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# Dynamical Critical Phenomena in three-dimensional Heisenberg Spin Glasses

## I Introduction

Chirality in frustrated magnets, which provides fascinating magnetic orderings and/or novel critical phenomena, has attracted interest in recent yearsChirality . In the spin-glass (SG) study, the chirality-driven mechanism has been proposed by KawamuraKawamura92  in order to explain the origin of experimentally observed SG phase transitions. The chirality scenario assumes that a chiral-glass (CG) long-range order exists at low temperatures with preserving the proper rotational symmetry in a fully isotropic SG model. By random magnetic anisotropy even of a small magnitude, which always exists in real experimental situations, a SG phase is expected to emerge as a result that the anisotropy mixes the two degrees of freedom, spin and chirality. Therefore, in the chirality-driven mechanism the SG phase transition experimentally observed in a class of compounds such as CuMn is essentially governed by the CG fixed point.

Some numerical results on equilibrium properties support that the chirality-driven phase transitions occur in a three dimensional ($`3D`$) Edwards-Anderson (EA) Heisenberg SG modelKawamura98 ; HukushimaKawamura00 ; KawamuraImagawa01  as well as in a $`3D`$ XY SG modelLi . The CG transition temperature and the critical exponents are estimated. They seem to be compatible with those observed experimentallyCampbell . However, some researchers have argued the possibility of a finite-temperature SG transitionMatsubara01 , or even simultaneous SG and CG transition in the $`3D`$ Heisenberg SG modelNakamura-Endoh01 . In a $`3D`$ XY SG model, large scale domain-wall renormalization group calculation at zero temperature suggests that a SG long-range order occurs at non-zero temperature below the CG transition temperatureMaucourt . A similar study obtained by different boundary conditions also support the existence of SG order at finite temperaturesKosteritz-Akino .

The observed critical behavior associated with the CG transition is found to be remarkably different from that observed in ordinary second-order phase transitions. For instance, the crossing of the Binder parameter of systems with different sizes at the transition temperature, which is usually observed in standard second-order transitions, never occurs in this modelHukushimaKawamura00 ; KawamuraImagawa01 . Furthermore, the previous study revealed that the CG phase of the $`3D`$ isotropic Heisenberg EA model had a peculiar feature which was consistent with one-step replica symmetry breaking (RSB) phaseHukushimaKawamura00 . Some mean-field SG models with the one-step RSB exhibit dynamical singularity at a temperature well above the static transition temperatureReview . Recent simulation on a mean-field SG modelBrangian  shows that dynamical finite-size scaling holds for the dynamical transition temperature which is different from the static one . It is of particular interest to clarify whether the CG phase of the $`3D`$ Heisenberg EA model belongs to this class or not.

Until now, there have been a few works on dynamical properties of the Heisenberg SG models. Olive et alOlive86  and Yoshino and one of the authors (HT)Yoshino93  investigated spin autocorrelation functions in equilibrium by Monte Carlo simulations. They found that, with the help of dynamical scaling analysis, the temperature dependence of the characteristic relaxation time is compatible with a zero-temperature SG transition. However, the corresponding CG relaxation time has not been investigated yet.

In the present paper, we study dynamical properties associated both with spin and chiral degrees of freedom above the transition temperature of the $`3D`$ Heisenberg EA model with and without anisotropic interactions. We developed an efficient method for extracting the equilibrium relaxation time from non-equilibrium simulation for a given finite-size system and analyzed the time scale by using the finite-size scaling. The results of our analyses on the isotropic Heisenberg SG model support the first assumption of the chirality mechanism, namely the existence of a finite temperature CG phase transition without a conventional SG long-range order. In particular, a crossover from high-temperature SG dominant regime to the CG dominant regime is clearly observed with decreasing temperature. In addition, by introducing a finite random anisotropic interaction, the SG relaxation time is found to be significantly enhanced at low temperatures and in systems with large sizes, while there is no such drastic change in the CG dynamics. This is consistent with the chirality mechanism.

Our work is distinct from the previous works in the following senses; (i) The CG dynamics as well as the SG ones have been studied systematically both above and around a transition temperature, (ii) The equilibrium relaxation is estimated from non-equilibrium MC simulations. These results may be complementary with the previous equilibrium studiesKawamura92 ; HukushimaKawamura00 .

The present paper is organized as follows. In section II, we explain the model and the method of our Monte Carlo simulation. We introduce a dynamical ratio function and discuss its characteristic features in section III . Finite-size scaling of the characteristic time is studied in section IV and section V is devoted to summary of the paper.

## II Model and simulations

The model studied is a classical Heisenberg model on a simple cubic lattice, defined by the Hamiltonian,

$$H(\stackrel{}{S})=\underset{ij}{}J_{ij}\stackrel{}{S}_i\stackrel{}{S}_j\underset{ij,\mu ,\nu }{}D_{ij}^{\mu \nu }S_i^\mu S_j^\nu ,$$
(1)
where $`\stackrel{}{S}_i=(S_i^x,S_i^y,S_i^z)`$ is a three-component unit vector, and the sum runs over all nearest-neighbor pairs with the total number of sites $`N=L\times L\times L`$. The nearest neighbor couplings $`J_{ij}`$ are random bimodal variables which take $`\pm J`$ with equal probability. The anisotropic interactions $`D_{ij}^{\mu \nu }`$ are also independent random variables obeying a box distribution with its range $`[D:D]`$. We assume that the anisotropic term is symmetric, $`D_{ij}^{\mu \nu }=D_{ij}^{\nu \mu }`$. A quite similar model has been studied by MC simulationMatsubara91  with some values of strength $`D`$, where the SG phase at low temperatures has been found around and above $`D/J0.05`$. We study the model system both with the isotropic case ($`D/J=0`$) and an anisotropic case ($`D/J=0.05`$).

We employ a standard heat-bath Monte Carlo method with two sub-lattice flipsOlive86 . One Monte Carlo step (MCS) is defined as $`N`$ spin trials. We perform MC procedure as follows; firstly spins are set as a random configuration, namely they are instantaneously quenched from the high temperature limit. The spin configuration is updated at a working temperature $`T`$ during a waiting time $`t_w`$, which is from $`10^0`$ to $`10^5`$. Subsequently, additional MC steps are performed for measurements. The lattice sizes $`L`$ studied are $`4`$, $`8`$, $`16`$ and $`32`$. In our simulations, we perform eight independent runs for each identical sample to take an average over initial conditions and different thermal noises. A typical number of samples averaged over is 40–960 depending on the system size.

In order to study non-equilibrium dynamics of the model, we calculate the spin autocorrelation function defined by

$$C_q(t_w,t)=\frac{1}{N}\underset{i}{}[\stackrel{}{S}_i(t_w)\stackrel{}{S}_i(t_w+t)],$$
(2)
where $`\mathrm{}`$ represents an average over initial conditions and $`[\mathrm{}]`$ over the bond disorder. In the long time limit ($`t\mathrm{}`$) after taking the equilibrium limit ($`t_w\mathrm{}`$) the autocorrelation, Eq. (2), converges to the SG order parameter originally proposed by Edwards and AndersonEA75 . We also calculate the corresponding chirality autocorrelation function, which allows us to detect a possible CG transition from the dynamical point of view. It is also defined as an overlap of the local chirality

$$C_\chi (t_w,t)=\frac{1}{3N}\underset{i}{}[\stackrel{}{\chi }_i(t_w)\stackrel{}{\chi }_i(t_w+t)],$$
(3)
where $`\chi _{i\mu }`$ is the local chirality at the $`i`$th site and in the $`\mu `$th direction defined by a scalar as

$$\chi _{i\mu }=\stackrel{}{S}_{i+\widehat{e}_\mu }(\stackrel{}{S}_i\times \stackrel{}{S}_{i\widehat{e}_\mu }),$$
(4)
with $`\widehat{e}_\mu (\mu =x,y,z)`$ being a unit lattice vector along the $`\mu `$ axis. The CG autocorrelation function in off-equilibrium has not been investigated extensively yet, except for Ref. Kawamura98, .

In Fig. 1, we show the SG and CG autocorrelation functions with the different waiting times $`t_w`$ against time $`t`$. In non-equilibrium dynamics, temporal correlation functions explicitly depend on not only $`t`$ but also $`t_w`$, which we call the breaking of time translational invariance. The longer is the waiting time, the slower becomes the relaxation. The curves with shorter waiting times start to deviate from an equilibrium function at the shorter time scales. Such a time scale, below which the time translational invariance holds effectively, is roughly proportional to the waiting time $`t_w`$.

In Fig. 2 we present the correlation functions with different system sizes for a fixed waiting time $`t_w=10^5`$. One can clearly see that the relaxation curves start to deviate from that of the thermodynamic limit. This implies that finite-size effects yield another characteristic relaxation time. The latter is related to the critical slowing down which we study in the present work.

Generally speaking, equilibrium MC simulations for SG models suffer from extremely slow dynamics and equilibration is hardly realized in large systems at low temperatures. One of the advantages of the non-equilibrium simulation is to practically avoid such a very slow equilibration process. In the present work, we focus our attention to the longest relaxation time of finite-size systems which is expected to diverge with the system size at and below the transition temperature. Our strategy of the non-equilibrium simulation is to take the equilibrium limit, i.e., $`t_w\mathrm{}`$, after extracting the characteristic relaxation time under off-equilibrium in finite systems and then take the thermodynamic limit $`L\mathrm{}`$.

## III Dynamical ratio function and relaxation time

According to the dynamic scaling ansatzHohenberg , the autocorrelation function in equilibrium near a second-order phase transition has the form

$$C(t_w=\mathrm{},t_w+t)t^\lambda f\left(t/\tau \right),$$
(5)
where $`\tau `$ is the relaxation time at a given temperature and $`\lambda `$ a critical exponent. This form represents a crossover around $`\tau `$ from the short-time critical behavior, $`t^\lambda `$, to the long-time relaxation described by $`f(t/\tau )`$. When the temperature approaches to the critical point $`T_c`$, the relaxation time $`\tau `$ diverges as $`\tau (T)|TT_c|^{z\nu }`$. Thus, the autocorrelation function follows a power law in $`t`$ at $`T_c`$.

One may consider that the critical temperature as well as the critical exponents associated with the transition can be easily obtained by the relaxation time near the critical temperature. There are, however, several difficulties in obtaining the relaxation time by MC simulations. One difficulty is due to extremely slow dynamics of SG systems as mentioned above. Another difficulty is that the method of obtaining the relaxation time requires accurate estimation of a long-time tail of the autocorrelation function. One way is to integrate $`C(t)`$ over time. A contribution to the integrated relaxation time is dominated by the long-time tail where $`C(t)`$ simulated is very small and largely fluctuating. Another method would be a fitting of $`C(t)`$ to a relaxation function with the scaled argument $`t/\tau `$. It is, however, difficult to know the functional form explicitly, which is often non-exponential as seen in Fig. 1.

In order to avoid the above mentioned difficulties, Bhatt and YoungBhatt-Young92  (hereafter referred to as BY) have introduced a dimensionless dynamic correlation function

$$R_q(t_w,t_w+t)=\frac{C_q(t_w,t_w+t)}{\sqrt{\left[\left(\frac{1}{N}_i\stackrel{}{S}_i(t_w)\stackrel{}{S}_i(t_w+t)\right)^2\right]}}.$$
(6)
The prefactor in Eq. (5) involving a power of $`t`$ is canceled out by taking the ratio of moments. A similar dimension-less dynamical function has also been studied in simple ferromagnetsJaster ; Okabe . The corresponding CG ratio function is defined as

$$R_\chi (t_w,t_w+t)=\frac{C_\chi (t_w,t_w+t)}{\sqrt{\left[\left(\frac{1}{N}_i\stackrel{}{\chi }_i(t_w)\stackrel{}{\chi }_i(t_w+t)\right)^2\right]}}.$$
(7)
Because these ratio functions are dimensionless such as the Binder parameter in the static case, the dynamical scaling form is expected to be given by a function of $`t/\tau `$ as

$$R(t)\overline{R}(t/\tau ),$$
(8)
where $`\overline{R}(x)`$ is a universal scaling function. BYBhatt-Young92  fixed the waiting time $`t_w`$ in Eq. (6) to $`t`$ because it was believed that equilibration of the autocorrelation function on a given time scale $`t`$ needed the waiting time $`t_w`$ of the same time scale as $`t`$. They studied the dimensionless function of the short range Ising SG and the mean-field Sherrington-Kirkpatrick models just at the known critical temperature and successfully obtained the dynamical critical exponent $`z`$ using the finite-size scaling for the relaxation times $`\tau (L,T_c)L^z`$.

In the present study, we systematically investigate the ratio function both for the SG and CG autocorrelation functions as bivariate functions of $`t`$ and $`t_w`$. Instead of taking the equilibrium limit of the ratio function or fixing the time scale $`t_wt`$ studied previously, we try to take the equilibrium limit $`(t_w\mathrm{})`$ of the relaxation time $`\tau (t,t_w)`$ obtained from the ratio function for several waiting times.

Equations (6) and (7) are the ratio of an odd moment of the autocorrelation function to an even one. Consequently, the ratio functions for a given $`t_w`$ decay from 1 at $`t=0`$ to zero as $`t`$ goes to infinity and they are sensitive to flips or rotations of the entire system, which are the longest mode of relaxation. Therefore we expect that the ratio functions pick up only slowest relaxation modes from the whole modes of $`C(t)`$. A typical example of the ratio function, as well as $`C(t)`$, is presented for the SG and CG autocorrelations in Fig. 3. As expected, the ratio functions are unity in the relatively short-time regime, implying that the denominator and the numerator coincide with each other. For the longer-time regime, as shown in the figure, the ratio functions of spin and chirality sector coincide with the tail of the corresponding autocorrelation function multiplied by a certain constant, which represents a statistical weight of the slowest modes in $`C(t)`$.

When the ratio function $`R(t)`$ extracts only one relaxation mode corresponding to the longest mode in the system, it is expected to show a universal scaling form and to be scaled as

$$R(t_w,t_w+t;T,L)R(t/\tau (t_w;T,L)).$$
(9)
Here we assume that the ratio functions depend on $`t_w,T`$ and $`L`$ only through the relaxation time. This may be an extension of the dynamical scaling (8) to an off-equilibrium situation, which is to be checked. We try to scale the observed ratio functions into a universal scaling function by appropriately choosing the time constant $`\tau `$ depending on $`t_w,T`$ and $`L`$. Figure 5 presents a result of the scaled ratio functions for $`D/J=0`$. In the figure, one sees that both the SG and CG ratio functions with various temperatures, system sizes and waiting times are almost scaled as a common universal function. Note that this finding allows us to compare the absolute values of the SG and CG relaxation time. Using the scaling of the ratio functions in this way, we obtain the characteristic relaxation times $`\tau (t_w;T,L)`$ for each set of parameters $`t_w,T`$ and $`L`$. We then let $`t_w`$ to go to infinity to obtain the characteristic relaxation times in equilibrium. We assume that the $`t_w`$-dependence of the relaxation times is described as

$$\tau (t_w;T,L)=\tau (t_w=\mathrm{};T,L)\alpha t_w^\beta ,$$
(10)
with $`\alpha ,\beta `$ being some constants and $`\tau (T,L)\tau (t_w=\mathrm{};T,L)`$ the equilibrium relaxation time.

Temperature dependences of $`\tau (T,L)`$ thus extracted are shown in Fig. 6 for the spin (upper) and chiral (lower) degrees of freedom. We first note that the CG relaxation time is almost independent of the strength of the magnetic anisotropy $`D`$. This is natural since the anisotropy breaks the rotational symmetry, but not the reflection symmetry which is spontaneously broken by the CG phase transition. On the other hand, as seen in Fig. 6, the random anisotropy changes drastically the behavior of the SG relaxation time. The SG relaxation time of $`D/J=0.05`$ increases rapidly around $`T/J=0.25`$ with decreasing the temperature. Such a drastic change of the behavior implies that the anisotropy mixes the chirality with spin degrees of freedom as predicted in the chirality scenario. This is the first observation of the effect of the anisotropy for the SG relaxation times.

We can show another evidence that the chirality dominates the phase transition in the isotropic $`3D`$ Heisenberg SG model. In Fig. 7, the time evolution of SG (broken line) and CG (solid line) ratio functions at $`T/J=0.40,0.30`$ and $`0.20`$ with $`L=16`$ and $`t_w=10^5`$ are shown simultaneously. The characteristic relaxation time of the CG ratio function becomes larger with decreasing temperature much more rapidly than that of the SG ratio function does and it finally exceeds the SG relaxation time at $`T/J=0.20`$. This fact strongly suggests that the CG degrees of freedom dominate large-scale and long-time phenomena at low temperatures, while the SG one dominates at relatively high temperatures. This type of crossover is observed at the first time in the present work. We can also see such a crossover in the resulting equilibrium relaxation time. Figure 8 shows the same data as shown in Fig. 6 but only for the isotropic case $`D/J=0`$. A characteristic temperature at which the two relaxation times cross each other shifts towards the high-temperature side as the system size increases. We emphasize that this crossover is not due to an apparent finite-size effect.

## IV Finite-size scaling

In the present section we discuss the finite-size-scaling analysis of the equilibrium relaxation time obtained in the previous section. According to a standard dynamical finite-size-scaling analysis, the scaling form of $`\tau (T,L)`$ is given by

$$\tau (T,L)L^z\overline{\tau }\left((TT_c)L^{1/\nu }\right),$$
(11)
where $`z`$ is the dynamical critical exponent and $`\nu `$ the correlation-length exponent. The scaling function becomes a constant just at the critical temperature, leading the finite-size scaling form, $`\tau (T_c,L)L^z`$, previously studiedBhatt-Young92 . We discuss asymptotic behavior of the scaling function $`\overline{\tau }(x)`$. In a large-system-size limit above $`T_c`$, i.e., $`x1`$, the scaling of Eq. (11) should recover an ordinary scaling form,

$$\tau (T,L=\mathrm{})(TT_c)^{z\nu }.$$
(12)
This leads that the scaling function behaves as

$$\overline{\tau }(x)x^{z\nu }$$
(13)
at $`x1`$. Assuming that the transition takes place at a finite temperature, the opposite limit, i.e. $`x1`$, can be also argued in the isotropic case where the system would entirely behave like a rigid magnet. For the SG ordering in $`D/J=0`$, such a system rotates globally as coherent diffusive motion with the relaxation time $`\tau _D`$ proportional to the bulk volume. This implies that the asymptotic scaling form of the SG relaxation time in $`D/J=0`$ is

$$\overline{\tau }(x)|x|^{(dz)\nu },$$
(14)
in the limit $`x1`$ with $`d`$ being the dimensionality. The asymptotic scaling function for the CG relaxation time, however, would follow an exponential activated type because of the discrete nature of chirality.

The situation is complicated in a system with $`T_c=0`$. In one case where the conventional form (11) holds with $`T_c=0`$ as in the standard second-order phase transition, the scaling function in the asymptotic limit at $`x1`$, $`\overline{\tau }(x=0)`$, becomes a constant. On the other hand, Yoshino and TakayamaYoshino93  proposed a modified scaling form which was a combination of the standard form (11) with $`T_c=0`$ and the diffusion relaxation time, $`\tau _DL^d/T`$. This form is compatible with (11) and (14) in the limit $`x1`$ if $`(dz)\nu =1`$ holds. In this case, the scaling exponents, $`z`$ and $`\nu `$, are no longer independent parameters.

### IV.1 Isotropic case: $`D/J=0`$

The result of the finite-size scaling analysis mentioned above is demonstrated for the SG relaxation times of the isotropic Heisenberg SG model in Fig. 9. As can be seen from the figure, the data points are found to collapse into the universal scaling function. From the scaling we estimate $`T_{\mathrm{SG}}=0.0(1)`$, $`\nu =1.4(2)`$ and $`z=4.4(4)`$. Our result for the SG transition temperature is roughly consistent with the zero-temperature phase transitionBanavar ; McMillan85 ; Olive86 ; Yoshino93 ; Matsubara91 , although we could not completely exclude the possibility of the SG phase transition at a very low but finite temperature. Assuming the zero-temperature transition, the scaling results suggest that relaxation times diverge with a power law of $`T`$ as $`T`$ goes to 0, but not an exponential divergence which occurs at the lower critical dimensions such as the two-dimensional Ising SG model.

We expect that the scaling function converges to a finite value in the limit $`x0`$ as in the standard second-order phase transition, though we don’t have enough data to confirm this convergence. The scaling plot may be consistent with a modified scaling from $`x1`$ to $`x1`$ proposed by Yoshino and TakayamaYoshino93 , but then temperature dependence of the relaxation time at low temperatures, $`\tau T^{(dz)\nu }`$ with $`z`$ and $`\nu `$ obtained above does not coincide with that expected from a simple diffusive relaxation time proportional to $`1/T`$. A further investigation is needed to clarify this point.

The present estimate for $`\nu `$ is compatible with the previous ones in other works; $`\nu =1.54(19)`$McMillan85  and $`2.0(2)`$Kawamura92  by a domain-wall renormalization group calculation at $`T=0`$, $`\nu =1.35(5)`$ by a MC simulationMatsubara91 , $`\nu 1.6`$ by an equilibrium dynamicsYoshino93  and $`\nu 1.14`$ by a MC simulationOlive86 .

We have also analyzed the CG relaxation time by a similar scaling. The best scaling shown in Fig. 10 is obtained by the following estimates: $`T_{\mathrm{CG}}=0.22(2)`$, $`\nu =1.1(3)`$ and $`z=4.1(4)`$. The estimate for $`T_{\mathrm{CG}}`$ is consistent with the recent equilibrium MC calculationsImagawa01 ; Hukushima02 . The present estimate for $`\nu `$ is rather close to the previous MC estimate for the Gaussian distribution, $`\nu 1.2`$HukushimaKawamura00 .

At the critical temperature, the autocorrelation function $`C_\chi `$ and also $`C_\chi /R_\chi `$ follow the algebraic decay (5) with the exponent $`\lambda =\beta /z\nu `$. In Fig. 11 we show $`C_\chi /R_\chi `$ as a function of time at $`T/J=0.20`$ close to the CG transition temperature. The data still depend on both the system size and the waiting time. As a preliminary study, we estimate the exponent $`\lambda =0.23(5)`$ from the slope of the plot, where the numerical error comes from the uncertainty of the critical temperature. This value combined with $`z`$ and $`\nu `$ by the finite-size scaling leads to another exponent, $`\beta 1.0`$, which is consistent with the previous workKawamura98 .

As mentioned in the introduction, the dynamical phase transition which is separated from the static one can exhibit at a finite temperature in some one-step RSB systems. It depends on whether the order parameter continuously appears or discontinuously jumps up at the static transition as the temperature decreases. Examples of the discontinuous one-step RSB transition are the mean-field $`p`$spin glass with $`p>2`$ and the mean-field $`q`$-state Potts glass with $`q>4`$, while those of the continuous one-step RSB transition are the mean-field $`q`$-state Potts glass with $`2.8<q4`$. Our estimation of the CG transition temperature by the dynamical finite-size scaling is consistent with the static transition temperature. This fact means that the CG phase belongs to the latter class of the one-step RSB.

### IV.2 Anisotropic case : $`D/J=0.05`$

The finite-size scaling plots of the CG relaxation times in the anisotropic $`3D`$ Heisenberg SG model is shown in Fig. 12. In the analysis we regard the CG critical temperature as a unique adjustable parameter, and obtain $`T_{CG}=0.24(2)`$. As seen in Fig. 12, the scaling analysis works well for both $`D/J=0.0`$ and $`0.05`$ with the common $`z`$ and $`\nu `$. This implies that the critical exponents associated with the CG critical phenomena as well as the scaling function are independent of the anisotropic term. This finding of our analysis is consistent with the expectation that the anisotropic interactions are expected not to affect the CG symmetry.

We believe that the SG phase transition also occurs in the anisotropic case at the same temperature as the CG transition temperature. In fact, we have found in Fig. 6 that the anisotropic term significantly enhances the SG relaxation time at low temperatures. Unfortunately, however, such enhanced relaxation time appears only in larger sizes and at lower temperatures. Therefore, these data points are not enough to test the finite-size scaling.

## V Discussions

We have studied dynamical critical phenomena in the $`3D`$ Heisenberg SG models using Monte Carlo simulations. Our results support the chirality scenario for realistic SG transitions. It is confirmed that in the fully isotropic model at low temperatures, the CG relaxation time exceeds the SG relaxation time. This result strongly suggests that long-time or large scale behavior is dominated by the CG ordering. The finite-size-scaling analysis of the relaxation time supports that the CG phase transition with the diverging relaxation time occurs at a finite temperature, while the SG phase transition takes place at a lower temperature, consistent with even at zero temperature as previously studiedBanavar ; McMillan85 ; Olive86 ; Yoshino93 ; Matsubara91 . In other words, the spontaneous breaking of discrete $`Z_2`$ symmetry likely occurs with preserving the proper rotational symmetry $`SO(3)`$. The SG and CG transition temperatures of our result are significantly separated with each other within numerical accuracy. This is the first support for the basic assumption of the chirality scenario from a dynamical point of view.

We have also studied an anisotropic $`3D`$ Heisenberg SG model in the similar way. It is found that by introducing the weak random anisotropy, the SG relaxation times in the large system sizes increase at low temperatures, similar to that observed in the CG relaxation time, although a finite-temperature SG phase transition cannot be directly determined by the finite-size-scaling analysis. Our finite-size-scaling analysis of the CG relaxation time strongly suggests, on the other hand, that the CG phase transition with the anisotropic interactions belongs to the same universality class as the isotropic case. When the SG phase transition in the anisotropic case is intrinsically dominated by the SG order parameter but not the CG order parameter, the observed CG critical behavior should be affected by the SG transition and it should be different from the fully isotropic case. Therefore, from this point of view, our result is consistent with the chirality mechanism where the phase transition is dominated by the CG order parameter. In order to further clarify the nature of phase transition in the anisotropic case, however, directly measurements of the SG phase transition and its critical exponents are required.

A standard scenarioMorris  based on the zero-temperature SG transition in the isotropic point says that the SG transition continuously approaches to zero in the zero anisotropy limit as $`T_{\mathrm{SG}}(D)D^{1/4}`$ ; see Fig. 13(a). Because the anisotropy reduces the symmetry of Hamiltonian, the universality class changes from the isotropic SG to the anisotropic SG. The latter is expected to be in the class of the Ising SG. On the other hand, according to the chirality mechanismKawamura92 , the random magnetic anisotropy $`D`$ plays a role of mixing the CG long-range order with the SG one. The SG transition temperature in the ideal zero anisotropy limit is predicted to coincide with $`T_{\mathrm{CG}}(D=0)`$ but not $`T_{\mathrm{SG}}(D=0)`$, as shown in Fig. 13(b). This may be true wherever $`T_{\mathrm{CG}}>T_{\mathrm{SG}}`$ at the isotropic limit even with $`T_{\mathrm{SG}}(D=0)>0`$. Once the CG has a long-range order, even the small anisotropy $`D`$ coherently breaks the rotational symmetry of the system. Consequently, the SG critical behavior observed in the anisotropic model is governed by the fixed point of the CG transition of the isotropic model. The two scenarios can in principle be distinguished by the phase boundary near the isotropic limit and the universality class along the phase boundary. Our findings that the CG universality class is not affected by the anisotropy $`D`$ and that $`T_{\mathrm{SG}}<T_{\mathrm{CG}}`$ in the isotropic system prefer the chirality scenario.

In summary, spin-glass and chiral-glass orderings in three-dimensional Heisenberg spin glass model are studied from the point of view of dynamics by off-equilibrium Monte Carlo simulations. Our results support the chirality scenario for the SG phase transition in three dimensions.

## Acknowledgements

The authors would like to thank H. Kawamura for useful discussions. This work is supported by a Grant-in-Aid for Scientific Research Program (# 12640367) and that for the Encouragement of Young Scientists(# 13740233) from the Ministry of Education, Science, Sports, Culture and Technology of Japan. The numerical calculations were mainly made by use of the Hitachi SR8000/60 at the Supercomputer Center, Institute for Solid State Physics, the University of Tokyo.


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# Introduction.

## Introduction.

This study was initiated by necessity to get thin timing detector for the HARP experiment (CERN-PS214). A multigap RPC operated in avalanche mode at atmospheric pressure was suggested to use as a Time-Of-Flight (TOF) detector in . Then a set of papers with results obtained during the ALICE TOF R&D tests were published (see, for example,,,). However, thickness of prototypes (chamber itself plus front-end electronics) developed for the ALICE experiment is rather few ten cm what did not satisfy a HARP request on a TOF system: it thickness should be less than 14 mm. A new R&D work had to be done.

As the final result of our work, the TOF system covering $`10m^2`$ and having 368 readout channels has been realized in the HARP experiment. Its construction and basic characteristics were given in. But a lot of interesting results obtained during the $`R\&D`$ study are not published yet and here we try to present them.

To minimize a number of resistive electrodes and thus to get thin detector we fixed our attention on a 4-gap RPC with gap thickness of $`0.3mm`$. Operation of this type of RPC working as TOF detector was described in. However, detector developed in  looks like array of $`32\times 32mm^2`$ independent cells mounted in two layers following a chess-board-like pattern. In our study we tried to get the TOF detector consisting of one chamber added with set of pick-up electrodes.

A tracking system of the HARP detector provides with coordinates of point where a particle crosses the TOF RPC what allows to do not worry about time propagation along the signal electrode because it can be taken into account. Testing chambers with different pad size we tried to understand how the time resolution depends on a signal electrode area for to minimize number of channels in the future TOF system. Furthermore we checked an idea to summarize (with electronics) signals arriving from several signal pads. First result on timing RPC with strip read-out line is presented.

## 1 Experimental setup.

Data were obtained at CERN in a T10 test area with the 7 GeV/c pion beam. In tests we used gas line, DAQ system and other set-up of the ALICE TOF group. Four trigger scintillating counters in the front and behind of our chambers provided a selection of beam particles inside of a $`1\times 1cm^2`$ spot. Last fact helps us do not worry about a time jitter coming from the difference in the propagation time. Start scintillating counters provided with $`30ps`$ time accuracy giving time mark for precise measurements. As working gas the following tetrafluorethane based mixture was used: $`C_2H_2F_4/C_4H_{10}/SF_6`$(90/5/5).

### 1.1 RPC construction

Several small 4-gap chambers have been built with use of two different kinds of glass: two chambers having $`130\times 200mm^2`$ active area were constructed with 1 mm glass taken from the CERN workshop, one smaller chamber of $`70\times 130mm^2`$ size and one long detector, $`70\times 1000mm^2`$, were made of 0.6 mm thick glass which is used to build prototypes of the ALICE TOF detector. A resistivity of 0.6 mm glass was measured by us (with a test voltage of 1 kV) as $`9\times 10^{12}\mathrm{\Omega }cm`$. For 1 mm glass plates we found that resistivity is $`7\times 10^{12}\mathrm{\Omega }cm`$. A construction was similar for all chambers. The cross-section of four-gap RPC is shown in fig.1: a pair of identical double-gap RPCs made of three glass plates with 0.3 mm (in diameter) fishing line as a spacer between plates, and peak-up electrodes, (pads or strips) between two double-gap chambers. In the counter made of 0.6 mm glass three fishing lines were put in each gas gap with spacing of 35 mm between them. Four fishing line with 40 mm space between them were in chambers made of $`130\times 200cm^2`$ plates. Few small drops of ’5 minutes’ epoxy were enough to fix fishing lines between glass plates. High voltage was applied to each of double-gap RPCs through electrodes made of high resistive ($`1M\mathrm{\Omega }/\mathrm{}`$) carbon film. Each of five chambers were put in its aluminum box. Two $`200\mu m`$ mylar sheets one at the top and one at the bottom provide with an isolation between high voltage electrodes and walls of boxes. Each box can be easily opened and a system of pads can be changed in few ten minutes.

### 1.2 Front-End Electronics

A front-end electronics (FEE) used in most of present tests consisted of four-input pre-amplifier and splitter/discriminator (SD), both ”home-made”. A scheme of the pre-amplifier is presented in fig.3. The input circuits contain KT368A9 transistors. Signals from four inputs are summarized with an AD8009AR amplifier having 1 GHz bandwidth. A variation in time of propagation for different inputs is about 10 ps. An accuracy of the amplitude summarizing is $`57\%`$. A coefficient of transformation for the pre-amplifier was measured as -85mV/pC. Inputs of pre-amplifier were connected to pads with short ($`13cm`$) wires. The thickness of aluminum box together with pre-amplifier PCB attached to the RPC cap (as it is schematically shown in fig.1) was about $`12mm`$.

A output of the pre-amplifier was connected by the coaxial cable to the SD with adjustable ($`310mV`$) threshold of discrimination. The SD module has two outputs: one for the analog signal and one for the discriminated signal (NIM level). The output with analog signal was directly fed to a LeCroy 2249W ADC. The digital signal was sent to a LeCroy 2229 TDC with a $`50ps`$ bin width. An information from ADC was used to find correlation between the ”time” and the ”amplitude” and then to correct the data on a time-charge slewing.

A time resolution of the FEE in described above set-up has been tested with pulse generator: we injected charge through the test input of the pre-amplifier and measured the time jitter between the generator pulse and output signal from the discriminator as a function of the input charge. Black circles in fig.3 describes the time resolution of the pre-amplifier when no one of inputs was connected to pads. During this measurement pre-amplifier was attached to the aluminum box of the RPC, but no high voltage was applied to the chamber. A vertical dashed line in the figure corresponds to chosen by us threshold of $`65fC`$.

Our home-made 4-input pre-amplifier and SD were taken as a prototypes for the HARP TOF electronics. When first examples of the 8-input pre-amplifier produced for the HARP detector was available we used one of them to see how time resolution changes if to summarize signals from several pads.

## 2 Experimental results.

The time resolution of a detector working near the threshold of electronics can be estimated after correction for a time-amplitude correlation. A example of typical time-charge scatter plot what we saw during tests of our RPCs is given in fig.4a. A solid curve in this figure presents result of the fit with polynomial expression. Polynomial functions obtained in such approximation were used to correct the time distribution for time-charge correlation. An example of the corrected time distribution obtained from the data shown in fig.4 is presented in fig.4b. Approximation of the corrected time distribution with a Gaussian law, as it is shown in fig.4b by curve, gives value of the time resolution ($`\sigma _t`$).

### 2.1 Time resolution and efficiency in dependence on pad size.

A working voltage (HV) for the chosen variant of four-gap RPC is relatively low. A behavior of $`\sigma _t`$ as a function of HV is presented in fig.6 as it was observed for chambers with different pad sizes: $`3\times 3`$ (triangles), $`10\times 10`$ (boxes) and $`11\times 18cm^2`$ (circles). Solid curves in the figure are drawn for the eyes guide. One pad only was connected to the amplifier in last measurement. The figure shows that the best time resolution can be reached at HV=6.2 kV. This conclusion was well for all chambers we tested in spite of differences in thickness of glass used to build chambers. The value of 6.2 kV was chosen as a working voltage in further tests.

In fig.6 and in all other figures where data on time resolution are plotted, errors in $`\sigma _t`$ shows an accuracy with which we could reproduce our results next time. All points presented in fig.6 were obtained with chambers passed training under high voltage during several days.

A charge distribution measured for induced signals at HV=6.2 kV is shown in the fig.6. A mean value of induced charge is $`1pC`$. Taking into account the FEE resolution as a function of the charge (fig.3) and the real charge distribution from fig.6, one can estimate the resolution what can be reached in our tests: it is $`65ps`$. Last estimation is ultimate - it does not includes deterioration in the resolution due to noise from pads when HV is on.

Just first our attempts to measure $`\sigma _t`$ showed that the data are unstable with time: improvement of the resolution was observed if to keep the chamber under working voltage for several days. A example is given in fig.8 demonstrate importance of the training process: if fresh chamber showed $`\sigma _t170ps`$, after 100 hours the resolution drops down below $`120ps`$. A chamber was considered completely trained, if after several days of the training process it showed the stable result on $`\sigma _t`$.

The time resolution dependently on pad area, $`S`$, is given in fig.8 with triangles for the case when one pad only was connected to the pre-amplifier. An approximation of the data obtained for the single pad with expression $`\sigma _t=A+BS`$ (solid line in the figure) brings $`A=70ps`$ and $`B=0.26ps/cm^2`$. A first value is close to the resolution what we expected from our electronics for the charge spectrum shown in fig.6. The parameter $`B`$ depends on how noisy chamber is.

All tested RPCs showed high efficiency. Two types of efficiency were considered by us: total efficiency, $`\epsilon `$, - probability to get a reply from chamber inside $`15ns`$ gate and so-called ’$`3\sigma `$-efficiency, $`\epsilon _{3\sigma }`$, as a probability that a reply is inside $`\pm 3\sigma _t`$ interval. Values of $`\epsilon `$ (closed circles) and $`\epsilon _{3\sigma }`$ (open circles) measured for chambers with different pads are given in fig.10 as a function of the pad size. Both efficiencies were calculated, of course, after correction for the time-charge correlation. Looking at fig.10 one can see that both efficiencies go down with growth of the pad size. Equaling to 97% for $`25cm^2`$-pad, the $`3\sigma `$-efficiency drops down to $`94\%`$ when pad size is $`200cm^2`$.

Another problem was found for big pads. It was appeared that for a pad having size of about $`10\times 10cm^2`$ and larger a value of time resolution is not uniform, it depends on a point of discharge inside RPC. A example of such non-uniformity is shown in fig.11a for $`11\times 18cm^2`$ pad. Ten dashed squares in this figure show places where beam crossed RPC during the pad scan. Two values at each dashed square present the time resolution (first value) and $`3\sigma `$-efficiency (second value). A deterioration in the resolution can be seen in the region close to the point where signal wire is soldered to pad. An attempts to eliminate the effect by changing of the amplifier input impedance brought no positive result.

All data in figures where time resolution is presented dependently on pad size were obtained with beam going through the pad center.

It was described above that $`\sigma _t`$ values were extracted from the time distribution after its off-line correction for the time-amplitude slewing. However, it was interesting for us to check a possibility to get ’on-line’ timing with use of a constant fraction discriminator (CFD). As CFD we took ORTEC CF4000 module. Because of a high level of discrimination in the CF4000, a gain of our ’standard’ amplifier was not enough to work with the CF4000. In operation with the CFD we organized a chain of two amplifiers: MAX3760 (first stage) and AD8009AR (second stage, gain=5). Results obtained with two-stage amplifier are shown in fig.10. Open circles describes the resolution obtained when the output of the MAX3760 amplifier was sent to the our SD. The off-line correction for the time-charge correlation was done before plotting these points. Closed circles show a data obtained with the CFD instead of the usual discriminator. The figure demonstrates a possibility to get good time resolution even without off-line correction if CFD is used.

### 2.2 Summing from several pads

After clear deterioration of the resolution with growth of the pad size was observed, we tried to improve situation by splitting one big pad into several smaller ones for to read them by one multi-input amplifier. Firstly we looked does any non-uniformity in efficiency and $`\sigma _t`$ for a system of small pads connected to one amplifier exist if to expose different places of the RPC. To check this we used the RPC having four pads with size of $`4.3\times 5.6cm^2`$ each. Pads were connected to different inputs of the 4-input amplifier. Results of the four-pad system scan are presented in fig.11. Dashed areas in the figure shows places where beam crossed the system of four electrodes. Two values written at each dashed square are: first - time resolution, second - $`3\sigma `$-efficiency. The figure demonstrate that in limit of our errors no variation in the $`\sigma _t`$ or $`\epsilon _{3\sigma }`$ depending on exposure place was observed even in the case when a axis of beam was between four adjacent pads. A main conclusion from the figure is that the amplifier summarizes signals without problem for the resolution or efficiency.

One module of 8-input amplifier produced as a final version for the HARP TOF system was used by us to see how resolution depends on ’read-out area’ if to summarize signals from set of small pads. Scheme and main parameters of final amplifier were practically the same as it was described above for 4-input. Eight pads having size of $`4.3\times 5.6cm^2`$ each were connected (one-by-one) to eight inputs and the time resolution degradation was studied. Fig.8 displays $`\sigma _t`$ as a function of the signal electrodes area for the case of the single pad (triangles) and for the case when several pads (boxes) are connected to one pre-amplifier. As it is seen from fig.8, a degradation of the resolution with growth of the area goes slower for the multi-pad system than for the single pad read-out. Two lines in the figure presents results of approximation with a linear law done separately for two sets of the data. A data obtained with the 8-input amplifier can be described with $`\sigma _t=0.71+0.13\times S`$ (dashed line in fig.8).

### 2.3 Strip read-out

To conclude what the time resolution can be reached if a long strip is taken instead of the pad, a 1 m length RPC was tested with a $`90cm`$ strip line having width of 2.5 cm. Each end of strip was connected to its own pre-amplifier. A impedance of the strip line was measured as $`20\pm 5\mathrm{\Omega }`$. To avoid possible oscillations due to reflection of the signal at ends, the strip line should be terminated with $`20\mathrm{\Omega }`$ loading. A resistor was added in the input circuit of the pre-amplifier to change it impedance to the needed value of $`20\mathrm{\Omega }`$.

Different places of the 1 m length RPC were exposed to the beam, and a reply of the detector was studied dependently on a distance, $`X`$, between the beam line and the strip end. Fig.12a shows a mean arrival time as a function of the $`X`$. Two sets of points in the figure, open and closed triangles, belong to different ends of one strip line. A linear approximation of the data gives a slope of $`50ps/cm`$.

The time jitter for half of a sum of corrected times coming from opposite ends, $`t_{12}=(t_1+t_2)/2`$, was measured along the strip for different distances taken relatively to one of ends. The results on $`t_{12}`$ resolution are in fig.12b. As the figure demonstrates, values of the resolution found during ”scanning” along the strip are inside of 110-120 ps. In the limit of experimental errors they do not depend on the $`X`$. If to read one end of the strip only, the time resolution was found to be about $`160ps`$.

Fig.12c presents the $`3\sigma `$-efficiency estimated from a width of $`t_{12}`$-distribution. No dependence of $`\epsilon _{3\sigma }`$ on $`X`$ is seen in the last figure.

### 2.4 Glass RPC at different particle rate

The glass is a high resistive material. That is why the glass RPC even operated in the avalanche mode should be sensitive to a particle rate.

Within set-up what we had in the T10 test area we estimated the rate using counting rates from set of scintillating counters installed in front and behind of our chambers. However, we could not control particle rate with accuracy better than $`30\%`$, because few detectors tested by other groups were installed at the same time in the beam line.

The rate what we show in the figures below was calculated as a number of particle crossing $`10\times 10mm^2`$ square (with center at beam line) per spill divided by spill duration of $`300ms`$. It should be noticed that because of a beam halo not only $`1\times 1cm^2`$ RPC area was exposed to the beam. A number of particles going through a $`4.5\times 5cm^2`$ scintillating counter installed just before tested RPC was $`15`$ times higher than the number of particles going trough the central $`10\times 10mm^2`$ area.

Fig.13 shows: (a) time resolution and (b) $`\epsilon _{3\sigma }`$ efficiency at different values of the rate. The RPC having $`10\times 15`$ single pad was exposed to beam to get these distributions. Both distributions shown in fig.13 demonstrate a deterioration in the RPC work with growth of the particle rate.

## Conclusions

We designed, built and tested prototypes of the thin TOF detector. Four-gap glass RPCs added with different pick-up electrodes were exposed to $`7Gev/c`$ pion beam to find what the time resolution and registration efficiency can be reached.

The time resolution as a function of the pad size show linear dependence on pad area ($`S`$): $`\sigma _t`$=$`A+B\times S`$, where $`A=70ps`$ is the intrinsic resolution of our FEE, and $`B=0.26ps/cm^2`$. The value of $`3\sigma `$-efficiency is 97% for the small pad ($`25cm^2`$) and drops down to 94% with growth of the pad area to $`200cm^2`$.

The situation with the time resolution and efficiency for the ’big’ read-out area can be improved if to split one pad into set of smaller ones and to read them with summing amplifier. Using 8-input amplifier we found that $`\sigma _t=0.71+0.13\times S`$.

We tested the timing RPC with the strip read-out. The resolution of $`110120ps`$ was reached for the 90 cm length strip having 2.5 cm width when signals from both ends were recorded.

Our results can be useful if development of large area TOF detector with thickness of $`1015mm`$ is needed.

Acknowledgment We would like to thank members of the ALICE TOF group, especially M.C.S Williams for enormous help with materials and equipment.

Furthermore we are very grateful to F.Dydak and J.Wotschack for their suggestions and for their constant interest on our study.


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# Disorder-driven magnetic field-dependent phases in an organic conductor

## Abstract

We report inter-plane ($`R_{zz}`$) electrical transport measurements in the $`\tau `$-phase series of organic conductors at very high magnetic fields. In the field range between 36 and 60 T $`R_{zz}`$ shows a very hysteretic first order phase transition from metallic to an insulating state. This transition does not affect the Shubnikov-de-Haas oscillations associated with the two-dimensional (2D) Fermi surface. We argue that this transition originates from inter-plane disorder which gives rise to incoherent transport along the least conducting axis. We conclude that this system becomes a strictly 2D Fermi-liquid at high magnetic fields.

Disorder and complexity play important roles in many systems of current interest in condensed matter physics. In colossal magnetoresistance (CMR) systemscmr  such as the manganites, magnetic disorder and inhomogeneity lead to dramatic changes in resistivity with magnetic field and temperaturetokura . In organic conductors with complex, polymeric anions and cation end-groups, conformational disorder may lead to insulating behavior, associated to the localization of the electron states, and to weak ferromagnetism even in the absence of magnetic ions welp ; shus . As recent reviews have shownross ; elbio , important mechanisms and physical properties are shared by organic and inorganic materials, particularly in layered, anisotropic systems. Recently “bad metal” (i.e. $`k_F\mathrm{}`$$`1`$) characteristics have been reported in a transition metal oxide (TMO) that paradoxically, exhibits Shubnikov de Haas oscillations ($`\omega _c\tau 1`$) at low temperaturescao . This also appears to be the case of the $`\tau `$-phase organic conductor series presented in this Letter, where disorder, magnetism, and high anisotropy play important roles in determining the ground state properties of layered materials.

Our main experimental result is the universal behavior of the inter-plane resistance ($`R_{zz}`$) of three isostructural members of the $`\tau `$-phase class of organic conductorspap90 ; ter ; zam ; pap95 ; pap96  in very high ($`B>36T`$) magnetic fields. Here we find a first order metal-to-insulator transition in $`R_{zz}`$ above a temperature-dependent threshold field $`B_{th}`$. An overview of the field-temperature phase diagram of these materials is shown in Fig. 1. What is remarkable about this transition is that unlike the well-known field induced spin density wave transitions in quasi-one dimensional organic conductorsish , where an orbital Fermi surface nesting effect is involvedosada , $`B_{th}`$ appears to be only weakly dependent on magnetic field direction. Hence the mechanism that drives the transition at $`B_{th}`$ may be primarily isotropic, or Zeeman-like in origin, and we must look for other physical characteristics of these materials which cause this dramatic transition to the insulating state.

The complexity and structure of the $`\tau `$-phase unit cell is unique amongst the general class of charge transfer salts (CTS)will . Three forms of the $`\tau `$-phase materials have been studied in the present work. The formula unit for the material we have most extensively studiedsto  (hereafter $`\tau `$-AuBr2) is $`\tau `$-(P-(*S,S*)-DMEDT-TTF)2(AuBr2)(AuBr2)y (where $`y0.75`$). The iodine anion system $`\tau `$-(P-(*S,S*)-DMEDT-TTF)2(AuI2)(AuI2)y (hereafter $`\tau `$-(AuI2) is also investigated in this work, as is a disordered racemic system with AuBr2(see below). The DMEDT-TTF donor is shown in the inset of Fig. 1. Unlike conventional CTS materials where the charge transfer is 2:1, here it is 2:(1+y) and the anions occupy two different sites in the unit cell: for instance the AuBr2 anion sits at the center of a square array of DMEDT-TTF donors in the conducting layerzam , and the (AuBr2)y anions are arranged in the inter-layer planes where their orientation alternates by 90o between successive layers. Since DMEDT-TTF is asymmetric, the donor stacking involves alternating directions within the donor layer. Hence, due to the very low symmetry of the donor and anion arrangement, four donor layers are necessary to complete the unit cellpap95 , and the result is an unusually large inter-planar dimension: $`(a,b,c7.4,7.4,68\AA )`$. Further disorder, beyond the non-stoichiometry of the anion structure, can be introduced into the $`\tau `$-phase system with a racemic mixture of two different isomers(R,R and S,S) of the donor moleculespap01a ; pap01b . In general the ratio of the two isomers is not fifty-fifty, and this enhances the disorder over crystals containing the pure (R,R or S,S) arrangements. The racemic system studied in the present work is $`\tau `$-(P-(r)-DMEDT-TTF)2(AuBr2)(AuBr2)y (hereafter $`\tau `$(r)-AuBr2).

In this investigation, single crystals of $`\tau `$-phase materials (square plates of average size $`1\times 1\times 0.2mm^3`$) were grown by electrochemical methods. All measurements were four-terminal, inter-plane resistance measurements with current values between 50 nA and 300 $`\mu A`$. Electrical contact was made to the samples with 25 micron gold wires connected with carbon or silver paint. Experiments were carried out at the National High Magnetic Field Laboratory (NHMFL) DC field facilities in Tallahassee with standard low frequency AC techniques, and at NHMFL-Los Alamos with pulsed magnets. For pulsed field measurements, forward and reverse DC current traces were taken to remove the induced *emf* signals.

The temperature dependence of the inter-plane resistance for different magnetic fields for the three $`\tau `$-phase materials studied is shown in Fig. 2. The following convention for presentation order is used in the figures: $`\tau (r)AuBr_2`$, $`\tau AuBr_2`$, and $`\tau AuI_2`$ to represent the level of disorder and/or anion radii (where Br is smaller than I ) respectively. Although the data in Fig. 2 differs in emphasis of field, temperature, and material studied, there are universal features that arise in all cases, as reflected in the phase diagram of Fig. 1. The inter-plane resistance $`R_{zz}`$ increases monotonically with decreasing temperature, but there is a characteristic temperature labelled $`T_a18K`$ where the resistance appears to be magnetic field independent. (The magnetoresistance is positive above $`T_a`$, and negative below $`T_a`$.) At lower temperatures an anomaly (plateau or kink) appears in $`R_{zz}`$ for zero field at $`T_b12K`$. The detailed structure of the feature in $`R_{zz}`$ at $`T_b`$ quickly disappears with increasing magnetic field. If the change of slope in the temperature dependence is monitored, $`T_b`$ first increases slightly, then decreases with increasing field. At fields greater than 5 T, the point where dR/dT changes sign can be easily determined. In all samples, at all fields, dR/dT eventually becomes negative with decreasing temperature. Both $`T_a`$ and $`T_b`$ are shown in Fig. 1 as derived from these observations in the field range 0 to 27 T.

The high magnetic field dependence of $`R_{zz}`$ of the $`\tau `$-phase materials has been investigated in a DC hybrid magnet up to 45 T ( Fig. 3), and in pulsed fields(6 ms rise-time) up to 60 T (Fig. 4). In all cases a transition between a metallic state and a highly insulating state is observed in $`R_{zz}`$ at a threshold field $`B_{th}`$. In Fig. 5 details of the Shubnikov-de Haas (SdH) effect are shown for representative low temperature hybrid data. (In the present work SdH frequencies were observed over a range of 500 to 800 T, depending on field orientation. See also Ref.sto ) There are several key points that may be drawn from Figs. 2-5. First is that between about 18 T and $`B_{th}`$ SdH oscillations are observed at low temperatures even though $`R_{zz}`$ exhibits a negative dR/dT in this activated region (Fig.1). Hence the sample is a quasi-two dimensional metal in this range. Second, the transition at $`B_{th}`$ is highly hysteretic, and therefore first order. For fields above $`B_{th}`$, the inter-plane resistance $`R_{zz}`$ increases by orders of magnitude, and in some cases becomes un-measurable by conventional transport methods. $`B_{th}`$ is temperature dependent, and moves to higher fields with increasing temperature. We note that the upper boundary of the high field phase in Fig. 1 approaches a value near $`T_a`$. Third, as Fig. 3 indicates, $`B_{th}`$ is only weakly dependent on field orientation, and unlike the case for an orbital Fermi surface nesting effect, $`B_{th}`$ actually reaches a minimum for in-plane magnetic field.

Before discussing the mechanism for this new high field state, it is instructive to consider some other details associated with the $`\tau `$-phase materials. Even in the absence of magnetic field, these materials have the appearance of “bad metals”. A simple evaluation of the carrier scattering time, based on either in-plane or inter-plane conductivity, over a broad temperature range, leads to a mean free path comparable to the unit cell dimensions (see also Ref. for ). In marked contrast, for moderate magnetic fields where quantum oscillations (SdH) are observed, we find a Dingle temperaturesto  of only 1.3 K which translates to a mean free path of about $`60\mu m`$. This difference is not easily reconciled based on any simple homogenous model. That the disorder may arise from the inter-plane sites comes from investigations of $`R_{zz}`$ in tilted magnetic fieldsbro ; sto  in $`\tau `$-AuBr2 which show no evidence for the “Yamaji effect”ish . That is, no angular dependent magnetoresistance oscillations(AMRO) in $`R_{zz}`$ associated with a finite inter-plane bandwidth and mean free path are observed. Hence the inter-planar coherence required for semi-classical trajectories on a warped cylindrical Fermi surface is not satisfied. Evidence for non-metallic behavior, coupled with the appearance of quantum oscillations in quasi-two dimensional metals are not without precedent, as recently reported in both organicbal ; wos  and TMOcao  systems.

Evidence for weak ferromagnetism has been reported in the EDO class of $`\tau `$-phase materialsmur1 ; yosh1 ; yosh2 ; kon1 ; kon2  where oxygen replaces the two nitrogen sites (N1 and N2 in Fig. 1) in the DMEDT-TTF donor. Since there is no magnetic ion present, magnetism must arise either from the bands or from disorder (localized moments). Band magnetism has recently been treated by Arita et al.ari , based on consideration of the very flat, narrow ($`E_F8meV`$) bands that appear at the Fermi level from the tight binding calculations. Although magnetization studies have shown a small (0.001 $`\mu _B`$/formula unit) moment, no hysteresis has been observed in magnetization datakon1 . Recent far infrared measurements indicate that the methyl groups show disorder, and it has been suggested that this may lead to electronic localization and magnetism at low temperaturesole .

One final important detail is the relative constancy of the SdH oscillation frequency in the vicinity of $`B_{th}`$, which indicates that there is no catastrophic change in the quasi-two dimensional (Q2D) electronic structure. Rather, the SdH waveforms (which appear only below about 1.5 K due to the large effective masssto ) remain observable until the resistance becomes forbiddingly large, either for increasing, or decreasing field through $`B_{th}`$. These effects are particularly evident in Figs. 4b and 5.

Based on the evidence above, we argue that the phenomena in the $`\tau `$-phase materials is linked to the disorder in the donor and anion structure. The influence of high magnetic fields on this disorder drives the system into a state of highly de-coupled two dimensional Fermi liquid layers. This conclusion is supported by noting that $`B_{th}`$ is the lowest in the most disordered (racemic) system. That the disorder, and the resulting incoherent transport is limited to the inter-planer layers, is evident from the presence of the SdH effect, and the absence (or attenuation) of semiclassical orbits (AMRO) in tilted magnetic fields. Hence it is unlikely that the mechanism that stabilizes the high field phase is a result of Fermi surface nesting, especially in light of the weak dependence of $`B_{th}`$ on magnetic field direction. When the field is aligned in-plane, $`B_{th}`$ actually reaches a minimum, and this may be due to further compression of the Q2D electron wave function expected for a quasi-two-dimensional conductor in this configuration.

A remaining question is how the magnetic field couples to the inter-planar disorder, and we may speculate about two possibilities. The first is simply through localized spins, where in the low field phase, magnetic polarization may reduce carrier scattering. This would give a negative magnetoresistance and allow the SdH effect to eventually appear. In the high field phase, magnetic order may set in, thereby making the inter-layer transport incoherent due to first order, domain-like structures. A second possibility may be diamagnetic in origin, arising from non-stoichiometric sites in the inter-layer anion structure. The high magnetic fields needed to cross $`B_{th}`$, and the linear shape of the anions make (normally weak) diamagnetic processes, that may alter the inter-layer structure, more probable. Either mechanism should be roughly isotropic with respect to magnetic field direction.

In summary, the similarities between organic molecular solids and the metal oxides (cuprates, manganites, ruthenates, etc.) continues to be the subject of general interest in materials science. These relationships may be even closer, as evidenced from the results presented in this Letter. Here, superimposed on the “conventional” picture of a quasi-two dimensional Fermi surface, we find evidence for phase transitions driven by disorder and magnetism.

###### Acknowledgements.

The FSU acknowleges support from NSF-DMR 99-71474. We thank B. Ward, L. Gor’kov, E. Dagotto, and R. McKenzie for valuable comments and suggestions.


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# Observation of sub-natural linewidths for cold atoms in a magneto-optic trap

## Abstract

We have studied the absorption of a weak probe beam through cold rubidium atoms in a magneto-optic trap. The absorption spectrum shows two peaks with the smaller peak having linewidth as small as 28% of the natural linewidth. The modification happens because the laser beams used for trapping also drive the atoms coherently between the ground and excited states. This creates “dressed” states whose energies are shifted depending on the strength of the drive. Linewidth narrowing occurs due to quantum coherence between the dressed states. The separation of the states increases with laser intensity and detuning, as expected from this model.

The use of near-resonant laser light to cool atoms from room temperature to ultra-low temperatures has become a standard technique for atomic physics experiments . Temperatures in the range of few microkelvin are routinely achieved using these methods. The cooled atoms can also be trapped by superposing a magnetic field on the laser beams in a configuration called a magneto-optic trap (MOT) . Cold atoms in a MOT form near-ideal laboratories to test our understanding of the fundamental laws of physics. There are two primary reasons for this. The first is that almost all laser cooling experiments are done on alkali atoms, and alkali atoms are attractive candidates for such fundamental experiments because their simple one-electron structure renders them amenable to theoretical calculations. For example, the alkali atom cesium has been used for high-precision experiments on atomic parity violation  because the experimental results can be compared to theoretical predictions based on the Standard Model. The second advantage of cold atoms in a MOT is that, if one is looking for spectroscopic signatures of some effect, then the use of ultra-cold atoms guarantees high precision because Doppler broadening is negligible. For example, a probe beam sent through a cloud of rubidium atoms in a MOT shows a Doppler width of 500 kHz, while the natural linewidth of the cooling transition is 6.1 MHz. However, the natural linewidth appears as a fundamental limit to the resolution achievable in these experiments. In addition, it is often necessary to turn off the MOT before doing any precision measurement because the trapping beams cause unwanted perturbation to the energy levels of the atoms. In this article, we show that, not only can the energy shift from the trapping beams be well understood from a simple theoretical model, but this can also lead to significant narrowing of the linewidth of the transition below the natural linewidth.

The MOT was first invented in 1987  and since then it has become the workhorse for any experiment that requires a cold and dense cloud of atoms. It is the starting point for experiments ranging from atomic fountain clocks to achieving Bose-Einstein condensation . We have been interested in a MOT primarily from its potential use in precision spectroscopy experiments. The standard MOT configuration consists of three pairs of counter-propagating laser beams in the three orthogonal directions, and a quadrupole magnetic field generated using two coils carrying current in opposite directions. The laser beams are circularly polarized and detuned below the resonance by 2 to $`3\mathrm{\Gamma }`$, where $`\mathrm{\Gamma }`$ is the natural linewidth of the cooling transition.

We work with 87Rb atoms in the MOT, for which the cooling transition is the $`5S_{1/2},F=25P_{3/2},F^{}=3`$ transition at 780 nm. The transition has a natural linewidth of 6.1 MHz and saturation intensity  of 1.6 mW/cm2. The laser beams are derived from a frequency-stabilized diode laser system locked near this transition. To prevent the atoms from optically pumping out of the cooling transition, a small amount of “repumping” light resonant with the $`5S_{1/2},F=15P_{3/2},F^{}=2`$ transition is mixed with the primary MOT beams. The repumping beam is obtained from a second tunable diode laser system. The experiments are done in a vacuum chamber maintained at a pressure below $`10^9`$ torr. Rb atoms are loaded into the trap using a getter source  that fills the chamber with Rb vapor when heated with a few amps of current. The low-energy tail from this background vapor is cooled and captured in the MOT.

The loading of atoms into the MOT follows an exponential growth curve . The time constant is a few seconds, so that, after about a minute, the MOT is in steady state with a number of atoms that stays constant as long as the source remains on. Under typical conditions, the steady-state MOT has about $`10^8`$ atoms at a temperature of 300 $`\mu `$K and density of $`10^{10}`$ atoms/cc. We have studied the absorption of a weak probe beam passing through the cold atoms in a MOT after it has attained steady state. The probe is linearly polarized and has an intensity of about 250 $`\mu `$W/cm2. A typical absorption spectrum as the probe laser is scanned across the $`5S_{1/2},F=25P_{3/2},F^{}=3`$ transition is shown in Fig. 1. The main features of the spectrum are that there are two peaks instead of one, and that the linewidth of the smaller peak is only 1.7 MHz, or about 28% of the natural linewidth.

To understand this we have to consider that, in the presence of the probe and trapping beams, the Rb atoms form an effective three-level system as shown in Fig. 2. In other words, the circularly-polarized trapping beam couples certain magnetic sublevels in the ground and excited state, while the linearly-polarized probe beam measures absorption from the same ground-state sublevel to a different excited-state sublevel. For the trapping beam, we only consider the stretched state, i.e. the magnetic sublevel where the projection of angular momentum ($`m_F`$) is maximum. The main reason for this is that, as the atoms move away from the trap center, they rapidly get optically pumped into this state. Once they are in this state they remain there until they go to the other side of the trap where they get optically pumped into the opposite stretched state. For example, the $`\sigma ^+`$ beam optically pumps atoms into the $`5S_{1/2},F=2,m_F=2`$ sublevel from where they cycle on the $`F=2,m_F=2F^{}=3,m_F^{}=3`$ transition, while on the other side of the trap, the $`\sigma ^{}`$ beam optically pumps atoms into the $`5S_{1/2},F=2,m_F=2`$ sublevel.

The primary purpose of the trapping beam is to provide a radiation pressure force that pushes the atoms towards the trap center. This force arises because the atom absorbs a laser photon, goes to the excited state, and then decays to the ground state through spontaneous emission. However, there is a small probability that the atom decays through stimulated emission induced by the same beam. The resulting force is called the stimulated force and causes the atom to be coherently driven between the ground and excited states. The frequency at which the probability swaps between the two states is called the Rabi frequency, $`\mathrm{\Omega }_R`$, and is determined by the laser intensity and the strength of the transition . Since we are going to be interested only in this coherent driving of the atom, this gives another justification for considering only the stretched state in our analysis: transitions starting from this state are the strongest in terms of relative oscillator strength.

The energy levels shown in Fig. 2 can now be understood more clearly. The $`\sigma ^+`$ trapping beam couples the $`5S_{1/2},F=2,m_F=2`$ and $`5P_{3/2},F^{}=3,m_F^{}=3`$ levels, while the probe measures absorption on the $`5S_{1/2},F=2,m_F=25P_{3/2},F^{}=3,m_F^{}=2`$ transition. The trapping beam has a detuning from resonance of $`\mathrm{\Delta }_t`$ and the probe beam has a detuning of $`\mathrm{\Delta }`$. The spontaneous decay rates from the excited levels, $`\mathrm{\Gamma }_{21}`$ and $`\mathrm{\Gamma }_{31}`$, are both equal to $`\mathrm{\Gamma }`$, which is 6.1 MHz. As discussed above, the trapping beam partly drives the atoms coherently. It is well known that this driving creates “dressed” states whose energies are shifted by the strength of the drive (also called the ac Stark shift) . The energy shift is analogous to the shift in the frequency of two classical oscillators that are coupled together, where the shift is proportional to the strength of the coupling. In fact, this analogy with coupled classical oscillators can be made more exact, and results in analogous definitions of classical dressed states and Rabi frequency .

In the presence of the dressed states, the probe-absorption spectrum splits into two peaks, called an Autler-Townes doublet . The location of the two peaks is given by :

$$\mathrm{\Delta }_\pm =\frac{\mathrm{\Delta }_t}{2}\pm \frac{1}{2}\sqrt{\mathrm{\Delta }_t^2+\mathrm{\Omega }_R^2},$$
(1)
where $`\mathrm{\Delta }_+`$ and $`\mathrm{\Delta }_{}`$ are the values of the probe detuning where the peaks occur. The corresponding linewidths ($`\mathrm{\Gamma }_\pm `$) of these peaks are different because of the coherence between the two dressed states, and given by

$$\mathrm{\Gamma }_\pm =\frac{\mathrm{\Gamma }}{2}\left(1\frac{\mathrm{\Delta }_t}{\sqrt{\mathrm{\Delta }_t^2+\mathrm{\Omega }_R^2}}\right).$$
(2)
It is clear from the above expression that, if $`\mathrm{\Delta }_t=0`$, the two peaks are symmetric and have identical linewidths of $`\mathrm{\Gamma }/2`$. However, for any non-zero detuning, the peaks have asymmetric linewidths. The first peak has larger linewidth while the second peak has smaller linewidth by precisely the same factor, in such a way that the sum of the two linewidths is equal to the unperturbed linewidth, $`\mathrm{\Gamma }`$.

The above analysis is for a stationary atom. If the atom is moving, the laser detuning as seen by the atom depends on its velocity. To obtain the probe absorption in a gas of moving atoms, the above expressions have to be corrected for the velocity of the atom and then averaged over the Maxwell-Boltzmann distribution of velocities. Such an analysis has been done by Vemuri et al. in Ref. . The important conclusion of that work is that the location of the peaks given in Eq. 1 does not change, but the linewidths are now given by

$$\mathrm{\Gamma }_\pm =\frac{\mathrm{\Gamma }+D}{2}\left(1\frac{\mathrm{\Delta }_t}{\sqrt{\mathrm{\Delta }_t^2+\mathrm{\Omega }_R^2}}\right).$$
(3)
Here, $`D`$ is the Doppler width, which is 0.5 MHz for Rb atoms at a temperature of 300 $`\mu `$K. This is negligible compared to the natural linewidth of 6.1 MHz. Therefore, for our conditions, Eqs. 1 and 2 can be taken as valid even at the finite temperature in the trap.

The probe-absorption spectrum presented in Fig. 1 can now be understood based on the above analysis. The trapping beam coherently drives the atoms and creates two dressed states near the original ground state. The probe beam measures absorption from the modified ground state and therefore shows two peaks. For non-zero detuning of the trapping beam, the linewidth of the smaller peak is much smaller than $`\mathrm{\Gamma }`$, as given in Eq. 2.

In order to verify that this model is correct, we have studied the probe absorption at different values of trapping-beam intensity (or Rabi frequency) and detuning. From Eq. 1, the separation of the two peaks in the absorption spectrum is $`\sqrt{\mathrm{\Delta }_t^2+\mathrm{\Omega }_R^2}`$, and should increase when either $`\mathrm{\Omega }_R`$ or $`\mathrm{\Delta }_t`$ is increased. The variation with laser intensity at three different values of $`\mathrm{\Delta }_t`$ is shown in Fig. 3. The solid line is a fit to the variation expected from Eq. 1 and matches the data quite well. However, for each curve, the $`y`$-intercept should be the detuning $`\mathrm{\Delta }_t`$. Instead, we find that the intercept is smaller by about 4 MHz. There could be several reasons for this. One likely explanation is that, because the atoms are in a linearly-varying magnetic field, the detuning of the trapping laser depends on the exact location of the atom. Atoms that get optically pumped into the stretched state are most likely to be near the periphery of the cloud. Taking into account the 4 mm size of the cloud and the magnetic-field gradient of 10 G/cm, the field at this location is about 2 G. For the stretched state, this would cause a decrease in detuning by 2.8 MHz, which is about the size of the decrease we measure. In addition, atoms away from the center of the trap have a non-zero velocity. Because the lasers are detuned below resonance, optical pumping into the stretched state is most likely when the atoms are moving towards the laser beam. The Doppler shift in this situation is such that it would again cause a reduction in the detuning. For atoms moving with the r.m.s. velocity in the trap, the Doppler shift is about 0.4 MHz.

Whatever be the exact cause for this change in detuning seen by the atoms, we can verify its effect further by studying the separation of the peaks as a function of detuning. In Fig. 4, we show the separation vs. detuning for different values of trapping-beam intensity. The solid lines are exact calculations from Eq. 1 and the measured points lie almost perfectly on these curves. However, to get this match, we had to use the effective detuning from the $`y`$-intercepts of Fig. 3, and not the zero-field detuning set in the laboratory. The excellent agreement with the theoretical prediction gives us confidence that the atoms are indeed seeing a smaller detuning.

There are other features of the absorption spectra that are clearly noticeable in the data. For example, the smaller peak becomes more prominent (relative to the larger peak) as the trapping-beam intensity is increased at a given detuning. Similarly, for a fixed intensity, the peak becomes more prominent at smaller detunings. Both these observations are consistent with the model of a driven two-level system, since the effect of the drive is stronger when the intensity is higher or when it is closer to resonance. However, there are some complications with this simple model that are also evident in the data. One problem is that the linearly-polarized probe laser can also couple to the $`F^{}=3,m_F^{}=1`$ sublevel, in addition to the $`F^{}=3,m_F^{}=2`$ sublevel already considered. The location of the $`F^{}=3,m_F^{}=1`$ absorption peak is slightly shifted due to the non-zero magnetic field. This transition is very weak in terms of relative strength compared to the transition to the $`F^{}=3,m_F^{}=2`$ level, therefore it would show up only in the primary absorption peak. But this implies that the primary peak is a convolution of two peaks. We see some evidence for this in the data because we find that the lineshape of the primary peak is non-Lorentzian. This makes it difficult to extract a reliable estimate of the linewidth of the peak but does not affect the location of the peak center that has been used for Figs. 3 and 4.

In conclusion, we have observed sub-natural linewidth for probe absorption through cold rubidium atoms in a MOT. The modification to the absorption spectrum arises because of dressed states created by the trapping beams. Perhaps the most useful way to understand this is in the context of driven three-level systems  and the phenomenon of electromagnetically induced transparency (EIT) . In EIT, an initially absorbing medium is made transparent to the probe when a strong control laser is applied to an auxiliary transition. In our case, the trapping laser itself plays the role of the control laser that modifies the absorption of the probe. It thus opens up new possibilities for EIT experiments using cold atoms, where phenomena such as gain without inversion, anomalous dispersion, and population trapping can be studied.

###### Acknowledgements.

This work was supported by a research grant from the Department of Science and Technology, Government of India.