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# Optical shielding of cold collisions in blue-detuned near-resonant optical lattices

## I Introduction

In laser cooling and trapping of neutral atoms spatial variations in the polarization and intensity of light can be effectively turned into potentials for atoms . Optical lattices are an important application of this technique . By using suitable laser field configurations and parameters one can achieve localization of atoms into lattice sites, at least for some period of time on average. In practice there are two distinct cases of optical lattices. For near-resonant light the lasers are responsible for both cooling and trapping of atoms, usually achieved by a strong scattering of photons (energy dissipation). The basic example is the Sisyphus or polarization gradient cooling mechanism . In contrast, with far off-resonant light we obtain only a conservative lattice potential without the cooling mechanism, with a strong reduction in photon scattering. This allows many delicate experiments involving quantum coherences, such as Bose-Einstein condensation .

At suitably large atomic densities, about $`10^{12}`$ atoms/cm3, the atom-atom interactions are expected to become important in laser cooling and trapping . For far off-resonant lattices their role can be easily controlled, and one can even consider studying controlled collisions , or using the atom-atom interactions to study quantum computing and entanglement . Recently it has become possible to make densely occupied far off–resonant lattices . For near-resonant optical lattices the situation is more complicated, because the main atom-atom effects are light-assisted inelastic collisions, which interfere with the laser cooling process. Another aspect is that although strong photon scattering leads typically to efficient dissipation and cooling, in suitably dense atomic gases the reabsorption of scattered photons causes also unwanted heating of the atomic cloud. Experimentally the case of densely populated near-resonant lattices has not been studied very much so far, as high occupation densities are hard to produce due to the above-mentioned problems. These problems are present also in basic magneto-optical traps (MOT) so one does not get much gain in density by using a MOT as a preliminary stage.

For near-resonant laser light we have two situations depending whether the laser frequency is slightly above the atomic transition (blue-detuned light) or slightly below it (red-detuned light). In the more commonly applied red-detuned case one obtains the lattice structure rather easily, and can go below the Doppler limit for laser cooling due to the Sisyphus cooling mechanism. For densely populated lattices this means, however, the above-mentioned appearance of strongly inelastic collisional radiative processes that cause heating and loss of atoms .

In this paper we look at the case of near-resonant blue-detuned lattice, which is different from the red-detuned case. It is not straightforward to construct a blue-detuned lattice with an efficient cooling mechanism. There are, however, schemes for doing this, based on applying an external magnetic field , and we have adapted one of them as the basis of our studies. The important benefit of using a near-resonant blue-detuned lattice is that the photon scattering is reduced strongly compared to the red-detuned case. This diminishes the role of photon reabsorption as a heating mechanism, and thus increases the relevance of the light-assisted collisions in the complicated thermodynamics of the atomic cloud.

With blue-detuned light the nature of the light-assisted collisions is also changed, and instead of strong inelastic processes we have optical shielding of collisions . For weak fields this mechanism is incomplete and can lead to some heating of atoms, but barely to any strong loss. For stronger fields the inelastic contribution disappears, also in the sense that optical shielding forbids close ground-ground encounters which can lead to atom loss or heating, in addition to the light-assisted processes. Optical shielding has been studied both experimentally  and theoretically  with laser cooled atoms in magneto-optical traps, but not in optical lattices to our knowledge. None of the theoretical studies so far have treated the cooling process and the shielding process simultaneously.

Thus we expect that, a priori, it is better to use blue-detuned lattices for efficient cooling while aiming at an increase in the atomic density in lattices. Matters are, however, complicated by the presence of the Zeeman states with different energies. Also, the mixing of cooling and collisions may produce unexpected effects if the two processes are not separable. Finally, there are indications in previous MOT studies that at very strong fields off-resonant processes can become important. Thus, by using the technique of our earlier study , we have examined the dynamics of two colliding atoms in a one-dimensional blue-detuned optical lattice. It turns out that all the above-mentioned aspects, incomplete and complete shielding, and the off-resonant processes, are present also for the blue-detuned lattices. But more importantly, it turns out that the shielding mechanism and the cooling and trapping mechanism can coexist without interfering with each other.

This paper is constructed as follows. First we briefly review in Sec. II the basic properties and construction of blue-detuned optical lattices, and in Sec. III the optical shielding process in collisions. In Sec. IV we present how to treat the two situations within the same dynamical model with Monte Carlo wave function (MCWF) simulations. The results are given in Sec. V and finally discussed in Sec. VI.

## II Blue-detuned near-resonant optical lattices

The light shifts of the sublevels of the atomic ground state energy states are positive for blue-detuned light. The stronger the coupling, the larger is the light shift, and the higher the level lies in energy. Therefore the optical potential minima may occur when the atomic ground state Zeeman sublevel is minimally coupled to the excited states. This implies that it should be possible to trap atoms with laser field polarization gradients around those points in space where there is no coupling to the excited state. For example, if the ground and excited states have an equal total angular momentum quantum number $`J`$, the ground state sublevel with angular momentum projection state $`m_g=J`$ is not coupled to the excited state when the light is $`\sigma ^+`$ polarized. The coupling strength and the optical potential increases when the atom moves away from the totally dark point, in this case away from the point of $`\sigma ^+`$ light polarization.

In the schemes for optical lattices which use e.g. only one ground and one excited state manifold ($`JJ`$), one of the light-shifted eigenstates is in fact a completely dark state which is not coupled to the excited state at any point of space. It would be ideal for trapping atoms but unfortunately the optical potential for this state is flat. This state can be used for efficient laser cooling , and the photon scattering is about two orders of magnitude smaller than in other near-resonant laser cooling and trapping schemes. In order to achieve a lattice structure one can add a magnetic field , which modifies the energy of the initially flat dark eigenstate in a periodic way. Instead of applying a magnetic field one can also avoid the flat dark state problem by using two different excited state hyperfine manifolds .

In our study we consider the magneto–optical $`JJ`$ lattice proposal of Grynberg and Courtois (GC) . The numerical simulations for dynamical collision studies in optical lattices are very demanding , and the GC scheme allows us to do numerical simulations with parameter values that are also experimentally realistic. We limit our study to the case where $`J_g=J_e=1`$. It is possible to find a level scheme like this in 87Rb which has $`F=1`$ hyperfine states for both the $`5S_{1/2}`$ ground and for the $`5P_{1/2}`$ excited state . We label the three ground state sublevels with $`|g_{\pm 1}>,|g_0>`$, and the three excited state sublevels with $`|e_{\pm 1}>,|e_0>`$, where the integer subscripts indicate the angular momentum projection quantum number $`m`$, see Fig. 1. We use the atomic mass of 87Rb in our simulations.

The laser field consists of two counter–propagating beams with orthogonal linear polarizations and with frequency $`\omega _L`$. For a zero magnetic field the laser detuning is $`\delta =\omega _L\omega _0`$, where $`\omega _0`$ is the atomic frequency. The total field has a polarization gradient in one dimension and reads (with suitable choices of phases of the beams and origin of the coordinate system)

$$𝐄(z,t)=_0(𝐞_xe^{ik_rz}i𝐞_ye^{ik_rz})e^{i\omega _Lt}+c.c.,$$
(1)
where $`_0`$ is the field amplitude and $`k_r`$ the wavenumber. With this field, the polarization changes from circular $`\sigma ^{}`$ to linear and then to circular in the opposite direction $`\sigma ^+`$ when $`z`$ changes by $`\lambda _L/4`$, where $`\lambda _L`$ is the wavelength of the laser light.

The intensity of the laser field and the strength of the coupling between the field and the atom is described by the Rabi frequency $`\mathrm{\Omega }=2d_0/\sqrt{2}\mathrm{}`$ where $`d`$ is the atomic dipole moment of the transition between the ground and excited states. In the level scheme used here all the allowed transitions are equally strong and the absolute value of the corresponding Clebsch–Gordan coefficient has been included in the definition of the Rabi frequency $`\mathrm{\Omega }`$ above.

The magnitude of the light shift is  (when taking into account the current level and coupling scheme)

$$U_0=\frac{1}{2}\mathrm{}\delta s_0,$$
(2)
where $`s_0`$ is the saturation parameter given by

$$s_0=\frac{\mathrm{\Omega }^2/2}{\delta ^2+\mathrm{\Gamma }^2/4}.$$
(3)
The magnetic field $`𝐁`$ is applied in the $`z`$–direction, $`B=B_z`$, which is also the quantization axis. The ground state $`m_g=0`$ is not Zeeman shifted but the states $`m_g=\pm 1`$ are shifted by $`|\mu B|=\mathrm{}\mathrm{\Omega }_B`$ into opposite directions with respect to each other. Here $`\mu `$ is the magnetic moment along the $`z`$–axis of the corresponding state. Thus the energy separation between $`m_g=\pm 1`$ states due to magnetic field is $`2\mathrm{}\mathrm{\Omega }_B`$.

If the light shift dominates over the Zeeman shift, $`\mathrm{}\mathrm{\Omega }_B<U_0`$, the lattice is paramagnetic . The atoms are trapped in potential wells located $`0.5\lambda `$ apart, either in the points of $`\sigma ^+`$ polarization or in the points of $`\sigma ^{}`$ polarization, depending on the direction of the applied magnetic field. If the Zeeman shift dominates, $`U_0<\mathrm{}\mathrm{\Omega }_B`$, the eigenstates of the system correspond to Zeeman sublevels onto which the light field induces perturbations. In this case the atoms are trapped in both $`\sigma ^{}`$ and $`\sigma ^+`$ light polarization points in space and the lattice behaviour is antiparamagnetic .

We have done our simulations in the antiparamagnetic regime where the Zeeman shift dominates over light shifts, $`U_0<\mathrm{}\mathrm{\Omega }_B`$. The polarization gradient of the laser field modifies the lattice potential as in the Sisyphus scheme , see Fig. 2. The atoms are cooled by optical pumping, and are trapped into the $`m_g=1`$ and $`m_g=+1`$ ground sublevels. Without the magnetic field there would be no cooling or trapping for $`J_g=J_e=1`$ system due to the dark state and the lack of motional coupling between the dark state and the coupled states .

Since the Zeeman shifts for $`m_g=1`$ and $`m_g=+1`$ are in opposite directions, their effective detuning from the resonance is not equal and consequently they experience different optical potential modulation depths $`U_{}`$ and $`U_+`$ respectively. The value of $`U_0`$ gives the optical potential modulation depth when the Zeeman shift is large compared to the detuning. This is the value which both $`U_{}`$ and $`U_+`$ approach when $`U_0`$ is kept fixed with increasing detuning. We show the schematic view of optical potentials for ground sublevels in Fig. 2. The relevant lattice properties along with simulation parameters are given in Tables I and II. We have performed a series of simulations for two fixed values of detuning, with a changing Rabi frequency, and another series for a fixed value of $`U_0`$, with a changing detuning and Rabi frequency.

## III Optical shielding

### A Collisions in the present of near-resonant light

Two slowly colliding atoms form a quasimolecule. When a laser field is present the quasimolecule may be resonantly excited at long range at the Condon point $`R_C`$ where the ground and excited molecular states become resonant. In this case the nature of the atomic collision depends on the sign of the detuning of the laser .

For a red-detuned laser the excitation is followed by an acceleration of the quasimolecule on an attractive excited state. The collision becomes inelastic when spontaneous decay back to the ground state occurs and the pair of colliding atoms gain kinetic energy. The shared energy increase corresponds to the acceleration on the excited state. This is the radiative heating and escape mechanism. In addition the atoms may also gain kinetic energy by a fine-structure changing mechanism. If the atom pair survives on the excited state to very small internuclear distances and there is a level crossing between two excited fine-structure states, the pair may change their internal state. When coming out of the collision on a fine structure state which is asymptotically below the state on which they entered the collision, the kinetic energy of the quasimolecule increases by the corresponding amount. For a review see Ref. .

When the laser field present is blue-detuned the situation is different. The resonant excitation of the quasimolecule at $`R_C`$ occurs now to a repulsive molecular state. The atom pair is prevented from approaching close to each other due to the reflection of motion on the repulsive state at the turning point $`R_{tp}`$, see Fig. 3. If the transfer of population back to the ground state is not complete when the quasimolecule traverses $`R_C`$ again the atom pair may gain kinetic energy. In this case the shielding is incomplete and the collision is inelastic. If the population transfer between the states is adiabatic and there is no time for spontaneous emission to occur during the process, shielding becomes complete and the laser-assisted collision between atoms is elastic.

It should be noted that despite strong localization of atoms into lattice sites, atoms still move from site to site to some extent. This is because the finite spatial extent of atomic wave packets and optical pumping process. Thus the localization does not mean that weak long-distance atom-atom interactions at relatively fixed atom-atom distances now dominate over the more stronger cold collisions between moving atoms.

### B Shielding of ground state processes

Efficient optical shielding can suppress the rates of unwanted processes which occur at short internuclear distances even in the absence of laser fields . Inelastic ground–ground processes are suppressed because complete shielding simply empties the quasimolecule ground state at $`R_C`$ and in principle the quasimolecule can never reach the internuclear distances $`R<R_C`$. Since for near-resonant light the values for $`R_C`$ are typically hundreds or thousands of Ångstroms, any small-distance molecular process such as a change of a hyperfine state or Penning ionisation, is prevented.

In the past the optical shielding and suppression has been studied experimentally e.g. in the following contexts: suppression of heating and escape of atoms in MOTs , shielding of photoassociative ionizing collisions , shielding of ionizing collisions of metastable xenon and krypton , and optical suppression in two-photon “energy pooling” collisions in Rb MOTs . Theoretical methods used for shielding studies include MCWF simulations , Landau–Zener  and three–dimensional Landau–Zener theory , and quantum close–coupling calculations . It should be noted that shielding does not help very much in achieving Bose-Einstein condensation as it involves actual resonant absorption and subsequent emission of photons, with the corresponding recoil momentum effects.

### C Shielding in optical lattices

When studying optical shielding in blue-detuned near-resonant optical lattices, there is no need for additional shielding lasers. The blue-detuned lattice laser itself acts as a shielding laser. Efficient shielding in blue-detuned lattices would make it possible to increase the occupation density even in the case of near-resonant lattices and without the problems arising from light-assisted inelastic collisions and photon reabsorption. This would be in contrast to the case of red-detuned near-resonant optical lattices where the inelastic processes dominate when the occupation density increases and atom–atom interactions are accounted .

Our simulation scheme and collision model is similar to the one we have used previously for collision studies in optical lattices and the details can be found in Ref. . The simulations require very large computational resources and we note again that we fix the position of one of the two colliding atoms in respect to the lattice. The small number of scattered photons means that in a high density atom cloud the radiation pressure due to reabsorbed photons decreases. This means that our purely collisional model becomes more realistic in the context of the thermodynamics of the atom cloud, compared to our previous studies of the red-detuned case .

## IV Framework for simulations

### A Product state basis and Hamiltonian

We formulate the problem in position space and use the two–atom product states . We do not use the adiabatic elimination of the excited states  since we want to account for the dynamical nature of atomic interactions in the presence of near-resonant light. The basis vectors are

$$|j_1m_1_1|j_2m_2_2,$$
(4)
where $`j_1`$ and $`j_2`$ denote the ground or excited state and $`m_1`$, $`m_2`$ denote the quantum number for the component of $`J`$ along the quantization axis $`z`$ for atom 1 and 2 respectively in our $`J_g=J_e=1`$ system. The total number of states in principle is $`6\times 6=36`$. In the current coupling and level scheme it is possible to simplify the problem and use only $`9`$ states, see below.

We have to fix the position of one atom, and the binary system wave function depends now only on the position $`z_2`$ of the moving atom 2

$$|\psi (z_2,t)=\underset{j_1,j_2,m_1,m_2}{}\psi _{j_2,m_2}^{j_1,m_1}(z_2,t)|j_1m_1_1|j_2m_2_2.$$
(5)
The atomic spatial dimensionality of the problem is reduced from numerically impossible two to numerically treatable one, see Ref.  for more discussion. The relative coordinate $`z`$ between atoms is now $`z=z_2z_f`$ where $`z_f`$ is the position of the fixed atom.

In the atomic product state basis , our system Hamiltonian is

$$H_S=H_1+H_2+V_{dip}.$$
(6)
Here, $`V_{dip}`$ includes the interaction between the atoms. $`H_1`$ and $`H_2`$ are the single atom Hamiltonians for atoms $`1`$ and $`2`$ respectively in product state space.

The single atom Hamiltonian for atom $`\alpha `$ ($`\alpha =1,2`$) in respective Hilbert spaces is, after the rotating wave approximation,

$$\stackrel{~}{H}_\alpha =\frac{p_\alpha ^2}{2M}\mathrm{}\delta P_{e,\alpha }+\stackrel{~}{V}_\alpha +\stackrel{~}{U}_\alpha .$$
(7)
Here, $`P_{e,\alpha }=_{m=1}^1|e_m_\alpha _\alpha e_m|`$, and the interaction between a single atom $`\alpha `$ and the field is

$`\stackrel{~}{V}_\alpha `$ $`=`$ $`i{\displaystyle \frac{\mathrm{}\mathrm{\Omega }}{\sqrt{2}}}\mathrm{sin}(kz_\alpha )\{|e_0_\alpha {}_{\alpha }{}^{}g_1|+|e_1_{\alpha }^{}{}_{\alpha }{}^{}g_0|\}`$ (9)
$`+{\displaystyle \frac{\mathrm{}\mathrm{\Omega }}{\sqrt{2}}}\mathrm{cos}(kz_\alpha )\{|e_1_\alpha {}_{\alpha }{}^{}g_0|+|e_0_{\alpha }^{}{}_{\alpha }{}^{}g_1|\}+h.c.,`$
where $`z_\alpha `$ is the position operator of atom $`\alpha `$. The dipole–dipole interaction potential $`V_{dip}`$ is the same as used in Refs.  and . The sum over the quantum number $`m`$ in Eq. (12) of Ref.  goes now from $`m=1`$ to $`m=+1`$ for the level scheme $`J_g=J_e=1`$ studied here.

The interaction of atom $`\alpha `$ with the magnetic field $`B`$ in Eq. (7) is

$$\stackrel{~}{U}_\alpha =\underset{i}{}m_i\mathrm{}\mathrm{\Omega }_{B_i}|i_\alpha _\alpha i|,$$
(10)
where the sum over $`i`$ includes all the ground and excited states, and the Zeeman shift factors $`\mathrm{\Omega }_{B_i}`$ are for the ground substates $`m=\pm 1`$ equal to $`\mathrm{\Omega }_B`$, see Tables I and II.

The description of optical shielding is usually given in terms of molecular potentials, see Sec. III. We note that we use the two-atom product state vectors due to their simplicity in treating quantums jumps for the current case. Molecular potentials can be obtained by diagonalizing $`V_{dip}`$ in Eq. (6).

In the antiparamagnetic regime of the GC optical lattice the values of detunings are such that the Zeeman shifts are not negligible in all simulations. The $`m_g=1`$ level is closer to resonance than the $`m_g=+1`$ level for the magnetic field orientation we use. Thus the optical potential modulation depth may also be different for the two states. The values of modulation depth $`U_{}`$ and $`U_+`$ for levels $`m_g=1`$ and $`m_g+1`$ respectively and Zeeman shifts are presented in Tables I and II. In the constant detuning simulations it is necessary to increase the Zeeman shift when going for stronger laser fields and deeper lattices, in order to stay in the antiparamagnetic regime.

### B Aspects of the simulation method

We use the MCWF method to solve the equation of motion for the density matrix of the two-atom system interacting with semiclassical light fields . A direct quantum mechanical solution of the density matrix master equation by other means is not feasible due to the large size of the density matrix and the coupling of atoms to a large number of vacuum modes of the electric field. The variant of Monte Carlo (MC) methods we use was developed by Dalibard, Castin and Mølmer . Application of the MCWF method for the study of cold collisions in optical lattices is not straightforward and we have given the details in our earlier publication . As a result of simulations we obtain a momentum distribution for an atom in the lattice. This distribution is the most informative result when studying optical shielding in the context presented here.

The laser field couples only states where $`\mathrm{\Delta }m=\pm 1`$. The Clebsch–Gordan coefficient between the states $`m_g=0`$ and $`m_e=0`$ is zero in the level scheme. It follows that optical pumping rapidly moves population to the ground levels $`m_g=\pm 1`$ which are coupled only to the excited level $`m_e=0`$. Thus there is population on only three levels for both of the colliding atoms, $`\mathrm{\Lambda }`$ scheme, and number of the used product state basis vectors can be reduced from 36 to $`3\times 3=9`$. This simplifies the problem considerably. The simulations take less computational resources and are much faster to perform. The dipole–dipole interaction does not change the scheme and it is confirmed by the results of the full simulation which includes all 36 states. From molecular potential point of view this means that only one attractive and one repulsive state is relevant instead of all four different attractive and four different repulsive states.

The number of collisions should be the same for simulations with different parameters for the results to be comparable with each other. The number of collisions is dictated by the number of spontaneously emitted photons. We fix the simulation time to constant value 120, in units of $`1/\mathrm{\Gamma }s_0`$. This guarantees that the average number of spontaneously emitted photons and the number of collisions remains roughly the same for all simulations. We have performed all the simulations for the $`1D`$ occupation density of $`25\%`$ of the lattice, i.e., every fourth lattice site is occupied on average.

## V Results

We present the momentum distributions of three simulation series in Figs. 4, 5, and 6. We do two simulation series with the constant values of detuning $`\delta `$ and changing the Rabi frequency $`\mathrm{\Omega }`$. We have $`\delta =5\mathrm{\Gamma }`$ and $`\delta =10\mathrm{\Gamma }`$, in Figs. 4 and 5, respectively. Figure 6 gives results for a constant optical potential modulation depth, $`U_0710E_r`$, and changing $`\delta `$. We compare the results between interacting and non–interacting atoms.

### A Constant detuning

For the smallest values of $`\mathrm{\Omega }`$, the constant detuning simulations show that optical shielding is not complete. Wide wings towards large momentum appear, Figs. 4a) and b), 5a) and b). The resonant excitation process at Condon point $`R_C`$ is not adiabatic and some atoms can move apart on repulsive molecular state after the collision. If the process terminates for spontaneous decay at $`r>R_C`$ the atom pair gains corresponding amount of kinetic energy by acceleration on repulsive molecular state, see Fig. 3.

The wings get narrower when we increase the value of $`\mathrm{\Omega }`$ and nearly vanish when the point of complete shielding is reached, Figs. 4c) and 5c). The resonant excitation process for the repulsive state at $`R_C`$ becomes adiabatic and hardly any change in $`p`$–distribution is visible when compared to non-interacting atoms. When atoms try to occupy the same lattice site, they collide elastically in this parameter regime.

When we further increase the Rabi frequency, the off-resonant effects come into play, Figs. 4d) and 5d). The momentum distribution begin to deviate again from the result for non–interacting atoms, and the qualitive character of momentum broadening is now different when compared to the small $`\mathrm{\Omega }`$ results. This indicates that the heating process does not arise from incomplete shielding. Additional shoulders that appear in both the interacting and non–interacting cases arise due to the difference in the depth of the two lattice potential wells, $`U_{\pm 1}`$. When we increase $`\delta `$, we note that the point of complete shielding moves towards larger $`U_0`$. In our case from $`\delta =5\mathrm{\Gamma }`$ and $`U_0=712E_r`$ to $`\delta =10\mathrm{\Gamma }`$ and $`U_0=2554E_r`$.

### B Constant lattice depth

Figure 6 shows results for the case of constant optical modulation depth $`U_0710E_r`$ and varying detuning. When the detuning is small the off-resonant effects heat the atomic cloud and small wings appear in momentum distribution, see Fig. 6a). For an intermediate detuning value the point of complete shielding is reached, Fig. 6b). Increasing $`\delta `$ further makes the shielding incomplete and subsequently wide wings appear in the momentum distribution, Figs. 6c) and d). This is in agreement with the study of off-resonant effects of the laser field in cold collisions in MOTs . Keeping the lattice depth constant and increasing the detuning means decreasing the ratio $`\mathrm{\Omega }/\delta `$, which reduces the role of off-resonant effects. Simulation studies reported in Ref.  show that for collisions in uniform blue-detuned laser fields the off–resonant effects vanish when $`\mathrm{\Omega }/\delta `$ decreases until for small values of $`\mathrm{\Omega }/\delta `$ the shielding effect is again incomplete. This is accordance with the optical lattice results presented here.

## VI Conclusions

Our simulations demonstrate clearly that optical shielding should be present in blue-detuned near-resonant optical lattices. The shielding process is not expected to be always perfect but with an appropriate choice of the detuning and the intensity of the trapping laser it is nevertheless possible to strongly suppress the rate of inelastic collisions. For example, with a detuning $`\delta =5.0\mathrm{\Gamma }`$ and a Rabi frequency $`\mathrm{\Omega }=3.0\mathrm{\Gamma }`$, giving $`U_0=710E_r`$ in our scheme, the optical shielding process is practically complete, see Fig. 4c). If the parameters are not chosen correctly, the shielding process can be either incomplete or reduced by the off-resonant excitation of the quasimolecule states related to attractive atom-atom potentials .

We have studied here the antiparamagnetic regime of a GC–lattice . In this case the cooling and trapping mechanism resembles the traditional Sisyphus mechanism , making comparisons between our previous study of the red-detuned case more appropriate. In this scheme the lattice depth depends on the intensity of the laser. The value of detuning for effective shielding increases when the laser intensity and thus the optical potential modulation depth $`U_0`$ is increased. Thus for shallow lattices effective shielding occurs at small detunings, in which case the two trapping potentials are not identical because of the non–negligible Zeeman shift compared to the detuning of the laser.

In the paramagnetic regime of a GC–lattice the lattice depth $`U_0`$ is dictated by the strength of the magnetic field more than by the laser intensity. This leaves more freedom for using both the intensity and detuning of the laser to optimize optical shielding for a given lattice depth. This is an interesting subject for possible future studies of collisions in blue-detuned near-resonant optical lattices.

Together with the reduced photon scattering and thus reduced heating of dense atomic clouds by photon reabsorption, optical shielding opens a way to achieve higher occupation densities and lower temperatures in blue-detuned near-resonant optical lattices, compared to the red-detuned case. Unlike in the red-detuned case, two atoms trying to occupy the same lattice site will at the worst case only repulse each other in an elastic process. It should be noted that optical shielding was originally introduced to e.g. suppress the hyperfine state changing ground-ground collisions during cooling and trapping of alkali-metal atoms , and this additional benefit is naturally present in blue-detuned lattices as well. More importantly, the strong Penning ionisation for metastable rare gas atoms  should be suppressed as well in blue-detuned lattices. An important benefit here is that all three processes, trapping, cooling and shielding, are produced by the same set of laser beams.

Considering what is already known about blue-detuned optical lattices, and about optical shielding in magneto-optical traps, our results appear rather obvious. However, they could have been different. Firstly, previous theoretical studies of optical shielding have excluded the actual cooling process . Our results show that the two can coexist at least in blue-detuned lattices without apparent problems even in the saturation limit, although the off-resonant excitation of quasimolecule states reduces the shielding efficiency. In experiments in magneto-optical traps shielding has been implemented typically with an additional catalyst laser, with the red-detuned cooling and trapping lasers either off or on. If the red-detuned cooling and trapping lasers are on, the near-resonant shielding studies become practically impossible due to the strong and usually unfavourable mixing of the two processes . In other words, we hope that our work serves as a motivation for experimentalists to perform shielding studies in near-resonant blue-detuned lattices in the presence of the cooling process. Although the densities that have been available so far have been rather low, the use of e.g. metastable rare gas atoms could provide useful information due to the clear ion signal that marks collision events .

Secondly, very few theoretical studies of shielding with near-resonant light have been done so far, as the interest has been mostly on the large-detuned laser fields. This is because the theoretical treatment is simplified when we can ignore the spontaneous emission (at large detunings the excited state potential is so steep that the resulting fast dynamics and slow spontaneous emission decouple trivially from each other). In an earlier near-resonant study  the possibility of spontaneous emission from the excited repulsive quasimolecule state during the slow-down of the relative motion of the two atoms was found to be suppressed by re-excitation, until the atoms had finally turned around, i.e., the efficiency of shielding increased without limit with laser intensity. Similarly, in our study there does not seem to be any evidence for breakdown of efficient shielding due to such a spontaneous emission effect.

Thirdly, experiments show clearly that the shielding efficiency of inelastic ground-ground collisions can saturate to some finite value as we increase the laser intensity . The reason for this is still unclear. It has been attributed to various processes, in addition to the above-mentioned premature termination of shielding via spontaneous emission . Other possibilities include counterintuitive or off-resonant processes involving different partial waves or other processes that similarly involve multiple states (in contrast to the basic two-state approaches ), or off-resonant excitation to the attractive molecular states . We find that off-resonant excitation is indeed present in our studies, where $`\delta 10\mathrm{\Gamma }`$, i.e., our detuning is small in general and comparable to the Rabi frequencies. This is in agreement with the much more simplified three-state study done earlier . When $`\mathrm{\Omega }/\delta 1`$, the steady state formation can surpass the dynamical resonant excitation process at suitably low collision velocities, and we see that indeed it is the near-zero region of the momentum distribution that gets depleted in Fig. 4(d), and not the near-average velocity region as in the red-detuned lattice case. However, as discussed before, this off-resonant process can not explain the observed saturation of shielding, as that happens at very large detunings, for which $`\mathrm{\Omega }/\delta 1`$, but $`\mathrm{\Omega }`$ is large enough for the situation to correspond mainly to Fig. 4(c), the case of complete shielding. There is no evidence of saturation of shielding in our studies, but due to the limitations of our model (one dimension only, and ignoring the very small scale molecular processes), we can not state conclusively that it would not be present in any experiments.

Thus, we have demonstrated that efficient optical shielding should be possible in near-resonant blue-detuned optical lattices. More precisely, it is mediated by the trapping and cooling lasers themselves but it does not interfere with the cooling process, unlike in basic magneto-optical traps created with strong red-detuned lasers. Especially, we have theoretically demonstrated optical shielding within a level scheme which is more complicated (and realistic) than the two-state models used so far . Our approach is fully quantum, takes spontaneous emission into account, and is applicable even for strong fields. Finally, our results show that by a suitable choice of lattice parameters it should be possible to obtain efficient cooling and trapping, together with efficient optical shielding of collisional processes, and yet to avoid any contributions from off-resonant excitation to the attractive quasimolecule states.

###### Acknowledgements.

We thank Kirstine Berg-Sørensen for helpful discussions. J.P. and K.-A.S. acknowledge the Academy of Finland (projects 43336 and 50314) and the European Union IHP CAUAC project for financial support, and the Finnish Center for Scientific Computing (CSC) for computing resources. J.P. acknowledges support from the National Graduate School on Modern Optics and Photonics.


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# On the heavy-fermion behavior of the pyrochlore transition-metal oxide 𝐿𝑖𝑉₂𝑂₄

\[

## Abstract

Motivated by the heavy fermion Fermi liquid (HFFL) features observed at low-$`T`$ in the pyrochlore $`LiV_2O_4`$, we consider a material-specific model that includes aspects of the local quantum chemistry, the geometrically frustrated lattice structure, and strong correlations in a single approach. In particular, we show how geometrical frustration (GF) gives rise to a crossover scale, $`T^{}<<J`$, the intersite (AF) exchange, below which the metallic system shows HFFL features. Our scenario is a specific realization of the importance of GF effects in driving HFFL behavior in $`LiV_2O_4`$, and provides a natural understanding of various puzzling features observed experimentally.

\]

Systems of the type $`AB_2O_4`$ with a magnetic $`B`$ site consistently show strange properties. In particular, systems with $`B=Ti,V,Cr`$ are interesting because the $`d`$ electrons occupy $`t_{2g}`$ orbitals that do not hybridize with the oxygen orbitals along certain directions. In the geometrically frustrated structure, the nearest neighbor exchange interaction dominates with a maximization of frustration. Concomitantly, only $`3d`$ bands ($`t_{2g}`$) cross the Fermi level $`(\mu )`$, leading one to have to deal with the ubiquitous strong correlations. With a divalent $`A`$-ion, the $`B`$ site has integral valence, giving rise to Mott insulating behavior with frustrated magnetism, e. g., in $`ZnV_2O_4`$. On the other hand, with a monovalent $`A`$ site, $`B`$ is mixed-valent, resulting in a narrow-band metal. This combination of frustrated magnetism and correlated metallic behavior leads to a range of complex and unusual manifestations, from superconductivity, for example in $`LiTi_2O_4`$, via heavy-fermion Fermi liquid (HFFL) behavior in $`LiV_2O_4`$, to spin-glass behavior in other systems.

The best example in the second category above is $`LiV_2O_4`$ , a paramagnetic metal for $`T>0.01`$K. The low-$`T`$ Sommerfeld constant achieves its highest value for a $`d`$-electron system, $`0.42J/mole/K^2`$ at $`T=1.5K`$. The resistivity, the Woods-Saxon ratio, as well as the Wilson ratio all exhibit behaviors expected for prototypical rare-earth based HFFL metals . Importance of geometrical frustration (GF) for magnetic properties is shown by the absence of a low-$`T`$ magnetic instability, and further vindicated by neutron scattering (INS) studies , which reveal a response characteristic of insulating, frustrated magnets. This leads one to ask: What is the role of GF in driving HFFL behavior? More precisely, how does one reconcile the HFFL behavior in thermodynamics and transport with a magnetic response characteristic of frustrated, insulating magnets? What is the role of strong correlations in the $`3d`$ bands? How do these two subsystems couple to (affect) each other at low-$`T`$?

Much attention has been devoted to these issues. LDA bandstructure calculations indeed show that the $`3d`$ $`t_{2g}`$ bands alone cross the Fermi level . A trigonal distortion splits the three-fold degenerate $`t_{2g}`$ states into the (lower lying) singlet $`A_{1g}`$ with a bandwidth of $`1eV`$, and an $`E_g`$ doublet with a bandwidth of $`2eV`$ in the solid. Given the formal $`d^{1.5}`$ state of $`V`$, the $`A_{1g}`$ band is half-filled, and the $`E_g`$ bands are quarter-filled, leading  to suggestions that an effective Anderson model could be used. However, approaches along these lines require the rather ad-hoc introduction of a large intersite Kondo coupling to counterbalance the strong local Hund’s rule coupling, the origin of which is unclear. Moreover, frustration effects are not important in these pictures. On the other side, Fulde et al.  have proposed that the $`V`$ lattice of corner-sharing tetrahedra frustrates charge ordering and leads instead to isolated finite chains of $`S=1/2`$ and $`S=1`$. The gapless fermionic spin excitations of the $`S=1/2`$ chains give the large $`\gamma `$ coefficient of the low-$`T`$ specific heat. This picture needs to be extended to derive the HFFL properties, and to make a detailed comparison with INS results. Varma  seeks to understand the HFFL properties by analyzing the energetics of the crossover which a $`S1/2`$ impurity must undergo in the Kondo effect. Frustration does not play any role here either. Recently, Burdin et al.  have studied the role of frustration effects in driving HFFL behavior. However, frustration effects are put in by hand, limiting a direct comparison with the actual material. Lacroix  has recently sketched the outlines of a picture for HFFL behavior in $`d`$-band oxides with geometrical frustration.

Here, we study a theoretical model that is material-specific and includes all the relevant degrees of freedom and explicitly address the questions above. In particular, we show how the HFFL properties are reconciled with the magnetic response characteristic of frustrated, insulating magnets. The choice of the model Hamiltonian is motivated by experimental constraints  as well as by results of first-principles LDA calculations :

$$H=H_s+H_b+H_{sb},$$
(1)
where $`H_s=_{ij}J_{ij}𝐒_i.𝐒_j`$ is the Heisenberg-like $`S=1/2`$ Hamiltonian describing the localized spin degrees of freedom originating from the half-filled narrow singlet $`A_{1g}`$ band. In $`LiV_2O_4`$, the next-nearest neighbor coupling may be important, though its magnitude is not reliably known.

$`H_b`$ $`=`$ $`{\displaystyle \underset{<ij>}{}}t_{ab}(c_{ia\sigma }^{}c_{jb\sigma }+h.c)+U{\displaystyle \underset{ia}{}}n_{ia}n_{ia}`$ (2)
$`+`$ $`U_{ab}{\displaystyle \underset{i,a,b}{}}n_{ia}n_{ib}`$ (3)
describes the electronic degrees of freedom for the $`E_g`$ bands. And $`H_{sb}=J_H_{i,a,b}𝐒_i.(\sigma _{ia}+\sigma _{ib})`$ describes the coupling of these two subsystems via a local Hund’s rule interaction.

In what follows, $`H`$ is defined on the fully-frustrated pyrochlore (FFL) lattice, entailing explicit consideration of geometrical frustration effects. To proceed in this complicated situation, and motivated by observations, we make the plausible assumption: The underlying $`A_{1g}`$ spin configuration does affect the charge dynamics in the $`E_g`$ band, but that there is no qualitative change in the localized magnetic response coming from the feedback effects due to this carrier dynamics. This assumption is justified later. With this, we follow the following strategy: $`(i)`$ Treat the spin correlations in the Heisenberg like model on the FFL within a cluster approach capable of correctly treating the short-range fluctuations which drive the spin liquid behavior as observed in INS experiments. $`(ii)`$ Use the fact that the $`A_{1g}`$ spins are coupled to the correlated electrons in the $`E_g`$ band(s), and modify the hopping, $`t_{ab}`$, to solve the modified electronic model within the $`d=\mathrm{}`$ approximation, which is the best technique to reliably access dynamical effects of strong, local correlations . As with the $`A_{1g}`$ spins, the $`E_g`$ electrons live on the FFL, a fact that is indeed important for a consistent understanding, as we show below.

On the FFL, the electronic dispersion relation (or the spin-wave dispersion for localized spins) has four branches corresponding to the four-sublattice structure inherent in this geometry; two branches are completely flat over the whole Brillouin zone, while the other two form dispersive bands in the solid. Mathematically, $`ϵ_\alpha (𝐤)=2t`$ for $`\alpha =1,2`$ and, $`ϵ_\alpha (𝐤)=2t(1\pm \sqrt{c_xc_y+c_yc_z+c_zc_x})`$ for $`\alpha =3,4`$ $`[c_acos(k_a/2)]`$. Notice that the free dispersion alone gives a two-band structure in the unperturbed DOS (see Fig. 2, with $`U_{ab}=0`$). For the $`A_{1g}`$ spins, one replaces $`ϵ(𝐤)`$ by $`J(𝐪)`$ and $`t`$ by $`J`$ in the above equations. From the susceptibility data , a large $`g=2.23`$ is inferred, suggesting strong ferromagnetic coupling between the carriers in the $`E_g`$ band and the “localized” spins in the $`A_{1g}`$ band (large $`J_H`$). So the carrier hopping rate is strongly coupled to, and reflects the underlying ($`A_{1g}`$) spin correlations: $`t_{ab}(𝐒)t_{ab}\sqrt{1+<𝐒_i.𝐒_j>/2S^2}`$ .

As mentioned before, we first focus on the $`A_{1g}`$ correlations, assuming, in accordance with LDA calculations, that this narrow band is completely occupied by one localized electron per site. Following , we employ a self-consistently embedded cluster approach that treats the spin correlations in one tetrahedron exactly and mimics the influence of the remaining tetrahedra by inhomogeneous, selfconsistently determined magnetic fields. The resulting static spin susceptibility is shown in Fig. 1. $`\chi _s(T)`$ shows a Curie-Weiss (CW)-like form at high-$`T`$, followed by a maximum at lower $`T^{}<<J`$. And $`\chi (𝐪,T)=g(𝐪)\chi (T)`$, consistent with . At very low $`T`$, a gap opens up in the spin excitation spectrum; by fitting $`\chi (𝐪,T)`$ to an exponential form, we extract the spin correlation length, which turns out to be weakly $`T`$-dependent and never exceeds a lattice spacing, in qualitative agreement with . The resulting physical picture is that of a strongly fluctuating spin system, with extreme short-range AF correlations and no long-range order down to $`T=0`$. This agrees with the absence of magnetic order found experimentally, as also with the fact that the CW constant corresponds to $`S=1/2`$, and that $`\mathrm{\Theta }_{CW}<0`$.

A potentially interesting situation now occurs: the carrier hopping, as mentioned above, reflects the $`A_{1g}`$ spin correlations as well as intrinsic geometric frustration effects from the FFL structure, preventing the tendency to charge- and/or orbital ordering (COO). This explicitly realizes the mechanism for suppression of COO proposed by Fulde et al. ; however, in our approach, it does not lead to formation of $`S=1/2`$ and $`S=1`$ rings and chains. The difference from the CMR manganites  also has a consistent explanation within this picture: the frustrated kinetic energy selfconsistently prevents the possibility for the $`A_{1g}`$ spins to align (via “double exchange”) ferromagnetically, in contrast to what happens in manganites .

Next, consider the $`E_g`$-band electrons strongly coupled to the $`A_{1g}`$ spins via a local (ferromagnetic) Hund’s rule coupling:

$`H_{el}`$ $`=`$ $`t{\displaystyle \underset{<ij>,\sigma }{}}(c_{ia\sigma }^{}c_{jb\sigma }+h.c.)+U{\displaystyle \underset{i,a}{}}n_{ia}n_{ia}`$ (4)
$`+`$ $`U_{ab}{\displaystyle \underset{i}{}}n_{ia}n_{ib}J_H{\displaystyle \underset{i}{}}𝐒_i.(\sigma _{ia}+\sigma _{ib}),`$ (5)
where $`a`$ and $`b`$ refer to the doubly degenerate $`E_g`$ states in the $`t_{2g}`$ sector, defined on the FFL. With the strong $`J_H`$, the “double exchange” projection transforms the problem to that of spinless fermions, but the hopping is modulated by the underlying, frustrated spin correlations in the $`A_{1g}`$ band. The Hamiltonian is,

$$H_{el}=\underset{<ij>,a,b}{}t_{ij}(𝐒)(c_{ia}^{}c_{jb}+h.c)+U_{ab}\underset{i}{}n_{ia}n_{ib},$$
(6)
where we set $`U,J_H\mathrm{}`$. Relabelling $`c_a=c_{}`$ and $`c_b=c_{}`$, we are left with a Hubbard-like model with a non-trivial hopping term:

$$H_{el}=\underset{<ij>,\sigma }{}t_{ij}^\sigma (𝐒)(c_{i\sigma }^{}c_{j\sigma }+h.c)+U_{ab}\underset{i}{}n_in_i.$$
(7)
We use the $`d=\mathrm{}`$ approximation to solve the Hubbard-like model on the FFL. This interesting problem has non-trivial solution(s), related to the one-electron dispersion on the FFL. In particular, close to $`n=1`$, non-Fermi liquid behavior is expected due to the strong scattering off the completely flat bands. Fortunately, for $`LiV_2O_4`$, one deals with an almost quarter-filled band, rendering the flat-band singularities irrelevant. The above electronic model is now solved using the iterated perturbation theory (IPT) at slightly less than quarter-filling and at finite $`T`$ .

Fig. 2 shows the evolution of the one-electron local spectral function, $`\rho (\omega )`$. As $`U_{ab}`$ increases, a sharp collective Kondo-like peak appears and gets narrower around $`\mu `$. The appearance of upper and lower “Hubbard” bands (these appear as shoulder-like features in the range $`2\omega 2`$ in Fig.2), reflecting suppression of charge fluctuations near quarter-filling, is also clear. Formation of heavy quasiparticles is reflected in the quasiparticle renormalization constant, $`Z(\mu )`$, defined as $`Z(\mu )=\left[1\frac{d\mathrm{\Sigma }^{}(\omega )}{d\omega }|_{\omega =\mu }\right]^1`$.

$`Z(\mu )`$ decreases monotonically with increasing $`U_{ab}`$. That this correlated metallic state with heavy fermion mass ($`m^{}/m=1/Z(\mu )`$) is a FL is clear from the fact that Im$`\mathrm{\Sigma }(\omega \mu )=b(\omega \mu )^2`$. Importance of the filling is shown by the fact that charge fluctuations are enhanced, while spin fluctuations diminish in importance as $`n`$ is decreased further (not shown). Our results are in complete agreement with those of Imai et al.  for a two-orbital Hubbard model with finite $`U`$ and $`J_H`$, and the HFFL behavior in our model should persist when large, finite $`U`$ and $`J_H`$ are included. The computed integrated photoemission lineshape in the HFFL phase is shown in Fig. 3. Signatures of strong electronic correlations in the $`E_g`$ band are visible as shake-up features: a broad, incoherent, lower Hubbard band feature well separated from the narrow quasiparticle resonance. This should provide evidence in favor of our modelling of the $`E_g`$ manifold.

Finally, consider the question of selfconsistency due to the coupling of the correlated carriers to the $`A_{1g}`$ spin fluctuations. At low $`T<T^{}`$, the dynamical spin susceptibility behaves like $`\chi \mathrm{"}(\mathrm{\Omega })(\mathrm{\Omega }/T^{})`$ in the HFFL regime (see below). The leading-order correction to the self-energy of the correlated carriers is $`\mathrm{\Sigma }(i\omega _n)=(J_H^2/\beta )_m\chi (i\mathrm{\Omega }_m)G(i\omega _ni\mathrm{\Omega }_m)`$. In the HFFL regime, $`G(\tau )(1/\tau )`$ for long times, and $`\mathrm{\Sigma }(\omega )`$ remains qualitatively unchanged from its FL-like form (see above) as long as $`\chi \mathrm{"}(\mathrm{\Omega })\mathrm{\Omega }/T^{}`$. This analysis ceases its validity above $`T^{}`$, where the susceptibility gets increasingly dominated by fluctuating local moment contributions. Inserting the resulting $`\mathrm{\Sigma }(\omega )`$ into the calculation for the susceptibility (notice that at low $`T`$, the spin susceptibility of the localized spins is gapped) leads again to the $`\mathrm{\Omega }/T^{}`$ form, apart from prefactors. Thus, at low $`T<T^{}`$, selfconsistency leads only to a minor quantitative modification of our results.

Let us discuss the implications of our calculation. Since the magnetic correlation length is $`T`$-independent below $`T^{}<<J`$ (corresponding to the point at which $`\chi (T)`$ shows a peak, see Fig. 1) this sets the scale below which the hopping, $`t`$, can be treated as constant in $`H_b`$. Above $`T^{}`$, the influence of the $`A_{1g}`$ spin correlations drive the system into a local-moment metallic regime, but below this scale, HFFL-like quasiparticles develop as shown above. We thus identify the low-$`T`$ crossover scale seen in experiments with the $`T`$-dependence of the frustrated spin dynamics in the $`A_{1g}`$ sector coupled to correlated $`E_g`$ carriers. This implies that the mechanism for HFFL behavior in our scenario is intimately linked to the local-moment magnetism of the FFL, and is drastically different from the conventional view, where a band of uncorrelated  carriers collectively screens localized moments at every site. Our calculation explicitly realizes the suggestions of Lacroix , but goes much further, showing clearly how short-ranged, spin-liquid-like local moment correlations in the $`A_{1g}`$ sector on the FFL are related to the onset of HFFL behavior. In our opinion, a mean-field-like decoupling cannot describe the crossover at $`T^{}`$ adequately, since the spin liquid behavior is driven precisely by strong fluctuations beyond the mean-field picture.

Given the HFFL metallic state below $`T^{}`$, the electronic specific heat, behaves like $`𝒞_{el}(T)(T/T^{})`$, with a peak at $`T^{}`$. The local dynamical spin susceptibility $`J\chi \mathrm{"}(\omega )(\omega /T^{})`$, so the NMR relaxation rate is Korringa like, $`1/T_1(T/JT^{})`$. The uniform spin susceptibility $`\chi O(1/J)`$ at low $`T`$. The calculation of the resistivity does not involve vertex corrections within DMFT. At low $`T`$, in the HFFL phase, we obtain $`\rho _{dc}(T)(T/T^{})^2`$, implying that the Kadowaki-Woods relation is obeyed, as in conventional heavy fermions. The Wilson ratio $`W=T\chi /C_{el}O(T^{}/J)`$, again as in the traditional case. All these results are indeed consistent with thermodynamic, transport and magnetic measurements performed on $`LiV_2O_4`$.

A detailed calculation of the dynamical spin response of the FFL is a fascinating problem in itself, and is intimately linked to the details of the $`T`$-dependence of various quantities as $`T`$ crosses $`T^{}`$. We plan to address this more detailed issue in a longer separate work.

To conclude, a theoretical understanding of the various physical features of the frustrated, 3d, heavy fermion metal, $`LiV_2O_4`$ is proposed. In particular, we have shown how the HFFL thermodynamics and transport  can be reconciled with a magnetic response characteristic of frustrated, insulating magnets  and how the experimentally observed crossover scale ($`T^{}`$) is directly related to the $`T`$ dependence of the frustrated spin dynamics in the $`A_{1g}`$ sector. To our knowledge, this is the first attempt that explicitly includes specific lattice structure, magnetic frustration and strong correlation effects within a single picture. Our picture is radically different from conventional ones, and is a concrete realization of the importance of geometrical frustration effects in driving HFFL behavior in $`LiV_2O_4`$.

MSL acknowledges the financial support of the SfB608 of the Deutsche Forschungsgemeinschaft. LC and MSL wish to thank P. Fulde for his kind hospitality at the Max-Planck-Institute für Physik komplexer Systeme.


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# Crossover effects in the bond-diluted Ising model in three dimensions

## 1 Introduction

The qualitative influence of quenched disorder at second-order phase transitions is well understood since Harris proposed a relevance criterion  based on the knowledge of the specific heat critical exponent $`\alpha _{\mathrm{pure}}`$ of the pure model: when $`\alpha _{\mathrm{pure}}`$ is positive, the disordered system will reach a new fixed point with new critical exponents whereas if $`\alpha _{\mathrm{pure}}`$ is negative, the same universality class will persist.

As a paradigmatic model, the three-dimensional (3D) disordered Ising model characterized by $`\alpha _{\mathrm{pure}}=0.109(4)`$ has been extensively studied by:

$``$ Renormalization group methods in the weak quenched dilution regime. The best estimates for the critical exponents obtained by this method are :

$`\nu =0.678\pm 0.010,`$

$`\eta =0.030\pm 0.003,`$

$`\gamma =1.330\pm 0.017`$.

$``$ Monte Carlo simulations of the site-diluted case for which the following exponents have been found :

$`\nu =0.6837\pm 0.0053,`$

$`\beta =0.3546\pm 0.0028,`$

$`\gamma =1.342\pm 0.010`$.

$``$ Experimental investigations.

For a review of these different results, see Ref. .

The general picture which is now widely accepted is that, starting from the pure Ising model (with exponents $`\nu =0.6304\pm 0.0013`$, $`\gamma =1.2396\pm 0.0013`$, $`\beta =0.3258\pm 0.0014`$, see Ref. ), the critical temperature decreases and eventually vanishes at the percolation threshold below which there is no longer any long-range order in the system, due to the absence of percolating clusters. In the dilution-temperature plane, the critical line $`T_c(p)`$ which delimits ferromagnetic and paramagnetic phases has two end-points (namely the pure system and the percolation point) described by unstable fixed points and it is commonly believed that the quenched disordered system has universal properties described by a unique stable fixed point. According to this picture, the competition between fixed points possibly leads to an effective variation of universal critical quantities.

In this paper, we first determine the phase diagram of the bond-diluted problem (up to now, only the site-diluted case has been studied) and compare it to a prediction in the single-bond effective-medium approximation and then we try to illustrate the competition between fixed points leading to crossover regimes in some physical quantities.

## 2 Phase diagram

The bond-diluted Ising model is defined by the following Hamiltonian with independent quenched random interactions:

$$\beta H=\underset{(i,j)}{}K_{ij}\delta _{\sigma _i,\sigma _j}(\sigma _i=\pm 1).$$
(1)
The coupling strengths are allowed to take two different values $`K_{ij}=KJ/k_BT`$ and $`0`$ with probabilities $`p`$ and $`1p`$, respectively,

$$P(K_{ij})=p\delta (K_{ij}K)+(1p)\delta (K_{ij}),$$
(2)
$`c=1p`$ being the concentration of missing bonds, which play the role of the non-magnetic impurities. The simulation technique is based on the Swendsen-Wang cluster algorithm with periodic boundary conditions in the three space directions.

The phase diagram is obtained numerically from the maxima of a diverging quantity (Fig. 1). Here we choose the susceptibility, since the stability of the disordered fixed point implies that the specific-heat exponent is negative in the random system. Thus, the error in this quantity is larger than for the susceptibility. The percolation threshold is located at $`p_c0.2488`$.

To get an accurate determination of the maxima of the susceptibility, we used the histogram reweighting technique with $`\mathrm{2\hspace{0.17em}500}`$ Monte Carlo sweeps (MCS) and between $`\mathrm{2\hspace{0.17em}500}`$ and $`\mathrm{5\hspace{0.17em}000}`$ samples of disorder. The number of Monte Carlo sweeps is justified by the increasing behaviour of the energy autocorrelation time and we chose for each size at least $`250`$ independent measurements of the physical quantities $`(N_{\mathrm{MCS}}>250\tau _E)`$.

For a second-order phase transition, the autocorrelation time is expected to behave as $`L^z`$ at the critical point where $`z`$ is the dynamical critical exponent (Fig. 2). For the disordered Ising model, we get the values of $`z`$ shown in Table 1. We see that the critical slowing down weakens for the disordered model and becomes smaller when the concentration of magnetic bonds $`p`$ decreases, but it is necessary to increase the number of disorder realisations when $`p`$ decreases because of the vicinity of the percolation threshold.

In order to check the quality of the averaging techniques, we can study the stability of the susceptibility for the largest size considered versus the number of Monte Carlo sweeps involved in the thermal average. The results are given in Table 2 for different samples as well as for the disorder average. With $`\mathrm{2\hspace{0.17em}500}`$ MCS, the accuracy of the results for a given sample is not perfect, of course, but the precision of the average over disorder is quite good on the other hand. The disorder average procedure has been investigated by computing the susceptibility $`\chi _j`$ for different samples, $`1jN_s`$, where $`N_s`$ is the total number of samples (Fig. 3). We can see that the dispersion of the values of $`\chi `$ is not very large because the fluctuations in the average value disappear after a few hundreds realisations.

The phase diagram obtained from the location of the maxima of the susceptibility for the largest lattice size as a function of the concentration of magnetic bonds is shown in Fig. 4. The simple mean-field transition temperature is drawn for comparison: it gives a linear behaviour as a function of the bond concentration $`p`$ and we can check that this approximation holds only in the low-dilution regime, $`p>0.8`$. On the other hand, the effective-medium approximation  gives very good agreement with the simulated transition line. Treating only a single bond in an effective medium leads to the following relation for the critical coupling:

$$K_c(p)=\mathrm{ln}\frac{(1p_c)\mathrm{}^{K_c(1)}(1p)}{pp_c}.$$
(3)
This relation is exact in the vicinity of both the pure system and the percolation threshold.

## 3 Competition between the fixed points

The main problem encountered in previous studies of the disordered Ising model was the question of measuring effective or asymptotic exponents. Although the change of universality class should happen theoretically for an arbitrarily low disorder, it can be very difficult to measure the new critical exponents because the asymptotic behaviour cannot always be reached practically. Another difficulty comes from the vicinity of the ratios $`\gamma /\nu `$ and $`\beta /\nu `$ in the pure and disordered universality classes. Indeed, these values for the pure model are :

$$\gamma /\nu =1.966(6),\beta /\nu =0.517(3),\nu =0.6304(13),$$

and for the disordered Ising model :

$$\gamma /\nu =1.96(3),\beta /\nu =0.519(8),\nu =0.6837(53).$$

Thus, from standard finite-size scaling techniques, the critical exponent $`\nu `$ only will allow us to discriminate between the two fixed points. This exponent can be evaluated from the finite-size scaling of the derivative of the magnetisation versus the temperature which is expected to behave as $`\frac{\mathrm{ln}m}{K}L^{1/\nu }`$. From this power-law behaviour, we have extracted the effective size-dependent exponent $`(1/\nu )_{\mathrm{eff}}`$ which is plotted against $`1/L_{\mathrm{min}}`$ for different bond concentrations $`p`$ in Fig. 5 where $`L_{\mathrm{min}}`$ is the smallest lattice size used in the fits.

We clearly see that in the regime of low dilution ($`p`$ close to $`1`$), the system is influenced by the pure fixed point. On the other hand, when the bond concentration is small, the vicinity of the percolation fixed point induces a decrease of $`1/\nu `$ below its expected disordered value. Indeed, the percolation fixed point is characterized by $`1/\nu 1.12`$ .

## 4 Conclusion

We have presented, from a numerical study, the influence of bond dilution on the critical properties of the 3D Ising model. The universality class of the disordered model is modified by disorder but its precise characterization is difficult because of the competition between the different fixed points which induce crossover effects, even for relatively large lattice sizes. The next step is to accurately locate the best dilution which minimizes these crossover effects.

We gratefully acknowledge financial support by the DAAD and EGIDE through the PROCOPE exchange programme. C.C. thanks the EU network “Discrete Random Geometries: from solid state physics to quantum gravity” for a postdoctoral grant. This work was supported by the computer-time grants 2000007 of the Centre de Ressources Informatiques de Haute-Normandie (CRIHAN) and hlz061 of NIC, Jülich.


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# Anomalously Soft Droplets and Aging in Short-ranged Spin Glasses

## Abstract

We extend the standard droplet scaling theory for isothermal aging in spin glasses assuming that the effective stiffness constant of droplets as large as extended defects is vanishingly small. A novel dynamical order parameter $`q_\mathrm{D}`$ and the associated dynamical susceptibility $`\chi _\mathrm{D}`$ emerge. Breaking of the fluctuation dissipation theorem takes place at $`q_\mathrm{D}`$ well below the equilibrium Edwards-Anderson order parameter $`q_{\mathrm{EA}}(>q_\mathrm{D})`$ at which the time translational invariance is strongly broken. The scenario is examined numerically in a 4 dimensional EA Ising spin glass model.

Recently aging in spin glasses APY-review ; Saclay ; Uppsala ; Review-Rieger ; BCKM  has attracted renewed interest both in experimental, numerical and theoretical studies. The phenomena provide very interesting and almost the only realistic way to explore large scale, non-trivial properties of glassy phases. A major theoretical progress was the development of dynamical mean-field theories (MFT) for spin glasses and related systems MFT  which lead to findings of some novel view points in glassy dynamics such as the concept of effective temperature CKP97 . However, the MFT themselves do not provide insights into what will become important in realistic finite dimensional systems, such as nucleation processes.

The droplet theory BM ; FH1 ; FH2  developed a scaling theory assuming droplet excitations as basic nucleation processes. It provides a perspective for equilibrium and dynamical properties of finite dimensional spin glasses. Though it was developed more than a decade ago, many of its predictions have remained to be clarified.

Recently, anomalous low energy and large scale excitations were found LEE  in active studies of spin-glass models at $`T=0`$. In the present letter, we develop a refined scenario for isothermal aging in spin glasses where such anomalous low energy excitations play a significant role. Most importantly, it explains the fundamental experimental observation that the field cooled (FC) susceptibility is larger than the zero field cooled (ZFC) susceptibility Uppsala ; Saclay . Such an anomaly was reproduced successfully in the dynamical MFT but not in the conventional droplet theory. To simplify notations, we discuss systems of $`N`$ Ising spins $`S_i=\pm 1`$ ($`i=1,\mathrm{},N`$) in a $`d`$-dimensional space coupled by short-ranged interactions of energy scale $`J`$ with random signs with no ferromagnetic or anti-ferromagnetic bias. Extension to other types of spin glasses can be done straightforwardly.

Fisher and Huse FH2  noticed that droplet excitations can be softened in the presence of a frozen-in defect or domain wall compared with ideal equilibrium with no extended defects. This is because droplets which touch the defects can reduce the excitation gap compared with those in equilibrium. Let us consider system with a frozen-in defect of size $`R`$: a large droplet of size $`R`$ is flipped with respect to $`\mathrm{\Gamma }`$, which is a ground state of an infinite system, and then it is frozen. The typical free-energy gap $`F_{L,R}^{\mathrm{typ}}`$ of a smaller droplet of size $`L`$ in the interior of the frozen-in defect is expected to scale as

$$F_{L,R}^{\mathrm{typ}}=\mathrm{{\rm Y}}_{\mathrm{eff}}[L/R](L/L_0)^\theta L<R$$
(1)
with $`L_0`$ being a certain microscopic length scale and $`\mathrm{{\rm Y}}_{\mathrm{eff}}[L/R]`$ being an effective stiffness which is only a function of the ratio $`y=L/R`$. We assume as usual that the probability distribution of the free-energy gap $`F_{L,R}`$ follows the scaling form $`\rho (F_{L,R})dF_{L,R}=\stackrel{~}{\rho }(F_{L,R}/F_{L,R}^{\mathrm{typ}})dF_{L,R}/F_{L,R}^{\mathrm{typ}}`$ with non-vanishing amplitude at the origin $`\stackrel{~}{\rho }(0)>0`$ which allows marginal droplets.

For $`y1`$, $`\mathrm{{\rm Y}}_{\mathrm{eff}}[y]`$ will decrease with $`y`$ as FH2

$$\mathrm{{\rm Y}}_{\mathrm{eff}}[y]/\mathrm{{\rm Y}}=1c_vy^{d\theta }\text{for}y1.$$
(2)
Here $`\mathrm{{\rm Y}}`$ is the original stiffness constant $`\mathrm{{\rm Y}}=\mathrm{{\rm Y}}_{\mathrm{eff}}(0)`$. A basic conjecture, on which our new scenario based, is that at the other limit $`y1`$ the effective stiffness vanishes as,

$$\mathrm{{\rm Y}}_{\mathrm{eff}}[y]/\mathrm{{\rm Y}}(1y)^\alpha y1$$
(3)
with $`0<\alpha <1`$ being an unknown exponent, and that the lower bound for $`F_{L,R}^{\mathrm{typ}}`$ should be of order $`J`$, say $`F_0`$.

In spin glasses of finite sizes $`R`$, it is likely that the existence of boundaries will intrinsically induce certain defects as compared with infinite systems NS ; M99 ; KYT . Then droplet excitations as large as the system size itself $`LR`$ may be anomalously soft as conjectured above. Such an anomaly is indeed found in recent studies LEE . It explains the apparently non-trivial overlap distribution function $`P(q)`$ found in numerous numerical studies of finite size systems low-temp-MC . Although there new exponent $`\theta ^{}=0`$ was conjectured LEE , we consider it better to attribute this to the zero stiffness constant $`\mathrm{{\rm Y}}_{\mathrm{eff}}[1]=0`$ as in (3). The stiffness exponent $`\theta >0`$, on the other hand, is associated with a defect in $`\mathrm{\Gamma }`$ as we adopt in (1).

To explain the consequence of our conjecture above introduced, let us consider thermal fluctuations and magnetic linear responses of droplet excitations of size $`L`$ within the frozen-in defect at scale $`R`$. Each droplet excitation will induce a random change of the magnetization of order $`M_Lm\sqrt{(L/L_0)^d}`$ where $`m`$ is the average magnetic moment within a volume of $`L_0`$. The thermal fluctuation can be measured by an order parameter $`q=N_d^1_iS_i^2`$ where the sum runs over sites in the interior of the frozen-in defect which contains $`N_d(R/L_0)^d`$ spins. The magnetic linear response by weak external magnetic field $`h`$ is measured by a linear susceptibility $`\chi =N_d^1_iS_i_h/h`$ where $`_iS_i_h`$ is the induced magnetization by the field. In the absence of any droplet excitations, $`q=1`$ holds due to the normalization of spins. The reduction from $`1`$ due to a droplet excitation at scale $`L`$ is of order $`M_L^2\stackrel{~}{\rho }(0)(k_\mathrm{B}T/F_{L,R}^{\mathrm{typ}})`$ with $`k_\mathrm{B}`$ being the Boltzmann constant. Correspondingly, the induced magnetization of droplets by $`h`$ at scale $`L`$ is of order $`M_L\stackrel{~}{\rho }(0)(hM_L/F_{L,R}^{\mathrm{typ}})`$.

Let us construct a toy droplet model FH1  defined on logarithmically separated shells of length scales $`L/L_0=a^k<R/L_0`$ with $`a>1`$ and $`0kn_2n_1`$ where $`R/L_0=a^{n_1}`$ and $`L_\mathrm{m}/L_0=a^{n_2}`$. For each shell an optimal  droplet is assigned whose free-energy gap is minimized within the shell. Then $`F_{L,R}^{\mathrm{typ}}`$ will be of order $`F_0`$ at the shell $`k=n_1`$ so that we have $`F_{L,R}^{\mathrm{typ}}=F_{L,R}^{\mathrm{typ}}(1\delta _{k,n_1})+F_0\delta _{k,n_1}`$. For simplicity, droplets at different scales are assumed to be independent from each other. Replacing the sum $`_{k=0}^{n_2}`$ by an integral $`_{L_0}^{L_\mathrm{m}}𝑑L/L`$ we obtain,

$`1q(L_\mathrm{m},R)=k_\mathrm{B}T\chi (L_\mathrm{m},R)=\stackrel{~}{\rho }(0)m^2k_\mathrm{B}T\times `$
$`{\displaystyle _{L_0}^{L_\mathrm{m}}}{\displaystyle \frac{dL}{L}}\left[{\displaystyle \frac{1\mathrm{\Delta }_a(\mathrm{ln}(L/R))}{F_{L,R}^{\mathrm{typ}}}}+{\displaystyle \frac{\mathrm{\Delta }_a(\mathrm{ln}(L/R))}{F_0}}\right].`$ (4)
where $`\mathrm{\Delta }_a(z)`$ is a pseudo $`\delta `$-function of width $`\mathrm{ln}a`$ note . Note that the fluctuation dissipation theorem (FDT) is satisfied.

It is useful to consider assymptotic behaviour at large sizes $`R/L_01`$ with the ratio $`x=L_\mathrm{m}/R`$ being fixed. We obtain for $`0<x1`$,

$$q(xR,R)=q_{\mathrm{EA}}+\frac{\stackrel{~}{\rho }(0)m^2k_\mathrm{B}T}{\mathrm{{\rm Y}}(R/L_0)^\theta }A(x)\frac{\stackrel{~}{\rho }(0)m^2k_\mathrm{B}T}{F_0}\mathrm{\Theta }_a(\mathrm{ln}x)$$
(5)
with $`\mathrm{\Theta }_a(z)`$ being a pseudo step-function of width $`\mathrm{ln}a`$ note  and $`A(x)=_x^{\mathrm{}}𝑑yy^{1\theta }_0^x𝑑yy^{1\theta }(\mathrm{{\rm Y}}/\mathrm{{\rm Y}}_{\mathrm{eff}}[y](1\mathrm{\Delta }_a(\mathrm{ln}y))1).`$ Note that the second integral converges because of (2) and the inequality $`\theta <(d1)/2`$ FH1 . Here $`q_{\mathrm{EA}}`$ is the usual Edwards-Anderson (EA) order parameter evaluated in the absence of any extended defects as

$$q_{\mathrm{EA}}\underset{L_\mathrm{m}\mathrm{}}{lim}\underset{R\mathrm{}}{lim}q(L_\mathrm{m},R)=1c\stackrel{~}{\rho }(0)m^2\frac{k_\mathrm{B}T}{\mathrm{{\rm Y}}}$$
(6)
with $`c=_1^{\mathrm{}}𝑑yy^{1\theta }`$. The order of the limits is crucial. Thus as far as $`0<x<1`$, the order parameter converges to the equilibrium EA order parameter $`q_{\mathrm{EA}}`$ in the large size limit. The associated equilibrium susceptibility $`\chi _{\mathrm{EA}}`$ is defined as $`k_\mathrm{B}T\chi _{\mathrm{EA}}1q_{\mathrm{EA}}`$.

In the intriguing case $`x1`$, $`A(x)`$ will remain finite as far as $`0<\alpha <1`$. At $`x1`$ the last term of (5) contributes and we obtain,

$`q(R,R)=q_\mathrm{D}+\stackrel{~}{\rho }(0)m^2{\displaystyle \frac{k_\mathrm{B}T}{\mathrm{{\rm Y}}(R/L_0)^\theta }}A(1),`$ (7)
where we have defined the dynamical order parameter

$$q_D\underset{R\mathrm{}}{lim}q(R,R)=q_{\mathrm{EA}}\stackrel{~}{\rho }(0)m^2\frac{k_\mathrm{B}T}{F_0}.$$
(8)
This is one of the main results of the present work. Naturally, we can define the associated dynamical linear susceptibility $`\chi _\mathrm{D}`$ as $`k_\mathrm{B}T\chi 1q_D`$. As we discuss below $`q_\mathrm{D}`$ and $`\chi _\mathrm{D}`$ play significantly important role in the dynamical observables of aging.

We are ready to consider a simple isothermal aging protocol: the temperature is quenched cooling rate  at time $`t=0`$ to a temperature $`T`$ below its transition temperature $`T_c`$ from above $`T_c`$ and the relaxational dynamics i.e., aging is monitored. The dynamical magnetic susceptibility is generally defined as $`\chi (t,t_\mathrm{w})=N^1M(t)/h`$ where $`M(t)`$ is the total magnetization measured at time $`t`$ and field $`h`$. In the thermoremanent magnetization (TRM) measurement the field is switched on for a waiting time $`t_\mathrm{w}`$ and then cut off: $`h(t)=h\theta (t_\mathrm{w}t)`$. On the other hand, in the ZFC magnetization measurement, the field is switched on after the waiting time: $`h(t)=h\theta (tt_\mathrm{w})`$. We denote the susceptibilities of these protocols as $`\chi _{\mathrm{TRM}}(t,t_\mathrm{w})`$ and $`\chi _{\mathrm{ZFC}}(t,t_\mathrm{w})`$. Another important quantity is the magnetic autocorrelation function, $`C(t,t_\mathrm{w})=N^1M(t)M(t_\mathrm{w})=N^1_iS_i(t)S_i(t_\mathrm{w})`$. The last equation follows in the absence of ferromagnetic or anti-ferromagnetic bias.

Within the droplet picture, aging proceeds by coarsening of domain walls FH2  as usual phase ordering processes B94 . Following FH2 , the whole process may be divided into epochs such that the typical size of the domain is $`L_0,aL_0,a^2L_0,\mathrm{},a^nL_0,\mathrm{}`$. At each epoch, droplets of various sizes up to that of the domain can be thermally activated or polarized by the magnetic field. Importantly the domain wall serves as the frozen-in extended defect for the droplets and reduces their stiffness constant.

In the droplet picture FH2  all dynamical processes, including both the domain growth and droplet excitations in the interior of the domains, are thermally activated processes which yield a logarithmic growth law of the time dependent length scale $`L(t)`$. In practice, empirical power laws with temperature dependent exponent work as wellKYT ; Uppsala-AC . However, the logarithmic growth law is supported by a recent experiment Uppsala-AC  where the effects of critical fluctuations are considered (see alsoHYT ; Saclay-AC ; YHT ; BB ). In the following, we focus on scaling properties of the two time quantities as functions of the dynamical length scale rather than on the growth law itself.

As far as $`L(\tau )L(t_\mathrm{w})`$, the autocorrelation function and the ZFC susceptibility are related to the generalized order parameter and linear susceptibility defined in (4) as $`C(\tau +t_\mathrm{w},t_\mathrm{w})=q(L(\tau ),L(t_\mathrm{w}))`$ and $`k_\mathrm{B}T\chi _{\mathrm{ZFC}}(\tau +t_\mathrm{w},t_\mathrm{w})=1C(\tau +t_\mathrm{w},t_\mathrm{w})`$ satisfying the FDT. Especially, the equilibrium correlation and response are obtained by taking the limit $`L(t_\mathrm{w})\mathrm{}`$ with fixed $`L(\tau )`$. In this special limit one finds FH2 , $`C_{\mathrm{eq}}(\tau )=q_{\mathrm{EA}}+c\stackrel{~}{\rho }(0)m^2(k_\mathrm{B}T/\mathrm{{\rm Y}})(L(\tau )/L_0)^\theta `$ and

$$\chi _{\mathrm{eq}}(\tau )\underset{t_\mathrm{w}\mathrm{}}{lim}\chi _{\mathrm{ZFC}}(\tau +t_\mathrm{w},t_\mathrm{w})=\chi _{\mathrm{EA}}c\frac{\stackrel{~}{\rho }(0)m^2}{\mathrm{{\rm Y}}(L(\tau )/L_0)^\theta }.$$
(9)
In the quasi-equilibrium regime $`L(\tau )<L(t_\mathrm{w})`$ waiting time dependence or violation of TTI (Time translational invariance) is present in a weak manner as correction terms to the ideal equilibrium behavior (9). The scaling form of the correction terms can be found using (2) which is relevant for relaxation of AC susceptibilities FH2 ; Uppsala-AC . Actually it allows one to set up numerical extrapolations to obtain the ideal equilibrium behavior KYT ; HYT ; YHT . In the limit $`L(t_\mathrm{w})\mathrm{}`$ with $`x=L(\tau )/L(t_\mathrm{w})<1`$ being flexed, we find $`Cq_{\mathrm{EA}}`$ and $`\chi _{\mathrm{ZFC}}\chi _{\mathrm{EA}}`$ (see Fig. 1). Much stronger violation of TTI shows up below $`q_{\mathrm{EA}}`$.

In the crossover regime $`L(\tau )L(t_\mathrm{w})`$, the anomalously soft droplets as large as the size of the domain $`L(t_\mathrm{w})`$ are also needed to be taken into account. From (7) we immediately find, $`C(\tau +t_\mathrm{w},t_\mathrm{w})|_{L(\tau )L(t_\mathrm{w})}q_\mathrm{D}+A(1)\stackrel{~}{\rho }(0)m^2(k_\mathrm{B}T/\mathrm{{\rm Y}})(L(t_\mathrm{w})/L_0)^\theta `$ where $`q_\mathrm{D}`$ is the novel dynamical order parameter we introduced above. Thus as a function of $`x`$, there should be a vertical drop from $`q_{\mathrm{EA}}`$ to $`q_\mathrm{D}`$ at $`x1`$ in the asymptotic limit $`L(t_\mathrm{w})\mathrm{}`$. Correspondingly, the ZFC susceptibility should jump up vertically from $`\chi _{\mathrm{EA}}`$ to $`\chi _\mathrm{D}`$ at $`x1`$ in the same asymptotic limit (see Fig. 1). Such an abruptness will be absent as functions of $`\tau /t_\mathrm{w}`$. Indeed it is well known in experiments Uppsala  that the so called relaxation rate $`S(t)=d\chi _{\mathrm{ZFC}}(\tau +t_\mathrm{w},t_\mathrm{w})/d\mathrm{log}(\tau /\tau _0)`$ has a pronounced peak at around $`\tau t_\mathrm{w}`$.

In the aging regime $`L(\tau )L(t)>L(t_\mathrm{w})`$ we expect,

$$C(t,t_\mathrm{w})q_\mathrm{D}\stackrel{~}{C}\left(\frac{L(t)}{L(t_\mathrm{w})}\right).$$
(10)
Here, following Fisher and Huse FH2 , we assume the scaling function $`\stackrel{~}{C}(x)`$ is related to a probability $`P_\mathrm{s}(L(t)/L(t_\mathrm{w}))`$ that a given spin belongs to the same domain at the two different epochs characterized by $`L(t)`$ and $`L(t_\mathrm{w})`$. It satisfies $`\stackrel{~}{C}(1)=1`$ and $`\stackrel{~}{C}(x)x^\lambda `$ at $`x1`$ with $`\lambda `$ being in the range $`d/2<\lambda <d`$. It should be emphasized that, in contrast to usual domain growth process B94 , we put the dynamical order parameter $`q_\mathrm{D}`$ rather than $`q_{\mathrm{EA}}`$ as the amplitude of $`C(t,t_\mathrm{w})`$ since we obtained $`C(t,t_\mathrm{w})|_{x1}q_\mathrm{D}`$ above.

The ZFC susceptibility in the aging regime becomes,

$`\chi _{\mathrm{ZFC}}(t,t_\mathrm{w})`$ $`\chi (L(\tau ),L(t))`$ (11)
$`+c^{\prime \prime }{\displaystyle _{L(t_\mathrm{w})}^{L(t)}}{\displaystyle \frac{dL}{L}}{\displaystyle \frac{\stackrel{~}{\rho }(0)m^2}{\mathrm{{\rm Y}}(L/L_0)^\theta }}\stackrel{~}{C}\left({\displaystyle \frac{L(t)}{L}}\right)`$
where $`c^{\prime \prime }`$ is a numerical constant. The first term is due to the response of the droplets equilibrated within the temporal domain of size $`L(t)`$ (see (4)). The second term represents contributions from the magnetizations (per spin) of order $`\stackrel{~}{\rho }(0)hm^2/\mathrm{{\rm Y}}(L/L_0)^\theta `$ due to droplets as large as $`L`$ which are induced by the field in the past epochs, say around $`t`$ with $`L(t)=L`$, and are depolarized by further domain growth. We also note that this term but with the integration from $`L_0`$ to $`L(t_\mathrm{w})`$ yields the TRM susceptibility written as FH2  $`\chi _{\mathrm{TRM}}(t=\tau +t_\mathrm{w},t_\mathrm{w})c_{\mathrm{nst}}\stackrel{~}{\rho }(0)m^2/\mathrm{{\rm Y}}(L(t_\mathrm{w})/L_0)^\theta (L(t)/L(t_\mathrm{w}))^\lambda `$ with $`c_{\mathrm{nst}}=c^{\prime \prime }_0^1𝑑yy^{1\theta +\lambda }>0`$. These susceptibilities satisfy the sum rule $`\chi _{\mathrm{ZFC}}(t,t_\mathrm{w})+\chi _{\mathrm{TRM}}(t,t_\mathrm{w})=\chi _{\mathrm{ZFC}}(t,0)`$ which must hold for linear responses.

In the special limit of $`t_\mathrm{w}=0`$ we obtain,

$`\chi _{\mathrm{ZFC}}(t,0)\chi _\mathrm{D}c^{\prime \prime \prime }{\displaystyle \frac{\stackrel{~}{\rho }(0)m^2}{\mathrm{{\rm Y}}(L(t)/L_0)^\theta }}`$ (12)
with $`c^{\prime \prime \prime }=A(1)c_{\mathrm{nst}}`$. Note that $`\chi _{\mathrm{ZFC}}(t,0)`$ converges to the dynamical susceptibility $`\chi _\mathrm{D}(>\chi _{\mathrm{EA}})`$ in the limit $`t\mathrm{}`$. This implies $`\chi _\mathrm{D}`$ is nothing but the field cooled (FC) susceptibility $`\chi _{\mathrm{FC}}`$ cooling rate , while $`\chi _{\mathrm{EA}}`$ is close to what is called the ZFC susceptibility $`\chi _{\mathrm{ZFC}}`$. Thus we expect the well known experimental observation Uppsala ; Saclay  $`\chi _{\mathrm{FC}}>\chi _{\mathrm{ZFC}}`$ is a dynamical but not a transient phenomenon .

The overall feature of the two time quantities so far discussed is displayed in Fig. 1. Note that a parametric plot of $`C`$ vs $`\chi _{\mathrm{ZFC}}`$ becomes radically different from the conventional picture BCKM ; FMGPP  in which the breaking of FDT and TTI are supposed to happen simultaneously at $`(q_{\mathrm{EA}},k_\mathrm{B}T\chi _{\mathrm{EA}})`$.

Finally let us briefly discuss some numerical results concerning our scenario. We performed Monte Carlo (MC) simulations of isothermal aging of a 4 dimensional EA spin-glass model (size $`24^4`$)with $`\pm J`$ interactions ($`T_c=2.0J`$, with $`k_\mathrm{B}=1`$ here and hereafter) starting from random initial conditions. A set of data of $`1C(\tau +t_\mathrm{w},t_\mathrm{w})`$ and $`(T/J)\chi _{\mathrm{ZFC}}(\tau +t_\mathrm{w},t_\mathrm{w})`$ at $`T/J=0.8`$ is plotted against $`L(\tau )^\theta `$ in Fig. 2. The field of strength $`h/J=0.1`$ was used and the linearity of the responses was checked by the sum rule, $`\chi _{\mathrm{ZFC}}(t,t_\mathrm{w})+\chi _{\mathrm{TRM}}(t,t_\mathrm{w})=\chi _{\mathrm{ZFC}}(t,0)`$. We used $`\theta =0.82`$ obtained by a defect free-energy analysis KH . For the growth law $`L(t)`$, we used the result of an independent measurement of the growth of domain HYT ; YHT . As explained in KYT ; HYT ; YHT  the analysis of the quasi-equilibrium yields the equilibrium limit curve shown at the bottom of the figure (See HYT ). It follows the scaling form (9) pointing toward $`(T/J)\chi _{\mathrm{EA}}0.18`$. The other extreme $`\chi _{\mathrm{ZFC}}(\tau ,0)`$ also becomes linear in this plot as expected in (12) pointing toward $`(T/J)\chi _\mathrm{D}0.34`$ well above $`\chi _{\mathrm{EA}}`$. Apparently FDT ($`(T/J)\chi =1C`$) is well satisfied at small $`\tau `$ and broken at large $`\tau `$. Interestingly enough, the break points of the FDT move further away from $`(T/J)\chi _{\mathrm{eq}}(\tau )`$ suggesting the separation of the breaking of FDT and TTI as we anticipated. Such a feature has not been reported in previous numerical studies FDT-MC .

We also confirmed most of other scaling ansatz of the two time quantities within the 4D EA model which will be presented elsewhere YHT . It will be certainly interesting to test our scenario by experiments such as noise measurements HO  and further numerical simulations.

###### Acknowledgements.

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, Culture, Sports, Science and Technology of Japan. The present simulations have been performed on Fujitsu VPP-500/40 at the Supercomputer Center, Institute for Solid State Physics, the University of Tokyo.