TY - JOUR
T1 - Suppression of tunneling two-level systems in ultrastable glasses of indomethacin
AU - Pérez-Castañeda, Tomás
AU - Rodríguez-Tinoco, Cristian
AU - Rodríguez-Viejo, Javier
AU - Ramos, Miguel A.
PY - 2014/8/5
Y1 - 2014/8/5
N2 - Glasses and other noncrystalline solids exhibit thermal and acoustic properties at low temperatures anomalously different from those found in crystalline solids, and with a remarkable degree of universality. Below a few kelvin, these universal properties have been successfully interpreted using the tunneling model, which has enjoyed (almost) unanimous recognition for decades. Here we present low-temperature specific-heat measurements of ultrastable glasses of indomethacin that clearly show the disappearance of the ubiquitous linear contribution traditionally ascribed to the existence of tunneling twolevel systems (TLS). When the ultrastable thin-film sample is thermally converted into a conventional glass, the material recovers a typical amount of TLS. This remarkable suppression of the TLS found in ultrastable glasses of indomethacin is argued to be due to their particular anisotropic and layered character, which strongly influences the dynamical network and may hinder isotropic interactions among low-energy defects, rather than to the thermodynamic stabilization itself. This explanation may lend support to the criticisms by Leggett and others [Yu CC, Leggett AJ (1988) Comments Condens Matter Phys 14(4):231-251; Leggett AJ, Vural DC (2013) J Phys Chem B 117(42):12966-12971] to the standard tunneling model, although more experiments in different kinds of ultrastable glasses are needed to ascertain this hypothesis.
AB - Glasses and other noncrystalline solids exhibit thermal and acoustic properties at low temperatures anomalously different from those found in crystalline solids, and with a remarkable degree of universality. Below a few kelvin, these universal properties have been successfully interpreted using the tunneling model, which has enjoyed (almost) unanimous recognition for decades. Here we present low-temperature specific-heat measurements of ultrastable glasses of indomethacin that clearly show the disappearance of the ubiquitous linear contribution traditionally ascribed to the existence of tunneling twolevel systems (TLS). When the ultrastable thin-film sample is thermally converted into a conventional glass, the material recovers a typical amount of TLS. This remarkable suppression of the TLS found in ultrastable glasses of indomethacin is argued to be due to their particular anisotropic and layered character, which strongly influences the dynamical network and may hinder isotropic interactions among low-energy defects, rather than to the thermodynamic stabilization itself. This explanation may lend support to the criticisms by Leggett and others [Yu CC, Leggett AJ (1988) Comments Condens Matter Phys 14(4):231-251; Leggett AJ, Vural DC (2013) J Phys Chem B 117(42):12966-12971] to the standard tunneling model, although more experiments in different kinds of ultrastable glasses are needed to ascertain this hypothesis.
KW - Glass transition
KW - Glassy anomalies
KW - Low-temperature properties of glasses
KW - Organic glasses
U2 - 10.1073/pnas.1405545111
DO - 10.1073/pnas.1405545111
M3 - Article
SN - 0027-8424
VL - 111
SP - 11275
EP - 11280
JO - Proceedings of the National Academy of Sciences of the United States of America
JF - Proceedings of the National Academy of Sciences of the United States of America
ER -