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# Quantum effects in the collective light scattering by coherent atomic recoil in a Bose-Einstein condensate

## Abstract

We extend the semiclassical model of the collective atomic recoil laser (CARL) to include the quantum mechanical description of the center-of-mass motion of the atoms in a Bose-Einstein condensate (BEC). We show that when the average atomic momentum is less than the recoil momentum $`\mathrm{}\stackrel{}{q}`$, the CARL equations reduce to the Maxwell-Bloch equations for two momentum levels. In the conservative regime (no radiation losses), the quantum model depends on a single collective parameter, $`\rho `$, that can be interpreted as the average number of photons scattered per atom in the classical limit. When $`\rho 1`$, the semiclassical CARL regime is recovered, with many momentum levels populated at saturation. On the contrary, when $`\rho 1`$, the average momentum oscillates between zero and $`\mathrm{}\stackrel{}{q}`$, and a periodic train of $`2\pi `$ hyperbolic secant pulses is emitted. In the dissipative regime (large radiation losses) and in a suitable quantum limit, a sequential superfluorescence scattering occurs, in which after each process atoms emit a $`\pi `$ hyperbolic secant pulse and populate a lower momentum state. These results describe the regular arrangement of the momentum pattern observed in recent experiments of superradiant Rayleigh scattering from a BEC.

PACS numbers: 42.50.Fx, 42.50.Vk, 03.75.Fi

With the realization of Bose Einstein condensation (BEC) in dilute alkali gases , it is now possible to study the coherent interaction between light and an ensemble of atoms prepared in a single quantum state. For example, Bragg diffraction  of a Bose-Einstein condensate by a moving optical standing wave can be used to diffract any fraction of a BEC into a selectable momentum state, realizing an atomic beam splitter. Among the multitude of experiments studying the behavior of a BEC under the action of external laser beams, only a small number have been devoted to the active role caused by the atoms in the condensate on the radiation. In particular, collective light scattering and matter-wave amplification caused by coherent center-of mass motion of atoms in a condensate illuminated by a far off-resonant laser were recently observed. These experiments have been interpreted in Ref. as superradiant Rayleigh scattering, and successively investigated in Ref.  and  using a quantum theory based on a quantum multi-mode extention of the collective atomic recoil laser (CARL) Hamiltonian model originally derived by Bonifacio et al.. In particular, the original semiclassical CARL model was extended in Ref. to include a quantum mechanical description of the center-of-mass motion of the atoms in the condensate. Whereas the analysis of ref. is limited to the study of the onset of the collective instability starting from quantum fluctuations, some nonlinear effects due to momentum population depletion were discussed in ref. and .

Recently, we have shown that the superradiant Rayleigh scattering from a BEC can be satisfactorily interpreted in terms of the CARL mechanism using a semiclassical model in the ’mean-field’ approximation, in which the rapid escape of the radiation from the condensate is modelled by a decay of the field amplitude at the rate $`\kappa _c=c/2L`$, where $`L`$ is the sample length. The main drawback of the semiclassical model is that, as it considers the center-of-mass motion of the atoms as classical, it cannot describe the discreteness of the recoil velocity, as has been observed in the experiment of Ref..

The aim of this work is to extend the semiclassical CARL model to include the quantum mechanical description of the center-of-mass motion of a sample of cold atoms. The quantum model that we obtain is equivalent to that derived by Moore and Meystre using second quantization techniques. However, whereas the work of Ref. is focussed on the linear regime and on the start-up of the instability, we study the full nonlinear regime and the quantum and classical limits of the model. Our basic result is that the atomic motion is quantized when the average recoil momentum is comparable to $`\mathrm{}\stackrel{}{q}`$ (where $`\stackrel{}{q}=\stackrel{}{k}_2\stackrel{}{k}_1`$ is the difference between the incident and the scattered wave vectors), i.e. the recoil momentum gained by the atom trading a photon via absorbtion and stimulated emission between the incident and scattered waves. In this limit, the quantum CARL equations reduce to the Maxwell-Bloch equations for two momentum levels. In the ’conservative’ (or ’hamiltonian’) regime, in which the radiation losses are negligible, this occurs for $`\rho <1`$, where the CARL parameter $`\rho `$ represents the average number of photons scattered per atom in the classical limit. In the superradiant regime, for $`\kappa >1`$ (where $`\kappa =\kappa _c/\omega _r\rho `$, $`\kappa _c`$ is the radiation loss, $`\omega _r\rho `$ is the collective recoil bandwidth, $`\omega _r=\mathrm{}|\stackrel{}{q}|^2/2M`$ is the recoil frequency and $`M`$ is the atomic mass), the atomic motion becomes quantized for $`\rho <\sqrt{2\kappa }`$. In this limit, we demonstrate that a sequential superfluorescence (SF) scattering occurs, in which, during each process, the atoms emit a $`\pi `$ hyperbolic secant pulse and populate a lower momentum level, as it has been observed in the MIT experiment.

Our starting point is the classical model of equations for $`N`$ two-level atoms exposed to an off-resonant pump laser, whose electric field $`\stackrel{}{E}_0=\widehat{e}_0\mathrm{cos}(\stackrel{}{k}_2\stackrel{}{x}\omega _2t)`$ is polarized along $`\widehat{e}`$, propagates along the direction of $`\stackrel{}{k}_2`$ and has a frequency $`\omega _2=ck_2`$ with a detuning from the atomic resonance, $`\mathrm{\Delta }_{20}=\omega _2\omega _0`$, much larger than the natural linewidth of the atomic transition, $`\gamma `$. We assume the presence of a scattered field (’probe beam’) with frequency $`\omega _1=\omega _2\mathrm{\Delta }_{21}`$, wavenumber $`\stackrel{}{k}_1`$ making an angle $`\varphi `$ with $`\stackrel{}{k}_2`$ and electric field $`\stackrel{}{E}=(\widehat{e}/2)[(t)e^{i(\stackrel{}{k}_1\stackrel{}{x}\omega _1t)}+\mathrm{c}.\mathrm{c}.]`$ with the same polarization of the pump field. In the absence of an injected probe field, the emission starts from fluctuations and the propagation direction of the scattered field is determined either by the geometry of the condensate (as in the case of the MIT experiment, where the condensate has a cigar shape) or by the presence of an optical resonator tuned on a selected longitudinal mode. By adiabatically eliminating the internal atomic degree of freedom, the following semiclassical CARL equations has been derived:

$`{\displaystyle \frac{d\theta _j}{d\tau }}`$ $`=`$ $`\overline{p}_j`$ (1)
$`{\displaystyle \frac{d\overline{p}_j}{d\tau }}`$ $`=`$ $`[\stackrel{~}{A}e^{i\theta _j}+\mathrm{c}.\mathrm{c}.]`$ (2)
$`{\displaystyle \frac{d\stackrel{~}{A}}{d\tau }}`$ $`=`$ $`{\displaystyle \frac{1}{N}}{\displaystyle \underset{j=1}{\overset{N}{}}}e^{i\theta _j}+i\delta \stackrel{~}{A}`$ (3)
where $`\tau =\rho \omega _rt`$ is the interaction time in units of $`\omega _r\rho `$, $`\theta _j=(\stackrel{}{k}_1\stackrel{}{k}_2)\stackrel{}{x}_j=qz_j`$ and $`\overline{p}_j=qv_{zj}/\rho \omega _r`$ (where $`q=|\stackrel{}{q}|`$) are the dimensionless position and velocity of the $`j`$-th atom along the axis $`\widehat{z}`$, $`\stackrel{~}{A}=i(ϵ_0/n_s\mathrm{}\omega \rho )^{1/2}(\tau )e^{i\delta \tau }`$, $`\delta =\mathrm{\Delta }_{21}/\omega _r\rho `$ and $`\rho =(\mathrm{\Omega }_0/2\mathrm{\Delta }_{20})^{2/3}(\omega \mu ^2n_s/\mathrm{}ϵ_0\omega _r^2)^{1/3}`$ is the collective CARL parameter. $`\mathrm{\Omega }_0=\mu _0/\mathrm{}`$ is the Rabi frequency of the pump, $`n_s=N/V`$ is the average atomic density of the sample (containing $`N`$ atoms in a volume $`V`$) and $`\mu `$ is the dipole matrix element. We assume $`\omega _2\omega _1=ck`$, so that $`q2k\mathrm{sin}^2(\varphi /2)`$. Eqs.(1)-(3) are formally equivalent to those of the free electron laser model. In order to quantize both the radiation field and the center-of-mass motion of the atoms, we consider $`\theta _j`$, $`p_j=(\rho /2)\overline{p}_j=Mv_{zj}/\mathrm{}q`$ and $`a=(N\rho /2)^{1/2}\stackrel{~}{A}`$ as quantum operators satisfying the canonical commutation relations $`[\theta _j,p_j^{}]=i\delta _{jj^{}}`$ and $`[a,a^{}]=1`$. With these definitions, Eqs.(1)-(3) are the Heisenberg equations of motion associated with the Hamiltonian:

$$H=\frac{1}{\rho }\underset{j=1}{\overset{N}{}}p_j^2+ig(\underset{j=1}{\overset{N}{}}a^{}e^{i\theta _j}\mathrm{h}.\mathrm{c}.)\delta a^{}\stackrel{~}{a}=\underset{j=1}{\overset{N}{}}H_j(\theta _j,p_j),$$
(4)
where $`g=\sqrt{\rho /2N}`$. We note that $`[H,Q]=0`$, where $`Q=a^{}a+_{j=1}^Np_j`$ is the total momentum in units of $`\mathrm{}q`$. In order to obtain a simplified description of a BEC as a system of $`N`$ noninteracting atoms in the ground state, we use the Schrödinger picture for the atoms (instead of the usual Heisenberg picture), i.e. $`|\psi (\theta _1,\mathrm{},\theta _N)=|\psi (\theta _1)\mathrm{}|\psi (\theta _N)`$, where $`|\psi (\theta _j)`$ obeys the single-particle Schrödinger equation, $`i(/\tau )|\psi (\theta _j)=H_j(\theta _j,p_j)|\psi (\theta _j)`$. In this paper we describe the light field classically. Hence, considering the field operator $`a`$ as a c-number, eq.(3) yields:

$$\frac{da}{d\tau }=i\delta a+g\underset{j=1}{\overset{N}{}}\psi (\theta _j)|e^{i\theta _j}|\psi (\theta _j).$$
(5)
Let now expand the single-atom wavefunction on the momentum basis, $`|\psi (\theta _j)=_nc_j(n)|n_j`$, where $`p_j|n_j=n|n_j`$, $`n=\mathrm{},\mathrm{}\mathrm{}`$ and $`c_j(n)`$ is the probability amplitude of the $`j`$-th atom having momentum $`n\mathrm{}\stackrel{}{q}`$. Introducing the collective density matrix:

$$S_{m,n}=\frac{1}{N}\underset{j=1}{\overset{N}{}}c_j(m)^{}c_j(n)e^{i(mn)\delta \tau },$$
(6)
a straightforward calculation yields, from Eqs.(4) and (5), the following closed set of equations:

$`{\displaystyle \frac{dS_{m,n}}{d\tau }}`$ $`=`$ $`i(mn)\delta _{m,n}S_{m,n}+{\displaystyle \frac{\rho }{2}}\left[A\left(S_{m+1,n}S_{m,n1}\right)+A^{}\left(S_{m,n+1}S_{m1,n}\right)\right]`$ (7)
$`{\displaystyle \frac{dA}{d\tau }}`$ $`=`$ $`{\displaystyle \underset{n=\mathrm{}}{\overset{\mathrm{}}{}}}S_{n,n+1}\kappa A,`$ (8)
where $`\delta _{m,n}=\delta +(m+n)/\rho `$ and we have redefined the field as $`A=\sqrt{2/\rho N}ae^{i\delta \tau }`$. We have also introduced a damping term $`\kappa A`$ in the field equation, where $`\kappa =\kappa _c/\omega _r\rho `$, $`\kappa _c=c/2L`$ and $`L`$ is the sample length along the probe propagation, which provides an approximated model describing the escape of photons from the atomic medium. In the presence of a ring cavity of length $`L_{\mathrm{cav}}`$ and reflectivity $`R`$, $`\kappa _c=(c/L_{\mathrm{cav}})\mathrm{ln}R`$, as shown in the usual ’mean-field’ approximation. Eqs.(7) and (8) are completely equivalent to the CARL equations (1)-(3) and determine the temporal evolution of the density matrix elements for the momentum levels. In particular, $`p_n=S_{n,n}`$ is the probability of finding the atom in momentum level $`|n`$, $`p=_nnS_{n,n}`$ is the average momentum and $`_nS_{n,n+1}`$ is the bunching parameter. Eqs.(7) and (8) are identical to these derived by Moore and coworkers second quantizing the single-particle Hamiltonian $`H_j`$ and introducing bosonic creation and annihilation operators of a given center-of-mass momentum. For a constant field $`A`$, Eq.(7) describes a Bragg scattering process, in which $`mn`$ photons are absorbed from the pump and scattered into the probe, changing the initial and final momentum states of the atom from $`m`$ to $`n`$. Conservation of energy and momentum require that during this process $`\omega _1\omega _2=(m+n)\omega _r`$, i.e. $`\delta _{m,n}=0`$. Eqs.(7) and (8) conserve the norm, i.e. $`_mS_{m,m}=1`$, and, when $`\kappa =0`$, also the total momentum $`Q=(\rho /2)|A|^2+p`$. Figure 1a shows $`|A|^2`$ vs. $`\tau `$, for $`\kappa =0`$, $`\delta =0`$ and $`A(0)=10^4`$, comparing the semiclassical solution with the quantum solution in the classical limit, $`\rho 1`$: the dashed line is the numerical solution of Eqs.(1)-(3), for a classical system of $`N=200`$ cold atoms, with initial momentum $`p_j(0)=0`$ (where $`j=1,\mathrm{},N`$) and phase $`\theta _j(0)`$ uniformly distributed over $`2\pi `$, i.e. unbunched; the continuous line is the numerical solution of Eqs.(7) and (8) for $`\rho =10`$ and a quantum system of atoms initially in the ground state $`n=0`$, i.e. with $`S_{n,m}=\delta _{n0}\delta _{m0}`$. Figure 1a shows that the quantum system behaves, with good approximation, classically. Because from Fig.1a the maximum dimensionless intensity is $`|A|^21.4`$, the constant of motion $`Q`$ gives $`p0.7\rho `$ and the maximum average number of emitted photons is about $`a^{}aN\rho `$. Hence, the CARL parameter $`\rho `$ can be interpreted as the maximum average number of photons emitted per atom (or equivalently, as the maximum average momentum recoil, in units of $`\mathrm{}q`$, acquired by the atom) in the classical limit. Figure 1b shows the distribution of the population level $`p_n`$ at the first peak of the intensity of fig.1a, for $`\tau =12.4`$. We observe that, at saturation, twenty-five momentum levels are occupied, with an induced momentum spread comparable to the average momentum.

Let us now consider the equilibrium state with no probe field, $`A=0`$, and all the atoms in the same momentum state $`n`$, i.e. with $`S_{n,n}=1`$ and the other matrix elements zero. This is equivalent to assume the temperature of the system equal to zero and all the atoms moving with the same velocity $`n\mathrm{}\stackrel{}{q}`$, without spread. This equilibrium state is unstable for certain values of the detuning. In fact, by linearizing Eqs.(7) and (8) around the equilibrium state, the only matrix elements giving linear contributions are $`S_{n1,n}`$ and $`S_{n,n+1}`$, showing that in the linear regime the only transitions allowed from the state $`n`$ are these towards the levels $`n1`$ and $`n+1`$. Introducing the new variables $`B_n=S_{n,n+1}+S_{n1,n}`$ and $`P_n=S_{n,n+1}S_{n1,n}`$, Eqs.(7) and (8) reduce to the linearized equations:

$`{\displaystyle \frac{dB_n}{d\tau }}`$ $`=`$ $`i\delta _nB_n{\displaystyle \frac{i}{\rho }}P_n`$ (9)
$`{\displaystyle \frac{dP_n}{d\tau }}`$ $`=`$ $`i\delta _nP_n{\displaystyle \frac{i}{\rho }}B_n\rho A`$ (10)
$`{\displaystyle \frac{dA}{d\tau }}`$ $`=`$ $`B_n\kappa A,`$ (11)
where $`\delta _n=\delta +2n/\rho `$. Seeking solutions proportional to $`e^{i(\lambda \delta _n)\tau }`$, we obtain the following cubic dispersion relation:

$$\left(\lambda \delta _ni\kappa \right)\left(\lambda ^21/\rho ^2\right)+1=0.$$
(12)
In the exponential regime, when the unstable (complex) root $`\lambda `$ dominates, $`B(\tau )e^{i(\lambda \delta _n)\tau }`$ and, from Eq.(9), $`P_n=\rho \lambda B_n`$. The semiclassical limit is recovered for $`\rho 1`$ (when $`\kappa =0`$) or $`\rho \sqrt{\kappa }`$ (when $`\kappa >1`$) and $`\delta _n\delta `$, i.e. neglecting the shift due to the recoil frequency $`\omega _r`$. In this limit, maximum gain occurs for $`\delta =0`$, with $`\lambda =(1i\sqrt{3})/2`$ when $`\kappa =0`$ or $`\lambda =(1+i)/\sqrt{2\kappa }`$ when $`\kappa >1`$. Furthermore, $`|S_{n,n+1}||S_{n1,n}|`$, so that the atoms may experience both emission and absorbtion. This result can be interpreted in terms of single-photon emission and absorpion by an atom with initial momentum $`n\mathrm{}\stackrel{}{q}`$. In fact, energy and momentum conservation impose $`\omega _1\omega _2=(2n1)\omega _r`$ (i.e. $`\delta _n=\pm 1/\rho `$) when a probe photon is emitted or absorbed, respectively. Because in the semiclassical limit the gain bandwidth is $`\mathrm{\Delta }\omega \omega _r\rho \omega _r`$ when $`\kappa =0`$ (or $`\mathrm{\Delta }\omega \kappa _c\omega _r`$ when $`\kappa >1`$) the atom can both emit or absorbe a probe photon. On the contrary, in the quantum limit the recoil energy $`\mathrm{}\omega _r`$ can not be neglected, and there is emission without absorbtion if $`|S_{n,n+1}||S_{n1,n}|`$, i.e. $`B_nP_n`$ and $`\lambda 1/\rho `$. This is true for $`\rho <1`$ when $`\kappa =0`$, with the unstable root $`\lambda 1/\rho +\delta _n^{}/21/2\sqrt{\delta _n^22\rho }`$ (where $`\delta _n^{}=\delta _n1/\rho `$), and for $`\rho <\sqrt{2\kappa }`$ when $`\kappa >1`$, with $`\mathrm{Re}\lambda 1/\rho +(\rho \delta _n^{}/2)/(\delta _n^2+\kappa ^2)`$ and $`\mathrm{Im}\lambda (\rho \kappa /2)/(\delta _n^2+\kappa ^2)`$. In both cases, maximum gain occurs for $`\delta _n=1/\rho `$ (i.e. $`\mathrm{\Delta }_{21}=(12n)\omega _r`$) within a bandwidth $`\mathrm{\Delta }\omega \omega _r\rho ^{3/2}`$ and $`\mathrm{\Delta }\omega \omega _r\rho ^2/\kappa `$ (respectively for $`\kappa =0`$ and $`\kappa >1`$), which are both less than the frequency difference $`2\omega _r`$ between the emission and absorbtion lines. Hence, in the quantum limit the optical gain is due exclusively to emission of photons, whereas in the semiclassical limit gain results from a positive difference between the average emission and absorbtion rates. When $`\kappa =0`$, the resonant gain in the limit $`\rho <1`$ is $`G_S=\omega _r\rho \sqrt{\rho /2}=\sqrt{3/8\pi }(\mathrm{\Omega }_0/2\mathrm{\Delta }_{20})\gamma \sqrt{N_{\mathrm{eff}}}`$, where $`\gamma =\mu ^2k^3/3\pi \mathrm{}ϵ_0`$ is the natural decay rate of the atomic transition and $`N_{\mathrm{eff}}=(\lambda ^2/A)(c/\gamma L)N`$ is the effective atomic number in the volume $`V=AL`$, where $`A`$ and $`L`$ are the cross section and the length of the sample. When $`\kappa >1`$, the resonant SF gain in the limit $`\rho <\sqrt{2\kappa }`$ is $`G_{\mathrm{SF}}=\omega _r\rho ^2/2\kappa =(3/4\pi )\gamma (\mathrm{\Omega }_0/2\mathrm{\Delta }_{20})^2(\lambda ^2/A)N`$.

The above results show that the combined effect of the probe and pump fields on a collection of cold atoms in a pure momentum state $`n`$ is responsible of a collective instability that leads the atoms to populate the adjacent momentum levels $`n1`$ and $`n+1`$. However, in the quantum limit $`\rho <1`$ when $`\kappa =0`$ (or $`\rho <\sqrt{2\kappa }`$ when $`\kappa >1`$) conservation of energy and momentum of the photon constrains the atoms to populate only the lower momentum level $`n1`$. This holds also in the nonlinear regime, as we have verified solving numerically Eqs.(7) and (8). In the quantum limit above, the exact equations reduce to those for only three matrix elements, $`S_{n,n}`$, $`S_{n1,n1}`$ and $`S_{n1,n}`$, with $`S_{n1,n1}+S_{n,n}=1`$. Introducing the new variables $`S_n=S_{n1,n}`$ and $`W_n=S_{n,n}S_{n1,n1}`$, Eqs.(7) and (8) reduce to the well-known Maxwell-Bloch equations:

$`{\displaystyle \frac{dS_n}{d\tau }}`$ $`=`$ $`i\delta _n^{}S_n+{\displaystyle \frac{\rho }{2}}AW_n`$ (13)
$`{\displaystyle \frac{dW_n}{d\tau }}`$ $`=`$ $`\rho (A^{}S_n+\mathrm{h}.\mathrm{c}.)`$ (14)
$`{\displaystyle \frac{dA}{d\tau }}`$ $`=`$ $`S_n\kappa A,`$ (15)
where $`\delta _n^{}=\delta +(2n1)/\rho `$. When $`\kappa =0`$ and $`\delta _n^{}=0`$, if the system starts radiating incoherently by pure quantum-mechanical spontaneous emission, the solution of Eqs.(13)-(15) is a periodic train of $`2\pi `$ hyperbolic secant pulses with $`|A|^2=(2/\rho )\mathrm{sech}^2[\sqrt{\rho /2}(\tau \tau _n)]`$, where $`\tau _n=(2n+1)\mathrm{ln}(\rho /2)/\sqrt{\rho /2}`$. Furthermore, the average momentum $`p=n+\mathrm{Th}^2[\sqrt{\rho /2}(\tau \tau _n)]1`$ oscillates between $`n`$ and $`n1`$ with period $`\tau _n`$. We observe that the maximum number of photons emitted is $`a^{}a_{\mathrm{peak}}=(\rho N/2)|A|_{\mathrm{peak}}^2=N`$, as expected. Figure 2 shows the results of a numerical integration of Eqs.(7) and (8), for $`\kappa =0`$, $`\rho =0.2`$ and $`\delta =5`$, with the atoms initially in the momentum level $`n=0`$ and the field starting from the seed value $`A_0=10^5`$. Figures 2a and b show the intensity $`|A|^2`$ and the average momentum $`p`$ vs. $`\tau `$, in agreement with the predictions of the reduced Eqs.(13)-(15).

In the superradiant regime, $`\kappa >1`$, Eqs.(13)-(15) describe a single SF scattering process in which the atoms, initially in the momentum state $`n`$, ’decay’ to the lower level $`n1`$ emitting a $`\pi `$ hyperbolic secant pulse, with intensity $`|A|^2=1/[4(\kappa ^2+\delta _n^2)]\mathrm{sech}^2[(\tau \tau _D)/\tau _{SF}]`$ and average momentum $`p=n(1/2)\{1+\mathrm{Th}[(\tau \tau _D)/\tau _{SF}]\}`$, where $`\tau _{SF}=2(\kappa ^2+\delta _n^2)/\rho \kappa `$ is the ’superfluorescence time’, $`\tau _D=\tau _{SF}\mathrm{Arcsech}(2|S_n(0)|)\tau _{SF}\mathrm{ln}\sqrt{2|S_n(0)|}`$ is the delay time and $`|S_n(0)|1`$ is the initial polarization. Figures 3a and b shows $`|A|^2`$ and $`p`$ vs. $`\tau `$ calculated solving Eqs.(7) and (8) numerically with $`\kappa =10`$, $`\rho =2`$, $`\delta =0.5`$ and the same initial conditions of fig. 2. We observe a sequential SF scattering, in which the atoms, initially in the level $`n=0`$, change their momentum by discrete steps of $`\mathrm{}\stackrel{}{q}`$ and emit a SF pulse during each scattering process. We observe that for $`\delta =1/\rho `$ the field is resonant only with the first transition, from $`n=0`$ to $`n=1`$; for a generic initial state $`n`$, resonance occurs when $`\delta =(12n)/\rho `$, so that in the case of figure 3a the peak intensity of the successive SF pulses is reduced (by the factor $`1/[\kappa ^2+(2n/\rho )^2]`$) whereas the duration and the delay of the pulse are increased. However, the pulse retains the characteristic sech<sup>2</sup> shape and the area remains equal to $`\pi `$, inducing the atoms to decrease their momentum by a finite value $`\mathrm{}\stackrel{}{q}`$. We note that, although the SF time in the quantum limit ($`\tau _{SF}=2\kappa /\rho `$ at resonance) can be considerable longer than the characteristic superradiant time obtained in the classical limit, $`\tau _{SR}=\sqrt{2\kappa }`$, the peak intensity of the pulse in the quantum limit is always approximately half of the value obtained in the semiclassical limit (see Ref. for details).

In conclusion, we have shown that the CARL model describing a system of atoms in their momentum ground state (as those obtained in a BEC) and properly extended to include a quantum-mechanical description of the center-of-mass motion, allows for a quantum limit in which the average atomic momentum changes in discrete units of the photon recoil momentum $`\mathrm{}\stackrel{}{q}`$ and reduce to the Maxwell-Bloch equations for two momentum levels. These results demonstrate that the regular arrangement of momentum pattern observed in the MIT experiment can be interpreted as being due to sequential superfluorescence scattering. A detailed study of this and other aspects of the MIT experiment will be the object of a future extended pubblication.

We thank G.R.M. Robb for a careful reading of the manuscript and for helpful discussions.


text:
# Hydrodynamics of an ultra-relativistic fluid in the flat anisotropic cosmological model

\[

## Abstract

Motion of an ultra-relativistic perfect fluid in space-time with the Kasner metrics is investigated by the Hamiltonian method. It is found that in the limit of small times a tendency takes place to formation of strong inhomogeneities in matter distribution. In the case of slow flows the effect of non-stationary anisotropy on dynamics of sound waves and behaviour of frozen-in vortices is considered. It is shown that hydrodynamics of slow vortices on the static homogeneous background is equivalent to the usual Eulerian incompressible hydrodynamics, but in the presence of an external non-stationary strain velocity field.

\]

Dynamics of a relativistic fluid in a gravitational field has a set of distinctive properties in comparison with hydrodynamics in a flat space-time ,. An explicit dependence of the metric tensor components $`g_{ik}(t,𝐫)`$ on time coordinate $`t`$ and spatial coordinates $`𝐫=(x,y,z)`$, together with back influence of the matter on gravitational field, result in a wide variety in behaviour of solutions for equations of motion. Many phenomena in the general-relativistic hydrodynamics have not been studied yet. In order to get a better understanding of various processes taking place in the system, it is useful to analyse simple limit cases, when only one of many general-relativistic effects is mostly important. If a dissipation may be neglected, then one can simplify significantly the analysis by using the Hamiltonian formalism, application of which to hydrodynamics has given many interesting results (see the reviews ,  and references therein). A brief discussion of adaptation of the Hamiltonian method for the relativistic hydrodynamics can be found, for instance, in the papers  and . So, in the work , slow isentropic flows of an ideal relativistic fluid have been considered and a partial study of influence of a spatial inhomogeneity on the motion of hydrodynamical vortices has been performed. On the contrary, in present work we suppose that the space is homogeneous and concentrate our attention on the effects of its non-stationary anisotropy. It is known that there exists the class of solutions of the Einstein equations for empty space-time, which has been found by Kasner in 1922, with metrics of the following form:

$$ds^2=dt^2t^{2/3}(t^{2\lambda _1}dx^2+t^{2\lambda _2}dy^2+t^{2\lambda _3}dz^2),$$
(1)
where $`\lambda _1,\lambda _2,\lambda _3`$ are any three numbers satisfying two conditions

$$\lambda _1+\lambda _2+\lambda _3=0,\lambda _1^2+\lambda _2^2+\lambda _3^2=2/3.$$
(2)
At small times, this metrics describes approximately also the case of Universe filled uniformly by a fluid, since in the limit $`t0`$ a back reaction of matter on the gravitational field appears to be negligible ,. In present work we have used this result and considered the hydrodynamics of a perfect fluid having ultra-relativistic equation of state, in the space-time with the fixed metrics (1). We have established that at early times, flows with a finite mean momentum are in such a dynamic regime that a motion of each fluid element is nearly independent on the motion of other fluid elements. Due to this reason, there exists a tendency to formation of strong inhomogeneities in the spatial distribution of the matter which is related to singularities of an approximate Lagrangian mapping. We have found also that even in the case of slow flows with zero mean momentum the nonstationary anisotropy influences strongly both on the dynamics of sound oscillations and on the vortex motion, making their properties be different in some aspects from properties of the analogous objects in the flat space-time.

The plan of further exposition is the following. At first, a necessary explanation will be given concerning the employed theoretical method, and the expression for the Lagrangian $``$ of relativistic ideal hydrodynamics in a given gravitational field will be written. After a brief discussion of specific properties of corresponding equations of motion, we shall pass to the Hamiltonian description of the system dynamics and we will introduce the exact expression for the Hamiltonian $``$ corresponding to the ultra-relativistic equation of state of the matter. Some important properties of the dynamics in the limit $`t0`$ will be discussed. A quadratic (on small deviations) part $`^{(2)}`$ of the Hamiltonian will be used for the derivation of simplified equations of motion for sound waves and vortices.

At first we introduce needed concepts. The energy density $`\epsilon `$, measured in the locally co-moving reference frame, and the density $`n`$ of number of conserved particles are connected by equation of state $`\epsilon =\epsilon (n)`$ . The scalar $`n`$ is equal to the length of the 4-vector of current $`n^i=n(dx^i/ds)`$ . Let us introduce the relative density $`\rho (t,𝐫)`$ in such a manner that it obeys the standard continuity equation

$$\rho _t+(\rho 𝐯)=0,$$
(3)
where 3-velocity field $`𝐯(t,𝐫)=v^\alpha =(v^x,v^y,v^z)`$ is defined as $`dx^\alpha /dt`$ on the world-line of the fluid point passing through $`(t,𝐫)`$. The equation (3) follows from the equation $`n_{;i}^i=0`$, expressing the conservation law for the fluid amount , if $`\rho `$ and $`n`$ are connected by the relation :

$$n=\frac{\rho }{\sqrt{|g|}}\sqrt{g_{00}+2g_{0\alpha }v^\alpha +g_{\alpha \beta }v^\alpha v^\beta },$$
(4)
where $`g=\text{det}g_{ik}`$ is the determinant of the metric tensor.

The action functional $`S=𝑑t`$ of relativistic hydrodynamics is defined through the Lagrangian $`=\{\rho ,𝐯\}`$ in the following way ,:

$$=\epsilon \left(\frac{\rho }{\sqrt{|g|}}\sqrt{g_{00}+2g_{0\alpha }v^\alpha +g_{\alpha \beta }v^\alpha v^\beta }\right)\sqrt{|g|}𝑑𝐫.$$
(5)
The equation of motion for the velocity field $`𝐯(t,𝐫)`$ has the structure (generalized Euler’s equation )

$$(_t+𝐯)\left(\frac{1}{\rho }\frac{\delta }{\delta 𝐯}\right)=\left(\frac{\delta }{\delta \rho }\right)\frac{1}{\rho }\left(\frac{\delta }{\delta v^\alpha }\right)v^\alpha .$$
(6)
This is merely the variational Euler-Lagrange equation expressing the least action $`S`$ principle for variations of world-lines of fluid particles. The 3-vector $`𝐩(t,𝐫)=(1/\rho )(\delta /\delta 𝐯)`$,

$$p_\alpha =\epsilon ^{}(n)\frac{(g_{0\alpha }+g_{\alpha \beta }v^\beta )}{\sqrt{g_{00}+2g_{0\alpha }v^\alpha +g_{\alpha \beta }v^\alpha v^\beta }},$$
(7)
is the canonical momentum of a liquid particle in the point $`(t,𝐫)`$. We see that the definition of the canonical momentum in relativistic hydrodynamics depends in a complicated manner on the equation of state. The relation (7) can be resolved respectively to the velocity, which gives the inverse dependence: $`𝐯=𝐯\{\rho ,𝐩\}`$. The remarkable equation for the vorticity field $`𝛀(𝐫,t)=\text{curl}𝐩(t,𝐫)`$

$$𝛀_t=\text{curl}[𝐯\times 𝛀],$$
(8)
can be obtained from the equation (6) by applying the curl-operator. It implies that vorticity is frozen in the fluid and the generalized Kelvin’s theorem (conservation of circulation of the field $`𝐩`$ along arbitrary closed contour $`\gamma (t)`$ transported by flow) holds:

$$_{\gamma (t)}(𝐩d𝐥)=\mathrm{\Gamma }_\gamma =const.$$

Passing to representation of flows in terms of the fields $`\rho `$ and $`𝐩`$ and defining the Hamiltonian $`\{\rho ,𝐩\}`$ in such a manner:

$$\{\rho ,𝐩\}=\left(\left(\frac{\delta }{\delta 𝐯}𝐯\right)𝑑𝐫\right)|_{𝐯=𝐯\{\rho ,𝐩\}}$$
(9)
we have the equations of motion in the form

$$\rho _t+\left(\frac{\delta }{\delta 𝐩}\right)=0,$$
(10)
$$𝐩_t=\left[\left(\frac{\delta }{\delta 𝐩}\right)\times \frac{\text{curl}𝐩}{\rho }\right]\left(\frac{\delta }{\delta \rho }\right).$$
(11)
In particular, for the potential flows, when the vorticity is equal to zero and $`𝐩=\phi `$, the dynamical variables $`\rho `$ and $`\phi `$ are canonically conjugated:

$$\rho _t=\frac{\delta \{\rho ,\phi \}}{\delta \phi },\phi _t=\frac{\delta \{\rho ,\phi \}}{\delta \rho }.$$
(12)
Equations (12) will be used further (in linearized form) for analysis of acoustic mode dynamics.

Other interesting dynamic regime can take place if there is an equilibrium solution $`\rho =\rho _0(𝐫)`$, $`𝐩=𝐩_0=const`$, independent on time. If vortical component of flow is small and the sound waves are excited weakly, then perturbations of density are negligibly small in comparison with its equilibrium value. In such circumstances a slow dynamics of the vorticity is described by the equation ,

$$𝛀_t=\text{curl}\left[\text{curl}\left(\frac{\delta _{}}{\delta 𝛀}\right)\times \frac{𝛀}{\rho _0(𝐫)}\right],$$
(13)
where the Hamiltonian of the vorticity $`_{}\{𝛀\}`$ is obtained from the quadratic (on $`\delta 𝐩=𝐩𝐩_0`$ and $`\delta \rho =\rho \rho _0`$) part $`^{(2)}\{\delta \rho ,\delta 𝐩\}`$ of the total Hamiltonian after fixing the potential $`\phi `$ by condition of zero density variation $`\delta ^{(2)}/\delta \phi =0`$:

$$_{}\{𝛀\}=^{(2)}\{0,\text{curl}^1𝛀+\phi \}|_{\delta ^{(2)}/\delta \phi =0}$$
(14)
It should be noted that although the equilibrium solution must be independent on time, the Hamiltonian itself may contain an explicit dependence on $`t`$. It is the case in the space-time with the Kasner metrics (1). In such a Universe the homogeneous equilibrium solutions $`\rho =\rho _0=const`$, $`𝐩=𝐩_0=const`$ are possible, which fact can easily be seen from equations of motion (3) and (6).

Now we pass to concrete calculations. We will use the Kasner metrics (1) and the ultra-relativistic equation of state

$$\epsilon (n)n^{4/3},$$
(15)
since $`n\mathrm{}`$ when $`t0`$ . For convenience, we change definition of the exponents: $`3\lambda _\alpha =2\mu _\alpha `$ and perform the substitution $`t^{2/3}=\tau `$ for the time coordinate in the action $`S`$, and also choose in an appropriate manner scales for spatial coordinates and for relative density $`\rho `$, in order to obtain

$$\{\rho ,𝐯\}=\frac{3}{4}\rho ^{4/3}\left(1\underset{\alpha }{}\tau ^{2\mu _\alpha }(v^\alpha )^2\right)^{2/3}𝑑𝐫.$$
(16)
The procedure of calculation of the Hamiltonian $`\{\rho ,𝐩\}`$, corresponding to this Lagrangian, includes first of all the solution of the relation $`𝐩=(1/\rho )(\delta /\delta 𝐯)`$, i.e.

$$p_\alpha =\rho ^{1/3}\left(1\underset{\beta }{}\tau ^{2\mu _\beta }(v^\beta )^2\right)^{\frac{1}{3}}\tau ^{2\mu _\alpha }v^\alpha ,$$
(17)
respectively to $`𝐯`$, and its substitution to (9). Let us introduce the notations

$$A=\underset{\beta }{}\tau ^{2\mu _\beta }(v^\beta )^2,Q=\rho ^{2/3}\underset{\beta }{}\tau ^{2\mu _\beta }p_\beta ^2.$$
(18)
We define the auxiliary function $`h(Q)`$ by the conditions

$$Q^3(1A)^2=A^3,h=\sqrt{AQ}+\frac{3}{4}(1A)^{2/3}.$$
(19)
The explicit expression $`h(Q)`$ can be found with the help of formula for roots of cubical polynome. Designating for brevity

$$R(Q)=2^{1/3}\left(272Q^3+3\sqrt{3}\sqrt{274Q^3}\right)^{1/3},$$
(20)
we obtain that

$$h(Q)=\frac{Q}{3}\left(Q+\frac{Q^2}{R(Q)}+R(Q)\right)$$

$$+\frac{3}{4}\left(1\frac{Q}{9}\left(Q+\frac{Q^2}{R(Q)}+R(Q)\right)^2\right)^{\frac{2}{3}}.$$
(21)
We plot the dependence $`h`$ versus $`\sqrt{Q}`$ in the Fig. 1.

At small $`Q`$, the approximate equality is valid

$$h(Q)\frac{3}{4}+\frac{Q}{2},Q1,$$
(22)
and at $`Q1`$ the following behaviour takes place:

$$h(Q)\sqrt{Q}+\frac{1}{4Q},Q1.$$
(23)
As the result, the Hamiltonian of the ultra-relativistic fluid in the Kasner space-time has the form

$$\{\rho ,𝐩\}=\rho ^{4/3}h\left(\rho ^{2/3}\underset{\alpha }{}\tau ^{2\mu _\alpha }p_\alpha ^2\right)𝑑𝐫.$$
(24)
For definiteness, we arrange the Kasner exponents in the order $`\mu _1<\mu _2<\mu _3`$. The constants $`\mu _\alpha `$ satisfy the inequalities

$$2<2\mu _1<1,1<2\mu _2<1,1<2\mu _3<2,$$
(25)
following from the conditions (2). Let us suppose $`z`$-component of the mean momentum be different from zero: $`p_{z0}0`$. We consider here the case when deviations of $`𝐩`$ from the mean value are comparatively small. Then at sufficiently small times the quantity $`Q`$ reaches large values, since the order of magnitude of quantities $`\rho `$ and $`𝐩`$ is conserved due to the conservation laws for fluid amount and for mean momentum. Asymptotics (23) gives the approximate Hamiltonian in this limit

$$\stackrel{~}{}\left\{\rho \left(\underset{\alpha }{}\tau ^{2\mu _\alpha }p_\alpha ^2\right)^{\frac{1}{2}}+\frac{\rho ^2/4}{\left(_\alpha \tau ^{2\mu _\alpha }p_\alpha ^2\right)}\right\}𝑑𝐫$$
(26)
If we neglect here the quadratic on $`\rho `$ term, where the coefficient in front of $`\rho ^2`$ is small in the limit of small times, then equation of motion for the canonical momentum field does not depend on $`\rho `$ at all. Each point of fluid, labeled by a label $`𝐚=a^\alpha `$, moves almost independently on other points in accordance with the approximate law

$$x^\alpha (\tau ,𝐚)a^\alpha +_0^\tau \frac{\tau ^{2\mu _\alpha }p_\alpha (𝐚)d\tau }{\sqrt{_\beta \tau ^{2\mu _\beta }p_\beta ^2(𝐚)}}$$

$$a^\alpha +\frac{p_\alpha (𝐚)\tau ^{1+\mu _32\mu _\alpha }}{|p_z(𝐚)|(1+\mu _32\mu _\alpha )}.$$
(27)
Deviations of arbitrary constants of motion $`𝐩(𝐚)`$ from the mean value make possible finite-time singularities of the mapping $`𝐫(\tau ,𝐚)`$. Accordingly, quasi-two-dimensional domains of pancake-like shape may arise in the space where the density is much larger than the mean density: $`\rho =\rho (𝐚)\text{det}𝐚/𝐫\rho _0`$. There, the neglection of the quadratic on $`\rho `$ term is no more valid, and actually a redistribution of momenta between fluid elements occurs.

To investigate slow flows on a resting background, it is necessary to obtain the expression for $`^{(2)}\{\delta \rho ,𝐩\}`$. Let us expand $`\{\rho ,𝐩\}`$ to the second order terms on $`\delta \rho (\tau ,𝐫)=\rho (\tau ,𝐫)\rho _0`$ and $`𝐩(\tau ,𝐫)`$. Then using of the expansion (22) gives

$$^{(2)}=\frac{\rho _0^{2/3}}{2}\underset{\alpha }{}\tau ^{2\mu _\alpha }p_\alpha ^2d𝐫+\frac{\rho _0^{2/3}}{3}\frac{(\delta \rho )^2}{2}𝑑𝐫.$$
(28)
Expression (28) and equations (12) allow us immediately to write the linearized equations of motion for the spatial Fourier-harmonics of sound waves:

$$\frac{d\phi _𝐤}{d\tau }=\frac{1}{3}\rho _0^{\frac{2}{3}}\rho _𝐤,\frac{d\rho _𝐤}{d\tau }=\rho _0^{\frac{2}{3}}\left(\underset{\alpha }{}\tau ^{2\mu _\alpha }k_\alpha ^2\right)\phi _𝐤.$$
(29)
We can reduce this system to one ordinary linear differential equation

$`{\displaystyle \frac{d^2\phi _𝐤(\tau )}{d\tau ^2}}+{\displaystyle \frac{1}{3}}\left({\displaystyle \underset{\alpha }{}}\tau ^{2\mu _\alpha }k_\alpha ^2\right)\phi _𝐤(\tau )=0.`$ (30)
If $`k_z^20`$, then behaviour of $`\phi _𝐤(\tau )`$ at small times is determined by the exponent $`\mu _3`$. Obviously, all solutions of equation (30) have in general an oscillating character at $`\tau >\tau _{}(𝐤)|k_z|^{1/(\mu _31)}`$. There is no oscillations at $`\tau \tau _{}(𝐤)`$. Among linearly independent solutions there exists one, which tends to zero at $`\tau 0`$ as $`\phi _𝐤^{(1)}\tau `$. Let us note that the corresponding $`\rho _𝐤^{(1)}`$ tends to some finite value as $`\tau 0`$. Another solution, linearly independent on first one, is finite in the zero, but its derivative diverges at $`\tau 0`$ as $`d\phi _𝐤^{(2)}/d\tau \tau ^{12\mu _3}`$, and this fact means unbounded growth of $`\rho _𝐤^{(2)}`$ and indicates transition of the system to the highly nonlinear dynamics regime described by the Hamiltonian (26).

For analysis of slow vortical flows, let us write explicitly the Hamiltonian $`_{}\{𝛀\}`$. For simplicity we put $`\rho _0=1`$. In accordance with the definition (14) and the expression (28), we obtain after simple calculations that

$$_{}\{𝛀\}=\frac{1}{8\pi }\frac{d𝐫_1d𝐫_2_\alpha \tau ^{2\mu _\alpha }\mathrm{\Omega }^\alpha (𝐫_1)\mathrm{\Omega }^\alpha (𝐫_2)}{\left(_\alpha \tau ^{2\mu _\alpha }(x_1^\alpha x_2^\alpha )^2\right)^{1/2}}.$$
(31)
Let us express the frozen-in field of the vorticity through the shape $`𝐑(\nu ,\xi ,\tau )`$ of vortex lines, (see , ,  for details):

$$𝛀(𝐫,\tau )=_𝒩d^2\nu \delta (𝐫𝐑(\nu ,\xi ,\tau ))\frac{𝐑}{\xi }𝑑\xi ,$$
(32)
where $`\nu `$ is a vortex line label, which belongs to the 2D manifold $`𝒩`$, $`\xi `$ is a longitudinal parameter along the line. The dynamics of vortex lines is determined by the variational principle $`\delta S_𝐑=\delta _𝐑𝑑\tau =0`$, with the Lagrangian of vortex lines having the following form , -:

$$_𝐑=\frac{1}{3}_𝒩d^2\nu \left(\left[𝐑_\tau \times 𝐑\right]𝐑_\xi \right)𝑑\xi _{}\{𝛀\{𝐑\}\},$$
(33)
where the subscripts $`\tau `$ and $`\xi `$ mean the corresponding partial derivatives. Performing the deformating substitution

$$𝐑=(X,Y,Z)=(\tau ^{\mu _1}\stackrel{~}{X},\tau ^{\mu _2}\stackrel{~}{Y},\tau ^{\mu _3}\stackrel{~}{Z}),$$
(34)
we obtain the Lagrangian for $`\stackrel{~}{𝐑}(\nu ,\xi ,\tau )`$:

$$_{\stackrel{~}{𝐑}}=\frac{1}{3}\left(\left[\stackrel{~}{𝐑}_\tau \times \stackrel{~}{𝐑}\right]\stackrel{~}{𝐑}_\xi \right)𝑑\xi d^2\nu $$

$$\frac{1}{8\pi }\frac{(\stackrel{~}{𝐑}_{\xi _1}(\nu _1,\xi _1)\stackrel{~}{𝐑}_{\xi _2}(\nu _2,\xi _2))}{|\stackrel{~}{𝐑}(\nu _1,\xi _1)\stackrel{~}{𝐑}(\nu _2,\xi _2)|}𝑑\xi _1d^2\nu _1𝑑\xi _2d^2\nu _2$$

$$\frac{1}{3\tau }(\stackrel{~}{X}_\xi \stackrel{~}{Y}\stackrel{~}{Z}(\mu _2\mu _3)+\stackrel{~}{Y}_\xi \stackrel{~}{Z}\stackrel{~}{X}(\mu _3\mu _1)$$

$$+\stackrel{~}{Z}_\xi \stackrel{~}{X}\stackrel{~}{Y}(\mu _1\mu _2))d\xi d^2\nu $$
(35)
It is interesting to note that the same Lagrangian for vortex lines corresponds to the usual Eulerian incompressible hydrodynamics in isotropic space with coordinates $`\stackrel{~}{𝐫}=(\stackrel{~}{x},\stackrel{~}{y},\stackrel{~}{z})=(\tau ^{\mu _1}x,\tau ^{\mu _2}y,\tau ^{\mu _3}z)`$, but in the presence of external straining potential velocity field

$$\stackrel{~}{𝐯}_{ext}(\tau ,\stackrel{~}{𝐫})=\tau ^1(\mu _1\stackrel{~}{x},\mu _2\stackrel{~}{y},\mu _3\stackrel{~}{z}).$$
(36)
In conclusion, let us say a few words about hydrodynamics in the homogeneous cosmological models of the other types , where the space is not flat. In this case, a quantitative analysis is difficult due to curvature of space and a complicated dependence of metrics on time, but the qualitative result about initial free motion regime for fluid elements remains valid. The reason is that an appropriately defined relative density $`\rho `$ is conserved in order of magnitude, as well as covariant components $`p_\alpha `$ of the momentum field, while contravariant components $`p^\alpha `$ tend to infinity at $`t0`$, like in the flat model. This fact means an infinite growth of the quantity $`p_\alpha p^\alpha `$ and approaching of the velocity magnitude $`\sqrt{v_\alpha v^\alpha }`$ to the speed of light, regardless field $`\rho `$. Therefore, a weak initial spatial inhomogeneity in distribution of $`p_\alpha (𝐚)`$ may result, after some time, in a strong spatial inhomogeneity of $`\rho `$.

These investigations were supported by the RFBR (grants 00-01-00929 and 99-02-16224), by the Russian State Program of Support of the Leading Scientific Schools (grants 00-15-96007 and 00-15-96699), and by the INTAS.


text:
# Spin fluctuations in a magnetically frustrated metal LiV₂O₄

\[

## Abstract

Inelastic neutron scattering is used to characterize spin fluctuations in the $`d`$-electron heavy fermion spinel $`\mathrm{LiV}_2\mathrm{O}_4`$. The spin relaxation rate, $`\mathrm{\Gamma }_Q`$, for $`Q=0.6`$ Å-1 is 1.4(2) meV at low temperatures and increases linearly with temperature at a rate of 0.46(8) kB. There is antiferromangetic short range order at low temperatures with a characteristic wave vector $`Q_c=0.64(2)`$ Å-1 and a correlation length of 6(1) Å. While warming shifts intensity towards lower $`Q`$, the staggered susceptibility peaks at a finite wave vector for $`T<80`$ K. The data are compared with conventional heavy fermion systems, geometrically frustrated insulating magnets, and recent theories for $`\mathrm{LiV}_2\mathrm{O}_4`$.

\]

Owing to geometrical frustration, magnetic B-site spinel systems $`\mathrm{AB}_2\mathrm{O}_4`$ consistently display unusual magnetic properties. Ti, V, and Cr spinels are particularly interesting because all 3d electrons occupy $`t_{2g}`$ orbitals that do not hybridize with oxygen orbitals. Accordingly, nearest neighbor magnetic exchange interactions dominate and this maximizes frustration. In addition such materials have only 3d $`t_{2g}`$ bands near the chemical potential and this leads to strong correlations in the charge sector as well. When the tetrahedral cation is di-valent (A=Zn, Mg) the octahedral B-site has integral valency and the materials are Mott insulators with geometrically frustrated magnetism. When the A-site is monovalent (Li) the B-site has non-integral valence resulting in a narrow-band metal. The combination of a strongly correlated metal and a spin system that cannot order due to geometrical frustration leads to materials with complex and unusual physical properties.

LiV2O4 is a case in point. A paramagnetic metal for $`T>0.01`$ K, the Sommerfeld constant increases below $`T=30`$ K reaching the largest value ever recorded in a d-electron system: 0.42 J mole-1K-2 for $`T=1.5`$ K. The susceptibility is also large at low $`T`$ and the Wilson ratio un-renormalized. To determine the origin of heavy fermion behavior in LiV2O4, we measured the generalized spin susceptibility as a function of energy ($`\mathrm{}\omega `$) and wave vector transfer ($`Q`$) using inelastic neutron scattering. At low temperatures ($`T`$), the response is indistinguishable from conventional rare earth or actinide heavy fermion system. $`\chi \text{}\text{}(Q,\omega )`$ peaks at a finite $`Q=0.64(2)`$ Å-1 and there is a small finite spin-relaxation rate, $`\mathrm{\Gamma }=1.4(2)`$ meV. On warming, the relaxation rate increases linearly with $`T`$ at a rate of $`0.46(8)k_B`$. Apart from the absence of a low $`T`$ phase transition, this behavior is reminiscent of insulating frustrated magnets. Our results strengthen the case that frustration is central to the physics of LiV2O4.

Since the discovery of heavy fermion behavior in LiV2O4, significant experimental and theoretical attention has been devoted to it. LDA band structure calculations have shown that 3d $`t_{2g}`$ orbital triplet bands are indeed alone in crossing the fermi level. While the trigonal splitting of the orbital triplet is less than 0.1 eV, the lower lying $`A_{1g}`$ singlet has a bandwidth of only 1 eV compared to the 2 eV bandwidth of the $`E_g`$ doublet. These observations have led to suggestions that an Anderson like model might describe LiV2O4 with the half filled $`A_{1g}`$ singlets playing the role of localized spins and the quarter filled $`E_g`$ doublet acting as the conduction band. While frustration plays a secondary role in these models, a recent paper by Fulde et al. proposes that the vanadium lattice of corner-sharing tetrahedra frustrates charge ordering and leads to isolated rings and finite length spin-1/2 and spin-1 chains. The latter have a Haldane spin gap, the former gapless excitations that are to account for the large linear term in the specific heat. A previous neutron scattering experiment reported a ferromagnetic (FM) to antiferromagnetic (AFM) cross over in LiV2O4. Our more complete data show that the staggered susceptibility peaks at a finite wave vector for $`T<80`$ K and that the heavy fermi liquid develops from a cooperative paramagnet with short range AFM spin correlations.

A 40 g powder sample of LiV2O4 was prepared by a solid state reaction technique described elsewhere. To reduce neutron absorption from 6Li we used 98.5% 7Li enriched starting materials. Rietveld refinement of neutron diffraction data showed that the sample is single phase spinel space-group $`Fd\overline{3}m`$ with lattice parameter $`a=8.227`$Å for $`T<70`$ K and oxygen on $`32e`$ sites with $`x`$=0.26122(2). We used the NIST cold neutron triple-axis spectrometer SPINS, with a large flat analyzer and a Position-Sensitive detector (PSD) to enhance the data collection rate. Full Width at Half Maximum energy resolution was 0.1 meV$`<\mathrm{\Delta }E<0.15`$ meV and angular resolution $`\mathrm{\Delta }2\theta 50^{}`$. Background was measured for all wave vectors and energy transfers reported. For large scattering angles ($`2\theta >20^o`$) this was done by detuning the analyzer. Smaller angle backgrounds were measured with the analyzer in reflection mode but no sample in the beam. The absolute efficiency of the instrument was

Fig. 1. Images of neutron scattering intensity from LiV2O4 versus wave vector and energy transfer at four temperatures.

measured to an accuracy of 15% using the (111) nuclear Bragg peak. The corresponding normalization factor was applied to background subtracted data to extract the normalized magnetic neutron scattering intensity

$`\stackrel{~}{I}(Q,\omega )={\displaystyle \frac{d\mathrm{\Omega }_{\widehat{𝐐}}}{4\pi }|\frac{g}{2}F(Q)|^2\underset{\alpha \beta }{}(\delta _{\alpha \beta }\widehat{Q}_\alpha \widehat{Q}_\beta )𝒮^{\alpha \beta }(𝐐,\omega )}.`$ (1)
Here $`F(Q)`$ is the magnetic form factor and $`𝒮^{\alpha \beta }(𝐐,\omega )`$ is the dynamic spin correlation function. For accurate determination of low $`T`$ relaxation rates (Figs. 2 and 3), we derived and then subtracted the $`T`$ independent elastic line shape by requiring that the resulting inelastic scattering satisfy detailed balance at all $`T`$.

Fig. 1 provides an overview of the data in the form of images of $`\stackrel{~}{I}(Q,\omega )`$ at four different temperatures. The horizontal yellow line is elastic nuclear incoherent scattering. Magnetic scattering is apparent at finite energy transfer and for $`Q<1`$ Å-1. In accordance with detailed balance, warming shifts intensity from positive to negative energy transfer. At low temperatures magnetic scattering is strongest at finite $`Q`$. At higher temperatures inelastic magnetic scattering increases monotonically with decreasing $`Q`$. The total magnetic scattering cross section is a measure of the fluctuating moment $`\delta m^2`$ within the dynamic range of the experiment. Integrating the low $`T`$ data over $`\mathrm{}\omega ϵ[0.2,3]`$ meV and $`Qϵ[0.4,0.9]`$ Å-1 we obtain $`\delta m^2=(2\mu _B)^2(3/2)\mathrm{}𝑑\omega Q^2𝑑Q\stackrel{~}{I}(Q,\omega )/Q^2𝑑Q=0.30(2)\mu _B^2/V`$. For comparison the squared effective  Fig. 2. (a)-(d) $`\stackrel{~}{I}(Q)`$ averaged over $`\mathrm{}\omega ϵ[0.2,0.8]`$ meV at various temperatures. Solid lines are guides to eye. (e)-(g) Dynamic susceptibility $`\chi \text{}\text{}(Q_0,\omega )`$ at $`Q_0=0.6`$ Å-1 derived from magnetic neutron scattering data via the fluctuation dissipation theorem. The solid lines are fits to Eq. 1. All frames show background subtracted data.

moment inferred from high temperature susceptibility measurements is 2.8$`\mu _B^2`$. Our data indicate a reduced moment in the low $`T`$ heavy fermion phase, which is consistent with a recent high field magnetization experiment.

From the birds eye view we proceed to examine constant$`\mathrm{}\omega `$ and constant$`Q`$ cuts through the data. The left column of Fig. 2 shows the $`Q`$-dependence of magnetic scattering intensity averaged over energy from 0.2 meV to 0.8 meV. At low temperatures, there is a broad peak centered at $`Q_c=0.64(2)`$ Å$`{}_{}{}^{1}=0.84(3)a^{}`$. Strong diffuse scattering at low $`T`$ is a hall-mark of frustrated magnets. The characteristic wave vectors for this scattering are $`Q_c=0.72(2)a^{}`$ for $`\mathrm{Y}_2\mathrm{Mo}_2\mathrm{O}_7`$, $`Q_c=1.01(2)a^{}`$ for $`\mathrm{ZnFe}_2\mathrm{O}_4`$, $`Q_c=1.7(1)a^{}`$ for $`\mathrm{ZnV}_2\mathrm{O}_4`$, and $`Q_c=1.98(6)a^{}`$ for $`\mathrm{ZnCr}_2\mathrm{O}_4`$. For $`\mathrm{ZnFe}_2\mathrm{O}_4`$ and $`\mathrm{ZnCr}_2\mathrm{O}_4`$ single crystals are available and it has been found that diffuse scattering is distributed over (different) parts of the Brillouin zone boundary.

It is interesting to note that $`Q_c`$ for $`\mathrm{LiV}_2\mathrm{O}_4`$ is close to values found in $`\mathrm{Y}_2\mathrm{Mo}_2\mathrm{O}_7`$ and $`\mathrm{ZnFe}_2\mathrm{O}_4`$, both materials that are expected to have longer range interactions than insulating Cr and V spinels. A possible interpretation is that longer range interactions are also present in metallic $`\mathrm{LiV}_2\mathrm{O}_4`$. Alternatively, and this could be checked by further analysis of existing band structure calculations, $`Q_c`$ for $`\mathrm{LiV}_2\mathrm{O}_4`$ may result from fermi surface nesting. The peak in the Q-dependence of magnetic neutron scattering from $`\mathrm{LiV}_2\mathrm{O}_4`$ has a Half Width at Half Maximum $`\kappa `$ 0.16(2) Å$`{}_{}{}^{1}0.24a^{}`$ at $`T=1.4`$ K corresponding to an AFM correlation length of only $`\xi 6(1)`$ Å$`=2.1(3)d_{VV}`$. Warming shifts intensity towards lower wave vectors until at $`T=80`$ K $`\stackrel{~}{I}(Q)`$ decreases monotonically with increasing $`Q`$ in the range probed.

The right column of Fig. 2 shows the corresponding excitation spectra. Following background subtraction, we used the fluctuation dissipation theorem to extract the imaginary part of the staggered spin susceptibility, $`\chi ^{\prime \prime }(Q,\omega )`$ from the data. Though the data were acquired at the “critical” wave vector $`Q_c=0.6`$ Å-1, $`Q`$averaged data were similar. Nonetheless, significant relaxation rate dispersion may be masked due to powder averaging. To parametrize the $`T`$ dependent spectra we used the following single imaginary pole susceptibility

$$\chi \text{}\text{}(Q,\omega )=\frac{\chi _Q\mathrm{\Gamma }_Q\omega }{\omega ^2+\mathrm{\Gamma }_Q^2}.$$
(2)
Here $`\mathrm{\Gamma }_Q`$ is the relaxation rate and $`\chi _Q`$ is the static staggered susceptibility. The lines through the data in Fig. 2 (e)-(h), show that Eq. 1 provides an adequate description of the spectra, as it does in many conventional heavy fermion systems.

To correlate changes in the $`Q`$dependence of scattering with anomalies in bulk properties, Fig. 3 shows the $`T`$dependence of inelastic magnetic neutron scattering at $`Q=0.6`$ Å-1 and 0.35 Å-1. Evolution from a finite $`Q`$ maximum to monotonically decreasing intensity with $`0.35<Q<1`$ Å-1 at $`\mathrm{}\omega =0.5`$ meV occurs in the same general temperature range as the low $`T`$ increase in the Sommerfeld ratio $`C/T`$. Thus as in conventional heavy fermion systems, the cross over to a coherent heavy fermi liquid is associated with the development of low energy, short-range AFM correlations. The squares show the difference between normalized horizontal and vertical field spin flip scattering at $`Q=0.35`$ Å-1 and provide proof that the low $`Q`$ scattering is indeed magnetic.

Fits to the data in Fig. 2 (e)-(h) yield the $`T`$ dependent staggered susceptibility and relaxation rate shown in Figs. 3 (b) and (c). Comparison to bulk ($`Q=0`$) susceptibility data (open symbols, frame (b)), reveals that the staggered susceptibility increases beyond the uniform susceptibility around $`T=80`$ K. Thus the Curie Weiss temperature $`|\mathrm{\Theta }_{CW}|=63`$ K, is the temperature scale for the appearance of short-range AFM correlations as is common for frustrated magnets. The solid line in Fig. 2 (b) shows that $`\chi _{Q_c}(T)`$ can be described by a Curie-Weiss law at high temperatures: $`\chi _{Q_c}(T)=(\mu _{Q_c}^2/3k_B\theta )/(1+T/\theta )`$ with $`\mu _{Q_c}=1.6(1)\mu _B`$, and $`\theta =7.5(10)`$ K. The reduced Curie Weiss temperature  Fig. 3. $`T`$ dependence of the following: (a) inelastic scattering intensity at two $`Q`$ and $`\mathrm{}\omega =0.5`$ meV. Open squares show the difference between horizontal and vertical field spin-flip neutron scattering at $`\mathrm{}\omega =0.5`$ meV and $`Q=0.35`$ Å-1. The data are normalized (left scale) and raw difference counts are on right axis. (b) bulk ($`Q=0`$) susceptibility and staggered susceptibility derived from fits to Eq. 1. (c) Relaxation rate from the same fits. Solid circles: $`Q_c=0.6`$ Å-1, triangles $`Q`$integrated data ($`0.6<Q<1.3`$ Å-1).

shows that magnetic neutron scattering at $`Q_c`$ is closer to accessing critical fluctuations than bulk $`Q=0`$ susceptibility data. The deviation from Curie Weiss behavior for $`T<T_c20`$ K (also seen at $`Q=0`$) indicates the development of correlations beyond nearest neighbors at the crossover to the coherent heavy fermion phase.

The relaxation rate versus temperature is shown in Fig. 3 (c). Solid and open symbols show fits to $`Q=0.6`$ Å-1 data and data integrated over the spherical shell in $`Q`$ space 0.6 Å$`{}_{}{}^{1}<Q<1.3`$ Å-1. As previously mentioned, the “critical” $`Q=Q_c`$ and “local” response have similar relaxation rates. Note however that a single-crystal is required to access the actual critical wave vector where the relaxation rate could be considerably reduced compared to powder data that only specify $`|Q|`$. The solid line in Fig. 3 (c) is a fit to $`\mathrm{\Gamma }_Q(T)=\mathrm{\Gamma }(0)+𝒞k_BT(T/\theta )^{\alpha 1}`$. The fit is to the higher quality $`Q=0.6`$ Å-1 data but similar numbers describe the wave vector averaged spin relaxation rate. We first discuss the residual $`T0`$ relaxation rate that refines to $`\mathrm{\Gamma }_Q(0)=1.4(2)`$ meV. In a crude band description of heavy fermion behavior, the product of the Sommerfeld constant and the low $`T`$ spin relaxation rate, $`\mathrm{\Gamma }(T=0)`$, should be proportional to the electron density but independent of the bandwidth. The low $`T`$ limit of this product is 0.60(4) meV J mole-1K-2=0.85(6) k$`{}_{}{}^{2}{}_{B}{}^{}`$/f.u. for $`\mathrm{LiV}_2\mathrm{O}_4`$ compared to an average of 1.0 $`k_B^2`$/f.u. for cerium heavy fermion systems. The numbers are consistent with a common link between spin fluctuations and the enhanced specific heat of these materials.

The $`T`$ dependence of $`\mathrm{\Gamma }_Q(T)`$ in $`\mathrm{LiV}_2\mathrm{O}_4`$ is close to linear ($`𝒞=0.46(8)`$ and $`\alpha =0.9(2)`$) in the range probed. While linear $`T`$ dependence of the spin relaxation rate is not unheard of in these materials, actinide and rare earth heavy fermion systems often display sub-linear $`T`$ dependence for $`T\mathrm{\Gamma }(T=0)/k_B`$. This behavior is generally associated with an unstable local moment. Linear $`T`$ dependence of the spin relaxation rate is however common among frustrated transition metal oxides. $`\mathrm{LiV}_2\mathrm{O}_4`$ has the largest Sommerfeld constant of the transition metal oxides. It is the only known vanadium oxide to remain cubic at low temperatures, and the compound borders an entropic spin glass phase in $`\mathrm{Li}_\mathrm{x}\mathrm{Zn}_{1\mathrm{x}}\mathrm{V}_2\mathrm{O}_4`$ for $`0.1<x<0.9`$. Our data for $`\mathrm{\Gamma }_Q(T)`$ provide an additional indication that the geometrically frustrated physics of spins on a lattice of corner-sharing tetrahedra is the crux of heavy fermion behavior in $`\mathrm{LiV}_2\mathrm{O}_4`$.

Theories of heavy fermion systems are generally non-lattice specific. While Fulde et al. were the first to focus on frustration, the theory appears to be inconsistent with our scattering data. The characteristic wave vector for fluctuations of spin-1/2 chain-lets and rings would be $`\pi /d_{VV}=\sqrt{2}a^{}`$, which is quite different from $`Q_c=0.84(3)a^{}`$ observed in Fig. 2 (d). Previous neutron scattering data from LiV2O4 were interpreted as indicating a cross over from AFM to FM fluctuations on heating above $`T=40`$ K. Fig. 3(b) shows that the uniform susceptibility is less than the staggered susceptibility for $`T<80`$ K, a clear indication that LiV2O4 enters the heavy fermion phase as an AFM correlated paramagnet. The apparent FM response in $`\mathrm{LiV}_2\mathrm{O}_4`$ may be a consequence of powder averaging scattering from a spin system where $`\kappa >Q_c`$. The previous scattering paper also concluded that the fluctuation rate of low Q decreased dramatically with increasing $`T`$. The present results indicate that this conclusion was an artifact of analyzing spectra taken at constant scattering angle. Constant-$`Q`$ spectra decouple changes in spatial and temporal correlations and show that the relaxation rate increases continuously in proportion to $`T`$ with no significant anomaly associated with entering the fermi liquid phase.

In summary, our experiment has revealed features both of a strongly correlated metal and of frustrated magnetism in LiV2O4. Short range correlations for $`T<<|\mathrm{\Theta }_{CW}|`$ and a linear rise in spin relaxation rate with $`T`$ are common features of insulating frustrated magnets. A residual low $`T`$ relaxation rate, a reduced effective moment at low energies, and an increasing AFM correlation length upon entering the coherent fermi liquid phase are features of a strongly correlated metal. Further progress towards understanding the mix of magnetic frustration and correlated electrons in LiV2O4 will require neutron scattering experiments on single crystalline samples and a lattice specific theory of heavy fermions.

We thank Y.B. Kim and D. Huse for helpful discussions. Work at SPINS is based upon activities supported by the NSF under DMR-9986442. Work at JHU was supported by the NSF through DMR-0074571.