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# Real space origin of temperature crossovers in supercooled liquids

## I Introduction

The aim of this paper is to critically reconsider the physical origin of the onset of dynamical arrest and the associated crossovers between distinct dynamical regimes displayed by liquids supercooled through their melting temperature towards the glass transition Ediger-et-al ; Angell ; Debenedetti-Stillinger ; Debenedetti . We do this by extending the real space theoretical framework based on dynamic facilitation of Refs. Garrahan-Chandler ; Berthier-Garrahan ; Garrahan-Chandler2 ; Berthier  to the moderately supercooled regime corresponding to the region where mode coupling theory (MCT) MCT  supposedly applies, as reviewed in MCT-experiments ; MCT-simulations . This novel approach takes directly into account the spatial aspects of the dynamics, in particular those related to dynamic heterogeneity DHReviews , in contrast with many other theories Debenedetti-Stillinger ; Debenedetti ; MCT . Our analysis shows that the onset of slowing down can be understood in a simple physical way in terms of the dynamical properties of effective excitations, or defects, as a progressive crossover from a regime of fast dynamics dense in defect clusters, to one of slow heterogeneous dynamics dominated by isolated localized defects. We demonstrate that this real space picture explains the observed crossover temperatures, challenges the idea that these crossovers are related to changes in the topography of the energy surface or to MCT singularities, and is able to account for the apparent correlations observed between “landscape” and dynamical properties.

The paper is organized as follows. In the rest of the Introduction we review the MCT and energy landscape points of view, discuss their problems and limitations, and describe the alternative real space perspective we will pursue. In Section II we develop the physical picture of the onset of slowing down and dynamical crossovers which emerges from our theoretical approach. In Section III we discuss its quantitative consequences and compare them to published numerical results. In Section IV we show how our approach also enables to derive the observed properties of the potential energy landscape of supercooled liquids. Finally, in Section V we discuss our results and state our conclusions.

### I.1 MCT/landscape scenario…

It is often assumed that the initial slowing down of the dynamics of supercooled liquids can be rationalized by MCT Ediger-et-al ; Angell ; Debenedetti-Stillinger ; Debenedetti ; MCT-experiments ; MCT-simulations . Numerical simulations are now able to investigate the first five decades in time of this slowing down MCT-simulations , so this is also the regime which has been studied in greatest microscopic detail. The degree of success of MCT is still a matter of debate. This is due to the fact that the central MCT prediction, a complete dynamical arrest at a temperature $`T_c`$ where the alpha-relaxation time diverges as a power law, $`\tau _\alpha (T)(TT_c)^\gamma `$, is actually never observed, but a power law fit to the data apparently works on a restricted time window MCT-experiments ; MCT-simulations . The appearance of new mechanisms for relaxation, often termed “activated processes”, but seldom described in any detail, is then invoked to explain the discrepancy between observations and MCT predictions. In fact, activated processes are actually quantitatively defined, within MCT, by deviations between data and predictions MCT-simulations ; Kob-Andersen ; thomas . It is believed that activated processes become relevant close to the dynamical singularity $`T_c`$, their main effect being to prevent the predicted transition.

From $`T_c`$ downwards it is assumed that the physics is dominated by activated processes, which determine also the canonical features of glass transition phenomena kivtar2 : non-exponential relaxation, strong and fragile liquid behaviours, decoupling between transport coefficients, etc. It is sometimes said that the relevant physics for the glass transition sets in at $`T_c`$, and is therefore out of reach of numerical simulations Donth . Crossovers into the activated dynamics regime are also reported to occur at temperatures $`T_x`$ Rossler-Sokolov  or $`T_B`$ Stickel-et-al , depending on which aspect of the physics is considered. It is believed that all these temperatures are close enough to be taken as equivalent, $`T_cT_xT_B`$ Angell-10Q .

The above scenario is apparently corroborated by the study of the statistical properties of the potential energy landscape of model liquids Goldstein ; Stillinger-Weber ; Stillinger ; Debenedetti-Stillinger . From the properties of the landscape two temperatures seem to emerge, $`T_o`$ and $`T_c`$ Sastry-et-al . The onset of slowing down of the dynamics takes place at $`T_o`$, and coincides with the temperature below which the average energy of inherent structures (IS), i.e., local minima of the potential energy Stillinger-Weber , $`e_{IS}(T)`$, starts to decrease markedly, see Fig. 1. This has been interpreted as the sign that the landscape starts to “influence” the dynamical behaviour Sastry-et-al . At $`T_c`$, it is further argued, a second change in the landscape properties takes place, which is indicated by several observations Sastry-et-al ; Buchner-Heuer1 ; Buchner-Heuer2 ; schroder ; jund ; keyes1 ; boson . For example, the mean-square displacement from an equilibrated configuration to its corresponding inherent structure, $`N^1_i(𝐫_i𝐫_i^{(\mathrm{IS})})^2`$, is proportional to $`T`$ below $`T_c`$, as expected from pure vibrations in quadratic wells, but the temperature dependence changes above $`T_c`$, revealing “anharmonicities” in the landscape Sastry-et-al ; Buchner-Heuer1 , see Fig. 1.

Another indication of a topological change in the energy landscape was discussed in Ref. Cavagna , in analogy with what happens in mean field models Kurchan-Laloux ; Cavagna-et-al : the vanishing as $`T`$ approaches $`T_c`$ of the mean intensive number of negative directions (intensive index) of stationary points of the potential energy, $`n_s(T)`$. Numerical simulations Broderix-et-al ; Angelani-et-al ; saddle2 ; doye ; stariolo ; dh2  found that $`n_s(T)`$ decreases with decreasing $`T`$, and fits were performed to show that $`n_s(T_c)=0`$ Broderix-et-al ; Angelani-et-al ; saddle2 . The physical interpretation of this result is the apparent existence at $`T_c`$ of a “geometric transition” between a “saddle dominated regime” above $`T_c`$ and a “minima dominated regime” below $`T_c`$ Cavagna2 . $`T_c`$ would then really coincide with the appearance of activated processes, described in a topographic language as “hopping” between minima of the landscape. Analogous findings had been previously reported from instantaneous normal mode analysis of equilibrium configurations laird , also supporting a qualitative change in the landscape topology close to $`T_c`$ INM ; keyes2 .

Figure 1 summarizes this MCT/landscape scenario with published numerical data Kob-Andersen ; kobsciortino ; Sastry-et-al  obtained for the standard supercooled liquid model of Ref. Kob-Andersen .

### I.2 … and its problems and contradictions

At first sight Fig. 1 appears as convincing evidence in favour of the MCT/landscape interpretation of the dynamics. On closer inspection, however, the above scenario is less robust. Several qualitative and quantitative observations do not fit into the picture presented above.

(i) Activated dynamics above $`T_c`$. The main idea behind the landscape approach Goldstein  is that vibrations and structural relaxations take place on very different time scales, so that the system is “trapped” and vibrates in one minimum before “hopping” to another minimum. This is indeed observed using the mapping from trajectories to IS Stillinger-Weber  in simulations of sufficiently small systems Doliwa-Heuer ; Denny-et-al . We have also discussed theoretically this issue in a recent work Berthier-Garrahan . Given that numerical studies were performed much above $`T_c`$, a crucial conclusion of Refs. Doliwa-Heuer ; Denny-et-al ; Berthier-Garrahan  is that “activated dynamics” is indeed present in this temperature regime.

(ii) Heterogeneous dynamics above $`T_c`$. It is now well-documented that the dynamics of supercooled liquids, even above the mode coupling temperature $`T_c`$, is heterogeneous in the sense that the local relaxation time has non-trivial spatial correlations Glotzer . This phenomenon is not very different from what happens experimentally close to the glass transition $`T_g`$ DHReviews . Besides, the decoupling between transport coefficients, which is also interpreted in terms of dynamical heterogeneity DHReviews ; kivtar3 , is observed in numerical simulations above $`T_c`$ Kob-Andersen , although the effect is quantitatively less pronounced than in experiments near $`T_g`$ gilles1 .

(iii) Presence of saddles below $`T_c`$. Despite claims based on numerical results that $`T_c`$ marks a real change in the topology of the landscape Angelani-et-al ; Broderix-et-al ; saddle2 , there are strong indications that this is at best only a crossover doye ; stariolo , and at worst a biased interpretation of numerical data dh2 . For instance, careful numerical studies have shown that the saddle index $`n_s(T)`$ remains positive even below $`T_c`$ doye . Moreover, Ref. dh2  argues convincingly that the data for $`n_s(T)`$ can be described by an Arrhenius law, $`n_s(T)\mathrm{exp}(E/T)`$, with $`E`$ an energy scale, which means that $`T_c`$ does not mark any particular change in the saddle index.

### I.3 Alternative: real space physics and coarse-grained models

The problems described above can be overcome through an alternative perspective on glass transition phenomena which puts the real space aspects of the dynamics at its core. This is the approach developed in Refs. Garrahan-Chandler ; Berthier-Garrahan ; Garrahan-Chandler2 ; Berthier . Interestingly, several of its central concepts, like the relevance to the dynamics of localized excitations Glarum ; Anderson  and the importance of effective kinetic constraints Fredrickson-Andersen ; Palmer-et-al , have been present in the literature for many years. Moreover, one of the original key observations of dynamic heterogeneity in glass formers was made by Harrowell and coworkers Harrowell  in the models of Ref. Fredrickson-Andersen . See Ref. Ritort-Sollich  for an exhaustive review.

Our approach relies on only two basic observations. (i) At low temperature mobility within a supercooled liquid is sparse and very few particles are mobile. This is somewhat equivalent to the statement that particles are “caged” for long period of times, as reflected by a plateau in the mean-square displacement of individual particles. (ii) When a microscopic region of space is mobile it influences the dynamics of neighbouring regions, enabling them to become mobile, and thus allowing mobility to propagate in the system. This is the concept of dynamic facilitation Anderson ; Fredrickson-Andersen . The observation that very mobile particles in a supercooled liquid move along correlated “strings” Glotzer  is a confirmation of this fundamental idea.

From these two concepts it is possible to build effective microscopic models for glass formers by means of a coarse-graining procedure. This procedure can be schematically described as follows Garrahan-Chandler2 . Spatially, the particles are coarse-grained over a length scale $`\delta x`$ of the order of the static correlation length given by the pair correlation function. This removes any static correlations between coarse grained regions of linear size $`\delta x`$. Cells are then identified according to their mobility by performing a coarse-graining on a microscopic time scale $`\delta t`$. In its simplest version cells are identified by a scalar “mobility field”, $`n(𝐫,t)=0,1`$, the values $`0/1`$ corresponding to an immobile/mobile cell at position $`𝐫`$ and time $`t`$. The next step is to replace continuous space by a lattice, $`n(𝐫,t)n_i(t)`$. Mobile or excited cells carry a free energy cost, so when mobility is low it is reasonable to describe their static properties with a non-interacting Hamiltonian Fredrickson-Andersen ,

$$H=\underset{i=1}{\overset{N}{}}n_i,$$
(1)
for a lattice of $`N`$ sites. The link between mobility and potential energy Garrahan-Chandler  has also been observed in numerical simulations Glotzer .

The coarse-graining procedure described above will generate local dynamical rules for the mobility field. The prominent feature of this dynamics will be dynamic facilitation, which in its simplest version states that a cell at site $`i`$ is allowed to move only if it has an excited nearest neighbour Fredrickson-Andersen ,

$$n_i=0\begin{array}{c}\stackrel{𝒞_ic}{}\\ \underset{𝒞_i\left(1c\right)}{\overset{}{}}\end{array}n_i=1,$$
(2)
where $`𝒞_i=1_{j,i}(1n_j)`$, and $`j,i`$ indicates nearest neighbour, and $`c`$ represents the average concentration of excited cells easily deduced from (1):

$$c(T)n_i=(1+e^{1/T})^1.$$
(3)
Explicit examples where dynamic facilitation is generated under coarse-graining can be found in Ref. Garrahan-Newman . Clearly, different models are defined simply by changing the kinetic rules, e.g., the number or directionality of mobile neighbours required to move Ritort-Sollich . Also, a more complex mobility field may be required to account quantitatively for all glass transition features Garrahan-Chandler2 .

Crucially, we will show that the physical mechanisms which explain the onset of slowing down and crossovers between different dynamical regimes in supercooled liquids are generic to this class of models. This means that we can use the simplest of them, the Fredrickson-Andersen (FA) model defined by Eqs. (1,2) in one spatial dimension (hereafter 1D FA model) to make detailed predictions and calculations.

## II Physical picture of dynamic crossovers

In order to understand the physics captured by the coarse-grained facilitated models defined above, it is useful to look at trajectories, that is, space-time representations of the dynamics Garrahan-Chandler . We show in Fig. 2 three representative trajectories for the 1D FA model, where mobile cells (defects) are black, and immobile ones are white. From the trajectories, the principal observation is the appearance at low temperatures of non-trivial spatio-temporal correlations, seen as spatially and temporally extended domains of immobile cells delimited by isolated defects Garrahan-Chandler . In 1D they look like “bubbles” Berthier-Garrahan , and trajectories are dense assemblies of these slow bubbles. This nanoscopic ordering in trajectory space is the cause of the phenomenon of dynamic heterogeneity observed experimentally and in simulations Garrahan-Chandler . Dynamic heterogeneity is the central aspect of the physics of supercooled liquids: it is naturally captured by our approach.

The statistical mechanics of trajectories, rather than configurations, determines the dynamical behaviour. For example, due to the non-interacting Hamiltonian (1), static correlations are trivial. However, when trajectories are considered, it is clear that cells become dynamically correlated. In other words, these models naturally predict the existence of a dynamical correlation $`\mathrm{}(T)`$ which grows when the dynamics slows down. This statement can be quantified Garrahan-Chandler ; Berthier ; silvio ; doliwa  by studying multi-point functions, for example, $`C(|ij|,t)=P_i(t)P_j(t)P_i(t)P_j(t)`$, where $`P_i(t)`$ is a dynamical correlator at site $`i`$ (below we will consider the persistence of site $`i`$). The spatial decay of a function like $`C(|ij|,t)`$ defines unambiguously the dynamical correlation length $`\mathrm{}(T)`$, as already discussed theoretically Garrahan-Chandler ; Berthier ; silvio  and measured in numerical simulations silvio ; Glotzer ; doliwa ; harro2 ; length . Furthermore, the joint distributions of time and length scales give rise to the canonical features of glass formers, like stretched relaxation, decoupling between transport coefficients, and (kinetic and thermodynamic) strong and fragile behaviours Garrahan-Chandler ; Berthier-Garrahan ; Garrahan-Chandler2 .

Let us take a closer look at the temperature evolution of the trajectories in Fig. 2. Starting from the very low temperatures where trajectories consist of a mixture of slow bubbles, the dynamics can be understood in terms of the opening and closing of bubbles, that is, the branching of an excitation line or the coalescence of two. As shown in Berthier-Garrahan , these events are the “hopping between minima” described in Ref. Goldstein . Therefore, we have a clear understanding of “activated processes” and of their statistical properties Berthier-Garrahan .

As temperature is increased more and more defects are present. This has several consequences. First, the typical spatial and temporal extension of bubbles reduces, that is, the system becomes faster and less heterogeneous. Second, clusters of defects become more common. These objects are important because their dynamics is completely different from that of isolated defects. In a cluster, defects do not have to diffuse and create or annihilate other defects but can instantaneously relax in a much faster process. At high temperature, the dynamics is fast because almost no bubbles are present, and the dynamics is governed by clusters of defects. Interestingly, at some intermediate temperature (middle frame in Fig. 2) a coexistence between clusters and isolated defects is observed, so that the dynamics has a “mixed” character.

Clusters of defects disappear much faster with decreasing temperature than the overall concentration of defects. The probability to have a cluster of $`k`$ defects is indeed $`p(k)c^k`$, so that at low $`T`$ we have $`p(1)p(2)\mathrm{}`$.

The coexistence of fast and slow processes with different temperature behaviour has a direct influence on the distribution of local relaxation times, which we present in Fig. 3 for various temperatures. At high temperature, $`T1.0`$, where fast processes are dominant, the distribution is exponential, with a mean which depends weakly on temperature (below we discuss in detail its temperature dependence). Around $`T=1.0`$, a shoulder develops in the large time tail of the distribution, corresponding to the appearance of the bubbles in the trajectories of Fig. 2. This marks the increasing relevance of slow processes and the growth of the dynamic correlation length beyond the microscopic high temperature value. This temperature corresponds therefore to the onset temperature, $`T_o=1.0`$.

Decreasing further the temperature, we clearly see a regime of mixed dynamics. At $`T=0.6`$, for instance, there are two peaks in the distribution, reflecting the coexistence of clusters and isolated defects. At this temperature, the time scale has already increased by several orders of magnitude, and the dynamic correlation length is about $`\mathrm{}(T=0.6)c^1(T=0.6)6`$.

Finally, further decrease in temperature makes clusters of defects very rare and we are left only with the contribution of isolated defects. This low temperature distribution is the one discussed in Refs. Garrahan-Chandler ; Berthier-Garrahan , which in turn implies the stretched exponential decay of dynamical correlators. The contribution of clusters becomes negligible beyond a second crossover temperature, here $`T_c=0.3`$. While this crossover temperature is not linked in any way to the mode coupling singularity $`T_c`$, this choice of notation will become clear shortly.

From these distributions, it is possible to propose an empirical but quantitative determination of $`T_o`$ and $`T_c`$. At each temperature $`T`$, the distribution is composed of fast processes, $`\tau <\tau _{}(T)`$, and slow processes, $`\tau >\tau _{}(T)`$, where $`\tau ^{}(T)`$ can be defined, e.g., as in Ref. heuer . Requiring that slow processes are a significant fraction (say 90%) of the distribution leads to the definition of $`T_c`$:

$$_{\tau _{}(T_c)}^{\mathrm{}}d\tau ^{}\pi (\tau ^{})=0.9,$$
(4)
where in an abuse of notation we also call $`\pi (\tau )`$ the distribution of persistence times. Requiring that slow processes, while not dominant in number, still contribute to a significant fraction of the mean relaxation time (say again 90%) leads to the definition of $`T_o`$:

$$_{\tau _{}(T_o)}^{\mathrm{}}d\tau ^{}\pi (\tau ^{})\tau ^{}=0.9\tau .$$
(5)
In Fig. 4, we summarize the physical picture that emerges from the considerations of this section. From the distributions of Fig. 3, we recognize that the dynamics becomes slow when the temperature is decreased below the onset temperature $`T_o`$. This distinguishes the trivial liquid and the slow glassy regimes. From the trajectories of Fig. 2, we were also able to distinguish between fast, non-activated processes (clusters), and slow, activated processes (isolated defects, bubbles). The former, typical of the liquid high-$`T`$ physics, become negligible below $`T_c`$, while the latter, typical of the low-$`T`$ physics, appear at the onset temperature $`T_o`$. As a consequence, the crossover region $`T_c<T<T_o`$ contains traces of both high-$`T`$ and low-$`T`$ physics, as observed in the time distributions of Fig. 3.

## III Quantitative consequences

The physical picture we have presented for the onset of slowing down, based on the increasing relevance of a dynamically heterogeneous evolution of the system, leads to quantitative predictions which are in good agreement with previous numerical and experimental studies, as we discuss in this section.

### III.1 Dynamical correlators

The basic dynamical quantities recorded in experiments and simulations of supercooled liquids are spatially averaged two-time functions. Simulations usually focus on the time domain and typically consider density-density correlation functions, while experimental results are often expressed in the frequency domain, measuring for instance dielectric susceptibilities. We will only consider systems in equilibrium so that the information content of both kinds of measurements is equivalent.

From the distributions of times, Fig. 3, it is easy to derive dynamical correlators for the 1D FA model considered here. The spatially averaged persistence function reads,

$$P(t)=_t^{\mathrm{}}d\tau ^{}\pi (\tau ^{}).$$
(6)
The behaviour of $`P(t)`$ as a function of time for various temperatures is shown in Fig. 5. At very low temperatures, the persistence function is known exactly due to the diffusion properties of isolated defects, and one gets

$$P(t)=\mathrm{exp}\left[\left(\frac{t}{\tau (T)}\right)^\beta \right],$$
(7)
where $`\tau (T)`$ is the relaxation time discussed in the next section. For the 1D FA model, $`\beta =1/2`$, but the stretching exponent might be temperature dependent in more elaborated (fragile) models Berthier-Garrahan ; Ritort-Sollich , as is indeed observed in experiments Ediger-et-al ; Angell .

We see from Fig. 5 that for $`T=0.2`$ and $`0.3`$ $`P(t)`$ is well approximated by Eq. (7) on the whole time window. For higher temperatures, $`T>T_c=0.3`$, the mixed character of the correlators is evident from the fact that Eq. (7) only describes the long time behaviour of the correlator, as expected. In this temperature regime, short times are best described by a simple exponential. In the high temperature regime, $`T>T_o=1.0`$, relaxation is just exponential for all times. We conclude that the appearance of isolated defects at $`T_o`$ is reflected in the long time behaviour of dynamical correlators. In the crossover region, $`T_c<T<T_o`$, more and more of the decorrelation is due to isolated defects when $`T`$ decreases. Below $`T_c`$ the entire decorrelation is due to these slow processes.

A confirmation of the progressive domination of slow over fast processes described above can be found in the numerical results of Ref. schroder . The similarity of Fig. 4 of Ref. schroder  and our Fig. 5 is in fact quite striking. In particular, Ref. schroder  calculated density-density correlations from both real configurations and their corresponding IS in a binary Lennard-Jones mixture. The latter, where thermal energies were removed in the quenching procedure, are the ones which have to be compared with Fig. 5, since fast vibrations are also removed in our coarse-grained approach.

An important conclusion is that the long-time decay of dynamical correlators, sometimes referred to as the alpha-relaxation, is due to the presence of isolated defects and therefore of heterogeneous dynamics, even in the $`T>T_c`$ regime. This means that activated dynamics, in the language of MCT, or hopping events in topographic terms, are responsible for the alpha-relaxation, even at temperatures well above $`T_c`$. This conclusion is unavoidable in view of the numerical data of Refs. schroder ; Doliwa-Heuer ; Denny-et-al .

### III.2 Relaxation time

The next natural quantity to consider, the relaxation time $`\tau (T)`$, is readily obtained from the dynamical correlators discussed in the previous subsection. From the discussion of section II, we expect a crossover from high-$`T`$ to low-$`T`$ at the onset temperature $`T_o`$, see Eq. (5). Our results for the 1D FA model are presented in Fig. 6, where $`\tau (T)`$ is defined as the time where the persistence function has decayed to the value $`1/e`$.

The simplest mean-field approximation to the dynamics of the FA model consists in a Hartree like decoupling of spatial correlations, $`n_in_jn_in_j`$, in the dynamical equation for $`n_i`$. This amounts to replacing the actual neighbourhood of site $`i`$ by an average neighbourhood, and spins are always facilitated with an average rate equal to $`c`$. This gives a mean-field estimate of the relaxation time schulz ,

$$\tau _{\mathrm{MF}}(T)c^1\mathrm{exp}\left(\frac{1}{T}\right).$$
(8)
Fig. 6 shows that this simple approximation accounts for the dependence of the relaxation time at high temperatures, $`TT_o`$.

The exact result for the relaxation time of the 1D FA model is obtained by realizing that isolated defects undergo diffusion with a temperature dependent diffusion constant, $`D(T)c\mathrm{exp}(1/T)`$. The system relaxes when defects have diffused over a distance given by the mean separation between defects, $`c^1`$, so that

$$\tau _{\mathrm{ex}}(T)D^1c^2\mathrm{exp}\left(\frac{3}{T}\right).$$
(9)
This mechanism relies on the notion of dynamic facilitation which implies that local fluctuations of the mobility determine the dynamics, and is essentially beyond reach of any mean-field type of approximation Harrowell . We see from Fig. 6 that Eq. (9) accounts for the behaviour at low temperatures, $`TT_o`$. Figure 6 also presents a fit to the data with an MCT power law form for the relaxation time MCT ,

$$\tau _{\mathrm{MCT}}(T)(TT_c)^\gamma ,$$
(10)
similar to the one obtained in Ref. Fredrickson-Andersen  for the 2-spin facilitated, two dimensional version of the FA model.

From Fig. 6, we draw the following conclusions. The behaviour of the relaxation time changes from the high-$`T`$ to low-$`T`$ behaviour close to the onset temperature $`T_o`$. The combination of simple mean-field at high-$`T`$ with the exact form at low-$`T`$ allows to describe the temperature dependence of the relaxation time over the whole temperature range. However, given that $`\tau (T)`$ smoothly interpolates between these two different functional forms, the MCT power law form, Eq. (10), appears to works reasonably well in a time window of about three decades (see inset in Fig. 6). This range of apparent power-law behaviour is in fact larger than the corresponding one in the canonical binary Lennard-Jones mixture of Ref. Kob-Andersen , where extensive tests of MCT have been performed. Remarkably, we also find that the $`T_c`$ extracted from the power law fit to the relaxation time coincides well with the temperature where fast processes cease to contribute in a significant manner to the distribution of relaxation times, Fig. 3. This explains our choice of notation for the lower crossover temperature, $`T_c`$.

Following the standard MCT reading of the data MCT-simulations ; Kob-Andersen ; MCT-experiments , we would erroneously conclude that activated processes only appear close to $`T_c=0.3`$, since these processes are often tautologically defined by the breakdown of the power law behaviour of the relaxation time MCT-simulations . Figs. 3, 5, and 6, prove instead that activated dynamics starts to be relevant at $`T_o`$, much above $`T_c`$, dominating the alpha-relaxation of the correlators, and hence the relaxation time of the system. The results of this section considerably weaken the possibility of the existence of a temperature regime in supercooled liquids where the relaxation time is correctly described by a power law behaviour. It follows that the standard determination of the location of the MCT “singularity” $`T_c`$ in experiments and simulations is physically unjustified tarjus ; tarjus2 . In fact, the issue of the location of $`T_c`$ has been recently addressed in Ref. reichman , where it was found that for a variety of systems, the temperature $`T_c`$ obtained from the actual MCT equations systematically coincides with the onset temperature $`T_o`$ discussed above.

### III.3 Crossover temperatures

Let us now consider the quantities shown in Fig. 1 as evidence in favour of the MCT/landscape picture in Lennard-Jones mixtures, from the perspective of dynamically facilitated models. In Fig. 7 we show for the 1D FA model a plot analogous to Fig. 1.

The first quantity presented in Fig. 7 is the logarithm of the relaxation time, $`\mathrm{log}\tau (T)`$, as a function of temperature, which we discussed in detail in the previous subsection.

The second quantity shown in Fig. 7 is the average energy of inherent structures, $`e_{IS}`$. For the 1D FA model it can be computed analytically by solving the zero-temperature dynamics of the model ritort ,

$$e_{IS}(T)=ce^c,$$
(11)
where the concentration of defects, $`c`$, is defined in Eq. (3). At high temperature $`e_{IS}`$ changes very slowly. When $`T`$ is reduced below $`T_o`$ the concentration of defects starts to decrease markedly, and $`e_{IS}`$ follows the same trend, as can be seen in Fig. 7. This change in behaviour at the onset temperature $`T_o`$ is due to the appearance of isolated defects, and therefore of a heterogeneous dynamics, and not to any special change of the potential energy surface. This is a very different interpretation of the physics from that of Ref. Sastry-et-al .

The third quantity shown in Fig. 7 is analogous to the distance between a configuration and its nearest IS (see Fig. 1). In the lattice models we are considering the natural quantity to compute is the concentration of sites which change during the descent towards the inherent structure, $`d(T)`$. Since only excited sites can change during this procedure, we get,

$$d(T)=ce_{IS}=c\left(1e^c\right).$$
(12)
Clearly, at low temperature $`dc^2\mathrm{exp}(2/T)`$. This behaviour is physically natural. Contributions to $`d(T)`$ come from clusters of defects, which are the only objects that can relax during the descent to an IS. Since the probability for a cluster of $`k`$ defects, $`p(k)`$, goes as $`p(k)c^k`$, the main non trivial contribution to $`d(T)`$ at low $`T`$ comes from the smallest clusters, $`k=2`$. These relax only one defect in the descent, so that $`dp(2)c^2`$. Moreover, our defect interpretation is consistent with real space observations in simulations of silica jund , where it was found that during the descent to the IS the major contributions to the distance comes from annihilation of localized topological defects of the amorphous structure.

The similarity of Fig. 7 to Fig. 1 is striking. The emerging physical picture is however completely different from the one of the MCT/landscape scenario. For example, while it may appear from the behaviour of $`d(t)`$ above $`T_c`$ that this quantity extrapolates to zero when $`TT_c`$ (see Fig. 7), the exact temperature dependence of $`d(T)`$ is purely Arrhenius. This means that $`T_c`$ has no particular importance \[$`T_c`$ would not look special in a plot of $`d(T)`$ versus $`1/T`$\]. Even if one accepts $`T_c`$ as delimiting two regimes with high and low concentrations of clusters of excitations, this apparent crossover is completely irrelevant as far as the long-time dynamics is concerned. These observations suggest that the crossover at $`T_c`$ from “landscape-influenced” to “landscape-dominated” of Ref. Sastry-et-al  is not physically significant for the alpha-relaxation.

## IV Interpretation of “landscape” properties

In recent years, the potential energy landscape of supercooled liquids has become an object of study per se Debenedetti-Stillinger . In Ref. Berthier-Garrahan , we have developed the idea that the main motivation behind these works was the observation of the separation between fast vibrations and slow hopping processes if sufficiently small systems are considered. This apparently harmless statement on the system size, we argued in Ref. Berthier-Garrahan , results in fact from the central feature of the dynamics of supercooled liquids: “sufficiently small” really means “if the system size is of the order of the dynamical correlation length $`\mathrm{}(T)`$” Buchner-Heuer2 ; Berthier-Garrahan . However, in a purely topographic description of the physics based on the statistical properties of minima, the relevance of the dynamical correlation length is not obvious ribbon . In that sense, a topographic description of the glass transition misses a central aspect of the physics.

We shall show below that using the very simple spatial approach described in previous sections, we can trivially derive the statistical properties of the landscape reported in recent years. This successful confrontation to such an amount of apparently non-trivial and detailed numerical results is again a strong indication of the validity of our approach.

### IV.1 Real space description of “minima” and “saddles”

Reference Berthier-Garrahan  described in detail the connection between the nanoscopic ordering in the trajectories of dynamically facilitated models and the dynamics between IS, “metabasins”, or “traps” observed in numerical simulations or experiments of supercooled liquids. This same approach can be extended to account for the properties of “saddles”, i.e., configurations related to transitions between IS.

Figure 8 zooms on the lowest temperature trajectory of Fig. 2. The top panel of Fig. 8 shows diffusion of isolated defects. It also shows coalescence and branching events, i.e., closing and opening of bubbles. These two kinds of processes correspond to “hopping” events between dynamical “traps” Berthier-Garrahan . Lets consider in detail one of these events, for example the coalescence process enlarged in the bottom left panel of Fig. 8. Isolated defects diffuse by first facilitating one of their neighbours, for instance,

$$101101.$$
(13)
For two defects to coalesce the minimum number of excitations that have to be present when they merge is three:

$$101111011010.$$
(14)
In this sequence, the total number of defects is 2 at the beginning, 3 at the transition, and 1 at the end. This process is schematically described in the bottom right panel of Fig. 8.

In topographic terms, an isolated defect corresponds to a local minimum of the energy, since such a configuration can only evolve by an energy increase, as in (13). On the other hand, a cluster of three excitations corresponds locally to a saddle point, since it is the transition configuration between two minima, as in (14) and Fig. 8. Larger clusters thus correspond to higher order saddles, since the larger the cluster the larger the number of possible moves into minima. The case $`k=2`$ is particular: it is not a minimum since it can relax one defect to decrease its energy, but it is not a saddle either since it does not correspond to a hopping event like that of Fig. 8. Clusters with $`k=2`$ are just ordinary points (i.e., not stationary points) of the landscape. The previous discussion generalizes in a natural way to the whole class of dynamic facilitated systems.

### IV.2 Absence of “geometric transition”

The above identification between the relevant dynamical objects, isolated defects and clusters of defects, and “landscape properties” allows one to compute quantities such as the mean saddle index, $`n_s(T)`$, and the corresponding mean energy of stationary points, $`e_s(T)`$.

The quantities $`n_s`$ and $`e_s`$ were estimated numerically in simulations of supercooled liquids Angelani-et-al ; Broderix-et-al . It was found that both functions decrease when $`T`$ decreases, and extrapolations were performed that indicated $`n_s(T_c)=0`$. Also, plotting the dependence of $`n_s`$ on $`e_se_{IS}`$ parameterized by the temperature, a simple linear relation was obtained, $`n_s(e_se_{IS})`$ Angelani-et-al ; Broderix-et-al ; saddle2 .

In the case of the 1D FA model, it is very simple to devise a procedure to go from an equilibrium configuration to the “nearest” stationary point. Isolated defects and clusters of defects with $`k3`$ are locally such points, so we only have to deal with $`k=2`$ clusters. From these we can either reach a “minimum” $`k=1`$ or a saddle with $`k=3`$. We respectively assign the probabilities $`p_s`$ and $`(1p_s)`$ to these two possibilities. We then have,

$$n_s(T)=\underset{k=1}{\overset{\mathrm{}}{}}p(k)n_s(k),$$
(15)
and

$$e_s(T)=\underset{k=1}{\overset{\mathrm{}}{}}p(k)e_s(k),$$
(16)
where $`p(k)=(1c)^2c^k`$ is the probability to have a cluster of size $`k`$. From the discussion above we know that $`n_s(1)=0`$, $`e_s(1)=1`$, $`n_s(2)=(1p_s)`$, $`e_s(2)=p_s+3(1p_s)`$, $`n_s(k3)=e_s(k3)=k`$. Putting all together we obtain,

$$n_s(T)=3c^2\left[(1p_s)(1c)^2+c\left(1\frac{2}{3}c\right)\right],$$
(17)
and

$$e_s(T)=c+(12p_s)c^2(1c)^2.$$
(18)
At low $`T`$ both quantities scale as $`n_sc^2`$ and $`e_sc`$. Three important conclusions can be drawn:

(i) It is obvious from Eq. (17) that $`n_s(T)>0`$ for $`T>0`$. This means that there is no “geometric transition” to a regime with vanishing saddle index.

(ii) The saddle index has a temperature dependence which follows closely that of the distance $`d(T)`$ discussed in the previous subsection. This is expected because they both receive their principal contribution, at low $`T`$, from clusters with $`k=2`$. In other words, the main objects for the low temperature dynamics, the isolated defects, do not contribute to these quantities. Therefore, as for the distance $`d(T)`$ in Fig. 7, the rapid decrease of $`n_s(T)`$ when the temperature decreases can easily be confused with a vanishing of the saddle index close to $`T_c`$.

(iii) The linear relation between $`n_s`$ and $`e_se_{IS}`$ becomes exact at low temperatures, see Eqs. (11,17,18). Again, the difference between $`e_s`$ and $`e_{IS}`$ comes from the clusters of defects which are relaxed during the descent to the inherent structure. In Fig. 9, we show the behaviour of $`n_s`$ versus $`e_se_{IS}`$ for the entire range $`T[0,\mathrm{})`$. Note that in Ref. Broderix-et-al  a linear behaviour between $`n_s`$ and $`e_s`$ was also reported. This is true at relatively high temperature, given that above $`T_o`$ the energy of inherent structure is almost constant while $`n_s`$ and $`e_s`$ change with temperature in the same way.

These results are valid beyond the FA model which we have used to illustrate them. The inexistence of the geometric transition where the saddle index vanishes follows from the observation that the low temperature behaviour of $`n_s`$ is given by the smallest cluster of defects necessary to make a transition, in the sense described in the previous section. Since these objects are spatially localized, their energy cost is $`O(1)`$, and they exist with non zero probability at finite temperature, $`T>0`$. This argument is close in spirit to Stillinger’s argument for the inexistence of an entropy crisis at the Kauzmann temperature involving point defects still . Moreover, as discussed in the introduction, careful numerical simulations both confirm that $`n_s(T<T_c)>0`$ doye ; stariolo , and report an Arrhenius behaviour $`n_s(T)`$ dh2 , in agreement with our results.

The relation between saddle index and energy,

$$n_s(e_se_{IS}),$$
(19)
which was first observed numerically Angelani-et-al ; Broderix-et-al ; saddle2 , is also a general result for dynamically facilitated systems. This relation contains two different pieces of information. First, it shows that the intensive saddle index is a number of $`O(1)`$. This is again a trivial consequence of the existence of the dynamical correlation length $`\mathrm{}(T)`$, so that a large sample can in fact be thought of an assembly of independent subsystems of linear size $`\mathrm{}(T)`$ Berthier-Garrahan . Second, and more interesting, is a connection between energy and saddle index, presented as a “general feature of the potential energy landscape of supercooled liquids” saddle2 , for which no theoretical explanation was however available. This feature is in fact almost a tautology in the context of facilitated models: the more defects are present, the more available directions to move, the higher the energy above that of the IS. The fact that relation (19) holds in different model liquids is another confirmation that dynamical facilitation is a key generic feature of the dynamics of supercooled liquids.

### IV.3 Thermodynamics and “anharmonicities”

Another common procedure of the landscape approach is to decompose configurations into vibrational and configurational components. Stillinger and Weber Stillinger  suggested to perform this decomposition at the level of the partition function,

$$Z(T)\underset{E_{IS}}{}\mathrm{\Omega }(E_{IS})\mathrm{exp}\left(\frac{E_{IS}+F(T;E_{IS})}{T}\right),$$
(20)
where the sum is over energies of IS, $`E_{IS}`$, their number is indicated by $`\mathrm{\Omega }(E_{IS})`$, and $`F(T,E_{IS})`$ is the “basin free energy” which takes into account fluctuations within an IS due to vibrations and possible “anharmonicities” (i.e., all the rest).

It is instructive to consider the calculation of the partition function in the case of the 1D FA model using the Stillinger and Weber decomposition. The thermodynamics of the FA model is that of a non-interacting gas of binary excitations. This simple thermodynamics, however, can be obtained with any dynamics obeying detailed balance with respect to the Hamiltonian (1), the actual FA dynamics defined by (2) being just one possibility. In this sense, the Stillinger and Weber prescription for thermodynamics is an approximation for the way a thermodynamic quantity would be calculated using a particular choice of dynamics to sample the configuration space. Inherent structures, basin free energies, etc., have no thermodynamic meaning, they only have a dynamical meaning associated with a particular choice of dynamics.

For the 1D FA model we can evaluate the Stillinger and Weber partition function exactly. We have:

$`Z_N(T)`$ $`=`$ $`{\displaystyle \underset{E_{IS}=0}{\overset{N/2}{}}}{\displaystyle \frac{\left(NE_{IS}\right)!}{E_{IS}!\left(N2E_{IS}\right)!}}`$ (21)
$`\times \mathrm{exp}\left({\displaystyle \frac{1}{T}}\left[E_{IS}+F_{\mathrm{anh}}(T;E_{IS})\right]\right).`$
The first factor counts the number of configurations of energy $`E_{IS}`$ with only isolated defects in a system of $`N`$ sites. Due to the coarse-grained nature of facilitated models the only contribution to the basin free energy comes from anharmonicities.

Performing the sum in Eq. (21) without the anharmonic contribution gives,

$$Z_N^{\text{harm}}(T)=\mathrm{exp}\left(\frac{N}{2T}\right)U_N\left[\frac{i}{2}\mathrm{exp}\left(\frac{1}{2T}\right)\right],$$
(22)
where $`U_N(x)`$ is the $`N`$-th Chebyshev polynomial of second kind. In the thermodynamic limit the above expression simplifies to give the free energy in the “harmonic” approximation,

$`f_{\text{harm}}(T)`$ $`=`$ $`\underset{N\mathrm{}}{lim}{\displaystyle \frac{T}{N}}\mathrm{ln}Z_N(T)`$ (23)
$`=`$ $`T\mathrm{ln}2T\mathrm{ln}\left(1+\sqrt{1+4e^{1/T}}\right).`$
In Fig. 10, we compare the approximation (23) to the exact expression for the free energy,

$$f_{\mathrm{ex}}(T)=T\mathrm{ln}\left(1+e^{1/T}\right).$$
(24)
As observed numerically in supercooled liquids Debenedetti-Stillinger , both thermodynamic evaluations, Eqs. (23) and (24), apparently coincide below $`T_c`$ when anharmonicities become negligible. From the previous sections we know that anharmonicities are just a consequence of the existence of clusters of defects. At low temperature the difference between (23) and (24) is therefore proportional to $`c^2`$, reflecting the fact that: (i) anharmonicities do not disappear below $`T_c`$, which again is no particular temperature in this context; (ii) anharmonicities are due to clusters of defects, $`k=2`$ being the leading term at low temperatures.

In the particular case of the FA model we can formulate an exact expression for the anharmonic free energy $`F_{\mathrm{anh}}`$. It is easy to check that the choice

$$F_{\mathrm{anh}}(T;E_{IS})=E_{IS}(T)f_{\mathrm{ex}}(T)$$
(25)
in Eq. (21) yields the exact expression for the free energy in the thermodynamic limit. This exact expression for the anharmonic part of the free energy is simple to understand. In an IS all defects are isolated. The contribution of clusters of defects is obtained from the probability that an isolated defect in the IS was a cluster in the original configuration, which is given by Eq. (25).

Interestingly, a numerical procedure to evaluate the anharmonic contributions can be proposed. First, the harmonic expression (23) is evaluated. Then, the approximate expression

$$F_{\mathrm{anh}}(T;E_{IS})E_{IS}(T)f_{\mathrm{harm}}(T)$$
(26)
can be used as an educated guess for the anharmonic contributions. This gives in turn a first order free energy, $`f_1(T)`$. The improvement on the harmonic evaluation can be judged in Fig. 10, where we see that $`f_1(T)`$ coincides with the exact free energy up to $`TT_o`$. This evaluation can then be improved iteratively using $`F_{\mathrm{anh}}(T;E_{IS})E_{IS}(T)f_1(T)`$ to get $`f_2(T)`$, and so on. It is easy to show that, in our particular case, $`lim_n\mathrm{}f_n(T)=f_{\mathrm{ex}}(T)`$.

Although these results could lead to an improvement on present evaluations of anharmonic contributions in studies of the thermodynamics of supercooled liquids, they also show that topographic concepts are very far from the physical objects they pretend to describe.

### IV.4 Failure of Adams-Gibbs relation

We end this section with a remark on the Adam-Gibbs relation, which is an attempt to connect dynamical properties to thermodynamic ones. The Adam-Gibbs formula relates the relaxation time of a glass former, $`\tau _\alpha `$, to the configurational entropy, $`S_c`$ \[which would correspond to $`S_c=\mathrm{ln}\mathrm{\Omega }(E_{IS})`$ in the IS formalism\]: $`\tau _\alpha \mathrm{exp}\left[1/(TS_c)\right]`$. Apparently, this relation has been seen to hold both in numerical simulations and in experiments of various systems Debenedetti-Stillinger . A careful look at the published data reveals however that the correlation between relaxation time and entropy does not quantitatively satisfy the Adams-Gibbs relation. This important observation is often not clearly stated Debenedetti-Stillinger .

Our analysis shows indeed that thermodynamic properties do not fully determine dynamical behaviours. Clearly, almost by definition, $`\tau _\alpha `$ increases and $`S_c`$ decreases as temperature is lowered, but that is where the connection ends. It is easy to check that the Adam-Gibbs formula fails completely when applied to dynamic facilitated systems. We find instead that time scales are broadly distributed, the distribution of times being the result of an integral over a distribution of length scales scale, $`\rho (\mathrm{})`$, imposed by thermodynamic equilibrium, Eq. (1). Crucially however, dynamics also enters the integral in the form of the conditional probability of time and length, $`\rho (t|\mathrm{})`$, which can be described, in a topographic language as containing informations on the relevant “barriers”, which have a priori no obvious link with the statistics of minima. As a consequence, thermodynamics alone cannot be used to predict the dynamical behaviour. Again, we find in the literature an excellent numerical confirmation of this statement. In Refs dh2 ; heuer , using a purely topographic description of a supercooled liquid, it was shown that the diffusion constant could be computed by a combination of thermodynamic and dynamical quantities, well in line with the above discussion.

## V Conclusions

In this paper, we have developed a spatial description of the physics of the progressive slowing down of supercooled liquids. The only ingredients in our method have been the notions of localized mobility excitations and facilitated dynamics Garrahan-Chandler ; Berthier-Garrahan ; Garrahan-Chandler2 ; Berthier . Our results were illustrated explicitly for the simplest case of the 1D FA model, but are generic for this theoretical approach, and are in very good agreement with experimental and numerical observations in supercooled liquids.

The physical picture which emerges from our work is however markedly different from that of the MCT/landscape scenario discussed in the Introduction.

At high temperatures, $`T>T_o`$, the dynamics is fast and liquid-like, corresponding to the relaxation of large clusters of defects. Dynamic facilitation plays no major role, and a simple mean-field Hartree-like decoupling of the equations of motion yields predictions in good agreement with numerical results.

When $`T<T_o`$, the dynamics becomes heterogeneous, in the sense that local relaxation times are spatially correlated in a non trivial way. This can be seen in the trajectories of Fig. 2 as the appearance of slow bubbles Garrahan-Chandler ; Berthier-Garrahan . The long-time dynamics of the system results from the wide joint distribution of length scales and time scales, and the relaxation becomes stretched. This dynamic heterogeneity, which can be thought of as the activated dynamics invoked, but never described, by MCT, determines the alpha-relaxation and its temperature dependence for $`T<T_o`$. Also, dynamic heterogeneity implies that decoupling of transport coefficients actually starts at $`T_o`$, as confirmed by the simulations. From a theoretical point of view, local fluctuations of mobility crucially influence the dynamical behaviour. Any mean-field like approach, no matter how involved, is most probably doomed to fail.

At $`T_o`$ not all trace of high-$`T`$ physics (clusters of defects) disappears. The dynamics has a mixed character in the range $`T_c<T<T_o`$, as seen for example in the behaviour of dynamical correlators like in Fig. 5. The temperature $`T_c`$ is just a crossover. It is the temperature below which isolated defects not only dominate the long time dynamics (as for $`T_c<T<T_o`$) but are also the most numerous dynamical objects, see Eq. (4). Clusters of defects, whose dynamics is homogeneous and non-activated, are responsible for the temperature dependence of several quantities, such as distance between configurations and IS, saddle index $`n_s(T)`$, and anharmonic contributions to the free energy. In numerical simulations, $`T_c`$ has been interpreted as a key temperature, in accordance with MCT for which it represents a dynamical singularity. We have shown, however, that all of these quantities have a smooth temperature dependence, as has been recently observed numerically doye ; stariolo ; dh2 . This means that $`T_c`$ does not correspond to a transition or singular point, but is at most a crossover. Crucially, the objects which display a crossover close to $`T_c`$ are also irrelevant for the long-time dynamics, so that the inexistence of the singularity $`T_c`$ is anyway not a physically important issue for the alpha-relaxation.

Below $`T_c`$, isolated defects are the only remaining objects and the dynamics is dominated by the nanoscopic demixing of slow and fast regions so that trajectories look like a dense mixture of slow bubbles, which in turn gives a natural theoretical interpretation of the canonical features of glass transition phenomena Garrahan-Chandler ; Berthier-Garrahan ; Garrahan-Chandler2 .

Our results, together with some other recent studies dh2 ; Doliwa-Heuer ; Denny-et-al ; gilles1 ; Harrowell ; heuer ; tarjus ; tarjus2 ; reichman ; Kivelson-et-al , suggest that several essential features of the dynamics of supercooled liquids need to be recognized and we now list some of them.

* The dynamics is heterogeneous and activated well above $`T_c`$.
* The dynamical slowing-down of supercooled liquids is due to the growth, below $`T_o`$, of a dynamic correlation length $`\mathrm{}(T)`$, or more precisely, of a whole distribution of length and time scales.
* The long-time dynamics, and therefore the relaxation time $`\tau _\alpha `$ of the liquid is dominated by heterogeneous “activated” dynamics below $`T_o`$.
* The MCT definition of activated processes as deviations from the ideal theory is incorrect. It is unlikely that the power law behaviour predicted by MCT correctly describes the temperature dependence of $`\tau _\alpha `$. The practical definition of the temperature $`T_c`$ cannot be used.
* No topological change of the potential energy landscape takes place close to $`T_c`$. Quantities such as the saddle index and anharmonicities do not vanish close to $`T_c`$ and have a smooth temperature behaviour. At best, they undergo a crossover from large to small which remains to be quantified.
* Even if one accepts $`T_c`$ as a crossover temperature, as in Eq. (4), quantities related to this crossover are unimportant for the long-time dynamics.
* Knowledge of thermodynamic properties is not enough to predict dynamical behaviour, which explains the quantitative failure of relations like the Adams-Gibbs formula.

The approach we developed in this paper, which is an extension of previous efforts Garrahan-Chandler ; Berthier-Garrahan ; Garrahan-Chandler2 ; Berthier , is generic. It can be applied both to systems like Lennard-Jones liquids or to hard sphere systems. It gives a perspective on the physics of glass formers which is clearly distinct to, and in many respects much more natural than, that of MCT or topographic approaches.

There are many important and interesting open questions which need to be addressed from this new perspective. This include, among others, understanding properly the origin of mobility excitations, and the breakdown of Stokes-Einstein-Debye relations and associated decouplings between transport coefficients.

A general conclusion that can be drawn from this work and our previous ones is that, in many respects, glass transition phenomena is more standard than often assumed, in the sense that it is determined by the interplay between growing dynamic lengthscales and timescales. This is obviously reminiscent of critical phenomena Berthier , meaning that it should be possible to adapt renormalization group techniques to study the dynamics of the glass transition.

###### Acknowledgements.

We are grateful to J.-P. Bouchaud, G. Biroli, A. Buhot, A. Heuer, D.R. Reichman, G. Tarjus, and especially D. Chandler for useful discussions. We acknowledge financial support from CNRS (France), EPSRC Grant No. GR/R83712/01, EU Marie Curie Fellowship No. HPMF-CT-2002-01927, the Glasstone Fund, and Worcester College Oxford. Some of the numerical results were obtained on Oswell at the Oxford Supercomputing Center, Oxford University.


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# REFERENCES

Comment on $`\mathrm{𝐄𝐥𝐞𝐜𝐭𝐫𝐨𝐧}`$ $`\mathrm{𝐒𝐩𝐞𝐜𝐭𝐫𝐚𝐥}`$ $`\mathrm{𝐅𝐮𝐧𝐜𝐭𝐢𝐨𝐧}`$ $`\mathrm{𝐚𝐧𝐝}`$
$`\mathrm{𝐀𝐥𝐠𝐞𝐛𝐫𝐚𝐢𝐜}`$ $`\mathrm{𝐒𝐩𝐢𝐧}`$ $`\mathrm{𝐋𝐢𝐪𝐮𝐢𝐝}`$ $`\mathrm{𝐟𝐨𝐫}`$ $`\mathrm{𝐭𝐡𝐞}`$ $`\mathrm{𝐍𝐨𝐫𝐦𝐚𝐥}`$ $`\mathrm{𝐒𝐭𝐚𝐭𝐞}`$ $`\mathrm{𝐨𝐟}`$
$`\mathrm{𝐔𝐧𝐝𝐞𝐫𝐝𝐨𝐩𝐞𝐝}`$ $`\mathrm{𝐇𝐢𝐠𝐡}`$ $`𝐓_𝐜`$ $`\mathrm{𝐒𝐮𝐩𝐞𝐫𝐜𝐨𝐧𝐝𝐮𝐜𝐭𝐨𝐫𝐬}`$

In a recent Letter , W. Rantner and X.-G. Wen made a theoretical prediction of the power-law behavior of the electron spectral function in the pseudogap phase of underdoped cuprates, reminiscent of that in the one-dimensional Luttinger liquid. This conclusion was drawn on the basis of the following (somewhat heuristic) propositions: 1) the properties of the pseudogap phase are described by the slave-boson $`QED_3`$-like effective theory formulated in terms of neutral spinons $`\psi `$, charged holons, and a gauge field $`A_\mu `$; 2) the propagator of physical electrons $`G_e`$ can be computed as a simple product of the spinon ($`G_s`$) and the holon ($`G_h`$) ones; 3) provided that the holons are (nearly) condensed ($`G_hconst`$), $`G_e`$ becomes proportional to the gauge-invariant spinon amplitude (here $`x_\mu =(t,𝐫)`$ is a position vector in the three-dimensional space-time)

$$G_s(x)=<\psi (x)\mathrm{exp}(i_\mathrm{\Gamma }A_\mu (z)𝑑z^\mu )\overline{\psi }(0)>$$
(1)
with the contour $`\mathrm{\Gamma }`$ chosen as a straight line between the end points; 4) the amplitude (1) decays algebraically, $`G_s(x)1/|x|^{2+\eta }`$, and the anomalous exponent $`\eta `$ is $`positive`$.

It turns out, however, that the value of $`\eta `$ quoted in Ref. and later derived in the original (the only one available at the time of submitting this Comment) version of Ref. had a wrong sign, as was pointed out in Ref. where instead a $`negative`$ value, $`\eta =32/3\pi ^2N`$, was obtained (the number $`N`$ of fermion species in cuprates is $`N=2`$).

In fact, thus far no physically motivated gauge-invariant alternative to Eq.(1) that would exhibit a power-law decay with a positive $`\eta `$ has ever been constructed, and it remains unknown if such a function can exist at all in the pure massless $`QED_3`$. In turn, the negative value of $`\eta `$ disqualifies Eq.(1) introduced in Ref. from being a viable candidate to the role of the gauge-invariant spinon propagator (let alone the physical electron one), because instead of the anticipated $`suppression`$ (as in other examples of doped Mott insulators governed by strong electron correlations), the amplitude (1) manifests $`enhancement`$ as compared to the mean-field ($`N=\mathrm{}`$) result.

The argument appears to be particularly compelling in the limit of zero doping, in which case, while preventing the electrons’ spatial motion by making $`G_e(x)`$ vanish for any $`𝐫\mathrm{𝟎}`$, the holon factor $`G_h(x)`$ does not affect the amplitude $`G_e(t,\mathrm{𝟎})`$ which is directly related to the $`physical`$ electron density of states (DOS) proportional to $`Im𝑑te^{iϵt}G_e(t,\mathrm{𝟎})|ϵ|^{1+\eta }`$. Therefore, a negative $`\eta `$ would have given rise to a sub-linear DOS which is increased with respect to the mean-field ”V-shaped” one.

Thus, taken at its face value, the negative $`\eta `$ invalidates the main prediction of Ref. regarding the Luttinger-like behavior of the electron spectral function $`A(ϵ,𝐩)ImG_e(ϵ,𝐩)`$ which, under the above assumptions, was identified in Ref. with the Fourier transform of Eq.(1). Moreover, once the holon factor $`G_h(x)`$ becomes non-trivial as well, the electron spectral function (now given by a convolution of the Fourier transforms of $`G_s(x)`$ and $`G_h(x)`$) can no longer feature a simple algebraic behavior, unless $`both`$ functions decay as power-law. In the absence of any evidence suggesting otherwise, however, the possibility of such a behavior for the holons seems to be even more remote than for the spinons.

Furthermore, unless proven wrong, the absence of a physically sensible alternative to Eq.(1) in massless $`QED_3`$ may indicate a need for a revision of some of the above propositions which the work of Ref. was based upon. Indeed, albeit obtained in the framework of a perturbative $`1/N`$-expansion, the unphysical behavior of $`A(ϵ,𝐩)`$ derived from Eq.(1) would have manifested itself at all energies/temperatures above a characteristic scale associated with such $`non`$-$`perturbative`$ effects as spinon chiral symmetry breaking, holon condensation, and/or gauge field instantons. At still lower energies/temperatures, however, any of the above mechanisms may generate a finite spinon and/or gauge field gap, thereby drastically altering the power-law decay of Eq.(1), consistent with the anticipated onset of such intrinsic instabilities of the pseudogap phase as antiferromagnetism, superconductivity and/or stripe order.

To conclude, despite its strong intellectual appeal, the $`QED_3`$-theory of underdoped cuprates has not yet provided a firm theoretical support for the Letter’s prediction of the Luttinger-like or $`algebraic`$ (which must be distinguished from both a $`generic`$ non-Fermi liquid, characterized by a mere absence of the quasiparticle peak, and a $`virtually`$ spin-charge separated Fermi liquid which has a small coherent peak at low energies) behavior of the electron spectral function, thus still leaving unsubstantiated the claim of its satisfactory agreement with the normal state photoemission data which was made in Ref. on the basis of the original erroneous evaluation of Eq.(1).

This research was supported by the NSF under Grant DMR-0071362.

$`𝐃.𝐕.\mathrm{𝐊𝐡𝐯𝐞𝐬𝐡𝐜𝐡𝐞𝐧𝐤𝐨}`$
Department of Physics and Astronomy, University of North Carolina, Chapel Hill, NC 27599


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# The StoreGate: a Data Model for the Atlas Software Architecture

## I INTRODUCTION

### Data Objects and Algorithms

The Gaudi software architectureGaudi  belongs to the blackboard familyblackboard : data objects produced by knowledge modules (called Algorithms in Gaudi) are posted to a common “in-memory data base” from where other modules can access them and produce new data objects.

This model greatly reduces the coupling between knowledge modules containing the algorithmic code for analysis and reconstruction, since one knowledge module does not need anymore to know which specific module can produce the information it needs nor which protocol it must use to obtain it (the ”interface explosion” problem described in component software systems). Algorithmic code is known to be the least stable component of software systems and the blackboard approach has been very effective at reducing the impact of this instability, from the Zebra system of the Fortran days to the InfoBus architecture for Java components. The trade-off of the data/knowledge objects separation is the need for knowledge objects to identify data objects to be posted on or retrieved from the blackboard. It is crucial to develop a data model optimized for the required access patterns and yet flexible enough to accommodate the unexpected ones.

### The Transient Data Store

The Transient Data Store (TDS) is the blackboard of the Gaudi architecture: a module creates a data object and post it to the TDS to allow other modules to access it111 to be precise the current TDS implements only a “passive” blackboard, since modules do not react to TDS events (e.g. executing after a data object is registered into the TDS) .

Once an object is posted on to the store, the TDS takes ownership of it and manages its lifetime according to preset policies, removing, for example, a TrackCollection when a new event is read. The TDS also manages the conversion of a data object from/to its persistent form and provides therefore an API to access data stored on persistent media.

## II StoreGate Design and Functionality

StoreGate (SG), in common with most other existing data models, is basically a dictionary of data objects which manages their memory and oversees conversion to/from persistency. The SG design process has been informal and iterative. We released early and often and used developers feedback to adjust our initial design concept222 which was in any case largely based on ideas which have worked in existing data models. The result may lack the coherency of a formal top-down design but it follows a few principles which have proved to be useful.

### Work with User Types

The success of the STL and of other public domain template libraries means that it has become vital to design an open system that can work with generic types that export an interface, in particular the STL containers, rather than forcing data objects to import a common interface. SG adapts its behavior to the functionality each data object exports. The only SG-imposed constraint on a data object333 this does not mean that the data model, simulation and reconstruction groups should not issue design guidelines to ensure that ATLAS data objects behave consistently in terms of memory management and persistability is to be an STL Assignable typeSTL .

### Avoid User-defined Keys

The disadvantage of the data/knowledge objects separation is the need for knowledge objects to identify data objects to be posted on or retrieved from the blackboard. It is crucial to develop a data model optimized for the required access patterns and yet flexible enough to accommodate the unexpected ones.

SG addresses this problem with a two-step approach: it defines a natural identifier mechanism for data objects and it transparently associates to each data object a default value of this identifier allowing developers to register and retrieve data objects without having to identify them explicitly.

The first component of the identifier is the data object type. Experience shows that HEP developers tend to group the objects they work on into collections. As a result the TDS will often contain a single instance of a data object type (say a TrackCollection or several closely related ones (e.g. a TrackCollection for each component of the Inner Detector). The SG retrieve interface covers these two use cases (see Fig. 1).

Type-based identification is not always sufficient. For example the TDS may contain several equivalent instances of a TrackCollection produced by alternative tracking algorithms. Therefore we need to add a second component to our identification mechanism: the identifier of the Algorithm instance that produced the data object we want444 notice that we need to identify the instance rather than the class. In an often quoted use case, clients may want to distinguish among tracks reconstructed by the same tracking algorithm using different jet cone sizes.. In the spirit of working with user types, the SG will allow developers to augment this history identifier with a generic key type optimized for their access patterns.

### Control Object Access and Creation

The TDS is the main channel of communication among modules. A data object is often the result of a collaboration among several modules. SG allows a module to use transparently a data object created by an upstream module or read from disk.

A Virtual ProxyGoF  defines and hides the cache-fault mechanism: upon request555 Currently the proxy uses lazy instantiation (i.e. the object is created only when the handle is dereferenced). , a missing data object instance can be transparently created and added to the TDS, presumably retrieving it from a persistent data-base or, in principle, even reconstructing it on demand.

To ensure reproducibility of data processing, a data object should not be modified after it has been published to the store, we use the same proxy scheme to enforce an “almost const” access policy: modules downstream of the publisher are only allowed to retrieve a constant iterator to the published object.

### Support Inter-object Relationships

SG supports uni-directional inter-objects relationships, or links, and will support bi-directional links in the future. A link is a persistable pointer. If the linked object is a data object then the proxy scheme described above is also used to implement the link. But typically links will refer to objects that are not data objects but are contained within a data object. The SG knows how to get to the container and the container knows how to return an element given its index. The job of the link is to find out the value of the index, persistify it and, later on, pass it on to the container and get back the linked object. In the next section we will discuss how links handle indices into generic containers.

## III Implementation Techniques

A big advantage that SG has compared to earlier data models implementations is that many compilers are catching up with the ISO/ANSI C++ standard. Because of that, a new generation of template libraries like boostboost  and lokiAlexandrescu  are bringing once-esoteric techniques like template meta-programming into the mainstream. Template meta-programming uses the compiler template expansion to control and generate running code based on static type information. In SG we have used some of its simpler techniques.

### Type Traits and Traits Types

The TDS memory management back-end manages the data objects as instances of a DataObject base class. Each class derived from DataObject has a unique ClassID. This allows, for example, to use an Abstract FactoryGoF  to create data object instances when reading from disk. SG wraps each stored data object into a templated DataObject

```
 template <typename DOBJ>
 class DataBucket : public DataObject {...}

```

If DOBJ does not inherit from DataObject we want the developer to define a ClassID for DOBJ that we will associate to the data object.

To determine, at compile time, if DOBJ inherits from DataObject we use the boost type trait boost::is\_base\_and\_derived$`<`$DOBJ,DataObject$`>`$, a template that evaluates to true when DOBJ can be assigned as a DataObjectboost ; Alexandrescu .

To associate the ClassID information to a data object type, say vector$`<`$double$`>`$, we define a ClassID\_traits structure that developers specialize for that data object (the struct is actually generated using a cpp macro)

```
 template <>
 struct ClassID_traits<vector<double> > {
    typedef type_tools::true_tag has_clID_tag;
    static const int ID = 1234;
    ....
 };

```

to manage the ClassIDs Atlas has developed a simple text-based “database” that is used both to generate theClassIDs of new types and to verify at run-time that there are no duplicated ClassIDs and no conflicts.

### Concept Checking

SG allows developers to use generic key types to identify objects of a given type. A key must of course define an ordering operation. For SG we also require keys to be persistable. In traditional OO programming these requirements would be expressed as an interface the key class imports. In generic programming interfaces are rather exported and hence verified by the clients. To this end, SG provides a KeyConcept built using the boost concept\_check library (see Fig. 2).

Inserting in the StoreGate API a call to boost::function\_requires$`<`$KeyConcept$`<`$KEY$`>`$$`>`$() we allow the compiler to check whether the template parameter KEY of a retrieve or register method is valid.

### Policy Classes

SG handle and link classes use policy classes to configure their behavior at compile time. A policyAlexandrescu  is a statically configured StrategyGoF . It can also be seen as a traits class that defines behavior rather than structure. Policies become powerful tools when they are combined: the compiler picks the right combinations and generates the code needed by the application. For example the element link class template ElementLink is implemented as a combination of two policies (see Fig. 3).

DataProxyStorage wraps the TDS back-end API, while IndexingPolicy defines the strategy the ElementLink uses to find a container element given its identifier, and viceversa. The type generator template GenerateIndexingPolicy looks at the data object type (STORABLE) and tries to provide a reasonable default strategy for that type.

We have defined indexing policy classes that can be used to index elements of all STL containers and to index nodes of an HepMC graphHepMC . Policies are flexible: if a developer introduces a new container type, all they have to do is to provide a matching indexing policy and the compiler will generate the new link type as needed.

## IV Status and Outlook

After three years of evolution, StoreGate has achieved a certain maturity. A lot of broad design principles have been established: work with user types, avoid user-defined keys, define an access control policy. The core data access API has been stable for several releases. The implementation has been reviewed and reengineered twice to improve robustness, physical design and to meet the strict performance requirement of Atlas trigger softwareAtlasTrigger .

In the spirit of the Gaudi open project we have started discussing our work with the LCG community and we hope the StoreGate ideas and code will be useful to developers inside and outside ATLAS.

## Acknowledgments

We would like to thank all ATLAS collaborators who contributed to the design and prototyping of SG. We are extremely grateful to many colleagues from other experiments who shared their experiences with us: M. Frank, V. Innocente, R. Kennedy, J. Kowalkowski, P. Mato, M. Paterno, S. Patton, S. Snyder and L. Tuura.

This work was supported in part by the Office of Science. High Energy Physics , U.S. Department of Energy under Contract No. DE-AC03-76SF00098.