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# Lithium-6 from Solar Flares

## 1 Introduction

The solar wind lithium isotopic ratio, (6Li/7Li)sw =0.032$`\pm `$0.004, has recently been determined from measurements in lunar soil (Chaussidon & Robert 1999). As these authors point out, this value greatly exceeds the expected photospheric ratio, based on the fact that 7Li in the photosphere is depleted by over a factor of 100 relative to its protosolar value (i.e. the photospheric vs. the meteoritic abundance, Grevesse, Noels, & Sauval 1996), and that this depletion, due to burning at the bottom of the convection zone (Brun, Turck-Chieze, & Zahn 1999), should lead to a much more severe depletion of 6Li, which burns at a lower temperature than 7Li. In addition, there exist observational upper limits on the photospheric ratio, (6Li/7Li)ph$``$0.01 (Müller, Peytremann, & de la Reza 1975) and (6Li/7Li)ph$``$0.03 (Ritzenhoff, Schröter, & Schmidt 1997). Chaussidon & Robert (1999) thus suggest that the measured solar wind 6Li must be solar flare produced. However, they only consider 6Li production by spallation from C, N and O. The demonstration that solar flares can indeed account for the 6Li in the solar wind has very important implications on many problems in solar physics.

Light element production by accelerated particle interactions was treated in detail (e.g. Ramaty et al. 1997). In non-solar settings, and for accelerated particles of predominantly low energy, the dominant reactions are 4He($`\alpha `$,p)7Li, 4He($`\alpha `$,n)7Be (with 7Be decaying to 7Li) and 4He($`\alpha `$,x)6Li (where x stands for either a proton and a neutron, or a deuteron). In solar flares, however, the reaction 4He(3He,p)6Li is also very important (Mandzhavidze, Ramaty, & Kozlovsky 1997a), both because of its very low threshold energy and because for solar energetic particles 3He/4He can be as large as 1 or even larger (e.g. Reames 1998). Such 3He/4He enhancements are one of the main characteristics of the acceleration mechanism responsible for impulsive solar energetic particle events, as distinguished from gradual events, based on the duration of the accompanying soft X-ray emission. The 3He enrichment is thought to be due to stochastic acceleration through gyroresonant wave particle interactions which preferentially accelerate the 3He (Temerin & Roth 1992; Miller & Viñas 1993). Concerning the particles which interact at the Sun, evidence for accelerated 3He enrichment was obtained from the detection (Share & Murphy 1998) of a gamma-ray line at 0.937 MeV produced by the reaction 16O(3He,p)18F (Mandzhavidze, Ramaty, & Kozlovsky 1997b; 1999). Using gamma-ray data from 20 flares, Mandzhavidze et al. (1999) showed that for essentially all of these flares 3He/4He can be as large as 0.1, while for some of them values as high as 1 are possible. In addition, they showed that for the particles that interact and produce gamma rays, 3He enrichments are present for both impulsive and gradual flares. Thus, we can expect 3He/4He$`\stackrel{>}{}`$0.1 for most flares that produce gamma rays and isotopes at the Sun.

In the present Letter we carry out new calculations of Li production and re-calculate (see Ramaty & Simnett 1991) the average accelerated ion irradiation of the Sun, to show that flare accelerated particle interactions produce enough 6Li which, combined with photospheric 7Li, can account for the solar wind 6Li/7Li measured in lunar soil.

## 2 Li Production

We employ the nuclear code described in detail in Ramaty et al. (1997) which includes, in addition to the $`\alpha `$$`\alpha `$ reactions mentioned above, also Li production from C, N and O. The cross section for the additional reaction, 4He(3He,p)6Li, is shown in Figure 1, together with the cross sections for the $`\alpha `$$`\alpha `$ reactions producing 6Li and 7Li. For the 3He induced reaction we obtained the cross section for 6Li production in the ground state, from threshold (2.34 MeV/nucleon) to 8.2 MeV/nucleon, by detailed balance using the cross section for the inverse exothermic reaction 6Li(p,3He)4He (Angulo et al. 1999). We added the contribution of the reaction for producing 6Li in the 3.56 MeV excited state which decays to the ground state by photon emission, using data from Harrison (1967). The total cross section at 9.3 MeV/nucleon is from Koepke and Brown (1977), and at 18 and 20.4 MeV/nucleon from Halbert, van der Woude, & O’Fallon (1973). At higher energies we extrapolated the cross section as expected for reactions with 2 particles in the exit channel.

Gamma-ray production in solar flares results predominantly from thick target interactions, meaning that particles accelerated in the upper portions of coronal loops produce nuclear reactions as they slow down in the denser chromospheric region of the loops (e.g. Ramaty & Murphy 1987). We adopt the same model for Li production. The upper panel in Figure 2 shows the resultant thick target 6Li yields, normalized to unit incident total number of protons of energy greater than 30 MeV, $`N_\mathrm{p}(>`$30)=1. The energy spectra of the accelerated particles are power laws in kinetic energy per nucleon, with spectral index $`s`$ (Ramaty, Mandzhavidze, & Kozlovsky 1996). The evidence for enhanced 3He/4He was mentioned above. There is also evidence that $`\alpha `$/p could exceed the canonical 0.1, with possible value around 0.5 (Share & Murphy 1997; Mandzhavidze et al. 1999). Thus in Figure 2 we show results for $`\alpha `$/p = 0.1 and 0.5, and 3He/4He=0, 0.1 and 1. We see in the upper panel that the 3He enrichment very significantly increases the lithium production, especially for steep spectra. That the lithium production is mainly due to $`\alpha `$ particles and 3He nuclei can be seen by comparing the six upper curves with the lowest one, for which we set the $`\alpha `$ particle and 3He abundances to zero, so that all the 6Li in this case is produced in C, N and O interactions. Considering the flare produced isotopic ratios in the lower panel, we see that while in the absence of 3He, 6Li/7Li is at most unity, much larger ratios are possible with enhanced 3He/4He.

## 3 Average Solar Proton Irradiation

To calculate the average flare produced lithium, we estimate the average proton irradiation of the Sun, $`\dot{N}_\mathrm{p}`$($`>`$30MeV) measured in protons per second, where the average is taken over a solar cycle. We follow the method described by Ramaty & Simnett (1991). We start with the flare size distribution measured in 0.3 to 1 MeV bremsstrahlung because observations in this energy range give the most complete sample of solar flare gamma-ray emission (see Vestrand et al. 1999). To minimize the effects of anisotropic electrons (e.g. Miller & Ramaty 1989) we employ the distribution derived for flares near the solar limb (Dermer 1987). For flares at heliocentric longitudes 60 to 90, observed from March 1980 to February 1986 (approximately half a solar cycle) the size distribution, measured in number of flares per unit $`F_\mathrm{B}`$, can be approximated by $`dn/dF_\mathrm{B}8.5F_\mathrm{B}^{1.1}`$, where 10$`\stackrel{<}{}F_\mathrm{B}\stackrel{<}{}`$6500 photons cm-2 is the observed 0.3 to 1 MeV bremsstrahlung fluence at Earth per flare . The total number of $`>`$0.3 MeV emitting flares per solar cycle is obtained by integrating the above expression multiplied by a factor of 12, where a factor of 6 takes into account the whole solar surface and a factor of 2 the other half of solar cycle. We thus obtain 375 flares, which compares well with the 175 flares listed by Vestrand et al. (1999) from which $`>`$0.3 MeV bremsstrahlung was observed with the Solar Maximum Mission (SMM) over almost a whole solar cycle. This latter number should be corrected for anisotropy effects, and must be multiplied by a factor of 2 since SMM only observes half the solar surface. The required average irradiation is then given by

$`\dot{N}_\mathrm{p}(>30)={\displaystyle \frac{12}{T}}{\displaystyle _{10}^{6500}}𝑑F_\mathrm{B}{\displaystyle \frac{dn}{dF_\mathrm{B}}}N_\mathrm{p}(F_\mathrm{B}),`$ (1)
where T is the number of seconds in 11 years and $`N_\mathrm{p}(F_\mathrm{B})`$ is the number of protons above 30 MeV expressed as a function of $`F_\mathrm{B}`$. To derive this relationship, we first employ the result of Murphy et al. (1990) that for flares near the limb $`F_\mathrm{B}/F_\mathrm{N}4.5`$, where $`F_\mathrm{N}`$ is the total nuclear deexcitation line emission fluence observed at Earth. Next we use the nuclear deexcitation code (e.g. Ramaty et al. 1996) to derive $`N_\mathrm{P}(>`$30)/$`F_\mathrm{N}`$. This ratio depends on the spectrum and composition of the accelerated particles, in particular $`\alpha `$/p. Ramaty et al. (1996) have derived the distribution of power law spectral indexes from gamma-ray data, showing that for a sample of 19 flares the mean $`s4`$. For this value of $`s`$ we find that $`N_\mathrm{p}(>`$30)/$`F_\mathrm{N}`$ = 1.7$`\times `$1029 and 6.6$`\times `$1029 protons/(nuclear deexcitation photons cm-2), for $`\alpha `$/p=0.5 and 0.1, respectively. By using $`F_\mathrm{B}/F_\mathrm{N}`$=4.5 and these $`N_\mathrm{p}(>`$30)/$`F_\mathrm{N}`$ to derive $`N_\mathrm{p}(F_\mathrm{B})`$, equation 1 yields $`\dot{N}_\mathrm{p}`$($`>`$30MeV)=3.5$`\times `$1025 and 1.4$`\times `$1026 protons s-1, for $`\alpha `$/p=0.5 and 0.1, respectively.

## 4 The Solar Wind 6Li/7Li

Even though a detailed treatment of the time dependent evolution of Li in the solar atmosphere is beyond the scope of this paper, we now show that 6Li production in solar flares could indeed account for the solar wind 6Li/7Li. To demonstrate this we assume the following: (i) all the flare produced 6Li is evacuated by the solar wind, (ii) the photospheric 6Li that is the remnant of its protosolar abundance is negligible, and (iii) the solar wind (7Li/H)sw is equal to the photospheric value (7Li/H)ph=1.4$`\times `$10-11 (Grevesse et al. 1996). The solar wind (6Li/7Li)sw is then given by

$`\left({\displaystyle \frac{{}_{}{}^{6}\mathrm{Li}}{{}_{}{}^{7}\mathrm{Li}}}\right)_{\mathrm{sw}}={\displaystyle \frac{\dot{N}_\mathrm{p}(>30)Q(^6\mathrm{Li})/\dot{F}_{\mathrm{sw}}}{(^7\mathrm{Li}/\mathrm{H})_{\mathrm{ph}}}},`$ (2)
where $`Q(^6\mathrm{Li})`$ is plotted in Figure 2 and $`\dot{F}_{\mathrm{sw}}`$$``$6$`\times `$1035 s-1 is the average solar wind proton flux (Dupree 1996). Taking $`s=4`$, 0.1$`<`$$`\alpha `$/p$`<`$0.5 and 0.1$`<`$3He/4He$`<`$1, we obtain 0.007$`<`$(6Li/7Li)sw$`<`$0.06. This range is consistent with the observed value of 0.032$`\pm `$0.004. Several effects could lead to lower or higher calculated (6Li/7Li)sw. Clearly there are uncertainties in our estimate of $`\dot{N}_\mathrm{p}(>`$30 MeV), in particular there could be a large number of smaller gamma-ray flares, which have not yet been observed, and if they had steep ion energy spectra and high 3He/4He they would contribute significantly to 6Li production. On the other hand, some of the flare-produced 6Li could be mixed downward to the photosphere and lost from the solar wind. The calculated (6Li/7Li)sw would also be lower if (7Li/H)sw were higher than (7Li/H)ph, a possibility since Li has low first ionization potential, a factor that biases coronal abundances relative to those of the photosphere (e.g. Reames 1998). Nevertheless, the better than order of magnitude agreement between the calculated and measured (6Li/7Li)sw provides good support to the possibility that the measured 6Li in lunar soil is indeed solar flare produced.

It is of some interest to compare the average 6Li production, 6$`\times `$1022$`<`$\[$`\dot{N}_\mathrm{p}`$$`(>`$30)$`Q(^6`$Li)\] $`<`$5$`\times `$1023 atoms s-1, with the contribution of the 19 large SMM flares from which gamma-ray line emission was observed. Using the method detailed in Mandzhavidze et al. (1999), for each flare we derive $`s`$ and $`N_\mathrm{p}`$($`>`$30). Then using $`Q`$(6Li) from Figure 2, taking into account that for 5 of the 19 flares $`\alpha `$/p$``$0.5 (Mandzhavidze et al. 1999), we obtain the flare-by-flare 6Li productions which yield averages over the 9 year SMM observing period of 1$`\times `$1022 and 7$`\times `$1022 6Li atoms s-1, if for all flares 3He/4He=0.1 and 1, respectively. Thus, about 15% of the 6Li production that we derived using the flare size distribution could result from 19 of the largest flares. Concerning the contributions of individual flares, as much as a few times 1030 Li atoms could be produced by a large flare and most of these would be 6Li (Mandzhavidze et al. 1997a)

## 5 Discussion and Conclusions

We demonstrated that it is possible to produce enough 6Li by flare accelerated particles to account for the measured 6Li/7Li in lunar soil that is thought to originate from solar wind implantation. The presence of enriched accelerated particle 3He is essential for the production of sufficient 6Li. We note that the radioactive 26Al in the early solar system is thought to be produced in 3He induced reactions (Lee et al. 1998). This raises the possibility that some of the meteoritic 6Li could also be of local early solar system origin.

Kotov et al. (1996) claimed that flare accelerated particle interactions could account for all the photospheric lithium. If this were true, since the solar wind acceleration is not expected to significantly alter the lithium isotopic ratio, the solar wind 6Li/7Li should exceed 0.2 (Figure 2), contrary to the observed value of 0.03. This confirms the previous result of Mandzhavidze et al. (1997a) that production in flares does not make a significant contribution to the average photospheric lithium. But the fact that as much as 1030 Li atoms are produced in large solar flares, suggests that flare produced lithium may be detected in a small area of the solar surface near the foot points of the flaring loops shortly after the time of the flare (see Livshits 1997). In this connection, it is interesting to point out that Ritzenhoff et al. (1997) don’t rule out the presence of 6Li near a sunspot at a value close to their reported upper limit 6Li/7Li$``$0.03, which in fact coincides with the measured solar wind value.

Further research in this area requires direct measurement of lithium and its isotopic ratio in the solar wind, spectroscopic measurements of 6Li in the photosphere, and the detection of gamma rays from small flares that would lead to a more precise determination of the proton irradiation of the Sun. All of these should lead to new insights into the processes of transport and mixing in the solar atmosphere and of the acceleration of the solar wind.


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# Gröbner Basis Techniques for Computing Actions of K-Categories KEYWORDS: Gröbner basis, K-category, Action, Kan extension.

## 1 Introduction

The paper is motivated by a question which arises from two pieces of research. Firstly, the work of Brown and Heyworth  which extends rewriting techniques to enable the computation of left Kan extensions over the category of sets. It is well known that left Kan extensions can be defined over categories other than $`\mathrm{𝖲𝖾𝗍𝗌}`$. Secondly, the ‘folklore’, made explicit in  that rewriting theory is a special case of noncommutative Gröbner basis theory. It is therefore natural to ask whether Gröbner bases can provide a method for computing Kan extensions beyond the special case of rewriting.

To answer this question completely, fully exploiting the computational power of Gröbner basis techniques relating to Kan extensions is the ultimate aim. This paper provides a first step by showing how standard noncommutative Gröbner basis procedures can be used to calculate left Kan extensions of $`K`$-category actions. In the final section of the paper a number of interesting problems arising from the work are identified.

## 2 Background

This paper builds on work of Brown and Heyworth  on extensions of rewriting methods.

The standard expression of rewriting is in terms of words $`w`$ in a free monoid $`\mathrm{\Delta }^{}`$ on a set $`\mathrm{\Delta }`$. This may be extended to terms $`x|w`$ where $`x`$ belongs to a set $`X`$ and the link between $`x`$ and $`w`$ is in terms of an action. More precisely, we suppose a monoid $`A`$ acts on the set $`X`$ on the right, and there is given a morphism of monoids $`F`$: $`AB`$ where $`B`$ is given by a presentation with generating set $`\mathrm{\Delta }`$. The result of the rewriting will then be normal forms for the induced action of $`B`$ on $`F_{}(X)`$. This gives an important extension of rewrite methods.

In fact monoids may be replaced by categories, and sets by directed graphs. This gives a formulation in terms of left Kan extensions, or induced actions of categories, which is explained in . Further, categories can be replaced by $`K`$-categories, as will be described later.

Let $`𝖠`$ be a category. A category action $`X`$ of $`𝖠`$ is a functor $`X:𝖠\mathrm{𝖲𝖾𝗍𝗌}`$. Let $`𝖡`$ be a second category and let $`F:𝖠𝖡`$ be a functor. Then an extension of the action $`X`$ along $`F`$ is a pair $`(E,\epsilon )`$ where $`E:𝖡\mathrm{𝖲𝖾𝗍𝗌}`$ is a functor and $`\epsilon :XEF`$ is a natural transformation. The left Kan extension of the action $`X`$ along $`F`$ is an extension of the action $`(E,\epsilon )`$ with the universal property that for any other extension of the action $`(E^{},\epsilon ^{})`$ there exists a unique natural transformation $`\alpha :EE^{}`$ such that $`\epsilon ^{}=\alpha \epsilon `$.

The problem that has been introduced is that of “computing a Kan extension”. In order to keep the analogy with computation and rewriting for presentations of monoids we propose a definition of a presentation of a left Kan extension. The papers  were very influential on our choices.

A left Kan extension data $`(X^{},F^{})`$ consists of small categories $`𝖠`$, $`𝖡`$ and functors $`X^{}:𝖠\mathrm{𝖲𝖾𝗍𝗌}`$ and $`F^{}:𝖠𝖡`$. A left Kan extension presentation is a quintuple $`𝒫:=kan\mathrm{\Gamma }|\mathrm{\Delta }|RelB|X|F`$ where $`\mathrm{\Gamma }`$ and $`\mathrm{\Delta }`$ are (directed) graphs; $`X:\mathrm{\Gamma }\mathrm{𝖲𝖾𝗍𝗌}`$ and $`F:\mathrm{\Gamma }P\mathrm{\Delta }`$ are graph morphisms to the category of sets and the free category on $`\mathrm{\Delta }`$ respectively; and $`RelB`$ is a set of relations on the free category $`P\mathrm{\Delta }`$.

Formally, we say $`𝒫`$ presents the left Kan extension $`(E,\epsilon )`$ of the left Kan extension data $`(X^{},F^{})`$ where $`X^{}:𝖠\mathrm{𝖲𝖾𝗍𝗌}`$ and $`F^{}:𝖠𝖡`$ if $`\mathrm{\Gamma }`$ is a generating graph for $`𝖠`$ and $`X:\mathrm{\Gamma }\mathrm{𝖲𝖾𝗍𝗌}`$ is the restriction of $`X^{}:𝖠\mathrm{𝖲𝖾𝗍𝗌}`$; $`cat\mathrm{\Delta }|RelB`$ is a category presentation for $`𝖡`$ and $`F:\mathrm{\Gamma }P\mathrm{\Delta }`$ induces $`F^{}:𝖠𝖡`$.

We expect that a left Kan extension $`(E,\epsilon )`$ is given by a set $`EB`$ for each $`B\mathrm{Ob}\mathrm{\Delta }`$ and a function $`Eb:EB_1EB_2`$ for each $`b:B_1B_2𝖡`$ (defining the functor $`E`$) together with a function $`\epsilon _A:XAEFA`$ for each $`A\mathrm{Ob}𝖠`$ (the natural transformation).

The main result of  defines rewriting procedures on $`T:=_{B\mathrm{Ob}\mathrm{\Delta }}_{A\mathrm{Ob}\mathrm{\Gamma }}XA\times P\mathrm{\Delta }(FA,B)`$ which is basically a set with a partial right action of the arrows of $`P\mathrm{\Delta }`$.

Two kinds of rewriting are involved here. The first is the familiar $`x|ulvx|urv`$ given by a relation $`(l,r)`$ – these rules are known as the ‘$`E`$-rules’. The second derives from a given action of certain words on elements, so allowing rewriting $`x|F(a)vxa|v`$ – these rules are known as the ‘$`\epsilon `$-rules’. Further, the elements $`x`$ and $`xa`$ may belong to different sets. When such rewriting procedures complete, the associated normal form gives in effect a computation of what we call the Kan extension defined by the presentation.

The ‘folklore’ of the relation of rewriting and Gröbner basis techniques, alluded to in  and  is made explicit in .

The polynomial ring $`K[X^{}]`$ consists of all polynomials having coefficients in the field $`K`$ and terms from $`X^{}`$ together with the usual operations of polynomial addition and (noncommutative) multiplication. Given a generating set for an ideal $`I`$ in this ring it is a problem to determine whether two given polynomials $`f`$ and $`g`$ are equivalent modulo the ideal i.e. whether they occur within the same congruence class. If a Gröbner basis $`G`$ can be constructed for $`I`$ from the original generating set then the congruence problem can be solved. The Gröbner basis calculation depends on a well-ordering of $`X^{}`$ and a definition of polynomial reduction, which is determined by comparing leading terms. In the noncommutative case it is not always successful.

The key observation is that the rewriting techniques used in calculating a monoid $`M`$ from a set of generators $`X`$ and a rewrite system $`R`$ compatible with an ordering $`>`$ corresponds step-by-step to the Gröbner basis techniques used in calculating the congruence classes of the polynomial ring $`K[X^{}]`$ with respect to the ideal generated by the difference binomials $`lr`$ for $`(l,r)`$ in $`R`$.

This provides the background to our problem of determining whether Gröbner bases can be used to calculate Kan extensions other than in the special case of rewriting systems. The first observation is that Gröbner bases involve polynomials, so we should examine how the addition operation is represented in categories.

## 3 $`K`$-Category Actions

We use the definitions of . Let $`K`$ be a field. A $`K`$-category is a category whose hom-sets (a hom-set is the set of all morphisms between a given pair of objects) are $`K`$-modules. A morphism of $`K`$-categories or $`K`$-functor $`F`$ preserves the $`K`$-module structure of the hom-sets so $`F(a+b)=F(a)+F(b),F(ka)=kF(a)`$ for all arrows $`a,b`$ such that $`a+b`$ is defined and scalars $`k`$ in $`K`$.

The free $`K`$-category on the graph $`\mathrm{\Delta }`$ is the category $`P_K\mathrm{\Delta }`$ whose objects are the objects of $`\mathrm{\Delta }`$ and whose arrows $`\mathrm{Arr}P_K\mathrm{\Delta }`$ are all polynomials of the form $`p=k_1m_1+\mathrm{}+k_nm_n`$ where $`k_1,\mathrm{},k_nK`$ and $`m_1,\mathrm{},m_nP\mathrm{\Delta }(B_1,B_2)`$ for some $`B_1,B_2\mathrm{Ob}\mathrm{\Delta }`$. We will refer to $`m_1,\mathrm{},m_n`$ as the terms which occur in $`f`$. Note that functions $`src`$ and $`tgt`$ are well-defined as $`src(f):=src(m_1)=\mathrm{}=src(m_n)`$ and $`tgt(f):=tgt(m_1)=\mathrm{}=tgt(m_n)`$.

The relations of a $`K`$-category can be of the form $`p=q`$ where both sides have the same source and target. Therefore $`R`$ will be assumed to be a set of polynomials $`pq`$ i.e. a subset of $`\mathrm{Arr}P_K\mathrm{\Delta }`$. If $`R=\{r_1,\mathrm{},r_n\}`$ is such a set of relations on $`P_K\mathrm{\Delta }`$ then the congruence generated by $`R`$ is defined as follows:

$$f=_Rh\text{ if and only if }f=h+k_1p_1r_1q_1+\mathrm{}+k_np_nr_nq_n$$

for some $`k_1,\mathrm{},k_nK`$ and $`p_1,\mathrm{},p_n,q_1,\mathrm{},q_n\mathrm{Arr}P_K\mathrm{\Delta }`$ where $`src(f)=src(h)=src(u_1)=\mathrm{}=src(u_n)`$ and $`tgt(f)=tgt(h)=tgt(v_1)=\mathrm{}=tgt(v_n)`$ and $`u_1r_1v_1,\mathrm{},u_nr_nv_n`$ are defined in $`\mathrm{Arr}P_K\mathrm{\Delta }`$. The $`K`$-category $`P_K\mathrm{\Delta }/=_R`$ whose elements are the congruence classes of $`\mathrm{Arr}P_K\mathrm{\Delta }`$ with respect to $`F`$ is known as the factor $`K`$-category.

###### Definition 3.1

Let $`K`$ be a field. A $`K`$-category presentation is a pair $`cat_K\mathrm{\Delta }|R`$ where $`\mathrm{\Delta }`$ is a graph and $`R\mathrm{Arr}P_K\mathrm{\Delta }`$. The $`K`$-category it presents is the factor category $`P_K\mathrm{\Delta }/=_R`$.

Our first result enables the use of Buchberger’s algorithm to compute Gröbner bases which enable the specification of the morphisms of a $`K`$-category presented in this way.

Let $`>`$ be an admissible well-ordering on $`\mathrm{Arr}P\mathrm{\Delta }`$ i.e. $`>`$ is Noetherian and compatible with the operation of path concatenation. Define the leading term of a polynomial $`f`$ to be the term occurring in $`f`$ which is the greatest path in $`\mathrm{\Delta }`$ with respect to $`>`$ and denote it $`\mathrm{𝙻𝚃}(f)`$. Define a reduction relation $`_R`$ on $`\mathrm{Arr}P_K\mathrm{\Delta }`$ by $`ffk_iu_ir_iv_i`$ when $`u_i(\mathrm{𝙻𝚃}(r_i))v_i`$ occurs in $`f`$ with coefficient $`k_iK`$ for $`u_i,v_i\mathrm{Arr}P\mathrm{\Delta }`$, $`r_iR`$. The reflexive, symmetric and transitive closure of $`_R`$ is denoted $`\underset{R}{\overset{}{}}`$. If the reduction relation $`_R`$ is complete (i.e. Noetherian and confluent) then we say that $`R`$ is a Gröbner basis.

###### Lemma 3.2

$$\frac{\mathrm{Arr}P_K\mathrm{\Delta }}{=_R}\frac{\mathrm{Arr}P_K\mathrm{\Delta }}{\underset{R}{\overset{}{}}}$$

Proof It is clear from the definitions that the equivalence relation $`\underset{R}{\overset{}{}}`$ is contained in $`=_R`$.

For the converse, suppose $`f=_Rh`$. Then there exist $`r_1,\mathrm{},r_nR`$ and $`p_1,\mathrm{},p_n,q_1,\mathrm{},q_nP_K\mathrm{\Delta }`$, such that $`f=h+p_1r_1q_1+\mathrm{}+p_nr_nq_n`$. By splitting $`p_i`$ and $`q_i`$ into their component terms for $`i=1,\mathrm{},n`$ we obtain $`f=h+k_1u_1r_1v_1+\mathrm{}+k_ju_jr_iv_j+\mathrm{}+k_tu_tr_nv_t`$ for some $`k_1,\mathrm{},k_tK`$, $`u_1,\mathrm{},u_t,v_1,\mathrm{},v_tP\mathrm{\Delta }`$. It follows immediately from this that $`f\underset{R}{\overset{}{}}h`$.  $`\mathrm{}`$

###### Proposition 3.3

The relation $`_R`$ is Noetherian on $`\mathrm{Arr}P_K\mathrm{\Delta }`$.

The matches of $`R`$ are the pairs of polynomials $`(r_1,r_2)`$ whose leading terms overlap on some subword i.e. $`u\mathrm{𝙻𝚃}(r_1)v=\mathrm{𝙻𝚃}(r_2)`$ or $`\mathrm{𝙻𝚃}(r_2)=u\mathrm{𝙻𝚃}(r_2)v`$ or $`u\mathrm{𝙻𝚃}(r_1)=\mathrm{𝙻𝚃}(r_2)v`$ or $`\mathrm{𝙻𝚃}(r_1)v=u\mathrm{𝙻𝚃}(r_2)`$ for some $`u,v\mathrm{Arr}P\mathrm{\Delta }`$. If there is a match between $`r_1`$ and $`r_2`$ we may write $`u_1\mathrm{𝙻𝚃}(r_1)v_1=u_2\mathrm{𝙻𝚃}(r_2)v_2`$ for some $`u,v\mathrm{Arr}P\mathrm{\Delta }`$. The S-polynomial resulting from a match is then the difference $`u_1r_1v_1u_2r_2v_2`$. The set of S-polynomials of a finite set of polynomials is finite and can be computed.

###### Lemma 3.4

If all S-polynomials resulting from matches of $`R`$ reduce to zero by $`_R`$ then $`_R`$ is confluent on $`\mathrm{Arr}P_K\mathrm{\Delta }`$.

Outline Proof Observing that $`\mathrm{Arr}P_K\mathrm{\Delta }`$ is a subset of the free $`K`$-algebra on $`(\mathrm{Arr}P\mathrm{\Delta })^{}`$ we can deduce that the relation $`_R`$ is confluent on the free $`K`$-algebra. The fact that $`_R`$ preserves source and target enables us to deduce that $`_R`$ cannot reduce an element of $`\mathrm{Arr}P_K\mathrm{\Delta }`$ to anything not defined in $`\mathrm{Arr}P_K\mathrm{\Delta }`$. Thus $`_R`$ is confluent on $`\mathrm{Arr}P_K\mathrm{\Delta }`$.  $`\mathrm{}`$

Buchberger’s algorithm calculates the S-polynomials of a system $`R`$ and attempts to reduce them to zero by $`_R`$. If an S-polynomial cannot be reduced it is added to the system. The S-polynomials of the modified system $`R^{}`$ are then computed – the process looping until a system is found whose S-polynomials can all be reduced to zero.

###### Theorem 3.5 (Buchberger’s Algorithm and $`K`$-category Presentations)

If it terminates, then Buchberger’s algorithm applied to $`(R,>)`$, will return a Gröbner basis for $`=_R`$ on $`\mathrm{Arr}P_K\mathrm{\Delta }`$.

Proof All that remains to be verified is that S-polynomials resulting from matches found in $`R`$ can be added to $`R`$ without altering $`\underset{R}{\overset{}{}}`$. We assume all polynomials in $`R`$ to be monic (possible since $`K`$ is a field). Now S-polynomials result from two types of overlap.

For the first case let $`r_1,r_2`$ be polynomials in $`R`$ such that $`u\mathrm{𝙻𝚃}(r_1)=\mathrm{𝙻𝚃}(r_2)v`$ for some $`u,v\mathrm{Arr}P\mathrm{\Delta }`$. Then the S-polynomial is $`s:=\mathrm{𝚛𝚎𝚖}(r_2)vu\mathrm{𝚛𝚎𝚖}(r_1)\mathrm{Arr}P_K\mathrm{\Delta }`$ where $`\mathrm{𝚛𝚎𝚖}(r_i):=r_i\mathrm{𝙻𝚃}(r_i)`$ for $`i=1,2`$. Now $`\mathrm{𝚛𝚎𝚖}(r_2)vu\mathrm{𝚛𝚎𝚖}(r_1)=ur_1r_2v`$ therefore $`s=\mathrm{𝚛𝚎𝚖}(r_2)vu\mathrm{𝚛𝚎𝚖}(r_1)=_R0`$, and hence the congruence generated by $`R^{}:=R\{s\}`$ coincides with $`=_R`$.

For the second case let $`r_1,r_2`$ be polynomials in $`R`$ such that $`u\mathrm{𝙻𝚃}(r_1)v=\mathrm{𝙻𝚃}(r_2)`$ for some $`u,v\mathrm{Arr}P\mathrm{\Delta }`$. Then the S-polynomial is $`s:=\mathrm{𝚛𝚎𝚖}(r_2)u\mathrm{𝚛𝚎𝚖}(r_1)v\mathrm{Arr}P_K\mathrm{\Delta }`$. Now $`\mathrm{𝚛𝚎𝚖}(r_2)u\mathrm{𝚛𝚎𝚖}(r_1)v=ur_1vr_2`$ therefore $`s=\mathrm{𝚛𝚎𝚖}(r_2)u(r_1)v=_R0`$, and hence the congruence generated by $`R^{}:=R\{s\}`$ coincides with $`=_R`$.  $`\mathrm{}`$

An example of an application of the results proved above can be found in Section 5.

## 4 Left Kan Extensions

We obtain a further result by expressing the presentation of a noncommutative polynomial algebra as a problem of computing a left Kan extension over framed modules $`\mathrm{𝖪𝖬𝗈𝖽𝗌}`$ (modules over a fixed field).

###### Definition 4.1

A left Kan extension data for $`\mathrm{K}`$-categories $`(M^{},F^{})`$ consists of small categories $`𝖠`$, $`𝖡`$ and functors $`M^{}:𝖠\mathrm{𝖪𝖬𝗈𝖽𝗌}`$ and $`F^{}:𝖠𝖡`$. A left Kan extension presentation for $`\mathrm{K}`$-categories is a quintuple $`𝒫:=kan\mathrm{\Gamma }|\mathrm{\Delta }|RelB|M|F`$ where

1. $`\mathrm{\Gamma }`$ and $`\mathrm{\Delta }`$ are (directed) graphs;
2. $`M:\mathrm{\Gamma }\mathrm{𝖪𝖬𝗈𝖽𝗌}`$ and $`F:\mathrm{\Gamma }P_K\mathrm{\Delta }`$ are graph morphisms to the category of $`K`$-modules and the free $`K`$-category on $`\mathrm{\Delta }`$ respectively;
3. and $`RelB`$ is a set of relations on the free $`K`$-category $`P_K\mathrm{\Delta }`$.

Formally, we say $`𝒫`$ presents the left Kan extension $`(E,\epsilon )`$ of the left Kan extension data $`(M^{},F^{})`$ where $`M^{}:𝖠\mathrm{𝖪𝖬𝗈𝖽𝗌}`$ and $`F^{}:𝖠𝖡`$ if $`\mathrm{\Gamma }`$ is a generating graph for $`𝖠`$ and $`M:\mathrm{\Gamma }\mathrm{𝖪𝖬𝗈𝖽𝗌}`$ is the restriction of $`M^{}:𝖠\mathrm{𝖪𝖬𝗈𝖽𝗌}`$; $`cat_K\mathrm{\Delta }|RelB`$ is a $`K`$-category presentation for $`𝖡`$ and $`F:\mathrm{\Gamma }P_K\mathrm{\Delta }`$ induces $`F^{}:𝖠𝖡`$.

We expect that a left Kan extension $`(E,\epsilon )`$ is given by a set $`EB`$ for each $`B\mathrm{Ob}\mathrm{\Delta }`$ and a function $`Eb:EB_1EB_2`$ for each $`b:B_1B_2𝖡`$ (defining the $`K`$-functor $`E`$) together with a function $`\epsilon _A:XAEFA`$ for each $`A\mathrm{Ob}𝖠`$ (the natural transformation).

For the following theorem it is helpful to note that $`=_{FQ}^r`$ will denote the right congruence generated by $`FQ`$. Square brackets $`[]_{FQ}^r`$ denote the corresponding congruence classes.

###### Theorem 4.2 (Congruences on Algebras are Kan Extensions)

Let $`𝒫:=kan\mathrm{\Gamma }|\mathrm{\Delta }|RelB|M|F`$ be a presentation of a Kan extension for $`K`$-categories where:

1. $`\mathrm{\Gamma }`$ is the graph with one object $`A`$ and a collection of arrows $`Q`$,
2. $`\mathrm{\Delta }`$ is the graph with one object $`B`$ and a set of arrows $`X`$,
3. $`RelB`$ is a set of polynomial relations $`RK[X^{}]`$,
4. $`M:𝖠\mathrm{𝖪𝖬𝗈𝖽𝗌}`$ maps $`A`$ to $`K[1]`$ and the arrows of A to the identity morphism,
5. $`F:𝖠P_K\mathrm{\Delta }`$ maps the arrows of $`𝖠`$ to polynomials of $`K[X^{}]`$

Then the left Kan extension presented by $`𝒫`$ is $`(E,\epsilon )`$ where

1. $`E(B)`$ is isomorphic to $`(K[X^{}]/=_R)/=_{FQ}^r`$,
2. $`E(b)`$ is defined by $`E(b)[p]_R:=[pb]_R`$,
3. $`\epsilon :MEF`$ is given by $`\epsilon _AM(q):=[[q]_R]_{FQ}^r`$.

Outline Proof It is required to verify that $`E`$, as defined above, is a well-defined $`K`$-functor. This is quite routine and comes from the fact that the congruence preserves addition, scalar multiplication and right-multiplication. To verify that $`\epsilon `$ is a natural transformation of $`K`$-functors is straightforward, remembering that $`M(q)`$ is the identity morphism on $`K[1]`$. To check the universal property we suppose there is another such pair $`(E^{},\epsilon ^{})`$ and by drawing the commutative diagram we find that there is a unique natural transformation $`\alpha :EE^{}`$ defined by $`\alpha (b):=E^{}(b)(\epsilon ^{}(1_A))`$ for $`bX^{}`$.  $`\mathrm{}`$

It is not claimed that this result is at all deep or difficult, given the results of  but it allows the possibility of using Gröbner bases to compute different types of left Kan extensions.

###### Corollary 4.3

Gröbner bases can be used to compute left Kan extensions of the above type.

Outline Proof Let $`𝒫`$ be as above. Define the $`P_K\mathrm{\Delta }`$-set as

$$T:=MA\times \mathrm{Arr}P_K\mathrm{\Delta }$$

and write the terms $`A|p`$ where $`p\mathrm{Arr}P_K\mathrm{\Delta }`$. Define the system of polynomials $`𝒮:=(S_E,S_\epsilon )`$ where

$$S_E:=R\text{ and }S_\epsilon :=\{A|FqA|1:qQ\}$$

The results in  describe Gröbner basis procedures for one-sided ideals in finitely presented noncommutative algebras over fields. The polynomials defining the $`K`$-algebra $`𝖡`$ as a quotient of the free $`K`$-algebra $`P_K\mathrm{\Delta }`$ are combined with the polynomials defining a right congruence $`=_{FQ}^r`$ of $`𝖡`$, by using a tagging notation. Standard noncommutative Gröbner basis techniques can then be applied to the mixed set of polynomials, thus calculating $`𝖡/=_{FQ}^r`$ whilst working in a free structure, avoiding the complication of computing in $`𝖡`$.

Suppose $`𝒢`$ is a Gröbner basis for $`𝒮`$. Then the Kan extension is given in the following way:

1. $`E(B):=\mathrm{𝙸𝚁𝚁}`$,
2. $`E(b):A|p\mathrm{𝚒𝚛𝚛}(A|pb)`$, for $`A|p`$ in $`E(B)`$, $`b`$ in $`K[X^{}]`$
3. $`\epsilon _A(1):=A|1`$

where $`\mathrm{𝚒𝚛𝚛}(A|pb)`$ is the irreducible result of repeated reduction of $`A|pb`$ by $`_𝒢`$ and $`\mathrm{𝙸𝚁𝚁}`$ is the set of all irreducible terms of $`T`$.  $`\mathrm{}`$

###### Remark 4.4

It is worth remarking that, as with the rewriting methods developed in , the Gröbner basis methods developed in  which are referred to above do not require changes in the existing programs. The use of tags enables the combination of polynomials giving the conditions for the action of the Kan extension together with the polynomials giving the conditions for the natural transformation.

## 5 Examples

The first example illustrates the previous section, showing that the standard Gröbner basis computation is the computation of a Kan extension and extending the example to make clear the type of calculation used for right congruences of algebras. The second example demonstrates the use of Gröbner bases to calculate the morphisms of a $`K`$-category given by a presentation. In each case we consider the left Kan extension given by a presentation $`𝒫:=\mathrm{\Gamma }|\mathrm{\Delta }|RelB|M|F`$.

###### Example 5.1

*Let $`\mathrm{\Gamma }`$ be the trivial graph with one object $`A`$. Let $`\mathrm{\Delta }`$ be the graph with one object $`B`$ and arrows $`X:=[e_1,e_2,e_3]`$. Let $`RelB`$ be the set of polynomials*

$$R:=\{e_1e_1e_1,e_2e_2e_2,e_3e_3e_3,e_3e_1e_1e_3,e_2e_1e_2e_1e_2e_1+\frac{2}{9}e_2\frac{2}{9}e_1,e_3e_2e_3e_2e_3e_2+\frac{2}{9}e_3\frac{2}{9}e_2\}.$$

*$`F:\mathrm{\Gamma }P_K\mathrm{\Delta }`$ be inclusion and define $`M(A):=K[1]`$. The system $`𝒮`$ consists only of untagged polynomials $`R`$ because there are no non-trivial arrows in $`𝖠`$. We use the length-lexicographic ordering with $`e_3>e_2>e_1`$ to obtain Gröbner basis for the congruence generated by $`𝒮`$ in $`K[X^{}]`$ by adding*

$$e_3e_2e_1e_3e_2e_3e_2e_1+\frac{2}{9}e_2e_1\frac{2}{9}e_1e_3$$

*to $`R`$. The irreducible terms $`\mathrm{𝙸𝚁𝚁}`$ in this case are sums of $`K`$-multiples of the following terms*

$`\{A|1`$, $`A|e_1,A|e_2,A|e_3`$, $`A|e_1e_2,A|e_1e_3,A|e_2e_1,A|e_2e_3,A|e_3e_2`$, $`A|e_1e_2e_1,A|e_1e_2e_3,A|e_1e_3e_2,A|e_2e_1e_3,A|e_2e_3e_2,A|e_3e_2e_1`$, $`A|e_1e_2e_1e_3,A|e_1e_2e_3e_2,A|e_1e_3e_2e_1,A|e_2e_1e_3e_2,A|e_2e_3e_2e_1\}.`$

*In this example the tag “$`A|`$” is redundant: the $`K`$-module $`EB`$ is a $`K`$-algebra, in fact it is the Hecke algebra $`H_4`$. Suppose now that $`\mathrm{\Gamma }`$ has one arrow $`q`$ whose image under $`F`$ is $`e_2e_1`$. The system of polynomials $`𝒮`$ for the Kan extension now has an $`\epsilon `$-polynomial namely $`A|e_2e_1A|1`$. Applying Buchberger’s Algorithm with the length-lexicographic ordering $`e_3>e_2>e_1>A|`$ results in a Gröbner basis of mixed polynomials:*

$`\{e_1e_1e_1,e_2e_2e_2,e_3e_3e_3,e_3e_1e_1e_3,e_2e_1e_2e_1e_2e_1+\frac{2}{9}e_2\frac{2}{9}e_1,e_3e_2e_3e_2e_3e_2+\frac{2}{9}e_3\frac{2}{9}e_2,`$

$`e_3e_2e_1e_3e_2e_3e_2e_1+\frac{2}{9}e_2e_1\frac{2}{9}e_1e_3,A|e_2e_1A|1,A|e_1A|1\}`$.

*The right congruence classes of $`e_2e_1`$ on $`H_4`$ are represented by sums of $`K`$-multiples of the following irreducible terms i.e. $`\mathrm{𝙸𝚁𝚁}`$ consists of:*

$`\{A|1`$, $`A|e_2,A|e_3`$, $`A|e_2e_3,A|e_3e_2`$, $`A|e_2e_3e_2,A|e_3e_2e_1`$, $`A|e_2e_3e_2e_1\}.`$

*Here the tag “$`A|`$” is necessary in the computation of the Gröbner basis. The final results may be written as right congruence classes $`[e_3e_2]^r`$, say, instead of tagged terms $`A|e_3e_2`$ but the representation as tagged terms allows us to determine whether $`e_1e_2e_3`$ and $`e_2e_3`$ occur in the same class: reducing $`A|e_1e_2e_3`$ and $`A|e_2e_3`$ has the same result, so they are congruent.*

###### Example 5.2

*Let $`𝖡`$ be the $``$-category generated by the graph $`\mathrm{\Delta }`$:*

*The arrows of the free category $`P_K\mathrm{\Delta }`$ are sums of $``$-multiples of terms occuring in the same column of the following table (the hom-sets consisting solely of identities are omitted):*

| $`B_1B_2`$ | $`B_1B_3`$ | $`B_1B_4`$ | $`B_1B_5`$ | $`B_2B_2`$ | $`B_2B_3`$ | $`B_4B_3`$ | $`B_5B_4`$ | $`B_5B_3`$ |
| --- | --- | --- | --- | --- | --- | --- | --- | --- |
| $`a`$ | $`ac`$ | $`h`$ | $`e`$ | $`1_{B_2}`$ | $`c`$ | $`g`$ | $`f`$ | $`j`$ |
| $`ab`$ | $`abc`$ | $`ef`$ |  | $`b`$ | $`bc`$ |  |  | $`fg`$ |
| $`ab^2`$ | $`ab^2c`$ |  |  | $`b^2`$ | $`b^2c`$ |  |  |  |
|  |  |  |  |  |  |  |  |  |
| $`ab^n`$ | $`ab^nc`$ |  |  | $`b^n`$ | $`b^nc`$ |  |  |  |

*Let $`R`$ be the relations defining $`𝖡`$*

$$R:=\{ab^3ab^2ab+a,b^3cb^2cbc+c,abc+defg,ac+dhg,fgj\}$$

*Applying the length-lexicographic ordering with $`a<b<c<d<e<f<g<h<j`$ it can be checked that $`R`$ is a Gröbner basis. It can therefore be immediately deduced that the arrows of $`𝖡`$ are uniquely represented by $``$-multiples of terms occurring in the same column of the following table:*

| $`B_1B_2`$ | $`B_1B_3`$ | $`B_1B_4`$ | $`B_1B_5`$ | $`B_2B_2`$ | $`B_2B_3`$ | $`B_4B_3`$ | $`B_5B_4`$ | $`B_5B_3`$ |
| --- | --- | --- | --- | --- | --- | --- | --- | --- |
| $`a`$ | $`ac`$ | $`h`$ | $`e`$ | $`1_{B_2}`$ | $`c`$ | $`g`$ | $`f`$ | $`j`$ |
| $`ab`$ | $`abc`$ | $`ef`$ |  | $`b`$ | $`bc`$ |  |  |  |
| $`ab^2`$ | $`ab^2c`$ |  |  | $`b^2`$ | $`b^2c`$ |  |  |  |
|  |  |  |  |  |  |  |  |  |
|  |  |  |  | $`b^n`$ |  |  |  |  |

## 6 Further Questions

### 6.1 Induced Modules

It would be useful to phrase the results of Section 4 in terms of induced modules, relating it to the commutative case in .

### 6.2 Extensions of Gröbner basis techniques

To apply rewriting to Kan extensions we had to generalise it. We have not yet discovered how precisely to generalise Gröbner bases to apply to *any* Kan extension of $`K`$-categories over $`\mathrm{𝖪𝖬𝗈𝖽}`$.

### 6.3 Rings with Many Objects

Mitchell’s classic work, generalises noncommutative homological ring theory to (pre)additive category theory . His work motivates the investigation of Gröbner basis techniques for $`K`$-categorical Kan extensions by the potential for Gröbner bases to provide more powerful methods of computation (of homology or cohomology) in this setting.

### 6.4 Term rewriting and Monads

Term rewriting systems, widely used throughout computer science, are similar to algebraic theories (algebraic theories declare term constructors, term rewriting systems declare term constructors and rewrite constructors). Algebraic theories can be modelled by finitary monads over $`\mathrm{𝖲𝖾𝗍𝗌}`$. Term rewriting systems can be modelled by finitary monads over the category of preorders $`\mathrm{𝖯𝗋𝖾}`$. This has been useful in providing categorical proofs of rewriting theories. The particularly interesting point is that term rewriting systems can be modelled as monads over a more complex base category. So $`𝖢`$-algebraic theories can be modelled by finitary monoids on $`𝖢`$. There is a relation between monads, adjoint functors and Kan extensions. We need to investigate the relation between string rewriting for Kan extensions and the monads modelling algebraic theories and term rewriting systems.

### 6.5 Petri nets

Gröbner basis procedures can be usefully applied in Petri net analysis. To every Petri net there is an associated category – a Petri category . How does the structure for Petri categories relate to Kan extensions? Are the Gröbner basis techniques usefully extended by relating these two areas or are they in fact the means by which the areas can be related?

### 6.6 Automatic Structure

For groups, monoids and coset systems there is a well-known concept of an automatic structure. These systems are special cases of Kan extensions so it is natural to ask what would be the definition of an automatic structure for a left Kan extension in general.


text:
# REFERENCES

A New Hypothesis for Layers of High Reflectivity Seen in MST Radar Observations

G. C. Asnani and M. K. Rama Varma Raja$`{}_{}{}^{}`$

Indian Institute of Tropical Meteorology, Dr. Homi Bhabha Road , Pune 411 008(India). E-mail: asnani@giaspn01.vsnl.net.in or Prof.asnani@vsnl.com

$`{}_{}{}^{}`$ Department of Physics, University of Pune, Pune 411 007(India). E-mail: rama@physics.unipune.ernet.in

We have worked with MST Radar located at Gadanki, Tirupati, India(13.47 degree N, 79.18 degree E). Altitude of the location is approximately 100 meters. This is the first and only MST Radar operating in India. It is in Tropical Monsoon region. Monsoon moves northward across Tirupati around 1st June and withdraws southward across Tirupati in the first week of December. Our interest has been to examine the characteristics of vertical velocity and other wind characteristics associated with monsoon. We examined the characteristics of range-compensated Signal-to-Noise ratio ($`r^2`$ SNR). We call this as Reflectivity. We examined the MST Radar data set for 14 months (September 1995 to November 1996 except May 1996). The height range considered for the analysis was between 3.6 km and 21 km above ground. Our findings have been on the following lines:

1) Except on Thunderstorm occasions, high reflectivity-regions are in the form of layers 1-2 km thick. One such high-reflectivity layer is always present near tropopause level 17 km. Below the tropopause, there is a bunch of such high-reflectivity layers, generally 3-4 in number, between 4 and 11 km. The atmospheric layer between 11 and 15 km is generally free from high reflectivity layer.

2) On a thunderstorm occasion, there is a deep high-reflectivity layer extending from 4-11 km. After the passage of the thunderstorm, this deep layer of high reflectivity breaks up into layers.

3) Layers of high reflectivity occur throughout the year even outside monsoon season, when ITCZ is far away from the region and they cannot be attributed as originating from deep convective clouds. When visual observation and MST observations are taken simultaneously at Gadanki, visual clouds are estimated to be at the same levels as the high reflectivity layers seen through MST observations. Indian satellite pictures over Gadanki also suggest similar heights of clouds as given by MST Radar for high reflectivity layers.

4) Satellite pictures in infra-red range show much more extensive areas of cloudiness than the pictures in the satellite visible range. In other words, there are extensive sub-visual clouds in the atmosphere.

5) Every month early morning and late evening, in twilight hours we see beautiful cirrus clouds in the form of cloud streets, streaks or sheets on several occasions which may or may not be clearly visible at other hours.

6) On looking at the sky frequently, one gets the impression that the sky is not clear even though we do not see clouds or haze layers. In these haze layers, appear clouds in the form of cloud streets, streaks or cloud sheets at some times. The appearance of these clouds gives the clear impression that there are waves in the atmosphere which give visible clouds in the region of upward motion associated with these waves. Again in each bigger wave cloud, there are smaller and smaller wave clouds and clearances; there are waves within waves. When the clouds disappear, they leave a sort of haze. Hence, the clouds form out of haze and leave some haze after dissipating. Even when there are no visible clouds during the day or night, the structure of the atmosphere is patchy in appearance. One gets a clear impression that there are waves and waves, bigger and smaller waves in the atmosphere which are creating patches of haze and sometimes visible clouds in the atmosphere. These are due to gravity-type waves with a very wide spectrum of horizontal and vertical wavelengths. As we know from theoretical and observational evidence, horizontal wavelengths are 1-2 orders of magnitude larger than vertical wavelengths. If and when they occur in the atmosphere, they have a tendency to take horizontally spread layered structure with vertical depth 1-2 orders of magnitude smaller than horizontal extent.

7) In the atmosphere, we visualize three classes of waves: a.Inertial waves or Rossby-type waves: Their horizontal extent is of the order of a few thousand kilometers and vertical wavelengths of the order of 10 km. In the mechanism of their formation, we have to consider the rotation of the earth and the resulting coriolis force. Their period is of the order of a few days. b. Gravity waves: These arise mainly from local horizontal pressure gradients arising out of gravitational weight of the overlying air column, air accelerating from higher pressure towards lower pressure. Horizontal accelerations and displacements are accompanied by appropriate vertical accelerations and displacements to conform to the requirements of law of conservation of mass i.e., equation of continuity.

Vertical displacements and accelerations of air parcels can also arise from buoyancy forces. Heavier parcel tends to sink down while lighter air parcels tend to rise up in an environment of horizontal density gradients. These are called Brunt-Vaisala oscillations. These horizontal gradients of density arise out of differences in temperature, humidity and hydro-meteor loading.

This hydrometeor-loading needs a little elaboration:

(i) Every parcel of cloud air contains at least one hydrometeor in liquid water or solid form. Inside each hydrometeor is an aerosol which acts as a nucleus which has induced condensation and/or freezing.

(ii) Invariably, hydrometeor has higher density than the surrounding air. As such, it tends to fall down due to gravitational force.

(iii) As it descends down, it exchanges sensible heat and moisture with its environment. Hence, its volume, mass, and density undergo a change during its descent.

(iv) As the hydrometeor descends down with gravitational acceleration through the air parcel, there is frictional resistance/viscous resistance to its vertical motion. soon, the hydrometeor loses its acceleration and descends down with what is called ”Terminal velocity”. Where has its weight gone? Its weight is taken up by the air parcel which is offering resistance to its vertical movement and acceleration. In other words, the air parcel becomes heavier to the extent it has taken over the gravitational acceleration of the falling hydrometeor. If the hydrometeor falls with its terminal velocity, it means that its entire weight is taken over by the air parcel. As such the air parcel has become heavier by the total weight of the hydrometeor; the density of the air parcel has effectively increased.

If only half of the gravitational acceleration of the descending hydrometeor has been taken over by the air parcel, then the weight of the air parcel has increased only by half the weight of the hydrometeor.

The hydrometeor gradually loses its gravitational acceleration and gives its weight to the surrounding air parcel gradually and not instantaneously. As such, the air parcel takes the load of the hydrometeor gradually during the downward trajectory of the descending hydrometeor.

In many calculations, for the sake of simplicity, it is assumed that as soon as condensation or freezing takes place in the atmosphere, the load of the hydrometeors is immediately taken over by the surrounding air. However, we have to recognize that the hydrometeor-loading occurs gradually through a finite interval of time.

We should also remember that during the fall, the hydrometeor is simultaneously undergoing a change in its volume, mass and density. Hence, a realistic, quantitative estimate of hydrometeor loading effect on the air parcel needs careful calculation. However, nature takes care of the process and creates varying density effects on the cloud air parcel as the hydrometeor descends.

(v) In addition to buoyancy fall of the hydrometeor, there are upward and downward motions of air parcels inside the cloud. These upward and downward motions of air parcels inside the cloud create further complications in the calculation of hydrometeor-loading effect on air parcel.

(vi) In addition to pure buoyancy forces operating in a class of waves called gravity waves, there also occur what are known as Kelvin-Helmholtz waves due to presence of vertical shear of horizontal winds which is almost always present.

(vii) This class of gravity waves of Kelvin-Helmholtz type have very small wavelengths of the order of centimeters and meters and correspondingly small periods of the order of a few minutes. Earth’s rotation or Coriolis force does not perceptibly come into the calculations for these waves.

c. Inertio-Gravity waves: Between the two extremes of large inertial waves and small gravity waves, there is an intermediate class of waves which may be termed as inertio-gravity waves in which Coriolis force plays some role along with gravity force. There is literature on the subject of inertio-gravity waves ( , , , etc.), but more work needs to be done on this class of waves. Orographic influence also come into play.

8) When we fly in an aircraft, large-scale weather and clouds are influenced by Rossby-type waves. When we look at the sky through cockpit or through the window near the window-seat, during day time, we immediately get the view of air clouds at different levels and also gravity waves of various dimensions near the flight level. We see fairly large waves with estimated wavelengths of the order of tens of kilometers, along with embedded smaller and smaller waves, thick clouds, thin clouds, thinner clouds, space filled with haze and space clear of visible clouds.

In our view, MST Radar reflectivity pattern gives us spot view of these numerous beautiful waves.

9) We have analyzed the field of MST Radar reflectivity as seen at Gadanki along with MST Radar measured wind fields. We have interpreted the reflectivity fields within a conceptual model given below:

(i) Inertio-gravity waves in the atmosphere generate layers of upward/downward motion, high/low humidity and high/low temperature lapse rates. The layers of upward and downward motion are regularly seen in the vertical wind field given by MST Radar. The vertical wavelength of these inertio-gravity waves has wide spectrum depending on orography and diabatic heating; vertical wavelength of about 5 km is a more frequently observed wavelength. The corresponding horizontal wavelength is of the order of 200 km, the more dominant wavelength visible in satellite picture is 500 km in the direction of wind and 1000 km across the wind.

The layers of high relative humidity created by inertio-gravity waves are favorable for the formation of layered clouds, which we call ”Mother Cloud Layers”; these clouds may be visible or sub-visible.

(ii) Hydrometeors inside a ”Mother Cloud Layer” tend to fall down attaining their respective terminal velocities. During their stay inside the clouds, the hydrometeors exchange heat, moisture, mass and momentum with the environmental air on small micro-scales. These exchanges between the hydrometeors and the ”Mother Clouds’s air” create strong gradients of temperature, humidity, density and momentum. Density variations are also created through hydrometeor-loading.

Electrical charges are also generated during the processes of condensation, evaporation, freezing, melting and sublimation.

These micro-physical gradients in density along with prevailing wind field in the vertical generate internal gravity waves in the form of Brunt-Vaisala oscillations, Kelvin-Helmholtz waves and other waves of different horizontal and vertical wavelengths. These wavelengths range from a few millimeters to tenths of meters in the vertical and from a few meters to about thousand meters in the horizontal. Known laws of physics and dynamics suggest that the wavelengths may be still smaller, equivalent to the distances between adjacent parcels of air exchanging heat moisture, mass and momentum, with the hydrometeor embedded in the parcel.

(iii) The strong gradients of temperature, humidity and density created by these micro-physical and micro-dynamical processes in the air surrounding the hydrometeor or an ensemble of hydrometeors cause strong variations in the refractive index of air parcel, in respect of electro-magnetic lidar and radar beams impinging on the air parcels. In turn, this causes high reflectivity/scatter of the impinging lidar/radar beam. In respect of VHF MST radar Bragg-type reflection/scatter is a dominant type of reflection/ scatter.

We examined the size of air parcels giving the highest values of reflectivity, at Gadanki. We came to the conclusion that their horizontal extent is of the order of 1 km while their vertical extent is of the order of 100 m.

Indian MST radar beam oriented in vertical has a half-wavelength of about 3m. As such, Indian MST radar is capable of detecting reflectivity patterns of vertical wavelengths of the order of about 6m. These small-scale variations in reflectivity appeared in the form of very delicate embroidery inside the large-scale reflectivity of the ”Mother Cloud Layer”.

(iv) These variations in the reflectivity pattern may look like turbulent fluctuation in the atmosphere. If we do not associate these fluctuations with clouds and hydrometeors inside the clouds, the clouds might appear as clear-air turbulence as has been prevalent in the current explanation appearing in literature connected with MST radars. This prevalent explanation has faced paradoxes, the main paradox being of thin horizontal sheets of turbulence.

If we free our thinking from the concept of clear-air turbulence and turn our thinking in the direction of visible or sub-visible clouds containing hydrometeors, the apparent paradoxes of clear-air turbulence causing high- MST radar reflectivity get immediately resolved.

The existence of sub-visible clouds occupying much larger area than the visible clouds has now been established beyond question, through latest observations by satellites in the infra-red range, by aircraft flying through cirrus cloud air and by lidars operating in high altitude aircraft sending their beams through visible and sub-visible cloud layers.

(v) Using over 2,50,000 observational data points for MST radar reflectivity and vertical wind shear (deduced from corresponding MST radar wind observations) spread over 14 months (from 1995 September to 1996 November), we plotted scatter diagrams of MST radar reflectivity versus vertical wind shear. We are pleasantly surprised to find that reflectivity decreases almost exponentially as vertical wind shear increases. If mechanical turbulence was the main cause of high reflectivity, we should see reflectivity increasing with vertical wind shear, and not decreasing almost exponentially. Scatter diagrams for each of the 14-months are presented in . Also, Scatter diagrams for four representative months (January, April, July and October), for Indian monsoon region, are presented in ,. This shows that mechanical turbulence is not the principal cause of high-MST radar reflectivity.  had hypothesized that turbulence may not be the primary cause of high-reflectivity seen in MST radars.

(vi) Knowing the importance of cirrus clouds, the world scientific community launched the programme known as FIRE (First ISCCP Regional Experiment). This FIRE programme concentrated on the study of layer clouds (Cirrus Clouds in the upper troposphere and low level stratus clouds in the lower troposphere). FIRE I programme was executed during the period 1985-1990 while FIRE II programme was executed during the period 1990-1995. FIRE III programme is proposed to be executed in the beginning of this new millennium, with particular emphasis on the tropics. Results of FIRE I have been summarized in a special issue of Monthly Weather Review (November, 1990); results of FIRE II have been summarized in a special issue of Journal of Atmospheric Sciences (December, 1995). This topic is an important component of CLIVAR programme in the tropics.

The results of FIRE I and FIRE II have broadly confirmed that there is fine micro structure inside the layered clouds which can be interpreted easily, atleast qualitatively, in terms of micro-physical and micro-dynamical processes presented above.

Also, the latest Numerical Modeling Work on Cirrus Clouds (for example , ,) show that there are fine-scale structures of various in-cloud parameters including temperature, humidity and ice-concentrations.

In fact in our view these fine scale structures created inside the visible or sub-visible ”Mother Cloud Layers” can cause steep refractive index gradients sufficient to cause high-MST radar reflectivity.

10) We expect that the conceptual model of MST radar reflectivity presented above will give a new orientation to the thinking and interpretation of MST radar reflectivity. It will provide a satisfactory, physically and dynamically acceptable, interpretation of the reflectivity patterns seen in the MST radar observation.

11) A few corollaries follow from this conceptual model:

(i) Since, high-MST radar reflectivity layer, 1-2 km thick, is always observed near the tropopause, it may or may not be directly connected to inertio-gravity waves. The mechanism for the formation and sustenance of high-reflectivity layer is realized as follows:

(a) The temperature near the tropopause level are very cold ( 200 K); temperature lapse rate is stable, 2-4 degree C/km; as such vertical mixing of air is inhibited and is weak. Relative humidity below the tropopause is high . Water substance and aerosols injected into the upper troposphere by deep convection near ITCZ remains below the tropopause while the relative humidity is very low above the tropopause. Water substance and aerosols form visible or sub-visible cirrus cloud layer or haze layer below the tropopause. Through the micro-physical and micro-dynamical processes mentioned earlier, the air layer develops strong vertical gradients or discontinuities in the refractive index with respect to MST radar beam impinging on the air there. This gives high-reflectivity echoes near the tropopause level on all days of the year.

When the cloud gets dissolved, it leaves large number of aerosols suspended there. By themselves, aerosols are not likely to be detected by MST radar. But the layer of high content of aerosols can be detected and has been detecting near the tropopause (,, etc.).

In the tropics, ITCZ injects aerosols and moisture which remain trapped in the layer immediately below the tropopause. In extra-tropics, this injection is done by extra-tropical cyclone waves and polar front. On the same reasoning, as given for tropics, a layer with high content of aerosols and thin cirrus ice crystals will also get formed below the tropopause in extra-tropics. Thus a layer having high content of aerosols and thin cirrus cloud is expected to envelope the whole earth’s atmosphere near tropopause. This has been substantiated by observations of (Nee et al., 1995, 1998; FIRE I and FIRE II observations and their results published in the Special issues of Monthly Weather in November 1990 and Journal of Atmospheric Sciences in December 1995 respectively). Asnani et al.  had hypothesized the existence of an aerosol layer near tropical tropopause, based on the same mechanism mentioned above.

(ii) As we have stated above, observations confirm existence of alternate layers of upward and downward motion with vertical depth of 2-3 km. We should expect accumulation and depletion of both water substance and aerosol substance near the levels of vertical convergence. Further vertical upward motion tends to create higher relative humidity and higher temperature lapse rate; vertical downward motion tends to do the opposite, creating stable lapse rate and drier air. Hence we should expect to find layers of high and low relative humidity in the vertical. Sensitive instrumentation is required to detect this type of structure in the atmosphere; this structure is likely to be missed by the ordinary radiosonde instruments. Such layers have been detected by special effort .

(iii) As stated earlier, these alternate layers of upward and downward motion are associated with inertio-gravity waves, which are always present in the atmosphere. These vertical wave motion will also tend to split large convective clouds, particularly in their decaying stage, into layered clouds. While convective instability in the atmosphere tends to generate deep convective clouds in the tropical atmosphere, these inertio-gravity waves inhibit the formation and sustenance of these deep convective clouds in the tropical atmosphere.

(iv) Cirrus clouds have a capacity to retain their existence for a long time, even away from the source of their formation. Hence, visible or sub-visible cirrus clouds are likely to be seen at many places, with or without deep convective clouds. The upward vertical motion associated with inertio-gravity waves tends to generate cirrus clouds, visible or sub-visible at many places in the atmosphere. If nothing else, these clouds influence the radiative heat budget of the earth’s atmosphere.

Acknowledgment: The authors thank Prof. D. Narayana Rao and his group at Department of Physics, Sri Venkateswara University, Tirupati (India) for considerable help in Indian MST Radar data collection and analysis. Mr. M. K. Rama Varma Raja thanks Dr. (Mrs.) P. S. Salvekar and the Director, Indian Institute of Tropical Meteorology for providing necessary support and facilities during the course of research work.


text:
# Haldane-gap excitations in the low-𝐻_𝑐 1-dimensional quantum antiferromagnet Ni(C5H14N2)2N3(PF6) (NDMAP).

## I Introduction

The unique properties of the one-dimensional (1D) integer-spin Heisenberg antiferromagnet (HAF) have captivated the minds of condensed matter physicists for the last 20 years. In total defiance of the quasi-classical picture of magnetism, the ground state in this system is a spin-singlet- a “quantum spin liquid” with only short-range (exponentially decaying) spin correlations. The excitation spectrum is also rather unique, and, even in the absense of any magnetic anisotropy, features a so-called Haldane energy gap. The wealth of theoretical and experimental results accumulated to date provide a fairly complete understanding of the physics involved, and few mysteries remain, as far as the behavior of the idealized model is concerned. Particularly revealing was the neutron scattering work done on real quasi-1D $`S=1`$ HAF compounds such as CsNiCl3, NENP (Ni(C2H8N2)2NO2(ClO4)), and Y2BaNiO5 (Ref. ).

One of the few remaining unresolved issues is the behavior of Haldane-gap antiferromagnets in high magnetic fields. An external magnetic field splits the triplet of Haldane excitations, driving one of the modes to zero energy at some critical field $`H_c`$. At this soft-mode quantum phase transition, static long-range antiferromagnetic correlations appear. In essence, the external field suppresses zero-point quantum spin fluctuations that are responsible for the destruction of long-range order in the spin-liquid state, and restores long-range spin coherency. Despite the success of high-field bulk studies of several material, it has been highly frustrating, that for most existing systems the actual values of the critical fields are unobtainable in neutron scattering experiments. As a result, the properties of the high-field phase are still largely unknown. It is even unclear, whether or not the high-field phase is commensurate, and virtually nothing is known about the excitation spectrum.

Traditionally, NENP was the workhorse of high-field studies. For this compound large single crystal samples can be fabricated, and the critical field $`H_c=9`$ T (when applied parallel to the chain-axis) is, in principle, accessible in a neutron-scattering experiment. In practice, it is however easier to perform measurements with a magnetic field applied perpendicular to the spin chains. The corresponding critical field for NENP is, unfortunately, much larger: $`H_c1113`$ T. In any case, measurements deep within the high-field phase are not possible. Moreover, due to certain structural features, the phase transition in NENP is smeared out. The g-tensors of the $`S=1`$ Ni2+ ions are staggered in this compound and lead to an effective staggered field when an external uniform field is applied. As a result, a static staggered magnetization appears at arbitrary weak applied fields, and, strictly speaking, no additional spontaneous symmetry breaking occurs at $`H_c`$.

The recent discovery of NDMAP (Ni(C5H14N2)2N3(PF6)), a relatively easily crystallized Haldane-gap compound with a critical field of only around 4 T, and no staggering of g-tensors within spin chains, promises to make the high-field phase readily accessible in neutron scattering studies. The crystal structure of this material is similar to that of NENP, and is visualized in Fig. 1. The AF spin chains run along the $`c`$ axis of the tetragonal structure (space group $`P_{nmn}`$, $`a=18.046`$ Å, $`b=8.705`$ Å, and $`c=6.139`$ Å), and are composed of octahedrally-coordinated $`S=1`$ Ni2+ ions bridged by triplets of nitrogen atoms. These long nitrogen bridges account for a realtively small in-chain AF exchange constant $`J=2.6`$ meV, as estimated from bulk $`\chi (T)`$ measurements. ESR and specific heat studies revealed a transition to the high-field phase at $`H_c^{}=3.4`$ T, and $`H_c^{}=5.8`$ T, extrapolated to $`T0`$, for a magnetic field applied parallel and perpendicular to the chain-axis, respectively. This anisotropy of critical field is attributed to single-ion easy-plane magnetic anisotropy of type $`DS_z^2`$. The anisotropy constant was obtained from bulk susceptibility data: $`D/J0.3`$. Using the well-known numerical result $`\mathrm{\Delta }_z0.41J+2pD`$, $`\mathrm{\Delta }_x0.41JpD`$, $`p2/3`$, one can thus estimate the Haldane gap energies: $`\mathrm{\Delta }_{}2.1`$ meV and $`\mathrm{\Delta }_{}0.54`$ meV.

While NDMAP appears to be an ideal model system for neutron scattering experiments in the high-field phase, additional characterization, particularly a measurement of inter-chain interactions and in-plane anisotropy, is required before such a study can be carried out. Finding the 3D AF zone-center is especially important, since it is at this wave vector that static long-range correlations are expected to appear in the high-field phase. Obviously, inelastic neutron scattering is the most direct method to obtain this information. In the present paper we report the results of a zero-field inelastic cold-neutron scattering study of deuterated NDMAP single-crystal samples, aimed at extracting this information.

## II Experimental procedures and results

Fully deuterated NDMAP single crystal samples were grown from solution as described in Ref. . It was observed that the crystals tend to shatter when cooled to low temperature, and even more so when warmed back up. When wrapped in aluminum foil the crystals do not fall apart, but the width of the mosaic distribution increases dramatically with thermal cycling. Most inelastic neutron scattering data were collected on a 140 mg single crystal sample that was taken trough the cooling cycle only twice. The mosaic of the as-grown sample was roughly $`0.3^{}`$ and increased to $`1.5^{}`$ and $`3^{}`$ after the first and second cooling, respectively. Inelastic neutron scattering measurements were performed on the SPINS 3-axis spectrometer installed on the cold neutron source at the National Institute of Standards and Technology Center for Neutron Research. Pyrolitic graphite crystals set for their (002) reflection were used as monochromator and analyzer. Beam divergences were approximately $`40^{}80^{}80^{}240^{}`$ through the instrument, with a cooled Be filter between the monochromator and sample. The measurements were done with a fixed final neutron energy $`E_f=2.8`$ meV. The crystal was mounted with either the $`a`$ or $`b`$ crystallographic axis vertical, making $`(0,k,l)`$ and $`(h,0,l)`$ reciprocal-space planes accessible to measurements. The sample was cooled to $`T=1.4`$ K in an ”ILL-Orange” cryostat with a 70 mm diameter sample well.

The primary goal of the experiment was to determine the $`a`$\- and $`b`$-axis dispersion relations and the polarizations of the two lower-energy Haldane-gap excitations, relevant for the soft-mode transition at $`H_c`$. Most of the data were collected in constant-$`Q`$ scans at the 1D AF zone-center $`l=0.5`$ in the energy transfer range 0–1 meV. In these dispersion measurements $`Q`$-resolution is particularly important, so a flat analyzer was used. Typical scans for different momentum transfers perpendicular to the $`c`$-axis are shown in Fig. 2. At all wave vectors a well-defined peak corresponding to the lower-energy Haldane excitation doublet is clearly seen around 0.5 meV energy transfer.

To observe the higher-energy Haldane-gap excitation and obtain an accurate measurement of the anisotropy constant we performed a constant-$`Q`$ scan in the range 0–2.4 meV (Fig. 3). To maximize intensity we used a horizontally-focusing analyzer pointing $`𝐜^{}`$ towards the analyzer to maintain wave vector resolution along the chain. The scattering angle was varied so the projection of wave vector transfer along the chain was $`0.5𝐜^{}`$ throughout the scan. In addition to the peak seen in the low-energy scans, a weaker feature is observed at $`\mathrm{}\omega 2`$ meV that can be attributed to the $`c`$-axis-polarized Haldane gap mode.

## III Data analysis and discussion

The measured constant-$`Q`$ scans were analyzed using a parameterized model cross section, numerically convoluted with the Cooper-Nathans 3-axis spectrometer resolution function. Near the 1D AF zone-center the single mode approximation (SMA) for the dynamic structure factor of isolated Haldane spin chain is known to work extremely well. For each channel of spin polarization the dynamic structure factor $`S^{(\alpha \alpha )}(𝒒,\omega )`$ can be written as:

$`S^{(\alpha \alpha )}(𝒒,\omega )|f(q)|^2(1{\displaystyle \frac{𝒒𝒆_\alpha }{q^2}})\times `$ (1)
$`\times {\displaystyle \frac{1\mathrm{cos}(𝒒𝒄)}{2}}{\displaystyle \frac{Zv}{\omega _{\alpha ,𝒒}}}\delta (\mathrm{}\omega \mathrm{}\omega _{\alpha ,𝒒}),`$ (2)
$`(\mathrm{}\omega _{\alpha ,𝒒})^2=\mathrm{\Delta }_\alpha ^2+v^2\mathrm{sin}^2(𝒒𝒄).`$ (3)
Here $`v`$ is the spin wave velocity, given by $`v2.49J`$. The dimension-less constant $`Z`$ defines the static staggered susceptibility of a Haldane spin chain: $`\chi _\pi =Zv/\mathrm{\Delta }`$.***Here we have adopted the notation used in Ref.  In the above expression we have included the magnetic form factor $`f(q)`$ for Ni2+ and the polarization factor $`\left(1\frac{𝒒𝒆_\alpha }{q^2}\right)`$. The structure factor for weakly-coupled chains can be calculated in the Random Phase Approximation (RPA). The expression for $`S^{(\alpha \alpha )}(𝒒,\omega )`$ does not change explicitly, but the excitations acquire dispersion perpendicular to the chain axis:

$$(\mathrm{}\omega _{\alpha ,𝒒})^2=\mathrm{\Delta }_\alpha ^2+v^2\mathrm{sin}^2(𝒒𝒄)+ZvJ^{}(𝒒).$$
(4)
In this formula $`J^{}(𝒒)`$ is the Fourier transform of inter-chain exchange interactions, that we assume to be isotropic (of Heisenberg type). According to numerical calculations $`Z1.26`$. The form of $`J^{}`$ can be guessed by looking at the crystal structure. The smallest inter-chain Ni-Ni distance (8.705Å) is along the $`b`$ crystallographic axis. We shall denote the corresponding exchange constant as $`J_y`$. The next-smallest inter-chain Ni-Ni distance (10.478Å) is along the (0.5,0.5,0.5) direction. This interaction, however, is frustrated by in-chain AF interactions (any site in one chain couples to two consecutive sites in another chain), and is thus irrelevant, within the RPA, at momentum transfers $`𝒒𝒄\pi `$. Finally, the third-smallest inter-chain distance (18.046Å) is along $`a`$. The corresponding coupling constant $`J_x`$ is expected to be very small, due to the large “bond” length. The Fourier transform of inter-chain interactions can thus be written as:

$$J^{}(𝒒)=2J_x\mathrm{cos}(𝒒𝒂)+2J_y\mathrm{cos}(𝒒𝒃).$$
(5)
The chain-axis exchange constant $`J`$ is not very important for our measurements: for scans collected at the 1D AF zone-center it only slightly influences the peak shapes, due to a non-zero $`Q`$-resolution along the chain-axis. We can therefore safely use the value previously obtained from susceptibility measurements. The relevant parameters of the model are thus the three gap energies $`\mathrm{\Delta }_x`$, $`\mathrm{\Delta }_y`$ and $`\mathrm{\Delta }_z`$, two inter-chain exchange constants $`J_x`$ and $`J_y`$ and an overall intensity prefactor. Three additional parameters were used to describe the background: an energy-independent component, and the intensity and width for a Lorenzian profile centered at $`\mathrm{}\omega =0`$ to account for incompletely resolved elastic scattering.

The difference between $`\mathrm{\Delta }_x`$ and $`\mathrm{\Delta }_y`$, usually a result of in-plane magnetic anisotropy of type $`E(S_x^2S_y^2)`$, is too small to observe two and separate corresponding peaks in any single constant-$`Q`$ scan. Distinct polarization factors for the two branches however allow us to extract both parameters in a global fit to the data measured at different momentum transfers perpendicular to the chain-axis. As a first step, we simultaneously analyzed the data collected in $`(0,k,l)`$ reciprocal-space plane (11 scans with a total of 382 data points). A very good global fit using Eqs. 2 and 4 is obtained with a residual $`\chi ^2=1.6`$. The solid lines in Fig. 2a–c were calculated from the globally optimized parameter set. The shaded areas represent the contribution of each mode, and the dashed lines show the background level. Figure 4 (right) shows the obtained $`b`$-axis dispersion relation (solid line), that has a minimum at $`k=0.5`$. Symbols in this figure represent the excitation energies obtained in fits to individual scans. A similar global fit (4 scans, 149 data points, $`\chi ^2=1.7`$) was applied to all constant-$`Q`$ scans measured in the $`(h,0,l)`$ scattering plane (solid lines in Fig. 2d and e). In this case the excitation energies at the zone-boundary $`(0,0,0.5)`$ were fixed to the values obtained from the $`(0,k,l)`$-plane global fit. Only the $`a`$-axis exchange constant $`J_x`$ was refined. Dispersion of magnetic excitations along this direction is barely detectable. The dispersion relation obtained from our fits is nontheless plotted in a solid line in Fig. 4 (left). The fitting analysis suggests a shallow minimum at $`h=0.5`$. From Eq. 5 we can thus guess that the global minimum of the 3D dispersion (3D AF zone-center) is located at $`(0.5,0.5,0.5)`$. The energy gap for $`c`$-axis polarized excitations was determined by fitting the model cross section to the wide-range constant-$`Q`$ scan measured with the horizontally-focusing configuration (Fig. 3, solid line). In this procedure the values of $`\mathrm{\Delta }_x`$ and $`\mathrm{\Delta }_y`$ were fixed. The parameters determined by the analysis described above are as follows: $`\mathrm{\Delta }_x=0.42(0.03)`$ meV, $`\mathrm{\Delta }_y=0.52(0.06)`$ meV, $`\mathrm{\Delta }_z=1.86(0.1)`$ meV, $`J_y=1.8(0.4)10^3`$ meV, and $`J_x=3.5(3.0)10^4`$ meV.

The in-chain exchange constant $`J`$ and anisotropy parameter $`D`$ are readily obtained from the measured gap energies: $`J0.81(\mathrm{\Delta }_x+\mathrm{\Delta }_y+\mathrm{\Delta }_z)=2.28`$ meV, $`D\frac{1}{4}(2\mathrm{\Delta }_z\mathrm{\Delta }_x\mathrm{\Delta }_y)=0.70`$ meV, and $`D/J=0.30`$, which is consistent with the bulk susceptibility result of Ref.  The relative strength of inter-chain interactions are $`J_y/J710^4`$ and $`J_x/J1.310^4`$. These ratios are very similar to those found in NENP.

## IV Summary

The small value of critical fields in NDMAP, compared to those in NENP, are a result of smaller in-chain exchange interactions and somewhat larger easy-plane magnetic anisotropy. The lowest-energy excitation in NDMAP is polarized along the crystallograhic $`a`$–axis. The 3D magnetic zone-center appears to be $`(0.5,0.5,0.5)`$. Future experimental studies of the high-field phase should thus concentrate on this region of reciprocal space.

###### Acknowledgements.

We would like to thank S. M. Shapiro for illuminating discussions, S.-H. Lee for his assistance with the measurements at NIST, and R. Rothe for technical support at BNL. Work at Brookhaven National Laboratory was carried out under Contract No. DE-AC02-98CH10886, Division of Material Science, U.S. Department of Energy. Work at JHU was supported by the NSF through DMR-9801742. This work used instrumentation supported by NIST and the NSF through DMR-9423101. Work at RIKEN was supported in part by a Grant-in-Aid for Scientific Research from the Japanese Ministry of Education, Science, Sports and Culture.