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# Crossover Temperature from Non-Fermi Liquid to Fermi Liquid Behavior in Two Types of Impurity Kondo Model

## 1 Introduction

Non-Fermi-liquid (NFL) behavior observed in some heavy fermion compounds and High $`T_\mathrm{c}`$ cuprates has stimulated intense studies for a variety of impurity models which have NFL quantum-critical points.$`^{\text{?}\text{}\text{?}\text{}\text{?}\text{}\text{?}\text{}\text{?}\text{)}}`$ While each of the models has its own energy scale $`T_\mathrm{K}`$ below which the thermodynamic and transport properties are geverned by the NFL fixed point, relevant perturbation which is normaly present in real systems introduces another energy scale $`T_\mathrm{x}`$ where crossover to the Fermi-liquid (FL) fixed point occurs. In other words, the NFL behavior can be observed only when $`T_\mathrm{x}/T_\mathrm{K}1`$. Since real systems would not be exactly on the critical points, it is important to know about the above condition that NFL behavior occurs. In this paper, we investigate the crossover energy scale $`T_\mathrm{x}`$ so that the condition $`T_\mathrm{x}/T_\mathrm{K}1`$ is specified in a microscopic sense by using the numerical renormalization-group (NRG) method$`^{\text{?}\text{}\text{?}\text{}\text{?}\text{)}}`$ for two types of the quantum impurity model, the two-channel Kondo model in the presence of a magnetic field and the two-impurity Kondo model, with a special emphasis on the effect of channel anisotropy.

The non-Fermi-liquid fixed point of the multichannel Kondo model in the overscreened case, i.e., when the number of channels $`n`$ is larger than twice the size of impurity spin $`S`$, is characterized by a degeneracy of the ground state which cannot be completely lifted by coupling to conduction electrons.$`^{\text{?, }\text{?}\text{)}}`$ The residual entropy is given by $`\mathrm{ln}[\mathrm{sin}[(2S+1)\pi /(n+2)]/\mathrm{sin}[\pi /(n+2)]]`$.$`^{\text{?}\text{}\text{?}\text{)}}`$ In temperature $`T`$ below the Kondo temperature $`T_\mathrm{K}`$, the specific heat coefficient $`\gamma `$ and magnetic susceptivility $`\chi `$ are $`T^{4/(n+2)1}`$, the electrical resistivity $`\rho `$ is $`const.\pm T^{2/(n+2)}`$.$`^{\text{?, ?, }\text{?}\text{}\text{?}\text{)}}`$ A magnetic field or channel anisotropy is relevant so that it brings about crossover to Fermi-liquid fixed points but $`\gamma `$, $`\chi `$ and $`\rho `$ keep the above scaling laws when $`T_\mathrm{x}TT_\mathrm{K}`$. Fig.1 presents a schematic phase diagram in the case of $`n=2`$, $`S=1/2`$ in which $`\gamma `$, $`\chi |\mathrm{ln}T|`$ and $`\rho const.\pm \sqrt{T}`$ in the region $`T_\mathrm{x}TT_\mathrm{K}`$. The two-channel Kondo model has been regarded as one of the most probable candidates responsible for the NFL behavior observed in U alloys.$`^{\text{?)}}`$ Recently, the multichannel Kondo model with channel anisotropy has been discussed in relation to singular effects of impurities in the region around the ferromagnetic quantum-critical point.$`^{\text{?}\text{)}}`$

The crossover behavior to the FL fixed point in the $`n=2`$, $`S=1/2`$ Kondo model with channel anisotropy and/or in the presence of a magnetic field has been investigated by a variety of methods.$`^{\text{?}\text{}\text{?}\text{}\text{?}\text{}\text{?}\text{}\text{?}\text{}\text{?}\text{}\text{?}\text{}\text{?}\text{)}}`$ It can be easily seen in the impurity entropy which decreases from $`\mathrm{ln}\sqrt{2}`$ to $`0`$ around $`T_\mathrm{x}`$ as temperature is lowered. The crossover temperature $`T_\mathrm{x}`$ is proportional to the square of relevant perturbation as follows:

$$T_\mathrm{x}h^2,$$
(1.1a)
in the presense of a magnetic field $`H`$ where $`h=\mu _\mathrm{B}H`$;

$$T_\mathrm{x}(J_1J_2)^2,$$
(1.1b)
in the channel anisotropic case where $`J_1`$ and $`J_2`$ are the exchange couplings for two channels, respectively.$`^{\text{?, ?)}}`$ On the other hand, the impurity free energy $`F_{\mathrm{imp}}`$ has the following scaling form:

$$F_{\mathrm{imp}}(r;T,h)=Tf(r,T/T_\mathrm{K},h/T),$$
(1.2)
where $`r`$ is a dimensionless function of $`D`$, $`J_1`$ and $`J_2`$ which depends on a cutoff scheme and in general unknown.$`^{\text{?)}}`$ Since $`r`$ represents channel anisotropy, $`r=0`$ if $`J_1=J_2`$. From eqs. (1.1a) and (1.2), we can easily see that $`T_\mathrm{x}h^2/T_\mathrm{K}`$ so that crossover from NFL to FL regime occurs if $`(h/T_\mathrm{K})^21`$ in the isotropic channel case.$`^{\text{?, ?, ?)}}`$ In the case of channel anisotropy, however, eqs. (1.1b) and (1.2) tell us nothing about the condition that the NFL behavior can be seen. Our main purpose is to identify this condition analyzing temperature dependence of the entropy by the NRG method and it will be emphasized that crossover from the NFL to FL regime can occur even if $`|J_1J_2|>T_\mathrm{K}`$.

The two-impurity Kondo model is also known to have a NFL critical point, which arises from competition between the interimpurity antiferromagnetic interaction and single-channel Kondo effects.$`^{\text{?)}}`$ The nature of criticality of this system has been well understood. $`^{\text{?, }\text{?}\text{}\text{?}\text{}\text{?}\text{}\text{?}\text{)}}`$ The residual entropy is $`\mathrm{ln}\sqrt{2}`$ at the critical point just like the $`n=2`$, $`S=1/2`$ single impurity Kondo model which was discussed in the above. The staggered impurity susceptibility $`\chi _\mathrm{s}`$ is $`|\mathrm{ln}T|`$ when $`T_\mathrm{x}TT_\mathrm{K}`$. Recently, it has been shown that a similar mechanism works in the model with the competition between the Kondo singlet and $`f^2`$-crystalline-electric-field singlet explaining the NFL behavior observed in R1-xUxRu2Si2 (R=Th, Y and La, $`x0.07`$).$`^{\text{?}\text{}\text{?}\text{)}}`$

The crossover temperature $`T_\mathrm{x}`$ of the two-impurity Kondo model is known to be proportinal to $`(K_\mathrm{c}K)^2`$ where $`K`$ is the interimpurity antiferromagnetic (RKKY) coupling constant and $`K_\mathrm{c}`$ is the critical coupling.$`^{\text{?)}}`$ We will also elucidate an explicit expression of the crossover temperature of this model and discuss similarities of the crossover behavior to that of the two-channel anisotropic Kondo model in a magnetic field.

The organization of this paper is as follows. In §2, we discuss effects of channel anisotropy and a magnetic field in the two-channel Kondo model. In §3, we study the crossover behavior of the two-impurity Kondo model around the criticality. Finally, we summarize our results in §4.

## 2 Anisotropic Two-Channel Kondo Model in a Magnetic Field

### 2.1 Model and numerical procedure

In this section, we discuss crossover from the NFL to FL regime in the $`n=2`$, $`S=1/2`$ Kondo model with channel anisotropy and in a magnetic field described by the following Hamiltonian:

$`H=H_\mathrm{K}+H_\mathrm{I}+H_\mathrm{Z},`$ (2.1)
$`H_\mathrm{K}={\displaystyle \underset{m=1,2}{}}{\displaystyle \underset{k,\sigma }{}}ϵ_kc_{km\sigma }^{}c_{km\sigma },`$ (2.2)
$`H_\mathrm{I}={\displaystyle \underset{m=1,2}{}}{\displaystyle \underset{k,k^{},\sigma ,\sigma ^{}}{}}J_mc_{km\sigma }^{}\stackrel{}{\sigma }_{\sigma \sigma ^{}}c_{k^{}m\sigma ^{}}\stackrel{}{S},`$ (2.3)
$`H_\mathrm{Z}=2hS_z.`$ (2.4)
Here $`m`$ ($`=1,2`$) is the index of two channels, $`\sigma `$ is the spin index, $`c_{km\sigma }^{}`$ is the creation operator of the conduction electron, $`\stackrel{}{S}`$ is the impurity spin and $`\stackrel{}{\sigma }`$ is the vector formed by the Pauli matrices. $`H_\mathrm{Z}`$ represents the Zeeman term where the $`g`$-factor is taken as $`2`$. When $`J_1`$=$`J_2`$ and $`h`$=$`0`$, one obtains the isotropic two-channel Kondo Hamiltonian leading to the NFL stable fixed point. The case of $`J_1`$$``$$`J_2`$ corresponds to the anisotropic two-channel Kondo Hamiltonian whose stable fixed point is that of FL.

To analyze the Hamiltonian eq. (2.1) by the NRG method,$`^{\text{?, ?, ?)}}`$ we transform eqs. (2.2) and (2.3) into

$`H_\mathrm{K}={\displaystyle \frac{(1+\mathrm{\Lambda }^1)D}{2}}{\displaystyle \underset{m=1,2}{}}{\displaystyle \underset{n=0}{\overset{\mathrm{}}{}}}{\displaystyle \underset{\sigma }{}}\mathrm{\Lambda }^{n/2}`$
$`\times (f_{m,n\sigma }^{}f_{m,n+1\sigma }+f_{m,n+1\sigma }^{}f_{m,n\sigma }),`$ (2.5)
$`H_\mathrm{I}={\displaystyle \frac{(1+\mathrm{\Lambda }^1)D}{2}}{\displaystyle \underset{m=1,2}{}}{\displaystyle \underset{\sigma ,\sigma ^{}}{}}J_mf_{m,0\sigma }^{}\stackrel{}{\sigma }_{\sigma \sigma ^{}}f_{m,0\sigma ^{}}\stackrel{}{S},`$ (2.6)
where $`f_{m,n}`$ $`(f_{m,n}^{})`$ is annihilation (creation) operator of the conduction electron in the Wannier representation whose extent $`k_\mathrm{F}^1\mathrm{\Lambda }^{n/2}`$. $`\mathrm{\Lambda }`$ is a logarithmic discretization parameter in NRG calculation, $`D`$ is half the bandwidth of the conduction electrons. Following an usual procedure of the NRG method, we define $`H_N`$ as

$`H_N`$ $`=`$ $`\mathrm{\Lambda }^{(N1)/2}[{\displaystyle \underset{m}{}}{\displaystyle \underset{\sigma }{}}{\displaystyle \underset{n=0}{\overset{N1}{}}}\mathrm{\Lambda }^{n/2}(f_{m,n\sigma }^{}f_{m,n+1\sigma }+\mathrm{h}.\mathrm{c})`$ (2.7)
$`+`$ $`J_m{\displaystyle \underset{\sigma ,\sigma ^{}}{}}f_{m,0\sigma }^{}\stackrel{}{\sigma }_{\sigma ,\sigma ^{}}f_{m,0\sigma ^{}}\stackrel{}{S}].`$
Then, the Hamiltonian (2.7) satisfies the recursion relation

$`H_{N+1}`$ $`=`$ $`\mathrm{\Lambda }^{1/2}H_N+{\displaystyle \underset{m,\sigma }{}}(f_{m,N\sigma }^{}f_{m,N+1\sigma }+f_{m,N+1\sigma }^{}f_{m,N\sigma }).`$ (2.8)
By repeated use of the recursive procedure, we can compute the eigen states and energy levels of Hamiltonians ($`H_N`$).

Once the energy levels of $`H_N`$ are obtained, the entropy can be calculated by the relation

$`S=\beta _N(H_NF_N),`$ (2.9)
in each $`N`$-step. Here $`H_N`$ and $`F_N`$ are defined as

$`H_\mathrm{N}`$ $`=`$ $`{\displaystyle \frac{\mathrm{Tr}H_Ne^{\beta _NH_N}}{\mathrm{Tr}e^{\beta _NH_N}}},`$
$`F_N`$ $`=`$ $`{\displaystyle \frac{1}{\beta _N}}\mathrm{ln}Z_N={\displaystyle \frac{1}{\beta _N}}\mathrm{ln}(\mathrm{Tr}e^{\beta _NH_N}),`$ (2.10)
where $`\beta _N=\mathrm{\Lambda }^{(N1)/2}/T`$. By setting $`TT_N\mathrm{\Lambda }^{(N1)/2}`$, we can obtain temperature dependence of the entropy with a good accuracy in NRG calculation.

In our calculation, we set $`\beta _N^1=0.5`$ and $`\mathrm{\Lambda }=3`$ and about 600 total states are retained at each iteration. Hereafter, we take the unit of energy as $`(1+\mathrm{\Lambda }^1)D/2`$.

### 2.2 Crossover temperature $`T_\mathrm{x}`$

In this subsection, we elucidate an explicit expression of the crossover temperature $`T_\mathrm{x}`$ of the model, eq. (2.1), from NRG results on the impurity entropy $`S_{\mathrm{imp}}(T)`$. As mentioned in §1, if $`0`$$`<`$$`T_\mathrm{x}/T_\mathrm{K}`$$``$$`1`$, $`S_{\mathrm{imp}}(T)`$ of this model decreases from $`1/2\mathrm{ln}2`$ to $`0`$ around $`T_\mathrm{x}`$ as $`T`$ is lowered. So $`T_\mathrm{x}`$ can be defined as temperature at which the entropy takes a value of $`S_{\mathrm{imp}}(T_\mathrm{x})`$=$`1/4\mathrm{ln}2`$, the middle point between NFL and FL fixed points. (For examples, see Fig. 2 below.)

Firstly, we investigate an effect of channel anisotropy on $`T_\mathrm{x}`$ for $`h=0`$. In this case, we can assume that $`T_\mathrm{x}`$ is described by a function of two parameters, i.e., $`J_{\mathrm{av}}(J_1+J_2)/2`$ and $`\mathrm{\Delta }JJ_1J_2`$. Our procedure to determine $`T_\mathrm{x}`$ is illustrated in Fig. 2 (a) and (b) which present NRG results on $`S_{\mathrm{imp}}(T)`$ for $`J_{\mathrm{av}}=0.1`$, $`\mathrm{\Delta }J=1.0\times 10^4`$ and for $`J_{\mathrm{av}}=10`$, $`\mathrm{\Delta }J=1.0\times 10^3`$, respectively. It is noted that $`T_\mathrm{x}/T_\mathrm{K}1`$ while $`\mathrm{\Delta }J>T_\mathrm{K}`$ in both (a) and (b). These examples lead us to the fact that $`T_\mathrm{x}`$ is not scaled as $`T_\mathrm{x}\mathrm{\Delta }J^2/T_\mathrm{K}`$. (If $`T_\mathrm{x}`$ were $`\mathrm{\Delta }J^2/T_\mathrm{K}`$, $`\mathrm{\Delta }J`$ should be much less than $`T_\mathrm{K}`$ for $`T_\mathrm{x}/T_\mathrm{K}1`$.) Actually, we have tested a bunch of parameter sets and found a function which reproduces the behavior of $`T_\mathrm{x}`$ as follows:

$`T_\mathrm{x}=\alpha \times (\mathrm{\Delta }\stackrel{~}{J}/\stackrel{~}{J}_{\mathrm{av}})^2e^{1/\stackrel{~}{J}_{\mathrm{av}}},`$ (2.11)
where $`\alpha `$ is a numerical constant which is taken to be $`\alpha =2.95`$ within the accuracy of our calculation, and

$`\mathrm{\Delta }\stackrel{~}{J}`$ $`=`$ $`A_\mathrm{\Lambda }\mathrm{\Delta }J,`$ (2.12)
$`\stackrel{~}{J}_{\mathrm{av}}`$ $`=`$ $`A_\mathrm{\Lambda }J_{\mathrm{av}},`$ (2.13)
$`A_\mathrm{\Lambda }`$ $`=`$ $`{\displaystyle \frac{1}{2}}{\displaystyle \frac{1+\mathrm{\Lambda }^1}{1\mathrm{\Lambda }^1}}\mathrm{ln}\mathrm{\Lambda }.`$ (2.14)
Here $`A_\mathrm{\Lambda }`$ is a revision factor of the density of states in NRG calculation. Fig. 3 shows that $`T_\mathrm{x}`$ is well fitted by eq. (2.11). From Fig. 3 (a) in which $`J_{\mathrm{av}}`$=$`0.3`$ is fixed, $`T_\mathrm{x}`$ can be seen to be proportional to $`\mathrm{\Delta }J^2`$, which is consistent with the results of Pang and Cox.$`^{\text{?)}}`$ On the other hand, from Fig. 3 (b) in which $`\mathrm{\Delta }J`$=$`1.0\times 10^3`$ is fixed, $`J_{\mathrm{av}}`$-dependence of $`T_\mathrm{x}`$ can be seen to be equivalent to that of the right hand side of eq. (2.11). In the weak-coupling case of $`J_{\mathrm{av}}`$$`<`$$`0.4`$, $`T_\mathrm{x}`$ is an increasing function of $`J_{\mathrm{av}}`$ as can be seen in Fig. 3 (b) while $`T_\mathrm{K}`$ is well known to be an increasing function $`J_{\mathrm{av}}e^{1/J_{\mathrm{av}}}`$ in the case of $`n=2`$ by the two-loop perturbative renormalization group theory. It is noted that if $`T_\mathrm{x}`$ were $`\mathrm{\Delta }J^2/T_\mathrm{K}`$, $`T_\mathrm{x}`$ should be a decreasing function of $`J_{\mathrm{av}}`$ in the weak-coupling regime. (See also Fig. 4 (b) for comparison.)

We have checked that eq. (2.11) can be adopted in a wide parameter region of $`J_{\mathrm{av}}`$ for the $`n=2`$, $`S=1/2`$ Kondo model with channel anisotropy. In the weak-coupling regime, from eq. (2.11) and $`T_\mathrm{K}J_{\mathrm{av}}e^{1/J_{\mathrm{av}}}`$, the condition that crossover from NFL to FL regime occurs, i.e. $`T_\mathrm{x}/T_\mathrm{K}`$$``$$`1`$, is given explicitly by $`\mathrm{\Delta }J^2/J_{\mathrm{av}}^3`$$``$$`1`$. This result indicates that the NFL behavior in the two-channel Kondo model is fairly robust against channel anisotropy.

Next, we investigate an effect of a magnetic field in the isotropic channel case of $`J_1`$=$`J_2`$$``$$`J`$. In this case, as mentioned in §1, $`T_\mathrm{x}`$ is $``$$`h^2/T_\mathrm{K}`$.$`^{\text{?, ?, ?)}}`$ As shown in Fig. 4 (a) and (b), it can be actually checked from our NRG results on the entropy that $`T_\mathrm{x}`$ can be well fitted by a function of

$`T_\mathrm{x}=\beta \times h^2/T_\mathrm{K},`$ (2.15)
where $`\beta `$ is a numerical constant of $`\beta =4.45`$. Here $`T_\mathrm{K}`$ is defined in terms of the dynamical impurity susceptibility $`\chi (\omega )`$ by

$`T_\mathrm{K}\underset{\omega 0}{lim}\underset{T0}{lim}\left[\mathrm{Im}\chi (\omega )\right]^1,`$ (2.16)
for the isotropic channel model in the absence of a magnetic field$`^{\text{?}\text{}\text{?}\text{}\text{?}\text{)}}`$ in which the value of $`T_\mathrm{K}`$ is normalized to coincide with $`Je^{1/J}`$ ($``$$`T_\mathrm{K}^p`$) at $`J`$=$`0.1`$.

Eq. (2.15) is valid in a wide region from weak to strong coupling. This suggests that eq. (2.16) is a good definition of $`T_\mathrm{K}`$. In Fig. 5, we show $`J`$-dependence of $`T_\mathrm{K}`$, which is defined by eq. (2.16), and of $`T_\mathrm{K}^p`$, which is the two-loop perturbative renormalization group result. While $`T_\mathrm{K}^p`$ is a monotonously increasing function of $`J`$, $`T_\mathrm{K}`$ exhibits a broad peak at or around $`J`$$``$$`1.3`$. The discrepancy between $`T_\mathrm{K}`$ and $`T_\mathrm{K}^p`$ indicates that the two-loop perturbative renormalization group result on the Kondo temperature is not sufficient for $`J>0.5`$.

### 2.3 Scaling function for entropy in the crossover regime

We have obtained an explicit expression of $`T_\mathrm{x}`$, eq. (2.11), in the conventional band-width cutoff scheme for the $`n=2`$, $`S=1/2`$ Kondo model with channel anisotropy. On the other hand, the thermodynamic Bethe ansatz (TBA) equations for the anisotropic multichannel Kondo model was obtained by Andrei and Jerez.$`^{\text{?)}}`$ While their cutoff scheme differs substantially from ours, and so does their expression of $`T_\mathrm{x}`$ ($`T_\mathrm{K}`$), their $`n=2`$, $`S=1/2`$ model must be in the same universality class as ours. It is thus possible to make a comparison of our NRG results with the TBA result by use of our expression of $`T_\mathrm{x}`$ (if necessary, $`T_\mathrm{K}`$). In this subsection, we concentrate on the crossover regime in which $`0<S_{\mathrm{imp}}(T)<\mathrm{ln}\sqrt{2}`$, $`T`$$``$$`T_\mathrm{K}`$, and explicitly show that our NRG results on the entropy can be fitted by a scaling function of $`T`$$`/`$$`T_\mathrm{x}`$.

First, we derive the scaling function in the crossover regime analytically from the TBA equations. In the scaling limit, the impurity part of the free energy is given by$`^{\text{?)}}`$

$$F_{\mathrm{imp}}(T)=\frac{T}{2\pi }_{\mathrm{}}^{\mathrm{}}\frac{\mathrm{ln}[1+\eta _1(\xi )]}{\mathrm{cosh}[\xi +\mathrm{ln}(T/T_\mathrm{K})]}d\xi ,$$
(2.17)
where $`\eta _1(\xi )`$ is determined by the TBA equations;

$`\mathrm{ln}\eta _1(\xi )=2r\mathrm{e}^\xi +G\mathrm{ln}[1+\eta _2(\xi )],`$ (2.18)
$`\mathrm{ln}\eta _2(\xi )=\mathrm{e}^\xi +G\mathrm{ln}[1+\eta _1(\xi )]+G\mathrm{ln}[1+\eta _3(\xi )],`$ (2.19)
$`\mathrm{ln}\eta _j(\xi )=G\mathrm{ln}[1+\eta _{j1}(\xi )]+G\mathrm{ln}[1+\eta _{j+1}(\xi )],j3,`$ (2.20)
with a boundary condition

$$\underset{j\mathrm{}}{lim}\frac{\mathrm{ln}\eta _j(\xi )}{j}=\frac{2h}{T}.$$
(2.21)
Here $`G\phi (\xi )_{\mathrm{}}^{\mathrm{}}G(\xi \xi ^{})\phi (\xi ^{})d\xi ^{}`$ and $`G(\xi \xi ^{})1/2\pi \mathrm{cosh}(\xi \xi ^{})`$. For $`TT_\mathrm{K}`$, the impurity free energy, eq. (2.17), is determined by the $`\xi `$$``$$`+\mathrm{}`$ asymptotic form of $`\eta _1`$. In the limit of $`\xi `$$``$$`+\mathrm{}`$, $`\eta _j`$ is given by

$$\eta _j(+\mathrm{})=\frac{\mathrm{sinh}^2[(j1)h/T]}{\mathrm{sinh}^2(h/T)}1,j2.$$
(2.22)
Firstly, we consider the case of $`T`$$``$$`h`$$``$$`T_\mathrm{K}`$. By eq. (2.22), $`\eta _3(+\mathrm{})\mathrm{exp}(2h/T)`$ and its corrections due to $`\xi `$ dependence can be neglected, so that eq. (2.19) leads to

$$\mathrm{ln}\eta _2(\xi )=\mathrm{e}^\xi +h/T+f(r,\mathrm{e}^\xi ,h/T),$$
(2.23)
where $`f`$ is defined by eq. (1.2). In eq. (2.23), the last term can be seen to compare negligibly with $`h/T`$ if we note that this term is $``$$`F_{\mathrm{imp}}(T)/T`$ in a region around $`\xi `$$``$$`\mathrm{ln}(T_\mathrm{K}/T)`$. Then, after some manipulations of eqs. (2.17), (2.18) and (2.23), we obtain

$$F_{\mathrm{imp}}(T)\frac{T}{2\pi }_{\mathrm{}}^{\mathrm{}}\frac{\mathrm{ln}[1+\mathrm{exp}((h/T)\epsilon (\zeta ))]}{\mathrm{cosh}[\zeta +\mathrm{ln}(h/T_\mathrm{K})]}d\zeta ,$$
(2.24)
where $`\epsilon (\zeta )`$ is given by

$`\epsilon (\zeta )`$ $`=`$ $`\mathrm{e}^\zeta \left(2r+{\displaystyle \frac{1}{2\pi }}\mathrm{ln}\left(1+\mathrm{e}^{2\zeta }\right){\displaystyle \frac{1}{\pi }}\mathrm{e}^\zeta \mathrm{tan}^1\left(\mathrm{e}^\zeta \right)\right),`$ (2.25)
$``$ $`\mathrm{e}^\zeta \left(2r\mathrm{e}^{2\zeta }/2\pi \right),\mathrm{for}\mathrm{e}^\zeta h/T_\mathrm{K}1.`$ (2.26)
The integral in eq. (2.24) has dominant contributions from a region around $`\zeta \mathrm{ln}(T_\mathrm{K}/h)`$. When $`r(h/T_\mathrm{K})^2`$, the second term can be neglected in eq. (2.26) so that the impurity free energy can be written in the following scaling form:

$$F_{\mathrm{imp}}(T)=T\stackrel{~}{f}(T/T_\mathrm{x}),$$
(2.27)
where the crossove temperature is given by $`T_\mathrm{x}=rT_\mathrm{K}`$ and $`\stackrel{~}{f}`$ is a scaling function in the crossover regime;

$`\stackrel{~}{f}(x)`$ $`=`$ $`{\displaystyle _{\mathrm{}}^{\mathrm{}}}{\displaystyle \frac{\mathrm{ln}[1+\mathrm{exp}(2\mathrm{exp}(\xi ))]}{2\pi \mathrm{cosh}[\xi +\mathrm{ln}(x)]}}d\xi `$ (2.28)
$`=`$ $`{\displaystyle \frac{1}{\pi x}}\mathrm{ln}{\displaystyle \frac{1}{\pi x}}{\displaystyle \frac{1}{\pi x}}\mathrm{ln}\mathrm{\Gamma }\left({\displaystyle \frac{1}{\pi x}}+{\displaystyle \frac{1}{2}}\right)+{\displaystyle \frac{1}{2}}\mathrm{ln}2\pi ,`$ (2.29)
where $`\mathrm{\Gamma }`$ is the gamma function. Then, the impurity entropy, $`S_{\mathrm{imp}}`$=$`F_{\mathrm{imp}}/T`$, is calculated as

$`S_{\mathrm{imp}}(T)`$ $`=`$ $`{\displaystyle \frac{1}{\pi (T/T_\mathrm{x})}}\psi \left({\displaystyle \frac{1}{\pi (T/T_\mathrm{x})}}+{\displaystyle \frac{1}{2}}\right){\displaystyle \frac{1}{\pi (T/T_\mathrm{x})}}`$ (2.30)
$`\mathrm{ln}\mathrm{\Gamma }\left({\displaystyle \frac{1}{\pi (T/T_\mathrm{x})}}+{\displaystyle \frac{1}{2}}\right)+{\displaystyle \frac{1}{2}}\mathrm{ln}2\pi ,`$
where $`\psi `$ is the digamma function. On the other hand, when $`r(h/T_\mathrm{K})^2`$, the first term can be neglected in eq.(2.26). In this case, if the crossover temperature is regarded as $`T_\mathrm{x}`$=$`h^2/4\pi T_\mathrm{K}`$, $`T`$-dependent contributions in the impurity free energy is given by $`T\stackrel{~}{f}(T/T_\mathrm{x})`$ and therefore eq. (2.30) is also available for the entropy.

Secondly, we consider the case of $`h`$$`<`$$`T`$$``$$`T_\mathrm{K}`$. By eqs. (2.19) and (2.22), $`\mathrm{ln}\eta _2(\xi )`$$``$$`\mathrm{e}^\xi `$ so that $`\mathrm{ln}\eta _1(\xi )`$$``$$`2r\mathrm{e}^\xi `$. Hence eq. (2.30) is available by $`T_\mathrm{x}`$=$`rT_\mathrm{K}`$. It is noted that if $`r(h/T_\mathrm{K})^2`$, $`T_\mathrm{x}`$=$`rT_\mathrm{K}`$$``$$`h`$$`<`$$`T`$ so that the entropy is $``$$`\mathrm{ln}\sqrt{2}`$, which is not sensitive to the value of $`T_\mathrm{x}`$.

In summary, a scaling function for entropy in the crossover regime is given by eq. (2.30) where $`T_\mathrm{x}`$=$`rT_\mathrm{K}`$ for $`r`$$``$$`(h/T_\mathrm{K})^2`$ and $`T_\mathrm{x}`$=$`h^2/4\pi T_\mathrm{K}`$ for $`r`$$``$$`(h/T_\mathrm{K})^2`$. For eq. (2.30), $`S_{\mathrm{imp}}`$$`(T_\mathrm{x})`$=$`0.99`$$`\times `$$`1/4`$$``$$`\mathrm{ln}2`$ so that $`T_\mathrm{x}`$ is about the same as we defined in the former subsection. (We must apologize for the normalization schemes on $`T_\mathrm{K}`$ which are different between the former and this subsections.)

Second, we compare our NRG results on entropy with eq. (2.30). Figures 6 and 7 present the results on entropy versus temperature scaled by $`T_\mathrm{x}`$, expressions of which are eq. (2.11) and eq. (2.15), in the anisotropic channel case and in the presence of a magnetic field, respectively. In both cases, the $`T`$ dependence of entropy can be fitted quite well in the crossover regime by the scaling function, eq. (2.30), derived from the TBA equations.

## 3 Two-Impurity Kondo Model

### 3.1 Model

In this section, we study the two-impurity Kondo model whose Hamiltonian is given by two independent Kondo models coupled by interimpurity exchange interaction ($`K`$) as follows:

$`H=H_\mathrm{K}+H_\mathrm{I}^{}+H_\mathrm{L},`$ (3.1)
$`H_\mathrm{K}={\displaystyle \underset{m=1,2}{}}{\displaystyle \underset{k,\sigma }{}}ϵ_kc_{km\sigma }^{}c_{km\sigma },`$ (3.2)
$`H_\mathrm{I}^{}={\displaystyle \underset{m=1,2}{}}J_m{\displaystyle \underset{k,k^{},\sigma ,\sigma ^{}}{}}c_{km\sigma }^{}\stackrel{}{\sigma }_{\sigma \sigma ^{}}c_{k^{}m\sigma ^{}}\stackrel{}{S}_m,`$ (3.3)
$`H_\mathrm{L}=K\stackrel{}{S}_1\stackrel{}{S}_2.`$ (3.4)
The notations are the same as before. In the original form of the two-impurity Kondo model studied by Jones et al., $`^{\text{?)}}`$ the Kondo exchange coupling between the conduction electrons and localized spin with both the same and different symmetry (specified by $`m`$) are taken into account, because they considered the case of the two impurities on different sites. In the present study, we neglect the Kondo exchange coupling between different symmetries, for simplicity. It is however noted that our model, eq. (3.1), itself can be considered to be a local-moment version of the two-orbital Anderson model with crystalline-electric-field (CEF) effect in a certain pseudospin representation.$`^{\text{?, ?)}}`$

The model, eq. (3.1) has a NFL fixed point at $`K`$=$`K_\mathrm{c}(J_1,J_2)`$ for a set of $`J_1`$ and $`J_2`$ due to competition between the single channel Kondo effects and the interimpurity antiferromagnetic interaction.$`^{\text{?, ?, ?, ?, ?, ?, ?, }\text{?}\text{)}}`$ In this section, we concentrate on the region around critical points of $`K`$=$`K_\mathrm{c}(J,J)`$. The definition of $`T_\mathrm{x}`$ is the same as that of the former section; $`S_{\mathrm{imp}}(T_\mathrm{x})`$=$`1/4\mathrm{ln}2`$.

### 3.2 Crossover temperature $`T_\mathrm{x}`$ in the region around critical points of $`K`$=$`K_\mathrm{c}(J,J)`$

Firstly, we consider cases in which $`K`$ is displaced slightly away from a critical value of $`K_\mathrm{c}`$$``$$`K_\mathrm{c}(J,J)`$ with $`J_1`$=$`J_2`$=$`J`$ fixed. It has already been discussed by using the conformal field theory that $`T_\mathrm{x}`$ is proportional to $`\mathrm{\Delta }K^2/T_\mathrm{K}`$, $`^{\text{?)}}`$ where $`\mathrm{\Delta }K`$=$`K_\mathrm{c}K`$. Here we define $`T_\mathrm{K}`$ by

$`T_\mathrm{K}\underset{\omega 0}{lim}\underset{T0}{lim}1/\mathrm{Im}\chi _\mathrm{s}(\omega ),`$ (3.5)
where $`\chi _\mathrm{s}`$ is the dynamical impurity susceptibility for $`\stackrel{}{S_1}\stackrel{}{S_2}`$. We have examined various parameter sets and confirmed that the crossover temperature $`T_\mathrm{x}`$ is given as

$`T_\mathrm{x}=\gamma \times \mathrm{\Delta }K^2/T_\mathrm{K},`$ (3.6)
where $`\gamma `$ is a numerical constant of $`\gamma `$=$`0.50`$ within the accuracy of our calculation. In fact, as shown in Fig. 8, the temperature dependence of entropy can be scaled by $`T_\mathrm{x}`$ defined by eq.(3.6) quite well.

Next, we consider cases in which $`J_2`$ is displaced slightly away from $`J_2`$=$`J`$ with $`J_1`$=$`J`$ and $`K`$=$`K_\mathrm{c}`$$``$$`K_\mathrm{c}(J,J)`$ fixed. In Fig. 9, we show the behavior of a crossover for $`J_1`$=$`0.3`$, $`J_2`$=$`0.297`$, and $`K`$=$`K_\mathrm{c}`$=$`0.195416`$, compared with the case of the two-channel Kondo model with $`J_1`$=$`0.3`$ and $`J_2`$=$`0.297`$. The isotropic channel cases in both models are also shown in this figure. In both cases, the small perturbation ($`J_1J_2`$) does not affect the high temperature behavior. Namely, it does not change $`T_\mathrm{K}`$. The temperature dependence of entropy in the anisotropic channel case is quite similar in both cases in the crossover regime. Hence $`T_\mathrm{x}`$ for the two-impurity model is also given by eq. (2.11).

## 4 Summary

In this paper, we have investigated effects of relevant perturbations, which bring about crossover from the NFL to FL regime, in the regions around quantum critical points of the two-channel and two-impurity Kondo models.

For the two-channel Kondo model in which $`T_\mathrm{K}`$ is defined by $`T_\mathrm{K}lim_{\omega 0}lim_{T0}[\mathrm{Im}\chi (\omega )]^1`$ (in the weak-coupling regime, $`T_\mathrm{K}`$$``$$`J_{\mathrm{av}}\mathrm{e}^{1/J_{\mathrm{av}}}`$), we have derived numerically exact expressions of the crossover temperature $`T_\mathrm{x}`$ from our NRG results on the entropy as follows: (1) in the anisotropic channel case, if $`T_\mathrm{x}`$/$`T_\mathrm{K}`$$``$1 (in the weak-coupling regime, $`\mathrm{\Delta }J^2/J_{\mathrm{av}}^3`$$``$1 ), crossover from the NFL to FL regime occurs around $`T_\mathrm{x}`$ which is given by $`T_\mathrm{x}`$=$`\alpha `$$`\times `$$`(\mathrm{\Delta }\stackrel{~}{J}/\stackrel{~}{J}_{\mathrm{av}})^2`$$`e^{1/\stackrel{~}{J}_{\mathrm{av}}}`$ with $`\alpha `$=$`2.95`$, where $`J_{\mathrm{av}}`$ and $`\mathrm{\Delta }J`$ are the average and difference of the exchange couplings $`J_1`$ and $`J_2`$, respectively (a swung dash means $`A_\mathrm{\Lambda }`$ times, $`A_\mathrm{\Lambda }`$ being a revision factor of the order of 1); (2) in the presence of a magnetic field, if $`(h/T_\mathrm{K})^2`$$``$1, crossover from the NFL to FL regime occurs around $`T_\mathrm{x}`$ which is given by $`T_\mathrm{x}`$=$`\beta \times h^2/T_\mathrm{K}`$, where $`\beta `$=$`4.45`$ in our normalization procedure on $`T_\mathrm{K}`$.

For the two-impurity Kondo model which has a NFL critical point at $`K`$=$`K_\mathrm{c}(J_1,J_2)`$ for a set of the Kondo exchange couplings $`J_1`$ and $`J_2`$, we have obtained NRG results on the entropy in the region around critical points of $`K`$=$`K_\mathrm{c}(J,J)`$ as follows: (1) when $`J_2`$ is displaced slightly away from $`J_2`$=$`J`$ with $`J_1`$=$`J`$ and $`K`$=$`K_\mathrm{c}(J,J)`$ fixed, crossover to a FL fixed point occurs around $`T_\mathrm{x}`$ which is given by that of the two-channel Kondo model with the same set of $`J_1`$ and $`J_2`$ in the absence of a magnetic field; (2) when interimpurity (RKKY) exchange coupling $`K`$ is displaced slightly away from the critical value of $`K_\mathrm{c}(J,J)`$ with $`J_1`$=$`J_2`$=$`J`$ fixed, crossover to a FL fixed point occurs around $`T_\mathrm{x}`$ which is given by $`T_\mathrm{x}`$=$`\gamma \times (K_\mathrm{c}K)^2/T_\mathrm{K}`$ with $`\gamma `$=$`0.50`$ where $`T_\mathrm{K}`$$``$$`lim_{\omega 0}`$$`lim_{T0}`$ $`\mathrm{Im}\chi _\mathrm{s}(\omega )`$.

In the present work, all the results on $`T_\mathrm{x}`$ can be adopted in a wide region of $`J`$ ($`J_{\mathrm{av}}`$) and all the temperature dependences of entropy in the crossover regime can be fitted quite well by a scaling function, eq. (2.30), derived from the TBA equations of the two-channel Kondo model with channel anisotropy and in the presence of a magnetic field. It is emphasized that the NFL behavior in the two channel Kondo model is fairly robust against channel anisotropy so that crossover from the NFL to FL regime can be seen even if $`\mathrm{\Delta }J`$$`>`$$`T_\mathrm{K}`$.

## Acknowledgments

We wish to thank C. M. Varma for valuable advice. We also would like to thank I. Affleck, D. L. Cox, H. Kohno, H. Kusunose and K. Miyake for helpful comments. H. M. is supported by Reserch Fellowship of Japan Society for the Promotion of Science for Young Scientists. This work is supported in part by the Grant-in-Aid for COE Research (10CE2004) of the Ministry of Education, Science, Sports and Culture.


text:
# Structural and magnetic properties of Fe/ZnSe(001) interfaces

## I Introduction

Spin electronics is one of the major topics of research nowadays where one combines the charge and spin degrees of freedom of carriers . This has got immense applications in modern technology e.g. magnetic recording industry and semiconductor appliances. The recent exciting suggestions are to fabricate spin transistors and spin polarized tunneling junctions made up of ferromagnetic metals and semiconductors. Large tunneling magnetoresistance (TMR) has been observed experimentally for heterostructures built of dilute magnetic semiconductors (DMS). There are also theoretical predictions of large TMR for heterostructures based on Fe and semiconductors . In this context, the interface between a metal and a semiconductor plays a crucial role in determining the magnetic and hence the transport properties of the hybrid systems as the injection of a spin-polarized electron from a magnetic material to the semiconductor depends crucially on the interface properties. The typical semiconductors used for these purposes are GaAs and ZnSe which belong to III-V and II-VI compounds respectively. In such devices Fe is one of the most commonly used 3d metal as it has got a high Curie temperature.

Informations about the structural and magnetic properties of the interface between Fe and ZnSe are available from experiments . Jonker et al. studied Fe growth on ZnSe(001) at 450 K. The growth was smooth and epitaxial. However, they observed a reduction in magnetic moment of Fe compared to the bulk value. Recently, Reiger et al.  studied Fe growth on ZnSe(001) at room temperature and found a three dimensional nucleation at the beginning of the growth process followed by a coalescence of the 3D islands around 7 monolayers(ML). There was no reduction of the Fe magnetic moment even for a low Fe coverage.

Theoretical investigations by ab-initio electronic structure calculations have been done for Fe/ZnSe interfaces and multilayers , , , . Continenza et al.  studied various Fe/ZnSe superlattices by all-electron full potential linearized augmented plane wave method within the local spin density approximation. They concluded that the enhanced Fe magnetism is suppressed as the Fe thickness is increased and the interface effects rapidly die out in the inner Fe layers. de Jonge et al.  have performed first principles electronic structure calculations of superlattices of Fe and several semiconductors (Ge, GaAs and ZnSe) by a localized spherical wave method. Butler et al.  studied the tunneling structures of ferromagnets and semiconductors by a layer Korringa-Kohn-Rostoker (LKKR) method. Moreover, they have investigated  extensively the transport properties of magnetotunnel junctions of Fe and ZnSe using Landauer approach for the calculation of conductance.

All the above theoretical calculations were done for ideal interfaces i.e. the metal and semiconductor atoms followed a regular stacking. In this paper, we study the relaxed Fe/ZnSe interface, i.e we allow for ionic, shape, and volume relaxations. We do not consider any temperature driven reconstruction except segregation, because it is known, that the semiconductor constitutents segregate  towards the surface when they are in contact with a metal. (We compared the total energies of different atomic configurations to investigate the surface segregation of Zn and Se.) We study (section III) the dependence of the interface electronic properties on the Fe film thickness and the semiconductor termination. Since, for a magnetotunnel structure, two interfaces are formed between Fe and ZnSe, we also studied (section IV) the reverse growth i.e. Zn or Se on a bcc Fe(001) substrate. Moreover, we investigate (section V) the importance of the semiconductor surface reconstruction for the interface formation.

## II Computational details

Calculations have been performed by a self-consistent first-principles plane wave pseudopotential code (VASP) . Vanderbilt type ultrasoft pseudopotentials  were used for the calculations which are reported to work well for transition metals . More accurate PAW (projector augmented wave)  pseudopotentials were also used in some cases for testing of accuracy. Calculations reveal that the ultrasoft pseudopotentials are good enough to reproduce results with reasonable accuracies. An energy cut-off of 250 eV was used for the kinetic energy of plane waves in the basis set. We have checked thoroughly that this cut-off energy is sufficient as it produces negligible Pulay stress. Perdew-Wang GGA(generalized gradient approximation) exchange -correlation  was used instead of LSDA (local spin density approximation). LSDA description of the Fe ground state structure is inappropriate and the structural informations of Fe layers obtained from geometry optimizations might be incorrect. We used a (1x1) unreconstructed surface cell with at least 10 Å vacuum and six monolayers of ZnSe (three Zn and three Se layers). The number of Fe atoms varied from 1 (0.5 ML) to 20 (10 MLs) in the unit cell. The bulk layer at the bottom was terminated with two pseudo hydrogen atoms to avoid charge sloshing . Two layers of ZnSe (one Zn and one Se) together with the pseudo hydrogen atoms were kept unrelaxed at the ideal bulk positions. It is to be noted that the lattice constant of bcc Fe is almost half of that of ZnSe. This helps Fe to grow in a bcc phase on a ZnSe(001) substrate without appreciable strain. Our calculations with GGA yield equilibrium lattice constants of bcc Fe and zinc-blende ZnSe systems to be 2.86 Å and 5.75 Å respectively. The experimental lattice constant of ZnSe is 5.66 Å and the overestimation of the calculated one is obvious for using GGA. Thus in experiment the Fe lattice constant is 1.4 % smaller than the ZnSe lattice constant, whereas in our calculation the Fe lattice constant is 0.5 % larger. The calculated direct band gap at the $`\mathrm{\Gamma }`$ point for the equilibrium lattice parameter is small (1.14 eV) compared to the experimental band gap (2.8 eV). As a first step, we didn’t attempt to correct that but this correction might be important from the point of view of metal-semiconductor junction properties. Total energies were always converged upto 10-4 eV for electronic relaxations and 10-3 eV for ionic relaxations. The atomic positions were relaxed alongwith the volume and shape of the unit cells. The full optimization with relaxations of internal and external degrees of freedom is important as far as magnetism is concerned. Forces were converged with a tolerance of 10-2 eV/Å . The Monkhorst-Pack scheme  was used for the generation of special k-points in the Brillouin zone. Convergence was checked carefully with respect to the number of k-points used. For example, a 6 $`\times `$ 6 $`\times `$ 2 mesh for k points was used for the largest unit cell containing 20 Fe atoms which yielded 36 k points in the irreducible Brillouin zone (IBZ) for the accurate calculation of DOS by tetrahedron method. For smaller cells, we used 108 k points in IBZ. For the relaxation of the atoms, smaller set of k-points were used (5 k-points in IBZ for a 20 atom cell) alongwith the Gaussian smearing of k-points. It should be mentioned here that there is no unambiguous way of determining the local properties e.g. local density of states, local magnetic moments etc. for a plane-wave method as the radius within which these properties are sought is not well defined. The plane wave components of the eigenstates were projected on linear combinations of spherical waves inside the atomic spheres around the atoms. The coefficients of the local spherical waves were used to construct the angular momentum projected local DOS. Details have been discussed by Eichler et al. . For the present calculations, the radii of Fe, Zn and Se atoms were chosen to be 1.41 Å 1.35 Å and 1.48 Å respectively. These values were taken from the calculations of bulk bcc Fe and bulk ZnSe systems.

## III Different Fe coverages

### A 0.5 ML coverage

We first present results for the calculations involving ideal stacking positions. Though this situation is not energetically favourable compared to the relaxed case, we investigate this as a starting point. Total energies are compared for the two cases (i) Fe is on the top of the ZnSe substrate in a regular stacking position (ii) Fe is in a substitutional Zn (Se) site in a subsurface layer in exchange with a Zn (Se) atom kept on the surface. We have found that Fe in a substitutional Zn site in the subsurface layer is more favourable than Fe being on the surface. The energy difference between the two configurations is 0.83 eV/cell. But, for Se substitution, Fe prefers to sit in the surface keeping the Se atom in the subsurface layer. Here, the energy difference is 0.40 eV/cell. However, these cases without relaxations are unfavourable compared to the relaxed case. It is well known that in the case of dilute magnetic semiconductors (DMS) of (Fe,Zn)Se , Fe prefers to sit in the cation site. For this case, the calculated Fe-Se distance (2.47 Å ) is slightly smaller than the Zn-Se bondlength (2.49 Å ), whereas the measured Fe-Se distance (2.48 Å ) is slightly larger than the measured Zn-Se bondlength (2.45 Å ). The magnetism is atomic like with an integer magnetic moment of 4.00 $`\mu _B`$/cell.

Now we discuss the results of the relaxation studies. The structure of the region very close to the interface of a metal and a semiconductor is an important factor for spin injection from a metal to a semiconductor. Since semiconductors have open structures, the metal atom will proceed inside the semiconducting substrate, where the charge overlap with the substrate atoms is increased. To investigate this possibility, an approximate energy landscape has been calculated by putting half a monolayer of Fe in different positions on and inside the host ZnSe lattice and comparing the total energies. The result is shown in Fig.1 for a Se-terminated surface. The energy difference is defined as $`\mathrm{\Delta }E=E_{tot}^BE_{tot}^S`$ where $`E_{tot}^S`$ is the total energy for an Fe atom sitting in the regular position on top of the surface and $`E_{tot}^B`$ is the total energy of the Fe atom sitting on different positions within the substrate. The most preferable position we found to be an interstitial one which is 2.875 Å below the surface. The corresponding total magnetic moments of the unit cells are plotted in the inset.

The final atomic configurations of the most preferable positions are shown in Fig. 2(a-c) and 3(a-c) for the Zn and Se terminated cases respectively. One can note the difference in the relaxations in the two cases: For a Zn-terminated case (shown in Fig. 2), with relaxations of atoms, the surface Zn atom moves upwards leaving a vacancy which is eventually occupied by the burried Fe. The topmost Zn atom occupies an ideal stacking position. This also conforms with the unrelaxed calculation mentioned above.

For a Se terminated case (shown in Fig. 3), starting from an identical situation as before, Se moves a little bit upwards. The burried Fe atom remains more or less in the interstitial position. So, the distinct difference in the two cases is the site occupancy of Fe. In both cases, relaxation leads to lower total energies compared to the cases of unrelaxed regular stacking as discussed before (0.03 eV/cell and 0.8 eV/cell lower for Zn and Se terminated cases respectively). It is seen that for Zn termination, the nearest Fe-Zn and Fe-Se distances are 2.49 Å and 2.37 Å respectively. For Se coverage, the distances are 2.96 Å and 2.52 Å respectively.

(So, magnetic moment is enhanced compared to that of bulk bcc Fe. However, it should be kept in mind that as we are using GGA, calculated value of magnetic moment (2.33 $`\mu _B`$) is greater than the experimental value of 2.2 $`\mu _B`$ for bulk bcc Fe.)

Atom and orbital projected DOSs are shown in Fig. 2(d-h) and Fig. 3(d-h) for Zn and Se terminated cases respectively. For both terminations, the majority Fe DOS has no states at the Fermi energy and we find an atomic like integer moment of 3.00 $`\mu _B`$ for the unit cell. This is not found for cases without relaxations described before. The magnetic moments for the unrelaxed cases are greater and of non-integer type. Half metallicity is seen only when relaxation is allowed. Half metallic systems (a system where one finds a metallic DOS for one spin channel and semiconducting DOS for the other showing 100 $`\%`$ spin polarization at the Fermi energy) are extremely important in the context of magnetoelectronics involving spin transport between ferromagnetic systems across a semiconducting/insulating barrier. However, with increased Fe coverage, this behavior dies out and we arrive at a normal metallic DOS. A similar calculation for Co for 0.5 ML coverage also yields an integer moment of 2.00 $`\mu _B`$/cell with both Zn and Se on top of burried Co.

Comparing this case with the total magnetic moment of 4.00 $`\mu _B`$ of a bulk DMS (Fe,Zn)Se, it is clear that the difference is due to the occupancy of the minority spin states of Fe as the majority states are completely occupied for the two cases. In DMSs, Hund’s rule for the atomic moment is followed resulting in the occupation of 5 and 1 electrons in the majority and minority spin channels of Fe $`d`$-states respectively. In the present case, again Hund’s rule for the atomic moment is followed, but Fe has gained one electron, such that now two electrons are in the minority spin channel. The reason is the following: At the ideal surface, i.e without Fe, the two Zn (Se) dangling bonds (DB) are each partially occupied with 0.5 (1.5) electrons. A semiconductor gains energy by having either occupied or unoccupied DB. Usually, anion DB (Se) are fully occupied and cation (Zn) DB are empty. Therefore, taking one electron from the Zn (Se) DB will lead to either occupied or unoccupied DB: for the Zn termination two empty DB and for the Se termination one empty and one occupied DB. This electron from the DB is transferred to Fe and gives rise to the two electrons in the d-minority channel.

Now, let us look at the projected DOS in detail. In both sets of figures (fig. 2(d-h) and fig. 3(d-h)), Fe s and d states, Zn s, p and d states and Se s and p states are shown (see figure captions for details). The energy scale is chosen to avoid showing the huge peak for Zn 3d state which is deep in energy and doesn’t hybridize with the Fe d states. For both terminations, the Fe DOS looks quite different from that of bcc bulk Fe. The majority spin states are filled up for Fe. For Zn termination, in Figs. 2(e) and 2(g), projected DOSs for surface(Zn1) and sub-surface Zn(Zn2) atoms are shown. The relative distribution of s and p states are different with the subsurface Zn (Fig.2(g)) having more bulk like character. Fe d states are narrower compared to the same for Se-terminated case (see Fig. 3(d)) due to less number of nearest neighbours in a substitutional position compared to an interstitial position for Se terminated case. This yields a slightly larger local magnetic moment of Fe for the Se terminated case (Table I). For Se termination, the effect of the Fe atom sitting in an interstitial position is pronounced even in the states of the atoms of deep subsurface layers e.g. Se2 and Zn2. The sharp peaks in the conduction bands have mostly Zn 4s and Se 4s and 4p characters. The induced spin polarizations of Zn and Se atoms at the surface are evident from the relative shift of majority and minority states (Table I).

### B 1.5 ML coverage

This case corresponds to 3 Fe atoms in the unit cell. As a complete Fe monolayer should contain 2 Fe atoms and already 1 Fe atom is burried in a subsurface layer, it is interesting to find the configuration with the segregated Se atom. For a Se terminated cases, we explored three different situations to find the lowest energy configuration (see Fig. 4). In Fig. 4(a), Se is sitting at a subsurface layer covered by a complete Fe layer at the surface. In Fig. 4(b), the surface is covered by 0.5 ML of Fe and Se is still in a subsurface layer. Finally, in Fig. 4(c), Se is at the surface followed by a complete Fe monolayer. The resulting sequence of energetics is Ec $`<`$ Eb $`<`$ Ea. The energy difference between configuration (c) and (b) is quite large (2.6 eV/cell). So, in summary, Se segregates towards the surface. In all cases, the magnetism is almost similar. In the most favourable case (c), the two Fe atoms (indexed 1 and 2 in the figure) below the surface have magnetic moments of 2.84 $`\mu _B`$ and 2.66 $`\mu _B`$ respectively. The burried Fe atom (indexed as 3) has a magnetic moment of 2.92 $`\mu _B`$. The surface Se atom (indexed as 4) attains an induced magnetic moment of 0.07 $`\mu _B`$. Fe(1)-Se(4) distance is 2.48 Å which is different than the cases where Fe and Se lie almost in the same layer. Though we have performed calculations for different thicknesses of Fe layers, we present only the details of the important ones. The next section describes a case with a relatively thick Fe layer.

### C 20 atoms (10 MLs) of Fe

To see the effect of the interface on the bulk Fe atom like layers, we performed calculations with 20 atoms of Fe on ZnSe substrate. We explored both the cases of Se-segregated and non segregated cases. The configuration with Se at the surface has the lower energy (energy difference between the surface segregated and non-segregated profiles is 1.5 eV/cell). For a Se-segregated case, the surface Fe-Se distance is 2.81 Å . Magnetic moment of the surface Fe atom is 2.96 $`\mu _B`$. The burried Fe atom in the interface has a moment of 2.88 $`\mu _B`$ with a Fe-Zn distance of 2.87 Å . Informations about the structural and magnetic properties are listed in table II for a few selected cases.

In Fig. 5, we have shown the layer projected local magnetic moments for the case of 20 Fe atoms deposited on ZnSe. The surface and the interface Fe atoms have large magnetic moments compared to the bulk value. But the atoms attain the magnetic moments of bulk bcc Fe very near to the interface. The induced moments on Se and Zn atoms close to Fe are parallel and antiparallel with respect to Fe moments. The corresponding projected DOSs are shown in Fig. 6. Figs. 6(a) and 6(b) show the surface Fe and Se atoms respectively. Fig. 6(c) shows the PDOS for an Fe atom in an intermediate Fe monolayer and (d) shows the same approaching the interface. Figs. 6(e) and (f) are PDOSs of burried interface Fe atom and Zn atom respectively. For the surface atom, the majority DOS is full whereas the minority DOS is partly occupied. Both the bonding and the antibonding d states of majority spin are filled whereas the bonding states for minority spin are occupied leaving the antibonding state fully empty. Fig. 6(c) corresponds to the bulk bcc Fe DOS where the majority states are occupied (both bonding and the antibonding states are filled) and the Fermi level lies at the pseudogap of the minority DOS separating bonding and antibonding d states. The majority DOS is more affected than the minority one while going from surface to the interface. Approaching the interface, the exchange splitting between the majority and minority DOSs increase and for the interface atom which is marked as FeI, the minority DOS is pushed towards the low energy side. DOS looks similar to that obtained by other authors . DOS at Fermi level is considerably different for different Fe atoms. The spin polarization SP is defined as SP=$`n(E_F)_{}n(E_F)_{}`$/$`n(E_F)_{}+n(E_F)_{}`$ where $`n(E_F)_\sigma `$ is the DOS at Fermi level for spin $`\sigma =,`$. SP is different for different Fe atoms. It is increased for the surface and the interface Fe atoms (negative) whereas it has got a lower value (positive) for the bulk like Fe atom.

In Fig. 7, we show the total and averaged magnetic moments of Fe atoms per unit cell as a function of Fe thickness. The values of the total magnetic moment increases linearly with Fe thickness. This is also seen in experiments . The value of the slope is close to the bulk Fe moment but still larger because of the presence of Fe surface atoms. For Fe/GaAs(001) interface, it is seen from experiments  that the extrapolated curve in a magnetic moment vs. thickness plot touches the thickness axis above the zero value. This means that for low thickness, magnetism of the interface is reduced compared to the bulk value. The same for Fe/ZnSe(001) interface doesn’t show any reduction of magnetic moment at the interface. The reason is that the p-d wavefunction overlap between Fe and As is stronger than between Fe and Se. For example, the Fe magnetic moment in an As environment is considerably reduced, whereas it is atomic like in a Se environemt. The inset shows the averaged magnetic moment per Fe atom in the cell as a function of Fe thickness. Averaged moment is defined as the ratio of the total magnetic moment and the number of Fe atoms in the unit cell. It is seen that this value decreases with thicker Fe layer and approaches the bulk magnetic moment of Fe. This is understandable because as we deposit more and more Fe atoms, the effect of surface and interface washes out and the bulk character is achieved.

The DOSs at the Fermi levels for both Se and Zn terminated cases are depicted in Fig. 8. It is to be noted that for these cases, surface segregation of Se and Zn atoms have also been considered. For that reason, a Zn atom is close to Fe for a Se-terminated case and a Se atom is close to Fe for a Zn-terminated case. A segregated profile for a Zn-terminated case has been chosen intentionally to have a comparative study with the Se-terminated case though Zn segregation has not been confirmed by the experiments. The sequence of the atoms from left to right is from the interface towards the bulk semiconductor. For 1 Fe atom, the spin polarization(SP) is -1.0(i.e. 100 $`\%`$ spin polarization). For 4 and 20 Fe atoms, the spin polarization is reduced. For the thickest layer i.e. 20 atoms of Fe, we find that the spin polarization reduces faster to zero as one approaches the bulk layers. For Se terminated cases (figs. 8(a-c)), spin polarization is always negative but for Zn terminated cases, the same for 4 and 20 atoms Fe (figs. 8(e-f)) shows positive values.

## IV Reverse growth

To prepare a magnetotunnel junction, one has to care for two interfaces. One where the semiconductor atoms are deposited on the metal electrode and the other where the metal electrode atoms are deposited on semiconductor substrate. It has been observed by transmission electron microscopy  that the interface structures are not the same for the two cases. The upper interface (Fe/ZnSe) is rougher than the lower one (ZnSe/Fe). To investigate this, we have done very simple calculations where we put either Zn or Se atoms on a bcc Fe(001) substrate. We compared the total energies of two configurations (i) Zn or Se atom is on top of Fe substrate (ii) Zn or Se atom is in a subsurface layer covered by one Fe layer at top. We have found that the semiconductor constituents prefer to sit on top of a Fe substrate indicating a sharp interface. For Se, the energy difference is 2.15 eV/cell whereas for Zn, it is 0.9 eV/cell. It suggests that Se/Fe interface is less probable to be a mixed one compared to the Zn/Fe interface. However, the magnetic moments are not changed appreciably for different configurations. We have already reported in the previous sections that for Fe/ZnSe interface, half a monolayer of Fe prefers to stay in a burried position in the ZnSe host. We can conclude that this interface is less sharp than the one with the reverse growth.

## V Fe on a reconstructed surface

In this section, we present the results of depositing Fe atoms on a Se-rich (2x1) reconstructed surface. It is already known from experiments  and theoretical calculations  that the Zn-rich and Se-rich surfaces undergo c(2x2) and (2x1) surface reconstructions respectively. For a Se-rich (2x1) reconstructed surface, a Se dimer of bond-length 2.40 Å is formed on the surface . We have put 2 Fe atoms on top of a Se-rich (2x1) reconstructed surface having a Se dimer (Se1 and Se2) and started relaxing the atoms. In the final relaxed configuration, 1 Fe atom sits in the same layer as one of the Se atoms(Se1) of the dimer breaking the Se dimer bond. The distance between Se1 and Se2 atoms becomes 5.24 Å . As the Se dimer is broken, the effect of the reconstructed semiconductor substrate is diminished. The other Se atom(Se2) goes beneath the layer. Another Fe atom goes to the surface. This is in accordance with all the cases where 1 Fe atom wants to be burried under the Zn or Se layer. The bond length between two Fe atoms and Se1 is 2.50 Å each. The magnetic moment is increased compared to the unreconstructed case by 0.5 $`\mu _B`$/cell. This increase is due to the lack of nearest neighbours of the topmost Fe atom. As the signature of the reconstructed semiconductor substrate is lost, we therefore conclude that the surface reconstruction has no dramatic effect in determining the properties of the Fe-ZnSe interfaces.

## VI Conclusion

In this paper, we have extensively studied structural and magnetic properties of Fe/ZnSe(001) interfaces. Geometry optimizations have provided useful structural informations of the interface. Our results show that half a monolayer of Fe prefers to sit below the surface. For the Se terminated case, Fe prefers to sit in the interstitial site whereas for Zn terminated case, Fe prefers a Zn substitutional site. We have observed surface segregation of Zn and Se atoms. However, the magnetic properties are not changed appreciably for segregated and non-segregated profiles. Magnetic moment of the interface Fe atom is increased compared to the bulk bcc Fe moment for both Zn and Se terminations. Fe attains its bulk moment very close to the interface. A reverse growth i.e. Zn or Se on top of the bcc Fe surface has also been studied. For a Se-rich (2x1) reconstructed surface, Fe breaks the Se dimer bond and sits in between to have a proper bonding configuration. Effect of the reconstructed semiconductor substrate is diminished.

###### Acknowledgements.

S.M. is grateful to the Swedish Natural Science Research Council and Göran Gustafsson Foundation for financial support.

TABLE I. Magnetic moments (in $`\mu _B`$) for 0.5 ML of Fe.

|  | Fe moment | surface Zn moment | surface Se moment | total moment/cell |
| --- | --- | --- | --- | --- |
| Zn-terminated | 2.93 | -0.023 |  | 3.00 |
| Se-terminated | 2.84 |  | 0.08 | 3.00 |

TABLE II. Structural and magnetic informations for selected thicknesses of Fe layers. All these results are for Se-terminated and segregated cases. The subscripts $`S`$ and $`I`$ denote surface and interface atoms. FeI is in the burried position close to the interface Zn atom. The values in the parentheses () and () are for FeS-ZnS and FeI-SeI distances for a Zn-terminated case with the corresponding local moment shown in ().

| Thickness of Fe | FeS-SeS | FeI-ZnI | FeI |
| --- | --- | --- | --- |
| layers | distance ( Å ) | distance ( Å ) | moment ($`\mu _B`$) |
| 0.5 ML | 2.52 (2.49) | 2.96 (2.37) | 2.84 (2.93) |
| 1.5 ML | 2.48 | 2.78 | 2.89 |
| 2.0 ML | 2.74 | 2.77 | 2.74 |
| 10.0 ML | 2.81 | 2.87 | 2.88 |


text:
# Symmetrical Temperature-Chaos Effect with Positive and Negative Temperature Shifts in a Spin Glass

## Abstract

The aging in a Heisenberg-like spin glass Ag(11 at% Mn) is investigated by measurements of the zero field cooled magnetic relaxation at a constant temperature after small temperature shifts $`|\mathrm{\Delta }T/T_g|<0.012`$. A crossover from fully accumulative to non-accumulative aging is observed, and by converting time scales to length scales using the logarithmic growth law of the droplet model, we find a quantitative evidence that positive and negative temperature shifts cause an equivalent restart of aging (rejuvenation) in terms of dynamical length scales. This result supports the existence of a unique overlap length between a pair of equilibrium states in the spin glass system.

Spin glasses can be considered as prototype systems for other, more complex, randomly frustrated and glassy systems JP . Experimental protocols proposed for spin-glasses sg-experiment-review ; sg-experiment-review-saclay ; jonas , have later been employed to study other slowly relaxing systems, e.g. orientational glasses doussineau , polymers bellon  and even interacting nanoparticle systems nanop , which all exhibit qualitatively the same effects of rejuvenation and memory as spin-glasses. The modeling of such non-equilibrium phenomena is thus of great importance for a broad range of physical systems. Various scenarios, based on quite different physical ideas, have been proposed to account for the empirical behavior, they include hierarchical models sg-experiment-review-saclay ; JP ; BDHV02 ; BB02  as well as the real space droplet model droplet ; YLB00 . The simultaneous occurrence of rejuvenation and memory in spin glass dynamics has been interpreted to favor the hierarchical scenario JP , which does not include the temperature chaos concept of the droplet model. On the other hand, it was recently found that a standard picture of the droplet model does allow a novel dynamical memory due to the existence of ’ghost domains’ YLB00 .

In this Letter we use zero-field-cooled (ZFC) relaxation measurements with $`T`$(temperature)-shifts to investigate rejuvenation in the canonical Heisenberg spin-glass Ag(11 at% Mn). By a new strategy, a dense set of data illustrating the crossover from fully accumulative to non-accumulative aging have been obtained. These results are then analyzed quantitatively within the droplet model droplet  using the concept of temperature-chaos and the recently derived parameters of the growth law for the spin glass domains of Ag(11 at% Mn) isothermal . Chaos with temperature is considered as a consequence of the subtle competition between fluctuations of the energy and entropy in randomly frustrated systems droplet ; SY . According to the droplet theory, typical spin configurations of a pair of equilibrium states at two different temperatures, say $`T_1`$ and $`T_2`$, are roughly the same at short length scales much below the so-called overlap length $`L_{\mathrm{\Delta }\mathrm{T}}`$ but completely different at large length scales much beyond $`L_{\mathrm{\Delta }\mathrm{T}}`$. The crossover between the two limits can be very slow. A remarkable feature is that the overlap length is finite for an arbitrary small but non-zero temperature difference $`\mathrm{\Delta }T=T_1T_2`$. Consequently, a continuous sequence of re-entrant like phase transitions should take place with decreasing temperature throughout the glassy phase.

The ZFC relaxation experiments were performed in a non-commercial squid magnetometer magetal97 , using the following protocol: the system is quenched from a temperature above the spin-glass transition temperature $`T_\mathrm{g}`$ ($`33`$ K) to an initial temperature $`T_i<T_\mathrm{g}`$, at which it is aged a time $`t_\mathrm{w}`$. The temperature is then shifted to a measurement temperature $`T_m=T_i+\mathrm{\Delta }T`$ with $`\mathrm{\Delta }T`$ being either positive or negative. Immediately after reaching temperature stability at $`T_m`$ a weak magnetic field is applied and the ZFC magnetization is recorded as a function of time. For convenience, let us refer to this $`T`$-shift experiment as $`(T_i,T_m)`$. The experiments were performed at temperatures between $`29.5`$ and $`30.5`$ K and the wait times at $`T_i`$ ranged from 100 to 100 000 s.

If temperature-chaos is absent, successive aging at the two different temperatures will add to each other in a fully accumulative way. In such a situation one expects to find an effective age $`t_{\mathrm{eff}}`$ such that the ZFC magnetization right after the $`T`$-shift is already relaxed as if it had spent a time $`t_{\mathrm{eff}}`$ by an isothermal aging at $`T_m`$. The effective age $`t_{\mathrm{eff}}`$ is a monotonically increasing function of $`t_\mathrm{w}`$ and also depends on the temperature protocol $`(T_i,T_m)`$. Conversely, $`t_\mathrm{w}`$ can be related to $`t_{\mathrm{eff}}`$ by an inverse function,

$$t_{\mathrm{eff}}=f(t_\mathrm{w},(T_i,T_m)),t_\mathrm{w}=f^1(t_{\mathrm{eff}},(T_i,T_m)),$$
(1)
It is useful to consider twin-experiments \- $`(T_1,T_2)`$ and its conjugate $`(T_2,T_1)`$ for a pair of temperatures $`T_1`$ and $`T_2`$ below $`T_g`$. In the absence of temperature-chaos, there must be a simple relation indicating the reversibility of the aging between the two temperatures, in such a way that for any time $`t`$,

$$f^1(t,(T_1,T_2))=f(t,(T_2,T_1)).$$
(2)
Let us call it criterion for accumulative aging. Any deviation from this simple relation means that non-accumulative effects exist. In the present article we demonstrate evidence for a violation of the criterion Eq. (2) (See Fig. 2) and show that the scaling ansatz for the temperature-chaos effect by the droplet theory can explain the effect quantitatively.

In an isothermal ZFC relaxation experiment in which the sample has been aged at the measurement temperature for a time $`t_\mathrm{w}`$, the relaxation rate $`S(t)=dM_{\mathrm{ZFC}}(t)/d\mathrm{log}(t)`$ shows a maximum at $`S(t_{\mathrm{max}})`$ with $`t_{\mathrm{max}}t_\mathrm{w}`$ lunetal83 , as illustrated in Fig. 1(a).

An effective age $`t_{\mathrm{eff}}`$ after a $`T`$-shift can accordingly be determined from the maximum of $`S(t)`$ measured after a $`T`$-shift sanetal88  (see Fig. 1(b)). Each ($`T_i,T_m`$) experiment is thus associated with the pair of times ($`t_\mathrm{w},t_{\mathrm{eff}}`$). However, due to the finite cooling rate in the experiments and the time needed to stabilize the temperature, a shortest measurable effective wait time of order 20 s is imposed on the system. In the analyzes below, all results from relaxation curves yielding $`t_{\mathrm{eff}}`$ 30 sec have therefore been discarded. As is seen in Fig. 1(b) there is, for $`\mathrm{\Delta }T>0`$, a significant broadening of the maxima in S(t) compared to the reference S(t) curves. This apparent broadening in time scale can, within the droplet scaling model, be translated to a dependence of the width of the domain boundaries on the sign of the temperature shifts. This subject will be further discussed in a forthcoming publication unp .

Fig. 2 shows a set of data from twin-experiments - $`(T_1,T_2)`$ and $`(T_2,T_1)`$. The results of $`(T_1,T_2)`$ experiments are shown with $`t_\mathrm{w}`$ on the horizontal axis and $`t_{\mathrm{eff}}`$ on the vertical axis. The results of $`(T_2,T_1)`$ experiments are shown in the reversed way - with $`t_{\mathrm{eff}}`$ on the horizontal axis and $`t_\mathrm{w}`$ on the vertical axis. The criterion for accumulative aging Eq. (2) will be satisfied if and only if the two data sets merge with each other in our plot. It can be seen that for small temperature differences the data sets merge almost completely which implies a fully accumulative effect. However for $`\mathrm{\Delta }T0.2`$K, it is seen that the criterion is severely violated and we conclude that a non-accumulative effect is detected.

In order to proceed to a quantitative analysis of the non-accumulative effect in terms of the droplet theory, one needs a good characterization of the growth law $`L_T(t)`$ for the spin-glass domains at a given temperature $`T`$ at time $`t`$ after the temperature quench. To this end, we employ the logarithmic domain growth law droplet ; isothermal

$$L_T(t)L_0\left[\frac{k_\mathrm{B}T}{\mathrm{\Delta }(T)}\mathrm{ln}\left(\frac{t}{\tau _0(T)}\right)\right]^{1/\psi }.$$
(3)
The effects of critical fluctuations are taken into account in a renormalized way by the characteristic energy scale $`\mathrm{\Delta }(T)`$ for the free-energy barrier and the characteristic time scale $`\tau _0(T)`$ for the thermally activated processes. They scale as $`\mathrm{\Delta }(T)/J=ϵ^{\psi \nu }`$ and $`\tau _0(T)/\tau _\mathrm{m}(\xi (T)/L_0)^z|ϵ|^{z\nu }`$ with $`ϵ=T/T_g1`$. The microscopic time scale is $`\tau _\mathrm{m}\mathrm{}/J10^{13}`$ s in spin systems, $`JT_g`$ sets the energy unit, and $`z`$ and $`\nu `$ are the dynamical critical exponent and the exponent for the divergence of the correlation length $`\xi (T)`$, respectively. In the following we use $`\tau _m=10^{13}`$ s, $`T_g=32.8`$ K, $`z\nu =7.2`$, $`\psi =1.2`$ (from isothermal ), $`J=T_g`$ and $`\nu =1.1`$. The value of $`\nu `$ is known to be around $`1.3\pm 0.2`$ LO86 . The length scale that we can explore in the experiments is much larger than in numerical simulations kometal2000 ; PRR01 ; BB02  but limited in the range between $`L_T130L_0`$ and $`L_T180L_0`$ at our working temperatures. The advantage of working in terms of dynamical length scale is that it allows an understanding of both temperature and time dependencies in a unified way.

Just after a temperature quench (with infinite cooling rate), the spin configuration would be completely out-of-equilibrium. However, in the experimental situation the cooling rate is finite (here 3K/min), and the initial spin configuration when attaining temperature stability at $`T_i`$ has a domain size $`L_{T_i}L_0`$ governed by the cooling rate. After the aging at the initial temperature $`T_i`$, the projection of the temporal spin configuration onto the typical spin configuration of the equilibrium state at $`T_i`$ will have a domain size of order $`L_{T_i}(t_\mathrm{w})`$. The spin configuration attained just at the end of the aging at $`T_i`$ is essentially the initial spin configuration after the small $`T`$-shift to the measurement temperature $`T_m`$. The projection of this configuration onto the typical equilibrium spin configuration at $`T_m`$ will have a certain spatial coherence, $`L_{\mathrm{eff}}`$. This length is determined as

$$L_{\mathrm{eff}}=L_{T_m}(t_{\mathrm{eff}}),$$
(4)
using the growth law Eq. (3) quoted above. In the absence of the temperature-chaos effect, one simply expects that aging should be fully accumulative i.e. $`L_{\mathrm{eff}}=L_{T_i}(t_\mathrm{w})`$, which satisfies the criterion for accumulative aging Eq. (2). In the presence of temperature-chaos, this is the case only at length scales $`L_{T_1}(t_\mathrm{w})L_{\mathrm{\Delta }\mathrm{T}}`$, where $`L_{\mathrm{\Delta }\mathrm{T}}`$ is the overlap length. $`L_{\mathrm{eff}}`$ saturates to $`L_{\mathrm{\Delta }\mathrm{T}}`$ on length scales $`L_{T_i}(t_\mathrm{w})L_{\mathrm{\Delta }\mathrm{T}}`$. A simple possibility is then that the two limits are connected by a crossover scaling form,

$$\frac{L_{\mathrm{eff}}}{L_{\mathrm{\Delta }\mathrm{T}}}=F\left(\frac{L_{T_i}(t_\mathrm{w})}{L_{\mathrm{\Delta }\mathrm{T}}}\right),$$
(5)
with a scaling function $`F(x)=x`$ for $`x1`$ (accumulative aging) and $`F(x)=1`$ for $`x1`$ (chaos). Note that the intermediate regime between the two extremes can be a very slow crossover.

In the limit of small temperature differences $`|\mathrm{\Delta }T/J|1`$, the overlap length between the two temperatures $`T_1`$ and $`T_2=T_1+\mathrm{\Delta }T`$ is supposed to scale as droplet

$$L_{\mathrm{\Delta }\mathrm{T}}L_0|\mathrm{\Delta }T/J|^{1/\zeta },\zeta =d_\mathrm{s}/2\theta ,$$
(6)
where $`\zeta `$ is the chaos exponent. $`d_s`$ is the fractal dimension and $`\theta `$ the stiffness exponent, which characterizes the surface volume and free-energy gap of the droplets, respectively.

In Fig. 3, we present the results of the twin-experiments - $`(T_1,T_2)`$ ,$`(T_2,T_1)`$ \- converting $`t_{\mathrm{eff}}`$ and $`t_\mathrm{w}`$ into the domain sizes $`L_{\mathrm{eff}}`$ and $`L_{T_i}(t_\mathrm{w})`$ using the growth law Eq. (3) and Eq. (4). It is seen that the data fulfilling the criterion for accumulative aging in Fig. 2 lie on the straight line corresponding to $`L_{\mathrm{eff}}=L_{T_i}(t_\mathrm{w})`$ and equally importantly that the data of the $`(T_1,T_2)`$ and $`(T_2,T_1)`$ experiments merge with each other. The latter clearly demonstrates that the effective domain size for a given pair of temperatures is the same which is consistent with the expectation that there is a unique overlap length between a given pair of temperatures.

Furthermore, the data with $`\mathrm{\Delta }T>0.1`$K shown in Fig. 3 lie below the straight line corresponding to $`L_{\mathrm{eff}}=L_{T_i}(t_\mathrm{w})`$, which indicates a finite overlap length, associated with the non-accumulative effects already observed in Fig. 2. Fig. 4 shows a scaling plot to fully test Eq. (5) using the data shown in Fig. 3 and an additional set of data for a variety of $`\mathrm{\Delta }T`$s. A good collapse of the data is obtained for $`1/\zeta =2.6\pm 0.5`$. It was found in Ref. isothermal  that $`\theta 1.0`$ in the present sample. Then the scaling relation Eq. (6) implies $`d_s=2.8`$ which is consistent with the boundaries droplet  $`d1<d_s<d`$ with $`d=3`$.

In the above discussion we have concentrated on one particular feature in the relaxation rate curves, the position of the maximum, $`t_{\mathrm{eff}}`$. The observation time where this occurs is then understood to reflect an effective domain size $`L_{\mathrm{eff}}`$ in the spin glass. Looking at the full relaxation rate curves there are of course other features that give additional information such as about the progressive change of the population of thermally active droplets in the interior of the domains which should enhance the response. Such additional features could also obscure the determination of $`t_{\mathrm{eff}}`$. An alternative method is then to derive $`t_{\mathrm{eff}}`$ from the out-of phase component of the ac-susceptibility as in previous studies of the effect $`T`$-shifts kometal2000 ; saclay ; BB02 . We have performed some preliminary measurements on the Ag(Mn) sample unp  using the method of kometal2000 ; saclay ; BB02 ; takhuk  following identical thermal protocols as in the current study and found that the obtained values of $`t_{\mathrm{eff}}`$ are consistent in-between the two methods.

In this article we have limited ourselves to investigate the small $`\mathrm{\Delta }T`$ case in order to elucidate universal features of the temperature-chaos effect. Although the departure from the fully accumulative limit is modest in terms of length scales as shown in Fig. 4, the impact is already striking in terms of time scales as seen in Fig. 2.

In experiments most systems appear less “chaotic” than the canonical Ag(Mn) and Cu(Mn) spin glasses saclay ; roland ; bellon ; doussineau ; nanop . An open question is if this is due to the absence of chaos or only a smaller $`1/\zeta `$, e.g. for Ising spin glasses $`\theta 0.2`$ imposes $`1/\zeta 1`$ compared to $`1/\zeta 2.6`$ for the Ag(Mn) spin glass. Hence, the droplet theory implies that Ising spin glasses should appear ’less’ chaotic than Heisenberg spin glasses due the smaller chaos exponent (i.e. larger $`L_{\mathrm{\Delta }\mathrm{T}}`$).

In summary, we have shown that results from $`T`$-shift experiments on the dynamic susceptibility of an archetypical spin glass when parametrized into a dynamical length scale (Fig. 3) yield an anticipated equivalence between positive and negative $`T`$-shifts and support the concepts of overlap length and temperature-chaos. The possibility to scale all data onto one master curve (Fig. 4) further confirms the applicability of the employed spin glass domain model droplet . We hope that the results of the present paper will stimulate further quantitative analyzes of rejuvenation-memory effects in spin-glasses and other slowly relaxing systems in terms of real space as well as hierarchical models to reach a consistent modeling of aging dynamics.

###### Acknowledgements.

We would like to thank Hajime Takayama, Koji Hukushima and Roland Mathieu for stimulating discussions. This work was financially supported by the Swedish Research Council (VR).