Lone Pair Rotational Dynamics in Solids

Remsing, Richard C.; Klein, Michael L.

doi:10.1103/PhysRevLett.124.066001

Title: Lone Pair Rotational Dynamics in Solids

Journal Article · 14 February 2020 · Physical Review Letters

DOI: https://doi.org/10.1103/PhysRevLett.124.066001 · OSTI ID:1601234

^[1]; Klein, Michael L. ^[2]

Rutgers Univ., Piscataway, NJ (United States); Temple University
Temple Univ., Philadelphia, PA (United States)

Traditional classifications of crystalline phases focus on nuclear degrees of freedom. Through examination of both electronic and nuclear structure, we introduce the concept of an electronic plastic crystal. Such a material is classified by crystalline nuclear structure, while localized electronic degrees of freedom — here lone pairs — exhibit orientational motion at finite temperatures. This orientational motion is an emergent phenomenon arising from the coupling between electronic structure and polarization fluctuations generated by collective motions, such as phonons. Using ab initio molecular dynamics simulations, we predict the existence of electronic plastic crystal motion in halogen crystals and halide perovskites, and suggest that such motion may be found in a broad range of solids with lone pair electrons. Finally, such fluctuations in the charge density should be observable, in principle via synchrotron scattering.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); Temple Univ., Philadelphia, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); US Army Research Office (ARO); National Science Foundation

Grant/Contract Number:: SC0012575

OSTI ID:: 1601234

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 6 Vol. 124; ISSN 0031-9007; ISSN PRLTAO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Lone Pair Rotational Dynamics in Solids

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