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# Effects of Disorder on Ferromagnetism in Diluted Magnetic Semiconductors

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## Abstract

We present results of a numerical mean field treatment of interacting spins and carriers in doped diluted magnetic semiconductors, which takes into account the positional disorder present in these alloy systems. Within our mean-field approximation, disorder enhances the ferromagnetic transition temperature for metallic densities not too far from the metal-insulator transition. Concurrently, the ferromagnetic phase is found to have very unusual temperature dependence of the magnetization as well as specific heat as a result of disorder. Unusual spin and charge transport is implied.

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Following the discovery of a ferromagnetic transition in Ga1-xMnxAs at temperatures in excess of 100 K , well above those found in counterparts based on II-VI semiconductors , there has been a surge in interest in the magnetic properties of diluted magnetic semiconductors (DMS). Theoretical models abound to explain the ferromagnetism . While it is generally accepted that the ferromagnetism is due to an effective interaction between the magnetic ions (Mn) mediated by mobile carriers (holes, since Mn, a group II element substitutes for Ga, a group III element), different models differ in detail, e.g. whether the interaction is RKKY or not, and also the approximations used to model the system.

In nonmagnetic doped semiconductors, such as phosphorus doped silicon , there has been no evidence for ferromagnetism due to carriers. Indeed, carrier hopping at low doping concentrations in the insulating phase is known to induce antiferromagnetic interactions between localized states, leading to a valence-bond-glass like state down to the lowest observable temperatures . In contrast, ferromagnetic tendencies were detected in doped diluted II-VI magnetic semiconductors already in the insulating regime at low temperatures , and subsequently ferromagnetism was observed in both II-VI and III-V semiconductors at metallic doping densities.

In insulating DMS, the presence of Mn has been shown to overwhelm the antiferromagnetic interaction between charge carriers,leading to an essentially ferromagnetic ground state. Monte Carlo simulations  for II-VI DMS in the insulating phase show that the ferromagnetic phase is very unusual, with a highly inhomogeneous magnetic profile, leading to unconventional properties such as M(T) curve that is not described by expansions around the critical point (critical point theories) or zero temperature (spin wave theories) over most of the ferromagnetic phase. By contrast, theoretical models for the metallic regime  have been based on the homogeneous electron gas, with a few exceptions, such as the possibility of phase separation .

It is well-known in conventional doped semiconductors that the carrier wavefunctions are those derived from an impurity band, for densities in the vicinity of the metal-insulator transition (MIT), up to factor of 3-5 above the MIT density, $`n_c`$. Density Functional calculations for a lattice of hydrogen atoms show this clearly. The variation of critical density with uniaxial stress in doped Si and Ge is in agreement with calculations based on impurity band wavefunctions . Local moments are known to dominate the low temperature behavior in doped semiconductors well into the metallic phase, and the effect is enhanced for compensated systems. Raman measurements in doped Si and infrared spectra in GaAs also show features in the metallic phase characteristic of the impurity wavefunction.

Ferromagnetism is found in Ga1-xMnxAs not far from a MIT, with insulating behavior seen both at low and high Mn concentration . Further, the system is heavily compensated  with a carrier density only around 10% the Mn density. (Mn is nominally an acceptor in GaAs and is expected to donate one hole per Mn). The vicinity of the MIT, and the large compensation, which implies large disorder, motivate studying a model that takes into account disorder as well as the impurity potential at the outset, to see what their effects are on the magnetic properties of the system.

Given the added complications of disorder, we study a model based on an impurity band of hydrogenic centers with spin-1/2 (instead of the more complex s=3/2 wavefunctions appropriate for acceptors), coupled to localized Mn d-electrons in their S=5/2 ground state. The s=3/2 case, while technically more complicated, should yield qualitatively similar conclusions. The impurity band is described in terms of a tight binding Hamiltonian of the ground state impurity wavefunctions at the impurity sites, which are distributed randomly on the Ga sites. As in previous work , the carriers are coupled to the Mn spins by an antiferromagnetic (AFM) Heisenberg exchange interaction. The Hamiltonian we study is thus:

$``$ $`=`$ $`{\displaystyle \underset{i,j}{}}t_{ij}c_{i\sigma }^{}c_{j\sigma }+{\displaystyle \underset{i,j}{}}J_{ij}\stackrel{}{S}(i)\left(c_{j\alpha }^{}{\displaystyle \frac{1}{2}}\stackrel{}{\sigma }_{\alpha \beta }c_{j\beta }\right)`$ (1)
$``$ $`g\mu _BH{\displaystyle \underset{i}{}}{\displaystyle \frac{\sigma }{2}}c_{i\sigma }^{}c_{i\sigma }\stackrel{~}{g}\mu _BH{\displaystyle \underset{i}{}}S^z(i)`$ (2)
Here, $`\stackrel{}{R}_i`$ ($`i=1,N_d`$) denotes the random positions of the Mn impurities, and $`c_{i\sigma }^{}`$ is the creation operator of a hole with spin $`\sigma `$ in the bound state associated with the $`i`$th Mn impurity. The first term in Eq. (1) describes the hopping of holes between various site, with the hopping matrix $`t_{ij}=t(|\stackrel{}{R}_i\stackrel{}{R}_j|)`$ given by $`t(r)=2\left(1+r/a_B\right)\mathrm{exp}(r/a_B)\text{Ry}`$ , where the Ry is the binding energy of the hole, $`E_b`$, and $`a_B=ϵ\mathrm{}^2/m^{}e^2`$ is the hydrogenic Bohr radius. The second term is the AFM interaction between Mn spins $`\stackrel{}{S}(i)`$ and hole spins. Since Mn spins are strongly localized, the exchange integral is simply given by $`J_{ij}=J\mathrm{exp}(2|\stackrel{}{R}_i\stackrel{}{R}_j|/a_B),`$ reflecting the probability of finding the hole in the impurity state around $`j`$ on the $`i`$th Mn spin. The last line in Eq. (1) describes interactions with an external magnetic field H.

We study finite size lattices containing $`L^3`$ simple cubic unit cells (lattice constant $`a`$) of the zinc-blende structure. $`N_d`$ of the Ga FCC sublattice are substituted at random by Mn, leading to a Mn concentration $`n_{Mn}=4x/a^3`$, where $`x=N_d/4L^3`$. The total number of holes is $`N_h=pN_d`$, implying a hole concentration $`n_h=pn_{Mn}`$. In all simulations presented in this paper we choose $`L`$ such that for the corresponding $`x`$ and $`p`$, we have $`N_h>50`$ and $`N_d>500`$, so as to minimize finite size effects. Thus, in the absence of external magnetic fields, the problem can be scaled in terms of four dimensionless parameters: $`J/E_b`$, $`a_B/a`$, $`n_ha_B^3`$ and $`x`$.

In this paper, we use parameters believed to be appropriate for Ga1-xMnxAs: lattice constant $`a=5.65\AA `$, hole binding energy $`E_b=112.4`$ meV=1Ry , with a consequent Bohr radius (in our model) of $`a_B=7.8\AA `$, and an exchange integral $`J=15`$ meV. Typical values of the Mn and hole concentrations are $`x=0.010.05`$ and $`p=510\%`$ . A more comprehensive study, including a number of effects left out of this model, is being completed. With these parameters, the typical hopping parameter is $`t(4a_B)=20`$meV, though it should be emphasized that $`t_{ij}`$ are distributed over a wide range.

We treat the AFM interaction within the mean-field approximation (MFA), which leads to the replacement $`\stackrel{}{S}(i)\widehat{\stackrel{}{s}}_j\stackrel{}{S}(i)\widehat{\stackrel{}{s}}_j+\stackrel{}{S}(i)\widehat{\stackrel{}{s}}_j\stackrel{}{S}(i)\widehat{\stackrel{}{s}}_j`$, where $`\widehat{\stackrel{}{s}}_j=c_{j\alpha }^{}\frac{1}{2}\stackrel{}{\sigma }_{\alpha \beta }c_{j\beta }`$. The charge carrier Hamiltonian now contains the hopping term and an effective on-site interaction $`_jϵ_{\alpha \beta }(j)c_{j\alpha }^{}c_{j\beta }`$, with $`ϵ_{\alpha \beta }(j)=\frac{1}{2}_iJ_{ij}\stackrel{}{\sigma }_{\alpha \beta }\stackrel{}{S}(i)`$, and can be numerically diagonalized for any configuration $`\stackrel{}{S}(i)`$ of the Mn spins, allowing the calculation of the charge carrier spin expectation values $`\widehat{\stackrel{}{s}}_j`$. In turn, these allow us to compute the new expectation values for the Mn spins, $`|\stackrel{}{S}(i)|=_S(\beta H_i),\stackrel{}{S}(i)\stackrel{}{H}_i`$, where $`\stackrel{}{H}_i=_jJ_{ij}\widehat{\stackrel{}{s}}_j`$ and $`_S(x)`$ is the Brillouin function.

The process is repeated until self-consistency is reached at each site . As usual in MFA, the symmetry to spin rotations is spontaneously broken and the expectation values are non-zero for some direction, which we choose

as the z-axis (this is equivalent to having an infinitesimally small magnetic field). The average contributions to the total magnetization of the Mn and hole spins are then proportional to $`S_{Mn}=1/N_d_iS^z(i)`$ and $`s_h=1/N_h_i\widehat{s}_i^z`$. As might be expected, below a temperature $`T_c`$, the system develops non zero expectation values for the Mn and hole magnetizations, through hole-induced alignment of the Mn spins. In Fig.1 we show the average Mn and hole spins as a function of temperature, $`T`$, for a system with $`x=0.00926`$ and $`p=10\%`$, for a typical random Mn distribution (full lines). For comparison, we also show the corresponding results (dashed lines) for a system with the same Mn concentration, but with Mn ions arranged on a simple cubic lattice, with a (super)lattice constant $`a_L=a/(4x)^{1/3}=3a`$. Due to their AFM interaction, the two expectation values have opposite signs, with the Mn spin saturating at $`\frac{5}{2}`$ and the hole spin saturating at $`\frac{1}{2}`$ at low temperatures. (The total magnetization $`M(T)`$ of the system has a T-dependence similar to that of $`S_{Mn}`$, since Mn spins outnumber holes ten to one, and also have a higher moment).

The first observation is that the magnetization of the disordered system does not have the Brillouin-function shape typical for uniform ferromagnets. This is in part due to the small carrier density relative to the Mn spin density; however, an even greater effect comes from the wide distribution of exchange couplings and hopping integrals, because of which many Mn spins do not order down to extremely low T. This is made clear in the inset for Fig.1, which compares the specific heat for the two configurations on a logarithmic scale for T: the disordered case shows a pronounced peak at temperatures well below $`T_c`$, and significantly below its lattice counterpart. Further, we find that the average Mn moment at $`T=0.2T_c`$ is well below the saturation value of 5/2, in accord with experimental data , but in contrast with results obtained from homogeneous electron gas models.

A second, surprising result is that randomness in the Mn positions leads to a significant increase in $`T_c`$. This is because, in the disordered system, holes prefer regions of higher local concentration of Mn, where they lower their total (magnetic and kinetic) energy, by polarizing the Mn spins and hopping among several nearby Mn sites. As a result, these regions of higher Mn concentration become spin-polarized at higher temperatures than in the uniform system, and the resultant $`T_c`$ is increased. This is similar to a percolation-like situation. We caution that this increase may be significantly overestimated in a MFA such as ours, since spin fluctuations between weakly coupled polarized clusters are not treated accurately.

On the other hand, in a disordered system, the lower density Mn regions have a lower than average probability to be visited by the holes, and as a result the Mn spins in these regions only align ferromagnetically at extremely low temperatures (see Fig.1); such an effect is probably well captured by our scheme. We would like to emphasize the fact that the holes at the Fermi energy at the densities studied are either itinerant, or close to being so. An analysis of hole wave-functions shows this delocalization, along with the higher weight of holes in the regions of high Mn concentration. This delocalization is responsible for alignment of the polarization at these high temperatures (relative to the insulating system). Holes traveling between various high-density regions force the alignment of Mn spins in each region to be the same, in order to minimize their kinetic energy.

This picture can be checked by “tuning” the amount of disorder (randomness) in the Mn positions. In Fig.2 we show the average hole and Mn spins curves, for four types of Mn distributions, with $`x=0.00926`$ and $`p=10\%`$. In order of increasing $`T_c`$, they are: (a) an ordered Mn cubic superlattice; (b) weak disorder, corresponding to randomly displacing each Mn in (a) to one of the 12 nearest neighbor sites of the underlying FCC sublattice;

(c) moderate disorder, corresponding to a random distribution of Mn on the FCC sublattice, subject to a constraint that all Mn-Mn distances are greater than $`2a`$; (d) completely random distribution of Mn on the FCC sublattice. With increasing randomness, $`T_c`$ increases, while saturation of $`M(T)`$ is simultaneously pushed to lower $`T`$. The sensitivity to disorder suggests that carrier density is not the only parameter characterizing the ferromagnetic behavior in DMS; indeed, since original submission of this manuscript, changes in M(T) curves with annealing time have been seen experimentally.

We find a qualitatively similar picture holds for higher Mn concentrations as well as higher hole densities, though the effects are quantitatively less. (Our model, which does not include band states, is likely to be less accurate at high densities). In Fig. 3 we show the Mn and hole spins for both the simple cubic superlattice and the random Mn distribution on the FCC sublattice for $`x=0.05`$ for two different $`p`$. While $`T_c`$ is again larger in the random system in MFA, the percentage increase is smaller than in the $`x=0.00926`$ case. Increasing the hole concentration from $`p=10\%`$ to $`p=30\%`$ makes the curves more Brillouin-like. This is because the fluctuations in the local doping are smaller at higher Mn concentrations, and increased hole doping further reduces the width of the exchange distribution.

Our model, being based on the low doping limit, likely overestimates the role of disorder; however, because ferromagnetism in DMS is seen at low doping densities, not too far from the metal-insulator transition, our work does strongly suggest that models based on the homogeneous electron gas (whether mean-field, or with perturbative RKKY exchange) will not correctly capture the nature of ferromagnetism. In particular, it casts doubt on their quantitative fits to the observed $`T_c`$ in Ga1-xMnxAs. Our calculation, while including the random positions of the Mn dopants, leaves out disorder effects due to compensation, as well as fluctuation effects left out in the MFA. At higher Mn concentrations, direct Mn-Mn interactions (which are needed to account for spin-glass like behavior seen in many II-VI DMS above 20% Mn) become important, while for higher hole concentrations, one may have to include the band states in addition to the impurity band, and possibly Coulomb interactions between carriers as well. While these will have quantitative effects on the results, the unusual shape of the magnetization curve and thermodynamic properties is likely to remain at low doping, judging from the results of numerical Monte Carlo simulations for the insulating phase of doped DMS. Local experimental probes such as ESR and NMR would be especially valuable in ascertaining any inhomogeneities in the magnetization and carrier density profile, and help uncover the nature of ferromagnetism in doped DMS at these low carrier densities.

In conclusion, the nature of ferromagnetism in doped DMS for low doping, not too far above the metal-insulator transition density, is strongly affected by disorder, which may, surprisingly, aid higher $`T_c`$ in this regime. Further, by appropriate tuning of various parameters, one may tailor the magnetic behavior M(H,T) in a manner not possible in simple uniform magnets. This versatility makes DMS ferromagnetism near the MIT a very interesting problem from a theoretical point of view. Adding to the richness are possible effects of direct Mn-Mn interactions in concentrated systems (which lead to spin-glass behavior in undoped II-VI DMS), the existence of a ferromagnetic metal-insulator transition (unlike conventional doped semiconductors and amorphous alloys), and the likely unusual electron and spin transport characteristics because of disorder.

This research was supported by NSF DMR-9809483. M.B. acknowledges support from NSERC, Canada. R.N.B. acknowledges the hospitality of the Isaac Newton Institute for Mathematical Sciences and of the Aspen Center for Physics while this research was ongoing.


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# Branch points in the complex plane and information loss in quantum systems at high level density

## I Introduction

Recently, the generic properties of many-body quantum systems are studied with a renewed interest. They are expressed mostly by their statistical properties, i.e. by comparing their level distributions with those following from random matrix ensembles. The generic properties are, as a rule, well expressed in the center of the spectra where the level density is high. As an example, the statistical properties of the shell-model states of nuclei around 24Mg are studied a few years ago  by using two-body forces which are obtained by fitting the low-lying states of different nuclei of the $`2s1d`$ shell. In the center of the spectra, the generic properties are well expressed in spite of the two-body character of the forces used in the calculations.

A surprising result is obtained recently in performing shell-model calculations for the same systems with random two-body forces. In spite of the random character of the forces, the regular properties of the low-lying states are described quite well  in these calculations. Further studies  proved the relevance of the results obtained and could explain in detail even the regular properties at the border of the spectra obtained from random two-body forces . Thus, generic properties of the spectra may arise from two-body forces, while regular properties may be described by means of random forces. This contra-intuitive result is, at present, not fully understood.

The spectra of microwave cavities are not determined by two-body forces. Nevertheless, the calculated spectra are similar to those from nuclear reactions . They show deviations from the spectra obtained from random matrix theory as well as similarities with them. The theoretical results obtained are confirmed by experimental studies . Most interesting are, however, the results of an analysis of the statistical properties of the city transport in Cuernavaca (Mexico). It is shown in  that the subsequent bus arrivals display probability distributions conforming to those given by the unitary ensemble of random matrices.

By all these studies, the question on the origin of the generic properties of many-body quantum systems, observed at high level density, is raised anew. As a result of these studies, neither two-body forces nor quantum effects are decisive. The study of the city transport in Mexico can be understood as an equilibrium state of an interacting one-dimensional gas under the assumption that the information contained in the positions of the individual gas particles is minimized . The minimum information is caused obviously by some information exchange with the environment.

Quantum systems having discrete states seem to exist isolated from an environment. It is therefore an interesting question whether or not some information exchange with the environment can, nevertheless, take place and provide a certain loss of information on the individual properties of the states.

The effect of avoided level crossing (Landau-Zener effect) is known and studied theoretically as well as experimentally for many years. It is a quite general property of the discrete states of a quantum system whose energies will never cross when there is a certain non-vanishing interaction between them. Instead, they avoid crossing in energy and their wave functions are exchanged when traced as a function of a certain tuning parameter. The avoided level crossings are related to the existence of exceptional points . The relation of these points to geometrical phases is studied experimentally  as well as theoretically  in a microwave resonator by deforming it cyclically. The results show non-trivial phase changes when degeneracies appear near to one another . The influence of level crossings in the complex plane onto the spectra of atoms is studied in . In this case, the crossings are called hidden crossings .

Usually, it is assumed that avoided level crossings do not introduce any correlations between the wave functions of the states as long as the system parameter is different from the critical one at which the two states avoided crossing. Counter-examples have been found, however, in recent numerical studies of the spectra of microwave cavities . The introduced correlations are traced back to branch points in the complex plane  which are the crossing points of the states when continued into the complex plane.

If it is really a general phenomenon that branch points in the complex plane introduce correlations between discrete states of a closed quantum system, then an information exchange with the environment would take place also in quantum systems. This fact could support the analogy of the statistical properties of the city transport to those of quantum systems and, above all, the interpretation of the statistical properties given in .

It is the aim of the present paper to study in detail the correlations in a quantum system which are introduced by branch points in the complex plane. First, the properties of the states of an open quantum system in the very neighbourhood of a branch point will be studied. In such a case, the $`S`$ matrix has a double pole and the interaction between the two states is maximum. The double pole coincides with the branch point in the complex plane. It is shown further, that the branch point influences the properties of the resonance states not only when the physical conditions for a double pole of the $`S`$ matrix are fulfilled but also when the states avoid crossing. This result corresponds to those obtained for the realistic case of laser induced continuum structures in atoms . The influence of the branch points is accompanied, in any case, by an exchange of the wave functions of the states.

The properties of resonance states in the neighbourhood of an avoided crossing are traced in the further studies of the present paper. More exactly: starting from the branch point where two resonance states with given widths $`\gamma _1^{\mathrm{cr}}`$ and $`\gamma _2^{\mathrm{cr}}`$ cross, the properties of two other states with $`\gamma _i`$ smaller or larger $`\gamma _i^{\mathrm{cr}}`$ are studied. For these two states, the physical conditions for the formation of a double pole of the $`S`$ matrix are not fulfilled. Finally, the $`\gamma _i`$ are chosen to be zero. This study allows to compare the properties of resonance states with finite lifetime with those of discrete states under the influence of a branch point in the complex plane. The results show how the branch points in the complex plane continue analytically into the function space of discrete states.

The paper is organized as follows. In section 2, the mathematical properties of branch points in the complex plane and their relation to avoided level crossings are sketched. In section 3, numerical results for states at a double pole of the $`S`$ matrix as well as for states with avoided crossing are given. The main point studied are the correlations of the wave functions introduced by an avoided level crossing. The results are discussed in the last section. They show that some information loss appears in quantum systems at high level density under the influence of the branch points in the complex plane. The information contained in the positions and wave functions of the individual states of the system is minimized in a similar manner as in the city transport in Mexico.

## II Branch points in the complex plane

The avoided crossing of discrete levels is related to the existence of branch points in the complex plane. In order to illustrate this relation, let us study the properties of the complex two-by-two Hamiltonian matrix

$`=\left(\begin{array}{cc}e_1(a)& 0\\ 0& e_2(a)\end{array}\right)\left(\begin{array}{cc}\frac{i}{2}\gamma _1(a)& \omega \\ \omega & \frac{i}{2}\gamma _2(a)\end{array}\right).`$ (5)
The unperturbed energies $`e_i`$ and widths $`\gamma _i`$ ($`i=1,2`$) of the two states depend on the parameter $`a`$ to be tuned in such a manner that the two states may cross in energy (and/or width) when $`\omega =0`$. The two states interact only via the non-diagonal matrix elements $`\omega `$ which may be complex, in general. The imaginary part of $`\omega `$ arises from the residuum of the integral describing the interaction via the continuum of decay channels, see e.g. . The real part contains both the direct interaction of the two states and the principal value integral which appears from the interaction via the continuum. In the following, we consider only real $`\omega `$ (and $`\gamma _i`$ independent of $`a`$) since we are interested in the influence of the branch points onto the avoided crossing of discrete states. The influence of complex $`\omega `$ on the crossing of resonance states will be considered in a forthcoming paper.

The eigenvalues of $``$ are

$$_\pm E_\pm \frac{i}{2}\mathrm{\Gamma }_\pm =\frac{ϵ_1+ϵ_2}{2}\pm \frac{1}{2}\sqrt{(ϵ_1ϵ_2)^2+4\omega ^2}$$
(6)
with $`ϵ_je_j\frac{i}{2}\gamma _j(j=1,2)`$. According to equation (6), two interacting discrete states (with $`\gamma _i=0`$) avoid always crossing since $`\omega `$ is real in this case. It is, however, possible to find the corresponding crossing point in the complex plane by considering non-vanishing values $`g_i`$ instead of the $`\gamma _i`$. Both, the $`g_i`$ and the $`\gamma _i`$, are proportional to the spectroscopic factors . The common energy dependent factor in the $`\gamma _i`$ causes $`\gamma _i0`$ in approaching the decay threshold where the resonance states become discrete. The common energy dependent factor in the $`g_i`$ is different from zero also for discrete states. The $`g_i`$ describe the transfer probability between different states.

It can further be seen from equation (6) that these crossing points are branch points in the complex plane. Equation (6) shows also that resonance states with non-vanishing widths $`\gamma _i`$ avoid mostly crossing since $`F(a,\omega )(ϵ_1ϵ_2)^2+4\omega ^2`$ is different from zero for all $`a`$, as a rule. Only when $`F(a,\omega )=0`$ at $`a=a^{\mathrm{cr}}`$ (and $`\omega =\omega ^{\mathrm{cr}}`$), the states cross. In such a case, the $`S`$ matrix has a double pole, see e.g. . Note that the branch point is determined by the values $`(\omega )^2`$ and $`(ϵ_1ϵ_2)^2`$ but not by the signs of these values. According to equation (6), it lies at $`X(1/2)\{ϵ_1(a^{\mathrm{cr}})+ϵ_2(a^{\mathrm{cr}})\}`$.

The left and right eigenfunctions, $`\mathrm{\Phi }_i^{\mathrm{lt}}`$ and $`\mathrm{\Phi }_i^{\mathrm{rt}}`$ ($`i=\pm `$), of a non-Hermitian matrix are different from one another. Since the matrix (5) is symmetrical, it follows

$$\mathrm{\Phi }_i^{}|=\mathrm{\Phi }_i^{}|_i\mathrm{and}|\mathrm{\Phi }_i=_i|\mathrm{\Phi }_i,$$
(7)
see e.g. . Therefore, $`\mathrm{\Phi }_i^{\mathrm{lt}}=\mathrm{\Phi }_i^{\mathrm{rt}}\mathrm{\Phi }_i^{}`$. The eigenfunctions of $``$ can be orthonormalized according to

$$\mathrm{\Phi }_i^{\mathrm{lt}}|\mathrm{\Phi }_j^{\mathrm{rt}}=\mathrm{\Phi }_i^{}|\mathrm{\Phi }_j=\delta _{ij}$$
(8)
where $`\mathrm{\Phi }_j^{\mathrm{rt}}\mathrm{\Phi }_j`$. Equation (8) provides the bi-orthogonality relations

$`\mathrm{\Phi }_i|\mathrm{\Phi }_i=\mathrm{}(\mathrm{\Phi }_i|\mathrm{\Phi }_i)=\mathrm{\Phi }_j|\mathrm{\Phi }_j`$ ; $`A\mathrm{\Phi }_i|\mathrm{\Phi }_i1`$ (9)
$`\mathrm{\Phi }_i|\mathrm{\Phi }_{ji}=i\mathrm{}(\mathrm{\Phi }_i|\mathrm{\Phi }_{ji})=\mathrm{\Phi }_{ji}|\mathrm{\Phi }_i`$ ; $`B|\mathrm{\Phi }_i|\mathrm{\Phi }_{ji}|0.`$ (10)
At the double pole, $`|\mathrm{\Phi }_i|\mathrm{\Phi }_i|\mathrm{}`$ and $`|\mathrm{\Phi }_i|\mathrm{\Phi }_{ji}|\mathrm{}`$ but $`\mathrm{\Phi }_i^{}|\mathrm{\Phi }_j=\delta _{ij}`$ according to equation (8). Numerical examples for the values $`\mathrm{\Phi }_i|\mathrm{\Phi }_j`$ with $`i=j`$ as well as with $`ij`$ can be found in . Further, at the double pole the two wave functions are related by $`\mathrm{\Phi }_i=\pm i\mathrm{\Phi }_{ji}`$ .

The eigenfunctions $`\mathrm{\Phi }_i`$ can be represented in the set of basic wave functions $`\mathrm{\Phi }_i^0`$ of the unperturbed matrix corresponding to $`\omega =0`$,

$$\mathrm{\Phi }_i=b_{ij}\mathrm{\Phi }_j^0.$$
(11)
In the critical region of avoided crossing, the eigenfunctions are mixed: $`b_{ii}=b_{jj}`$ and $`b_{ij}=b_{ji}`$ for $`ij`$. The $`b_{ij}`$ are normalized according to equation (8).

## III Numerical results

The numerical results obtained by diagonalizing the matrix (5) are shown in figures 1 to 6. In all cases $`e_1=1a/2,e_2=a`$ and $`\omega =0.05`$. The $`\gamma _i`$ do not depend on the tuning parameter $`a`$. At $`a=a^{\mathrm{cr}}=2/3`$, the two levels cross when unperturbed (i.e. $`\omega =0`$) and avoid crossing, as a rule, when perturbed by the interaction $`\omega `$. When $`\gamma _1/2=\gamma _1^{\mathrm{cr}}/2=1.0,\gamma _2/2=\gamma _2^{\mathrm{cr}}/2=1.1`$, the $`S`$ matrix has a double pole meaning that the two resonance states cross in spite of $`\omega 0`$. According to equation (6), the double pole of the $`S`$ matrix is a branch point in the complex plane.

In figure 1, the energies $`E_\pm `$, widths $`\mathrm{\Gamma }_\pm `$ and wave functions $`b_{ij}`$ of the two states are shown as a function of the parameter $`a`$ in the very neighbourhood of the branch point. Approaching the branch point at $`a^{\mathrm{cr}}`$, $`|\mathrm{}(b_{ij})|\mathrm{}`$ and $`|\mathrm{}(b_{ij})|\mathrm{}`$. While $`\mathrm{}(b_{ij})`$ does not change its sign by crossing the critical value $`a^{\mathrm{cr}}`$, the phase of $`\mathrm{}(b_{ij})`$ jumps from $`\pm `$ to $``$. The orthogonality relations (8) are fulfilled for all $`a`$ including the critical value $`a^{\mathrm{cr}}`$.

Figure 2 shows the energies $`E_\pm `$ and widths $`\mathrm{\Gamma }_\pm `$ of the two states for values of $`\gamma _i`$ just above and below the critical ones $`\gamma _i^{\mathrm{cr}}`$ and for $`\gamma _i=0`$, i.e. for discrete states. When $`\gamma _i>\gamma _i^{\mathrm{cr}}`$, the widths of the two states approach each other near $`a^{\mathrm{cr}}`$ but the width of one of the states remains always larger than the width of the other one. The two states cross freely in energy, and the wave functions are not exchanged after crossing the critical value $`a^{\mathrm{cr}}`$.

The situation is completely different when $`\gamma _i<\gamma _i^{\mathrm{cr}}`$. In this case, the states avoid crossing in energy while their widths cross freely. After crossing the critical value $`a^{\mathrm{cr}}`$, the wave functions of the two states are exchanged. An exchange of the wave functions takes place also in the case of discrete states ($`\gamma _i=0`$). This latter result is well known as Landau-Zener effect. It is directly related to the branch point in the complex plane at $`a^{\mathrm{cr}}`$ as can be seen from figure 2.

The wave functions $`b_{ij}`$ are shown in figure 3. The states are mixed (i.e. $`|b_{ii}|1`$ and $`b_{iji}0`$) in all cases in the neighbourhood of $`a^{\mathrm{cr}}`$. In the case without exchange of the wave functions, $`\mathrm{}(b_{ij})`$ as well as $`\mathrm{}(b_{ij})`$ behave smoothly at $`a^{\mathrm{cr}}`$ while this is true only for $`\mathrm{}(b_{ij})`$ in the case with exchange of the wave functions. In this case, $`\mathrm{}(b_{ij})`$ jumps from a certain finite value $`y`$ to $`y`$ at $`a^{\mathrm{cr}}`$. The $`\mathrm{}(b_{ij})`$ of discrete states are zero. Thus, a jump in the $`\mathrm{}(b_{ij})`$ can not appear. The $`\mathrm{}(b_{ij})`$, however, show a dependence on $`a`$ which is very similar to that of resonance states with exchange of the wave functions ($`\gamma _i<\gamma _i^{\mathrm{cr}}`$).

In order to trace the influence of the branch point in the complex plane onto the correlations of discrete states, the differences $`\delta =|b_{ii}|^2|b_{iji}|^2`$ and the values $`|b_{ij}|^2`$ are shown in figures 4 and 5 for different values $`\gamma _i`$ from $`\gamma _i>\gamma _i^{\mathrm{cr}}`$ to $`\gamma _i=0`$. Most interesting is the change of the value $`\delta `$ from 1 to 0 at $`\gamma _i^{\mathrm{cr}}`$. The relation $`|b_{ii}|^2=|b_{iji}|^2`$ at $`\gamma <\gamma _i^{\mathrm{cr}}`$ is the result from interference processes. It holds also at $`\gamma _i=0`$, i.e. for discrete states. In this case, $`|b_{ii}|^2=|b_{iji}|^2=0.5`$ at $`a^{\mathrm{cr}}`$.

The values $`A`$ and $`B`$ characterizing the bi-orthogonality of the two wave functions are shown in figure 6 for the same values of $`\gamma _i`$ as in figures 4 and 5. The $`A`$ and $`B`$ are similar for $`\gamma _i\gamma _i^{\mathrm{cr}}=\pm \mathrm{\Delta }`$ as long as $`\mathrm{\Delta }`$ is small. They approach $`A1`$ and $`B0`$ for $`\gamma _i0`$.

In figure 7, the energies $`E_i`$ and mixing coefficients $`|b_{ij}|^2`$ are shown for illustration for four discrete states with three neighboured avoided crossings as a function of $`a`$. In analogy to (5), the matrix is

$`^{(4)}=\left(\begin{array}{cccc}e_1(a)& 0& 0& 0\\ 0& e_2(a)& 0& 0\\ 0& 0& e_3(a)& 0\\ 0& 0& 0& e_4(a)\end{array}\right)\left(\begin{array}{cccc}0& \omega _{12}& \omega _{13}& \omega _{14}\\ \omega _{21}& 0& \omega _{23}& \omega _{24}\\ \omega _{31}& \omega _{32}& 0& \omega _{34}\\ \omega _{41}& \omega _{42}& \omega _{43}& 0\end{array}\right).`$ (20)
The correlations introduced by the avoided crossings remain at all values of the parameter $`a`$ at high level density. They are the result of complicated interference processes. This can be seen best by comparing the two pictures with four interacting states (top and middle in figure 7) with those of only two interacting states (bottom of figure 7 and bottom right of figure 5). Figure 7 bottom shows the large region of the $`a`$ values around $`a^{\mathrm{cr}}`$ for which the two wave functions remain mixed: $`|b_{ii}|^21`$ and $`|b_{iji}|^20`$ for $`aa^l`$ with $`|a^la_{34}^{\mathrm{cr}}||a_{i4}^{\mathrm{cr}}a_{34}^{\mathrm{cr}}|;i=1,2`$. The avoided crossings between neighboured states do, therefore, not occur between states with pure wave functions and it is impossible to identify the $`|b_{ij}|^2`$ unequivocally (figure 7 right top and middle).

## IV Discussion of the results

Most calculations represented in the present paper are performed for two states which cross or avoid crossing under the influence of an interaction $`\omega `$ which is real. A general feature appearing in all the results is the repulsion of the levels in energy (except in the very neighbourhood of $`a^{\mathrm{cr}}`$ when $`\gamma _i\gamma _i^{\mathrm{cr}}`$). This result follows analyically from the eigenvalue equation (6). It holds quite generally for real $`\omega `$ as discussed by means of the spectra of microwave cavities  and laser-induced continuum structures in atoms . The level repulsion in energy is accompanied by an approaching of the lifetimes (widths) of the states.

The value $`a^{\mathrm{cr}}`$ is determined by the free crossing in energy of the two non-interacting states $`\mathrm{\Phi }_i^0`$ (corresponding to $`\omega =0`$) in the cases considered. The avoided level crossing at the critical value $`a^{\mathrm{cr}}`$ can be seen clearly only when the interaction $`\omega `$ is small. For larger $`\omega `$, the avoided crossings are washed out and are difficult to identify without performing a detailed analysis of the data. As a consequence, there are much more avoided level crossings in quantum systems at high level density than usually believed and the influence of the branch points may be quite important. The last point does not coincide with any intuitive assumptions.

The value of the (real) interaction $`\omega `$ in relation to the value of the widths $`\gamma _i`$ is decisive whether or not the states will be exchanged at the critical value $`a^{\mathrm{cr}}`$ of the tuning parameter, i.e. whether or not the states avoid crossing. When $`\omega `$ is so small that the difference of the widths $`\mathrm{\Gamma }_+\mathrm{\Gamma }_{}`$ is different from zero at $`a^{\mathrm{cr}}`$ then the states will not be exchanged. If, however, $`\mathrm{\Gamma }_+=\mathrm{\Gamma }_{}`$ at $`a^{\mathrm{cr}}`$, the states will be exchanged. The exchange occurs due to interferences between the different components of the wave functions. This can be seen best for resonance states with $`\gamma _i0`$ where interferences between the real and imaginary parts of the wave functions play an important role (see figure 5).

At the double pole of the $`S`$ matrix, not only $`\mathrm{\Gamma }_+=\mathrm{\Gamma }_{}`$ but also $`E_+=E_{}`$ for $`a^{\mathrm{cr}}`$. Here, the real and imaginary parts of all components of the wavefunctions increase boundless and $`\mathrm{\Phi }_i\pm i\mathrm{\Phi }_{ji}`$ . Avoided level crossings are characterized by $`E_+E_{}`$ at $`a^{\mathrm{cr}}`$. In these cases, the increase of the components of the wave functions at $`a^{\mathrm{cr}}`$ is reduced due to interferences. The interferences can be seen, e.g., from the differences $`\delta =|b_{ii}|^2|b_{iji}|^2`$ which jump from 1 to 0 at the branch point (see figure 4). This jump is related to the normalization condition (8) which is fulfilled also at the double pole of the $`S`$ matrix. The jump makes possible the exchange of the wave functions. The value $`\delta =0`$ remains when $`(\gamma _1/2\gamma _2/2)^2<4\omega ^2`$, i.e. also for discrete states.

The bi-orthogonality (10) of the wave functions characterizes the avoided crossing of resonance states. It increases boundless at the double pole of the $`S`$ matrix and vanishes in the case of an avoided crossing of discrete states (figure 6).

The results of all the calculations presented in the present paper show very clearly that, from a mathematical point of view, the branch points in the complex plane continue analytically into the function space of discrete states. Their influence on the properties of discrete states cannot be neglected.

Another result of the present study is the influence of the branch points in the complex plane onto the purity of the wave functions $`\mathrm{\Phi }_\pm `$. At $`a^{\mathrm{cr}}`$, the wave functions are not only exchanged but become mixed. The mixing occurs not only at the critical point $`a^{\mathrm{cr}}`$ but in a certain region around $`a^{\mathrm{cr}}`$ when the crossing is avoided. This fact is important at high level density where, as a rule, an avoided crossing with another level appears before $`\mathrm{\Phi }_i\mathrm{\Phi }_j^0`$ is reached. As a result, all the wave functions of closely-lying states are strongly mixed, i.e. the states are strongly correlated at high level density (see figure 7).

The strong mixing of the wave functions of a quantum system at high level density means that the information on the individual properties of the states $`\mathrm{\Phi }_i^0`$ is lost. While the exchange of the wave functions itself is of no interest for a statistical consideration of the states, the accompanying correlation of the states is decisive for the statistics. This fact is discussed also in . As shown in the present paper, the correlation of the states may be traced back to the existence of branch points in the complex plane. The number of branch points in the complex plane is large at high level density. Therefore, the discrete states of quantum systems at high level density lose any information on their individual properties. That means, they contain minimum information.

Thus, there is an information exchange between a (closed) quantum system and the continuum due to the analyticity of the wave functions. The branch points in the complex plane are hidden crossings, indeed. They play an important role not only in atoms, as supposed in , but determine the properties of all quantum systems at high level density.

The loss of information on the properties of discrete states of a quantum system under the influence of branch points in the complex plane is in complete analogy to the conclusion drawn from the statistical properties of the city transport in Cuernavaca (Mexico) . Also in this case, an information exchange with the environment leads to an information loss in the system.

It follows further that the statistical properties of quantum systems at high level density are different from those at low level density. States at the border of the spectrum are almost not influenced by branch points in the complex plane since their number is small. There are almost no states which could cross or avoid crossing with others states. The properties of these states are expected therefore to show more individual features than those at high level density. In other words, the information on the individual properties of the states $`\mathrm{\Phi }_i^0`$ at the border of the spectrum is kept to a great deal in contrast to that on the states in the center of the spectrum.

Summarizing the results, it can be stated the following. Branch points in the complex plane cause an exchange of the wave functions and, above all, create correlations between the states of a quantum system at high level density even if the system is closed and the states are discrete. These correlations are equivalent to a loss of information on the individual basic states. This result may explain the similarity between the statistical properties of the city transport in Cuernavaca (Mexico) and those of a quantum system at high level density.

Acknowledgment: Valuable discussions with E. Persson, J.M. Rost, P. $`\stackrel{ˇ}{\mathrm{S}}`$eba and E.A. Solov’ev are gratefully acknowledged. I am indebted to M. Sieber for a critical reading of the manuscript.


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# Multi-particle States in Spin-1 Chain System 𝐂𝐬𝐍𝐢𝐂𝐥_𝟑

\[

## Abstract

A continuum of magnetic states has been observed by neutron scattering from the spin-1 chain compound $`\mathrm{CsNiCl}_3`$ in its disordered gapped one-dimensional phase. Results using both triple-axis and time-of-flight spectrometers show that around the antiferromagnetic point $`Q_\mathrm{c}=\pi `$, the continuum lies higher in energy than the Haldane gapped excitations. At $`6\mathrm{K}`$ the integrated intensity of the continuum is about 12(2)% of the total spectral weight. This result is considerably larger than the 1-3% weight predicted by the non-linear sigma model for the 3-particle continuum.

\]

The excitations of one-dimensional (1D) Heisenberg antiferromagnets have attracted much experimental and theoretical attention ever since Haldane  predicted that the excitations of integer spin and half-integer spin chains are different. Half-integer spin chains have no spin gap and exhibit a spinon continuum extending to zero energy . For integer-spin chains the spectrum is at low temperatures dominated by well-defined single particle excitations corresponding to a triplet of spin-1 particles that exhibit a large energy gap . These have been thoroughly studied by neutron scattering from spin-1 chain compounds and it has been shown that the well-defined excitations largely exhaust the total scattering . Nonetheless, a continuum of multi-particle scattering was predicted by Haldane and others , but as yet no experiment has established its existence. To search for such a continuum we have measured the inelastic neutron scattering of $`\mathrm{CsNiCl}_3`$ in its paramagnetic 1D phase using time-of-flight and triple-axis spectrometers. We find a neutron scattering continuum at energies higher than the well-defined single particle excitation, whose integrated intensity is bigger than predicted for the multi-particle scattering.

$`\mathrm{CsNiCl}_3`$ is magnetically a quasi 1D spin-1 chain compound with the Ni chains along the c-axis of the hexagonal unit cell. Each unit cell contains two Ni atoms and the Hamiltonian is

$$H=J\underset{i}{\overset{\mathrm{chain}}{}}\stackrel{}{S}_\mathrm{i}\stackrel{}{S}_{\mathrm{i}+1}+J^{}\underset{<i,j>}{\overset{\mathrm{plane}}{}}\stackrel{}{S}_\mathrm{i}\stackrel{}{S}_\mathrm{j}D\underset{i}{}(\stackrel{}{S_\mathrm{i}^z})^2.$$
(1)
The exchange interaction $`J=2.28\mathrm{meV}`$ along the $`c`$-axis is much stronger than the exchange interaction in the basal plane $`J^{}=0.044\mathrm{meV}`$ . The weak Ising anisotropy $`D=4\mu \mathrm{eV}`$ is small enough that $`\mathrm{CsNiCl}_3`$ is a good example of an isotropic Heisenberg antiferromagnet. Below $`T_\mathrm{N}=4.85\mathrm{K}`$ the interchain coupling causes long-range ordering of the magnetic moments. Above $`T_\mathrm{N}`$ $`\mathrm{CsNiCl}_3`$ is in a 1D magnetic phase for which the magnetic exchange interaction along the $`c`$-axis dominates the spin dynamics, except close to $`T_\mathrm{N}`$.

The sample of $`\mathrm{CsNiCl}_3`$ was a single crystal $`20\mathrm{mm}\times 5\mathrm{mm}\times 5\mathrm{mm}`$ and was mounted with its ($`hhl`$) crystallographic plane in the principal scattering plane. Inelastic neutron scattering experiments were carried out with the time-of-flight spectrometer, MARI, at the ISIS facility of the Rutherford Appleton Laboratory and with reactor-based triple-axis spectrometers, DUALSPEC at the Chalk River Laboratories and RITA at $`\mathrm{Ris}\mathrm{ø}`$ National Laboratory.

For the experiment using MARI the incoming neutron energy was $`20`$ and $`30\mathrm{meV}`$. The energy resolution was $`0.35`$ and $`0.4\mathrm{meV}`$, as determined from the full width at half maximum (FWHM) of the quasi-elastic peak. The resolution in wave-vector transfer at zero energy transfer was typically $`0.02\mathrm{\AA }^1`$ along the $`c^{}`$-axis and along the $`[110]`$ direction and up to $`0.19\mathrm{\AA }^1`$ perpendicular to the scattering plane if only the central detector bank was used. Both the energy and the wave-vector resolution improved with increasing energy transfer. The measurements were performed with the sample at temperatures between 6.2 and $`12\mathrm{K}`$.

The measurements at the DUALSPEC triple-axis spectrometer were performed at $`8.5\mathrm{K}`$ with a fixed scattered neutron energy of $`14.51\mathrm{meV}`$ and with a graphite filter to absorb the higher order reflections from the pyrolytic graphite monochromator and analyzer. The collimation from reactor to detector was $`0.65^\mathrm{o}`$-$`0.6^\mathrm{o}`$-$`1.4^\mathrm{o}`$-$`2.0^\mathrm{o}`$ and gave an energy resolution of $`1.94\mathrm{meV}`$, as determined from the quasi-elastic peak. In the case of the RITA triple-axis spectrometer, supermirror guides and a rotating velocity selector produced a variable energy monochromatic neutron beam with suppressed higher order contamination. The scattered neutrons were analyzed using the Soller geometry with a fixed energy of $`5\mathrm{meV}`$ and a cooled beryllium filter between the sample and analyzer. The effective collimation was $`1.45^\mathrm{o}`$-$`1.45^\mathrm{o}`$-$`1^\mathrm{o}`$-$`2.0^\mathrm{o}`$ and the energy resolution was $`0.35\mathrm{meV}`$ as determined from the quasi-elastic peak.

The measurements with MARI at temperatures between $`6.2`$ and $`12\mathrm{K}`$ were performed with the c-axis of the sample either perpendicular or parallel to the incoming beam. The dynamic structure factor $`S(\stackrel{}{Q},E)`$ was measured for wave-vector transfers along the c-axis between $`l0.175`$ and $`1.5`$, where the wave-vector along the chain is $`\frac{2\pi l}{c}`$. Because there are two Ni atoms in each unit cell along c, $`l=1`$ corresponds to the antiferromagnetic (AF) wave-vector, $`\pi `$, generally used in theoretical work on AF chains. The data with $`l>1.5`$ was contaminated by phonon scattering and so no analysis of the magnetic contribution was then attempted.

Constant-$`l`$ scans were constructed from the measured $`S(\stackrel{}{Q},E)`$ by mapping on ($`l,E`$)-space (Fig. 1). This data was then averaged in stripes with a width $`\mathrm{\Delta }l=0.050.10`$ and corrected for neutron absorption. Fig. 1 shows directly the continuum scattering. It is stronger at AF momenta around $`l=1`$ than in the region near $`l=0.2`$, which is known to carry vanishing magnetic weight , and the zone boundary region $`l=0.5`$ A detailed description of the analysis of the experiment will be given elsewhere . Here, we focus only on the scattering close to the AF point as measured in the central detector bank. As shown in Fig. 2a) the response at $`Q_\mathrm{c}=\pi `$ consists of the sharp mode observed previously but also has a component that extends to high frequencies. This continuous spectrum has not been observed before. It is well above background and moreover is seen to be much larger than the scattering near $`Q_\mathrm{c}=0`$ where the magnetic scattering is expected  to be vanishingly small. We will show below that the continuum cannot arise from resolution broadening of the well-defined mode.

The magnetic excitations in the MARI experiment were best fitted by an antisymmetrized Lorentzian peak weighted with the detailed balance factor and convoluted with the line-shape of the quasi-elastic incoherent scattering, which is a good estimate of the resolution line-shape particularly at low energy transfers. An intrinsic Lorentzian peak is supported by a recent theoretical prediction  and a recent experiment . It gives an excellent fit to the low energy resonant Haldane peak. Nevertheless we see in Fig. 2a) that the scattering intensity at energies above the gap energy is significantly higher than expected from the fits to the sharp peak. The continuum scattering is clearly observed for $`0.6<l<1.4`$ (Fig. 1). At $`6.2\mathrm{K}`$, the integrated intensity of the continuum is 10(4)% of the total magnetic scattering at the AF point. The continuum was also observed in an experiment in a different configuration at $`12\mathrm{K}`$, where the c-axis was parallel to the incoming beam.

Calculations were made using an ISIS spectrometer simulation programme which takes into account the spectrometer parameters such as the detailed pulse line-shape, chopper characteristics etc. and predicts the scattering line-shape for a particular sample orientation and model of the scattering cross-section. We find that the resolution function reproduced the measured line-shape of the quasi-elastic incoherent scattering and of the well-defined excitations, but that it cannot give rise to a high-energy tail in the region of the continuum.

The continuum scattering was investigated further using the triple-axis spectrometer DUALSPEC at Chalk River Laboratories and constant-$`\stackrel{}{Q}`$ scans were performed at $`8.5\mathrm{K}`$ for various wave-vectors in reciprocal space. The energy scans close to the AF point $`l=1`$ revealed considerable continuum scattering above the well-defined Haldane excitation. The continuum extends up to $`12\mathrm{meV}`$ as shown in Fig. 2b) for the energy scan at $`(\mathrm{0.31\hspace{0.33em}0.31\hspace{0.33em}1})`$. This wave-vector was chosen to be close to the 3D ordering wave-vector such that the Haldane excitation was at the lowest energy to give the largest possible energy window for the observation of the continuum. The scattering intensity at the AF zone boundary, $`l=1.5`$, below and above the sharp excitation is considerably lower than the intensity at $`l=1`$. The magnetic excitation was then fitted by a dispersion relation (an antisymmetrized Lorentzian weighted by the Bose factor) convoluted with the resolution ellipsoid given by Cooper-Nathans’s expression . The dispersion relation has been given by , and at $`6\mathrm{K}`$ the zone boundary energy is $`6\mathrm{meV}`$, the gap at $`(\mathrm{0.81\hspace{0.33em}0.81\hspace{0.33em}1})`$ is $`1.23\mathrm{meV}`$  and the bandwidth of the gap along $`[110]`$ direction is given by the gap at $`(\mathrm{0.33\hspace{0.33em}0.33\hspace{0.33em}1})`$, which is $`0.35\mathrm{meV}`$ . The Lorentzian half width of the excitation is $`0.35\mathrm{meV}`$ . The fit gives an excellent account of the right-hand-side of the peak, as shown in Fig. 2b), but it cannot explain the slowly decreasing scattering continuum at energies above $`4\mathrm{meV}`$.

The integrated intensity for the DUALSPEC data at the AF point $`l=1`$ was inferred by scaling the peak intensity for $`l=1.5`$ according to the $`l`$-dependence of the intensity measured by the MARI experiment. The integrated intensity of the continuum at $`8.5\mathrm{K}`$ is found to be about $`12(3)\%`$ of the overall scattering at the AF wave-vector. This confirms the results obtained using the MARI spectrometer.

The temperature dependence of the continuum scattering was further investigated using the RITA triple-axis spectrometer at $`\mathrm{Ris}\mathrm{ø}`$ and constant-$`\stackrel{}{Q}`$ scans were performed at the 1D point $`(\mathrm{0.81\hspace{0.33em}0.81\hspace{0.33em}1})`$. In Fig. 3 we show that the peak broadens and increases in energy with increasing temperature as reported elsewhere . The well-defined peak was well fitted by an antisymmetrized Lorentzian weighted by the Bose factor and convoluted with the resolution ellipsoid. The flat background was determined from the scattered intensity below $`25\mathrm{K}`$ at the highest energy transfers measured ($`E>12\mathrm{meV}`$), where the scattering was temperature independent and assumed to be non-magnetic. At low temperatures and energies higher than the well-defined peak energy, there was considerable continuum scattering (Fig. 3). After correction for neutron absorption, the total integrated intensity at $`6\mathrm{K}`$ and $`12\mathrm{K}`$ was about 14(3)% and 13(6)% of the integrated scattering at $`l=1`$, respectively. At higher temperatures, the Lorentzian peak increases in energy and broadens so that the continuum could not be clearly identified. Nevertheless there was more scattering around $`812\mathrm{meV}`$ energy transfer at $`6`$ and $`9\mathrm{K}`$ than at $`30\mathrm{K}`$ (see Fig. 3).

There are a number of theoretical predictions for the strength of a continuum at $`l=1`$. A numerical diagonalization of a spin-1 chain with $`N=20`$ sites and nearest-neighbor exchange interaction showed that at zero temperature the continuum above the Haldane excitation carries $`3\%`$ of the total weight . In the non-linear sigma model ($`\mathrm{NL}\sigma \mathrm{M}`$), a continuum arises from 3-particle scattering, and its integrated intensity is about $`2\%`$ of the spectral weight . If the coupling of the magnetic chain is taken into account via a Random Phase Approximation (RPA), the 3-particle scattering becomes dependent on the wave-vector transfer perpendicular to the 1D axis, but its integrated intensity remains between 0.5 and $`2.25\%`$ of the total spectral weight .

The portion of the intensity in the continuum scattering for $`\mathrm{CsNiCl}_3`$ is about $`12(2)\%`$ for $`l=1`$. Our measurements for $`\mathrm{CsNiCl}_3`$ show that the intensity between $`l=1`$ and $`l=1.5`$ reduces by a factor of $`5.4`$, which is substantially lower than the theoretical prediction of $`8.9`$. The absolute intensity of continuum scattering may therefore be only $`7(2)\%`$ of the theoretical predicted intensity, but this is nevertheless much greater than the theoretical predictions.

A considerably stronger 3-particle continuum of about 17% is predicted by the Majorana Fermion Theory (MFT), which describes 1D magnetic systems in terms of a perturbation theory about the Heisenberg point of a model with biquadratic interactions as strong as the bilinear exchange . It is unclear whether this model is applicable for $`\mathrm{CsNiCl}_3`$. Furthermore, no indication of the pronounced peak at four times the gap energy, which is predicted for this model, was found in our measurements. Finally the MFT results are not in agreement with the numerical calculations of Takahashi .

In order to confirm that the continuum scattering arises from 3-particle scattering as predicted by the $`\mathrm{NL}\sigma \mathrm{M}`$ we have searched for the onset of the continuum at $`3\mathrm{\Delta }`$ and for the pronounced maximum of the continuum at $`6\mathrm{\Delta }`$ as predicted by the $`\mathrm{NL}\sigma \mathrm{M}`$. With $`\mathrm{\Delta }=0.94\mathrm{meV}`$, our resolution is more than adequate to observe an increasing continuum intensity between $`3\mathrm{\Delta }=2.8\mathrm{meV}`$ and $`6\mathrm{\Delta }=5.6\mathrm{meV}`$, but instead the spectrum shows a steadily decreasing intensity (Fig. 2, 3). This may arise because the 3D interactions in $`\mathrm{CsNiCl}_3`$ cause a change in the excitation spectrum which is not properly taken into account via RPA and the pronounced maximum at $`6\mathrm{\Delta }`$ gets much broader as expected from kinematics. Possibly the effect can also account for the observed continuum intensity being higher than predicted for a 1D chain.

The observed continuum, Fig. 1, 2, 3, has intensity extending to approximately $`12\mathrm{meV}`$, which is twice the maximum 1-particle energy for $`\mathrm{CsNiCl}_3`$. Because similar measurements near $`l=0,2`$ show no evidence of scattering, we conclude that the continuum is strongest in a broad region where the AF fluctuations are largest. It is then possibly worth commenting that qualitatively the continuum scattering has features that are similar to the continuum found for $`S`$=$`1/2`$ systems (Fig. 1) .

It is clear that further theoretical work is needed to understand these results. It is unclear firstly whether a quantitative theory can be obtained from the 3-particle picture of the $`\mathrm{NL}\sigma \mathrm{M}`$ or whether it is more appropriate to use another development such as the MFT approximation  to the Heisenberg model with biquadratic exchange and secondly whether the form of the scattering depends on the inter-chain coupling or is characteristic of coupled chains.

In summary, we have measured the continuum scattering of the spin-1 chain compound $`\mathrm{CsNiCl}_3`$ in a broad region that favours antiferromagnetic fluctuations and shown that it is stronger than expected for an ideal spin-1 chain both from numerical diagonalization and field theoretical calculations involving the $`\mathrm{NL}\sigma \mathrm{M}`$. These results are presented as observations from experiment, and while we cannot explain them we hope that they will stimulate further theoretical work.

We would like to thank Z. Tun for his assistance and Ian Affleck and A. M. Tsvelik for helpful discussions. Financial support for the experiments was provided by the EPSRC, by the EU through its Large Installations Program and by the British Council-National Research Council Canada Program. ORNL is managed for the U.S. D.O.E. by UT-Battelle, LLC, under contract no. DE-AC05-00OR22725. One of the authors (M. K.) is supported by a TMR-fellowship from the Swiss National Science Foundation under contract no. 83EU-053223.


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# Comment on ‘Decomposition of pure states of a quantum register’

## I Decomposition of qubits and qu$`n`$its

Result of  is proved with using simplicial complexes, etc., but it can be shown also with less special constructions. Such simplification may be useful because it makes possible to apply similar construction not only for qubit spaces $`^2\mathrm{}^2`$, but also for ‘qu$`n`$it’ spaces $`^n\mathrm{}^n`$. Here is represented only short introduction to construction with arbitrary $`n`$, because the result is already known and described in .

The result of  is related with possibility of exclusion by local unitary transformations of $`l`$ terms with one ‘unit’ like $`|100\mathrm{}0`$, $`|010\mathrm{}0`$, etc., from general $`l`$-qubit state with $`2^l`$ terms.

To show it, let us consider some state $`|h=\alpha |00\mathrm{}0+\alpha _1|10\mathrm{}0+\mathrm{}`$, where $`\alpha `$ may be zero. It is possible with using a local unitary transformation in first qubit $`U_1:(\alpha ,\alpha _1)(\alpha ^{},0)`$ to produce state $`|h^{}=\alpha ^{}|00\mathrm{}0+0|10\mathrm{}0+\mathrm{}`$, where $`|\alpha ^{}|^2=|\alpha |^2+|\alpha _1|^2`$. Next, because $`|h^{}=\alpha ^{}|00\mathrm{}0+\alpha _2|01\mathrm{}0+\mathrm{}`$, it is possible to eliminate $`\alpha _2`$ by a local unitary transformation of second qubit and with $`l`$ similar steps we can produce some state $`|h^{(1)}`$. If $`|h`$ is product state, then $`|h^{(1)}`$ has only one nonzero term, but in general case it is possible to produce sum with no more than $`2^ll`$ terms only by iterating the process: $`|\stackrel{~}{h}=lim_N\mathrm{}|h^{(N)}`$.

To check convergence let us consider a slightly different algorithm, when $`N`$’th step is elimination of term with one unit in position $`i_N`$ where coefficient $`\alpha _{i_N}^{(N)}=\alpha _{\mathrm{max}}^{(N)}`$ is maximal between $`l`$ similar terms. Absolute value of coefficient $`\alpha ^{(N)}`$ of term $`|00\mathrm{}0`$ is always limited $`|\alpha ^{(N)}||h|1`$ and meets an equation: $`|\alpha ^{(N)}|^2=|\alpha |^2+_{K=1}^N|\alpha _{\mathrm{max}}^{(K)}|^2`$. So $`_{N=1}^{\mathrm{}}|\alpha _{\mathrm{max}}^{(N)}|^2=|\stackrel{~}{\alpha }|^2|\alpha |^2`$ and then $`\underset{N\mathrm{}}{lim}\alpha _{\mathrm{max}}^{(N)}=0`$.

To generalize the method to arbitrary $`n>2`$ (‘qu$`n`$it’ ) let us consider first $`n=3`$ (‘qutrit’ ). If we start with some state $`|h=\alpha |00\mathrm{}0+\alpha _1|10\mathrm{}0+\beta _1|20\mathrm{}0+\mathrm{}`$, it is possible with using a local unitary $`SU(3)`$ transformation in first qutrit $`U_1:(\alpha ,\alpha _1,\beta _1)(\alpha ^{},0,0)`$ to produce state $`|h^{}=\alpha ^{}|00\mathrm{}0+0|10\mathrm{}0+0|20\mathrm{}0+\mathrm{}`$ with $`|\alpha ^{}|^2=|\alpha |^2+|\alpha _1|^2+|\beta _1|^2`$ and algorithms similar with discussed above may eliminate $`2l`$ components with one ‘1’ or ‘2’ and $`l1`$ ‘0’.

But in the case it is not all components appropriate for exclusion. Let us write state $`|g`$ without the $`2l`$ term as: $`|g=\gamma |11\mathrm{}1+\gamma _1|21\mathrm{}1+\mathrm{}`$. Because it is possible to transform qutrit space without change of component $`|0`$, i.e., $`U_1:(\alpha ,\gamma ,\gamma _1)(\alpha ,\gamma ^{},0)`$ we can exclude all $`l`$ components with one ‘2’ and $`l1`$ ‘1’ and so it is possible to have no more than $`3^l3l`$ components.

The similar process is possible to apply to arbitrary qu$`n`$it $`^n`$. First, we can exclude $`(n1)l`$ terms with one ‘1’ and $`l1`$ ‘0’. Second, $`(n2)l`$ terms with one ‘2’ and $`l1`$ ‘1’. After $`n1`$ iterations we can neglect $`((n1)+(n2)+\mathrm{}+1)l=n(n1)l/2`$ terms and so we have no more than

$$n^l\frac{1}{/}2n(n1)l$$

components. For $`l=2`$ we have $`n^2n(n1)2/2=n`$ terms of usual Schmidt decomposition.

## Acknowledgements

Author is grateful to R. Zapatrin and C. Zalka for explanations and comments. Many thanks to A. Sudbery for reference to the work .