Thermodynamic signature of growing amorphous order in glass-forming liquids

Biroli, Giulio; Bouchaud, Jean‐Philippe; Cavagna, Andrea; Grigera, Tomás S.; Verrocchio, P.

doi:10.1038/nphys1050

Cited by 343 publications

(510 citation statements)

References 32 publications

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“…More recently, approaches that detect the growth in static correlations while staying clear of any specific proposal about local order, i.e., "order-agnostic" approaches, have been developed. Among these proposals, we note patch repetition lengths [30,31], length scales extracted from information theoretic analysis [32,33] or from finite-size studies of the configurational entropy [34], and other "point-to-set" correlation lengths [35][36][37][38][39][40].…”

Section: Introductionmentioning

confidence: 99%

Decorrelation of the static and dynamic length scales in hard-sphere glass formers

Charbonneau

Tarjus

2013

Phys. Rev. E

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We show that, in the equilibrium phase of glass-forming hard-sphere fluids in three dimensions, the static length scales tentatively associated with the dynamical slowdown and the dynamical length characterizing spatial heterogeneities in the dynamics unambiguously decorrelate. The former grow at a much slower rate than the latter when density increases. This observation is valid for the dynamical range that is accessible to computer simulations, which roughly corresponds to that accessible in colloidal experiments. We also find that, in this same range, no one-to-one correspondence between relaxation time and point-to-set correlation length exists. These results point to the coexistence of several relaxation mechanisms in the dynamically accessible regime of three-dimensional hard-sphere glass formers.

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Section: Introductionmentioning

confidence: 99%

Decorrelation of the static and dynamic length scales in hard-sphere glass formers

Charbonneau

Tarjus

2013

Phys. Rev. E

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“…As an example the temperature dependence of the static length scale can be obtained from the system size dependence of some relevant observable by analyzing the data using finite size scaling. In the glass community the existence and usefulness of a static length scale is still debated; even if one can extract some static length scale by doing some sophisticated analysis [5][6][7], the slow growth of this length scale makes it difficult to extract reliable insights . Nevertheless finite size effects in the dynamics of the supercooled liquids certainly exist, notwithstanding the fact that the characteristic length scale may not change very much.…”

Section: Introductionmentioning

confidence: 99%

“…A clear advantage of our proposed length scale [3] is that it is relatively easy to extract both in simulations and in experiments [24] as compared to the other length scales like point-to-set [5] and patch length scale [25,26]. While we can compute our length scale for larger range of temperature this is prohibitive for the other length scales, thus at this time there is not enough data to provide a conclusive comparison between these length scales.…”

Section: Introductionmentioning

confidence: 99%

Finite-size scaling for the glass transition: The role of a static length scale

Karmakar

Procaccia

2012

Phys. Rev. E

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Over the last decade computer simulations have had an increasing role in shedding light on difficult statistical physical phenomena and in particular on the ubiquitous problem of the glass transition. Here in a wide variety of materials the viscosity of a super-cooled liquid increases by many orders of magnitude upon decreasing the temperature over a modest range. A natural concern in these computer simulation is the very small size of the simulated systems compared to experimental ones, raising the issue of how to assess the thermodynamic limit. Here we offer a theory for the glass transition based on finite size scaling, a method that was found very useful in the context of critical phenomena and other interesting problems. As is known, the construction of such a theory rests crucially on the existence of a growing static length scale upon decreasing the temperature. We demonstrate that the static length scale that was discovered in Ref.[3] fits the bill extremely well, allowing us to provide a finite size scaling theory for the α relaxation time of the glass transition, including predictions for the thermodynamic limit based on simulations in small systems.

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“…1 Department of Chemistry, Columbia University, 3000 Broadway, New York, New York 10027, USA, 2 Institute of Physics, University of Tsukuba, Tennodai 1-1-1, Tsukuba, 305-8571, Japan, 3 School of Chemistry, The Sackler Faculty of Exact Sciences, Tel Aviv University, Tel Aviv 69978, Israel. *e-mail: rabani@tau.ac.il; drr2103@columbia.edu.…”

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confidence: 99%

Quantum fluctuations can promote or inhibit glass formation

et al. 2011

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Glasses are dynamically arrested states of matter that do not exhibit the long-range periodic structure of crystals 1-4 . Here we develop new insights from theory and simulation into the impact of quantum fluctuations on glass formation. As intuition may suggest, we observe that large quantum fluctuations serve to inhibit glass formation as tunnelling and zero-point energy allow particles to traverse barriers facilitating movement. However, as the classical limit is approached a regime is observed in which quantum effects slow down relaxation making the quantum system more glassy than the classical system. This dynamical 'reentrance' occurs in the absence of obvious structural changes and has no counterpart in the phenomenology of classical glass-forming systems.Although a wide variety of glassy systems ranging from metallic to colloidal can be accurately described using classical theory, quantum systems ranging from molecular, to electronic and magnetic form glassy states 5,6 . Perhaps the most intriguing of these is the coexistence of superfluidity and dynamical arrest, namely the 'superglass' state suggested by recent numerical, theoretical and experimental work [7][8][9] . Although such intriguing examples exist, at present there is no unifying framework to treat the interplay between quantum and glassy fluctuations in the liquid state.To attempt to formulate a theory for a quantum liquid to glass transition, we may first appeal to the classical case for guidance. Here, a microscopic theory exists in the form of mode-coupling theory (MCT), which requires only simple static structural information as input and produces a full range of dynamical predictions for time correlation functions associated with single-particle and collective fluctuations 10 . Although MCT has a propensity to overestimate a liquid's tendency to form a glass, it has been shown to account for the emergence of the non-trivial growing dynamical length scales associated with vitrification 11 . Perhaps more importantly, MCT has made numerous non-trivial predictions ranging from logarithmic temporal decay of density fluctuations and reentrant dynamics in adhesive colloidal systems to various predictions concerning the effect of compositional mixing on glassy behaviour 12,13 . These have been confirmed by both simulation and experiment [14][15][16] .A fully microscopic quantum version of MCT (QMCT) that requires only the observable static structure factor as input may be developed along the same lines as the classical version. Indeed, a zero-temperature version of such a theory has been developed and successfully describes the wave-vector-dependent dispersion in superfluid helium 17 . In the Supplementary Information, we outline the derivation of a full temperature-dependent QMCT. In the limit of high temperatures, our theory reduces to the hard-sphere fluid. φ is the volume fraction, Λ * = (βh 2 /mσ 2 ) 1/2 is the thermal wavelength in units of inter-particle separation σ , and β = 1/k B T is the inverse temperature. The approach by which the...

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Thermodynamic signature of growing amorphous order in glass-forming liquids

Cited by 343 publications

References 32 publications

Decorrelation of the static and dynamic length scales in hard-sphere glass formers

Decorrelation of the static and dynamic length scales in hard-sphere glass formers

Finite-size scaling for the glass transition: The role of a static length scale

Quantum fluctuations can promote or inhibit glass formation

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