Vibrational spectra and nonlinear optical coefficients of rhombohedral CsGeX3 halide compounds with X=I , Br, Cl

Huang, Ling-yi; Lambrecht, Walter R.  L.

doi:10.1103/PhysRevB.94.115202

Title: Vibrational spectra and nonlinear optical coefficients of rhombohedral $CsGe X_{3}$ halide compounds with $X = I$ , Br, Cl

Abstract

The zone-center phonons are calculated here for rhombohedral CsGeX₃ compounds with X=I, Br, Cl using density functional perturbation theory in a plane-wave pseudopotential method. The infrared absorption and reflection spectra are simulated and show that the absorption has a strong contribution from the LO as well asTO modes. Both the lowest and highest IR active modes have strong oscillator strengths for each symmetry (A₁ and E) and correspond to motions of either the Cs or Ge ions relative to the halogen ions. respectively. The intermediate modes have low oscillator strength because their mode pattern shows less clearly a dipole pattern.The polarization dependent Raman spectra for various back scattering configurations are simulated. Only the highest modes of each symmetry have a strong Raman intensity. The findings for the Raman spectra are found to be in good agreement with the available experimental data for polycrystalline films when averaging over directions. The Born effective charges and high and low frequency dielectric tensors as well as the second-order nonlinear optical coefficients are calculated. The ratio of the static to the high-frequency dielectric constants are extremely high and analyzed in terms of the contribution of each mode to the Lyddane-Sachs-Teller relation. The nonlinear optical coefficientsmore »« less

Authors:

Huang, Ling-yi ^[1]; Lambrecht, Walter R. L. ^[2]

Case Western Reserve Univ., Cleveland, OH (United States); California State Univ. (CalState), Long Beach, CA (United States)
Case Western Reserve Univ., Cleveland, OH (United States)

Publication Date:: Mon Sep 12 00:00:00 EDT 2016

Research Org.:: Case Western Reserve Univ., Cleveland, OH (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1591889

Alternate Identifier(s):: OSTI ID: 1324020

Grant/Contract Number:: SC0008933

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 94; Journal Issue: 11; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; phonons; halide perovskites; Raman non-linear optics

Citation Formats


                    Huang, Ling-yi, and Lambrecht, Walter R.  L. Vibrational spectra and nonlinear optical coefficients of rhombohedral CsGeX3 halide compounds with X=I , Br, Cl.  United States: N. p., 2016. 
Web.  doi:10.1103/PhysRevB.94.115202.

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                    Huang, Ling-yi, & Lambrecht, Walter R.  L. Vibrational spectra and nonlinear optical coefficients of rhombohedral CsGeX3 halide compounds with X=I , Br, Cl.  United States.  https://doi.org/10.1103/PhysRevB.94.115202

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                    Huang, Ling-yi, and Lambrecht, Walter R.  L. Mon .  
"Vibrational spectra and nonlinear optical coefficients of rhombohedral CsGeX3 halide compounds with X=I , Br, Cl".  United States.  https://doi.org/10.1103/PhysRevB.94.115202.  https://www.osti.gov/servlets/purl/1591889.

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@article{osti_1591889,

  title        = {Vibrational spectra and nonlinear optical coefficients of rhombohedral CsGeX3 halide compounds with X=I , Br, Cl},

  author       = {Huang, Ling-yi and Lambrecht, Walter R.  L.},

  abstractNote = {The zone-center phonons are calculated here for rhombohedral CsGeX3 compounds with X=I, Br, Cl using density functional perturbation theory in a plane-wave pseudopotential method. The infrared absorption and reflection spectra are simulated and show that the absorption has a strong contribution from the LO as well asTO modes. Both the lowest and highest IR active modes have strong oscillator strengths for each symmetry (A1 and E) and correspond to motions of either the Cs or Ge ions relative to the halogen ions. respectively. The intermediate modes have low oscillator strength because their mode pattern shows less clearly a dipole pattern.The polarization dependent Raman spectra for various back scattering configurations are simulated. Only the highest modes of each symmetry have a strong Raman intensity. The findings for the Raman spectra are found to be in good agreement with the available experimental data for polycrystalline films when averaging over directions. The Born effective charges and high and low frequency dielectric tensors as well as the second-order nonlinear optical coefficients are calculated. The ratio of the static to the high-frequency dielectric constants are extremely high and analyzed in terms of the contribution of each mode to the Lyddane-Sachs-Teller relation. The nonlinear optical coefficients decrease strongly from I to Br to Cl in reverse order of the band gaps and are foundto be consistent with available experimental results},

  doi          = {10.1103/PhysRevB.94.115202},

  journal      = {Physical Review B},

  number       = 11,

  volume       = 94,

  place        = {United States},

  year         = {Mon Sep 12 00:00:00 EDT 2016},

  month        = {Mon Sep 12 00:00:00 EDT 2016}

}

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Works referencing / citing this record:

Synthesis of Lead‐free CsGeI ₃ Perovskite Colloidal Nanocrystals and Electron Beam‐induced Transformations
journal, May 2018

Wu, Xiaotong; Song, Weidong; Li, Qian
Chemistry – An Asian Journal, Vol. 13, Issue 13
DOI: 10.1002/asia.201800573

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Title: Vibrational spectra and nonlinear optical coefficients of rhombohedral CsGe X 3 halide compounds with X = I , Br, Cl

Abstract

Citation Formats

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Title: Vibrational spectra and nonlinear optical coefficients of rhombohedral $CsGe X_{3}$ halide compounds with $X = I$ , Br, Cl

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Electronic band structure trends of perovskite halides: Beyond Pb and Sn to Ge and Si
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Ab initio calculation of phonon dispersions in semiconductors
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Infrared properties of CsGe(Br x Cl 1− x ) 3 , nonlinear optical rhombohedral semiconductor
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Relativistic separable dual-space Gaussian pseudopotentials from H to Rn
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Hybrid Germanium Iodide Perovskite Semiconductors: Active Lone Pairs, Structural Distortions, Direct and Indirect Energy Gaps, and Strong Nonlinear Optical Properties
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Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites
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New infrared nonlinear optical crystal CsGeBr ₃ : synthesis, structure and powder second-harmonic generation properties
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