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# Theory of four-wave mixing and accompanying dissociation and population transfer controlled with laser-induced continuum structures

## Contents

1. Introduction 2

2. Four-wave mixing, absorption and refractive indices in ladder
energy-level schemes controlled by interference of two LICS 4
2.1. Equations for coupled electromagnetic waves and their solution 4
2.2. Density matrix master equations and their solutions 5
2.3. Laser-induced structures in absorption and refraction spectra
at discrete and continuous transitions 9
2.4. Resonance sum-frequency generation in strongly-absorbing media
enhanced by quantum interference 12
2.5. Absorption and dispersive spectra at Doppler-broadened transitions 17

3. Four-wave mixing, dissociation and population transfer controlled
by LICS in folded energy-level schemes 19
3.1. Quasistationary solution of density matrix equations 21
3.1.1. Open configuration 24
3.1.2. Closed configuration 25
3.2. Numerical analysis 26
3.2.1. Coherent control of populations and dissociation in folded schemes 27
3.2.2. Coherent control of generated radiation in folded schemes 29

Conclusions 33

## 1 Introduction

The opportunities of laser control of optical properties and chemical reactivity of substances associated with the continuum energy states of atoms and molecules, and based on nonlinear quantum coherence and interference processes, have attracted considerable attention since their theoretical prediction GP2 , GP3  and experimental realization GP9 . These effects were shown to provide the feasibility of manipulating the spectral characteristics of the absorption, refraction, and nonlinear-optical conversion of weak radiations by an additional strong field, which is in resonance with a transition between an excited vacant level and a state in the continuum. The strong-field effects in such coupling configuration manifest themselves by the appearance of spectral autoionizing-like laser-induced continuum structures (LICS). In the presence of a real resonance autoionizing level a strong field has a strong influence on the spectral characteristics of this resonance too AI1 , AI2 , AI3 , Gel . The effects of the LICS on the absorption, refraction, nonlinear-optical generation and photoionization may differ significantly (see, for example, Refs Gel , Kn , Fau , 2a , 2c , Cav , 2d1 , bull , Kimb , 2e  and the references therein). Most of the recent publications consider LICS in photoionization. The influence of real autoionizing levels and of the LICS on nonlinear susceptibility and four-wave mixing (FWM) has been investigated for frequencies of the other fields far from one-photon resonances 2c , Kimb . The interference of two LICS was shown to bring new qualitative effects in spectral properties of absorption, refraction and nonlinear optical generation of short-wavelength radiation Kimb .

Recently, the laser and chemical communities have focused on coherent quantum control of chemical reactions and other dissipation processes like photodissociation of molecules and photoionization of atoms TR1 , BrSh , TR2 , Br1 , D1 , Sh1 , D2 , U1 , U2 , 1D , 1DD , D4 , D3 , Br2 , R1 , Br3 , Br4 , Br5 , D5 , D8 , D9 , R2 , R3 , R4 , Gor1 , Sh2 , Sh3 , 102 , Mcool , R5 , R6 , R9 , Band , Br6 , R7 , R8 , 117 . In many cases, such control is based on implementation of the interference of different quantum channels, which give rise to laser-induced continuum structures (LICS) in the dissociation and ionization continua. Recent experiments aimed at control of photoionization of metastable helium atoms and some other processes making use of this technique are reported elsewhere Half , Yats , Berg .

This paper further develops theoretical approaches to these problems and reports novel opportunities for manipulating spectral characteristic of short-wavelength generation and photodissociation through the interplay of two LICS induced by strong continuous-wave laser fields coupling the dissociation continuum to two different bound states. Primary attention is paid to two important applications: (1) coherent control of sum-frequency short-wavelength generation in a ladder-type energy-level scheme (depicted in Fig. 1) and (2) coherent control of dissociation, population transfer and four-wave mixing feasible in a folded-type scheme (depicted in Fig. 9).

As concerns the first problem, we generalize our investigation of the LICS to the case of several strong control fields in situations when one can expect the strongest enhancement of the generated power. We consider the combined influence of the interference of two laser-induced structures in the continuum and of the laser-induced transparency (for the one-photon-resonant initial radiation and for the generated radiation) on the processes of nonlinear-optical generation of short-wavelength radiation. We demonstrate for the first time that nonlinear interference resonances in the output power of the radiation generated in an absorbing medium may differ considerably from the corresponding resonances in a transparent medium because of the combined influence of the nonlinear resonances in the nonlinear polarization and in absorption of both the initial and generated radiations.

A two-photon dissociation ($`\mathrm{\Lambda }`$-scheme) controlled by an auxiliary laser field coupling continuum with another discrete state ($`V`$-configuration) is investigated for the second problem. All the coupled radiations are strong enough to drive molecular transitions. The proposed technique enables the coherent laser control of dissociation related to the lower laying molecular ’dark’ states that are not connected with the ground one by the allowed transition. On the other hand, the scheme under consideration enables one to transfer the population between two upper bound states which are not connected directly by the allowed transition. An analytical solution of the corresponding master density matrix equations of the problem is obtained, and a numerical analysis for relevant experimental conditions Half , Berg  is performed. The possibility of manipulating the dissociation spectra and populations of excited states at the expense of the interference of quantum pathways through a variety of continuum states is explored. The dependence of the effects on the composed Fano parameters related to high excited levels, on the detuning between two LICS and on the intensities of the laser radiation is investigated.

## 2 Four-wave mixing, absorption and refractive indices in ladder energy-level schemes controlled by interference of two LICS

### 2.1 Equations for coupled electromagnetic waves and their solution

Let us consider four plane-polarized electromagnetic waves travelling along the $`z`$ axis of an isotropic medium,

$`E^j(z,t)=\mathrm{Re}\{E_j(z)\mathrm{exp}[\mathrm{i}(\omega _jtk_jz)]\},`$ (2.1)
where $`k_j`$ is the complex wave-number corresponding to the frequency $`\omega _j`$ ($`j=1,2,3,S`$). We assume that the fields $`E_1`$ and $`E_S`$ are weak compared to the driving fields $`E_2`$ and $`E_3`$, which do not vary along the medium. On the contrary, the fields $`E_1`$ and $`E_S`$ can change considerably along the medium, because of both absorption and nonlinear-optical conversion. Then the spacial behavior of the waves $`E_S`$ and $`E_1`$ is described by two coupled reduced wave equations,

$`dE_S(z)/dz`$ $`=\mathrm{i2}\pi k_S^{}\chi _S^{(3)}E_2E_3E_1(z)\mathrm{exp}(\mathrm{i}\mathrm{\Delta }kz),`$
$`dE_1(z)/dz`$ $`=\mathrm{i2}\pi k_1^{}\chi _1^{(3)}E_2^{}E_3^{}E_S(z)\mathrm{exp}(\mathrm{i}\mathrm{\Delta }kz).`$ (2.2)
Here $`k_j=k_j^{}\mathrm{i}k_j^{\prime \prime }=(2\pi \omega _j/c)\chi _j`$, $`k_j^{\prime \prime }=\alpha _j/2`$, and $`\chi _j,\alpha _j`$ are the effective linear susceptibilities and absorption indices for the corresponding radiations, and $`\chi _1^{(3)},\chi _S^{(3)}`$ are the nonlinear susceptibilities describing the four-wave mixing processes: $`\omega _S\omega _1+\omega _2+\omega _3`$, $`\mathrm{\Delta }k=k_Sk_1k_2k_3`$. The quantum conversion efficiency of the radiation $`E_1`$ into $`E_S`$ varies along the medium as

$`\eta _\mathrm{q}=(k_1^{}/k_S^{})|E_S(z)/E_1(0)|^2\mathrm{exp}(\alpha _Sz).`$ (2.3)
Let us first consider the case of low efficiency, for which the change in the $`E_1`$ caused by the nonlinear-optical conversion can be ignored. Then the second equation in (2.2) can be ignored as well and, with the account of the boundary condition $`E_S(z=0)=0`$, one obtains the following for the generated radiation and quantum conversion efficiency:

$`E_S(z)=(2\pi k_S^{}/\mathrm{\Delta }k)\chi _S^{(3)}E_1E_2E_3[\mathrm{exp}(\mathrm{i}\mathrm{\Delta }kz)1],`$ (2.4)
$`\eta _\mathrm{q}(z)=k_S^{}k_{1}^{}{}_{}{}^{}(\left|2\pi \chi _S^{(3)}E_2E_3\right|^2/|\mathrm{\Delta }k|^2)\mathrm{exp}(\alpha _Sz)\left|\mathrm{exp}(\mathrm{i}\mathrm{\Delta }kz)1\right|^2.`$ (2.5)
If the medium length is much shorter than the minimum absorption length $`L_{abs}=\mathrm{min}\{L_1=2/\alpha _1,L_S=2/\alpha _S\}`$ and both of these are assumed much shorter than the coherence length $`L_{coh}=\mathrm{\Delta }k^1`$, then Eq. (2.5) reduces to the approximate formula

$`\eta _\mathrm{q}=k_{S}^{}{}_{}{}^{}k_{1}^{}{}_{}{}^{}\left|2\pi \chi _S^{(3)}E_2E_3\right|^2L_\mathrm{e}^2,`$ (2.6)
where $`L_\mathrm{e}`$ represents either the length of the medium (in the case of weak absorption) or the optimal length of the order of $`\mathrm{min}\{L_{abs},L_{coh}\}`$.

For a medium with substantial absorption dispersion ($`\alpha _1\alpha _S`$), but $`\mathrm{\Delta }k^{}=0`$ and $`\chi _1^{(3)}=\chi _S^{(3)}`$, the solution of equations (2.2), for the more general case of considerable conversion, takes the form tim

$`\eta _\mathrm{q}(z)=4{\displaystyle \frac{\stackrel{~}{\eta }_{\mathrm{q0}}}{|b|}}\mathrm{exp}\left[(\alpha _1+\alpha _S){\displaystyle \frac{z}{2}}\right]\left[\mathrm{sinh}^2\left(\sqrt{{\displaystyle \frac{(|b|b)}{2}}}{\displaystyle \frac{z}{2}}\right)+\mathrm{sin}^2\left(\sqrt{{\displaystyle \frac{(b+b)}{2}}}{\displaystyle \frac{z}{2}}\right)\right].`$ (2.7)
Here $`\stackrel{~}{\eta }_{q0}=k_1^{}k_S^{}2\pi \chi _S^{(3)}E_2E_3^2`$ is the conversion efficiency per unit of the medium length under constant fundamental radiations, and $`b=4\stackrel{~}{\eta }_{q0}(\alpha _1\alpha _S)^2/4`$ defines the difference between the rates of absorption and nonlinear-optical conversion of the radiations. If $`b<0`$, the conversion rate of $`\mathrm{}\omega _1`$ photons into $`\mathrm{}\omega _S`$ photons is less than their absorption rate; if $`b=0`$, the photon absorption and conversion rates are equal; and if $`b>0`$, the nonlinear-optical conversion rate exceeds the absorption rate. In the latter case, one can expect an oscillatory dependence of the transfer of the weak radiations from one to the another and back along the medium.

The susceptibilities $`\chi _S^{(3)}`$, $`\chi _1^{(3)}`$, $`\chi _S`$ and $`\chi _1`$ can be derived from the medium polarizations at the corresponding frequencies:

$`P(\omega _j)=\chi _jE_j,P^{\mathrm{NL}}(\omega _S)=\chi _S^{(3)}E_1E_2E_3,P^{\mathrm{NL}}(\omega _1)=\chi _1^{(3)}E_SE_2^{}E_3^{}.`$ (2.8)
These components can be calculated conveniently with the aid of a density matrix, $`\rho _{ij}`$, as

$$𝒫(\omega _j)=N\rho _{ij}(\omega _j)d_{ji}+\mathrm{c}.\mathrm{c}.,$$
(2.9)
where $`N`$ is the atomic number density in the medium, and $`d_{ji}`$ is a matrix element of the projection of the transition electric-dipole moment along the direction of the electric vector of the corresponding field. The problem of finding and optimizing the quantum efficiency of the conversion process thus reduces to finding the off-diagonal elements of the density matrix.

### 2.2 Density matrix master equations and their solutions

First, we shall consider the transition scheme depicted in Fig. 1. A strong field $`E_2`$ at frequency $`\omega _2`$ is close to resonance with the transition between levels $`m`$ and $`n`$, while the strong fields $`E`$ and $`E_3`$ at frequencies $`\omega `$ and $`\omega _3`$ are in resonance with the transitions between levels $`f`$ and $`n`$ and some states in the continuum. Radiation at the frequency $`\omega _S`$ can be either a probe or generated by four-wave mixing. We shall investigate the influence of the strong fields on the spectral characteristics of the absorption of the radiations $`E_1`$ and $`E_S`$ at the frequencies $`\omega _1`$ and $`\omega _S`$ (both as independent probe radiations or, alternatively, as the frequencies linked through generation, $`\omega _S=\omega _1+\omega _2+\omega _3`$). The field $`E_1`$ is assumed close to resonance with the transition from the ground state to the level $`m`$ and $`E_S`$ to the transition from the ground state to the continuum. These radiations are weak, so that a change in the level populations due to all resonant couplings can be ignored. We neglect the degeneration of all states, including those in the continuum. In addition to the contribution of the off-resonant continuum states, we account for the contribution of discrete off-resonant levels which are combined to form the level $`k`$ in Fig. 1. We suppose that the detunings $`\omega _1`$-$`\omega _{gm}`$, $`\omega _1+\omega _2\omega _{gn}`$ and $`\omega \omega _3\omega _{nf}`$ are considerably less than all the other detunings.

The equations for the density matrix, considered in the interaction representation to within the first order of perturbation theory in weak fields, can be written as follows:

$`d\rho _{gm}/dt+\mathrm{\Gamma }_{gm}\rho _{gm}=\mathrm{i}(\rho _{gg}V_{gm}+\rho _{gn}V_{nm}),`$
$`d\rho _{gn}/dt+\mathrm{\Gamma }_{gn}\rho _{gn}=\mathrm{i}{\displaystyle \rho _{g\epsilon }V_{\epsilon n}𝑑\epsilon }+\mathrm{i}\rho _{gm}V_{mn}+\mathrm{i}{\displaystyle \rho _{gk}V_{kn}},`$
$`d\rho _{gf}/dt+\mathrm{\Gamma }_{gf}\rho _{gf}=\mathrm{i}{\displaystyle \rho _{g\epsilon }V_{\epsilon f}𝑑\epsilon }+\mathrm{i}{\displaystyle \rho _{gk}V_{kf}},`$ (2.10)
$`d\rho _{g\epsilon }/dt=\mathrm{i}(\rho _{gg}V_{g\epsilon }\text{+}\rho _{gn}V_{n\epsilon }\text{+}\rho _{gf}V_{f\epsilon }),`$
$`d\rho _{gk}/dt+\mathrm{\Gamma }_{gk}\rho _{gk}=\mathrm{i}(\rho _{gn}V_{nk}+\rho _{gf}V_{fk}).`$
Here, the index $`\epsilon `$ denotes the continuum states; $`V_{mn}=G_{mn}\mathrm{exp}[\mathrm{i}(\omega _2\omega _{nm})t],V_{g\epsilon }=G_{g\epsilon }\mathrm{exp}[\mathrm{i}(\omega _S\omega _{g\epsilon })t],V_{n\epsilon }=G_{n\epsilon }\mathrm{exp}[\mathrm{i}(\omega _3\omega _{n\epsilon })t],V_{gm}=G_{gm}\mathrm{exp}[\mathrm{i}(\omega _1\omega _{gm})t],V_{f\epsilon }=G_{f\epsilon }\mathrm{exp}[\mathrm{i}(\omega \omega _{f\epsilon })t],V_{kn}=G_{kn}\mathrm{exp}[\mathrm{i}(\omega \omega _{kn})t],V_{kf}=G_{kf}\mathrm{exp}[\mathrm{i}(\omega _3\omega _{kf})t]`$ are the matrix elements of the Hermitian interaction Hamiltoman $`\widehat{V}`$, considered in the electric-dipole approximation and in the interaction representation (in units of $`\mathrm{}`$); $`V_{ij}`$ = $`V_{ji}^{};G_{mn}=E_2d_{mn}/2\mathrm{},G_{g\epsilon }=E_4d_{g\epsilon }/2\mathrm{},`$ etc.; and $`\mathrm{\Gamma }_{ij}`$ is the homogeneous half-width of the $`ij`$ transition. In the approximation of the weak fields $`E_1`$ and $`E_S`$, we obtain $`\rho _{gg}1,\rho _m\rho _n\rho _f<<1.`$

Under steady-state conditions, each off-diagonal element of the density matrix is a sum of two components, which may oscillate at different frequencies:

$`\rho _{g\epsilon }`$ $`=r_{g\epsilon }\mathrm{exp}[\mathrm{i}(\omega _S\omega _{g\epsilon })t]+R_{g\epsilon }\mathrm{exp}[\mathrm{i}(\omega _1+\omega _2+\omega _3\omega _{g\epsilon })t],`$
$`\rho _{gn}`$ $`=r_{gn}\mathrm{exp}[\mathrm{i}(\omega _S\omega _3\omega _{gn})t]+R_{gn}\mathrm{exp}[\mathrm{i}(\omega _1+\omega _2\omega _{gn})t],`$
$`\rho _{gm}`$ $`=r_{gm}\mathrm{exp}[\mathrm{i}(\omega _S\omega _3\omega _2\omega _{gm})t]+R_{gm}\mathrm{exp}[\mathrm{i}(\omega _1\omega _{gm})t],`$ (2.11)
$`\rho _{gf}`$ $`=r_{gf}\mathrm{exp}[\mathrm{i}(\omega _S\omega \omega _{gf})t]+R_{gf}\mathrm{exp}[\mathrm{i}(\omega _1+\omega _2+\omega _3\omega \omega _{gf})t],`$
$`\rho _{gk}`$ $`=r_{gk}\mathrm{exp}[\mathrm{i}(\omega _S\omega _3\omega \omega _{gk})t]+R_{gk}\mathrm{exp}[\mathrm{i}(\omega _1+\omega _2\omega \omega _{gk})t].`$
By substituting (2.11) into (2.10), one can see that the set of differential equations under consideration reduces to two independent sets of algebraic equations, where each refers to the processes determined by only one weak field:

$`\mathrm{i}R_{gm}D_{gm}=G_{gm}R_{gn}G_{nm},D_{gm}=\mathrm{\Gamma }_{gm}+\mathrm{i}(\omega _1\omega _{gm}),`$
$`\mathrm{i}R_{gn}D_{gn}={\displaystyle R_{g\epsilon }G_{\epsilon n}𝑑\epsilon }R_{gm}G_{mn}R_{gk}G_{kn},D_{gn}=\mathrm{\Gamma }_{gn}+\mathrm{i}(\omega _1+\omega _2\omega _{gn}),`$
$`\mathrm{i}R_{g\epsilon }D_{g\epsilon }=R_{gn}G_{n\epsilon }R_{gf}G_{f\epsilon },D_{g\epsilon }=\mathrm{i}(\omega _1+\omega _2+\omega _3\omega _{g\epsilon }),`$ (2.12)
$`\mathrm{i}R_{gf}D_{gf}={\displaystyle R_{g\epsilon }G_{\epsilon f}𝑑\epsilon }R_{gk}G_{kf},D_{gf}=\mathrm{\Gamma }_{gf}+\mathrm{i}(\omega _1+\omega _2+\omega _3\omega \omega _{gf}),`$
$`\mathrm{i}R_{gk}D_{gk}=(R_{gn}G_{nk}R_{gf}G_{fk}),D_{gk}=\mathrm{\Gamma }_{gk}+\mathrm{i}(\omega _1+\omega _2\omega \omega _{gk}),`$
$`\mathrm{i}r_{g\epsilon }p_{g\epsilon }=G_{g\epsilon }r_{gn}G_{n\epsilon }r_{gf}G_{f\epsilon },p_{g\epsilon }=\mathrm{i}(\omega _S\omega _{g\epsilon }),`$
$`\mathrm{i}r_{gn}p_{gn}={\displaystyle r_{g\epsilon }G_{\epsilon n}𝑑\epsilon }r_{gm}G_{mn}r_{gk}G_{kn},p_{gn}=\mathrm{\Gamma }_{gn}+\mathrm{i}(\omega _S\omega _3\omega _{gn}),`$
$`\mathrm{i}r_{gm}p_{gm}=r_{gn}G_{nm},p_{gm}=\mathrm{\Gamma }_{gm}+\mathrm{i}(\omega _S\omega _3\omega _2\omega _{gm}),`$ (2.13)
$`\mathrm{i}r_{gf}p_{gf}={\displaystyle r_{g\epsilon }G_{\epsilon f}𝑑\epsilon }r_{gk}G_{kf},p_{gf}=\mathrm{\Gamma }_{gf}+\mathrm{i}(\omega _S\omega \omega _{gf}),`$
$`\mathrm{i}r_{gk}p_{gk}=r_{gn}G_{nk}r_{gf}G_{fk},p_{gk}=\mathrm{\Gamma }_{gk}+\mathrm{i}(\omega _S\omega _3\omega \omega _{gk}).`$
Here and later the repeated index $`k`$ indicates summation over all discrete off-resonant levels combined to form the level $`k`$.

Equations (2.12) describe the absorption of $`E_1`$ and generation at the frequency $`\omega _S`$, whereas (2.13) presents the absorption of $`E_S`$ and parametric conversion of $`E_S`$ back into $`E_1`$. One can solve (12) by substituting the third equation into the second and fourth. Then, in the calculation of the integrals, one can employ the $`\zeta `$-function,

$`[\mathrm{i}(\omega _S\omega _{\epsilon g})]^1=\pi \delta (\omega _S\omega _{\epsilon g})+\mathrm{i}𝒫(\omega _S\omega _{\epsilon g})^1,`$ (2.14)
where $`\delta (\xi )`$ is the delta function, and $`𝒫`$ is the principal value obtained by integration. This leads to the following equations:

$`R_{g\epsilon }=\mathrm{i}[G_{n\epsilon }G_{f\epsilon }(\gamma _{nf}/\gamma _{ff})\beta _f(1\mathrm{i}q_{nf})/X_f]R_{gn}/D_{g\epsilon },`$
$`R_{gm}=\mathrm{i}{\displaystyle \frac{G_{gm}+R_{gn}G_{nm}}{X_m\mathrm{\Gamma }_{gm}}},R_{gn}={\displaystyle \frac{G_{gm}G_{mn}X_f}{\mathrm{\Gamma }_{gf}\mathrm{\Gamma }_{gn}X_m(1+g_{nn})(X_nX_fK+A_mX_f)}},`$ (2.15)
where

$`\beta _f`$ $`=g_{ff}/(1+g_{ff}),\beta _n=g_{nn}/(1+g_{nn}),g_{nn}=\gamma _{nn}/\mathrm{\Gamma }_{gn},g_{ff}=\gamma _{ff}/\mathrm{\Gamma }_{gf},`$
$`K`$ $`=\beta _f\beta _n(1\mathrm{i}q_{nf})^2,A_m=g_{mn}/X_m(1+g_{nn}),g_{mn}=|G_{mn}|^2/\mathrm{\Gamma }_{gm}\mathrm{\Gamma }_{gn};`$
$`q_{ij}`$ $`=\delta _{ij}/\gamma _{ij},\gamma _{ij}=\pi \mathrm{}G_{i\epsilon }G_{\epsilon j}_{\epsilon =\mathrm{}\omega _S}+\mathrm{Re}(G_{ik}G_{kj}/p_{gk}),`$
$`\delta _{ij}`$ $`=\mathrm{}P{\displaystyle 𝑑\epsilon \frac{G_{i\epsilon }G_{\epsilon j}}{(\mathrm{}\omega _S\epsilon )}}+\mathrm{Im}[G_{ik}G_{kj}/p_{gk}],`$
$`X_i`$ $`=1+\mathrm{i}x_i,x_n=(\mathrm{\Omega }_1+\mathrm{\Omega }_2\delta _{nn})/(\mathrm{\Gamma }_{gn}+\gamma _{nn}),x_m=\mathrm{\Omega }_1/\mathrm{\Gamma }_{gm},`$
$`x_f`$ $`=(\mathrm{\Omega }_1+\mathrm{\Omega }_2\mathrm{\Omega }_L\delta _{ff})/(\mathrm{\Gamma }_{gf}+\gamma _{ff})=(\omega _1+\omega _2+\omega _3\omega \omega _{gf}\delta _{ff})/(\mathrm{\Gamma }_{gf}+\gamma _{ff}),`$
$`\mathrm{\Omega }_L`$ $`=(\omega +\omega _{gf})(\omega _3+\omega _{gn}),\mathrm{\Omega }_1=\omega _1\omega _{gm},\mathrm{\Omega }_2=\omega _2\omega _{mn}.`$ (2.16)
Here $`\mathrm{\Omega }_L`$ is the spacing between the quasi-levels induced by the radiations $`E`$ and $`E_3`$ in the continuum. The Fano parameters $`q_{ij}`$ fano  are assumed real and indicate the ratio of the light-induced shifts and the broadening of the corresponding resonances by the control fields. In the adopted approximation, these parameters are independent of the field intensities and are governed solely by the properties of the investigated atom.

Following the same procedure as above and bearing in mind the condition $`\omega _S=\omega _1+\omega _2+\omega _3`$, one finds from the set of equations (2.13) that

$`r_{g\epsilon }`$ $`=\mathrm{i}\{G_{g\epsilon }G_{f\epsilon }(\gamma _{gf}/\gamma _{ff})\beta _f(1\mathrm{i}q_{gf})/X_f+r_{gn}[G_{n\epsilon }G_{f\epsilon }(\gamma _{nf}/\gamma _{ff})\beta _f(1\mathrm{i}q_{nf})/X_f]\}/p_{g\epsilon },`$
$`r_{gm}`$ $`=\mathrm{i}{\displaystyle \frac{r_{gn}G_{nm}}{X_m\mathrm{\Gamma }_{gm}}},r_{gn}={\displaystyle \frac{(1\mathrm{i}q_{fn})(1\mathrm{i}q_{gf})\gamma _{gf}\gamma _{fn}/(\mathrm{\Gamma }_{gf}+\gamma _{ff})(1\mathrm{i}q_{gn})X_f\gamma _{gn}}{(1+g_{nn})\mathrm{\Gamma }_{gn}(X_fX_nK+A_mX_f)}}.`$ (2.17)
The calculation of $`R_{gm}`$ from (2.15) and $`r_{g\epsilon }`$ from (2.17), and application of formulas (2.8) and (2.9) after integration over the continuum states, gives the following expressions for the absorption and refractive indices at the frequencies $`\omega _1`$ and $`\omega _S`$, respectively:

$`{\displaystyle \frac{\alpha (\omega _1)}{\alpha _{10}}}`$ $`=\mathrm{Re}F_1,{\displaystyle \frac{n(\omega _1)1}{2(n_{1\mathrm{max}}1)}}=\mathrm{Im}F_1,`$
$`F_1`$ $`={\displaystyle \frac{1}{X_m}}\left[1{\displaystyle \frac{A_mX_f}{X_nX_f+A_mX_fK}}\right],`$ (2.18)
$`{\displaystyle \frac{\alpha (\omega _S)}{\alpha _{S0}}}`$ $`=\mathrm{Re}F_S,{\displaystyle \frac{n(\omega _S)1}{2(n_{S\mathrm{max}}1)}}=\mathrm{Im}F_S,`$
$`F_S`$ $`=\left[1{\displaystyle \frac{X_fX_n(A_n+A_f)U+A_mA_fX_f}{X_fX_nK+A_mX_f}}\right]`$
$`=\left[1A_fA_n{\displaystyle \frac{K(A_n+A_f)UA_mA_nX_f}{X_fX_nK+A_mX_f}}\right]`$
$`=\left[1A_f\stackrel{~}{A}_n{\displaystyle \frac{K(\stackrel{~}{A}_n+A_f)U}{X_f\stackrel{~}{X}_nK}}\right].`$ (2.19)
Here $`\alpha _{10}`$ is the absorption index with the fields intensities and detunings turned to zero, and $`\alpha _{S0}`$ is the similar quantity for a transition to the continuum; $`n_{1\mathrm{max}}`$ and $`n_{S\mathrm{max}}`$ are the maximum values of the corresponding refractive indices under control fields turned off; and

$$A_f=\beta _f(1\mathrm{i}q_{gf})^2/X_f;A_n=\beta _n(1\mathrm{i}q_{gn})^2/X_n;U=2\beta _f\beta _n(1\mathrm{i}q_{gf})(1\mathrm{i}q_{fn})(1\mathrm{i}q_{ng}).$$

The functions $`\stackrel{~}{A}_n=\beta _n(1\mathrm{i}q_{gn})^2/\stackrel{~}{X}_n`$ and $`\stackrel{~}{X}_n=X_n+A_m`$ account for the perturbation of a two-photon resonance with the level $`n`$ by the strong fields. The expressions for the refractive index are obtained on the assumption that this index is close to unity in the absence of the fields.

The calculation of $`R_{g\epsilon }`$ and $`r_{gm}`$ from the expressions (2.15) and (2.17), which is carried out making use of formulas (2.8) and (2.9) and integration over the states in the continuum, gives expressions for the FWM nonlinear susceptibility at $`\omega _S=\omega _1+\omega _2+\omega _3`$ as

$`{\displaystyle \frac{\chi ^{(3)}(\omega _S)}{\chi _{S0}^{(3)}}}={\displaystyle \frac{X_f\beta _f(1\mathrm{i}q_{nf})(1\mathrm{i}q_{fg})/(1\mathrm{i}q_{ng})}{X_m(1+g_{nn})(X_nX_fK+A_mX_f)}},`$ (2.20)
and for the nonlinear susceptibility determining conversion of the $`E_S`$ radiation back into the radiation of frequency $`\omega _1`$ as

$`{\displaystyle \frac{\chi ^{(3)}(\omega _1)}{\chi _{10}^{(3)}}}={\displaystyle \frac{X_f\beta _f(1\mathrm{i}q_{nf})(1\mathrm{i}q_{fg})/(1\mathrm{i}q_{ng})}{X_m(1+g_{nn})(X_nX_fK+A_mX_f)}}`$ (2.21)
In the expressions (2.20) and (2.21), the quantities $`\chi _{S0}^{(3)}`$ and $`\chi _{10}^{(3)}`$ are fully-resonant nonlinear susceptibilities for non-perturbative weak fields.

### 2.3 Laser-induced structures in absorption and refraction <br>spectra at discrete and continuous transitions

In this subsection, we analyze and compare the effects of strong fields on discrete and continuous spectra with the aid of the derived formulas. An important difference is seen as compared with similar effects if solely discrete transitions are involved Sok , Vved . The results given below demonstrate considerable perturbations of discrete spectra by the radiations coupled to the continuum. The first term in (2.18) represents the field-unperturbed absorption coefficient for the $`gn`$ transition, and the second term refers to the cumulative effects of the strong fields. The coefficient $`A_m`$ represents splitting of a resonance into two components by the strong field $`E_2`$ Sok , Vved  and modified by the strong field $`E_3`$. The function $`K`$ describes modification of these effects by the strong field $`E`$. It is proportional to the product of the intensities of the fields $`E`$ and $`E_3`$. The effects in question disappear when any of these fields is turned off. Since the field $`E_2`$ is in resonance with a discrete transition and the fields $`E_3`$ and $`E`$ are coupled to the continuum, the spectral properties of the corresponding contributions are different. If $`E_3=0`$ ($`\gamma _n=0,\beta _n=0,K=0,g_{nn}=0`$), the equation for absorption in (2.18) converges to the standard one for three-level nonlinear spectroscopy Sok , Vved ,

$$\alpha (\omega _1)/\alpha _{01}=\text{Re }\left[X_n/\left(X_nX_m+\frac{g_{mn}}{1+g_{nn}}\right)\right].$$
(2.22)
The factor in the parentheses in the above formula has two singularities with respect to $`x_m`$, which indicates splitting of the resonance into two maxima. The positions of these maxima and their relative amplitudes may vary depending on the parameters of the fields and transitions. Resonance splitting is stipulated by the appearance of coherence at the transition $`ng`$ and by the consequent appearance of additional quantum transitions in which photons of frequency $`\mathrm{}\omega _1`$ may participate. The phase and relaxation properties of the corresponding term in nonlinear polarization at the frequency $`\omega _1`$ are represented by the dispersion function $`X_n`$. The additional strong fields $`E_3`$ and $`E`$ perturb the quantum system, which, as pointed out earlier, causes additional modification of the laser-induced quasi-levels and resonances. The changes in the refractive index can he explained similarly.

The spectral characteristics of absorption at the frequency $`\omega _S`$ are governed by the interference between three quantum pathways: directly to the continuum, to level $`f`$, and also to the superposition of levels $`n`$ and $`m`$. The influence of the first two processes was investigated earlier in Refs. GP2 , GP3 , Kn , Vved  and is accounted for by the function $`\stackrel{~}{A}_l`$ in the equations (2.19). The strong fields $`E_3`$ and $`E_2`$ lead to additional changes in the spectra. The additional independent structure, described in these expressions by the function $`\stackrel{~}{A}_n`$, is supplemented by the interference structures proportional to the functions $`K`$ and $`U`$, which disappear when any of the fields $`E_3`$ or $`E`$ is turned off or when the spacing between the quasi-levels $`\mathrm{\Omega }_L`$ is increased.

Figure 2 shows the dependence of the absorption index at $`\omega _1`$ on the scaled detunings from the bare-state one-photon resonance $`\mathrm{\Omega }_1/\mathrm{\Gamma }_{gm}`$. The dashed plot at Fig. 2(b) shows the lineshape of the dispersive index at the frequency $`\omega _1`$ for the same parameters. The plot indicates very strong dispersion, induced by the dressing fields coupled to both discrete and continuum states. Figures 2(c) and 2(d) illustrate the sensitivity of the spectra, induced jointly by two dressing fields $`E_3`$ and $`E`$, on the Fano parameter $`q_{fn}`$. One can create transparency in certain frequency intervals of the discrete transitions or, on the contrary, eliminate effects of the dressing fields with the aid of destructive interference by varying the intensities and detunings of the driving fields as well as the coupled levels.

Figures 3(a) and 3(b) show the dependence of the absorption index at the frequency $`\omega _S`$ (reduced by its value in the absence of the dressing fields) on the scaled detuning $`\mathrm{\Omega }/\mathrm{\Gamma }_{fg}=(\omega _S\omega \omega _{fg})/\mathrm{\Gamma }_{gf}`$. The plots indicate the sensitivity of the probe field absorption on the Fano parameters (in the considered cases on $`q_{gf}`$ and $`q_{gn}`$) and demonstrate new possibilities for manipulation of LICS with extra dressing fields coupling adjacent transitions. Interference contributions, which disappear in the absence of either the $`E`$ or $`E_3`$ field, are shown in the inputs to the figure. Figure 3(c) demonstrates the sensitivity of the absorption spectrum on the strength of the driving field $`E_3`$ as well as on the spacing of two quasi-levels, induced in the continuum (on two-photon detuning $`\mathrm{\Omega }_L=\omega \omega _3\omega _{fn}`$). The figures show possible manipulation of LICS in the absorption index for a probe radiation (including formation of transparency windows). This is brought about by the interference of two LICS (quantum pathways via discreet and continuum states), induced by the fields at $`\omega _3`$ and $`\omega `$ and modified by the strong field at $`\omega _2`$.

The refractive index is proportional to the derivative of the structures over frequency. The plots 3(d,e,f) display the potential of manipulating the magnitude and lineshape of the factor $`(n(\omega _S)1)/(n_{S\mathrm{max}}1)`$ with the change of intensities and detunings of the dressing fields, as well as strong dependence on the Fano parameters, which may find applications in short-wavelength optics.

The nonlinear interference effects involving quantum transitions may influence differently the linear and nonlinear susceptibilities. Therefore, under certain conditions a reduction in the absorption of the initial and generated radiations can be simultaneously followed by an increase in the nonlinear polarization caused by the resonant effects and by the constructive interference in the strong fields. It is thus possible to increase considerably the power of the generated short-wavelength radiation.

### 2.4 Resonance sum-frequency generation in strongly-absorbing media enhanced by quantum interference

In weak fields the nonlinear susceptibility increases strongly upon approaching to discrete resonances, but this is accompanied by enhancement of the absorption of the initial radiations. Depending on the detunings from the resonances, on the ratio of the oscillator strengths of the transitions, and on the radiation intensities, either the absorption of the initial radiation $`E_1`$ or of the generated radiation may predominate. A numerical analysis of the influence of these factors on changes in the frequency dependence of the power of the generated short-wavelength radiation during the course of propagation in an optically dense medium can be made if the quantum efficiency of conversion given by expression (2.7) is rewritten in the form:

$$\eta _\mathrm{q}(z)=\frac{4\overline{\eta }_{\mathrm{q0}}}{|\overline{b}|}\mathrm{exp}\left[(\overline{\alpha }_1+C\overline{\alpha }_S)z_0\right]\left\{\mathrm{sinh}^2\left[\sqrt{(|\overline{b}|\overline{b})C/2}z_0\right]+\mathrm{sin}^2\left[\sqrt{(\overline{b}+\overline{b})C/2}z_0\right]\right\},$$
(2.23)
where $`\overline{\eta }_{\mathrm{q0}}=\stackrel{~}{\eta }_{\mathrm{q0}}/(\alpha _{10}\alpha _{S0}),\overline{b}=b/(\alpha _{10}\alpha _{S0})=4\overline{\eta }_{\mathrm{q0}}(\overline{\alpha }_1C\overline{\alpha }_S)^2/4C,\overline{\alpha }_1=\alpha _1/\alpha _{10};\overline{\alpha }_S=\alpha _S/\alpha _{S0},C=\alpha _{S0}/\alpha _{10},andz_0=z\alpha _{10}/2`$.

The expression for $`\overline{\eta }_{\mathrm{q0}}`$, describing the quantum efficiency of conversion over a distance $`1/\sqrt{\alpha _{10}\alpha _{S0}}`$, considered within the approximation of ignoring absorption of given fields, becomes

$$\overline{\eta }_{\mathrm{q0}}=\eta _{\mathrm{q0}}^0|\overline{\chi }^{(3)}|^2g_{mn}g_{nn},$$
(2.24)
where $`\eta _{\mathrm{q0}}^0`$ is the quantum efficiency of conversion based on the resonant unperturbed nonlinearity over a distance $`1/\sqrt{\alpha _{10}\alpha _{S0}}`$ in fields corresponding to $`g_{mn}=g_{nn}=1;\overline{\chi }^{(3)}=\chi ^{(3)}/\chi _0`$. We shall henceforth use the following approximate expressions:

$`\alpha _{10}=4\pi \omega _1|d_{gm}|^2/c\mathrm{}\mathrm{\Gamma }_{gm},\alpha _{S0}=4\pi ^2(\omega _S/c)|d_{g\epsilon }|^2|_{\epsilon =\mathrm{}\omega _3},`$
$`|\chi _0|^2=(\pi /2\mathrm{}^2)^2(1+q_{gn}^2)|d_{gm}d_{mn}d_{n\epsilon }d_{\epsilon g}|^2(\mathrm{\Gamma }_{gm}\mathrm{\Gamma }_{gn})^2.`$ (2.25)
In this approximation the factor $`\eta _{\mathrm{q0}}^0`$ is determined completely by the Fano parameter $`q_{gn}`$:

$$\eta _{\mathrm{q0}}^0=k_1^{}k_S^{}|2\pi \chi _0|^2|/d_{mn}d_{n\epsilon }|^2\pi (16\mathrm{}^3\mathrm{\Gamma }_{gm}\mathrm{\Gamma }_{gn}^2)^1\alpha _{10}\alpha _{S0}=(1+q_{gn}^2).$$
(2.26)
As pointed our earlier, the laser-induced absorption and transparency resonances of the radiation $`E_1`$ can be interpreted as splitting of the level $`m`$ into quasi-levels by the strong field $`E_2`$ (in combination with the fields $`E_3`$ and $`E`$). The laser-induced resonances of the generated radiation are determined by two quasi-levels in the continuum and appear near the frequencies $`\omega _{ng}+\omega _3`$ and $`\omega _{fg}+\omega `$. These quasi-levels are separated by an energy $`\mathrm{}\mathrm{\Omega }_L`$. The detuning of the generated radiation frequency from the first resonance amounts to $`\mathrm{\Omega }_S=\mathrm{\Omega }_1+\mathrm{\Omega }_2`$, and that from the second resonance is $`\mathrm{\Omega }=\mathrm{\Omega }_S\mathrm{\Omega }_L`$. The corresponding quantum channels may interfere differently when the detunings $`\mathrm{\Omega }_1,\mathrm{\Omega }_2`$ and $`\mathrm{\Omega }_L`$ are altered, which is manifested in the spectral characteristics of the absorption and nonlinear-optical generation processes. The relative role of these channels is governed by the intensities of the radiations, by their detunings from the resonances, and by the ratio of the oscillator strengths for the $`gm`$ and $`g\epsilon `$ transitions. We shall now illustrate these relationships by considering several numerical models.

Figure 4 illustrates the case when the integral oscillator strength for a transition to an energy interval $`E`$ (of the order of the level widths) in the continuum is considerably less than for the $`gm`$ transition $`(C=10^5)`$. The frequencies $`\omega _1`$ and $`\omega _2`$ are detuned far from their one-photon transitions, but the frequency sum is close to a perturbed two-photon resonance. It is evident from Fig. 4 that changes in $`\mathrm{\Omega }_L`$ (because of variation of the frequencies $`\omega `$ or $`\omega _3`$) reduce, for the selected Fano parameters and radiations, the absorption coefficient $`\alpha _1`$ by approximately threefold, increase $`\alpha _S`$ approximately by a factor of 3.8 in one detuning interval, and reduce considerably this coefficient in the other interval, whereas the square of the modulus of the nonlinear polarization (proportional to $`\overline{\eta }_{\mathrm{q0}}`$) increases by a factor of 1.9 (these changes are relative to the values of the corresponding parameters in the far wings where the effects of the strong field $`E`$ do not appear) \[Fig. 4 (a)\]. The absorption coefficient for a transition to the continuum remains on the whole much less than $`\alpha _1`$ ($`\alpha _S/\alpha _1=C\overline{\alpha }_S/\overline{\alpha }_110^2`$). In a certain range of $`\mathrm{\Omega }_L`$, the sign of $`\overline{b}`$ becomes positive, and the nonlinear-optical conversion rate begins to exceed the rate of absorption of the radiation. It is in this interval that there is a sharp maximum of the quantum efficiency of conversion (the dependence of this conversion efficiency on the optical thickness and on $`\mathrm{\Omega }_L`$ is demonstrated in Fig. 4 (c), where the maximum $`\eta _{\mathrm{q}\mathrm{max}}=0.29`$ is reached for $`z\alpha _{10}=4000`$). The absorption of the radiation $`E_1`$ alters considerably the dependence of the power of the generated radiation on $`\mathrm{\Omega }_L`$ along the medium \[Fig. 4 (b)\].

Figure 5 is computed for the case where the detuning from a one-photon resonance is still large, but the oscillator strengths for a discrete transition and a transition to the continuum differ less $`(C=310^2)`$. Then, under the action of the field $`E`$, variation of $`\mathrm{\Omega }_L`$ can reduce the absorption coefficient $`\alpha _1`$ by a factor of just 1.5, whereas the absorption coefficient $`\alpha _S`$ increases approximately threefold in one interval, but falls considerably in the other interval; practically throughout the whole range of the detuning $`\mathrm{\Omega }_L`$, the dominant effect is the absorption transition into the continuum ($`\alpha _S/\alpha _170`$), and $`\overline{\eta }_{\mathrm{q0}}`$ increases by a factor of 1.9 \[Fig. 5(a)\]. The quantity $`\overline{b}`$ is always positive and has a characteristic maximum in a certain interval of $`\mathrm{\Omega }_L`$. For a given detuning, the rate of conversion begins to exceed the rate of absorption so much that an oscillatory regime appears along the medium. Propagation in an optically-dense medium makes the spectrum of the output power significantly dependent on the optical length of the medium, i.e., on $`z`$ or on the concentration $`N`$ of atoms. The absolute amplitude and the position of the maximum change, and new resonances appear \[Fig. 5(b)\]. At the first maximum (corresponding to $`z\alpha _{10}125`$) the quantum efficiency of conversion can reach 0.9 \[Fig. 5(c)\], which is three times greater than in the preceding case.

In view of the nonresonant nature of the interaction, the attainment of such high values of the quantum efficiency of conversion requires high intensities of the $`E_2`$ and $`E_3`$, radiations, and also long lengths (or high densities of atoms) of the medium. The use of resonant processes makes it possible to reduce the required intensities and to reach considerable values of the quantum efficiency by optimization of the bleaching and interference effects. Figure 6 illustrates the case where the ratio of oscillator strengths is the same as in Fig. 5, but there is no detuning from a one-photon resonance. At intensities of the $`E_2`$ radiation three orders of magnitude less than in the preceding case, it is possible to reduce the absorption coefficient of the $`E_1`$ radiation approximately by a factor of 10 compared with the value of this coefficient in the absence of strong fields (the maximum effect of the field $`E`$ is a reduction in this coefficient by a factor of 1.5) \[Fig. 6(a)\]. In the region of reduction in $`\alpha _1`$, the value of $`\alpha _S`$ increases approximately threefold and $`\overline{\eta }_{\mathrm{q0}}`$ by a factor of 4.7. The absorption coefficients $`\alpha _1`$ and $`\alpha _S`$ are then comparable, and the nonlinear-optical conversion rate exceeds considerably, in a wide range of $`\mathrm{\Omega }_L`$, the rates of absorption of the radiations, reaching a sharp maximum at $`\mathrm{\Omega }_L/\mathrm{\Gamma }_{gf}=250`$. This gives rise to an oscillatory regime of generation along the medium in this detuning range \[Figs. 6(b,c)\], i.e., it leads to the feasibility of total (apart from that lost by absorption) conversion of the radiations $`E_1`$ and $`E_S`$ (and vice versa) for certain products of the length of the medium and the concentration of atoms. For the selected parameters, the conversion efficiency at the first maximum (where $`z\alpha _{10}5`$) reaches 0.54. This is less than in the preceding case because of the much greater absolute values of the absorption coefficient, but this efficiency is reached at much lower intensities and for much smaller lengths of the nonlinear medium and much lower concentration of atoms in this medium.

### 2.5 Absorption and dispersive spectra at Doppler-broadened transitions

A Lorentzian line profile with near natural linewidth can be observed only by making use special techniques, like atomic jets. Analysis shows that the contributions of atoms at different velocities in a Doppler-broadened medium may completely change the features described above. Figures 7 and 8 demonstrate that proper adjustment of the orientation of the wavevectors, along with the intensities and detunings of the coupled waves, provides additional means to manipulate the lineshape. Moreover, enhanced subDoppler structures can be formed by the compensation for Doppler shifts by power shifts. For details of the physics, see Sh , Ba  and references therein. The plots dshow that the interference of contributions from the atoms at different velocities brings an important distinction in appearance of quantum interference processes at coupled discrete and continuous states. The figures show that the appearance of quantum interference at Doppler-broadened transitions also may be both constructive and distractive, depending on the detunings of $`\omega \omega _3`$ from $`\omega _{nf}`$, on the Fano parameters, on the detunings from the two-photon resonance $`gn`$, on the ratios of the wavenumbers, and on orientations of the wavevectors.

## 3 Four-wave mixing, dissociation and population transfer controlled by LICS in folded energy-level schemes

Here, we will consider the folded scheme, which is characteristic for molecules with low-lying predissociation states. Such a coupling configuration allows coherent laser control of dissociation through the ’dark’ states that are not connected with the ground one by the allowed transition. On the other hand, the scheme under consideration enables one to transfer the population between two upper bound states which are not connected directly too. Thus, we will explore the possibilities of manipulating dissociation and populations of excited states through implementation of the interference of quantum pathways via a variety of low-lying continuum states.

The proposed coupling scheme is illustrated in the energy level diagram depicted in Fig. 9. The radiation at frequency $`\omega _1`$ couples the bound-bound transition $`mn`$, and radiations at the frequencies $`\omega _2`$ and $`\omega _3`$ couple the bound states $`n`$ and $`f`$ with the states of dissociation continuum $`\epsilon `$, as shown in the picture. Density matrix equations, which are employed for investigating population transfer, account for both relaxation and incoherent excitation of the discrete states:

$`\dot{\rho }_{n\epsilon }=i\left(\rho _{nn}V_{n\epsilon }+\rho _{nf}V_{f\epsilon }\right),`$
$`\dot{\rho }_{f\epsilon }=i\left(\rho _{ff}V_{f\epsilon }+\rho _{fn}V_{n\epsilon }\right),`$
$`\dot{\rho }_{m\epsilon }=i\left(\rho _{mn}V_{n\epsilon }+\rho _{mf}V_{f\epsilon }\right),`$
$`\dot{\rho }_{mn}+\mathrm{\Gamma }_{mn}\rho _{mn}=i\left(\rho _{mm}V_{mn}+{\displaystyle 𝑑\epsilon \rho _{m\epsilon }V_{\epsilon n}}V_{mn}\rho _{nn}\right),`$
$`\dot{\rho }_{mf}+\mathrm{\Gamma }_{mf}\rho _{mf}=i\left({\displaystyle 𝑑\epsilon \rho _{m\epsilon }V_{\epsilon f}}V_{mn}\rho _{nf}\right),`$ (3.27)
$`\dot{\rho }_{nf}+\mathrm{\Gamma }_{nf}\rho _{nf}=i\left({\displaystyle 𝑑\epsilon \rho _{n\epsilon }V_{\epsilon f}}{\displaystyle 𝑑\epsilon V_{n\epsilon }\rho _{\epsilon f}}V_{nm}\rho _{mf}\right),`$
$`\dot{\rho }_{\epsilon \epsilon }=2\text{Re }\left(i{\displaystyle 𝑑\epsilon V_{\epsilon n}\rho _{n\epsilon }}+i{\displaystyle 𝑑\epsilon V_{\epsilon f}\rho _{f\epsilon }}\right),`$
$`\dot{\rho }_{nn}+\mathrm{\Gamma }_n\rho _{nn}=2\text{Re }\left(i{\displaystyle 𝑑\epsilon V_{n\epsilon }\rho _{\epsilon n}}+iV_{nm}\rho _{mn}\right)+Q_n,`$
$`\dot{\rho }_{ff}+\mathrm{\Gamma }_f\rho _{ff}=2\text{Re }\left(i{\displaystyle 𝑑\epsilon V_{f\epsilon }\rho _{\epsilon f}}\right)+Q_f,`$ (3.28)
$`\dot{\rho }_{mm}+\mathrm{\Gamma }_m\rho _{mm}=2\text{Re }\left(iV_{mn}\rho _{nm}\right)+Q_m+w_{nm}\rho _{nn}.`$
Here, $`Q_i`$ is the rate of incoherent excitation to level $`i`$, $`\mathrm{\Gamma }_i\rho _{ii}`$ is the rate of relaxation, $`w_{nm}`$ is the probability of excitation of level $`m`$ due to the relaxation transitions from level $`n`$, and $`V_{jk}`$ and $`V_{j\epsilon }`$ are the corresponding matrix elements of the quasi-resonant electrodipole interaction of the driving field and molecules scaled to Planck’s constant $`\mathrm{}`$. The system of equations (3.28) corresponds to the case of an open energy level configuration. This implies that all the levels coupled with the driving fields, including level $`m`$, can be incoherently excited from the reservoir of much greater populated lower levels, so that the parameters $`Q_j`$ are constant.

For the closed schemes, i.e., the schemes where level $`m`$ is a ground one, and therefore incoherent excitation of the upper levels depends on population transfer stimulated by the applied fields, the equations for the populations take the form

$`\dot{\rho }_{ff}+\mathrm{\Gamma }_f\rho _{ff}=2\text{Re }\left(i{\displaystyle 𝑑\epsilon V_{f\epsilon }\rho _{\epsilon f}}\right)+w_f\rho _{mm},`$
$`\dot{\rho }_{nn}+\mathrm{\Gamma }_n\rho _{nn}=2\text{Re }\left(i{\displaystyle 𝑑\epsilon V_{n\epsilon }\rho _{\epsilon n}}+iV_{nm}\rho _{mn}\right)+w_n\rho _{mm},`$ (3.29)
$`\rho _{mm}=1\rho _{nn}\rho _{ff}{\displaystyle \dot{W}𝑑t}.`$
Here, $`w_i`$ describes the probability of excitation to level $`i`$ from the ground state, and $`\dot{W}`$ is rate of dissociation.

In the equations (3.27), the terms like $`\rho _{\epsilon k}V_{kj}`$ ($`j,k=n,m`$) are discarded. This is valid because coherence at discrete-discrete two-photon transitions is usually much stronger than that at bound-free two-photon transitions. The driving fields couple the interval of continuum states in the vicinity of the resonant energy $`\epsilon _0`$ that is roughly equal to the width of the coupled power-broadened discrete levels. However, the oscillation strength at a bound-free transition is distributed over a much wider energy interval. Therefore, the fraction of oscillator strength attributed to the coupled energy interval is usually relatively small. The requirement derived with the aid of the Laplace transformation indicates that the indicated terms in the above equations can be neglected until

$`f/\epsilon _{\epsilon =\epsilon _0}>>\mathrm{}|V_{jk}|^2f/\epsilon _{\epsilon =\epsilon _0}^2,`$ (3.30)
where $`f(\epsilon )`$ is the energy density of the transition oscillator strength. Such a requirement is fulfilled practically for all realistic atomic and molecular continua in the energy range that is well above the ionization or dissociation threshold.

### 3.1 Quasistationary solution of density matrix equations

In this section we shall assume that all radiations are continuous waves or rectangular pulses with duration $`\tau `$ that is much greater than all relaxation times in the quantum system under investigation. We will consider also the case of small loss of molecules due to dissociation for the period of measurement or the pulse duration, so that the quasi-stationary regime is established. The corresponding requirement is

$`{\displaystyle \underset{0}{\overset{\tau }{}}}\dot{W}𝑑t=W(\tau )<<1,`$ (3.31)
where the dissociation yield $`\dot{W}dt`$ is described by the equation

$`\dot{W}=\dot{\rho }_\epsilon =2\text{Re }\left(i{\displaystyle 𝑑\epsilon V_{\epsilon n}\rho _{n\epsilon }}+i{\displaystyle 𝑑\epsilon V_{\epsilon f}\rho _{f\epsilon }}\right).`$ (3.32)
Quasi-stationary solutions of the density matrix can be found in the form

$`\rho _{ii}=r_i(i=m,n,f),\rho _{ij}=r_{ij}\mathrm{exp}(i\mathrm{\Omega }_{ij}t),\rho _{j\epsilon }=r_{j\epsilon }\mathrm{exp}(i\mathrm{\Omega }_{j\epsilon }t),`$
$`V_{ij}=G_{ij}\mathrm{exp}(i\mathrm{\Omega }_{ij}t),V_{j\epsilon }=G_{j\epsilon }\mathrm{exp}(i\mathrm{\Omega }_{j\epsilon }t).`$ (3.33)
Here, $`G_{ij}=E_kd_{ij}/2\mathrm{}`$, $`G_{j\epsilon }=E_kd_{j\epsilon }/2\mathrm{}`$, $`\mathrm{\Omega }_{mn}=\omega _1\omega _{mn}`$, $`\mathrm{\Omega }_{nf}=\omega _3\omega _2\omega _{nf}`$, $`\mathrm{\Omega }_{mf}=\omega _1\omega _2+\omega _3\omega _{mf}`$, $`\mathrm{\Omega }_{n\epsilon }=\omega _2\omega _{n\epsilon }`$, $`\mathrm{\Omega }_{f\epsilon }=\omega _3\omega _{f\epsilon }`$, and $`\mathrm{\Omega }_{m\epsilon }=\omega _1\omega _2\omega _{m\epsilon }`$. The amplitudes of the resonant fields $`E_k`$ (see Fig. 9), and consequently all amplitudes $`r_i`$, $`r_{ij}`$, and $`r_{j\epsilon }`$, are assumed to be independent of time. Then, by introducing the expressions (3.33) to the equations (3.27), we can reduce them to a system of algebraic ones:

$`ir_{n\epsilon }p_{n\epsilon }=r_nG_{n\epsilon }r_{nf}G_{f\epsilon },p_{n\epsilon }=i(\omega _2\omega _{n\epsilon });`$
$`ir_{f\epsilon }p_{f\epsilon }=r_fG_{f\epsilon }r_{fn}G_{n\epsilon },p_{f\epsilon }=i(\omega _3\omega _{f\epsilon });`$
$`ir_{m\epsilon }p_{m\epsilon }=r_{mn}G_{n\epsilon }r_{mf}G_{f\epsilon },p_{m\epsilon }=i(\omega _1\omega _2\omega _{m\epsilon });`$
$`ir_{mn}p_{mn}={\displaystyle 𝑑\epsilon r_{m\epsilon }G_{\epsilon n}}r_mG_{mn}+G_{mn}r_n,p_{mn}=\mathrm{\Gamma }_{mn}+i(\omega _1\omega _{mn});`$ (3.34)
$`ir_{mf}p_{mf}={\displaystyle 𝑑\epsilon r_{m\epsilon }G_{\epsilon f}}+G_{mn}r_{nf},p_{mf}=\mathrm{\Gamma }_{mf}+i(\omega _1\omega _2+\omega _3\omega _{mf});`$
$`ir_{nf}p_{nf}={\displaystyle 𝑑\epsilon r_{n\epsilon }G_{\epsilon f}}+{\displaystyle 𝑑\epsilon G_{n\epsilon }r_{\epsilon f}}+G_{nm}r_{mf},p_{nf}=\mathrm{\Gamma }_{fn}\pm i(\omega _3\omega _2\omega _{nf}).`$
Further by introducing the solutions of the first, second and third equations to the integrals and with the aid of the $`\zeta `$-function (2.14), we obtain

$`r_{mn}\left[\delta _{nn}^m\mathrm{\Omega }_{mn}+i(\mathrm{\Gamma }_{mn}+\gamma _{nn}^m)\right]=\left(r_nr_m\right)G_{mn}r_{mf}\left(\delta _{fn}^m+i\gamma _{fn}^m\right),`$
$`r_{mf}\left[\delta _{ff}^m\mathrm{\Omega }_{mf}+i(\mathrm{\Gamma }_{mf}+\gamma _{ff}^m)\right]=G_{mn}r_{nf}r_{mn}\left(\delta _{nf}^m+i\gamma _{nf}^m\right),`$ (3.35)
$`r_{nf}\left[\delta _{ff}^n\delta _{nn}^f\mathrm{\Omega }_{nf}+i(\mathrm{\Gamma }_{nf}+\gamma _{ff}^n+\gamma _{nn}^f)\right]=G_{nm}r_{mf}+r_f\left(\delta _{nf}^fi\gamma _{nf}^f\right)r_n\left(\delta _{nf}^n+i\gamma _{nf}^n\right),`$
where

$`\gamma _{nn}^m=\pi \mathrm{}G_{n\epsilon _{12}}G_{\epsilon _{12}n}+\text{Re }\left(G_{nk}G_{kn}/p_{mk}\right),`$
$`\delta _{nn}^m=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{n\epsilon }G_{\epsilon n}/(\epsilon _{12}\epsilon )}+\text{Im }\left(G_{nk}G_{kn}/p_{mk}\right);`$
$`\gamma _{ff}^m=\pi \mathrm{}G_{f\epsilon _{12}}G_{\epsilon _{12}f}+\text{Re }\left(G_{fk}G_{kf}/p_{mk}\right),`$
$`\delta _{ff}^m=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{f\epsilon }G_{\epsilon f}/(\epsilon _{12}\epsilon )}+\text{Im }\left(G_{fk}G_{kf}/p_{mk}\right);`$
$`\gamma _{nf}^m=\pi \mathrm{}G_{n\epsilon _{12}}G_{\epsilon _{12}f}+\text{Re }\left(G_{nk}G_{kf}/p_{mk}\right),`$ (3.36)
$`\delta _{nf}^m=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{n\epsilon }G_{\epsilon f}/(\epsilon _{12}\epsilon )}+\text{Im }\left(G_{nk}G_{kf}/p_{mk}\right);`$
$`\gamma _{fn}^m=\pi \mathrm{}G_{f\epsilon _{12}}G_{\epsilon _{12}n}+\text{Re }\left(G_{fk}G_{kn}/p_{mk}\right),`$
$`\delta _{fn}^m=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{f\epsilon }G_{\epsilon n}/(\epsilon _{12}\epsilon )}+\text{Im }\left(G_{fk}G_{kn}/p_{mk}\right);`$
$`\gamma _{nn}^n=\pi \mathrm{}G_{n\epsilon _2}G_{\epsilon _2n}+\text{Re }\left(G_{nk}G_{kn}/p_{kn}\right),`$
$`\delta _{nn}^n=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{n\epsilon }G_{\epsilon n}/(\epsilon _2\epsilon )}+\text{Im }\left(G_{nk}G_{kn}/p_{kn}\right);`$
$`\gamma _{ff}^n=\pi \mathrm{}G_{f\epsilon _2}G_{\epsilon _2f}+\text{Re }\left(G_{fk}G_{kf}/p_{kn}\right),`$
$`\delta _{ff}^n=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{f\epsilon }G_{\epsilon f}/(\epsilon _2\epsilon )}+\text{Im }\left(G_{fk}G_{kf}/p_{kn}\right);`$
$`\gamma _{nf}^n=\pi \mathrm{}G_{n\epsilon _2}G_{\epsilon _2f}+\text{Re }\left(G_{nk}G_{kf}/p_{kn}\right),`$ (3.37)
$`\delta _{nf}^n=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{n\epsilon }G_{\epsilon f}/(\epsilon _2\epsilon )}+\text{Im }\left(G_{nk}G_{kf}/p_{kn}\right);`$
$`\gamma _{fn}^n=\pi \mathrm{}G_{f\epsilon _2}G_{\epsilon _2n}+\text{Re }\left(G_{fk}G_{kn}/p_{kn}\right),`$
$`\delta _{fn}^n=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{f\epsilon }G_{\epsilon n}/(\epsilon _2\epsilon )}+\text{Im }\left(G_{fk}G_{kn}/p_{kn}\right);`$
$`\gamma _{nn}^f=\pi \mathrm{}G_{n\epsilon _3}G_{\epsilon _3n}+\text{Re }\left(G_{nk}G_{kn}/p_{kf}\right),`$
$`\delta _{nn}^f=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{n\epsilon }G_{\epsilon n}/(\epsilon _3\epsilon )}+\text{Im }\left(G_{nk}G_{kn}/p_{kf}\right);`$
$`\gamma _{ff}^f=\pi \mathrm{}G_{f\epsilon _3}G_{\epsilon _3f}+\text{Re }\left(G_{fk}G_{kf}/p_{kf}\right),`$
$`\delta _{ff}^f=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{f\epsilon }G_{\epsilon f}/(\epsilon _3\epsilon )}+\text{Im }\left(G_{fk}G_{kf}/p_{kf}\right);`$
$`\gamma _{nf}^f=\pi \mathrm{}G_{n\epsilon _3}G_{\epsilon _3f}+\text{Re }\left(G_{nk}G_{kf}/p_{kf}\right),`$ (3.38)
$`\delta _{nf}^f=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{n\epsilon }G_{\epsilon f}/(\epsilon _3\epsilon )}+\text{Im }\left(G_{nk}G_{kf}/p_{kf}\right);`$
$`\gamma _{fn}^f=\pi \mathrm{}G_{f\epsilon _3}G_{\epsilon _3n}+\text{Re }\left(G_{fk}G_{kn}/p_{kf}\right),`$
$`\delta _{fn}^f=\mathrm{}𝒫{\displaystyle 𝑑\epsilon G_{f\epsilon }G_{\epsilon n}/(\epsilon _3\epsilon )}+\text{Im }\left(G_{fk}G_{kn}/p_{kf}\right).`$
and

$`\epsilon _{12}`$ $`=\mathrm{}(\omega _1\omega _2),\epsilon _2=E_n\mathrm{}\omega _2,\epsilon _3=E_f\mathrm{}\omega _3,`$ (3.39)
$`p_{mk}`$ $`=\mathrm{\Gamma }_{mk}+i(\omega _1\omega _2\omega _{mk}),p_{kn}=\mathrm{\Gamma }_{kn}+i(\omega _{kn}\omega _2),p_{kf}=\mathrm{\Gamma }_{kf}+i(\omega _{kf}\omega _3).`$
Besides the continuum states, a contribution of other non-resonant levels $`k`$ is taken into account too and a sum over repeating $`k`$ index is assumed. The contribution from these levels may occur commensurable to that of the continuum states. As seen from the equations (3.35), the values $`\gamma _{ij}`$ and $`\delta _{ij}`$ describe light-induced broadening and shifts of discrete resonances stipulated by the induced transitions between them through the continuum. The parameters $`q_{ij}=\delta _{ij}/\gamma _{ij}`$ are analogous to the Fano parameters for autoionizing states. Within the validity of (3.30), their dependence on the field intensities can be neglected. These parameters determine the most important features of the processes under investigation since they characterize the relative integrated contribution of all off-resonant quantum states compared to the resonant ones.

With the aid of (3.34), the equation for the dissociation rate (3.32) takes the form

$`\dot{W}=\dot{r}_\epsilon =2\left[\gamma _{nn}^nr_n+\gamma _{ff}^fr_f+2\text{Re }(\gamma _{fn}r_{nf})\right].`$ (3.40)
The first two terms on RHS describe induced transitions to the continuum from the corresponding discrete levels, whose populations are determined by a variety of processes. Most important is the last term describing quantum interference, which occurs if two LICS overlap. Let us consider specific features of the processes in both open and closed energy level configurations.

#### 3.1.1 Open configuration

In this case in the same way as above, one obtains

$`r_m\mathrm{\Gamma }_m=w_{nm}r_n+Q_m2\text{Re }(iG_{mn}r_{nm}),`$
$`r_f(\mathrm{\Gamma }_f+2\gamma _{ff}^f)=Q_f2\text{Re }\left(r_{nf}[\gamma _{fn}^f+i\delta _{fn}^f]\right),`$ (3.41)
$`r_n(\mathrm{\Gamma }_n+2\gamma _{nn}^n)=Q_n2\text{Re }(iG_{nm}r_{mn}+r_{nf}[(\gamma _{fn}^ni\delta _{fn}^n]).`$
Then the solution of (3.35) and (3.41) can be presented in the form

$`r_{nf}=\left\{(r_nr_m)|G_{mn}|^2\gamma _{nf}^m(1iq_{nf}^m)[r_f\gamma _{nf}^f(1+iq_{nf}^f)+r_n\gamma _{nf}^n(1iq_{nf}^n)]Y\right\}Z^1,`$
$`r_m=(L_1C_1+L_2S_1)/(C_1C_2S_1S_2),r_n=(L_2+S_2r_m)/C_1,`$
$`r_f=[Q_f+2r_nB_4^{fn}+2(r_mr_n)M_4^{fm}]Y_f^1.`$ (3.42)
The notations introduced here are as follows:

$`C_1=Y_{nm}Y_fL_1L_2,C_2=[\mathrm{\Gamma }_m+2(GM_1^{mm})]Y_f4M_4^{fm}M_3^{mf},`$
$`S_1=[w_{nm}+2(G+M_1^{mn}D)]Y_f+2L_2M_3^{mf},S_2=PY_f+2M_4^{fm}L_1,`$
$`F_1=Q_mY_f+2Q_fM_3^{mf},F_2=Q_nY_fQ_fL_1,P=2(GM_1^{nm}+D),`$
$`L_1=2(B_3^{nf}2M_3^{mf}),L_2=2(B_4^{fn}M_4^{fm}),Y_f=\stackrel{~}{\mathrm{\Gamma }}_f2B_2^{ff},`$
$`Y_{nm}=\stackrel{~}{\mathrm{\Gamma }}_n+2(GB_1^{nn}+M_1^{mn}D),G=|G_{mn}|^2\text{Re }(y_{mf}/Y),`$
$`B_i^{jl}=\gamma _{nn}^j\gamma _{nn}^l\text{Re }(b_i^{jl}Y/Z),M_i^{jl}=|G_{mn}|^2\gamma _{nn}^j\gamma _{ff}^l\text{Re }(b_i^{jl}/Z),`$
$`D=|G_{mn}|^4\gamma _{nn}^m\gamma _{ff}^m\text{Re }[k_1^{mm}/(YZ)],j,l=m,n,f;`$
$`Y=y_{mn}y_{mf}\gamma _{nn}^m\gamma _{ff}^mb_1^{mm},Z=y_{mf}y_{nf}y_{mn}\gamma _{nn}^m\gamma _{ff}^mb_1^{mm}y_{nf}+|G_{mn}|^2y_{mn},`$
$`y_{mn}=\stackrel{~}{\mathrm{\Gamma }}_{mn}+i(\mathrm{\Omega }_{mn}\delta _{nn}^m),y_{mf}=\stackrel{~}{\mathrm{\Gamma }}_{mf}+i(\mathrm{\Omega }_{mf}\delta _{ff}^m),`$
$`y_{nf}=\stackrel{~}{\mathrm{\Gamma }}_{nf}+i(\mathrm{\Omega }_{nf}+\delta _{nn}^f\delta _{ff}^n),b_1^{jl}=k_o(1iq_{fn}^j)(1iq_{nf}^l),`$
$`b_2^{jl}=k_o(1+iq_{fn}^j)(1+iq_{nf}^l),b_3^{jl}=k_o(1iq_{fn}^j)(1+iq_{nf}^l),`$
$`b_4^{jl}=k_o(1+iq_{fn}^j)(1iq_{nf}^l),k_o=(\gamma _{nf}^j\gamma _{fn}^l)/(\gamma _{nn}^j\gamma _{ff}^l),\stackrel{~}{\mathrm{\Gamma }}_{nf}=\mathrm{\Gamma }_{nf}+\gamma _{nn}^f+\gamma _{ff}^n,`$
$`\stackrel{~}{\mathrm{\Gamma }}_{mn}=\mathrm{\Gamma }_{mn}+\gamma _{nn}^m,\stackrel{~}{\mathrm{\Gamma }}_{mf}=\mathrm{\Gamma }_{mf}+\gamma _{ff}^m,\stackrel{~}{\mathrm{\Gamma }}_n=\mathrm{\Gamma }_n+2\gamma _{nn}^n+w_{nm},\stackrel{~}{\mathrm{\Gamma }}_f=\mathrm{\Gamma }_f+2\gamma _{ff}^f.`$ (3.43)
First, consider the effect of the interference of two LICS in the case where the laser field at discrete transition is turned off ($`G_{mn}=0`$). Then the solution (3.42) takes the more simple form of

$`r_{nf}=[r_f\gamma _{nf}^f(1+iq_{nf}^f)+r_n\gamma _{nf}^n(1iq_{nf}^n)]y_{nf}^1,r_m=Q_m/\mathrm{\Gamma }_m+w_{nm}r_n,`$
$`r_n=(Q_nY_f2Q_f\gamma _{nn}^n\gamma _{ff}^f\text{Re }\left(b_3^{nf}/y_{nf}\right))/\mathrm{\Delta },`$
$`r_f=(Q_fY_n+2Q_n\gamma _{nn}^f\gamma _{ff}^n\text{Re }\left(b_4^{fn}/y_{nf}\right))/\mathrm{\Delta },`$
$`Y_n=\stackrel{~}{\mathrm{\Gamma }}_n2\gamma _{nn}^n\gamma _{ff}^n\text{Re }\left(b_1^{nn}/y_{nf}\right),Y_f=\stackrel{~}{\mathrm{\Gamma }}_f2\gamma _{nn}^f\gamma _{ff}^f\text{Re }\left(b_2^{ff}/y_{nf}\right),`$
$`\mathrm{\Delta }=Y_fY_n4(\gamma _{nn}^n\gamma _{nn}^f)^2\text{Re }\left(b_4^{fn}/y_{nf}\right)\text{Re }\left(b_3^{nf}/y_{nf}\right).`$ (3.44)
The process of dissociation is described by the formula (3.40) with the aid of (3.44). All the terms proportional to $`\text{Re }(\mathrm{})`$ describe interference processes and disappear for either of the driving fields $`E_2`$ or $`E_3`$ being turned off. The corresponding spectral structures are power broadened (terms with $`\gamma `$) and of an asymmetric shape that is determined by the power-shifts (terms with $`\delta `$) and by the Fano parameters $`q`$ for the corresponding coupled excited levels. The position and shape of the laser-induced autoionizing-like resonance within the continuum can be varied with the change of the frequencies and intensities of the driving fields. Constructive interference can be turned into destructive by small variation of the overlap of two LICS, which forms a basis for coherent quantum control of photophysical processes by the driving lasers. This will be illustrated below with numerical examples.

If either $`E_2`$ or $`E_3`$ is turned off ($`\gamma _{nf}^j=0`$), the equations (3.42) take the standard form that accounts for power-broadening of the level $`f`$ or $`n`$ depending on which field is turned off. When $`E_3=0`$, we obtain

$`r_m`$ $`={\displaystyle \frac{Q_m+Q_nw_{nm}/\stackrel{~}{\mathrm{\Gamma }}_n+2(Q_m+Q_n)|G_{mn}|^2/|y_{mn}|^2}{\mathrm{\Gamma }_m+2(\mathrm{\Gamma }_m+\stackrel{~}{\mathrm{\Gamma }}_nw_{nm})|G_{mn}|^2/|y_{mn}|^2}},r_f=Q_f/\stackrel{~}{\mathrm{\Gamma }}_f,`$
$`r_n`$ $`={\displaystyle \frac{Q_m\mathrm{\Gamma }_m/\stackrel{~}{\mathrm{\Gamma }}_n+2(Q_m+Q_n)|G_{mn}|^2/|y_{mn}|^2}{\mathrm{\Gamma }_m+2(\mathrm{\Gamma }_m+\stackrel{~}{\mathrm{\Gamma }}_nw_{nm})|G_{mn}|^2/|y_{mn}|^2}},\dot{W}=2\gamma _{nn}^nr_n.`$ (3.45)
These expressions describe a process of two-photon dissociation without any interference phenomena in the spectral continuum. Opportunities for manipulating dissociation and population transfer through the interference of two LICS follows from a comparison of equations (3.42) and (3.45).

#### 3.1.2 Closed configuration

Assuming $`\dot{W}𝑑t<<1`$ in (3.29), so that $`r_m+r_n+r_f1`$, the equations for levels populations in a closed scheme can be written as

$`r_n\stackrel{~}{\mathrm{\Gamma }}_n`$ $`=2\text{Re }\left[iG_{nm}r_{mn}+r_{nf}(\gamma _{fn}^n+i\delta _{fn}^n)\right]+w_nr_m,`$
$`r_f\stackrel{~}{\mathrm{\Gamma }}_f`$ $`=2\text{Re }\left[r_{fn}(\gamma _{nf}^f+i\delta _{nf}^f)\right]+w_fr_m,r_m=1r_nr_f.`$ (3.46)
Then, with the aid of (3.35), the solution for the populations of the excited levels can be presented in the form

$`r_m=`$ $`1r_nr_f,r_n=\left[Y_f(w_n+P)+L_1(w_f+2M_4^{fm})\right]\mathrm{\Delta }_{c}^{}{}_{}{}^{1},`$
$`r_f=`$ $`\left[Y_{nm}(w_f+2M_4^{fm})+L_2(w_n+P)\right]\mathrm{\Delta }_{c}^{}{}_{}{}^{1},`$ (3.47)
$`\mathrm{\Delta }_c=`$ $`(\stackrel{~}{\mathrm{\Gamma }}_n+w_n+4G2B_1^{nn})(Y_f+w_f+2M_4^{fm})(w_f2B_4^{fn})(w_n+PL_1).`$ (3.48)
The other notation are the same as in (3.43). Equations (3.48) describe similar interference structures as discussed in the previous sections, but account for the effects of driving fields on incoherent excitation. For $`E_1`$ turned off, these equations describing LICS reduce to

$`r_n`$ $`=\left(Y_fw_n+k_nw_f\right)/\mathrm{\Delta }_c^{},r_f=\left(Y_nw_f+k_fw_n\right)/\mathrm{\Delta }_c^{},`$
$`\mathrm{\Delta }_c^{}`$ $`=(Y_f+w_f)(Y_n+w_n)k_nk_f,`$ (3.49)
$`k_n`$ $`=2\gamma _{nn}^n\gamma _{ff}^f\text{Re }\left(b_3^{nf}/y_{nf}\right)w_n,k_f=2\gamma _{nn}^n\gamma _{ff}^f\text{Re }\left(b_4^{fn}/y_{nf}\right)w_f,`$ (3.50)
and the dissociation rate is calculated with the aid of equation (3.40). In the case of $`E_3=0`$, dissociation from an incoherently populated level $`n`$ is described by the equation in the common form of

$`\dot{W}/2=\gamma _{nn}^nw_n/(\mathrm{\Gamma }_n+2\gamma _{nn}^n+w_n).`$ (3.51)
Two-photon dissociation from the ground level, when the field $`E_3`$ is off, can be analyzed with the formula

$`\dot{W}/2={\displaystyle \frac{\gamma _{nn}^n(w_n+2|G_{mn}|^2\stackrel{~}{\mathrm{\Gamma }}_{mn}/|y_{mn}|^2)}{\stackrel{~}{\mathrm{\Gamma }}_n+w_n+4|G_{mn}|^2\stackrel{~}{\mathrm{\Gamma }}_{mn}/|y_{mn}|^2}}.`$ (3.52)
To a some extent, LICS can be treated as dressed multiphoton resonances accompanied by the interference of different quantum pathways. As follows from (3.42) and (3.48), when such resonances are not fulfilled and $`|y_{nf}|,|y_{mf}|\gamma ,|G_{mn}|`$, all interference structures disappear. The possibility of coherent quantum control of photodissociation based on the derived equations is illustrated below with the aid of a numerical model relevant to electronic-vibration-rotation terms of the molecule Na<sub>2</sub> in the next section.

### 3.2 Numerical analysis

Many experiments on coherent control of branching chemical reactions have been carried out with sodium dimers Na<sub>2</sub>. In this case, level $`m`$ of our model (Fig. 9) can be attributed to the state $`X^1\mathrm{\Sigma }_g^+(v=0,J=45)`$ for the close configuration and $`X^1\mathrm{\Sigma }_g^+(v=14,J=45)`$ for the open one, levels $`n`$ and $`f`$ to the states $`A^1\mathrm{\Sigma }_u^+(v=6,J=46)`$ and $`B^1\mathrm{\Pi }_u(v=5,J=45)`$ correspondingly, and the continuum states $`\epsilon `$ to the dissociation continuum Na(3s)+Na(3s). The relevant relaxation constants are: $`\mathrm{\Gamma }_m=210^7c^1`$, $`\mathrm{\Gamma }_n=\mathrm{\Gamma }_f=1.210^8c^1`$. The relaxation rates for coherence (off-diagonal elements of the density matrix) are estimated as half of the sum of the corresponding rates for the diagonal elements.

#### 3.2.1 Coherent control of populations and dissociation in folded schemes

Numerical simulation for a closed-type scheme for the quasi-stationary case shows the possibilities of manipulation of continuum resonances through the effects of the interference caused by a strong laser field. Due to the action of strong radiation at a discrete transition, a split of level $`n`$ appeares. Two LICS in the dissociation continuum can be detected by variation of the detunings $`\mathrm{\Omega }_{nf}`$ through the change of frequency of the laser field at the adjacent transition to the continuum $`(f\epsilon )`$.

Figure 10 shows that the dissociation rate can be considerably eliminated or alteratively enhanced by varying either the intensity of the splitting field or the detuning $`\mathrm{\Omega }_{nf}`$. The spectral lineshape at constant field intensities has a well-known asymmetrical Fano profile. The plot (b) shows opportunities for manipulating the population of level $`f`$.

The properties of LICS are essentially determined by the Fano parameters, which indicate an asymmetry in the distribution of the oscillator strength over the continuum, which is illustrated in Fig. 11. By varying the position of the LICS within the continuum, the intensities of the strong laser radiation and the one-photon detuning $`\mathrm{\Omega }_1`$, one can manipulate the properties of the laser-induced structures. Large two-photon detunings lead to the vanishing of any interference phenomena in the continuum and thus is equivalent to the field $`E_3`$ being turned off.

The above obtained results show that dissociation and population transfer through the continuum can be controlled by the field coupled to the discrete transition. Figure 12 displays a very trivial behavior for $`E_1`$ turned off. Other opportunities of manipulating two-photon dissociation and populations transfer are associated with the control field coupling discrete and continuous states.

In the next subsection, we investigate how such behavior may exhibit itself in difference-frequency four-wave mixing and nonlinear-optical generation of frequency-tunable radiation through the continuous states in folded schemes.

#### 3.2.2 Coherent control of generated radiation in folded schemes

Here we consider the case where the fundamental $`E_1`$ and generated $`E_S`$ fields are weak. Then the solution of the density matrix equations (Section 3.1) for a closed-type scheme takes the form

$`r_{mn}=iG_{mn}y_{mf}/(y_{mn}y_{mf}b_1^{mm}),`$
$`r_{mf}=iG_{mn}\gamma _{nf}^m(1iq_{nf})/(y_{mn}y_{mf}b_1^{mm}).`$ (3.53)
Similarly, for the case where the field $`E_S`$ is the probe radiation and $`E_1`$ is the generated one, we obtain

$`R_{mf}=iG_{mf}y_{mn}/(y_{mn}y_{mf}b_1^{mm}),`$
$`R_{mn}=iG_{mf}\gamma _{fn}^m(1iq_{fn})/(y_{mn}y_{mf}b_1^{mm}).`$ (3.54)
Then the wave equations for weak fields, coupled by the four-wave mixing process $`\omega _S\omega _1\omega _2+\omega _3`$, have the form

$`dE_S(z)/dz`$ $`=\mathrm{i2}\pi k_S^{}\chi _S^{(3)}E_2^{}E_3E_1(z)\mathrm{exp}(\mathrm{i}\mathrm{\Delta }kz),`$
$`dE_1(z)/dz`$ $`=\mathrm{i2}\pi k_1^{}\chi _1^{(3)}E_2E_3^{}E_S(z)\mathrm{exp}(\mathrm{i}\mathrm{\Delta }kz),`$ (3.55)
where $`\mathrm{\Delta }k=k_Sk_1+k_2k_3`$.

Analogously to (2.2), the solution of equations (3.55) can be presented like (2.23) with $`\overline{\eta }_{\mathrm{q0}}=\eta _{\mathrm{q0}}^0|\overline{\chi }^{(3)}|^2g_ng_f`$, where $`g_n=\gamma _{nn}/\mathrm{\Gamma }_{mn}`$, $`g_f=\gamma _{ff}/\mathrm{\Gamma }_{mf}`$. With the aid of the approximate expressions

$`\alpha _{10}=4\pi \omega _1|d_{mn}|^2/c\mathrm{}\mathrm{\Gamma }_{mn},\alpha _{S0}=4\pi \omega _S|d_{mf}|^2/c\mathrm{}\mathrm{\Gamma }_{mf},`$
$`|\chi _0|^2=(\pi /8\mathrm{}^2)^2(1+q_{nf}^2)|d_{mn}d_{n\epsilon }d_{\epsilon f}d_{fm}|^2(\mathrm{\Gamma }_{mn}\mathrm{\Gamma }_{mf})^2,`$ (3.56)
we obtain that $`\eta _{\mathrm{q0}}^0=(\pi /2)^2(1+q_{nf}^2)`$. Other notations are the same as in Section 2.4.

Figure 13 illustrates the case where the strong fields are so large that power-broadening exceeds the half-width of the transitions ($`\mathrm{\Gamma }_{ij}`$), and also $`g_f>>g_n`$. Then the generation maximum falls to the parameter range for which absorbtion of the fundamental radiation becomes minimum and the rate of conversion is positive. With that, an oscillation regime appears. Within the interval of $`\mathrm{\Omega }_{nf}/\mathrm{\Gamma }_{mf}`$ from $`1000`$ to $`3000`$, the rates of absorbtion and generation are almost equal ($`b_00`$), and the oscillations reduce to only one maximum of $`\eta _q`$. Figure 14 depicts the case where both driving parameters are equal ($`g_n=g_f=6000`$). Here the maximum of $`\eta _q`$ also falls within the range of minimum absorption of the fundamental radiation, and a conversion dip corresponds to the maximum of $`\alpha _1`$. Interference of LICS along with splitting of the discrete resonance give rise to complex structures in $`\eta _q`$ while the waves propagate through the nonlinear medium \[see Fig. 14(c)\]. For the driving parameters about three order less than in the previous case, and $`g_n=g_f`$, the implementation of interference allows one to achieve four orders of increase of the conversion rate $`b_0`$ (Fig. 15). The maximum in $`\eta _q`$ becomes somehow smaller but is reached at a much shorter length of the nonlinear medium. With greater Fano parameters $`q_{nf}`$, the potential enhancement of the output of generation through manipulating the interplay of LICS becomes greater. As shown in Fig. 16, $`\eta _q1`$ with $`q_{nf}\mathrm{}`$ provided by the appropriate choice of the control fields intensity. Maxima of the quantum efficiency of conversion process reach $`0.996`$ for $`q_{nf}=100`$, $`0.919`$ for $`q_{nf}=5`$ and $`0.569`$ for $`q_{nf}=0`$. At greater magnitudes of $`q_{nf}`$, the resonance broadening increases, which leads to the requirement of longer nonlinear medium. This is seen from comparison of Figs. 17(a) and 17(b). It is seen from comparison of Figs. 16(b) and 18(b) that most of the opportunities for manipulation appear at moderate detunings $`\mathrm{\Omega }_{mn}`$.

## Conclusions

The technique of quantum control of such processes as ionization, chemical reactivity through dissociation of molecules and population transfer, and four-wave mixing is further developed. Other applications involve discrete and broad-band spectra in solids. The approach is based on manipulating constructive and destructive interference of several quantum pathways involving both discrete energy levels (bound states) and energy continua (free states). Analytical and numerical solutions of the set of coupled density-matrix equations and Maxwell equations for travelling electromagnetic waves are found for the continuous-wave regime.

Novel opportunities are shown for suppression or alternatively enhancement of photophysical processes as well as photochemical processes related with branching chemical reactions. These opportunities are associated with the overlap of two laser-induced continuum structures induced by two control fields, while the third strong field controls a discrete transition. The expressions obtained and numerical models developed are used to demonstrate the feasibility of manipulation of the spectral characteristics of the absorption and dispersion both for discrete transitions and the spectral continua in the presence of additional strong laser radiations. Related opportunities to form laser-induced transparency and to enhance four-wave-mixing nonlinear-optical polarizations are investigated as well. It is shown that the implementation of such nonlinear interference effects makes it possible to utilize the advantages of multiple resonances and strong radiations for considerable improvement of the generation of short-wavelength radiation. Among the important features discovered is the fact that the constructive or destructive nature of interference is governed not only by the ratio of the intensities and by the detunings from the discrete resonances, but also by the composite Fano parameters for transitions between high-lying discrete levels over the continuum states. The results can be generalized to higher-order processes. The matrix elements of the interaction Hamiltonian should then be replaced with the corresponding composite multiphoton matrix elements.

## Acknowledgments

This work has been supported in part by the International Association (INTAS) of the European Community for the promotion of cooperation with scientists from the New Independent States of the former Soviet Union (Grant INTAS-99-00019), by the Ministry of Industry and Science of Russian Federation (The 6-th examination contest of projects of young scientists of the Russian Academy of Sciences, Grant #61) and by the Russian Foundation for Basic Research (Grant 02-02-16325a). The authors are grateful to K. Bergmann for discussions and encouragement over the course of this work.


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# Global Regularity for the Viscous Boussinesq Equations

## 1 Introduction

In the numerical studies  and , different observations have been reported on the question of finite time singularities of solutions to the inviscid Boussinesq equations:

$`\theta _t+u\theta =0,`$
$`u_t+uu+p=\left(\begin{array}{c}0\\ \theta \end{array}\right),`$
$`u=0.`$
Here $`\theta `$ is the temperature, $`u=(u_1,u_2)`$ is the velocity, $`p`$ is the pressure. In , Pumir and Siggia observed that the cap of a symmetric rising bubble collapses in a finite time. In contrast, E and Shu in  reported that the motion of the bubble cap is a very unlikely candidate for finite time singularity formation.

In this paper, we prove the global regularity for the viscous Boussinesq equations:

$`\theta _t+u\theta =\kappa \mathrm{\Delta }\theta ,`$
$`u_t+uu+p=\left(\begin{array}{c}0\\ \theta \end{array}\right)+\nu \mathrm{\Delta }u,`$ (1.4)
$`u=0.`$
Here, $`\kappa `$ is the heat diffusion constant, $`\nu `$ is the viscosity constant.

The approach of the proof follows from that of   . Nevertheless, we follow closely . An possible alternative approach is the Galerkin approximation approach as in chapter $`9`$ of .

## 2 Formulation of the Theorem

Consider Eq.(1.4) under the initial conditions:

$$u(0)=b,\theta (0)=\beta ;$$
(2.1)
where $`b`$ is $`C^{\mathrm{}}`$ smooth, divergence free, and compactly supported; $`\beta `$ is also $`C^{\mathrm{}}`$ smooth, compactly supported. Then the question of global regularity is as follows: Does a smooth solution to the Cauchy problem (1.4;2.1) exists for all time ? For any fixed $`T`$, we call a solution of (1.4;2.1) that is in

$$L^{\mathrm{}}([0,T];L^2(R^2))L^2([0,T];H_1(R^2)),$$

a weak solution; a solutions of (1.4;2.1) that is in

$$L^{\mathrm{}}([0,T];H_1(R^2))L^2([0,T];H_2(R^2)),$$

a strong solution. It is known that strong solutions are actually smooth . We will prove the following:

###### Theorem 2.1

The solution to the Cauchy problem (1.4;2.1) for $`\kappa >0`$, $`\nu >0`$ is strong and hence smooth on the time interval \[$`0,T`$\].

and the following:

###### Corollary 1

The solution to the Cauchy problem (1.4;2.1) for $`\kappa >0`$, $`\nu =0`$ satisfies:

$$uL^{\mathrm{}}([0,T];H_1(R^2)),\theta L^{\mathrm{}}([0,T];H_1(R^2))L^2([0,T];H_2(R^2)).$$

## 3 Proof of the Theorem

Consider the mollified equation:

$`\theta _t+u^{(\delta )}\theta =\kappa \mathrm{\Delta }\theta ,`$
$`u_t+u^{(\delta )}u+p=\left(\begin{array}{c}0\\ \theta \end{array}\right)+\nu \mathrm{\Delta }u,`$ (3.3)
$`u=0.`$
In which,

$$u^{(\delta )}=\varphi _\delta u,u^{(\delta )}=0,\varphi _\delta =\delta ^2\varphi (x/\delta ,y/\delta );$$

where $`\varphi `$ is smooth, compactly supported, and has integral equal to 1;

$$\left(\varphi _\delta u\right)(t,x,y)=_{R^2}\varphi _\delta (xx_1,yy_1)u(t,x_1,y_1)𝑑x_1𝑑y_1.$$

It is known that solutions to the Cauchy problem (3.3;2.1) are smooth on any time interval \[$`0,T`$\] . The proof consists of $`a`$ $`posteriori`$ estimates on the mollified equations. The goal is to find uniform bounds in the limit $`\delta 0`$ and pass to the limit to get conclusion for the original Cauchy problem (1.4;2.1).

From the first equation in (3.3), we get

$$\theta ^2(T)+2\kappa _0^T|\theta |^2\beta ^2.$$
(3.4)
Here $``$ stands for $`_{R^2}𝑑x𝑑y`$, $`_0^T`$ stands for $`_0^T𝑑t`$, and $`\theta (T)=\theta (T,x,y)`$. From the second equation in (3.3), we get

$$\frac{d}{dt}|u|^2+2\nu |u|^2=2\theta u_2.$$
(3.5)
Apply Schwarz inequality to the right hand side of (3.5), and use inequality (3.4), we have

$$|u(T)|^2+2\nu _0^T|u|^2\mathrm{\Gamma }_1,$$
(3.6)
where $`\mathrm{\Gamma }_1`$ is a constant depending only on $`b`$, $`\beta `$ and $`T`$. By inequalities (3.4;3.6), we see that solutions to the Cauchy problem (3.3;2.1) are uniformly bounded for $`\delta 0`$ in

$$L^{\mathrm{}}([0,T];L^2(R^2))L^2([0,T];H_1(R^2)).$$

The difficult part is to prove the solutions are uniformly bounded in

$$L^{\mathrm{}}([0,T];H_1(R^2))L^2([0,T];H_2(R^2)).$$

Differentiating (3.3), we get

$`\left[/t+u^{(\delta )}\kappa \mathrm{\Delta }\right]\theta _x`$ $`=`$ $`\{\theta ,u_2^{(\delta )}\},`$ (3.7)
$`\left[/t+u^{(\delta )}\kappa \mathrm{\Delta }\right]\theta _y`$ $`=`$ $`\{\theta ,u_1^{(\delta )}\},`$ (3.8)
$`\left[/t+u^{(\delta )}\nu \mathrm{\Delta }\right]\omega `$ $`=`$ $`\theta _x+\{u_1,v_1^{(\delta )}\}+\{u_2,v_2^{(\delta )}\}.`$ (3.9)
Here, $`\omega =u_1/yu_2/x`$, $`\theta _x=\theta /x`$, $`v^{(\delta )}=uu^{(\delta )}`$, and

$$\{p,q\}=\frac{p}{x}\frac{q}{y}\frac{p}{y}\frac{q}{x}.$$

From (3.7;3.8;3.9), we have:

$`{\displaystyle \frac{d}{dt}}{\displaystyle \theta _x^2}+2\kappa {\displaystyle |\theta _x|^2}`$ $`=`$ $`2{\displaystyle \theta _x\{\theta ,u_2^{(\delta )}\}},`$ (3.10)
$`{\displaystyle \frac{d}{dt}}{\displaystyle \theta _y^2}+2\kappa {\displaystyle |\theta _y|^2}`$ $`=`$ $`2{\displaystyle \theta _y\{\theta ,u_1^{(\delta )}\}},`$ (3.11)
$`{\displaystyle \frac{d}{dt}}{\displaystyle \omega ^2}+2\nu {\displaystyle |\omega |^2}`$ $`=`$ $`2{\displaystyle }\theta _x\omega +2{\displaystyle }\omega [\{u_1,v_1^{(\delta )}\}`$
$`+`$ $`\{u_2,v_2^{(\delta )}\}].`$
The key for the proof below is that we can estimate (3) first, using the inequality (3.4). Then, we estimate (3.10; 3.11), using the estimates to be obtained for (3). Notice some simple facts:

$`{\displaystyle \omega ^2}={\displaystyle |u|^2},`$ (3.13)
$`{\displaystyle |\omega |^2}={\displaystyle |u|^2},`$ (3.14)
$`{\displaystyle |v^{(\delta )}|^2}A_1\delta ^2{\displaystyle \omega ^2},`$ (3.15)
$`{\displaystyle |v^{(\delta )}|^2}A_2{\displaystyle \omega ^2},`$ (3.16)
where $`A_1,A_2`$ are constants. Next, we estimate (3). By integration by part, we have

$$\omega \{u_1,v_1^{(\delta )}\}=v_1^{(\delta )}\{\omega ,u_1\},\omega \{u_2,v_2^{(\delta )}\}=v_2^{(\delta )}\{\omega ,u_2\}.$$

Then, by Schwarz inequality, we get

$$2\left|\omega [\{u_1,v_1^{(\delta )}\}+\{u_2,v_2^{(\delta )}\}]\right|4\left\{ϵ|\omega |^2+ϵ^1|v^{(\delta )}|^2|u|^2\right\},$$
(3.17)
where $`ϵ`$ is a small constant to be chosen later on. Moreover,

$$|v^{(\delta )}|^2|u|^2\left[|v^{(\delta )}|^4\right]^{1/2}\left[|u|^4\right]^{1/2}.$$
(3.18)
By the Gagliardo-Nirenberg inequality:

$$\left[|v^{(\delta )}|^4\right]^{1/2}C_1\left[|v^{(\delta )}|^2\right]^{1/2}\left[|v^{(\delta )}|^2\right]^{1/2},$$

and identities (3.15;3.16), we get

$$\left[|v^{(\delta )}|^4\right]^{1/2}C_2\delta \omega ^2.$$
(3.19)
From now on, $`C_j`$ $`(j=1,2,\mathrm{})`$ are all constants. By the same Gagliardo-Nirenberg inequality and identities (3.13;3.14), we get

$$\left[|u|^4\right]^{1/2}C_3\left[|\omega |^2\right]^{1/2}\left[\omega ^2\right]^{1/2}.$$
(3.20)
From (3.18;3.19;3.20) and an algebraic inequality, we get

$$4ϵ^1|v^{(\delta )}|^2|u|^2C_4\left\{ϵ|\omega |^2+ϵ^3\delta ^2\left[\omega ^2\right]^3\right\}.$$
(3.21)
Thus, by (3.17;3.21), we have

$$2\left|\omega [\{u_1,v_1^{(\delta )}\}+\{u_2,v_2^{(\delta )}\}]\right|(4+C_4)ϵ|\omega |^2+C_4ϵ^3\delta ^2\left[\omega ^2\right]^3.$$
(3.22)
Finally, we have the estimate for (3):

$`{\displaystyle \frac{d}{dt}}{\displaystyle \omega ^2}+2\nu {\displaystyle |\omega |^2}`$ $``$ $`2\left[{\displaystyle \theta _x^2}\right]^{1/2}\left[{\displaystyle \omega ^2}\right]^{1/2}`$
$`+`$ $`(4+C_4)ϵ{\displaystyle |\omega |^2}+C_4ϵ^3\delta ^2\left[{\displaystyle \omega ^2}\right]^3.`$
Choose

$$ϵ=\frac{\nu }{4+C_4},$$

we get

$$\frac{d}{dt}\omega ^2+\nu |\omega |^22\left[\theta _x^2\right]^{1/2}\left[\omega ^2\right]^{1/2}+C_5\nu ^3\delta ^2\left[\omega ^2\right]^3.$$
(3.24)
Notice that the term

$$\left[\theta _x^2\right]^{1/2}$$

in (3.24) is integrable in time by virtue of (3.4). Solving the above inequality for $`\omega ^2`$, and choose $`\delta `$ such that

$$C_5\nu ^3\delta ^2\left\{2\left[\omega ^2(0)\right]^{1/2}+2_0^T\left[\theta _x^2\right]^{1/2}\right\}^4T1,$$

we get

$$\omega ^2(T)4\left\{\left[\omega ^2(0)\right]^{1/2}+\left(\frac{1}{2}T\kappa ^1\theta ^2(0)\right)^{1/2}\right\}^2.$$
(3.25)
By virtue of (3.25), we have from (3.24) that

$$_0^T|\omega |^2\mathrm{\Gamma }_2,$$
(3.26)
where $`\mathrm{\Gamma }_2`$ is a constant depending only on $`b`$, $`b`$, $`\beta `$, and $`T`$. By (3.25;3.26), we see that $`u`$ is uniformly bounded for $`\delta 0`$ in

$$L^{\mathrm{}}([0,T];H_1(R^2))L^2([0,T];H_2(R^2)).$$

Next we go back to estimate (3.10;3.11). By Schwarz inequality, we have

$$\frac{d}{dt}|\theta |^2+2\kappa |\theta |^28\left[|\theta |^4\right]^{1/2}\left[|u^{(\delta )}|^2\right]^{1/2}.$$
(3.27)
Notice that

$$|u^{(\delta )}|^2C_6|u|^2;$$

then (3.25) implies that

$$\left[|u^{(\delta )}|^2\right]^{1/2}D,$$
(3.28)
where $`D`$ is a constant depending on $`T`$. By the Gagliardo-Nirenberg inequality:

$$\left[|\theta |^4\right]^{1/2}C_7\left[|\theta |^2\right]^{1/2}\left[|\theta |^2\right]^{1/2},$$

we get

$$\frac{d}{dt}|\theta |^2+2\kappa |\theta |^28DC_8\left[ϵ_1|\theta |^2+ϵ_1^1|\theta |^2\right].$$

Choose

$$8DC_8ϵ_1=\kappa ,$$

we get

$$\frac{d}{dt}|\theta |^2+\kappa |\theta |^2D_1\kappa ^1|\theta |^2,$$
(3.29)
where $`D_1`$ is a constant depending on $`T`$. Then, we have

$$|\theta (T)|^2D_2|\beta |^2,_0^T|\theta |^2\mathrm{\Gamma }_3;$$

where $`D_2`$ and $`\mathrm{\Gamma }_3`$ are constants depending on initial data and $`T`$ only. Thus $`\theta `$ is also uniformly bounded for $`\delta 0`$ in

$$L^{\mathrm{}}([0,T];H_1(R^2))L^2([0,T];H_2(R^2)).$$

For this sequence of solutions parametrized by $`\delta `$, there exists a subsequence which converges to a solution to the original Cauchy problem (1.4;2.1); moreover, it inherits the bounds, hence it is a strong solution. Since strong solutions are actually smooth and unique, the theorem is proved. $`\mathrm{}`$

Next, we prove the corollary. Notice that the estimate for $`\omega ^2(T)`$ in (3.25) is independent of $`\nu `$; thus, we can take the limit $`\nu 0`$ to get solution to the Cauchy problem (1.4;2.1) for $`\kappa >0`$, $`\nu =0`$

$$uL^{\mathrm{}}([0,T];H_1(R^2)).$$

All the estimates for $`\theta `$ are still true. This completes the proof of the corollary. $`\mathrm{}`$

## 4 Conclusion

The global regularity for the viscous Boussinesq equations is proved, by following the approach in .