Age and structure of a model vapour-deposited glass

Glass films prepared by a process of physical vapour deposition have been shown to have thermodynamic and kinetic stability comparable to those of ordinary glasses aged for thousands of years. A central question in the study of vapour-deposited glasses, particularly in light of new knowledge regarding anisotropy in these materials, is whether the ultra-stable glassy films formed by vapour deposition are ever equivalent to those obtained by liquid cooling. Here we present a computational study of vapour deposition for a two-dimensional glass forming liquid using a methodology, which closely mimics experiment. We find that for the model considered here, structures that arise in vapour-deposited materials are statistically identical to those observed in ordinary glasses, provided the two are compared at the same inherent structure energy. We also find that newly deposited hot molecules produce cascades of hot particles that propagate far into the film, possibly influencing the relaxation of the material.

[1]  Steven J. Plimpton,et al.  STRINGLIKE COOPERATIVE MOTION IN A SUPERCOOLED LIQUID , 1998 .

[2]  J. D. de Pablo,et al.  A molecular view of vapor deposited glasses. , 2011, The Journal of chemical physics.

[3]  Schofield,et al.  Three-dimensional direct imaging of structural relaxation near the colloidal glass transition , 2000, Science.

[4]  Robert J. McMahon,et al.  Organic Glasses with Exceptional Thermodynamic and Kinetic Stability , 2007, Science.

[5]  M. Klein,et al.  Nosé-Hoover chains : the canonical ensemble via continuous dynamics , 1992 .

[6]  C. Angell,et al.  Formation of Glasses from Liquids and Biopolymers , 1995, Science.

[7]  K. Samwer,et al.  Ultrastable Metallic Glass , 2013, Advanced materials.

[8]  J. P. Garrahan,et al.  Preparation and relaxation of very stable glassy states of a simulated liquid. , 2011, Physical review letters.

[9]  I. B. Ivanov,et al.  Mechanism of formation of two-dimensional crystals from latex particles on substrates , 1992 .

[10]  L Yu,et al.  Amorphous pharmaceutical solids: preparation, characterization and stabilization. , 2001, Advanced drug delivery reviews.

[11]  J. Dyre,et al.  Structural Relaxation Monitored by Instantaneous Shear Modulus , 1998 .

[12]  Lian Yu,et al.  Influence of substrate temperature on the stability of glasses prepared by vapor deposition. , 2007, The Journal of chemical physics.

[13]  Kurt Binder,et al.  Supercooled Liquids and the Glass Transition , 2011 .

[14]  Kenneth L. Kearns,et al.  High‐Modulus Organic Glasses Prepared by Physical Vapor Deposition , 2010, Advanced materials.

[15]  Richard A. Vaia,et al.  Accurate Simulation of Surfaces and Interfaces of Face-Centered Cubic Metals Using 12−6 and 9−6 Lennard-Jones Potentials , 2008 .

[16]  Lian Yu,et al.  Surface self-diffusion of organic glasses. , 2013, The journal of physical chemistry. A.

[17]  John D. Hunter,et al.  Matplotlib: A 2D Graphics Environment , 2007, Computing in Science & Engineering.

[18]  M. Sierka,et al.  The atomic structure of a metal-supported vitreous thin silica film. , 2012, Angewandte Chemie.

[19]  Kenneth L. Kearns,et al.  Hiking down the energy landscape: progress toward the Kauzmann temperature via vapor deposition. , 2008, The journal of physical chemistry. B.

[20]  J. Pablo,et al.  Tunable molecular orientation and elevated thermal stability of vapor-deposited organic semiconductors , 2015, Proceedings of the National Academy of Sciences.

[21]  Robert Hovden,et al.  Direct imaging of a two-dimensional silica glass on graphene. , 2012, Nano letters.

[22]  P. Steinhardt,et al.  Bond-orientational order in liquids and glasses , 1983 .

[23]  J. Rodríguez-Viejo,et al.  Evaluation of growth front velocity in ultrastable glasses of indomethacin over a wide temperature interval. , 2014, The journal of physical chemistry. B.

[24]  Pekka Koskinen,et al.  Structural relaxation made simple. , 2006, Physical review letters.

[25]  R. McMahon,et al.  Highly Stable Vapor-Deposited Glasses of Four Tris-naphthylbenzene Isomers , 2011 .

[26]  Hajime Tanaka,et al.  Frustration on the way to crystallization in glass , 2006 .

[27]  G. Maret,et al.  Local crystalline order in a 2D colloidal glass former , 2008, The European physical journal. E, Soft matter.

[28]  M. Oguni,et al.  Character of devitrification, viewed from enthalpic paths, of the vapor-deposited ethylbenzene glasses. , 2011, The journal of physical chemistry. B.

[29]  Steve Plimpton,et al.  Fast parallel algorithms for short-range molecular dynamics , 1993 .

[30]  Sindee L. Simon,et al.  Volume and enthalpy recovery of polystyrene , 2001 .

[31]  Glen M. Hocky,et al.  Equilibrium ultrastable glasses produced by random pinning. , 2014, The Journal of chemical physics.

[32]  Claude M. Penchina,et al.  The physics of amorphous solids , 1983 .

[33]  R. Zallen,et al.  The Physics of Amorphous Solids: ZALLEN:PHYSICS OF AMORPHO O-BK , 2005 .

[34]  Juan J de Pablo,et al.  Ultrastable glasses from in silico vapour deposition. , 2013, Nature materials.

[35]  Chi-Hang Lam,et al.  Glass Transition Dynamics and Surface Layer Mobility in Unentangled Polystyrene Films , 2010, Science.

[36]  P. Pieranski,et al.  Two-Dimensional Interfacial Colloidal Crystals , 1980 .

[37]  Feng Wang,et al.  Glass transitions in quasi-two-dimensional suspensions of colloidal ellipsoids. , 2011, Physical review letters.

[38]  F. Stillinger,et al.  Properties of model atomic free-standing thin films. , 2011, The Journal of chemical physics.

[39]  M D Ediger,et al.  Surface self-diffusion of an organic glass. , 2011, Physical review letters.

[40]  J. Perepezko,et al.  Increasing the kinetic stability of bulk metallic glasses , 2016 .

[41]  J. D. de Pablo,et al.  Model vapor-deposited glasses: growth front and composition effects. , 2013, The Journal of chemical physics.

[42]  Lian Yu,et al.  Generality of forming stable organic glasses by vapor deposition , 2010 .