# Quantum Spinodal Decomposition in Multicomponent Bose-Einstein Condensates

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## Abstract

We investigate analytically the non-equilibrium spatial phase segregation process of a mixture of alkali Bose-Einstein condensates. Two stages (I and II) are found in analogy to the classical spinodal decomposition. The coupled non-linear Schrödinger equations enable us to give a quantitative picture of the present dynamical process in a square well trap. Both time and length scales in the stage I are obtained. We further propose that the stage II is dominated by the Josephson effect between different domains of same condensate different from scenarios in the classical spinodal decomposition. Its time scale is estimated.

PACS$`\mathrm{\#}`$: 03.75.Fi; 64.75.+g

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The recent realizations of two  and three  component alkali Bose-Einstein condensates (BEC’s) in one trap provide us with new systems to explore the physics in otherwise unachievable parameter regimes . These systems have two noticeable advantages: the easy control of experimental parameters and the relative simplicity of the mathematical description. A direct comparison between theoretical calculations and experimental observations can be made. The purpose of the present paper is to explore one of main questions in the non-equilibrium statistical physics using those new systems: spinodal decomposition in a binary-solution system. It is a typical example of phase ordering dynamics: the growth of order through domain coarsening when a system is quenched from the homogeneous phase into a broken-symmetry phase . Systems quenched from a disordered phase into an ordered phase do not order instantaneously. Instead, different length scales set in as the domains form and grows with time, and different broken symmetry phases compete to select the equilibrium state. We show that it is possible to have an analogous spinodal decomposition in BEC’s, which manifests all the main phenomenology except those constrained by the trap size. In the following, we shall study the main features in this dynamical evolution process, starting from the homogeneous unstable state of BEC’s. To differentiate the present situation from the usual one, we shall call the present one the quantum spinodal decomposition, and the previous ones the classical spinodal decomposition.

We start from the time dependent non-linear Schrödinger equations

$`i\mathrm{}{\displaystyle \frac{}{t}}\psi _1`$ $`=`$ $`\left[{\displaystyle \frac{\mathrm{}^2}{2m_1}}^2+(U_1(x)\mu _1)+G_{11}|\psi _1|^2\right]\psi _1`$ (2)   
$`+G_{12}|\psi _2|^2\psi _1,`$   
and

$`i\mathrm{}{\displaystyle \frac{}{t}}\psi _2`$ $`=`$ $`\left[{\displaystyle \frac{\mathrm{}^2}{2m_2}}^2+(U_2(x)\mu _2)+G_{22}|\psi _2|^2\right]\psi _2`$ (4)   
$`+G_{12}|\psi _1|^2\psi _2.`$   
Here $`\psi _j(x,t)`$, $`m_j`$, $`U_j`$ with $`j=1,2`$ are the effective wave function, the mass, and the trapping potential of the $`j`$th condensate. The repulsive interaction between the $`j`$th condensate atoms is specified by $`G_{jj}`$, and that between 1 and 2 by $`G_{12}`$. The Lagrangian multipliers, the chemical potentials $`\mu _1`$ and $`\mu _2`$, are fixed by the relations $`d^3x|\psi _j(x,t)|^2=N_j,j=1,2`$, with $`N_j`$ the number of the $`j`$th condensate atoms. Eq. (1) and (2) are mean field equations, since we treat the effective wave functions as $`c`$ numbers, corresponding to the Hartree-Fock-Bogoliubov approximation. They provide a good description for the slow dynamics in both alkali BEC’s and the superfluid He4  on length scale larger than the range of microscopic interaction.

Experimentally, the trapping potentials $`\{U_j\}`$ are simple harmonic in nature. For the sake of simplicity and to illustrate the physics we shall consider a square well trapping potential $`U_j=U`$: zero inside and large (infinite) outside, unless otherwise explicitly specified.

We consider the strong mutual repulsive interaction

$$G_{12}>\sqrt{G_{11}G_{22}}.$$
(5)   
In this regime the equilibrium state for two Bose-Einstein condensates is a spatial segregation of two condensates, where two phases, the weakly and strong segregated phases, characterized by the healing length and the penetration depth, have been predicted . We shall use Eq. (1) and (2) under the condition (3) to study a highly non-linear dynamical process: The two condensates are initially in a homogeneously mixed state, then eventually approach the phase segregated state. In the same mean field treatment as in Ref., we find that this dynamical process can be classified into two main stages: The initial highly non-equilibrium dynamical growth in the stage I, where the dynamics is governed by the fastest growth mode, and the stage II of approach to equilibrium where the dynamics is governed by the slowest mode. The stage II is typical of a relaxation process near equilibrium. However, we shall show again it is governed by a quantum effect, namely, the Josephson effect.

Stage I: Fastest Growth Mode.  The coupled non-linear Schrödinger equations have an obvious homogeneous solution: Inside the trap the condensate densities $`|\psi _j|^2=\rho _{j0}`$, $`\rho _{j0}=N_j/V,`$ with $`V`$ the volume of the square well potential trap, and the chemical potentials $`\mu _1=G_{11}\rho _{10}+G_{12}\rho _{20}`$ and $`\mu _2=G_{22}\rho _{20}+G_{12}\rho _{10}`$. This is the initial condition of the present problem.

To look for the fastest growth mode out of the homogeneous state, we start with small fluctuations from the homogeneous state. This is consistent with the usual stability analysis . Our approach here is to emphasize the connection with the physics of the classical spinodal decomposition and the role played by the Josephson relationships. Define

$$\psi _j(x,t)=\sqrt{\rho _j(x,t)}e^{i\theta _j(x,t)},$$
(6)   
and define the density fluctuations $`\delta \rho _j=\rho _j\rho _{j0}`$ and the phase fluctuations $`\theta _j`$, and assume they are small: $`|\delta \rho _j|/\rho _j,|\theta _j|<<1`$. The definition of the phase fluctuations here has made use of the implicit assumption that there is no net current in the condensate. To the linear order, we have from Eqs.(1,2), after eliminating the phase variables,

$$\frac{^2}{t^2}\left(\begin{array}{c}\delta \rho _1\\ \delta \rho _2\end{array}\right)=\left(\begin{array}{cc}b_1& \frac{\rho _{10}}{m_1}G_{12}^2\\ \frac{\rho _{20}}{m_2}G_{12}^2& b_2\end{array}\right)\left(\begin{array}{c}\delta \rho _1\\ \delta \rho _2\end{array}\right).$$
(7)   
with $`b_j=\frac{\mathrm{}^2}{4m_j^2}^4+\frac{\rho _{j0}}{m_j}G_{jj}^2`$. We look for the solution of the form

$`\left(\begin{array}{c}\delta \rho _1\\ \delta \rho _2\end{array}\right)=\left(\begin{array}{c}A\\ B\end{array}\right)e^{i(𝐪𝐫\omega t)},`$

with $`A,B`$ constants. There are two branches of solution for Eq. (5). For one branch, the frequency is always real. For another branch which we denote by $`\omega _{}`$, it can be imaginary. An imaginary frequency $`\omega _{}`$ shows that the initial homogeneously mixed state is unstable. It is straightforward to verify that the sufficient condition for the appearance of imaginary frequency for small enough wave number $`q`$ is the validity of the inequality Eq.(3). The modes with imaginary frequencies will then grow exponentially with time. Unlike the usual situation near equilibrium, this growth from the present non-equilibrium homogeneously mixed state will be dominated by the fastest growth mode. This is precisely the same case as in the initial stage of the classical spinodal decomposition.

To get a concrete understanding of the physical implications of Eq. (5) in the stage I we consider a case relevant to recent experiments where particles of the two condensates have the same mass, $`m_1=m_2=m`$. In this case we find the wavenumber corresponding to the most negative $`\omega _{max}^2`$ is

$$q_{max}^2=\frac{m}{\mathrm{}^2}\left[\sqrt{b_0^2+4\rho _{10}\rho _{20}G_{11}G_{22}\left(\frac{G_{12}^2}{G_{11}G_{22}}1\right)}b_0\right],$$
(8)   
and

$$\omega _{max}=i\frac{\mathrm{}}{2m}q_{max}^2,$$
(9)   
with $`b_0=\rho _{10}G_{11}+\rho _{20}G_{22}`$. The physics implied in Eqs. (6,7) is as follows. Starting from the initial homogeneous mixture of the two condensates, on the time scale given by

$$t_I=1/|\omega _{max}|,$$
(10)   
domain patterns of the phase segregation with the characteristic length

$$l_I=1/q_{max}$$
(11)   
will appear. Particularly, for the weakly segregated phase of $`G_{12}^2/G_{11}G_{22}10`$, we have the length scale $`l_I^1=\sqrt{2}/\sqrt{\mathrm{\Lambda }_1^2+\mathrm{\Lambda }_2^2}`$, and for the strongly segregated phase of $`G_{12}^2/G_{11}G_{22}1\mathrm{}`$, we have $`l_I^1=\sqrt{2}/\sqrt{\mathrm{\Lambda }_1\mathrm{\Lambda }_2}`$. Here $`\mathrm{\Lambda }_j=\xi _j/\sqrt{G_{12}/\sqrt{G_{11}G_{22}}1}`$ and $`\xi _j=\sqrt{\mathrm{}^2/2m_j\mathrm{\hspace{0.33em}1}/\rho _{j0}G_{jj}}`$ are the penetration and healing lengths in the binary BEC mixture . Those length and times scales can be measured experimentally. We will come back to the experimental situation below.

After the stage I of fast growth into the domain pattern characterized by the length scale $`l_I`$, the system will gradually approach the true ground state of the complete phase segregation: one condensate in one region and the second condensate in another region. This stage is slow, dominated by the slowest mode, and is the subject of stage II.

It is now evident that the stage I of the growth of binary BEC’s shares the same phenomenology of the initial stage of the classical spinodal decomposition: the domination of the fastest growth mode, the appearance of domains of segregated phases, and the conservation of particle numbers. There are, however, two important differences. First, the dynamical evolution of the binary BEC’s is governed by a coupled nonlinear time dependent Schrödinger equations, not by a nonlinear diffusion equation supplemented with the continuity equation, the Cahn-Hilliard equation. There is no external relaxation process for the present wave functions. Secondly, the energy of the binary BEC’s is conserved during the growth process, not as in the case of classical spinodal decomposition where the system energy always decreases.

Stage II: Merging and Oscillating between Domains.  The BEC binary mixture occurs in a trap. This finite size effect of the droplet leads to the broken symmetry of the condensate profiles , which tends to separate the condensates in mutually isolated regions. This implies that there is no contact between different domains of the same condensates formed in the stage I. The classical spinodal process involves diffusion. An estimate of the diffusion constant for the BEC system can be made from kinetics theory. The ratio of the time scales for quantum and classical particle transport is of the order of the ratio of the BEC cloud size to the de Broglie wavelength. This is much smaller than one for the experimental systems of interest. The classical diffusion process is thus not important. Because the domains are not connected and because the diffusion for the BEC mixture is extremely low, all the mechanisms for the late stage classical spinodal decomposition are not applicable. We propose that it is the Josephson effect that is responsible for the approach to equilibrium in the stage II. Two models for the Josephson effect, the ‘rigid pendulum’ model and the ‘soft pendulum’ model will be discussed. They both give the same time scale when the ‘Rabi’ frequency is small.

Let us consider the specific case of two domains of condensate 1 separated by a domain with width $`d`$ of condensate 2. The ability of condensate 1 to tunnel through condensate 2 is described by the penetration depth $`\mathrm{\Lambda }`$, as discussed in Ref. . Hence the probability of condensate 1 to tunnel through condensate 2 can be estimated as

$$p=e^{2d/\mathrm{\Lambda }},$$
(12)   
when $`p`$ is much smaller than 1. The finiteness, though small, of the tunneling probability suggests that it is the Josephson effect responsible for the relaxation process in the stage II. The Josephson effect leads to the merging of two domains of the same condensate. The dynamics of such motion may be governed by the ‘rigid pendulum’ Hamiltonian for a Josephson junction :

$`H(\varphi ,n)=E_J(1\mathrm{cos}\varphi )+{\displaystyle \frac{1}{2}}E_Cn^2,`$

where $`E_J`$ is the Josephson coupling energy determined by the tunneling probability, $`n=(n_xn_y)/2`$ is the particle number difference between the numbers of particles, $`n_x`$ and $`n_y`$, in the two domains, and $`E_C\mu /n`$ is the ‘capacitive’ energy due to interactions. In the absence of external constraints, $`\mu =E_Cn`$. The phase difference $`\varphi `$ between the two domains is conjugated to $`n`$, as in usual Josephson junctions. Under the appropriate condition, such as low temperature and smallness of the capacitive energy, there may be an oscillation between the two domains of condensate 1 separated by condensate 2. In such a case, we may estimate that the oscillation period $`t_{II}=2\pi /\omega _{JP}`$, with the so-called Josephson plasma frequency

$$\omega _{JP}=\frac{\sqrt{E_CE_J}}{\mathrm{}}.$$
(13)   
For small tunneling probability, the Josephson junction energy may be estimated as $`E_J=n_T^{1/3}\mathrm{}\omega _0e^{2d/\mathrm{\Lambda }}`$, and the capacitive energy as $`E_C=\frac{2}{5}\left(n_T/2\right)^{0.6}\left(15a_{11}/a_0\right)^{0.4}\mathrm{}\omega _0`$. Here $`\omega _0`$ is the harmonic oscillator frequency for condensate 1 in a harmonic trap, $`a_0=\sqrt{\mathrm{}/m_1\omega _0}`$ is the corresponding oscillator length, the $`a_{11}`$ is the scattering length of condensate 1, and $`n_T=n_x+n_y`$ is the total number of particles in domain $`x`$ and $`y`$. The oscillatory time scale between the domains determines by the Josephson plasma frequency

$$t_{II}^1=\left(\frac{2a_0}{15a_{11}n_T}\right)^{2/15}\frac{\omega _0}{2\pi }e^{d/\mathrm{\Lambda }}.$$
(14)   
The rigid pendulum Hamiltonian would give a good description when $`n<<n_T`$. Another description of the Josephson effect uses the ‘soft pendulum’ Hamiltonian proposed in Ref. . In the parameter regime relevant current experimental situations both of them give the same order of magnitude estimate for $`t_{II}`$.

Given the Josephson effect is the dominant mechanism in the stage II, the time scale to arrive at the ground state will be determined by the Josephson effect at the final two domains, in which the two domains of condensate 1 is separated by the domain of condensate 2, in the manner of $`\mathrm{1\hspace{0.17em}2\hspace{0.17em}1\hspace{0.17em}2}`$ spatial configuration for the case of equal numbers of the condensates. The width $`d`$ of each domain is then $`D/4`$, with $`D`$ the size of the trap. According to the above analysis, the largest time scale determined by Eq.(12), the slowest mode, in the stage II is $`t_{II}`$. The arrangement of $`\mathrm{1\hspace{0.17em}2\hspace{0.17em}1}`$ spatial configuration may also occur here, in which it is more likely for condensate 2 to tunnel through 1 to the edge of the trap, because of the larger tunneling probability. We next turn our attention to the experimental situation.

The first question is whether the quantum spinodal decomposition discussed above can happen or not. In terms of the atomic scattering lengths of condensate atoms $`a_{jj}`$, the interactions are $`G_{jj}=4\pi \mathrm{}^2a_{jj}/m_j`$. The typical value of $`a_{jj}`$ for <sup>87</sup>Rb is about $`50`$Å. The typical density realized for the binary BEC mixture is about $`\rho _{i0}10^{14}/cm^3`$. Hence the healing length is $`\xi =\sqrt{(\mathrm{}^2/2m)(1/G_{jj}\rho _{j0})}=\sqrt{1/(8\pi a_{jj}\rho _{j0})}3000`$Å. For the different hyperfine states of <sup>87</sup>Rb, it is known now that $`G_{12}/\sqrt{G_{11}G_{22}}>1`$. Hence the ground state of the phase segregated phase can be realized. Also, that both the healing length and the penetration depth are smaller than the trap size  validates the application of results obtained in the square well trapping potential to the harmonic one. Therefore, the quantum spinodal decomposition can happen.

Experimentally, starting from the initially homogeneous state, after a short period of time a domain pattern does appear. Then a damped oscillation between the domain pattern has been observed. Eventually the binary BEC mixture sets to the segregated phase . If we take $`G_{12}/\sqrt{G_{11}G_{22}}=1.04`$, the penetration depth is $`\mathrm{\Lambda }=\xi /\sqrt{G_{12}/\sqrt{G_{11}G_{22}}1}1.5\mu `$m. The length scale $`l_I`$ determined by Eq.(9) in the stage I is $`1.5\mu `$m, which is the same order of magnitude in comparison with experimental data. This length is also comparable to the domain wall width seen experimentally. The corresponding time scale $`t_I`$ (Eq. (8)) is then 6 ms, again the same order of magnitude, though both estimated $`l_I`$ and $`t_I`$ are somewhat smaller. For stage II, $`d/\mathrm{\Lambda }`$ is of the order of $`n_d`$, the number of domains formed in stage I. For the experiment of interest to use, $`n_d2`$. If we assume that the damped oscillation to equilibrium observed experimentally is the stage II discussed here, taking the total number of particle $`N_1=10^6`$, we find the period according to Eq. (12) is 30 ms, comparable to the experimental value.

For the stage I, our above analysis shows that it is insensitive to the damping. At this moment we do not have a reliable estimation of the damping in the Josephson oscillation, whose existence has been indicated experimentally. Nevertheless, given the uncertainty in the value of $`G_{12}`$ or $`a_{12}`$, we conclude that the stage II of the quantum spinodal decomposition may have been observed.

Periodic-like structures have also been observed in the phase segregation of spin 1 Na mixtures . For the definiteness of analysis we have presently focused on the binary case, but we believe a similar physical picture of quantum spinodal decomposition applies to that case as well.

Finally, we point out that the length and time scales for Rb mixtures is controlled by the difference of $`r=G_{12}/\sqrt{G_{11}G_{22}}`$ and 1. Since $`r`$ is close to 1 experimentally, the data can provide for a very sensitive estimate of r-1. Since this parameter determines $`\mathrm{𝐛𝐨𝐭𝐡}`$ the time and length scale of stage I, it is a self-consistent check on the physical picture provided here.

This work was supported in part by a grant from NASA (NAG8-1427), and by Swedish NFR (PA). One of us (PA) thanks the Bartol Research Institute as well as the Department of Physics at University of Delaware for the pleasant hospitality, where the main body of the work was completed. We also thank the D. S. Hall for sending us their data.