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# Local Inhomogeneity Effects on Nucleation Process in a High External Bias Submitted to Phys. Rev. B.

## I Introduction

Nucleation process is one of the most universal phenomena found in various areas in physics from cosmology to condensed matter physics providing the mechanism for the onset of first-order transitions . Besides classical nucleation due to thermal fluctuations, nucleation due to quantum tunneling has attracted interest for many years as macroscopic quantum phenomena. Although quantum nucleation has been studied theoretically in the pioneering issue , it is just recently that observation of quantum nucleation has become possible owing to the progress in experimental techniques. At present, quantum nucleation has been observed experimentally in low-temperature condensed-matter systems: $`{}_{}{}^{4}\mathrm{He}`$-$`{}_{}{}^{3}\mathrm{He}`$ liquid solutions , cavitation in $`{}_{}{}^{4}\mathrm{He}`$ liquid , nucleation of $`{}_{}{}^{4}\mathrm{He}`$ solids . Nucleation of magnetic domain in thin films has also been discussed theoretically . Quantum creation of a kink-antikink pair can be regarded as one-dimensional nucleation, and has been studied both experimentally and theoretically in dislocation motion in solids , and sliding of charge density waves (CDWs) , though in the latter system interpretations of the experimental results are not settled . I believe that long Josephson junctions  are also suitable to observe quantum nucleation of a soliton pair.

In many theoretical issues, nucleation processes have been restricted to the situation that a stable phase is formed in the otherwise homogeneous background of an unstable phase. In several literatures, the nucleation rates in the presence of strong inhomogeneities have also been studied by using a single-variable model . In such studies, direct evaluation of the impurity strength from the nucleation rate is difficult, because the parameters of the single-variable model cannot be related clearly to the impurity strength. In this paper, we study moderate inhomogeneities, which can be controlled by an external parameter from the nearly-homogeneous region to the strongly-inhomogeneous region. This crossover region has not been studied in detail, and provides useful information of the impurity strength, because the nucleation rates are very sensitive to the impurity strength in this region.

In this paper, we study how the nucleation process changes in the presence of local moderate inhomogeneity. As a starting point, a highly-biased region is investigated where the potential can be expressed by a cubic polynomial. The nucleation rate is calculated based on the ‘bounce’ method  for quantum tunneling regimes, and on Kramers’ law for thermal activation regimes . We concentrate on nucleation processes in one-dimensional systems which correspond to the kink-antikink nucleation. We show that extension to higher dimensions is not easy since the nucleation rates are affected by details of local inhomogeneity profiles such as an impurity size.

The nucleation rate is expressed in the form $`\mathrm{\Gamma }=A\mathrm{exp}(B/\mathrm{})`$, where $`A`$ and $`B`$ are called as a prefactor and an exponent, respectively. The exponent $`B`$ depends on the bias $`f`$ as

$$B(f_cf)^\gamma ,$$
(1)
where $`f_c`$ is a classical threshold bias at which the potential barrier disappears. It should be stressed that the value of $`\gamma `$ is modified by inhomogeneities. The modification of $`\gamma `$ has first been discussed in the quantum sliding of CDWs by Yumoto et.al . They have calculated the nucleation rate by reducing the model to a single-variable problem with use of path integrals, and have reported that the value of $`\gamma `$ increases as the impurity strength is enlarged. This method, however, is so complicated that it is difficult to discuss the origin of the change of $`\gamma `$ clearly, and also to examine the validity of the approximation adopted there. In this paper, we study inhomogeneity effects without any reduction to a single-variable problem. It is claimed that our results are explained by the ‘dimensionality’ of nucleation, which has been pointed out by the author in ref. .

We consider one isolated impurity in a system with the size $`L`$. The results obtained in this paper are also applicable to systems with the dilute impurities by taking the average impurity distance as $`L`$. In the limit $`L\mathrm{}`$, nucleation occurs dominantly in homogeneous regions of the samples, and no impurity effects appear. The inhomogeneity effects appear only when $`L`$ is below a crossover value $`L_{\mathrm{cr}}`$. Within the bounce method, $`L_{\mathrm{cr}}`$ is shown to be obtained by calculating the prefactor $`A`$. Here, we should note that the validity of the bounce method is not guaranteed generally for the many-body problems. We also discuss the validity of the bounce method when it is applied to the nucleation problem in the presence of the impurities.

This paper is organized as follows. The model Hamiltonian is given in Sec. II. The quantum tunneling rate is formulated and calculated for one-dimensional systems in Sec. III. We study the thermal regime in Sec. IV briefly, and the extension to higher-dimensional systems and justification of the bounce method are discussed in Sec. V. Finally, results are summarized in Sec. VI.

## II Model

In this paper, nucleation rates are calculated based on the equation of motion

$$\varphi _{tt}^2\varphi +\frac{V}{\varphi }=0.$$
(2)
Here, $`\varphi (\stackrel{}{x},t)`$ is a $`(d+1)`$-dimensional field, and $`x`$ and $`t`$ are scaled by the characteristic length and time, respectively. Dissipation is assumed to be weak enough, but not extremely weak so that the system is in a thermal equilibrium in a metastable well. We concentrate on one-dimensional systems described by the equation

$$\varphi _{tt}\varphi _{xx}+\frac{V}{\varphi }=0,$$
(3)
and the higher-dimensional systems are discussed only in Sec. V. The potential energy is assumed to consist of two parts as $`V(\varphi ,x)=V_0(\varphi )+V_{\mathrm{imp}}(\varphi ,x)`$, where $`V_0(\varphi )`$ is a homogeneous part and $`V_{\mathrm{imp}}(\varphi ,x)`$ describes an inhomogeneity.

As for the homogeneous part $`V_0(\varphi )`$, we assume: (1) the potential has at least one metastable point $`\varphi _0`$; (2) the energy barrier in $`V_0(\varphi )`$ is controlled by an external parameter like an external field. One typical example for $`V_0(\varphi )`$ is a tilted cosine potential

$$V_0(\varphi )=(1\mathrm{cos}\varphi )f\varphi .$$
(4)
Another example is the $`\varphi ^4`$-model with a bias

$$V_0(\varphi )=\frac{\varphi ^2}{2}+\frac{\varphi ^4}{4!}f\varphi .$$
(5)
The type in (4) has been used for long Josephson junctions, dislocation in solids, and CDW systems, while the type in (5) describes an effective model for nucleation of a stable phase from an unstable background.

In this paper, the characteristic action of the systems is assumed to be large as compared with the Planck constant. In such situations, the quantum nucleation appears only when the bias $`f`$ is controlled near the classical threshold $`f_c`$ at which the metastable state of the potential $`V_0(\varphi )`$ disappears. Note that $`f_{\mathrm{c},0}=1`$ for the tilted cosine potential and $`f_{\mathrm{c},0}=2\sqrt{2}/3`$ for the $`\varphi ^4`$-model in the absence of impurities. Near $`f=f_{\mathrm{c},0}`$, the potentials in (4) and (5) form can be approximated commonly by quadratic-plus-cubic polynomials around a metastable point $`\varphi =\varphi _0`$ as

$`V_0(\varphi )V_0(\varphi _0)`$ $``$ $`{\displaystyle \frac{a(f_{\mathrm{c},0}f)^{1/2}}{2}}(\varphi \varphi _0)^2`$ (6)
$``$ $`{\displaystyle \frac{b}{6}}(\varphi \varphi _0)^3.`$ (7)
Here, $`a=O(1)`$ and $`b=O(1)`$. To be explicit, $`a=2^{1/2}`$, $`b=1`$ for the tilted cosine potential (4), while $`a=2^{3/4}`$, $`b=2^{1/2}`$ for the $`\varphi ^4`$-model (5).

The equation of motion (3) describes dynamics of a string in the potential $`V(\varphi )`$ shown in Fig. 1. When the string is initially located in a metastable well, it stays there for a while, and then begins to move towards lower energy states. If the system size is large enough, the transition from metastable states to moving states occurs through local deformation of the string accompanied with the creation of one kink-antikink pair. This transition can be regarded as ‘nucleation’ when the metastable(stable) state is related to the metastable(stable) phase.

The local inhomogeneity is introduced by $`V_{\mathrm{imp}}(\varphi )`$ as

$$V_{\mathrm{imp}}(\varphi ,x)=\delta (x)h(\varphi ),$$
(8)
where $`\delta (x)`$ is a delta function, and $`h(\varphi )`$ is a function defined around the metastable point. This type of impurity potentials has been studied theoretically in CDW systems  and long Josephson junctions . The potential form (8) can be obtained not only for impurities but also for inhomogeneities of external forces, modulation of barrier heights, and edge effects. (Details are summarized in Appendix A.) At high biases, since the impurity effect is determined by a small modulation of $`\varphi `$ around the metastable point $`\varphi _0`$, the inhomogeneity potential can be approximated as

$$V_{\mathrm{imp}}(\varphi ,x)\epsilon \delta (x)(\varphi \varphi _0).$$
(9)
Here, $`\epsilon `$ describes the impurity strength. This local potential can be regarded as a local force on a string at $`x=0`$ as shown in Fig. 1. For $`\epsilon >0`$ ($`\epsilon <0`$), the string is attracted towards the positive(negative) direction of $`\varphi `$. As a result, the nucleation is enhanced around $`x=0`$ for $`\epsilon >0`$, and suppressed for $`\epsilon <0`$.

The appearance of the impurity effect is explained intuitively as follows. The nucleation rate $`\mathrm{\Gamma }`$ is expected to consist of two parts as $`\mathrm{\Gamma }=\mathrm{\Gamma }_{\mathrm{bulk}}+\mathrm{\Gamma }_{\mathrm{imp}}`$. Here, $`\mathrm{\Gamma }_{\mathrm{bulk}}`$ is the nucleation rate in the homogeneous region far from an impurity, and $`\mathrm{\Gamma }_{\mathrm{imp}}`$ is a contribution near the impurity. Using the system size $`L`$, the bulk part is estimated as $`\mathrm{\Gamma }_{\mathrm{bulk}}\mathrm{\Gamma }_0L`$, where $`\mathrm{\Gamma }_0`$ is the nucleation rate per unit length in the absence of the impurities. The impurity part $`\mathrm{\Gamma }_{\mathrm{imp}}`$ is independent of $`L`$, and is estimated as $`\mathrm{\Gamma }_{\mathrm{imp}}\mathrm{\Gamma }_0\mathrm{exp}(\mathrm{\Delta }U/\mathrm{}\omega _0)`$, where $`\mathrm{\Delta }U`$ is the energy gain at the impurity site, and $`\omega _0`$ is an attempt frequency around the metastable state. If the system size $`L`$ is large enough, the bulk part $`\mathrm{\Gamma }_{\mathrm{bulk}}`$ dominates the impurity part $`\mathrm{\Gamma }_{\mathrm{imp}}`$, and no impurity effects appear. However, by controlling $`\mathrm{\Delta }U`$, $`\mathrm{\Gamma }_{\mathrm{imp}}`$ can dominate $`\mathrm{\Gamma }_{\mathrm{bulk}}`$. The inequality $`\mathrm{\Gamma }_{\mathrm{imp}}\mathrm{\Gamma }_{\mathrm{bulk}}`$ leads

$$\mathrm{\Delta }U\mathrm{}\omega _0\mathrm{log}L.$$
(10)
Since the condition (10) shows of a weak system-size dependence of the condition (10) through the logarithmic function of $`L`$, it is expected to be feasible in experimental systems. The inequality (10), which can be derived more accurately in Sec. III D, will be assumed in the next section.

In this paper, we further assume $`\epsilon >0`$ in (9), because $`\mathrm{\Gamma }_{\mathrm{imp}}`$ never dominates the bulk part $`\mathrm{\Gamma }_{\mathrm{bulk}}`$ in case of $`\epsilon <0`$.

## III QUANTUM TUNNELING REGIME

### A Formulation and Scaling Analysis

The quantum nucleation rate in the presence of the impurity is formulated by a semiclassical method as follows. The partition function of the system is expressed in terms of path integrals as

$`Z`$ $`=`$ $`{\displaystyle 𝒟\varphi (x,\tau )\mathrm{exp}\left(\frac{S[\varphi (x,\tau )]}{\mathrm{}}\right)},`$ (11)
$`S[\varphi (x,\tau )]`$ $`=`$ $`{\displaystyle _{L/2}^{L/2}}\mathrm{d}x{\displaystyle _0^\mathrm{}\beta }\mathrm{d}\tau [{\displaystyle \frac{1}{2}}\varphi _x^2+{\displaystyle \frac{1}{2}}\varphi _\tau ^2`$ (12)
$`+`$ $`V_0(\varphi )+V_{\mathrm{imp}}(x,\varphi )],`$ (13)
where $`\mathrm{}`$ is a dimensionless Planck constant normalized by the characteristic frequency, length, and energy of the system, $`\tau =it`$ is an imaginary time, and $`\beta =1/k_\mathrm{B}T`$ is an inverse temperature. The potential forms are given by (7) and (9). By rescaling the variables as

$`x`$ $`=`$ $`x^{}\left(a\sqrt{f_{\mathrm{c},0}f}\right)^{1/2},`$ (14)
$`\tau `$ $`=`$ $`\tau ^{}\left(a\sqrt{f_{\mathrm{c},0}f}\right)^{1/2},`$ (15)
$`\varphi `$ $`=`$ $`{\displaystyle \frac{a\sqrt{f_{\mathrm{c},0}f}}{b}}\phi +\varphi _0,`$ (16)
the action is rewritten as

$`S[\phi (x,\tau )]={\displaystyle \frac{a^2(f_{\mathrm{c},0}f)}{b^2}}{\displaystyle _{\stackrel{~}{L}/2}^{\stackrel{~}{L}/2}}dx^{}{\displaystyle _0^{\mathrm{}\stackrel{~}{\beta }}}d\tau ^{}`$ (17)
$`\times \left[{\displaystyle \frac{1}{2}}\phi _x^2+{\displaystyle \frac{1}{2}}\phi _\tau ^2+{\displaystyle \frac{1}{2}}\phi ^2{\displaystyle \frac{1}{3!}}\phi ^3\stackrel{~}{\epsilon }\delta (x^{})\phi \right].`$ (18)
Here, $`\stackrel{~}{L}=La^{1/2}(f_{\mathrm{c},0}f)^{1/4}`$ and $`\stackrel{~}{\beta }=\beta a^{1/2}(f_{\mathrm{c},0}f)^{1/4}`$ is a scaled length and inverse temperature, respectively. The impurity effect is described only through an effective impurity strength $`\stackrel{~}{\epsilon }`$ defined by

$$\stackrel{~}{\epsilon }=\epsilon a^{3/2}b(f_{\mathrm{c},0}f)^{3/4}.$$
(19)
This effective impurity strength depends on both the bare impurity strength $`\epsilon `$ and external bias $`f`$. Even if $`\epsilon `$ is fixed, we can control the strength of the impurity effect by changing the external current; the impurity effect is enhanced by controlling the external current near the threshold current $`f_c`$.

The partition function given in (11) and (13) is evaluated by integrating the partition function around stationary solutions up to second-order fluctuations. The stationary solutions are determined by

$$\frac{\delta S}{\delta \phi }=\phi _{\tau ^{}\tau ^{}}\phi _{x^{}x^{}}+\phi \frac{\phi ^2}{2}\stackrel{~}{\epsilon }\delta (x^{})=0.$$
(20)
There exist two types of solutions for this equation. One is a stable solution $`\phi _0(x^{})`$ independent of $`\tau ^{}`$, and the other is a ‘bounce’ solution $`\phi _\mathrm{B}(x^{},\tau ^{})`$. Since the system has a metastable state, the free energy $`F=\beta ^1\mathrm{log}Z`$ gains an imaginary part. Then, the decay rates are given by $`\mathrm{\Gamma }=2\mathrm{I}\mathrm{m}F`$. This formula, derived through the ‘bounce’ method, was first applied to the thermal activation regime , and extended to the quantum tunneling regime . The nucleation rate is now written in the form

$$\mathrm{\Gamma }=A\mathrm{exp}(B/\mathrm{}),$$
(21)
and the exponent $`B`$ and prefactor $`A`$ are given as

$`B`$ $`=`$ $`S[\phi _\mathrm{B}(x^{},\tau ^{})]S[\phi _0(x^{})],`$ (22)
$`A`$ $`=`$ $`{\displaystyle \frac{\overline{a}(T)}{\beta \mathrm{}}}{\displaystyle \underset{i=1}{\overset{\mathrm{}}{}}}\left({\displaystyle \frac{|\lambda _i^{(\mathrm{B})}|}{\lambda _i^{(0)}}}\right)^{1/2}.`$ (23)
Here, $`\overline{a}(T)`$ is a temperature-dependent factor, and takes 1 for $`T<T_0`$, and $`T_0/T`$ for $`T>T_0`$ , and $`\lambda _i^{(\mathrm{B})}`$s ($`\lambda _i^{(0)}`$s) are the frequencies of eigenmodes around the bounce(stable) solution determined by the equation

$`(_{\tau ^{}\tau ^{}}_{x^{}x^{}}+1\varphi _{\mathrm{B},0}(x^{},\tau ^{}))\psi _i^{(\mathrm{B},0)}(x^{},\tau ^{})`$ (24)
$`=\lambda _i^{(\mathrm{B},0)}\psi _i^{(\mathrm{B},0)}(x^{},\tau ^{}).`$ (25)
All the eigenvalues around the stable solution are positive ($`\lambda _i^{(0)}1`$). The lowest eigenvalue $`\lambda _1^{(B)}`$ is negative due to the metastability of the bounce solution $`\phi _\mathrm{B}`$. The second lowest eigenvalue $`\lambda _2^{(B)}`$ is always zero due to the translational symmetry of $`\phi _\mathrm{B}`$ in the $`\tau `$ direction. This mode must be treated by the Fadeev-Popov method, and the expression of the prefactor is modified as

$$\frac{1}{\sqrt{\lambda _2^{(B)}}}\sqrt{\frac{B}{2\pi \mathrm{}}}_0^{\mathrm{}\stackrel{~}{\beta }}𝑑\tau _0^{},$$
(26)
where $`\tau _0^{}`$ denotes the center position of the bounce. For the weak impurity, the third eigenvalue $`\lambda _3^{(B)}`$ also approaches zero due to the translational symmetry of $`\phi _\mathrm{B}`$ in the $`x`$-direction. We study this mode in Sec. III D in detail.

### B Dimensional Crossover

The bias dependence of the exponent $`B`$ can be discussed from the viewpoint of the ‘dimensional crossover’. This viewpoint has been discussed in several physical systems such as CDWs , and long Josephson junctions  in the context of the system-size dependences. The application to impurity problems has been discussed recently in ref. . Here, we briefly summarize this viewpoint.

For the weak impurity $`\stackrel{~}{\epsilon }1`$, the bias-dependence of the exponent $`B`$ is obtained as

$$B(f_{\mathrm{c},0}f)^{\frac{3}{2}\frac{d+1}{4}}.$$
(27)
Note that the exponent of $`(f_{\mathrm{c},0}f)`$ depends crucially on the spatial dimension $`d`$. The factor $`3/2`$ comes from the bias dependence of the barrier height $`\mathrm{\Delta }U(f_{\mathrm{c},0}f)^{3/2}`$, while the factor $`(d+1)/4`$ comes from the fact that the typical size of the bounce solution in the spatial(temporal) coordinates is given by $`(f_{\mathrm{c},0}f)^{1/4}`$ for each of original coordinates ($`x`$, $`\tau `$). (See (14) and (15).)

The impurity effect can be explained by the change in the dimension: the strong impurity changes the spatial dimensionality $`d`$ to zero. The classical threshold bias is also modified from $`f_{\mathrm{c},0}`$ to $`f_\mathrm{c}`$. As a result, the bias-dependence of $`B`$ becomes

$$B(f_cf)^{\frac{3}{2}\frac{1}{4}}=(f_cf)^{5/4}$$
(28)
in the presence of strong impurities. In this region, the nucleation process is well described by a local deformation of the field, and is reduced to a one-variable problem.

This viewpoint is valid in the one-dimensional case as shown in the subsequent sections. In the $`d2`$ case, however, the viewpoint of the dimensional crossover in this paper cannot be discussed, since the impurity potential cannot be described by the delta function in (9), as will be discussed in Sec. V.

### C Exponent

For one-dimensional systems, the exponent $`B`$ is calculated in a form $`B=\sigma \stackrel{~}{B}(\stackrel{~}{\epsilon })`$. The factor $`\sigma =a^2(f_cf)/b^2`$ describes the bias-dependence in the absence of the impurities, while the scaled exponent $`\stackrel{~}{B}(\epsilon )`$ is calculated as

$`\stackrel{~}{B}(\stackrel{~}{\epsilon })`$ $`=`$ $`\stackrel{~}{S}[\phi _\mathrm{B}(x^{},\tau ^{})]\stackrel{~}{S}[\phi _0(x^{})],`$ (29)
$`\stackrel{~}{S}[\phi (x^{},\tau ^{})]`$ $`=`$ $`{\displaystyle _{\stackrel{~}{L}/2}^{\stackrel{~}{L}/2}}dx^{}{\displaystyle _0^{\mathrm{}\stackrel{~}{\beta }}}d\tau ^{}[{\displaystyle \frac{1}{2}}\phi _x^{}^2+{\displaystyle \frac{1}{2}}\phi _\tau ^{}^2`$ (30)
$`+`$ $`{\displaystyle \frac{1}{2}}\phi ^2{\displaystyle \frac{1}{6}}\phi ^3\stackrel{~}{\epsilon }\delta (x^{})\phi ].`$ (31)
The impurity effect appears only through $`\stackrel{~}{B}(\stackrel{~}{\epsilon })`$. In the homogeneous case, $`\stackrel{~}{B}(\stackrel{~}{\epsilon })`$ is obtained as

$$\stackrel{~}{B}(0)=\stackrel{~}{S}[\phi _\mathrm{B}(x^{},\tau ^{};\stackrel{~}{\epsilon }=0)]=31.00,$$
(32)
and the exponent behaves as $`B=\stackrel{~}{B}(0)\sigma (f_cf)^1`$. As the effective impurity strength $`\stackrel{~}{\epsilon }`$ increases, $`\stackrel{~}{B}(\stackrel{~}{\epsilon })`$ is suppressed, and the tunneling rate is enhanced. At a critical value $`\stackrel{~}{\epsilon }_{\mathrm{cl}}=4/\sqrt{3}2.31`$, the potential barrier disappears, and the exponent $`B`$ is reduced to zero. Note that before the exponent $`B`$ becomes zero, the bounce method becomes invalid because it is justified only in the semiclassical condition $`B/\mathrm{}1`$. However, the region where the bounce method is broken down is narrow since the normalized Planck constant $`\mathrm{}`$ is assumed to be small enough.

We calculate the function $`\stackrel{~}{B}(\stackrel{~}{\epsilon })`$ by solving the equation (20) numerically. The Newton method is used by dividing the $`x^{}`$-$`\tau ^{}`$ ($`x^{}>0`$, $`\tau ^{}>0`$) space into $`64\times 64`$ cells. The result is shown in Fig. 2 by square dots.

Analytical expressions of $`\stackrel{~}{B}(\stackrel{~}{\epsilon })`$ can be obtained in the limiting cases . For the weak impurity ($`\stackrel{~}{\epsilon }1`$), $`\stackrel{~}{B}(\stackrel{~}{\epsilon })`$ is evaluated by using the bounce solution in the homogeneous case $`\stackrel{~}{\epsilon }=0`$ as

$`\stackrel{~}{B}(\stackrel{~}{\epsilon })`$ $`=`$ $`\stackrel{~}{S}_0\stackrel{~}{\epsilon }{\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑\tau ^{}\phi _\mathrm{B}(0,\tau ^{};\stackrel{~}{\epsilon }=0)+O(\stackrel{~}{\epsilon }^2)`$ (33)
$`=`$ $`31.0016.43\stackrel{~}{\epsilon }+O(\stackrel{~}{\epsilon }^2).`$ (34)
This result is shown in Fig. 2 by the dashed line.

For the strong impurity $`\stackrel{~}{\epsilon }\stackrel{~}{\epsilon }_{\mathrm{cl}}`$, the local modulation of the field becomes relevant, and a one-mode approximation is effective. We first evaluate the solutions of (20) for $`\stackrel{~}{\epsilon }=\stackrel{~}{\epsilon }_{\mathrm{cl}}`$. The bounce solution $`\phi _\mathrm{B}(x^{})`$ agrees with the stable solution $`\phi _0(x^{})`$, and is obtained analytically as

$$\phi _\mathrm{B}(x^{};\stackrel{~}{\epsilon }_{\mathrm{cl}})=\frac{3}{\mathrm{cosh}^2((x^{}+a_{\mathrm{cl}})/2)},$$
(35)
where $`\mathrm{tanh}(a_{\mathrm{cl}}/2)=1/\sqrt{3}`$. At the critical point $`\stackrel{~}{\epsilon }=\stackrel{~}{\epsilon }_{\mathrm{cl}}`$, there appears the zero frequency mode ($`\lambda _1^{(B)}=0`$) around the solution $`\phi _\mathrm{B}(x;\stackrel{~}{\epsilon }_{\mathrm{cl}})`$. The eigenfunction of this mode is obtained from (25) as

$$\psi _1^{(B)}(x^{};\stackrel{~}{\epsilon })=\frac{C\mathrm{sinh}((x^{}+a_{\mathrm{cl}})/2)}{\mathrm{cosh}^3((x^{}+a_{\mathrm{cl}})/2)},$$
(36)
where $`C`$ is a normalization factor determined from $`|\psi _1^{(B)}|^2𝑑x^{}=1`$, and is given by

$$C=\sqrt{\frac{135}{8(92\sqrt{3})}}1.746.$$
(37)
When $`\stackrel{~}{\epsilon }`$ is slightly smaller than $`\stackrel{~}{\epsilon }_{\mathrm{cl}}`$, this mode describes slow dynamics of the system, and is related to the tunneling process. Hence, we can approximate the bounce solution as

$$\phi _\mathrm{B}(x^{},\tau ^{};\stackrel{~}{\epsilon })\phi _\mathrm{B}(x^{};\stackrel{~}{\epsilon }_{\mathrm{cl}})+X(\tau ^{})\psi _1^{(\mathrm{B})}(x^{}),$$
(38)
where $`X(\tau ^{})`$ is a tunneling variable denoting the dynamics of the local deformation at the impurity site. By substituting (38) into the action (31), we obtain the action in terms of $`X(\tau ^{})`$ as

$`\stackrel{~}{S}[X(\tau ^{})]`$ $`=`$ $`{\displaystyle _0^{\mathrm{}\stackrel{~}{\beta }}}𝑑\tau ^{}\left[{\displaystyle \frac{1}{2}}\left({\displaystyle \frac{dX}{d\tau ^{}}}\right)^2+V(X)\right]`$ (39)
$`V(X)`$ $`=`$ $`{\displaystyle \frac{2\sqrt{3}}{9}}(\stackrel{~}{\epsilon }_{\mathrm{cl}}\stackrel{~}{\epsilon })CX{\displaystyle \frac{4}{243}}(CX)^3.`$ (40)
This action corresponds to one-particle dynamics in a cubic potential $`V(X)`$. The potential barrier $`\mathrm{\Delta }U`$ and frequency of small oscillation around the metastable state $`\omega _0`$ are given as

$`\mathrm{\Delta }U`$ $`=`$ $`2^{5/2}\times 3^{5/4}(\stackrel{~}{\epsilon }_{\mathrm{cl}}\stackrel{~}{\epsilon })^{3/2}`$ (41)
$`\omega _0`$ $`=`$ $`2^{5/4}\times 3^{11/8}C(\stackrel{~}{\epsilon }_{\mathrm{cl}}\stackrel{~}{\epsilon })^{1/4}`$ (42)
By applying the standard bounce technique  to this potential, the function $`\stackrel{~}{B}(\stackrel{~}{\epsilon })`$ is obtained

$$\stackrel{~}{B}(\stackrel{~}{\epsilon })=\frac{36\mathrm{\Delta }U}{5\mathrm{}\omega _0}11.25(\stackrel{~}{\epsilon }_{\mathrm{cl}}\stackrel{~}{\epsilon })^{5/4}.$$
(43)
This result, shown in Fig. 2 by a solid line, agrees with the numerical result for the strong impurity strength, and gives a good estimate even for the weak impurity. The expression (43) may be useful to analyze experimental data.

In order to analyze experimental results, it is convenient to draw the graph of $`\stackrel{~}{B}(\stackrel{~}{\epsilon })`$. The feature of impurity effects can be obtained by this analysis. Concerning the highly-biased region, this plot is universal in the sense that it does not depend on the bare impurity strength $`\epsilon `$.

In order to apply the viewpoint of the dimensional crossover, the bias-dependence of the exponent $`\stackrel{~}{B}`$ is discussed. For simplicity, the cosine potential with a bias term (4) is considered with a notation $`f_{\mathrm{c},0}=1`$, (see above Eq. (7)) $`a=\sqrt{2}`$, $`b=1`$ (see below Eq. (7)). We use the bias parameter $`\eta =(f_{\mathrm{c},0}f)/(f_{\mathrm{c},0}f_\mathrm{c})`$. It takes 0 and 1 corresponding the classical threshold ($`f=f_{\mathrm{c},0}=1`$) in the absence of the impurities and to the critical bias ($`f=f_c`$) in the presence of the impurities, respectively. Here, $`f_\mathrm{c}`$ is defined by $`\stackrel{~}{\epsilon }_{\mathrm{cl}}=4/\sqrt{3}=\epsilon (2(1f_\mathrm{c}))^{3/4}`$. The graph of $`\stackrel{~}{B}`$ as a function of $`\eta `$ is shown in Fig. 3. The numerical result is shown by square dots. Analytical results for the weak and strong impurities are also shown by the dashed and solid curves, respectively.

The dimensional crossover discussed in Sec. III B can be clarified in this figure. In the region $`\eta 1`$ where the effective impurity strength $`\stackrel{~}{\epsilon }`$ becomes small, $`\stackrel{~}{B}`$ becomes almost independent of the bias as seen in Fig. 3, and the exponent $`B`$ behaves as $`B(f_{\mathrm{c},0}f)^1`$ as expected in (27). As $`\eta `$ approaches the critical threshold $`\eta =1`$, the effective impurity strength is enhanced, and the exponent is suppressed. The analytical expression near $`\eta =1`$ is obtained from (43) as

$$B22.36(\eta 1)^{5/4}.$$
(44)
Hence, the exponent behaves as $`B(f_cf)^{5/4}`$ as expected in (28). We show the bias-dependences near $`\eta =1`$ in the inset of Fig. 3. The exponent, thus, behaves as $`B(f_cf)^{3/2(d+1)/4}`$, and the spatial dimension $`d`$ seems to be reduced to zero by the strong impurities accompanied with the change of the classical threshold $`f_c`$.

Finally, we show the bounce solution $`\phi _\mathrm{B}(x,\tau )`$ in Fig. 4 in the region $`x>0`$, $`\tau >0`$. Note that the bounce solution has a reversal symmetry $`\phi _\mathrm{B}(x,\tau )=\phi _\mathrm{B}(x,\tau )=\phi _\mathrm{B}(x,\tau )`$. The bounce solution is expected to describe the feature of the nucleation process; $`\phi (x,\tau )`$ describes the shape of the field variable $`\phi `$ at the imaginary-time $`\tau `$. As the effective impurity strength increases, the boundary condition for the bounce solution $`\phi _\mathrm{B}(x,\pm \mathrm{})=\phi _0(x)`$ is modified at the impurity site. As seen in Fig. 4, the nucleation process occurs only at the small region near the impurity site for the strong impurities. This change of the nucleation process is responsible for the qualitative difference between the weak and strong impurities.

### D Prefactor

The prefactor $`A`$ is ordinarily a minor factor which is hard to be measured experimentally. However, it describes the system-size ($`L`$) dependence of the nucleation rate, which may be observed. Here, we study the prefactor $`A`$ analytically in the limiting cases within the bounce method, and discuss the $`L`$-dependence of the nucleation rate.

The prefactor is formulated in (23) with the improvement (26) due to the zero mode ($`\lambda _2^{(B)}=0`$). In the absence of the impurities, not only the second but also the third lowest modes become the zero modes ($`\lambda _3^{(B)}=0`$), which need to be treated by the Fadeev-Popov method as

$$\frac{1}{\sqrt{\lambda _3^{(\mathrm{B})}}}\sqrt{\frac{\sigma \stackrel{~}{B}(0)}{2\pi }}_{\stackrel{~}{L}/2}^{\stackrel{~}{L}/2}𝑑x_0^{},$$
(45)
where $`x_0^{}`$ denotes a position of the bounce center. This treatment gives the correct system-size dependence, $`\mathrm{\Gamma }L`$.

As for the weak impurity, the frequency of the third lowest mode is lifted to a small positive frequency. Also in this case, the replacement in (45) is needed in order to obtain the correct system-size dependence. As a result, the tunneling rate is calculated as

$$\mathrm{\Gamma }=\mathrm{\Gamma }_0\left[\stackrel{~}{L}+_{\stackrel{~}{L}/2}^{\stackrel{~}{L}/2}𝑑x_0^{}(e^{\sigma \stackrel{~}{\epsilon }f(x_0^{})}1)\right],$$
(46)
where $`\mathrm{\Gamma }_0`$ is the nucleation rate per unit length in the absence of the impurities, and the function $`f(x_0^{})`$ is defined by

$$f(x_0^{})=_{\mathrm{}}^{\mathrm{}}𝑑\tau ^{}\phi _\mathrm{B}(x_0^{},\tau ^{};\stackrel{~}{\epsilon }=0).$$
(47)
From this expression, the tunneling rate can be divided into two parts as

$`\mathrm{\Gamma }_{\mathrm{bulk}}`$ $`=`$ $`\mathrm{\Gamma }_0\stackrel{~}{L},`$ (48)
$`\mathrm{\Gamma }_{\mathrm{imp}}`$ $`=`$ $`\mathrm{\Gamma }_0{\displaystyle _{\stackrel{~}{L}/2}^{\stackrel{~}{L}/2}}𝑑x_0^{}(e^{\sigma \stackrel{~}{\epsilon }f(x_0^{})}1).`$ (49)
The bulk part $`\mathrm{\Gamma }_{\mathrm{bulk}}`$ is proportional to the system size $`\stackrel{~}{L}`$, while the impurity part $`\mathrm{\Gamma }_{\mathrm{imp}}`$ is independent of the system size for $`\stackrel{~}{L}1`$.

Within the bounce method, the $`L`$-dependence is naturally described as follows. For large $`L`$, $`\mathrm{\Gamma }_{\mathrm{bulk}}`$ alway dominates $`\mathrm{\Gamma }_{\mathrm{imp}}`$, and no impurity effects appear. As $`L`$ is reduced, the bulk part is suppressed, and below a crossover length $`\stackrel{~}{L}_{\mathrm{cr}}`$, the impurity part may overcome the bulk part. Only in this region, the impurity effect is clearly observed experimentally. The ratio $`\mathrm{\Gamma }_{\mathrm{imp}}/\mathrm{\Gamma }_{\mathrm{bulk}}`$ is determined by the scaled length $`\stackrel{~}{L}`$ and the impurity factor $`\sigma \stackrel{~}{\epsilon }`$ in (49). For $`\stackrel{~}{L}1`$, the crossover length $`\stackrel{~}{L}_{\mathrm{cr}}`$ can be obtained as a function of $`\sigma \stackrel{~}{\epsilon }`$ by taking the ratio as $`\mathrm{\Gamma }_{\mathrm{imp}}/\mathrm{\Gamma }_{\mathrm{bulk}}=1`$. Thus, the phase diagram is obtained by Fig. 5, where the crossover length is shown by the solid curve. In the upper region of the phase diagram, the nucleation occurs dominantly in the bulk region, while in the lower region, the impurity part dominates the bulk part, and inhomogeneity effects appear clearly.

The intuitive discussion about the appearance of the impurity effect in Sec. II can be now clarified in detail. The asymptotic form of the crossover length $`\stackrel{~}{L}_{\mathrm{cr}}`$ for $`\sigma \stackrel{~}{\epsilon }1`$ is obtained analytically by applying the stationary method to the integral (49) as

$$\mathrm{log}\stackrel{~}{L}_{\mathrm{cr}}16.43(\sigma \stackrel{~}{\epsilon })0.211\frac{1}{2}\mathrm{log}(\sigma \stackrel{~}{\epsilon }).$$
(50)
This result is shown in Fig. 5 by the dashed curve. The predominant term in (50) can be related to the enhancement of the exponent $`\mathrm{\Delta }B`$ defined by

$$\mathrm{\Delta }B=\sigma \stackrel{~}{\epsilon }_{\mathrm{}}^{\mathrm{}}𝑑\tau ^{}\phi _\mathrm{B}(x=0,\tau ^{};\stackrel{~}{\epsilon }=0),$$
(51)
as $`\mathrm{log}\stackrel{~}{L}_{\mathrm{cr}}=\mathrm{\Delta }B`$. Since $`\mathrm{\Delta }B`$ is estimated by the local suppression of the potential barrier $`\mathrm{\Delta }U`$ and the typical attempt frequency $`\omega _0`$ as $`\mathrm{\Delta }B\mathrm{\Delta }U/\mathrm{}\omega _0`$, the expression in (10) can be reproduced qualitatively.

Beyond the perturbational analysis of $`\stackrel{~}{\epsilon }`$, it is difficult to calculate the prefactor, because the low-frequency modes may couple with each other. It would be a future problem to consider the nucleation rates in this regime. (See also Sec. V B.) Only for the strong impurity, the prefactor can be calculated by assuming $`\stackrel{~}{L}\stackrel{~}{L}_{\mathrm{cr}}`$ and by applying standard procedures  to one-variable problem (39) with (40) as

$$A\sqrt{60}\sqrt{\frac{\stackrel{~}{B}(0)}{2\pi }},$$
(52)
although the crossover length $`\stackrel{~}{L}_{\mathrm{cr}}`$ cannot be easily obtained even in this case.

## IV THERMAL ACTIVATION REGIME

At high temperatures, nucleation is caused by thermal fluctuations. Since the nucleation rate has already been studied in this region in ref. , we only summarize the feature of the impurity effect.

In the thermal activation regime, the nucleation rate is evaluated by Kramers’ formula

$$\mathrm{\Gamma }=A\mathrm{exp}(\mathrm{\Delta }U/k_\mathrm{B}T).$$
(53)
The potential barrier $`\mathrm{\Delta }U`$ is calculated as

$`\mathrm{\Delta }U`$ $`=`$ $`U[\phi _B(x^{})]U[\phi _0(x^{})],`$ (54)
$`U[\phi (x^{})]`$ $`=`$ $`{\displaystyle \frac{a^{5/2}(f_cf)^{5/4}}{b^2}}{\displaystyle _{\stackrel{~}{L}/2}^{\stackrel{~}{L}/2}}𝑑x^{}`$ (55)
$`\times `$ $`\left({\displaystyle \frac{1}{2}}\phi _x^{}^2+{\displaystyle \frac{1}{2}}\phi ^2{\displaystyle \frac{1}{6}}\phi ^3\stackrel{~}{\epsilon }\delta (x^{})\phi (x^{})\right).`$ (56)
Here, $`\phi _0(x^{})`$ ($`\phi _\mathrm{B}(x^{})`$) is the stable (unstable) stationary solution satisfying

$$\frac{\delta U}{\delta \phi (x^{})}=\phi _{x^{}x^{}}+\phi \frac{\phi ^2}{2}\stackrel{~}{\epsilon }\delta (x^{})=0.$$
(57)
The same result can be derived by applying the bounce method to a finite temperature region . Within the bounce method, the feature at high temperatures is explained as follows. At high temperatures, the bounce solution becomes independent of $`\tau ^{}`$, since the interval in the $`\tau `$ direction becomes short. It means that the temporal dimension become irrelevant. Hence, the relevant dimension of the bounce is reduced from $`(d+1)`$ to $`d`$. Except for the absence of the temporal dimension, we can discuss the dimensional crossover in the same way as Sec. III B: the energy barrier behaves as $`\mathrm{\Delta }U(f_cf)^{5/4}`$ for the weak impurity, while as $`\mathrm{\Delta }U(f_cf)^{3/2}`$ for the strong impurity.

The barrier height is calculated in a form

$$\mathrm{\Delta }U=\frac{a^{5/2}(f_cf)^{5/4}}{b^2}\mathrm{\Delta }\stackrel{~}{U}(\stackrel{~}{\epsilon }).$$
(58)
The impurity effects appear only through the normalized potential barrier $`\mathrm{\Delta }\stackrel{~}{U}`$. We show $`\mathrm{\Delta }\stackrel{~}{U}`$ as a function of the effective impurity strength $`\stackrel{~}{\epsilon }`$ in Fig. 6 by the square dots. The critical impurity strength is given by $`\stackrel{~}{\epsilon }_{\mathrm{cl}}=4/\sqrt{3}`$ which is the same as the quantum tunneling regime. The exponent is obtained analytically for the weak impurity $`\stackrel{~}{\epsilon }1`$ as

$$\mathrm{\Delta }\stackrel{~}{U}(\stackrel{~}{\epsilon })=24/53\stackrel{~}{\epsilon },$$
(59)
while for the strong impurity $`\stackrel{~}{\epsilon }\stackrel{~}{\epsilon }_{\mathrm{cl}}`$ as

$$\mathrm{\Delta }\stackrel{~}{U}(\stackrel{~}{\epsilon })=1.433(\stackrel{~}{\epsilon }_{\mathrm{cl}}\stackrel{~}{\epsilon })^{3/2}.$$
(60)
These results are shown in Fig. 6 by the dashed and solid curves. The feature of the impurity effect is the same as the zero-temperature case shown in Fig. 2.

## V DISCUSSION

### A Extension to the $`d2`$ case

First, let us discuss the two-dimensional systems. The stable solution $`\phi _0(x^{},y^{})`$ is determined by

$$\phi _{x^{}x^{}}+\phi _{y^{}y^{}}=\phi \frac{1}{2}\phi ^2\stackrel{~}{\epsilon }\delta (x^{})\delta (y^{}),$$
(61)
where the last term describes the impurity located at $`(x^{},y^{})=0`$. For the stationary solution having a rotational symmetry around the origin $`(x^{},y^{})=(0,0)`$, this equation is reduced, by using the radius coordinate $`r=\sqrt{x^2+y^2}`$, to

$$\frac{1}{r}\frac{}{r}\left(r\frac{\phi }{r}\right)=\phi \frac{1}{2}\phi ^2\stackrel{~}{\epsilon }g(r).$$
(62)
Here, $`g(r)`$ is a modified delta function satisfying $`g(r)=0`$ for $`r>0`$, $`g(r)=\mathrm{}`$ for $`r=0`$, and

$$_0^{\mathrm{}}𝑑r2\pi rg(r)=1.$$
(63)
From (62) and (63), the boundary condition at $`r=0`$ is obtained as

$$\underset{r0}{lim}r\frac{\phi }{r}=\frac{\stackrel{~}{\epsilon }}{2\pi }.$$
(64)
Since the function $`r\phi _r`$ is a continuous function at $`r>0`$, if we take an arbitrary constant $`A`$ ($`<\stackrel{~}{\epsilon }/2\pi `$), there exists a constant $`a`$, and for all $`r`$ in the range $`0<ra`$

$$r\frac{\phi }{r}A$$
(65)
is satisfied. As a result, $`\phi (r)`$ is evaluated for $`0<r<a`$ as

$$\phi (r)A\mathrm{log}\left(\frac{a}{r}\right)+\phi (a),$$
(66)
and the value of $`\phi `$ diverges at $`r=0`$. Since $`\phi `$ must be finite in the present model, this divergence means that the local inhomogeneity cannot be described by the delta function in the two-dimensional systems. In other words, if we approximate the delta function as $`g(r)=1/\pi r_0^2`$ for $`0<r<r_0`$ and as $`g(r)=0`$ for $`r_0<r`$, the value of $`\phi (0)`$ depends crucially on the impurity size $`r_0`$, and diverges in the limit $`r_00`$. Also in the $`d=3`$ case, the field $`\phi (r)`$ diverges at $`r=0`$, since the bounce solution behaves $`\phi (r)1/r`$ near $`r=0`$, where $`r=\sqrt{x^2+y^2+z^2}`$,

These results indicate that in the highly-biased region, the system is sensitive to local inhomogeneities. To clarify the inhomogeneity effects in the $`d2`$ case, it is needed to consider the detailed profiles of the inhomogeneities beyond the local approximation adopted in this paper.

### B Validity of the bounce method

In this paper, the nucleation rate is calculated by the bounce method. Although this method has been applied to multi-variable tunneling problems for many years, we should be careful of its validity. In principle, the exact tunneling rate should be determined by the full information about the action $`S[\varphi (x^{})]`$. The bounce solution can extract important informations from the action; the exponent $`B`$ is a difference of the action between the bounce and stable solutions, while the prefactor $`A`$ is determined by the second-order fluctuations around both the solutions. While the bounce method is a convenient method to evaluate the tunneling rate, some informations which may affect the tunneling rate are dropped.

It is expected that the bounce method can be justified in the following conditions : (1) we can define the tunneling variable describing slow dynamics among the many degrees of freedom, and (2) this tunneling variable is well separated from the other variables with fast dynamics. In these conditions, the system can be reduced to the one-variable tunneling problem where the bounce method is justified well. Here, let us consider the model adopted in this paper. For the strong impurity, it has been shown that the single-mode approximation gives a good estimate of the exponent $`B`$. In this region, the bounce method is expected to give correct results for both the exponent and the prefactor for $`LL_{\mathrm{cr}}`$, though the crossover length $`L_{\mathrm{cr}}`$ itself cannot be evaluated. For the moderate impurity, however, there appears another low-frequency mode related to the Goldstone mode. This low-frequency mode is expected to couple with the tunneling mode. Hence, the bounce method may give an incorrect result especially for the prefactor determined only by the information about second-order fluctuations. It is a future problem to improve the bounce method in this situation.

## VI SUMMARY

The local inhomogeneity effects on nucleation processes have been studied within the bounce method at high biases. The nucleation rate has been calculated in a form $`\mathrm{\Gamma }=A\mathrm{exp}(B/\mathrm{})`$. It has been found that the effective impurity strength $`\stackrel{~}{\epsilon }`$ can be controlled not only by the bare impurity strength $`\epsilon `$ but also by the external bias $`f`$. The exponent $`B`$ has been calculated as a function of the effective impurity strength $`\stackrel{~}{\epsilon }`$ without reduction to a single-variable tunneling problem. It has been shown that these results are well reproduced for the weak impurity by a perturbational analysis and for the strong impurity by a one-mode approximation. It has been clarified that the results can be explained by the reduction of the effective dimensionality of the system due to the impurity. By calculating the prefactor $`A`$, the condition of the appearance of the impurity effects has been discussed, and the phase diagram has been obtained.

There remain future problems. One of them is to study the inhomogeneity effect in higher-dimensional systems. As discussed in Sec. V, the local approximation does not hold for the $`d2`$ case. From this result, it is conjectured that the sample inhomogeneities may become essentially important for higher-dimensional systems. I think that the study of the inhomogeneity effects in high-dimensional systems would give an important aspect about the interplay of quantum tunneling and randomness.

###### Acknowledgements.

I wish to acknowledge M. Yumoto for suggestions and helpful discussions.

## A Relevance of the Local Impurity Model to Experimental Systems

In this paper, the inhomogeneity effect is described by the potential

$$V_{\mathrm{imp}}(x,\varphi )=\epsilon (x)h(\varphi ).$$
(A1)
If the function $`\epsilon (x)`$ changes only in a narrow region at the impurity site compared with the typical length scale ($`a^{1/2}(ff_c)^{1/4}`$), it can be replaced with the delta function $`\delta (x)`$ in (8). The potential form (A1) can be realized in various experimental situations. One typical example is a spatial inhomogeneity of the bias. If the bias is assumed not to be uniform but to have a spatial dependence as $`f+\epsilon (x)`$, then we have the potential form (A1). Another example is the inhomogeneity of the amplitude of the potential barrier in $`V_0(\varphi )`$. If we replace, for example, the cosine potential in (4) with $`(1+\epsilon (x))(1\mathrm{cos}\varphi )`$, then the form (A1) is also obtained. As for the Josephson junction systems, the coupling to the derivative of the field $`\varphi _x(x)`$ can also be introduced by applying the magnetic field . If the coupling is denoted with $`b(x)\varphi _x(x)`$, the potential form (A1) is derived by taking the function $`\epsilon (x)`$ as $`b_x(x)`$.

In addition to the above situations, boundaries play a role of local inhomogeneities. The potential barrier $`\mathrm{\Delta }U`$ is reduced to $`\mathrm{\Delta }U/2`$ at open edge. Hence, the nucleation occurs dominantly at the boundary. The prefactor $`A`$ of the nucleation rate is always independent of the system size, while the exponent $`B`$ is affected by the boundary condition. Assuming that the field $`\phi (x^{})`$ is defined at $`x^{}0`$, and that the boundary condition is given as

$$\phi _x^{}(x^{}=0)=h,$$
(A2)
it can be shown easily that this boundary effect corresponds to the local inhomogeneity by taking $`\stackrel{~}{\epsilon }=2h`$. Thus, the exponent $`B_{\mathrm{edge}}`$ is obtained as

$$B_{\mathrm{edge}}=\frac{1}{2}\sigma \stackrel{~}{B}(\stackrel{~}{\epsilon }=2h).$$
(A3)
By changing the boundary condition at the edge, the impurity effects on the exponent can also be observed. Actually, this tendency has been observed in experiments .


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# Nonequilibrium Electron Distribution in Presence of Kondo Impurities

## Abstract

We study the energy relaxation of quasiparticles in voltage biased mesoscopic wires in presence of magnetic impurities. The renormalization of the exchange interaction of Kondo impurities coupled to conduction electrons is extended to the case of a nonequilibrium electron distribution, which is determined self–consistently from a Boltzmann equation with a collision term due to Kondo impurity mediated electron–electron scattering. The approach leads to predictions in quantitative agreement with recent experiments by Pothier et al. \[Phys. Rev. Lett. 79, 3490 (1997)\].

In 1997 the mesoscopic physics community was puzzled by two experimental findings. On the one hand Mohanty, Jariwala, and Webb  have extracted the electron dephasing time from weak localization measurements of one–dimensional gold wires and found larger dephasing rates than predicted by the standard theory of Altshuler and Aronov (AA) . In the same year, Pothier et al.  published data on the nonequilibrium electron distribution in mesoscopic copper wires in presence of an applied voltage. The electron–electron scattering rate gained from these data was shown to exceed predictions based on the AA theory. It was intuitively clear that these two observations are very likely due to a common origin, and in the last three years a large body of work has proposed all kinds of mechanisms ranging from interaction with two–level systems , heating by radiation , $`1/f`$ noise  to intrinsic dephasing at zero temperature . None of these predictions could give a quantitative description of the experiments or they were ruled out by subsequent experimental studies. Finally, a scenario based on the two channel Kondo effect of symmetrical two level systems has recently been proposed by Kroha . For a rather complete discussion and analysis of available experimental data on both the weak localization and nonequilibrium electron distribution measurements in various metals we refer to the thesis by Pierre .

Already Mohanty et al.  have demonstrated that iron impurities added to the gold wires can lead to similar effects than those observed in nominally pure wires. In fact, equating the pair breaking rate in superconductors containing magnetic impurities  with the magnetic contribution to the dephasing rate in normal metals , one obtains a satisfactory explanation of the weak localization data near and above the Kondo temperature, where the theory is valid . On the other hand, the effect of Kondo impurities on electron–electron scattering has been addressed only very recently. Kaminski and Glazman (KG)  have determined the two–particle t–matrix mediated by magnetic impurities for an equilibrium system. The renormalization of the exchange coupling was studied with poor man’s scaling using the applied voltage $`V`$ as a low–energy cutoff. While the theory can explain the order of magnitude of the observed electron–electron scattering rate, it does not reproduce the correct voltage dependence but leads to more than an order of magnitude deviations from the data over the range of parameters investigated experimentally . In this work we demonstrate that it is essential to go beyond poor man’s scaling since deviations from AA predictions are pronounced only below the Kondo temperature. Most importantly, the renormalization flow has to be determined in presence of a nonequilibrium electron distribution calculated self–consistently from the Boltzmann equation. The collision term then depends on the distribution function not only through the occupation probabilities of in– and outgoing electrons but also via the renormalized interaction kernel.

We start by describing briefly the experimental situation: A mesoscopic wire of length $`L`$ with diffusion constant $`D`$ is attached to leads biased by a voltage $`V`$. (For details cf. Refs.  and ). The nonequilibrium electron distribution function $`f(ϵ,x)`$ in presence of a steady state current can be determined from the Boltzmann equation for a diffusive mesoscopic wire

$$\frac{1}{\tau _D}\frac{^2f(ϵ,x)}{x^2}=I_{\mathrm{coll}}$$
(1)
with the boundary conditions $`f(ϵ,0)=f_F(ϵeV/2)`$ and $`f(ϵ,1)=f_F(ϵ+eV/2)`$ imposed by the leads. Here $`x`$ is the position within the wire measured in units of $`L`$, and $`\tau _D=L^2/D`$. In the simple case of vanishing interaction $`I_{\mathrm{coll}}=0`$ we obtain a double step function

$$f_0(ϵ,x)=(1x)f_F(ϵeV/2)+xf_F(ϵ+eV/2).$$
(2)
The interaction smears these steps, and in the limit of strong electron–electron interaction leads to a Fermi function with an effective temperature of the electrons . The distribution function $`f(ϵ,x)`$ is determined in the experiment at various locations by tunneling spectroscopy.

Assuming a local interaction, the collision integral reads

$`I_{\mathrm{coll}}(x,ϵ,\{f\})`$ $`=`$ $`{\displaystyle 𝑑\omega 𝑑ϵ^{}K(\omega ,ϵ,ϵ^{})}`$ (5)
$`\times \{f(ϵ)f(ϵ^{})[1f(ϵ\omega )][1f(ϵ^{}+\omega )]`$
$`[1f(ϵ)][1f(ϵ^{})]f(ϵ\omega )f(ϵ^{}+\omega )\}`$
with an interaction kernel $`K(\omega ,ϵ,ϵ^{})`$. Not to overload the notation we suppress here and in the sequel the spatial dependence of the kernel and the distribution function. To determine the kernel $`K(\omega ,ϵ,ϵ^{})`$, we follow KG and start from the s–d exchange Hamiltonian

$$H=H_0+H_I$$
(6)
whereby

$$H_0=\underset{k\sigma }{}ϵ_kC_{k\sigma }^{}C_{k\sigma }$$
(7)
describes free quasiparticles with one–particle energies $`ϵ_k`$ and creation (annihilation) operators $`C_{k\sigma }^{}`$ ($`C_{k\sigma }`$) of states $`k\sigma `$. We assume that the density of impurities is small enough to treat the interaction with each impurity independently. Then, for a single impurity

$$H_I=J\underset{kk^{}\sigma \sigma ^{}}{}𝐒𝐬_{\sigma \sigma ^{}}C_{k\sigma }^{}C_{k^{}\sigma ^{}},$$
(8)
where $`𝐒`$ is the impurity spin operator and $`𝐬`$ the vector of Pauli matrices. Further $`J`$ is the exchange interaction.

Let us first address the electron–electron interaction mediated by Kondo impurities in an equilibrium metal. We rewrite the most singular parts of the interaction in terms of single–particle t–matrices and include renormalization effects for lower temperatures by an approach due to Zittartz and Müller–Hartmann  based on the Nagaoka equations . This theory, though not able to describe the zero temperature limit correctly, leads to meaningful results at higher temperatures down to temperatures well below the Kondo temperature .

For an effective two–particle interaction, the kernel $`K(\omega ,ϵ,ϵ^{})`$ is essentially given by the modulus squared of the on–shell two–particle t–matrix. Further, one has to sum over all final electron spins $`\sigma _f,\sigma _f^{}`$ and the initial spin $`\sigma ^{}`$ of the second electron and average over the initial spin $`\sigma `$ of the first electron and the impurity spin $`S`$. For impurities with density $`C_{\mathrm{imp}}`$ the kernel then takes the form

$$K(\omega ,ϵ,ϵ^{})=C_{\mathrm{imp}}\rho ^3\frac{\pi }{2\mathrm{}}\underset{\sigma \sigma _f\sigma ^{}\sigma _f^{}S}{}S||T_{k\sigma ,k^{}\sigma ^{}k_f\sigma _f,k_f^{}\sigma _f^{}}|^2|S$$
(9)
where $`\rho `$ is the electronic density of states at the Fermi level. The two–particle t–matrix is defined by

$$T_{k\sigma ,k^{}\sigma ^{}k_f\sigma _f,k_f^{}\sigma _f^{}}=k_f\sigma _f,k_f^{}\sigma _f^{}|T|k\sigma ,k^{}\sigma ^{}$$
(10)
and does not depend on the directions of the incoming and outgoing electrons. Hence, the wave numbers $`k,k^{}`$ and $`k_f,k_f^{}`$ are characterized by the energies $`ϵ_k=ϵ`$, $`ϵ_k^{}=ϵ^{}`$, and $`ϵ_{k_f}=ϵ\omega `$, $`ϵ_{k_f^{}}=ϵ^{}+\omega `$, respectively, cf. Fig. 1. Unlike an effective potential mediated by the impurity spin , the t–matrix here is an operator in impurity spin space. As usual, the operator $`T`$ is defined by the series

$$T(ϵ)=H_I\underset{n=0}{\overset{\mathrm{}}{}}\left(\frac{1}{ϵH_0}H_I\right)^n.$$
(11)
Our interest is in the retarded t–matrix where the energy $`ϵ`$ is determined by the outgoing electrons, i.e., $`ϵ=ϵ_{k_f}+ϵ_{k_f^{}}+i\delta `$. Performing perturbation theory up to fifth order in the coupling $`J`$, we get for the inelastic processes

$`K(\omega ,ϵ,ϵ^{})`$ $`=`$ $`{\displaystyle \frac{1}{\omega ^2}}{\displaystyle \frac{\pi }{2\mathrm{}}}{\displaystyle \frac{C_{\mathrm{imp}}}{\rho }}S(S+1)(\rho J)^4`$ (14)
$`\{1+\rho J[g(ϵ)+g(ϵ^{})+g^{}(ϵ\omega )+g^{}(ϵ^{}+\omega )]\}`$
$`+\mathrm{l}.\mathrm{s}.+𝒪(\rho J)^6`$
where l.s. means less singular terms in $`1/\omega `$. To leading order in $`J`$, this result agrees with the findings of KG. The less singular terms omitted arise from energy denominators that include an intermediate electronic energy to be summed over, leading at most to a logarithmic singularity for $`\omega 0`$. Further, the auxiliary function $`g(ϵ)`$ is given by

$$g(ϵ)=𝑑ϵ^{}\left[f(ϵ^{})\frac{1}{2}\right]\frac{\stackrel{~}{\rho }(ϵ^{})}{ϵϵ^{}+i\delta }$$
(15)
where $`\stackrel{~}{\rho }(ϵ)`$ is the normalized density of states of the electrons with $`\stackrel{~}{\rho }(0)=1`$.

To go beyond perturbation theory we consider the t–matrix in operator form $`(\text{11})`$. We are interested in the most divergent terms for $`\omega 0`$ and therefore search for energy denominators of the form $`1/(ϵH_0)=\pm 1/\omega `$. Since $`ϵ=ϵ_{k_f}+ϵ_{k_f^{}}=ϵ_k\omega +ϵ_k^{}+\omega =ϵ_k+ϵ_k^{}`$, the intermediate energy must include both $`ϵ_{k_f}`$ and $`ϵ_k^{}`$ or $`ϵ_{k_f^{}}`$ and $`ϵ_k`$, i.e., two unperturbed electron lines must lead to this intermediate state. Therefore, in leading order in $`1/\omega `$ we may decompose the two–particle t–matrix into two single–particle t–matrices, one acting on the $`k`$–quasiparticle and the other on the $`k^{}`$–quasiparticle, cf. Fig. 1,

$`T_{k\sigma ,k^{}\sigma ^{}k_f\sigma _f,k_f^{}\sigma _f^{}}`$ $`=`$ $`T_{k\sigma k_f\sigma _f}{\displaystyle \frac{1}{\omega }}T_{k^{}\sigma ^{}k_f^{}\sigma _f^{}}`$ (17)
$`+T_{k^{}\sigma ^{}k_f^{}\sigma _f^{}}{\displaystyle \frac{1}{\omega }}T_{k\sigma k_f\sigma _f}+\mathrm{l}.\mathrm{s}..`$
Here, the operator character of the t–matrices in impurity spin space plays an essential role since all commuting terms cancel.

To proceed we follow Zittartz  and decompose the single–particle t–matrix into a non–spin flip and a spin flip amplitude

$$T_{k\sigma k_f\sigma _f}=t_{kk_f}\delta _{\sigma \sigma _f}I_S+\tau _{kk_f}𝐒𝐬_{\sigma \sigma _f}.$$
(18)
Here, $`I_S`$ means the identity in impurity spin space, and $`t_{kk_f}`$ and $`\tau _{kk_f}`$ are the t–matrices in the non–spin flip and spin flip channel, respectively. Since the identity commutes with other spin matrices, it does not lead to a leading order contribution in $`1/\omega `$. Inserting the two–particle t–matrix $`(\text{17})`$ with $`(\text{18})`$ into Eq. $`(\text{9})`$ we get

$$K(\omega ,ϵ,ϵ^{})=\frac{1}{\omega ^2}\frac{\pi }{2\mathrm{}}C_{\mathrm{imp}}S(S+1)\rho ^3|\tau (ϵ)\tau (ϵ^{})|^2+\mathrm{l}.\mathrm{s}..$$
(19)
Comparing this expression with the perturbative result $`(\text{14})`$, we see that the bare coupling $`J`$ is replaced by the renormalized quantity $`\tau _{kk_f}=\tau (ϵ_{k_f})`$. This result $`(\text{19})`$ is of central importance for the analysis below. Note that the expression $`(\text{19})`$ displays an explicit $`1/\omega ^2`$ dependence which is crucial for the experimentally observed scaling behavior . The kernel for the effective electron–electron scattering depends on the off–shell spin flip part of the t–matrix which has a different behavior than the on–shell non–spin flip part of the t–matrix responsible for the temperature dependence of the resistance. In our approach the $`1/\omega ^2`$ algebraic factor emerges analytically from this representation of $`K(\omega ,ϵ,ϵ^{})`$ .

Zittartz  has shown that the Nagaoka equations lead to a single–particle t–matrix in the spin–flip channel of the form

$$\tau (ϵ)=\frac{J}{\varphi (ϵ)}.$$
(20)
With Hamann’s solution  of the Nagaoka equations, the denominator reads

$$\varphi (ϵ)=[X(ϵ)^2+S(S+1)(\pi \rho J)^2]^{1/2}.$$
(21)
Here

$$X(ϵ)=1S(S+1)(\pi \rho J)^2/4\rho JR(ϵ)$$
(22)
is temperature dependent via the function

$$R(ϵ)=\mathrm{ln}\left(\frac{\omega +iT}{i\mathrm{\Lambda }}\right)$$
(23)
where $`\mathrm{\Lambda }`$ is the electronic bandwidth. $`R(ϵ)`$ is an equilibrium approximation of the auxiliary function $`g(ϵ)`$ introduced in Eq. $`(\text{15})`$. By inserting the solution $`(\text{20})(\text{23})`$ into the kernel $`(\text{19})`$ and expanding in $`J`$, we can indeed recover the perturbative result $`(\text{14})`$.

Let us now turn to a nonequilibrium situation. Since in equilibrium and nonequilibrium the t–matrix expansions differ only in the occupation probabilities of intermediate states, we can use the result for the equilibrium t–matrix replacing the distribution of intermediate states by their (unknown) nonequilibrium form. In the solution $`(\text{20})(\text{22})`$ occupation probabilities only effect the function $`R(ϵ)`$ which in a nonequilibrium system is no longer of the form $`(\text{23})`$ but has to be replaced by $`g(ϵ)`$. Of course, then the nonequilibrium single–particle t–matrix in the spin flip channel depends via $`g(ϵ)`$ on the nonequilibrium distribution function $`f(ϵ)`$. The resulting form of the collision kernel is fully consistent with perturbation theory up to fifth order in $`J`$ and it includes correctly the leading logarithmic terms.

To proceed, the t–matrix and the distribution function need to be determined self–consistently. Both quantities depend on the position $`x`$ within the wire. We start with the initial nonequilibrium distribution function $`(\text{2})`$, determine the t–matrix from Eqs. $`(\text{20})(\text{22})`$, and the collision kernel from Eq. $`(\text{19})`$. An improved distribution function is then obtained from the Boltzmann equation $`(\text{1})`$, which gives rise to an improved kernel. This procedure converges after about $`20`$ iterations.

First, we compared our results with recent experimental data  on the energy relaxation in Au wires in presence of Fe impurities. In these experiments all parameters were determined by independent measurements. For instance, for sample $`2`$ measured at $`T=33`$mK the diffusion time $`\tau _D=1.8`$ns. The impurity density was determined from the temperature dependence of the resistance as $`C_{\mathrm{imp}}55`$ ppm. We set the impurity spin to $`S=1/2`$ and the Kondo temperature to $`T_K=1`$K which is a typical value for Fe in Au . Further, we used a density of states of $`\rho =0.25/\mathrm{site}\mathrm{eV}`$ .

Pothier et al.  have noticed that the distribution functions $`f(ϵ,V)`$ exhibit scaling behavior so that as a function of $`ϵ/eV`$ all data at a given position $`x`$ fall on a single line. In Fig. 2 we show our findings for the distribution function using the parameters of Pierre et al.  for various voltages $`V=0.10.4`$meV and two positions $`x=0.25,0.5`$. They are compared with the experimental data points  and we find excellent agreement without adjustable parameters. We emphasize that the result is independent of the choice of the bandwidth and is insensitive to the Kondo temperature as long as $`TT_K`$. For other values of $`x`$ the curves coincide likewise.

On the other hand, for higher temperatures $`T>T_K`$ where poor man’s scaling holds, the kernel varies logarithmically with the applied voltage $`V`$  and the distribution function cannot be written as a function of $`ϵ/eV`$ only. We have also analyzed the data by Pothier et al.  on Cu wires and find again good agreement assuming a density $`C_{\mathrm{imp}}=14`$ppm of $`S=1/2`$ impurities with a Kondo temperature above $`200`$mK (see Fig. 2). Small deviations between the theoretical and experimental results are likely due to heating in this first experiment .

To see the effect of the nonequilibrium electronic distribution on the renormalization of the exchange interaction, we show in Fig. 3 for sample $`2`$ of Pierre et al.  the real part of the single–particle t–matrix in the spin flip channel $`\rho \tau (E)`$ for $`V=0.2`$meV at $`x=0.5`$ (left panel) and $`x=0.25`$ (right panel). The solid line gives the self–consistent solution obtained from the iteration explained above, while the dotted line depicts the result obtained for the distribution $`(\text{2})`$ in absence of energy relaxation. We see that the coupling changes significantly with the distribution function. Using only the initial t–matrix does not suffice to explain the experimental data. Comparing t–matrices for various voltages, we find weak dependence between the Fermi points $`ϵ=\pm eV/2`$. This gives rise to the scaling behavior of the distribution function, while poor man’s scaling  implies a significant voltage dependence of the scaled data in conflict with experiments .

To complete our discussion we should have included spin dynamics which cuts off the $`1/\omega ^2`$ divergence of $`K(\omega ,ϵ,ϵ^{})`$ for small frequencies . This is crucial for effects that depend strongly on the low frequency limit, such as dephasing. However, the distribution function $`f(ϵ)`$ determined from the Boltzmann equation $`(\text{1})`$ is almost insensitive to this low frequency cutoff since the collision integral remains finite even in absence of a cutoff. Hence, for the problem considered here, one can disregard the impurity spin relaxation.

In summary we have determined the effective electron–electron collision kernel mediated by magnetic impurities for nonequilibrium wires at temperatures below the Kondo temperature. We found excellent agreement with recent experimental findings . In particular, we have demonstrated that the distribution function displays scaling only in the regime below the Kondo temperature.

The authors would like to thank the authors of Ref.  for valuable discussions. Financial support was provided by the Deutsche Forschungsgemeinschaft (DFG) and the Deutscher Akademischer Austauschdienst (DAAD).