. We have performed the experiments in two regimes of irradiation: The SR and the FR. Depending on which regime is chosen, different outcomes result in.

One of the common features observed in both regimes, during the irradiation process, is the formation of a micro-lens at the incidence point due to thermal effects induced by the pump beam. Formation of the micro-lens is implied by the appearance of a circular interference pattern on the screen (Fig. 2 top left). This pattern is generated due to interference of the reflected beams from the front and back sides of the sample, which have obtained different radii of curvatures (In the SR, the formation of this micro-lens is initiated beyond a threshold of $`P_t4`$ W). For a fixed intensity of the pump beam, the radii of these pattern rings increase with the exposure time up to a limiting value for which a local thermal equilibrium has been achieved. The other common feature, observed in both regimes, is the appearance of a 410 nm band peak and weakening of the peak at the UV region of the absorption spectra (Fig.3).In this work, all spectra have been measured using a Varian Cary-5 UV-Vis-NIR spectrophotometer. The dimension-less quantity $`D`$ in the absorption spectra refers to the optical density

$$D=\mathrm{log}(\frac{I}{I_0}),$$
(1)
where, $`I`$ is the intensity of the probe beam and $`I_0`$ is the intensity of the reference beam in the spectrophotometer. The 410 nm peak is resulted from the excitation of the surface plasmons of neutral silver clusters. The neutral silver clusters can be created through different possible processes. In a fragmentation process, an ionized cluster may decay to smaller parts, one of which could be a neutral cluster. These fragmentation processes are discussed in detail in section 3. Another process could be the capture of the electron, detached from another cluster.

However, there are remarkable differences in the spectra of the two regimes: In the FR (curve 1 of Fig. 4), the 410 nm peak is narrower and higher than that of the SR (curve 2 of Fig.4). In addition, a blue-shift is modulated on the UV peak of the FR spectra compared to that of the SR. The blue-shift in the spectra of the FR implies the production of smaller clusters due to fragmentation The difference in the shapes of the 410 nm peaks in the two regimes originates from the different size distributions of the clusters in the irradiated samples. In general, a sharper peak implies a sharper size distribution of clusters.

### 2.1 Results under the Slow Regime

Under the SR condition, we notice the creation of neutral Ag clusters, which is implied by the appearance of a 410 nm band peak in the absorption spectra (Curve 2, Fig. 4).

To analyze the spectra from different parts of the interaction region, we have divided the circular-shape interaction region into smaller sub-regions, along the diameter, separated by $`0.2mm`$ and have measured their respective spectra. The results are shown in Fig. 5. Labels 1, 2, $`\mathrm{}`$, 12 in Fig. 5 correspond to the sub-regions from the outer parts towards the center of the interaction region, respectively. As is seen, with moving towards the center, the height of the 410 nm peak increases and at the same time, the height of the UV-region peak decreases. This decrease is accompanied by a blue-shift. These behaviors are explained as follows. It is well-known that the intensity profile across the laser beam is Gaussian, i.e., the central part of the interaction region receives more photons than the outer parts. Knowing this fact, and considering the curves 1, 2, $`\mathrm{}`$, 12 of Fig. 5 one can argue that, the more photons received by the sample glass, the more fragmentations of the clusters are induced. As a result of these fragmentations, the neutral Ag clusters are produced. We will show in section 3 that for large ionized clusters the fragmentations in which one of the products is neutral, are most favored (evaporation processes).

In Fig. 6, we have plotted the height of the 410 nm absorption peak as a function of the radial distance in the interaction region. The heights are normalized to the maximum height at the center. The center of the interaction region is located at point 2.4 mm (The size of the interaction region is taken to be 4.8 mm). This plot re-confirms the Gaussian intensity distribution.

The relative blue-shifts of the peaks at the UV region of the absorption spectra in different sub-regions (Fig. 5), imply that the sizes of the clusters decrease as we move towards the central sub-region (the UV peak corresponds to the volume plasmon excitations of Ag clusters \[See Ref. References, page 35\]). At the same time, one sees that the height of the UV peak decreases by moving towards the central sub-region. This weakening is due to the decrease in the concentration of clusters as a result of interaction with the pump beam. In fact, the pump beam causes the clusters fragment and scatter in such a way that the conservation of momentum is satisfied.

Some of the mechanisms underlying the production of the neutral clusters, responsible for the 410 nm peak, could be the following chain fragmentation:

$`\mathrm{Ag}_N^++\mathrm{photon}`$ $``$ $`\mathrm{Ag}_{Np}^++\mathrm{Ag}_p,`$ (2)
$`\mathrm{Ag}_{Np}^++\mathrm{photon}`$ $``$ $`\mathrm{Ag}_{Npp^{}}^++\mathrm{Ag}_p^{},`$
$`\mathrm{Ag}_{Npp^{}}^++\mathrm{}`$ $``$ $`\mathrm{}.`$
The fragmentation of large multiply ionized clusters (if any) are less favored because, they require photons with higher energies. The theoretical calculations related to the fragmentations of silver clusters has been discussed in section 3.

Another mechanism for production of the neutral clusters is recombination of the singly ionized clusters with the electrons detached from other possible neighboring sources (glass matrix):

$$\mathrm{Ag}_M^++\mathrm{e}^{}\mathrm{Ag}_M.$$
(3)
Heating the non-irradiated ion-exchanged samples, under the normal atmosphere conditions for temperature beyond the ion-exchange temperature, leads to the appearance of 410 nm peak in the absorption spectra and a red-shift in the UV peak of the absorption spectra (Fig. 7). This experimental observation justifies the mechanism of Eq. (3).

### 2.2 Results under the fast regime

Under the FR condition, as under the SR, the creation of the 410 nm peak is observed. Comparing the absorption spectra of the central parts of the interaction regions in the two regimes, reveal that in the FR, this peak is narrower and higher; and in addition, the UV peak is blue-shifted as well as decreased relative to that in the SR results (Curve 1, Fig. 4). As mentioned before, a sharper peak corresponds to a sharper size distribution of clusters, and the blue-shift of the UV peak is related to the production of smaller clusters. To understand the detailed mechanisms responsible for these differences between the SR and the FR, more experimental investigations are needed.

In addition to the above-mentioned differences, under the FR, we have observed the generation of micrometer clusters. This experimental fact is discussed as follows.

After the irradiation under the FR, the appearance of large ($`\mu m`$) neutral Ag clusters has been observed at both sides of the sample. The distributions of the $`\mu `$m-clusters at the two sides have significant differences. The observations have been done by an optical microscope using bright-field photography method.

On the front side, the neutral $`\mu `$m-clusters are resided in a ring-shape area as islands. Each of these islands is formed, at a nucleation center, by absorbing its surrounding nano-clusters \[Fig. 8(a)-(c)\]. The nucleation centers mostly lie in relatively cold regions in the glass matrix which corresponds to the lower-intensity parts of the incidence area (the laser beam has a gaussian profile of intensity). However, because of the inhomogenity of the glass matrix, some parts in the inner region have also higher viscousities which serve as nucleation centers. Due to the radial gradient in the laser-beam intensity, the radiation pressure varies in the radial direction which, in turn, cause the relatively larger clusters ($`d\lambda /20`$)in the central-part be pushed away from the center. The radial velocities of the clusters decrease with distance from the center. Thus, they can aggregate mostly in the ring-shape region. On the back side of the sample, on the other hand, the $`\mu `$m-clusters are seen to be distributed more or less uniformly in a disc-shape area, centered at the beam center \[Fig. 8(d), (e)\]. This difference in the distributions at the front and back sides can easily be explained by comparing the beam intensities at these two sides. On measuring the transmittance of the beam for each line of the laser beam, we conclude that during the irradiation, the intensity at the back side is much less than the front side (Table 2), so that the mobility of the clusters is much less than that of the front side. This cause the back-side clusters not to be pushed away from the center but, just aggregate at those nucleation centers which correspond to the more viscous parts of the glass matrix. To our knowledge, the formation of the $`\mu `$m-sized silver clusters in the glass matrix under the action of a CW laser beam has not been reported.

## 3 Theoretical study of the fragmentation processes

In the context of stabilized jellium model (SJM) and self-consistent solution of the Kohn-Sham (KS) equations in the density functional theory with local spin-density approximation, we have calculated the total energies of Ag clusters and thereby obtained the energies needed for the fragmentation via different decay channels. In the SJM, the discrete ions are replaced by a uniform positive charge background of density $`n=3/4\pi r_s^3`$ in which $`r_s`$ is the bulk value of the Wigner-Seitz (WS) radius of the valence electrons of the metal and for Ag, $`r_s=3.02bohrs`$. The geometry chosen for the positive background is spherical. We have studied the binary decay processes of positively charged Ag$`{}_{}{}^{+}{}_{N}{}^{}`$, Ag$`{}_{}{}^{2+}{}_{N}{}^{}`$ clusters containing up to $`N=100`$ atoms in all possible channels. We have considered the following possible decay processes for singly ionized Ag clusters

$$\mathrm{Ag}_N^{1+}\mathrm{Ag}_{Np}^{1+}+\mathrm{Ag}_p^0,p=1,2,\mathrm{},N1.$$
(4)
For doubly charged clusters, the decays can proceed via two different processes. The first one is the evaporation process

$$\mathrm{Ag}_N^{2+}\mathrm{Ag}_{Np}^{2+}+\mathrm{Ag}_p^0,p=1,2,\mathrm{},N3$$
(5)
and the second one is fission into two charged products

$$\mathrm{Ag}_N^{2+}\mathrm{Ag}_{Np}^{1+}+\mathrm{Ag}_p^{1+},p=1,2,\mathrm{},[N/2].$$
(6)
In evaporation processes, the negativity of the difference between total energies before and after fragmentation (dissociation energy),

$$D^Z(N,p)=(E_{Np}^Z+E_p^0)E_N^Z,$$
(7)
is sufficient to have a spontaneous decay. However, in fission processes, because of the possible existence of a fission barrier, the negativity of the dissociation energy is not a sufficient condition for the fission of the parent cluster. In Fig. 9, the fission of a $`Z`$-ply charged $`N`$-atom cluster into two clusters of respective sizes $`N_1,N_2=NN_1`$, and respective charges $`z_1,z_2=Zz_1`$ is schematically shown. For the fission, we have used the two-spheres approximation. $`Q_f`$ is the energy release, $`B_c`$ is the fusion barrier which is equal to the maximum energy of the Coulomb interaction of two positively-charged conducting spheres, taking their polarizabilities into account. $`B_f`$ is the fission barrier height which is defined as

$$B_f=Q_f+B_c.$$
(8)
The Coulomb interaction energy of two charged metal spheres has been numerically calculated using the classical method of image charges. The calculations show that the maximum of the interaction energy is achieved for separations $`d_0R_1+R_2`$. The most favored channel for the evaporation is defined as the channel for which the dissociation energy is minimum. Similarly, the most favored channel for the fission has the minimum of the barrier height.

### 3.1 Calculation of the total energy of a cluster

In the context of the SJM, the total energy of an $`N`$-atom $`Z`$-ply charged cluster is given by

$`E_{\mathrm{SJM}}[n_{},n_{},n_+]`$ $`=`$ $`E_{\mathrm{JM}}[n_{},n_{},n_+]+\left(\epsilon _M(r_s^B)+\overline{w}_R(r_s^B,r_c^B)\right){\displaystyle 𝑑𝐫n_+(𝐫)}`$ (9)
$`+\delta v_{\mathrm{WS}}(r_s^B,r_c^B){\displaystyle 𝑑𝐫\mathrm{\Theta }(𝐫)\left[n(𝐫)n_+(𝐫)\right]},`$
where

$`E_{\mathrm{JM}}[n_{},n_{},n_+]`$ $`=`$ $`T_s[n_{},n_{}]+E_{xc}[n_{},n_{}]`$ (10)
$`+{\displaystyle \frac{1}{2}}{\displaystyle 𝑑𝐫\varphi ([n,n_+];𝐫)\left[n(𝐫)n_+(𝐫)\right]}`$
and

$$\varphi ([n,n_+];𝐫)=𝑑𝐫^{}\frac{\left[n(𝐫^{})n_+(𝐫^{})\right]}{\left|𝐫𝐫^{}\right|}.$$
(11)
Here, $`n=n_{}+n_{}`$ which satisfies $`𝑑𝐫n(𝐫)=NZ`$, and $`n_+`$ is the jellium density which satisfies $`𝑑𝐫n_+(𝐫)=N`$. $`\mathrm{\Theta }(𝐫)`$ takes the value of unity inside the jellium background and zero, outside. The first and second terms in the right hand side of Eq.(10) are the non-interacting kinetic energy and the exchange-correlation energy, and the last term is the Coulomb interaction energy of the system. The quantity $`\delta v_{\mathrm{WS}}`$ is the average of the difference potential over the Wigner-Seitz cell and the difference potential, $`\delta v`$, is defined as the difference between the pseudo-potential of a lattice of ions and the electrostatic potential of the jellium positive background. All equations throughout this paper are expressed in atomic units ($`\mathrm{}=e^2=m=1`$), otherwise, they will be explicitly specified. Using the Eq. (21) of Ref. \[References\], this average value is given by

$$\delta v_{\mathrm{WS}}(r_s^B,r_c^B)=\frac{3(r_c^B)^2}{2(r_s^B)^3}\frac{3}{10r_s^B},$$
(12)
where, $`r_c^B`$ is the core radius of the pseudo-potential and is given by

$$r_c^B=\frac{1}{3}(r_s^B)^{3/2}\left\{\left[2t_s(r_s)\epsilon _x(r_s)+r_s\frac{}{r_s}\epsilon _c(r_s)\epsilon _M(r_s)\right]_{r_s=r_s^B}\right\}^{1/2}.$$
(13)
The quantities $`t_s`$, $`\epsilon _x`$, and $`\epsilon _c`$ are the kinetic, exchange, and correlation energies per electron, respectively. The effective potential, used in the self-consistent KS equations, is obtained by taking the variational derivative of the SJM energy functional with respect to the spin densities as

$`v_{eff}^\sigma ([n_{},n_{},n_+];𝐫)`$ $`=`$ $`\varphi ([n,n_+];𝐫)+v_{xc}^\sigma ([n_{},n_{}];𝐫)+\mathrm{\Theta }(𝐫)\delta v_{\mathrm{WS}}(r_s^B,r_c^B),`$ (14)
where $`\sigma =,`$. By solving the KS equations

$$\left(\frac{1}{2}^2+v_{eff}^\sigma (𝐫)\right)\psi _i^\sigma (𝐫)=\epsilon _i^\sigma \psi _i^\sigma (𝐫),\sigma =,,$$
(15)
and finding the self-consistent values for $`\epsilon _i^\sigma `$ and $`\psi _i^\sigma `$, with

$$n(𝐫)=\underset{i(occ),\sigma =,}{}|\psi _i^\sigma (𝐫)|^2,$$
(16)
the total energy of a cluster is calculated.

### 3.2 Results of Calculations

After the self-consistent calculations, we have calculated the total energies of Ag$`{}_{}{}^{Z}{}_{N}{}^{}`$ ($`Z`$=0,1,2) for different cluster sizes $`(1N100)`$. Then, using Eqs. (7) and (8), we have calculated the dissociation energies and the fission barriers.

In Fig. 10, we have plotted the dissociation energies of the most favored evaporation channels of the singly ionized clusters. We have shown the most favored value of $`p`$ by $`p^{}`$. The solid small square symbols show the most favored values $`p^{}`$ on the right vertical axis whereas, the corresponding dissociation energies, $`D^{1+}(N,p^{})`$, are shown on the left vertical axis by large open squares. As is seen in the figure, there exist some maxima and minima. The maxima of the $`D^Z(N,p^{})`$ correspond to the closed-shell Ag$`{}_{}{}^{+}{}_{N}{}^{}`$ clusters with $`N`$=3, 9, 19, 35, 59,$`\mathrm{}`$. These clusters have high stabilities compared to their neighboring sizes. On the other hand, the minima correspond to the sizes which decay into two closed-shell clusters (for example, Ag$`{}_{11}{}^{+}`$Ag$`{}_{9}{}^{+}+`$Ag2). A negative value for the dissociation energy implies that the cluster is unstable against the spontaneous decay.

In Fig. 11(a), we have shown the most favored products Ag$`{}_{}{}^{0}{}_{p^{}}{}^{}`$ and the dissociation energies $`D^{2+}(N,p^{})`$ for the decay of Ag$`{}_{}{}^{2+}{}_{N}{}^{}`$ via evaporation channel. It is seen that the most favored products are mainly monomers, dimers and octamers. On the other hand, here, the mean dissociation energy is higher than that in the evaporation of singly ionized clusters. That is, here, the number of clusters stable against the spontaneous evaporation is larger than that in the singly ionized case. Evaporation is not the only decay mechanism for multiply charged clusters, and they can also decay via fission processes in which both fragments are charged.

Figure 11(b) shows the barrier heights $`B_f(N,p^{})`$ for the most favored fission channels $`\mathrm{Ag}_N^{2+}\mathrm{Ag}_{Np^{}}^++\mathrm{Ag}_p^{}^+`$. By definition, the most favored fission channel has a minimum value for the barrier height. As is seen, for small clusters, the majority have negative barrier heights. That is, most of them are unstable against spontaneous fission. However, as $`N`$ increases, the number of clusters with negative barrier heights decreases and beyond a certain size range, all the barrier heights become positive.

A doubly charged cluster decays both via evaporation and fission. At small sizes ($`N<21`$), the fission process dominates because, the barrier heights for the fission are lower than the dissociation energies for the evaporation. This situation is shown in Fig. 11(c). As is seen, the competition between the evaporation and fission starts at $`N`$=21. This competition continues with some fluctuations until the evaporation dominates completely. Since, the cluster sizes in the a ion-exchanged sample are of order $``$5 nm, which corresponds to $`N21`$, the fragmentations mostly proceed via the evaporation mechanism.

## 4 Conclusion

We have studied the interaction of a CW laser beam with the clusters embedded in glass matrix. The study consists of two regimes of fast and slow. In both regimes, neutral clusters are generated (creation of a 410 nm band peak). Depending on the regime, different results are obtained. In the slow regime, the absorption peak in the UV region of the spectrum is blue-shifted relative to that of non-irradiated samples, which implies the generation of smaller clusters. On the other hand, under the fast regime, in addition to the fragmentations, clusters of $`\mu `$m size are created. The experimental results show that heat treatment of the ion-exchanged sample under the normal atmosphere conditions also gives rise to the appearance of neutral clusters. The theoretical calculations show that doubly ionized clusters of size $`N21`$ decay mostly via the evaporation mechanism which is one of the possible mechanism for the generation of neutral clusters.

Acknowledgement

The authors are grateful to M. T. Tavassoli for his advice in some experiments. They also appreciate A. Ghoreyshi for determination of components of glass samples. The financial support of this work is provided by research council of the Institute for Advanced Studies in Basic Sciences.


text:
# Information theoretic approach to single-particle and two-particle interference in multi-path interferometers

(18 February 2003)

## Abstract

We propose entropic measures for the strength of single-particle and two-particle interference in interferometric experiments where each particle of a pair traverses a multi-path interferometer. Optimal single-particle interference excludes any two-particle interference, and vice versa. We report an inequality that states the compromises allowed by quantum mechanics in intermediate situations, and identify a class of two-particle states for which the upper bound is reached. Our approach is applicable to symmetric two-partite systems of any finite dimension.

Interference effects of two kinds can be observed in quantum processes that involve pairs of particles. There are the usual single-particle interference fringes and there are phase-dependent coincidence probabilities that constitute two-particle interferences (see, e.g., Horne+1:85 ; Greenberger+2:93 ). As Horne and Zeilinger noted already in 1985 Horne+1:85 , there is a certain complementarity between the two types of interference: Optimal interference of one kind excludes any interference of the other.

The various quantitative studies of the possible trade-off between single-particle and two-particle interference that are on record (see Jaeger+2:93 ; Jaeger+2:95  in particular) are dealing with two-path interferometers for the single particles. It is then possible to measure the strength of the single-particle interference by the familiar Michelson fringe visibility —the difference of maximal and minimal probabilities in one output divided by their sum— and introduce a matching measure for the two-particle interference.

There is, however, no unique analog for multi-path interferometers, even for single-particle interference Weihs+3:96 ; Zukowski+2:97 . Dürr has recently compiled a list of desirable properties of any multi-path generalization of Michelson’s two-path visibility Durr:01 , but quite a few of equally plausible definitions meet the criteria Englert+2:03 , and the extension to two-particle interference is largely unexplored territory.

In an attempt to close this gap, at least partly, we introduce here an information-theoretic definition of the measure of the strength of two-particle interference. It exploits the mutual information contained in the coincidence probabilities. The corresponding single-particle measure is, in some sense, the fringe-contrast analog of the entropic measure for path knowledge that was first used by Wootters and Żurek Wootters+1:79  in 1979 in the context of a two-path interferometer (Young’s double slit), and later also by others (see, e.g., Mittelstaedt+2:87 ; Lahti+2:91 ). But entropic measures of this kind have never been popular and have been criticized occasionally Jaeger+2:95 ; Durr:01 .

Yet, we think that they possess certain advantages. In particular, there is the immediate benefit that the dimensionality of the systems is irrelevant (although we assume, for the purposes of this paper, that the two systems are of the same dimension).

Let us close these introductory remarks by mentioning that the problem studied here is very closely linked with the relations between single-particle fringe visibility and which-path knowledge in quantitative studies of wave-particle duality. Going back to Einstein’s 1905 paper on the photo-electric effect, this intriguing aspect of quantum mechanics is as old as quantum theory itself. Recent studies include Jaeger+2:93 ; Jaeger+2:95 ; Englert:96 ; Englert+1:00 ; Durr:01 ; Jakob+1:03  where also the earlier literature can be found.

Consider an interferometric experiment of the kind that is sketched in Fig. 1. A source emits pairs of entangled particles, one of each pair propagating to observer Alice (A) on the left, the other to Bob (B) on the right, $`N`$ paths being available on either side. Before its registration by the respective detectors, each particle undergoes a unitary transformation consisting of the action of phase shifters (phases $`\varphi _k^{(\mathrm{A})}`$ and $`\varphi _l^{(\mathrm{B})}`$, respectively) and an unbiased symmetric multiport beam splitter. The latter effects the unitary discrete Fourier transformation, $`F`$, that is specified by the matrix elements $`F_{mn}=\gamma _N^{mn}/\sqrt{N}`$ where $`\gamma _N=\mathrm{exp}(2\pi i/N)`$ is the basic $`N`$-th root of unity. Depending on the two-particle state emitted by the source, the resulting paired detector clicks may exhibit correlations that originate in the path interference that is tested by the Fourier transformation in conjunction with the phase shifters. It is our objective here to quantify the strength of the interference observed in experiments of this kind.

The experimental data are the $`N^2`$ coincidence probabilities $`p_{mn}^{(\mathrm{AB})}=p_{mn}^{(\mathrm{AB})}(\varphi _1^{(\mathrm{A})},\mathrm{},\varphi _N^{(\mathrm{A})};\varphi _1^{(\mathrm{B})},\mathrm{},\varphi _N^{(\mathrm{B})})`$, of unit sum, between Alice’s $`m`$-th detector and Bob’s $`n`$-th detector ($`m,n=1,2,\mathrm{},N`$). The relative frequencies of Alice’s and Bob’s individual detection events are given by the marginal sums of $`p_{mn}^{(\mathrm{AB})}`$,

$`p_m^{(\mathrm{A})}(\varphi _1^{(\mathrm{A})},\mathrm{},\varphi _N^{(\mathrm{A})})`$ $`=`$ $`{\displaystyle \underset{n=1}{\overset{N}{}}}p_{mn}^{(\mathrm{AB})},`$
$`p_n^{(\mathrm{B})}(\varphi _1^{(\mathrm{B})},\mathrm{},\varphi _N^{(\mathrm{B})})`$ $`=`$ $`{\displaystyle \underset{m=1}{\overset{N}{}}}p_{mn}^{(\mathrm{AB})}.`$ (1)
In their dependence on the local interferometric phases, $`p_m^{(\mathrm{A})}`$ and $`p_n^{(\mathrm{B})}`$ contain the pertinent information about the phase relations between the $`N`$ paths on Alice’s and Bob’s side, respectively, and information about the $`N^2`$ path pairs can be extracted from the coincidence probabilities $`p_{mn}^{(\mathrm{AB})}`$.

We have mentioned above that Michelson’s standard definition of the fringe visibility for two-path interferometers has no unique generalization for multi-path interferometers. This is so for a simple reason: a single number cannot do full justice to the complex pattern displayed by $`p_m^{(\mathrm{A})}(\varphi _1^{(\mathrm{A})},\mathrm{},\varphi _N^{(\mathrm{A})})`$ or $`p_n^{(\mathrm{B})}(\varphi _1^{(\mathrm{B})},\mathrm{},\varphi _N^{(\mathrm{B})})`$. Thus one must make a judicious choice among the various possible definitions that meet the reasonably obvious criteria on Dürr’s list Durr:01 .

Here we opt for measuring the various interference strengths in terms of the respective Shannon entropies. We shall continue to speak of “visibility” although the analogy with the usual two-path visibility is a bit remote. Alice’s single-particle visibility $`V^{(\mathrm{A})}`$ is then defined in accordance with

$$V^{(\mathrm{A})}=\underset{\varphi _1^{\left(\mathrm{A}\right)},\mathrm{},\varphi _N^{\left(\mathrm{A}\right)}}{\mathrm{max}}\left[1H_N\left(p^{(\mathrm{A})}\right)\right],$$
(2)
where

$$H_N\left(p^{(\mathrm{A})}\right)=\underset{m=1}{\overset{N}{}}p_m^{(\mathrm{A})}\mathrm{log}_Np_m^{(\mathrm{A})}$$
(3)
is the normalized Shannon entropy of her marginal probability distribution, and Bob’s single-particle visibility $`V^{(\mathrm{B})}`$ is defined analogously. For convenient normalization, we take the logarithm to base $`N`$ so that, by construction, both $`H_N\left(p^{(\mathrm{A})}\right)`$ and $`V^{(\mathrm{A})}`$ are nonnegative numbers that do not exceed unity.

The definition of $`V^{(\mathrm{A})}`$ in (2) exploits the fact that path knowledge after a Fourier transformation corresponds to interference strength before the transformation Englert+2:03 . The largest amount of terminal path knowledge that is potentially available for optimally set phase shifters is thus a self-suggesting measure for the interference strength at the input, and the Shannon entropy is one natural quantitative measure of knowledge about a probability distribution—the one we find particularly useful here. This a priori justification of our definition of $`V^{(\mathrm{A})}`$ is, of course, no more than an appeal at plausibility; the definition is ultimately justified by the consequences that we report below.

We note that $`V^{(\mathrm{A})}`$ of (2) reaches its upper bound of unity only for certain pure states of Alice’s particle, namely those for which it is possible to adjust the phases $`\varphi _k^{(\mathrm{A})}`$ such that the particle is surely directed to one particular detector, which is to say that the arriving particle must follow each path with the same probability of $`1/N`$ and that there must be definite relative phases between the paths. It is equally important that $`V^{(\mathrm{A})}`$ vanishes if Alice’s particle arrives along one particular path, in which situation there is no room for relative phases between the paths. Accordingly, $`V^{(\mathrm{A})}`$ vanishes also if the statistical operator $`\rho ^{(\mathrm{A})}`$ of Alice’s particle is a convex sum of pure states that refer to definite paths. In the case of the totally mixed state $`\rho ^{(\mathrm{A})}=1/N`$, we face the extreme situation of utter ignorance in which nothing is predictable about the particle’s path before or after the Fourier transformation.

The single-particle visibility of (2) also meets the indispensable criterion of convexity: The visibility of a convex sum of states cannot exceed the convex sum of the individual visibilities. This is an immediate consequence of the concavity of the Shannon entropy.

As a preparation for the definition of the two-particle visibility $`V^{(\mathrm{AB})}`$ in (5) below, we now consider the interferometric experiment from the perspective of information theory. Imagine that the source and beam splitters are contained in a black box and only the detectors are accessible. We observe paired clicks of the detectors with the coincidence probabilities $`p_{mn}^{(\mathrm{AB})}`$ and, on either side, individual clicks with the marginal probabilities $`p_m^{(\mathrm{A})}`$ and $`p_n^{(\mathrm{B})}`$, respectively. We then wonder about the strength of correlations between clicks of pairs of detectors at opposite sides of the experiment. Obviously, the quantitative measure of two-particle interference should vanish if there are no correlations between the clicks for any setting of the phase shifters and it should be maximal if perfect correlations can be achieved for some setting.

A good candidate for a measure having these properties, and the natural one to accompany the single-particle visibility of (2), is the maximal value of the mutual information $`I\left(p^{(\mathrm{AB})}\right)`$ contained in the $`p_{mn}^{(\mathrm{AB})}`$’s, which is the relative Shannon entropy between the probability distributions $`p_{mn}^{(\mathrm{AB})}`$ and $`p_n^{(\mathrm{A})}p_m^{(\mathrm{B})}`$, that is: between the actual coincidence probabilities and the corresponding products of the marginal probabilities.

For a particular setting of the phase shifters, we have

$`I\left(p^{(\mathrm{AB})}\right)`$ $`=`$ $`H_N\left(p^{(\mathrm{A})}\right)+H_N\left(p^{(\mathrm{B})}\right)H_N\left(p^{(\mathrm{AB})}\right)`$ (4)
$`=`$ $`{\displaystyle \underset{m,n=1}{\overset{N}{}}}p_{mn}^{(\mathrm{AB})}\mathrm{log}_N{\displaystyle \frac{p_{mn}^{(\mathrm{AB})}}{p_n^{(\mathrm{A})}p_m^{(\mathrm{B})}}}.`$
If the two distributions happen to be equal, $`p_{mn}^{(\mathrm{AB})}=p_n^{(\mathrm{A})}p_m^{(\mathrm{B})}`$, then the stochastic variables $`n`$ and $`m`$ are statistically independent, the detector clicks are not correlated, and the mutual information vanishes accordingly. Since it is also bounded, $`0I\left(p^{(\mathrm{AB})}\right)1`$, we are invited to define the two-particle visibility as

$$V^{(\mathrm{AB})}=\underset{\varphi _k^{\left(\mathrm{A}\right)},\varphi _l^{\left(\mathrm{B}\right)}}{\mathrm{max}}I\left(p^{(\mathrm{AB})}\right).$$
(5)
Before proceeding we should not fail to mention the alternative proposal by Jaeger, Horne, and Shimony Jaeger+2:93 . In the context of two-path interferometers, they define a two-particle visibility by a Michelson-type formula for the extremal values of the *difference* $`p_{mn}^{(\mathrm{AB})}p_n^{(\mathrm{A})}p_m^{(\mathrm{B})}`$, and it appears that a systematic study of the possible generalization to multi-path interferometers is lacking. By contrast, our definition involves (the logarithm of) the *ratio* $`p_{mn}^{(\mathrm{AB})}/\left(p_n^{(\mathrm{A})}p_m^{(\mathrm{B})}\right)`$ and is immediately applicable to multi-path interferometers.

We note that the two-particle visibility (5) is maximal, $`V^{(\mathrm{AB})}=1`$, if the source emits a maximally entangled state such as

$$\rho _{\mathrm{max}.\mathrm{ent}.}^{(\mathrm{AB})}=\frac{1}{N}\underset{j,k=1}{\overset{N}{}}|jjkk|,$$
(6)
where $`|jk`$ is the ket vector for one particle in Alice’s $`j`$-th path and the other in Bob’s $`k`$-th path. And if the source emits a product state,

$$\rho ^{(\mathrm{AB})}=\rho ^{(\mathrm{A})}\rho ^{(\mathrm{B})},\rho ^{(\mathrm{A})}=\mathrm{tr}_\mathrm{B}\rho ^{(\mathrm{AB})},\rho ^{(\mathrm{B})}=\mathrm{tr}_\mathrm{A}\rho ^{(\mathrm{AB})},$$
(7)
then $`p_{mn}^{(\mathrm{AB})}=p_n^{(\mathrm{A})}p_m^{(\mathrm{B})}`$ and $`V^{(\mathrm{AB})}=0`$. This limit is also reached in the case of the maximally mixed, or chaotic, state

$$\rho _{\mathrm{chaos}}^{(\mathrm{AB})}=\frac{1}{N^2}\underset{j,k=1}{\overset{N}{}}|jkjk|=\frac{1}{N^2}.$$
(8)
All these features are in complete agreement with what one would expect from a reasonably defined two-particle visibility.

The stage is now set for presenting the central result: For correlations generated by quantum mechanics (arbitrary joint probabilities $`p_{mn}^{(\mathrm{AB})}`$ do not have this property), the inequalities

$$V^{(\mathrm{A})}+V^{(\mathrm{AB})}1,V^{(\mathrm{B})}+V^{(\mathrm{AB})}1$$
(9)
are obeyed by the single-particle visibilities $`V^{(\mathrm{A})}`$, $`V^{(\mathrm{B})}`$ and the two-particle visibility $`V^{(\mathrm{AB})}`$, and there are families of pure two-particle states, $`\rho _\lambda ^{(\mathrm{AB})}=|\lambda \lambda |`$ with $`0\lambda 1`$, for which the equal signs hold with each visibility covering the whole range from $`0`$ to $`1`$. In other words, the inequalities can be saturated.

In view of the complete symmetry between Alice and Bob, it suffices to prove one of the inequalities, say the first one. Consider the experiment of Fig. 2, where we have two observers who can apply arbitrary $`U(N)`$ transformations, $`U_\mathrm{A}`$ and $`U_\mathrm{B}`$, to their respective incoming particles, which arrive in some state $`\rho ^{(\mathrm{AB})}`$ that could be pure or mixed. Since there is no restriction here to Fourier transformations, the more general single-particle visibility $`\stackrel{~}{V}^{(\mathrm{A})}`$ bounds $`V^{(\mathrm{A})}`$ from above,

$$V^{(\mathrm{A})}\stackrel{~}{V}^{(\mathrm{A})}=\underset{U_\mathrm{A}}{\mathrm{max}}\left[1H_N\left(p^{(\mathrm{A})}\right)\right]=1S_N\left(\rho ^{(\mathrm{A})}\right),$$
(10)
where $`S_N(\rho )=\mathrm{tr}\left\{\rho \mathrm{log}_N\rho \right\}`$ is the scaled von Neumann entropy of the reduced state $`\rho ^{(\mathrm{A})}`$. The maximum in (10) is reached for those $`U_\mathrm{A}`$ that diagonalize $`\rho ^{(\mathrm{A})}`$.

To find a corresponding upper bound for the two-particle visibility, we first note that

$`V^{(\mathrm{AB})}\stackrel{~}{V}^{(\mathrm{AB})}`$ $`=`$ $`\underset{U_\mathrm{A},U_\mathrm{B}}{\mathrm{max}}[H_N\left(p^{(\mathrm{A})}\right)+H_N\left(p^{(\mathrm{B})}\right)`$ (11)
$`H_N\left(p^{(\mathrm{AB})}\right)]`$
and then observe that

$`H_N\left(p^{(\mathrm{AB})}\right)H_N\left(p^{(\mathrm{B})}\right)`$ $`=`$ $`{\displaystyle \underset{m,n=1}{\overset{N}{}}}p_{mn}^{(\mathrm{AB})}\mathrm{log}_N{\displaystyle \frac{p_{mn}^{(\mathrm{AB})}}{\underset{m^{}}{}p_{m^{}n}^{(\mathrm{AB})}}}`$ (12)
$``$ $`0.`$
As a consequence, we get $`V^{(\mathrm{AB})}\stackrel{~}{V}^{(\mathrm{AB})}S_N\left(\rho ^{(\mathrm{A})}\right)`$. In conjunction with (10) this implies the first inequality in (9), and then the second inequality follows from the symmetry of the setup.

Alternatively, we can estimate the two-particle visibility by an information-theoretic argument. When Bob performs his unitary transformation $`U_\mathrm{B}`$ and then registers a click of his $`n`$-th detector, it is *as if* he prepared Alice’s particle in the state described by

$$\rho _n^{(\mathrm{A})}=\frac{1}{p_n^{(\mathrm{B})}}\mathrm{tr}_\mathrm{B}\left\{P_n^{(\mathrm{B})}U_\mathrm{B}^{}\rho ^{(\mathrm{AB})}U_\mathrm{B}\right\},$$
(13)
where $`P_n^{(\mathrm{B})}`$ is the projector corresponding to a click of his $`n`$-th detector. In effect, Alice applies her $`U_\mathrm{A}`$ to $`\rho _n^{(\mathrm{A})}`$ and then detects her particle.

The process of finding the two-particle visibility in the experiment can now be understood as a communication protocol where Alice and Bob collaborate to obtain the maximal mutual information in the B-to-A quantum channel with the restriction that only projective measurements are allowed. The well known Holevo bound Holevo:73  limits the available mutual information in situations of this kind. In the particular case under consideration, the Holevo bound reads

$$I\left(p^{(\mathrm{AB})}\right)S_N\left(\rho ^{(\mathrm{A})}\right)\underset{U_\mathrm{B}}{\mathrm{min}}\left\{\underset{n=1}{\overset{N}{}}p_n^{(\mathrm{B})}S_N\left(\rho _n^{(\mathrm{A})}\right)\right\}.$$
(14)
Since the subtracted term is nonnegative, it follows that $`V^{(\mathrm{AB})}S_N\left(\rho ^{(\mathrm{A})}\right)`$, and the argument concludes as above.

To prove the second assertion at (9), namely that the upper bound for the sums of single-particle and two-particle visibilities in (9) is tight, we consider the following one-parameter family of pure states

$$\rho _\lambda ^{(\mathrm{AB})}=|\lambda \lambda |,|\lambda =\frac{|0(1\lambda )+|1\lambda \sqrt{N}}{\sqrt{1+(N1)\lambda ^2}},$$
(15)
where we have, for $`\lambda =0`$, the ket vector

$$|0=\frac{1}{\sqrt{N}}\underset{k=1}{\overset{N}{}}|kk$$
(16)
of the maximally entangled state (6) and, for $`\lambda =1`$, the ket vector

$$|1=\frac{1}{N}\underset{j,k=1}{\overset{N}{}}|jk=\left(F_\mathrm{A}F_\mathrm{B}\right)^1|NN$$
(17)
of the product state that is obtained from $`|NN`$ by two-fold inverse Fourier transformation. The normalizing denominator in (15) takes $`0|1=1/\sqrt{N}`$ into account.

If the source emits the two-particle state $`\rho _\lambda ^{(\mathrm{AB})}`$ and all phases $`\varphi _k^{(\mathrm{A})}`$, $`\varphi _l^{(\mathrm{B})}`$ are set to zero, then the coincidence probabilities are $`p_{mn}^{(\mathrm{AB})}=\left|mn|\lambda \right|^2`$. The ingredients of the probability amplitude are

$`mn|F_\mathrm{A}F_\mathrm{B}|0`$ $`=`$ $`{\displaystyle \frac{\delta _{m+n,N}^{(N)}}{\sqrt{N}}},`$
$`mn|F_\mathrm{A}F_\mathrm{B}|1`$ $`=`$ $`mn|NN=\delta _{m,N}^{(N)}\delta _{n,N}^{(N)},`$ (18)
where the periodic Kronecker delta $`\delta _{j,k}^{(N)}`$ is $`1`$ if $`j=k`$ modulo $`N`$, and $`0`$ otherwise. The resulting probabilities

$$p_{mn}^{(\mathrm{AB})}=\frac{\left[(1\lambda )\delta _{m+n,N}^{(N)}+N\lambda \delta _{m,N}^{(N)}\delta _{n,N}^{(N)}\right]^2}{N[1+(N1)\lambda ^2]}$$
(19)
exhibit perfect correlations inasmuch as for each $`m`$ value there is only one $`n`$ value for which $`p_{mn}^{(\mathrm{AB})}0`$. As a consequence then, all summands vanish in the double sum of (12), which in turn implies

$$1=\left[1H_N\left(p^{(\mathrm{A})}\right)\right]+I\left(p^{(\mathrm{AB})}\right)V^{(\mathrm{A})}+V^{(\mathrm{AB})}1,$$
(20)
so that equal signs must hold throughout. Indeed, the upper bound in (9) is reached for all $`\lambda `$, with $`V^{(\mathrm{AB})}=1`$ for $`\lambda =0`$ and $`V^{(\mathrm{AB})}=0`$ for $`\lambda =1`$, and all intermediate values in between.

###### Acknowledgements.

MŻ and BGE gratefully acknowledge the splendid hospitality extended to them at the National University of Singapore. This work was supported by AStar Grant No. 012-104-0040, by KBN project No. 5 PO3B 088 20, and also by the Telecommunication and Informatics Task Force (TITF) initiative of Texas A&M University.