Spin crossover transition driven by pressure: Barocaloric applications

Reis, Mario; Cheng, Yongqiang; dos Santos, Antonio M.

doi:10.1016/j.physb.2024.415689

Spin crossover transition driven by pressure: Barocaloric applications

Journal Article · Tue Jan 16 00:00:00 EST 2024 · Physica. B, Condensed Matter

DOI:https://doi.org/10.1016/j.physb.2024.415689· OSTI ID:2283839

Reis, Mario ^[1]; Cheng, Yongqiang ^[2]; ^[2]

Universidade Federal Fluminense, Rio de Janiero (Brazil); Universidad de Sevilla (Spain)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

This article describes a mean-field theoretical model for Spin-Crossover (SCO) materials and explores its implications. It is based on a simple Hamiltonian that yields the high spin molar fraction as a function of temperature and pressure, as well as a temperature–pressure phase diagram for the SCO transition. In order to test the model, it was compared with the giant Barocaloric Effect (BCE) of the SCO material [FeL₂][B₄]₂. Furthermore, we found that optical phonons are responsible for 92% of the total barocaloric entropy change. DFT calculations successively indicates that, as expected, the majority of this effect can be traced to low frequencies modes of vibration (400 cm^-1), associated to the Fe coordination.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Compute and Data Environment for Science (CADES)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2283839

Journal Information:: Physica. B, Condensed Matter, Journal Name: Physica. B, Condensed Matter Vol. 677; ISSN 0921-4526

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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