Excitation protocols for non-linear phononics in bismuth and antimony

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Autori principali: Haldar, Anubhab, Huang, Zhengjie, Ma, Xuedan, Darancet, Pierre, Sharifzadeh, Sahar
Natura: Preprint
Pubblicazione: 2023
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author Haldar, Anubhab
Huang, Zhengjie
Ma, Xuedan
Darancet, Pierre
Sharifzadeh, Sahar
author_facet Haldar, Anubhab
Huang, Zhengjie
Ma, Xuedan
Darancet, Pierre
Sharifzadeh, Sahar
contents We study the optical generation and control of coherent phonons in elemental bismuth (Bi) and antimony (Sb) using a classical equation of motion informed by first-principles calculations of the potential energy surface and the frequency-dependent macroscopic dielectric function along the zone-centered optical phonons coordinates. Using this approach, we demonstrate that phonons with the largest optomechanical couplings, also have the strongest degree of anharmonicity among the zone-centered modes, a result of the broken symmetry structural ground state of Bi and Sb. We show how this anharmonicity, explaining the light-induced phonon softening observed in experiments, prevents the application of standard phonon-amplification and annihilation protocols. We introduce a simple linearization protocol that extends the use of such protocols to the case of anharmonic phonons in broken symmetry materials, and demonstrate its efficiency at high displacement amplitudes. Our formalism and results provide a path for improving optical control in non-linear phononics.
format Preprint
id arxiv_https___arxiv_org_abs_2307_11854
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Excitation protocols for non-linear phononics in bismuth and antimony
Haldar, Anubhab
Huang, Zhengjie
Ma, Xuedan
Darancet, Pierre
Sharifzadeh, Sahar
Materials Science
We study the optical generation and control of coherent phonons in elemental bismuth (Bi) and antimony (Sb) using a classical equation of motion informed by first-principles calculations of the potential energy surface and the frequency-dependent macroscopic dielectric function along the zone-centered optical phonons coordinates. Using this approach, we demonstrate that phonons with the largest optomechanical couplings, also have the strongest degree of anharmonicity among the zone-centered modes, a result of the broken symmetry structural ground state of Bi and Sb. We show how this anharmonicity, explaining the light-induced phonon softening observed in experiments, prevents the application of standard phonon-amplification and annihilation protocols. We introduce a simple linearization protocol that extends the use of such protocols to the case of anharmonic phonons in broken symmetry materials, and demonstrate its efficiency at high displacement amplitudes. Our formalism and results provide a path for improving optical control in non-linear phononics.
title Excitation protocols for non-linear phononics in bismuth and antimony
topic Materials Science
url https://arxiv.org/abs/2307.11854