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Computation of Atmospheric Concentrations of Molecular Clusters from ab initio Thermochemistry

Computation of Atmospheric Concentrations of Molecular Clusters from ab initio Thermochemistry

Published on: April 8, 2020

Thermodynamics of atomic clusters using variational quantum hydrodynamics.

Sean W Derrickson¹, Eric R Bittner

¹Department of Chemistry and Center for Materials Chemistry, University of Houston, Houston, Texas 77204, USA.

The Journal of Physical Chemistry. A

|August 7, 2007

Summary

Quantum delocalization in neon (Ne)n clusters impacts their thermodynamics and structure. Small clusters exhibit a surprising negative heat capacity due to nonadditive free-energy effects.

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Area of Science:

Quantum physics
Thermodynamics
Materials science

Background:

Rare-gas clusters serve as model systems for quantum effects.
Understanding quantum delocalization is key to molecular-scale systems.

Purpose of the Study:

Investigate the structure and dynamics of neon (Ne)n clusters.
Examine quantum delocalization's influence on thermodynamics and structure.
Analyze clusters from T = 0 K to the solid-to-liquid transition.

Main Methods:

Variational quantum hydrodynamic approach.
Inclusion of finite temperature effects via an "entropy" potential.
Analysis of (Ne)n clusters with n up to 100 atoms.

Main Results:

Predicted negative heat capacity for very small neon clusters.
Observed effects of quantum delocalization on cluster structure and dynamics.
Characterized thermodynamic properties across temperature ranges.

Conclusions:

Nonadditive free-energy contributions are significant in small clusters.
Quantum hydrodynamics provides insights into rare-gas cluster behavior.
Negative heat capacity is a consequence of system size and quantum effects.