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# Diffusion processes with Non-Markovian Transport Coefficients

## I Introduction

The fluctuation-dissipation theorem is a fundamental relationship in open system problems such as the Brownian motion . The most famous one is the Einstein relation, which connects the diffusion coefficient to the friction coefficient with the temperature as the proportional coefficient. This relationship can be easily derived if the bare potential for the Brownian particle, or more generally the collective motion, is flat and if the environment can be approximated by a canonical distribution. It has to be modified if the quantum fluctuation becomes comparable to the thermal fluctuation. When the bare potential for the collective motion is a parabolic well, the modified formula is well known. It resembles the original Einstein relation, in which temperature is replaced by an effective temperature . The effective temperature converges to the genuine temperature when the thermal energy dominates the quantal zero point motion energy of the collective motion, and it converges to the zero point motion energy in the opposite limit.

However, there exist only a few investigations when the bare potential of the collective motion is not a potential well but a potential barrier . The aim of this paper is to address to this question. Following the standard treatment for deriving the fluctuation-dissipation relation for motion in a potental well, we investigate the connection between moments of the response and the correlation functions for the motion along a potential barrier. We wish to emphasize that this study is important in various problems. One of the examples is the stability of nuclear collective excitation . Another example is the fusion between two very heavy nuclei, which is used to try to synthesize superheavy elements. In this case, the fission barrier locates inside the fusion barrier. Consequently, it is not sufficient to overcome the fusion barrier in order for the two nuclei to fuse. They have to overcome also the fission barrier. One possible theoretical approach to this problem is to apply the Fokker Planck equation, which has been originally put forward by Kramers  to describe nuclear fission and chemical reactions, to describing the time evolution from the fusion point to the region inside the fission barrier. Though several pioneering works in this method have already been published , it is not obvious whether one can apply the original Fokker Planck equation of Kramers as it is. For example, it is required to synthesize superheavy elements at temperatures as low as possible in order to sustain the shell correction energy which yields the barrier against fission by quantum effect. On the other hand, the curvature of the fission barrier is of the order of 1 MeV. One will then need to care about the quantum fluctuation. In this connection, it is highly desirable to generalize the original Fokker Planck equation by Kramers by taking quantum fluctuation into accont for the diffusion process along a potential barrier. The formalism presented here provides a first step in this direction. Following a weak-coupling treatment, we derive a generalized Fokker-Planck equation which incorporates quantum statistical effects in terms of non-Markovian transport coefficients.

The paper is organized as follows. In section II, we sketch the basic ideas of our theory to describe the time evolution of coupled collective and microscopic motions. It is a generalization of the quasi linear response theory in ref.  to include a quantum effect of the collective motion. We thus derive the generalized Fokker-Planck equation for the collective motion with non-Markovian transport coefficients. In section III, we discuss the properties of the force exerted by the microscopic motion, which we sometimes call the bath space, to determine the average classical trajectory of the collective motion. In section IV, we represent the response and the correlation functions in terms of the spectral functions , and discuss their symmetry properties. In section V, we discuss the memory times of the response and the correlation functions. In order to have some concrete ideas, we resort to the Caldeira-Leggett model  to this end. Section VI deals with the collective motion in a flat potential or in a parabolic well and derives the well known fluctuation dissipation relation including the effect of quantum fluctuation. In sect.VII we consider the case of Ohmic dissipation of the Caldeira-Leggett model, and give the explicit expressions of the odd moment of the response function and the even moment of the correlation function for the motion in a potential well and the odd moment of the response function for the motion along a potential barrier. In sect.VIII we study the properties of the even moment of the correlation function for the collective motion along a parabolic potential barrier by taking the case of the Ohmic dissipation of the Caldeira-Leggett model with a cut-off function as an example. We show the strong time dependence of the even moment of the correlation function and show that the asymptotic value as the time goes to infinity converges to a classical expectation value at high temperatures, but significantly deviates from it at low temperatures. We summarize the paper in sect. IX. Appendix A gives the main steps of the perturbation treatment of the coupled von-Neumann equations for the collective and microscopic motions and show how the reduced von-Neumann equation with non-Markovian transport coefficients is obtained. Appendix B is added to briefly sketch the symmetry property of the spectral function which is useful to derive the fluctuation-dissipation theorem. Appendix C collects some basic formulae and the spectral function of the Caldeira-Legget model. In Appendix D we present a general expression of the m-th moment of the response function for the Caldeira-Leggett model. We give an explicit expression of the linear friction for the case of Ohmic dissipation. Also we show that the linear friction is absent in the case of the super-Ohmic dissipation, and that the leading order is the n-th oder friction if the spectral density is proportional to $`\omega ^n`$.

## II Basic equations of the quasi linear response theory

### A Galilei transformation

We call the subspace of the collective motion and that of microscopic motions or environments as the subspaces A and B, respectively, and use A and B as the indices to distinguish the quantities referring to each subspace. The mass, coordinate and momentum for the collective motion are denoted by $`M`$, $`q`$ and $`p`$, respectively, while those for the environments by $`m_i,x_i,p_i,i`$ being 1,2….. We often use $`x`$ to denote the ensemble of the coordinates of the environmental degrees of freedom. As often done, quantum operators are distinguished from the corresponding c-numbers $`𝒪(t)`$ with $`\widehat{𝒪}`$.

We assume that the Hamiltonian for the total system is given by

$`\widehat{H}=\widehat{H}_A+\widehat{H}_B+\widehat{V}_c(\widehat{q},\widehat{x})`$ (1)
with

$`\widehat{H}_A={\displaystyle \frac{\widehat{p}^2}{2M}}+\widehat{U}(\widehat{q})`$ (2)
where $`\widehat{U}(\widehat{q})`$ and $`\widehat{V}_c(\widehat{q},\widehat{x})`$ are the bare potential for the collective motion and the coupling Hamiltonian, respectively. The time evolution of the density operator of the total sysytem is determined by the von-Neumann equation,

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{\rho }(t)=[\widehat{H},\widehat{\rho }(t)]`$ (3)
We first introduce the classical variables $`q(t)`$ and $`p(t)`$ in the spirit of the Ehrenfest theorem by

$`q(t)=Tr(\widehat{q}\widehat{\rho }(t)),p(t)=Tr(\widehat{p}\widehat{\rho }(t)).`$ (4)
Eq.3 leads to

$`\dot{q}(t)`$ $`=`$ $`{\displaystyle \frac{p(t)}{M}},`$ (5)
$`\dot{p}(t)`$ $`=`$ $`{\displaystyle \frac{1}{i\mathrm{}}}Tr([\widehat{p},\widehat{H}]\widehat{\rho }(t))`$ (6)
$`=`$ $`{\displaystyle \frac{1}{i\mathrm{}}}Tr(\{[\widehat{p},\widehat{U}(\widehat{q})]+[\widehat{p},\widehat{V}(\widehat{q},\widehat{x})]\}\widehat{\rho }(t))`$ (7)
We then introduce the Galilei transformation operator and the density operator in the Galilei transformed coordinate system by

$`\widehat{G}(t)=exp[{\displaystyle \frac{i}{\mathrm{}}}(p(t)\widehat{q}q(t)\widehat{p})]`$ (8)
$`\widehat{\rho }(t)=\widehat{G}(t)\widehat{\rho }_G(t)\widehat{G}^{}(t)`$ (9)
It is easy to prove that

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{\rho }_G(t)=[\widehat{H}_G(t),\widehat{\rho }_G(t)]`$ (10)
with

$`\widehat{H}_G(t)=\widehat{G}^{}(t)\widehat{H}\widehat{G}(t)i\mathrm{}\widehat{G}^{}(t){\displaystyle \frac{}{t}}\widehat{G}(t)`$ (11)
The Galilei transformation is convenient to describe a large amplitude collective motion, because one then needs to handle only the fluctuations around the mean values. Noting that,

$`\widehat{G}^{}(t)\widehat{q}\widehat{G}(t)=\widehat{q}+q(t)`$ (12)
$`\widehat{G}^{}(t)\widehat{p}\widehat{G}(t)=\widehat{p}+p(t)`$ (13)
we expand $`\widehat{H}_G`$ in the power series of the operators of the collective motion

$`\widehat{H}_G`$ $`=`$ $`cnumber+\widehat{p}\{{\displaystyle \frac{p(t)}{M}}\dot{q}(t)\}+\widehat{q}\{\dot{p}(t)+{\displaystyle \frac{U(q(t))}{q(t)}}+{\displaystyle \frac{V_c(q(t),\widehat{x})}{q(t)}}\}`$ (14)
$`+`$ $`\widehat{H}_B(\widehat{x})+V_c(q(t),\widehat{x})+{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}({\displaystyle \frac{^2U}{q^2}}+{\displaystyle \frac{^2V_c}{q^2}})_{q(t)}\widehat{q}^2+\widehat{𝒱}^{(3)}`$ (15)
where $`(\frac{^2U}{q^2}+\frac{^2V_c}{q^2})_{q(t)}`$ is the value of $`(\frac{^2U}{q^2}+\frac{^2V_c}{q^2})`$ at $`q=q(t)`$ and $`\widehat{𝒱}^{(3)}`$ is the third and higher order terms in fluctuating quantities. We note that by taking the time derivative of the equation

$`Tr(\widehat{p}\widehat{\rho }_G(t))=0`$ (16)
we obtain

$`\dot{p}(t)={\displaystyle \frac{U}{q}}Tr({\displaystyle \frac{V_c(q(t),\widehat{x})}{q}}\widehat{\rho }_G(t))+`$ (17)
where $``$ is the force exerted by the third or higher order fluctuations and it reads

$`={\displaystyle \frac{1}{3!}}Tr\{({\displaystyle \frac{^3U}{q^3}}+{\displaystyle \frac{^3V_c}{q^3}})\widehat{q}^3\widehat{\rho }_G(t)\}+\mathrm{}\mathrm{}..`$ (18)
We ignore the $`\widehat{𝒱}^{(3)}`$ in eq.(15) and correspondingly the force $``$ in eq.(17) in this work. On the other hand, the $`\widehat{q}^2`$ term on the right hand side of eq.(15), which has been ignored in , is essential to discuss the quantum fluctuation, which is the major issue in this paper. Using eqs.(5) and (17) the Hamiltonian in the Galilei transformed coordinate system can be written as

$`\widehat{H}_G`$ $`=`$ $`cnumber+\widehat{q}\widehat{F}(q(t),\widehat{x})+\widehat{h}_B(t)+{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(q(t))\widehat{q}^2`$ (19)
where $`\widehat{h}_B(t)`$, the effective Hamiltonian for the subspace B at time t, the effective coupling force $`\widehat{F}(q(t),\widehat{x})`$ and the curvature parameter $`C(q(t))`$ are given by

$`\widehat{h}_B(t)=\widehat{H}_B(\widehat{x})+V_c(q(t),\widehat{x})`$ (20)
$`\widehat{F}(q(t),\widehat{x})={\displaystyle \frac{V_c(q(t),\widehat{x})}{q}}Tr({\displaystyle \frac{V_c(q(t),\widehat{x})}{q}}\widehat{\rho }_G(t))`$ (21)
$`C(q(t))=({\displaystyle \frac{^2U}{q^2}}+{\displaystyle \frac{^2V_c}{q^2}})_{q(t)}`$ (22)
The von-Neumann equation for $`\widehat{\rho }_G(t)`$ reads

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{\rho }_G(t)=[\widehat{h}_B(t)+\widehat{q}\widehat{F}(q(t),\widehat{x})+{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(q(t))\widehat{q}^2,\widehat{\rho }_G(t)].`$ (23)
### B Fokker-Planck equation for the collective motion

We now introduce the time evolution operator for the subspace B, $`\widehat{u}_B`$, by

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{u}_B(t,t_0)=\widehat{h}_B(t)\widehat{u}_B(t,t_0)`$ (24)
with the initial condition

$`\widehat{u}_B(t_0,t_0)=1`$ (25)
and the density operator $`\widehat{D}(t)`$ by

$`\widehat{\rho }_G(t)=\widehat{u}_B(t,t_0)\widehat{D}(t)\widehat{u}_B^{}(t,t_0)`$ (26)
The density operator $`\widehat{D}(t)`$ obeys

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{D}(t)=[\widehat{q}\widehat{f}(q(t),\widehat{x}),\widehat{D}(t)]+[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(q(t))\widehat{q}^2,\widehat{D}(t)]`$ (27)
where

$`\widehat{f}(t)=\widehat{u}_B^{}(t,t_0)\widehat{F}\widehat{u}_B(t,t_0)`$ (28)
We introduce the reduced density operators for the subspaces A and B by

$`\widehat{D}_A(t)=Tr_B\widehat{D}(t),\widehat{D}_B(t)=Tr_A\widehat{D}(t)`$ (29)
and the correlation density by

$`\widehat{D}_C(t)=\widehat{D}(t)\widehat{D}_A(t)\widehat{D}_B(t)`$ (30)
These density operators obey the following coupled equations

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{D}_A(t)`$ $`=`$ $`Tr_B[\widehat{q}\widehat{f}(q(t),\widehat{x}),\widehat{D}_C(t)]+[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(q(t))\widehat{q}^2,\widehat{D}_A(t)]`$ (31)
$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{D}_B(t)`$ $`=`$ $`Tr_A[\widehat{q}\widehat{f}(q(t),\widehat{x}),\widehat{D}_C(t)]`$ (32)
$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{D}_C(t)`$ $`=`$ $`[\widehat{q}\widehat{f}(q(t),\widehat{x}),\widehat{D}_A(t)\widehat{D}_B(t)]+(1\widehat{D}_A(t)Tr_A\widehat{D}_B(t)Tr_B)[\widehat{q}\widehat{f}(q(t),\widehat{x}),\widehat{D}_C(t)]`$ (33)
$`+`$ $`[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(q(t))\widehat{q}^2,\widehat{D}_C(t)]`$ (34)
Following a similar treatment presented in , whose major steps are briefly described in the Appendix A, we derive a diffusion equation for the collective motion by handling eqs.(31) through (34) in the second order perturbation theory with respect to the fluctuating force $`\widehat{f}`$. In the derivation, we ignore the time dependence of the curvature parameter C, and introduce the moment functions $`𝒞(t,t_1)`$ and $`𝒮(t,t_1)`$ by

$`\widehat{u}_A^{(0)}(t,t_1)\widehat{q}\widehat{u}_A^{(0)}(t,t_1)=𝒞(t,t_1)\widehat{q}𝒮(t,t_1)\widehat{p}`$ (35)
where

$`\widehat{u}_A^{(0)}(t,t_1)=exp[{\displaystyle \frac{1}{i\mathrm{}}}\{{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(q(t))\widehat{q}^2\}(tt_1)]`$ (36)
They are

$`𝒞(t,t_1)`$ $`=`$ $`cos[\mathrm{\Omega }(tt_1)]`$ (37)
$`𝒮(t,t_1)`$ $`=`$ $`{\displaystyle \frac{1}{\sqrt{MC}}}sin[\mathrm{\Omega }(tt_1)]`$ (38)
with

$`\mathrm{\Omega }=\sqrt{{\displaystyle \frac{C}{M}}}`$ (39)
when $`C0`$ and

$`𝒞(t,t_1)`$ $`=`$ $`cosh[\mathrm{\Omega }(tt_1)]`$ (40)
$`𝒮(t,t_1)`$ $`=`$ $`{\displaystyle \frac{1}{\sqrt{M|C|}}}sinh[\mathrm{\Omega }(tt_1)]`$ (41)
with

$`\mathrm{\Omega }=\sqrt{{\displaystyle \frac{|C|}{M}}}`$ (42)
when $`C<0`$.

Furthermore we define the response and the correlation functions by

$`\chi _{\alpha \beta }^{()}(t,t_1)`$ $`=`$ $`{\displaystyle \frac{i}{\mathrm{}}}Tr_B([\widehat{f}_\alpha (t),\widehat{f}_\beta (t_1)]\widehat{D}_B(t_1))`$ (43)
$`\chi _{\alpha \beta }^{(+)}(t,t_1)`$ $`=`$ $`{\displaystyle \frac{1}{2}}Tr_B([\widehat{f}_\alpha (t),\widehat{f}_\beta (t_1)]_+\widehat{D}_B(t_1))`$ (44)
and their moments by

$`\chi _{\alpha \beta }^{(E)}(t)`$ $`=`$ $`{\displaystyle _{t_0}^t}𝑑t_1𝒞(t,t_1)\chi _{\alpha \beta }^{()}(t,t_1)`$ (45)
$`\chi _{\alpha \beta }^{(O)}(t)`$ $`=`$ $`{\displaystyle _{t_0}^t}𝑑t_1𝒮(t,t_1)\chi _{\alpha \beta }^{()}(t,t_1)`$ (46)
$`\chi _{\alpha \beta }^{(+E)}(t)`$ $`=`$ $`{\displaystyle _{t_0}^t}𝑑t_1𝒞(t,t_1)\chi _{\alpha \beta }^{(+)}(t,t_1)`$ (47)
$`\chi _{\alpha \beta }^{(+O)}(t)`$ $`=`$ $`{\displaystyle _{t_0}^t}𝑑t_1𝒮(t,t_1)\chi _{\alpha \beta }^{(+)}(t,t_1)`$ (48)
In these equations the lower indices $`\alpha `$ and $`\beta `$ represent the spatial component in the case when the diffusion process takes place in a multi-dimensional space. The upper indices $`E`$ and $`O`$ stand for even and odd, respectively. The von-Neumann equation for $`\widehat{D}_A(t)`$ is then given by

$`{\displaystyle \frac{}{t}}\widehat{D}_A(t)`$ $`=`$ $`{\displaystyle \frac{1}{i\mathrm{}}}[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C\widehat{q}^2,\widehat{D}_A(t)]`$ (49)
$``$ $`{\displaystyle \frac{1}{\mathrm{}^2}}[\widehat{q}_\alpha ,[\chi _{\alpha \beta }^{(+E)}(t)\widehat{q}_\beta \chi _{\alpha \beta }^{(+O)}(t)\widehat{p}_\beta ,\widehat{D}_A(t)]]`$ (50)
$``$ $`{\displaystyle \frac{1}{2i\mathrm{}}}[\widehat{q}_\alpha ,[\chi _{\alpha \beta }^{(E)}(t)\widehat{q}_\beta \chi _{\alpha \beta }^{(O)}(t)\widehat{p}_\beta ,\widehat{D}_A(t)]_+]`$ (51)
Taking the Wigner transform of each side of eq.(LABEL:DAvonNeuF) we obtain the Fokker Planck equation for the Wigner distribution function for the subspace of the collective motion $`D_{AW}(q,p,t)`$  defined by

$`D_{AW}(p,q,t)={\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑re^{ipr/\mathrm{}}<q+{\displaystyle \frac{1}{2}}r|\widehat{D}_A(t)|q{\displaystyle \frac{1}{2}}r>`$ (53)
The result reads

$`{\displaystyle \frac{}{t}}D_{AW}(t)`$ $`=`$ $`({\displaystyle \frac{1}{M}}p_\alpha {\displaystyle \frac{}{q_\alpha }}+Cq_\alpha {\displaystyle \frac{}{p_\alpha }}\chi _{\alpha \beta }^{(E)}q_\beta {\displaystyle \frac{}{p_\alpha }}+{\displaystyle \frac{1}{M}}\chi _{\alpha \beta }^{(O)}{\displaystyle \frac{}{p_\alpha }}p_\beta )D_{AW}(p,q,t)`$ (54)
$`+`$ $`({\displaystyle \frac{1}{M}}\chi _{\alpha \beta }^{(+O)}{\displaystyle \frac{^2}{p_\alpha q_\beta }}+\chi _{\alpha \beta }^{(+E)}{\displaystyle \frac{^2}{p_\alpha p_\beta }})D_{AW}(p,q,t)`$ (55)
This is a generalization of the well known Fokker Planck equation in literatures . Although it appears to be a Markovian equation, the memory effects are effectively incorporated in the transport coefficients. As a result, the formalism provides a basis for describing quantum statistical effects of collective motion. We also note that, since the derivation of eq.(55) is based on a perturbation theory with respect to the fluctuating force $`\widehat{f}`$, the formalism is valid in the weak coupling limit, where the time scales of the response and correlation functions, i.e. their memory times $`\tau _c^{()}`$ and $`\tau _c^{(+)}`$ , are much shorter than the time scale, i.e. the relaxation time $`\tau _R`$, of the collective motion . In sect.V, we discuss the properties of the response and correlation functions for the Caldeira-Leggett model, and show that their memory times $`\tau _c^{()}`$ and $`\tau _c^{(+)}`$ get very small if the cut-off frequency is large. This is consistent with the well known fact that the memory time gets very short if the collective motion couples with many incoherent degrees of freedom.

### C Coupled equations to determine fluctuations of the collective motion

We note that the average values of $`q`$ and $`p`$ are zero in the Galilei transformed space, and that the solution of eq.(55) is a Gaussian. Therefore, one can put

$`D_{AW}(p,q,t)`$ $`=`$ $`{\displaystyle \frac{1}{(2\pi )^{3/2}\mathrm{\Delta }^{1/2}}}\times exp\left[{\displaystyle \frac{1}{2\mathrm{\Delta }}}{\displaystyle \underset{i,j=1,2}{}}y_iy_j\stackrel{~}{\sigma }_{i,j}\right]`$ (56)
$`\mathrm{\Delta }`$ $`=`$ $`\sigma _{qq}\sigma _{pp}\sigma _{qp}^2`$ (57)
where $`y_1=q`$ and $`y_2=p`$ and the 2$`\times `$2 matrix $`\stackrel{~}{\sigma }`$ is the inverse matrix of the 2$`\times `$2 matrix

$`\left(\begin{array}{cc}\sigma _{qq}\hfill & \sigma _{qp}\hfill \\ \sigma _{qp}\hfill & \sigma _{pp}\hfill \end{array}\right)`$ (60)
which determines the fluctuations, i.e. the mean square deviations from the average values. The values of $`\sigma _{ij}`$ are obtained by solving the following coupled equations given by eq.(55),

$`{\displaystyle \frac{d}{dt}}\left(\begin{array}{c}\sigma _{qq}(t)\hfill \\ \sigma _{qp}(t)\hfill \\ \sigma _{pp}(t)\hfill \end{array}\right)=\left(\begin{array}{ccc}0\hfill & \frac{2}{M}\hfill & 0\hfill \\ (C\chi ^{(E)})\hfill & \frac{\chi ^{(O)}}{M}\hfill & \frac{1}{M}\hfill \\ 0\hfill & 2(C\chi ^{(E)})\hfill & 2\frac{\chi ^{(O)}}{M}\hfill \end{array}\right)\left(\begin{array}{c}\sigma _{qq}(t)\hfill \\ \sigma _{qp}(t)\hfill \\ \sigma _{pp}(t)\hfill \end{array}\right)+\left(\begin{array}{c}0\hfill \\ \frac{\chi ^{(+O)}}{M}\hfill \\ 2\chi ^{(+E)}\hfill \end{array}\right)`$ (73)
### D The Wigner distribution function in the original space

The Wigner distribution function for the collective motion in the original space fixed frame is given by

$`\rho _{AW}(q,p,t)=D_{AW}(qq(t),pp(t),t)`$ (74)
once the Wigner distribution function in the Galilei transformed space $`D_{AW}`$ is obtained from eqs.(56) and (73).

## III Classical trajectory of the collective motion

The classical trajectory of the collective motion given by $`q(t)`$ and $`p(t)`$ are determined by eqs.(5) and (17). Let us express the force induced by the coupling to microscopic motions in terms of the response function. It is useful, for example, to discuss the fluctuation-dissipation theorem. We first note that to the same order as eq.(LABEL:DAvonNeuF) the density operator for the subspace B, $`\widehat{\rho }_B(t)=Tr_A\widehat{\rho }(t)`$, obeys the following von-Neumann equation

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{\rho }_B(t)=[\widehat{h}_B(t),\widehat{\rho }_B(t)]`$ (75)
We determine $`\widehat{\rho }_B(t)`$ by a perturbation theory up to the second order of the coupling $`V_c`$. The effective force exerted on the collective motion from the bath space is then given by

$`F`$ $`{}_{BA}{}^{}=Tr_B({\displaystyle \frac{V_c(q(t),\widehat{x})}{q}}\widehat{\rho }_B(t))`$ (76)
$`=`$ $`Tr_B({\displaystyle \frac{V_c(q(t),\widehat{x})}{q}}e^{\frac{1}{i\mathrm{}}\widehat{H}_B(tt_0)}\widehat{\rho }_B(t_0)e^{\frac{1}{i\mathrm{}}\widehat{H}_B(tt_0)})`$ (77)
$``$ $`{\displaystyle \frac{1}{i\mathrm{}}}{\displaystyle _{t_0}^t}𝑑t_1Tr_B({\displaystyle \frac{V_c(q(t),\widehat{x})}{q}}[e^{\frac{1}{i\mathrm{}}\widehat{H}_B(tt_1)}V_c(q(t_1),\widehat{x})e^{\frac{1}{i\mathrm{}}\widehat{H}_B(tt_1)},e^{\frac{1}{i\mathrm{}}\widehat{H}_B(tt_0)}\widehat{\rho }_B(t_0)e^{\frac{1}{i\mathrm{}}\widehat{H}_B(tt_0)}])`$ (78)
### A Limit of ignoring the quantal effect

There are two alternative ways to write down the connection between the friction tensor and the moments of the response function. The standard way is to ignore the quantum or the memory effect and relate the friction coefficient to the first moment of the response function. As often done, in this approach, we approximate $`\widehat{\rho }_B(t_0)`$ by a canonical distribution $`\widehat{\rho }_B^{(eq)}(t)=e^{\beta (t)(\widehat{H}_B)}`$, ignore the time variation of $`\beta `$, and expand $`V_c(q(t_1),\widehat{x})`$ in the square bracket on the r.h.s. of eq.(78) around $`t_1=t`$. We then obtain

$`F_{BA}`$ $`=`$ $`Tr_B({\displaystyle \frac{V_c(q(t),\widehat{x})}{q}}\widehat{\rho }_B^{(eq)}(t))`$ (79)
$``$ $`{\displaystyle \frac{1}{i\mathrm{}}}{\displaystyle _0^{tt_0}}𝑑\tau Tr_B([{\displaystyle \frac{V_c(q(t),\widehat{x})}{q}},e^{\frac{1}{i\mathrm{}}\widehat{H}_B\tau }V_c(q(t),\widehat{x})e^{\frac{1}{i\mathrm{}}\widehat{H}_B\tau }]\widehat{\rho }_B^{(eq)}(t))`$ (80)
$``$ $`\dot{q}(t)\chi ^{(1)}(t)+\mathrm{}..`$ (81)
where the first moment of the response function $`\chi ^{(1)}(t)`$ is defined by

$`\chi _{\alpha \beta }^{(1)}(t)={\displaystyle _{t_0}^t}𝑑t_1(tt_1)\chi _{\alpha \beta }^{()}(t,t_1)`$ (82)
Eq.(81) is the expansion with respect to the moments of the response function, whose higher order terms can be ignored if the memeory time is short enough. It shows that the linear friction coefficient is given by the first moment of the response function in such cases. Note, however, that it becomes zero in some cases. As we show in Appendix D, the super-Ohmic dissipation is one of such examples.

### B Inclusion of quantum effect

The second way is to take the quantum or the memory effects into account and represent the friction coefficient in terms of the odd moment of the response function $`\chi ^{(O)}`$ to be consistent with eq.(55). In this method, we first remark the following relationship between the classical variables at two different times,

$`q(t_1)=𝒞(t,t_1)q(t)M𝒮(t,t_1)\dot{q}(t).`$ (83)
This is valid when the classical motion evolves along a parabolic potential well or a parabolic barrier without friction ,i.e. in the harmonic approximation. We expand $`V_c(q(t_1),\widehat{x})`$ in the last term on the r.h.s. of eq.(78) in powers of $`q(t_1)q(t)`$ around $`q(t)`$, and use eq.(83). This is allowed to the lowest order of the coupling strength. We then obtain

$`F_{BA}`$ $`=`$ $`Tr_B({\displaystyle \frac{V_c(q(t),\widehat{x})}{q}}\widehat{\rho }_B^{(eq)}(t))`$ (84)
$``$ $`{\displaystyle \frac{1}{i\mathrm{}}}{\displaystyle _0^{tt_0}}𝑑\tau Tr_B([{\displaystyle \frac{V_c(q(t),\widehat{x})}{q}},e^{\frac{1}{i\mathrm{}}\widehat{H}_B\tau }V_c(q(t),\widehat{x})e^{\frac{1}{i\mathrm{}}\widehat{H}_B\tau }]\widehat{\rho }_B^{(eq)}(t))`$ (85)
$`+`$ $`q(t){\displaystyle _{t_0}^t}𝑑t_1\left[𝒞(t,t_1)1\right]\chi ^{()}(t,t_1)`$ (86)
$``$ $`M\dot{q}(t)\chi ^{(O)}(t)+\mathrm{}..`$ (87)
We note that the odd moment of the response function $`\chi _{\alpha \beta }^{(O)}(t)`$ converges to the first moment of the response function in the limit of small $`\mathrm{\Omega }`$, i.e. in the limit of small $`C`$. More precisely, for small $`\mathrm{\Omega }`$

$`\chi ^{(O)}(t)=\{\begin{array}{cc}\frac{1}{M}\chi ^{(1)}(t)𝒪(\mathrm{\Omega }^2)\hfill & (C>0)\hfill \\ \frac{1}{M}\chi ^{(1)}(t)+𝒪(\mathrm{\Omega }^2)\hfill & (C<0)\hfill \end{array}`$ (90)
The results in eqs.(81) and (87) agree to each other in this limit.

## IV Properties of the response and the correlation functions in the linear response theory

### A Spectral function

We first note that $`Tr_B(\widehat{f}_\alpha (t)\widehat{f}_\beta (t_1)\widehat{D}_B(t_1))`$, which appears in the definition of the response and the correlation functions, can be rewritten as

$`Tr_B(\widehat{f}_\alpha (t)\widehat{f}_\beta (t_1)\widehat{D}_B(t_1))=Tr_B(\widehat{F}_\alpha (t)\widehat{u}_B(t,t_1)\widehat{F}_\beta (t_1)\widehat{u}_B^{}(t,t_1)\widehat{\rho }_B(t))`$ (91)
where

$`\widehat{u}_B(t,t_1)=\widehat{u}_B(t,t_0)\widehat{u}_B^{}(t_1,t_0)`$ (92)
Similarly,

$`Tr_B(\widehat{f}_\beta (t_1)\widehat{f}_\alpha (t)\widehat{D}_B(t_1))=Tr_B(\widehat{u}_B(t,t_1)\widehat{F}_\beta (t_1)\widehat{u}_B^{}(t,t_1)\widehat{F}_\alpha (t)\widehat{\rho }_B(t))`$ (93)
We consider the collective motion in the weak coupling limit, for which $`\tau _c^{(,+)}<<\tau _R`$, so that the change of the collective variable during the decay time $`\tau _c^{(,+)}`$ of the collision kernel is small. Then, we can approximate these relations by

$`Tr_B(\widehat{f}_\alpha (t)\widehat{f}_\beta (t_1)\widehat{D}_B(t_1))`$ $``$ $`Tr_B(\widehat{F}_\alpha (t)\widehat{u}_B(t,t_1)\widehat{F}_\beta (t)\widehat{u}_B^{}(t,t_1)\widehat{\rho }_B(t))`$ (94)
$`Tr_B(\widehat{f}_\beta (t_1)\widehat{f}_\alpha (t)\widehat{D}_B(t_1))`$ $``$ $`Tr_B(\widehat{u}_B(t,t_1)\widehat{F}_\beta (t)\widehat{u}_B^{}(t,t_1)\widehat{F}_\alpha (t)\widehat{\rho }_B(t))`$ (95)
where the time evolution operator $`\widehat{u}_B(t,t_1)`$ is given by

$`\widehat{u}_B(t,t_1)=Te^{\frac{1}{i\mathrm{}}_{t_1}^t\widehat{h}_B(t^{})𝑑t^{}}`$ (96)
with the time ordering operator $`T`$. For time intervals much shorter than the relaxation time of the collective motion, it can be apparoximated as,

$`\widehat{u}_B(t,t_1)=\widehat{u}_B(t;\tau =tt_1)e^{\frac{1}{i\mathrm{}}\widehat{h}_B(t)\tau }`$ (97)
We now define the spectral functions by

$`J_{\alpha ,\beta }(t;\omega )`$ $`=`$ $`{\displaystyle _{\mathrm{}}^+\mathrm{}}𝑑\tau e^{i\omega \tau }Tr_B(\widehat{F}_\alpha (t)\widehat{u}_B(t;\tau )\widehat{F}_\beta (t)\widehat{u}_B^{}(t;\tau )\widehat{\rho }_B(t))`$ (98)
$``$ $`{\displaystyle _{\mathrm{}}^+\mathrm{}}𝑑\tau e^{i\omega \tau }Tr_B(\widehat{F}_\alpha (t)e^{\frac{i}{\mathrm{}}\widehat{h}_B(t)\tau }\widehat{F}_\beta (t)e^{\frac{i}{\mathrm{}}\widehat{h}_B(t)\tau }\widehat{\rho }_B(t))`$ (99)
Inversion of these equations yields,

$`Tr_B(\widehat{F}_\alpha (t)\widehat{u}_B(t;\tau )\widehat{F}_\beta (t)\widehat{u}_B^{}(t;\tau )\widehat{\rho }_B(t))`$ $`=`$ $`{\displaystyle _{\mathrm{}}^+\mathrm{}}{\displaystyle \frac{d\omega }{2\pi }}e^{i\omega \tau }J_{\alpha ,\beta }(t;\omega )`$ (100)
$`Tr_B(\widehat{u}_B(t;\tau )\widehat{F}_\beta (t_1)\widehat{u}_B^{}(t;\tau )\widehat{F}_\alpha (t)\widehat{\rho }_B(t))`$ $`=`$ $`{\displaystyle _{\mathrm{}}^+\mathrm{}}{\displaystyle \frac{d\omega }{2\pi }}e^{i\omega \tau }J_{\beta ,\alpha }(t;\omega )`$ (101)
### B Symmetry properties

We introduce a further approximation by replacing the density operator of the subspace B with a canonical distribution,

$`\widehat{\rho }_B(t)exp\{\beta (t)(\widehat{h}_B(t))\}`$ (102)
As we show in Appendix B, the resultant specral function has the following symmetry property

$`J_{\beta ,\alpha }(t;\omega )=e^{\beta (t)\mathrm{}\omega }J_{\alpha ,\beta }(t;\omega )`$ (103)
One can then rewrite eq.(101) as

$`Tr_B(\widehat{u}_B(t;\tau )\widehat{F}_\beta (t_1)\widehat{u}_B^{}(t;\tau )\widehat{F}_\alpha (t)\widehat{\rho }_B(t))={\displaystyle _{\mathrm{}}^+\mathrm{}}{\displaystyle \frac{d\omega }{2\pi }}e^{i\omega \tau }e^{\beta (t)\mathrm{}\omega }J_{\alpha ,\beta }(t;\omega )`$ (104)
Consequently, the response and the correlation functions can be expressed as

$`\chi _{\alpha ,\beta }^{(+)}(t,t_1)=\chi _{\alpha ,\beta }^{(+)}(t;\tau =tt_1)`$ $`=`$ $`{\displaystyle _{\mathrm{}}^{\mathrm{}}}{\displaystyle \frac{d\omega }{2\pi }}e^{i\omega \tau }{\displaystyle \frac{1+e^{\beta (t)\mathrm{}\omega }}{2}}J_{\alpha ,\beta }(t;\omega )`$ (105)
$`\chi _{\alpha ,\beta }^{()}(t,t_1)=\chi _{\alpha ,\beta }^{()}(t;\tau =tt_1)`$ $`=`$ $`{\displaystyle _{\mathrm{}}^{\mathrm{}}}{\displaystyle \frac{d\omega }{2\pi }}e^{i\omega \tau }{\displaystyle \frac{i}{\mathrm{}}}\{1e^{\beta (t)\mathrm{}\omega }\}J_{\alpha ,\beta }(t;\omega )`$ (106)
Also, one can prove the following symmetry properties

$`\chi _{\alpha ,\alpha }^{(+)}(t;\tau )`$ $`=`$ $`\chi _{\alpha ,\alpha }^{(+)}(t;\tau )`$ (107)
$`\chi _{\alpha ,\alpha }^{()}(t;\tau )`$ $`=`$ $`\chi _{\alpha ,\alpha }^{()}(t;\tau )`$ (108)
Furthermore, if we define

$`\stackrel{~}{\chi }_{\alpha ,\alpha }^{(+)}(t;\omega )`$ $`=`$ $`{\displaystyle _0^{\mathrm{}}}𝑑\tau cos\omega \tau \chi _{\alpha ,\alpha }^{(+)}(t;\tau )`$ (109)
$`\stackrel{~}{\chi }_{\alpha ,\alpha }^{()}(t;\omega )`$ $`=`$ $`{\displaystyle _0^{\mathrm{}}}𝑑\tau sin\omega \tau \chi _{\alpha ,\alpha }^{()}(t;\tau )`$ (110)
then we obtain

$`\stackrel{~}{\chi }_{\alpha ,\alpha }^{(+)}(t;\omega )`$ $`=`$ $`{\displaystyle \frac{1}{2}}{\displaystyle \frac{1+e^{\beta (t)\mathrm{}\omega }}{2}}J_{\alpha ,\alpha }(t;\omega )`$ (111)
$`\stackrel{~}{\chi }_{\alpha ,\alpha }^{()}(t;\omega )`$ $`=`$ $`{\displaystyle \frac{1}{2\mathrm{}}}\{1e^{\beta (t)\mathrm{}\omega }\}J_{\alpha ,\alpha }(t;\omega )`$ (112)
## V Memory times of the response and correlation functions

An important issue to further proceed is the memory times of the response and the correlation functions. In order to see their connection to various quantities of the system such as the properties of the environments, or the coupling Hamiltonian and the temperature, we consider explicitly the case of Feynman-Vernon model , which is a popular model in open system problems and has been widely used to discuss the macroscopic quantum tunneling since the seminal work of Caldeira and Leggett . Here we discuss the case of Ohmic dissipation. It is easy to show that the response function is given by

$`\chi _{\alpha ,\alpha }^{()}(t;\tau )`$ $`=`$ $`{\displaystyle \frac{2}{\pi }}({\displaystyle \frac{df}{dq}})^2\eta {\displaystyle _0^{\mathrm{}}}sin(\omega \tau )\omega g(\omega )𝑑\omega `$ (113)
where $`g(\omega )`$ is the cut off function (see Appendix C). Using its explicit form, we have

$`\chi _{\alpha ,\alpha }^{()}(t;\tau )`$ $`=`$ $`\{\begin{array}{cc}\frac{1}{2\sqrt{\pi }}(\frac{df}{dq})^2\eta \omega _c^3\tau e^{\frac{1}{4}\omega _c^2\tau ^2}\hfill & (Gaussiancutoff)\hfill \\ (\frac{df}{dq})^2\eta \omega _c^2e^{\omega _c\tau }\hfill & (Druderegularization)\hfill \end{array}`$ (116)
Eq.(116) shows that the memory time gets shorter for larger cut-off frequency. On the other hand, the correlation function is given by

$`\chi _{\alpha ,\alpha }^{(+)}(t;\tau )`$ $`=`$ $`{\displaystyle \frac{\mathrm{}\eta }{\pi }}({\displaystyle \frac{df}{dq}})^2T{\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑\omega cos(\omega \tau ){\displaystyle \frac{\omega }{2T}}coth({\displaystyle \frac{\beta (t)\mathrm{}\omega }{2}})g(\omega )`$ (117)
Figure 1 shows the correlation function $`\chi ^{(+)}(t,\tau )`$ as a function of $`\tau `$ for three values of the cut-off frequency and for a given temperature T=1 MeV. Since we consider a linear coupling, $`\chi ^{(+)}(t;\tau )`$ is independent of time t, so that we denoted the ordinate as $`\chi ^{(+)}(\tau )`$ instead of $`\chi ^{(+)}(t,\tau )`$. The correlation function is normalized to 1.0 at $`\tau =0`$. It decreases rapidly with $`\tau `$ and converges to zero after passing through a minimum as $`\tau `$ approaches infinity. Figure 2 shows the correlation function as a function of $`\tau `$ for three values of temperature and for $`\mathrm{}\omega _c=20.0`$ MeV . It exhibits a similar behavior as in figure 1. We define the memory time $`\tau _c^{(+)}`$ as the time interval during which the correlation function becomes $`e^1`$ of its value at $`\tau =0`$. The horizontal dashed line in Figs.1 and 2 denotes the position of $`e^1`$. Figure 3 shows the deduced memory time of the correlation function as a function of the cut-off frequency for three temperatures studied in Fig.2. The memory times for T=0.1 MeV and 1.0 MeV are indistinguishable in the figure. Figure 4 shows the memory time as a function of the temperature for three values of the cut-off frequency. These results show that the memory time is nearly independent of temperature T and the cut-off frequency $`\omega _c`$ provided $`\mathrm{}\omega _c>5`$ MeV, and its magnitude is around $`\tau _c^{(+)}(0.53)10^{22}`$ second. Consequently, when the temperature is comparable or even lower than the energy of the quantum zero point motion, a sufficiently large cut-off frequency guarantees a short memory time even at such low temperatures.

## VI Fluctuation-dissipation theorem for a flat potential or a potential well in the short memory time approximation

We are now ready to derive the fluctuation-dissipation theorem in the case, where $`C0`$, i.e. for the diffusion process in a flat potential or in a potential well. We first change the integration variable in eq.(46) from $`t_1`$ to $`\tau =tt_1`$

$`\chi _{\alpha \alpha }^{(O)}(t)`$ $`=`$ $`{\displaystyle _0^{tt_0}}𝑑\tau 𝒮(t;\tau )\chi _{\alpha \alpha }^{()}(t;\tau )`$ (118)
where the quantity $`𝒮(t;\tau )`$ is given by,

$`𝒮(t,t_1)=𝒮(t;\tau =tt_1)={\displaystyle \frac{1}{\sqrt{MC}}}sin[\mathrm{\Omega }\tau ]`$ (119)
We assume that the memory time of the response function $`\tau _c^{()}`$ is much shorter than the relaxation time of the collective motion $`\tau _R`$. This condition is satisfied in the weak coupling limit if the collective motion couples with many incoherent environmental degrees of freedom as mentioned before, or if the cut off frequency is high in the case of Caldeira-Leggett model as shown explicitly by eq.(116). Then, replacing the upper limit of the integration in eq.(118) by $`\mathrm{}`$, the odd moment of the response function becomes,

$`\chi _{\alpha \alpha }^{(O)}(t)`$ $``$ $`{\displaystyle \frac{1}{\sqrt{MC}}}{\displaystyle _0^{\mathrm{}}}𝑑\tau sin\mathrm{\Omega }\tau \chi _{\alpha \alpha }^{()}(t;\tau )`$ (120)
$`=`$ $`{\displaystyle \frac{1}{\sqrt{MC}}}\stackrel{~}{\chi }_{\alpha ,\alpha }^{()}(t;\mathrm{\Omega })`$ (121)
$`=`$ $`{\displaystyle \frac{1}{\sqrt{MC}}}{\displaystyle \frac{1}{2\mathrm{}}}\{1e^{\beta (t)\mathrm{}\mathrm{\Omega }}\}J_{\alpha ,\alpha }(t;\mathrm{\Omega })`$ (122)
Assuming that the memory time of the correlation function is also much shorter than the relaxation time of the collective motion, i.e. by assuming $`\tau _c^{(+)}<<\tau _R`$, we obtain

$`\chi _{\alpha \alpha }^{(+E)}(t)={\displaystyle \frac{1}{2}}{\displaystyle \frac{1+e^{\beta (t)\mathrm{}\mathrm{\Omega }}}{2}}J_{\alpha ,\alpha }(t;\mathrm{\Omega })`$ (123)
Eqs.(122) and (123) lead to the well known quantum fluctuation-Dissipation relation,

$`{\displaystyle \frac{\chi _{\alpha \alpha }^{(+E)}(t)}{\chi _{\alpha \alpha }^{(O)}(t)}}=MT^{}`$ (124)
with the effective temperature given by

$`T^{}`$ $`=`$ $`{\displaystyle \frac{1}{2}}\mathrm{}\mathrm{\Omega }coth({\displaystyle \frac{1}{2}}\beta (t)\mathrm{}\mathrm{\Omega })`$ (125)
$`=`$ $`\{\begin{array}{cc}T\hfill & (T>>\mathrm{}\mathrm{\Omega })\hfill \\ \frac{1}{2}\mathrm{}\mathrm{\Omega }\hfill & (T<<\mathrm{}\mathrm{\Omega })\hfill \end{array}`$ (128)
## VII Dissipation coefficient for the Caldeira-Leggett model with a cut-off frequency

In this section, we derive explicit expressions of the odd moment of the response function for the case of Ohmic dissipation of the Caldeira-Leggett model.

### A Collective motion in a flat potential or in a potential well

We first consider a collective motion in a flat potential or in a potential well. Using the definition of the odd moment of the response function given by eq.(46) and the expressions derived in sect.V for the response function, we obtain for the Ohmic disspation

$`\chi _{\alpha \alpha }^{(O)}(t)={\displaystyle \frac{1}{M}}({\displaystyle \frac{df}{dq}})^2\eta g(\mathrm{\Omega })`$ (129)
Note that the magnitude of the cut-off function $`g(\mathrm{\Omega })`$ is almost one as long as the cut-off frequency is much larger than the curvature parameter $`\mathrm{\Omega }`$ of the bare potential of the collective motion. On the other hand, the corresponding $`\chi _{\alpha \alpha }^{(+E)}(t)`$ is given by

$`\chi _{\alpha \alpha }^{(+E)}(t)=\eta ({\displaystyle \frac{df}{dq}})^2{\displaystyle \frac{1}{2}}\mathrm{}\mathrm{\Omega }g(\mathrm{\Omega })coth({\displaystyle \frac{1}{2}}\beta (t)\mathrm{}\mathrm{\Omega })`$ (130)
Eqs.(129) and (130) guarantee the fluctuation-dissipation theorem eq.(124).

### B Collective motion along a potential barrier

We next consider a collective motion along a potential barrier, where the curvature parameter C is negative. In this case, eqs.(46), (41) and (113) lead to

$`\chi _{\alpha \alpha }^{(O)}(t)={\displaystyle \frac{2}{\pi }}\eta {\displaystyle \frac{1}{\sqrt{M|C|}}}({\displaystyle \frac{df}{dq}})^2{\displaystyle _0^{tt_0}}𝑑\tau sinh(\mathrm{\Omega }\tau ){\displaystyle _0^{\mathrm{}}}𝑑\omega sin\omega \tau \omega g(\omega )`$ (131)
for the case of Ohmic dissipation. For the Gaussian cut-off and the Drude reguralization, it becomes,

$`\chi _{\alpha \alpha }^{(O)}(t)`$ $`=`$ $`\{\begin{array}{cc}\frac{1}{2\sqrt{\pi }}\eta \frac{1}{\sqrt{M|C|}}(\frac{df}{dq})^2\omega _c^3_0^{tt_0}𝑑\tau sinh(\mathrm{\Omega }\tau )\tau e^{\frac{1}{4}(\omega _c\tau )^2}\hfill & (Gaussiancutoff)\hfill \\ \eta \frac{1}{\sqrt{M|C|}}(\frac{df}{dq})^2\omega _c^2_0^{tt_0}𝑑\tau sinh(\mathrm{\Omega }\tau )e^{\omega _c\tau }\hfill & (Druderegularization)\hfill \end{array}`$ (134)
Furthermore, by replacing the upper limit of the $`\tau `$ integral with $`\mathrm{}`$, we obtain

$`\chi _{\alpha \alpha }^{(O)}(t)`$ $`=`$ $`\{\begin{array}{cc}\frac{1}{M}(\frac{df}{dq})^2\eta e^{(\frac{\mathrm{\Omega }}{\omega _c})^2}\hfill & (Gaussiancutoff)\hfill \\ \frac{1}{M}(\frac{df}{dq})^2\eta \frac{\omega _c^2}{(\omega _c\mathrm{\Omega })(\omega _c+\mathrm{\Omega })}\hfill & (Druderegularization)\hfill \end{array}`$ (137)
where $`\omega _c>\mathrm{\Omega }`$ has been assumed for the case of the Drude regularization. These expressions resemble the result for the collective motion in a flat potential or in a potential well given by eq.(129). It is, however, interesting to notice that the effect of the frequency cut-ff appears in a slightly different way.

The results in this section seem to indicate that the dissipation coefficient is almost independent of the temperature of the environmental space. However, this should not be taken as a general conclusion, but rather as a feature of the linear harmonic oscillator coupling model. For example, the friction coefficient, which is calculated in a random matrix model in  for describing energy dissipation in deep inelastic heavy-ion collisions, rapidly increases with temperature.

## VIII Connection between the moments of the response and correlation functions for the diffusion along a potential barrier

Similar expression to eq.(131) can be obtained for the moment of the correlation function by using eqs.(47), (40),(105) and (C4). It reads

$`\chi _{\alpha \alpha }^{(+E)}(t)`$ $`=`$ $`{\displaystyle \frac{\mathrm{}}{\pi }}\eta ({\displaystyle \frac{df}{dq}})^2{\displaystyle _0^{tt_0}}𝑑\tau cosh(\mathrm{\Omega }\tau ){\displaystyle _0^{\mathrm{}}}𝑑\omega cos\omega \tau \omega g(\omega ){\displaystyle \frac{1+e^{\beta (t)\mathrm{}\omega }}{1e^{\beta (t)\mathrm{}\omega }}}`$ (138)
$`=`$ $`{\displaystyle \frac{\mathrm{}}{\pi }}\eta ({\displaystyle \frac{df}{dq}})^2{\displaystyle \frac{1}{2}}{\displaystyle _0^{tt_0}}𝑑\tau cosh(\mathrm{\Omega }\tau ){\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑\omega cos\omega \tau \omega g(\omega ){\displaystyle \frac{1+e^{\beta (t)\mathrm{}\omega }}{1e^{\beta (t)\mathrm{}\omega }}}`$ (139)
$`=`$ $`{\displaystyle \frac{\mathrm{}}{\pi }}\eta ({\displaystyle \frac{df}{dq}})^2{\displaystyle \frac{1}{2}}{\displaystyle _0^{tt_0}}𝑑\tau cosh(\mathrm{\Omega }\tau ){\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑\omega cos\omega \tau \omega g(\omega )coth\{{\displaystyle \frac{\beta (t)\mathrm{}\omega }{2}}\}`$ (140)
We first perform the $`\tau `$ integral analytically, then the $`\omega `$ integral using Cauchy’s residue theorem. The time integral introduces a pole at $`\omega =\pm i\mathrm{\Omega }`$, and the last factor introduces series of poles associated with the Matsubara frequency $`(2\pi /\mathrm{}\beta )n_i`$, $`n_i`$ being an integer. There appears another pole at $`\omega =\pm i\omega _c`$ if we use the Drude regularization for the high frequency cut-off. The resultant formula reads

$`\chi _{\alpha \alpha }^{(+E)}(t)={\displaystyle \frac{\mathrm{}}{\pi }}\eta ({\displaystyle \frac{df}{dq}})^2(Y_1+Y_2+Y_3)`$ (141)
with

$`Y_1`$ $`=`$ $`{\displaystyle \frac{\pi }{4}}\omega _c^2e^{\omega _c(tt_0)}cot({\displaystyle \frac{1}{2}}\beta (t)\mathrm{}\omega _c)\{{\displaystyle \frac{1}{\omega _c\mathrm{\Omega }}}e^{\mathrm{\Omega }(tt_0)}+{\displaystyle \frac{1}{\omega _c+\mathrm{\Omega }}}e^{\mathrm{\Omega }(tt_0)}\}`$ (142)
$`Y_2`$ $`=`$ $`{\displaystyle \frac{\pi }{\mathrm{}\beta (t)}}{\displaystyle \underset{n=1,2,\mathrm{}}{}}e^{\frac{\pi 2n}{\mathrm{}\beta (t)}(tt_0)}{\displaystyle \frac{\pi 2n}{\mathrm{}\beta (t)}}{\displaystyle \frac{\omega _c^2}{\omega _c^2(\frac{\pi 2n}{\mathrm{}\beta (t)})^2}}`$ (143)
$`\{{\displaystyle \frac{1}{\frac{\pi 2n}{\mathrm{}\beta (t)}\mathrm{\Omega }}}e^{\mathrm{\Omega }(tt_0)}+{\displaystyle \frac{1}{\frac{\pi 2n}{\mathrm{}\beta (t)}+\mathrm{\Omega }}}e^{\mathrm{\Omega }(tt_0)}\}`$ (144)
$`Y_3`$ $`=`$ $`\pi {\displaystyle \frac{\omega _c^2}{\omega _c^2\mathrm{\Omega }^2}}{\displaystyle \frac{1}{2}}\mathrm{\Omega }cot({\displaystyle \frac{1}{2}}\beta (t)\mathrm{}\mathrm{\Omega })`$ (145)
Note that the $`Y_1`$ term should be ignored in the limit of large $`\omega _c`$. If $`\omega _c>>T>>\mathrm{\Omega }`$, then keeping only n=1 term we have

$`Y_2{\displaystyle \frac{\pi }{\mathrm{}\beta (t)}}e^{(\mathrm{\Omega }\frac{2\pi }{\mathrm{}\beta (t)})(tt_0)}`$ (146)
and

$`Y_3{\displaystyle \frac{\pi }{\mathrm{}\beta (t)}}`$ (147)
If we keep only the $`Y_3`$ term in this case, asymptotically, i.e. as time goes to infinity, we have

$`\chi _{\alpha \alpha }^{(+E)}(t\mathrm{})\eta ({\displaystyle \frac{df}{dq}})^2{\displaystyle \frac{1}{\beta (t)}}`$ (148)
which together with eq.(137) leads to the classical fluctuation-dissipation theorem.

The even moment of the correlation function $`\chi ^{(+E)}(t)`$ is the momentum diffusion coefficient. At low temperatures, a significant deviation in the diffusion coefficient from the classical value eq.(148) is expected from quantal effects . In order to see this explicitly, in figure 5 we illustrate the normalized diffusion coefficient $`Y(t)=[Y_1(t)+Y_2(t)+Y_3(t)]\frac{\mathrm{}}{\pi }`$ as a function of time $`t`$ for several temperatures for the collective frequency $`\mathrm{}\mathrm{\Omega }=1.0`$ MeV and the cut-off frequency $`\mathrm{}\omega _c=20.0`$ MeV. The horizontal lines show the classical values determined by temperature $`Y_{clas}=T`$. At high temperatures, the normalized diffusion coefficient monotonically increases with time and gradually approaches to its classical value. However, the behavior of the diffusion coefficient is very different at low temperatures. After a sharp rise, it undershoots the classical value and may even become negative for large times. We note that a similar behaviour of the diffusion coefficient has been discussed also in  in connection with non-Markovian effects.

## IX Summary

We discussed the quantum effects on the transport coefficients for a large amplitude collective motion. To that end, we derived a Fokker Planck equation with non-Markovian transport coefficients based on a time dependent perturbation theory. We studied both cases, where the collective motion moves in a flat potentail or in a potential well, and along a potential barrier. We have shown that our formalism naturally leads to the known generalized fluctuation-dissipation theorem which combines the thermal and quantal fluctuations when the bare potential is a potential well. In the case when the collective motion moves along a potential barrier, the well known classical behaviour of the moment of the correlation function which governs the fluctuation is realized only at high temperatues. Using a numerical evaluation of the moment of the correlation function, we demonstrated that it significantly deviates from the classical expectation at low temperatures, both with respect to the time dependence and the asymptotic value.

###### Acknowledgements.

We thank M. Abe, A. Bulgac, P.G. Rheinhart and D.M. Brink for useful discussions. This work is supported in part by the Grand-in-Aid for Scientific Research from Ministry of Education, Culture, Sports, Science and Technology under Grant No. 12047203 and No. 13640253, also under the Special Area Research, Contract number 08640380, and by the Japan Society for the Promotion of Science for Young Scientists under the contract No. 12006231, and by the US DOE grant No.DE-FG05-89ER40530. N.T. thanks Tennessee Technological University for support and hospitality during his visits.

## A Derivation of the reduced von Neumann equation in the Galilei transformed coordinate system

In this Appendix, we explain the major steps to derive eq.(LABEL:DAvonNeuF) from eqs.(31) through (34) by the second order perturbation theory. We first multiply a parameter $`\lambda `$ to the fluctuating force $`\widehat{f}`$, and use it as a parameter of the perturbation theory.

As usual in the perturbation theory, we expand the reduced density operators as

$`\widehat{D}_A(t)`$ $`=`$ $`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}\lambda ^n\widehat{𝒟}_A^{(n)}(t)`$ (A1)
$`\widehat{D}_B(t)`$ $`=`$ $`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}\lambda ^n\widehat{𝒟}_B^{(n)}(t)`$ (A2)
$`\widehat{D}_C(t)`$ $`=`$ $`{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}\lambda ^n\widehat{𝒟}_C^{(n)}(t)`$ (A3)
To the zeroth order with respect to $`\lambda `$, we have

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{𝒟}_A^{(0)}(t)`$ $`=`$ $`[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(t)\widehat{q}^2,\widehat{𝒟}_A^{(0)}(t)]`$ (A4)
$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{𝒟}_B^{(0)}(t)`$ $`=`$ $`0`$ (A5)
$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{𝒟}_C^{(0)}(t)`$ $`=`$ $`[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(t)\widehat{q}^2,\widehat{𝒟}_C^{(0)}(t)]`$ (A6)
whose solutions are

$`\widehat{𝒟}_A^{(0)}(t)`$ $`=`$ $`\widehat{U}_A^{(0)}(t)\widehat{𝒟}_A^{(0)}(t_0)[\widehat{U}_A^{(0)}(t)]^{}`$ (A7)
$`\widehat{𝒟}_B^{(0)}(t)`$ $`=`$ $`\widehat{𝒟}_B^{(0)}(t_0)`$ (A8)
$`\widehat{𝒟}_C^{(0)}(t)`$ $`=`$ $`\widehat{U}_A^{(0)}(t)\widehat{𝒟}_C^{(0)}(t_0)[\widehat{U}_A^{(0)}(t)]^{}=0`$ (A9)
with

$`\widehat{U}_A^{(0)}(t)=T\{exp[{\displaystyle \frac{1}{i\mathrm{}}}{\displaystyle _{t_0}^t}({\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(t_1)\widehat{q}^2)𝑑t_1]\}`$ (A10)
where $`T`$ is the time ordering operator. We have assumed that the two subspaces A and B are decoupled at $`t=t_0`$, so that $`\widehat{𝒟}_C^{(0)}(t_0)=0`$.

To the 1st order with respect to $`\lambda `$, we have

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{𝒟}_A^{(1)}(t)`$ $`=`$ $`Tr_B[\widehat{q}\widehat{f}(t),\widehat{𝒟}_C^{(0)}(t)]+[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(t)\widehat{q}^2,\widehat{𝒟}_A^{(1)}(t)]`$ (A11)
$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{𝒟}_B^{(1)}(t)`$ $`=`$ $`Tr_A[\widehat{q}\widehat{f}(t),\widehat{𝒟}_C^{(0)}(t)]`$ (A12)
$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{𝒟}_C^{(1)}(t)`$ $`=`$ $`[\widehat{q}\widehat{f}(t),\widehat{𝒟}_A^{(0)}(t)\widehat{𝒟}_B^{(0)}(t)]+[\widehat{q}\widehat{f}(t),\widehat{𝒟}_C^{(0)}(t)]`$ (A15)
$`\widehat{𝒟}_A^{(0)}(t)Tr_A[\widehat{q}\widehat{f}(t),\widehat{𝒟}_C^{(0)}(t)]\widehat{𝒟}_B^{(0)}(t)Tr_B[\widehat{q}\widehat{f}(t),\widehat{𝒟}_C^{(0)}(t)]`$
$`+[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(t)\widehat{q}^2,\widehat{𝒟}_C^{(1)}(t)],`$
where eq.(A15) can be solved by the method of variational constant by putting

$`\widehat{𝒟}_C^{(1)}(t)=\widehat{U}_A^{(0)}(t)\widehat{C}(t)[\widehat{U}_A^{(0)}(t)]^{}`$ (A16)
The result reads

$`\widehat{𝒟}_C^{(1)}(t)`$ $`=`$ $`\widehat{U}_A^{(0)}(t)\widehat{𝒟}_C^{(1)}(t_0)[\widehat{U}_A^{(0)}(t)]^{}`$ (A17)
$`+`$ $`{\displaystyle \frac{1}{i\mathrm{}}}{\displaystyle _{t_0}^t}𝑑t_1[\widehat{U}_A^{(0)}(t,t_1)\widehat{q}[\widehat{U}_A^{(0)}(t,t_1)]^{}\widehat{f}(t_1),\widehat{U}_A^{(0)}(t,t_1)\widehat{𝒟}_A^{(0)}(t_1)[\widehat{U}_A^{(0)}(t,t_1)]^{}\widehat{𝒟}_B^{(0)}(t_1)]`$ (A18)
with

$`\widehat{U}_A^{(0)}(t,t_1)=\widehat{U}_A^{(0)}(t)\widehat{U}_A^{(0)}(t_1)^{}`$ (A19)
Now we note that we have

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{D}_A^{(2)}(t)=Tr_B[\widehat{q}\widehat{f}(t),\widehat{D}_C^{(1)}(t)]+[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(t)\widehat{q}^2,\widehat{D}_A^{(2)}(t)]`$ (A20)
in the second order approximation. Note that

$`\widehat{D}_A^{(2)}(t)`$ $`=`$ $`\widehat{𝒟}_A^{(0)}(t)+\lambda \widehat{𝒟}_A^{(1)}(t)+\lambda ^2\widehat{𝒟}_A^{(2)}(t)`$ (A21)
$`\widehat{D}_C^{(1)}(t)`$ $`=`$ $`\widehat{𝒟}_C^{(0)}(t)+\lambda \widehat{𝒟}_C^{(1)}(t)`$ (A22)
Eq.(A18) then leads to

$`i\mathrm{}{\displaystyle \frac{}{t}}\widehat{𝒟}_A^{(2)}(t)`$ $`=`$ $`{\displaystyle \frac{1}{i\mathrm{}}}{\displaystyle _{t_0}^t}dt_1Tr_B[\widehat{q}\widehat{f}(t),[\widehat{U}_A^{(0)}(t,t_1)\widehat{q}[\widehat{U}_A^{(0)}(t,t_1)]^{}\widehat{f}(t_1),`$ (A24)
$`\widehat{U}_A^{(0)}(t,t_1)\widehat{𝒟}_A^{(0)}(t_1)[\widehat{U}_A^{(0)}(t,t_1)]^{}\widehat{𝒟}_B^{(0)}(t_1)]]+[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(t)\widehat{q}^2,\widehat{D}_A^{(2)}(t)]`$
$``$ $`{\displaystyle \frac{1}{i\mathrm{}}}{\displaystyle _{t_0}^t}𝑑t_1Tr_B[\widehat{q}\widehat{f}(t),[\widehat{U}_A^{(0)}(t,t_1)\widehat{q}[\widehat{U}_A^{(0)}(t,t_1)]^{}\widehat{f}(t_1),\widehat{D}_A^{(2)}(t)\widehat{D}_B^{(2)}(t_1)]]`$ (A25)
$`+`$ $`[{\displaystyle \frac{\widehat{p}^2}{2M}}+{\displaystyle \frac{1}{2}}C(t)\widehat{q}^2,\widehat{D}_A^{(2)}(t)]`$ (A26)
The transformation from eq.(A24) to eq.(A26) is consistent with the second order perturbation theory. It is now straightforward to transform eq.(A26) into the form of eq.(LABEL:DAvonNeuF).

## B Symmetry property of the spectral function

The spectral function is given by

$`J_{\alpha ,\beta }(t;\omega )={\displaystyle _{\mathrm{}}^+\mathrm{}}𝑑\tau e^{i\omega \tau }Tr_B(\widehat{F}_\alpha (t)e^{\frac{i}{\mathrm{}}\widehat{h}_B(t)\tau }\widehat{F}_\beta (t)e^{\frac{i}{\mathrm{}}\widehat{h}_B(t)\tau }\widehat{\rho }_B(t))`$ (B1)
for a slow collective motion. We assume that the density operator of the bath space $`\widehat{\rho }_B(t)`$ can be approximated by a canonical distribution $`e^{\beta (t)(\widehat{h}_B(t))}`$. The spectral function then reads

$`J_{\alpha ,\beta }(t;\omega )={\displaystyle _{\mathrm{}}^+\mathrm{}}𝑑\tau e^{i\omega \tau }Tr_B(\widehat{F}_\alpha (t)e^{\frac{i}{\mathrm{}}\widehat{h}_B(t)\tau }\widehat{F}_\beta (t)e^{\frac{i}{\mathrm{}}\widehat{h}_B(t)\tau }e^{\beta (t)(\widehat{h}_B(t))})`$ (B2)
The key step is to insert two delta functions as follows

$`J_{\alpha ,\beta }(t;\omega )`$ $`=`$ $`{\displaystyle _{\mathrm{}}^+\mathrm{}}d\tau e^{i\omega \tau }Tr_B(\widehat{F}_\alpha (t)e^{\frac{i}{\mathrm{}}\widehat{h}_B(t)\tau }{\displaystyle _{\mathrm{}}^{\mathrm{}}}dE\delta (E\widehat{h}_B(t))\widehat{F}_\beta (t)`$ (B3)
$`{\displaystyle _{\mathrm{}}^{\mathrm{}}}dE^{}\delta (E^{}\widehat{h}_B(t))e^{\frac{i}{\mathrm{}}\widehat{h}_B(t)\tau }e^{\beta (t)(\widehat{h}_B(t))})`$ (B4)
We then obtain

$`J_{\alpha ,\beta }(t;\omega )=2\pi i{\displaystyle _{\mathrm{}}^+\mathrm{}}𝑑E{\displaystyle _{\mathrm{}}^+\mathrm{}}𝑑E^{}\delta (EE^{}\mathrm{}\omega )j_{\alpha ,\beta }(E,E^{})\rho _{eq}(E^{})`$ (B5)
where

$`j_{\alpha ,\beta }(E,E^{})=Tr_B(\widehat{F}_\alpha (t)\delta (E\widehat{h}_B(t))\widehat{F}_\beta (t)\delta (E^{}\widehat{h}_B(t))`$ (B6)
$`\rho _{eq}(E)=e^{\beta (t)(E)}`$ (B7)
One can easily prove the following symmetry relations

$`j_{\beta ,\alpha }(E^{},E)=j_{\alpha ,\beta }(E,E^{})`$ (B8)
$`[j_{\alpha ,\beta }(E,E^{})]^{}=j_{F_\alpha ^{},F_\beta ^{}}(E^{},E)`$ (B9)
We now consider

$`J_{\beta ,\alpha }(t;\omega )=2\pi i{\displaystyle _{\mathrm{}}^+\mathrm{}}𝑑E{\displaystyle _{\mathrm{}}^+\mathrm{}}𝑑E^{}\delta (EE^{}\mathrm{}\omega )j_{\beta ,\alpha }(E,E^{})\rho _{eq}(E^{})`$ (B10)
Using eqs.(B8) and (B7) and interchanging the integration variables $`E`$ and $`E^{}`$, one can prove that

$`J_{\beta ,\alpha }(t;\omega )=e^{\beta (t)\mathrm{}\omega }J_{\alpha ,\beta }(t;\omega )`$ (B11)
This proves eq.(103) in the main text.

## C Basic formulae for the Feynman-Vernon-Caldeira-Leggett model in the linear response theory

In this Appendix, we collect several basic formulae for the case, where the environment is represented by an aggregate of harmonic oscillators, and where the collective motion couples them linearly with respect to their coordinates . The unperturbed Hamiltonian of the bath space $`\widehat{H}_B`$, the coupling Hamiltonian $`\widehat{V}_c(q(t),\widehat{x}`$ and the force operator $`\widehat{F}_\alpha (q(t),\widehat{x})`$ read

$`\widehat{H}_B={\displaystyle \underset{i}{}}({\displaystyle \frac{1}{2m_1}}\widehat{p}_i^2+{\displaystyle \frac{1}{2}}m_i\omega _i^2\widehat{x}_i^2)`$ (C1)
$`\widehat{V}_c(q(t),\widehat{x})=f(q(t)){\displaystyle \underset{i}{}}c_i\widehat{x}_i`$ (C2)
$`\widehat{F}_\alpha (q(t),\widehat{x})={\displaystyle \frac{df(q(t))}{dq_\alpha }}{\displaystyle \underset{i}{}}c_i\{\widehat{x}_iTr(\widehat{x}_i\widehat{\rho }_B(t))\}`$ (C3)
In the linear response theory, we replace the $`\widehat{\rho }_B(t)`$ and $`\widehat{h}_B(t)`$ on the r.h.s. of eq.(99) by the canonical distribution $`e^{\beta (t)(\widehat{H}_B)}`$ and $`\widehat{H}_B`$, respectively. Eqs.(C1) through (C3) then lead to

$`J_{\alpha \alpha }^{(CLLR)}(t;\omega )=2\pi ({\displaystyle \frac{df}{dq}})^2{\displaystyle \underset{i}{}}c_i^2{\displaystyle \frac{\mathrm{}}{2m_i\omega _i}}\{\delta (\omega +\omega _i){\displaystyle \frac{e^{\beta (t)\mathrm{}\omega _i}}{1e^{\beta (t)\mathrm{}\omega _i}}}+\delta (\omega \omega _i){\displaystyle \frac{1}{1e^{\beta (t)\mathrm{}\omega _i}}}\}`$ (C4)
One can easily prove that this expression satisfies the symmetry property eq.(103). It would be physically reasonable to assume that all $`\omega _i`$ are positive. Then, for $`\omega >0`$, the relevant part of the spectral function is

$`J_{\alpha \alpha }^{(CLLR)}(t;\omega )=2\pi ({\displaystyle \frac{df}{dq}})^2{\displaystyle \underset{i}{}}c_i^2{\displaystyle \frac{\mathrm{}}{2m_i\omega _i}}\delta (\omega \omega _i){\displaystyle \frac{1}{1e^{\beta (t)\mathrm{}\omega _i}}}(\omega >0)`$ (C5)
We now define the spectral density $`J(\omega )`$ by

$`J(\omega )={\displaystyle \underset{i}{}}c_i^2{\displaystyle \frac{1}{m_i\omega _i}}\delta (\omega \omega _i)`$ (C6)
Following , we assume that

$`J(\omega )={\displaystyle \frac{2}{\pi }}\eta {\displaystyle \frac{1}{\omega _0^{n1}}}\omega ^ng(\omega )`$ (C7)
The cases of n=1 and n=3 correspond to the Ohmic and super Ohmic dissipations, respectively. In eq.(C7),we have introduced $`\omega _0`$ in oredr to keep the dimension of $`\eta `$ independent of $`n`$. $`g(\omega )`$ is the cut-off function, for which we assume two-types of functional forms

$`g(\omega )`$ $`=`$ $`g_1(\omega )=e^{(\frac{\omega }{\omega _c})^2}`$ (C8)
$`g(\omega )`$ $`=`$ $`g_2(\omega )={\displaystyle \frac{1}{1+(\frac{\omega }{\omega _c})^2}}.`$ (C9)
We call the first and the second the Gaussian cut off and the Drude regularization, respectively.

## D General expression of the m-th moment of the response function for the Caldeira-Leggett model

We consider

$`\chi _n^{(m)}(t)={\displaystyle \frac{2}{\pi }}\eta ({\displaystyle \frac{df}{dq}})^2{\displaystyle \frac{1}{\omega _0^{n1}}}{\displaystyle _0^{\mathrm{}}}𝑑\tau \tau ^m{\displaystyle _0^{\mathrm{}}}𝑑\omega sin\omega \tau \omega ^ng(\omega )`$ (D1)
where both n and m are integers; n,m=1,2,…. This will be the m-th moment of the response function if the spectral density is given by

$`{\displaystyle \underset{i}{}}c_i^2{\displaystyle \frac{1}{m_i\omega _i}}\delta (\omega \omega _i)={\displaystyle \frac{2}{\pi }}\eta {\displaystyle \frac{1}{\omega _0^{n1}}}\omega ^ng(\omega )`$ (D2)
One can show

$`\chi _n^{(m)}(t)`$ $`=`$ $`\eta ({\displaystyle \frac{df}{dq}})^2{\displaystyle \frac{1}{\omega _0^{n1}}}(1)^{[\frac{m}{2}]+1}{\displaystyle _{\mathrm{}}^{\mathrm{}}}𝑑\omega \omega ^ng(\omega ){\displaystyle \frac{d^m}{d\omega ^m}}\delta (\omega )`$ (D3)
$`=`$ $`\eta ({\displaystyle \frac{df}{dq}})^2{\displaystyle \frac{1}{\omega _0^{n1}}}(1)^{[\frac{m}{2}]+1}(1)^m[{\displaystyle \frac{d^m}{d\omega ^m}}\{\omega ^ng(\omega )\}]_{\omega =0}`$ (D4)
Epecially,

$`\chi _1^{(1)}(t)`$ $`=`$ $`\eta ({\displaystyle \frac{df}{dq}})^2g(0)`$ (D5)
$`\chi _3^{(1)}(t)`$ $`=`$ $`0`$ (D6)
Eq.(D5) agrees with the results eq.(90) together with eqs.(129) and (137). On the other hand, eq.(D6) means that there exists no linear friction in the case of super Ohmic dissipation. Eq.(D4) shows that the lowest order friction is n-th order friction if the spectral density is proportional to $`\omega ^n`$ as given in eq.(D2) and the friction coefficient is given by the n-th moment of the response function.

Figure captions

Figure 1. The normalized correlation function $`\chi ^{(+)}(\tau )`$ as a function of $`\tau `$ for three values of the cut-off frequency and for a temperature T=1 MeV. The horizontal dashed line shows the value $`e^1`$.

Figure 2. The normalized correlation function $`\chi ^{(+)}(\tau )`$ as a function of $`\tau `$ for three values of temperature and for a cut-off frequency $`\mathrm{}\omega _c=20.0`$ MeV. The horizontal dashed line shows the value $`e^1`$.

Figure 3. Memory time of the correlation function $`\tau _c^{(+)}`$ as a function of cut-off frequency $`\mathrm{}\omega _c`$ for three values of temperature.

Figure 4. Memory time of the correlation function $`\tau _c^{(+)}`$ as a function of temperature for three values of the cut-off frequency $`\mathrm{}\omega _c`$.

Figure 5. The normalized diffusion coefficent $`Y(t)`$ as a function of $`t`$ for several values of temperature and for a collective frequency $`\mathrm{}\mathrm{\Omega }=1.0`$ MeV and a cut-off frequency $`\mathrm{}\omega _c=20.0`$ MeV. The horizontal dashed lines show the corresponding classical values.


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# Physics potential and present status of neutrino factories

## 1 Introduction

The observation of atmospheric neutrinos (See, e.g., Ref.$`^\mathrm{?}`$) and solar neutrinos (See, e.g., Ref.$`^\mathrm{?}`$) gives the information on the mass squared differences and the mixings, which can be written in the three flavor framework of neutrino oscillations as ($`|\mathrm{\Delta }m_{32}^2|`$, $`\theta _{23}`$) and ($`\mathrm{\Delta }m_{21}^2`$, $`\theta _{12}`$), where I have adopted the standard parametrization $`^\mathrm{?}`$ for the $`3\times 3`$ MNSP $`^{\mathrm{?},\mathrm{?}}`$ matrix. On the other hand, the CHOOZ result $`^\mathrm{?}`$ tells us that $`|\theta _{13}|`$ has to be small ($`\mathrm{sin}^22\theta _{13}<0.1`$). So the MNSP matrix looks like

$`U_{MNSP}\left(\begin{array}{ccc}c_{}& s_{}& ϵ\\ s_{}/\sqrt{2}& c_{}/\sqrt{2}& 1/\sqrt{2}\\ s_{}/\sqrt{2}& c_{}/\sqrt{2}& 1/\sqrt{2}\end{array}\right),`$ (4)
where I have used $`\theta _{23}\pi /4`$, $`\mathrm{sin}^22\theta _{12}\mathrm{sin}^22\theta _{}0.8`$ and $`|ϵ|1`$.

The next thing to do is to determine $`\theta _{13}`$, the sign of $`\mathrm{\Delta }m_{32}^2`$ and the CP phase $`\delta `$. During the past few years a lot of research have been done on the possibilities of future long baseline experiments. One is a super-beam experiment and the other one is a neutrino factory. The former is super intense conventional neutrino beam which is obtained from pion decays while the latter is from muon decays in a storage ring. The background fraction $`f_B`$ in the case of super-beams $`^\mathrm{?}`$ is of order $`10^2`$, while in the case of a neutrino factory $`^\mathrm{?}`$ it is or order $`10^5`$. The advantage of a neutrino factory is such low background fraction and neutrino factories are expected to enable us to determine $`\theta _{13}`$ and the sign of $`\mathrm{\Delta }m_{32}^2`$ ($`\delta `$) for $`\mathrm{sin}^22\theta _{13}>10^5`$ ($`10^3`$), respectively.

In this talk I will mainly discuss measurements of the CP phase $`\delta `$ at neutrino factories and will try to clarify the reason why some group obtains different results for the optimized muon energy and baseline.

## 2 Measurements of the CP phase at neutrino factories

Measurement of the CP phase in neutrino oscillations is difficult not only because CP violating contribution in the oscillation probability is in general small but also because there is matter effect. Namely, the dependence of the probabilities for $`\nu `$ and $`\overline{\nu }`$ on $`\delta `$ and $`A`$ is given by $`P(\nu _\mu \nu _e)=f(E,L;\theta _{ij},\mathrm{\Delta }m_{ij}^2,\delta ;A)`$ and $`P(\overline{\nu }_\mu \overline{\nu }_e)=f(E,L;\theta _{ij},\mathrm{\Delta }m_{ij}^2,\delta ;A)`$, where $`f`$ is a certain function and $`A\sqrt{2}G_FN_e`$ stands for the matter effect. The quantity obtained from experiments on $`\overline{\nu }`$ is not $`f(\mathrm{},\delta ;A)`$, so that direct comparison between $`f(\mathrm{},\delta ;A)`$ and $`f(\mathrm{},\delta ;A)`$ is impossible in a strict sense. The situation here is different from the the $`K^0\overline{K}^0`$ system where the quantity $`N(K_L2\pi )/N(K_L3\pi )`$ immediately gives us evidence for CP violation. Hence I have to compromise and adopt a kind of indirect measurement of CP violation, i.e., I deduce the values of $`\delta `$ etc. by comparing the energy spectra of the data and of the theoretical prediction with neutrino oscillations assuming the three flavor mixing. In determining $`\delta `$, there are other oscillation parameters as well as the density of the Earth whose values are not exactly known, so that I have to take into account correlations of errors of these parameters.aaaCorrelations of errors at neutrino factories were studied in Ref. $`^{\mathrm{?},\mathrm{?},\mathrm{?},\mathrm{?},\mathrm{?}}`$. Thus I introduce the following quantity to see the significance of the case with nonvanishing $`\delta `$:

$`\mathrm{\Delta }\chi ^2\underset{_{\overline{\theta _k\mathrm{}},\overline{\mathrm{\Delta }m_k\mathrm{}^2},\overline{A}}}{\mathrm{min}}`$ $`{\displaystyle \underset{j}{}}`$ $`\{{\displaystyle \frac{\left[N_j(\nu _e\nu _\mu )\overline{N}_j(\nu _e\nu _\mu )\right]^2}{\sigma _j^2}}`$ (5)
$`+`$ $`{\displaystyle \frac{\left[N_j(\overline{\nu }_e\overline{\nu }_\mu )\overline{N}_j(\overline{\nu }_e\overline{\nu }_\mu )\right]^2}{\sigma _j^2}}`$
$`+`$ $`{\displaystyle \frac{\left[N_j(\nu _\mu \nu _\mu )\overline{N}_j(\nu _\mu \nu _\mu )\right]^2}{\sigma _j^2}}`$
$`+`$ $`{\displaystyle \frac{\left[N_j(\overline{\nu }_\mu \overline{\nu }_\mu )\overline{N}_j(\overline{\nu }_\mu \overline{\nu }_\mu )\right]^2}{\sigma _j^2}}\},`$
where $`N_j(\nu _\alpha \nu _\beta )N_j(\nu _\alpha \nu _\beta ;\theta _k\mathrm{},\mathrm{\Delta }m_k\mathrm{}^2,\delta ,A)`$, $`\overline{N}_j(\nu _\alpha \nu _\beta )\overline{N}_j(\nu _\alpha \nu _\beta ;\overline{\theta _k\mathrm{}},\overline{\mathrm{\Delta }m_k\mathrm{}^2},\overline{\delta }=0,\overline{A})`$ stand for the numbers of events of the data and of the theoretical prediction with a vanishing CP phase, respectively, and $`\sigma _j^2`$ stands for the error which is given by the sum of the statistical and systematic errors. At neutrino factories appearance and disappearance channels for $`\nu `$ and $`\overline{\nu }`$ are observed, and I have included the numbers of events of all the channels in (5) to gain statistics. In the present analysis, $`N_j(\nu _\alpha \nu _\beta )`$ is substituted by theoretical prediction with a CP phase $`\delta `$ and $`\mathrm{\Delta }\chi ^2`$ obviously vanishes if $`\delta =0`$.bbbThis is the reason why the quantity in (5) is denoted as $`\mathrm{\Delta }\chi ^2`$ instead of absolute $`\chi ^2`$. $`\mathrm{\Delta }\chi ^2`$ represents deviation from the best fit point rather than the goodness of fit. The quantity $`\mathrm{\Delta }\chi ^2`$ reflects the strength of the correlation of the parameters, i.e., if $`\mathrm{\Delta }\chi ^2`$ turns out to be very small for a certain value of $`\overline{A}`$ then the correlation between $`\delta `$ and $`A`$ would be very strong and in that case there would be no way to show $`\delta 0`$. To reject a hypothesis “$`\delta =0`$” at the 3$`\sigma `$ confidence level I demand

$`\mathrm{\Delta }\chi ^2\mathrm{\Delta }\chi ^2(3\sigma CL)`$ (6)
where the right hand side stands for the value of $`\chi ^2`$ which gives the probability 99.7% in the $`\chi ^2`$ distribution with a certain degrees freedom, and $`\mathrm{\Delta }\chi ^2(3\sigma CL)`$=20.1 for 6 degrees freedom. From (6) I get the condition for the detector size to reject a hypothesis “$`\delta =0`$” at 3$`\sigma `$CL.

On the other hand, Koike et al.$`^\mathrm{?}`$ claim that another quantity

$`\mathrm{\Delta }\stackrel{~}{\chi }^2\underset{_{\overline{\theta _k\mathrm{}},\overline{\mathrm{\Delta }m_k\mathrm{}^2},\overline{A}}}{\mathrm{min}}{\displaystyle \underset{j}{}}{\displaystyle \frac{1}{\sigma _j^2}}\left[{\displaystyle \frac{N_j(\nu _e\nu _\mu )}{N_j(\overline{\nu }_e\overline{\nu }_\mu )}}{\displaystyle \frac{\overline{N}_j(\nu _e\nu _\mu )}{\overline{N}_j(\overline{\nu }_e\overline{\nu }_\mu )}}\right]^2`$ (7)
should be used since this particular combination improves the correlation between $`\delta `$ and $`A`$. In my opinion, however, both analyses with $`\mathrm{\Delta }\chi ^2`$ and $`\mathrm{\Delta }\stackrel{~}{\chi }^2`$ are based on indirect measurements of CP violation anyway and there is no reason why one has to discard other information on $`\delta `$. In fact it turns out that (7) is a combination in which the correlation between $`\delta `$ and $`A`$ improves for low energy and worsens at high energy.

It should be pointed out here that indirect measurements of CP violation are also considered in the $`B^0\overline{B}^0`$ system.cccThe term ”indirect” in the B system is different from that in neutrino oscillations. To measure the phase $`\varphi _1`$, direct CP violating process $`B(\overline{B})J/\psi K_s`$ is used $`^{\mathrm{?},\mathrm{?}}`$, while those to measure $`\varphi _2`$ and $`\varphi _3`$ are $`B2\pi `$ $`^\mathrm{?}`$ and $`BDK`$ $`^\mathrm{?}`$, which are not necessarily CP–odd processes. Their strategy is to start with the three flavor framework, to use the most effective process, which may or may not be CP–odd, to determine the CP phases and to check unitarity or consistency of the three flavor hypothesis.

The optimized muon energy $`E_\mu `$ and baseline $`L`$ for the measurement of CP the phase at a neutrino factory have been investigated by several groups by taking into consideration the correlations of $`\delta `$ and all other parameters and the results are summarized in Table 1. The results in Ref.$`^\mathrm{?}`$ are given in Fig. 2, which shows that the more uncertainty I have in the density, the shorter baseline I have to choose because the correlation between $`\delta `$ and $`A`$ becomes stronger for larger baseline and muon energy. The works $`^{\mathrm{?},\mathrm{?},\mathrm{?}}`$, which basically used $`\mathrm{\Delta }\chi ^2`$ in (5), agree with each other to certain extent (there are some differences on the reference values for the oscillation parameters) while the result by Koike et al.$`^\mathrm{?}`$ is quite different from others. This discrepancy is due to the fact that they adopted $`\mathrm{\Delta }\stackrel{~}{\chi }^2`$ in (7) as was mentioned above. There are slight differences between the results by the group $`^{\mathrm{?},\mathrm{?}}`$ and those by the other $`^\mathrm{?}`$ and this appears to come from different statistical treatments. In the future it should be studied what makes a difference to get the optimum set $`(E_\mu ,L)`$. The detector size required to reject a hypothesis ”$`\delta `$=0” as a function of $`\theta _{13}`$ is given in Figure 3 (taken from Ref.$`^\mathrm{?}`$). Figure 3 shows the sensitivity of neutrino factories to the CP phase.

## 3 High energy behaviors of $`\mathrm{\Delta }\chi ^2`$

Some people have questioned whether the sensitivity to the CP phase at a neutrino factory increases infinitely as the muon energy increases, and Lipari$`^\mathrm{?}`$ concluded that the sensitivity is lost at high energy. In the work $`^\mathrm{?}`$ the behaviors of $`\mathrm{\Delta }\chi ^2`$ in (5) was studied analytically for high muon energy and it was shown after the correlations between $`\delta `$ and any other oscillation parameter or $`A`$ is taken into account that

$`\mathrm{\Delta }\chi ^2\left({\displaystyle \frac{J}{\mathrm{sin}\delta }}\right)^2{\displaystyle \frac{1}{E_\mu }}\left(\mathrm{sin}\delta +\text{const}{\displaystyle \frac{\mathrm{\Delta }m_{32}^2L}{E_\mu }}\mathrm{cos}\delta \right)^2`$ (8)
for large $`E_\mu `$, where $`J(c_{13}/8)\mathrm{sin}2\theta _{12}\mathrm{sin}2\theta _{13}\mathrm{sin}2\theta _{23}\mathrm{sin}\delta `$ stands for the Jarlskog parameter. The behavior (8) is the same as that for $`\mathrm{\Delta }\stackrel{~}{\chi }^2`$ in (7) and it is qualitatively consistent with the claim by Lipari $`^\mathrm{?}`$. It is remarkable that (8) is different from a naively expected behavior

$`\mathrm{\Delta }\chi _{\text{naive}}^2E_\mu (\mathrm{cos}\delta 1)^2.`$
This is because the correlation between $`\delta `$ and other parameters is taken into account. Koike et al.$`^\mathrm{?}`$ criticize the analysis with $`\mathrm{\Delta }\chi ^2`$ by saying that this quantity looks mainly at the CP conserving part at high muon energy (10GeV$`<E_\mu <`$50GeV). The behavior (8) indicates, however, that CP violating part becomes dominant after the correlation between $`\delta `$ and other parameters is taken into consideration and the criticism by Koike et al.$`^\mathrm{?}`$ does not apply.

## 4 Parameter degeneracy

The discussions in the previous sections have been focused on rejection of a hypothesis “$`\delta =0`$”. Once $`\delta `$ is found to be nonvanishing, it becomes important to determine the precise value of $`\delta `$. It has been pointed out that various kinds of parameter degeneracy exist. Burguet-Castell et al.$`^\mathrm{?}`$ found degeneracy in ($`\delta `$, $`\theta _{13}`$), Minakata and Nunokawa $`^\mathrm{?}`$ found the one in the sign of $`\mathrm{\Delta }m_{32}^2`$, and Barger et al.$`^\mathrm{?}`$ found the one in the sign of $`\pi /4\theta _{23}`$. To understand the four-fold ambiguity it is instructive to draw a trajectory in the $`P(\nu _\mu \nu _e)`$$`P(\overline{\nu }_\mu \overline{\nu }_e)`$ plane (See Figure 4 taken from Ref.$`^\mathrm{?}`$). From Figure 4 it is obvious that there exists four-fold ambiguity for a given set of the oscillation parameters. Also the position of the ellipse has degeneracy in interchanging $`\theta _{23}\pi /2\theta _{23}`$, so that in general eight-fold degeneracy is expected. $`^\mathrm{?}`$ It was proposed $`^{\mathrm{?},\mathrm{?},\mathrm{?}}`$ to do experiments at two baselines to remove this degeneracy. In reality one has to evaluate numbers of events for $`\nu _\mu \nu _e`$ and $`\overline{\nu }_\mu \overline{\nu }_e`$ (Notice that Figure 4 deals with the probabilities only), and the correlations of errors have to be taken into consideration as well, so determination of the oscillation parameters is even more difficult than what Figure 4 indicates.

## 5 Summary

People in the field reached consensus that neutrino factories can measure the CP phase $`\delta `$ with the detector size larger than $`10^{21}\mu `$100kt$``$yr for $`\mathrm{sin}^22\theta _{13}>10^3`$ unless $`|\delta |`$ is small. The detailed study on the optimized muon energy and baseline still needs to be done.

## Acknowledgments

I would like to thank Noriaki Kitazawa for useful discussions on CP violation in the B meson system and for providing references on the subject. This research was supported in part by a Grant-in-Aid for Scientific Research of the Ministry of Education, Science and Culture, #12047222, #13640295.

## References


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# References

PARAMETER MISMATCHES AND PERFECT ANTICIPATING SYNCHRONIZATION IN BI-DIRECTIONALLY COUPLED EXTERNAL CAVITY LASER DIODES

E. M. Shahverdiev, S.Sivaprakasam and K. A. Shore

School of Informatics, University of Wales, Bangor, Dean Street, Bangor, LL57 1UT, Wales, UK

ABSTRACT

We study perfect chaos synchronization between two bi-directionally coupled external cavity semiconductor lasers and demonstrate for the first time that mismatches in laser photon decay rates can explain the experimentally observed anticipating time in synchronization.
PACS numbers(s):05.45.Xt,05.45.Vx,42.55.Px,42.65.Sf
Chaos synchronization  is of fundamental importance in a variety of complex physical, chemical and biological systems . Application of chaos synchronization has been advanced in secure communications, optimization of non-linear system performance, modeling brain activity and pattern recognition . Time-delay systems are ubiquitous in nature, technology and society because of finite signal transmission times, switching speeds and memory effects . Therefore the study of chaos synchronization in these systems is of considerable practical significance. Because of their ability to generate high-dimensional chaos, time-delay systems are good candidates for secure communications based on chaos synchronization. In this context particular emphasis is given to the use of chaotic external cavity semiconductor lasers .
Following the discovery of anticipating synchronization by Voss , Masoller studied theoretically and numerically anticipating synchronization in unidirectionally coupled lasers and showed that the anticipating time should be equal to the difference between round-trip time of the light in the transmitter’s external cavity and the time of flight between the lasers . The first experimental observation of anticipating synchronization between two bi-directionally coupled external cavity laser diodes was reported recently .In a bi-directional system such anticipating chaos is rather robust but it has proved to be rather difficult to obtain a reproducible demonstration of anticipating synchronization in unidirectionally coupled laser diodes. It is noted also that it was found experimentally  that the solitary receiver laser anticipates the chaotic transmitter by the time of flight between the lasers. At present there is no full theoretical explanation of the experimental results.
In this Brief Report we demonstrate the possibility of perfect chaos synchronization between two bi-directionally coupled external cavity semiconductor lasers. We demonstrate, for the first time, that mismatches in laser photon decay rates can explain the time of flight anticipating time synchronization between the laser diodes. In a recent paper  we have demonstrated the role which parameter mismatches plays in the explanation of the coupling-delay lag time synchronization in uni-directionally coupled systems. Knowledge of the exact time shift between the synchronized states is of obvious considerable practical importance for the recovery of message at the receiver of a chaotic communication system .
An appropriate framework for treating the evolution of the electric field of external cavity laser diodes is provided by the widely utilised Lang-Kobayashi equations . Suppose that the master laser is described by the equations

$$\frac{dE_1}{dt}=\frac{(1+ı\alpha _1)}{2}(\frac{G_1(N_1N_{01})}{1+s_1|E_1|^2}\gamma _1)E_1(t)+k_1E_1(t\tau _1)\mathrm{exp}(ı\omega \tau _1)+k_3E_2(t\tau _2)\mathrm{exp}(ı\omega \tau _2),$$

$$\frac{dN_1}{dt}=J_1\gamma _{e1}N_1\frac{G_1(N_1N_{01})}{1+s_1|E_1|^2}|E_1|^2,(1)$$

is coupled bidirectionally with the slave laser described by equations

$$\frac{dE_2}{dt}=\frac{(1+ı\alpha _2)}{2}(\frac{G_2(N_2N_{02})}{1+s_2|E_2|^2}\gamma _2)E_2(t)+k_2E_2(t\tau _1)\mathrm{exp}(ı\omega \tau _1)+k_3E_1(t\tau _2)\mathrm{exp}(ı\omega \tau _2),$$

$$\frac{dN_2}{dt}=J_2\gamma _{e2}N_2\frac{G_2(N_2N_{02})}{1+s_2|E_2|^2}|E_2|^2,(2)$$

where $`E_{1,2}`$ are the slowly varying complex fields for the master and slave lasers,respectively;$`N_{1,2}`$ are the carrier densities;$`\gamma _{1,2}`$ are the cavity losses;$`\alpha _{1,2}`$ are the linewidth enhancement factors;$`G_{1,2}`$ are the optical gains;$`k_{1,2}`$ are the feedback levels;$`k_3`$ is the coupling rate;$`\omega `$ is the optical frequency without feedback (no frequency detuning between the two lasers);$`\tau _1`$ is the round-trip time in the external cavity;$`\tau _2`$ is the time of flight between the master laser and the slave laser-coupling delay time;$`J_{1,2}`$ are the injection currents;$`\gamma _{e1,e2}^1`$ are the carrier lifetimes;$`s_{1,2}`$ are the gain saturation coefficients.
We show that mismatches between the master and slave laser photon decay rates $`\gamma _1\gamma _2`$ can result in the experimentally observed time of flight anticipating synchronization time. Mathematically the intensities of the master and slave lasers should be related by

$$I_1=I_{2,\tau _2}(3)$$

Throughout this paper $`x_\tau x(t\tau )`$. We also assume an analogous synchronization manifold for the carrier densities:$`N_1=N_{2,\tau _2}`$. Using eq.(2) we write the dynamical equation for the $`E_{2,\tau _2}`$ in the following manner:

$$\frac{dE_{2,\tau _2}}{dt}=\frac{(1+ı\alpha _2)}{2}(\frac{G_2(N_{2,\tau _2}N_{02})}{1+s_2|E_{2,\tau _2}|^2}\gamma _2)E_{2,\tau _2}+k_3E_{1,2\tau _2}\mathrm{exp}(ı\omega \tau _2),$$

In accordance with experiments  we consider the case of a solitary slave laser,i.e. $`k_2=0`$. It is assumed that, except for the photon decay rates, the laser parameters are identical. Then we find that the equations for $`E_1`$ and $`E_{2,\tau _2}`$ will be identical and therefore perfect synchronization (3) will be possible if conditions

$$\frac{(1+ı\alpha )}{2}\gamma _1=\frac{(1+ı\alpha )}{2}\gamma _2k_3\mathrm{exp}(ı\omega \tau _2),(4)$$

(where $`\alpha =\alpha _1=\alpha _2`$)
and

$$k_1E_1(t\tau _1)\mathrm{exp}(ı\omega \tau _1)=k_3E_1(t2\tau _2)\mathrm{exp}(ı\omega \tau _2).(5)$$

are met.
One can easily re-write condition (4) in the more appealing form:

$$(\gamma _1\gamma _2)^2=\frac{4k_3^2}{1+\alpha ^2},(6)$$

At first glance it may seems rather unusual to impose conditions on the chaotic transmitter itself as in (5). But, given the presence of six free parameters, this condition is not particulary restrictive.
(Indeed ,in certain cases no such restrictions are needed at all. For example, assuming $`\tau _1=2\tau _2`$ one finds that the perfect synchronization manifold (3) exists for $`k_1=k_3`$ and $`\omega \tau _2=2\pi n`$(where $`n=0,1,2\mathrm{}`$). We also notice that the synchronization manifolds $`I_1=I_{2,\tau _2}`$ and $`I_1=I_{2,\tau _1\tau _2}`$ are identical for $`\tau _1=2\tau _2`$, but in general, $`I_1=I_{2,\tau _1\tau _2}`$ is not the synchronization manifold.) Our approach, in principle allows also for anticipating synchronization with time of flight anticipation time, even in the case when $`\tau _1=\tau _2`$, as was reported experimentally . Thus we conjecture that mismatches in laser cavity decay rates- as could be expected in practice- renders practically impossible the observation of anticipating synchronization between unidirectionally coupled lasers. Here we would like to underline that mismatches in laser cavity decay rates are perfectly adequate to explain the time of flight lag time synchronization in uni-directionally coupled chaotic external cavity laser diodes . In  it is shown that the perfect lag synchronization manifold $`I_2=I_{1,\tau _2}`$ exists simply under the conditions (4) and $`k_1=k_2`$.
We conclude this Brief Report with the following remarks. Usually parameter mismatches are considered to have a detrimental effect on the synchronization quality between coupled identical systems: in the case of small parameter mismatches the synchronization error does not decay to zero with time, but can show small fluctuations about zero or even a non-zero mean value . Larger values of parameter mismatches can even result in the loss of synchronization. However it appears that in reality the relation between chaos synchronization in time-delayed systems and parameter mismatches is quite intricate and complex. In a recent paper  we have shown that parameter mismatches can change the time shift between the synchronized states;moreover we have presented an example where the presence of parameter mismatches is the only way to achieve chaos synchronization between two unidirectionally coupled time-delayed systems. In the present Brief Report we have shown that perfect anticipating synchronization between two bi-directionally coupled external cavity laser diodes is possible in the presence of parameter mismatches. As knowledge of the time shift between the synchronized states is of considerable practical importance for the message recovery in communications and information processing using chaos control methods, further research on relation between chaos synchronization and parameter mismatches would be desirable.
This work is supported by UK EPSRC under grants GR/R22568/01 and GR/N63093/01.