Theoretical study of finite temperature spectroscopy in van der Waals clusters. II Time-dependent absorption spectra
F. Calvo, F. Spiegelman, D. J. Wales
Abstract
Using approximate partition functions and a master equation approach, we investigate the statistical relaxation toward equilibrium in selected CaArn clusters. The Gaussian theory of absorption (previous article) is employed to calculate the average photoabsorption intensity associated with the 4s2-> 4s14p1 transition of calcium as a function of time during relaxation. In CaAr6 and CaAr10 simple relaxation is observed with a single time scale. CaAr13 exhibits much slower dynamics and the relaxation occurs over two distinct time scales. CaAr37 shows much slower relaxation with multiple transients, reminiscent of glassy behavior due to competition between different low-energy structures. We interpret these results in terms of the underlying potential energy surfaces for these clusters.
Create a lesson
Related papers
Molecular Geometry Understanding Has Unintendedly Emerged in Frontier Large Language Models
Gregorii A. Semakin, Timofey V. Losev, Ilya V. Prolomov et al.
Truncated automatic sparse differentiation for machine learning interatomic potentials
Marcel F. Langer, Adrian Hill, Michele Ceriotti
Collective Ion Dynamics from Finite-Volume Fluctuations in Model Explicit-Solvent Electrolytes
Jeongmin Kim
FOSY: Segmental Backbone Assignment in Intrinsically Disordered Proteins
Dmitry M. Lesovoy, Tatiana Agback, Panagiota S. Georgoulia et al.
Efficient tensorized evaluation of permutation invariant polynomials for representing potential energy surfaces
Junhong Li, Kaisheng Song, Hua Guo et al.
DFT GGA based datasets for H2O potential energy surfaces, permanent moment and polarizability tensors
Anoop Ajaya Kumar Nair, Elvar Örn Jónsson