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Title: Excitation protocols for nonlinear phononics in bismuth and antimony

Journal Article · · Physical Review Materials
ORCiD logo [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Boston Univ., MA (United States)
  2. Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
  3. Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM); Northwestern-Argonne Institute of Science and Engineering, Evanston, IL (United States); Univ. of Chicago, IL (United States)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM); Northwestern-Argonne Institute of Science and Engineering, Evanston, IL (United States)
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Here, 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 phonon 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 nonlinear phononics.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357; SC0023402
OSTI ID:
2281394
Journal Information:
Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 1 Vol. 8; ISSN 2475-9953
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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36 MATERIALS SCIENCE
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