Melting entropy of crystals determined by electron-beam-induced configurational disordering

Upon melting, the molecules in a crystal explore numerous configurations, reflecting an increase in disorder. The molar entropy of disorder can be defined by Boltzmann's formula Δ = ln( ), where is the increase in the number of microscopic states, so far inaccessible experimentally. We found th...

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Bibliographic Details
Published in:Science (American Association for the Advancement of Science) 2024-06, Vol.384 (6701), p.1212-1219
Main Authors: Liu, Dongxin, Fu, Jiarui, Elishav, Oren, Sakakibara, Masaya, Yamanouchi, Kaoru, Hirshberg, Barak, Nakamuro, Takayuki, Nakamura, Eiichi
Format: Article
Language:English
Subjects:
Crystals
Electron beams
Electron diffraction
Entropy
Inelastic scattering
Melting
Organic crystals
Scattering cross sections
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Summary:Upon melting, the molecules in a crystal explore numerous configurations, reflecting an increase in disorder. The molar entropy of disorder can be defined by Boltzmann's formula Δ = ln( ), where is the increase in the number of microscopic states, so far inaccessible experimentally. We found that the Arrhenius frequency factor of the electron diffraction signal decay provides through an experimental equation = , where is an inelastic scattering cross section. The method connects Clausius and Boltzmann experimentally and supplements the Clausius approach, being applicable to a femtogram quantity of thermally unstable and biomolecular crystals. The data also showed that crystal disordering and crystallization of melt are reciprocal, both governed by the entropy change but manifesting in opposite directions.
ISSN:0036-8075
1095-9203
DOI:10.1126/science.adk3620