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Title: Role of orbital filling on nonlinear ionic Raman scattering in perovskite titanates

Journal Article · · Physical Review. B
 [1];  [1]
  1. Northwestern Univ., Evanston, IL (United States)
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The linear and nonlinear phononic interactions between an optically excited infrared (IR) or hyper-Raman mode and a driven Raman mode are computed for the d0 (CaTiO3) and d1 (LaTiO3) titanates within a first-principles density functional framework. We calculate the potential energy surface expanded in terms of the Ag or B1g mode amplitudes coupled to the Au or the B3u mode and determine the coupling coefficients for these multimode interactions. We find that the linear-quadratic coupling dominates the anharmonicities over the quadratic-quadratic interaction in the perovskite titanates. The IR and Raman modes both modify the electronic structure with the former being more significant but occurring on a different time scale; furthermore, the coupled-mode interactions lead to sizable perturbations to the valence bandwidth (~100 meV) and band gap (~ 50 meV). By comparing the coupling coefficients of undoped CaTiO3 and LaTiO3 to those for electron-doped (CaTiO3) and hole-doped (LaTiO3) titanates, we isolate the role of orbital filling in the nonlinear coupling process. We find that with increasing occupancy of the d manifold, the linear-quadratic interaction decreases by approximately 30% with minor changes induced by the cation chemistry (that mainly affect the phonon mode frequencies) or by electron correlation. We identify the importance of the Ti-O bond stiffness, which depends on the orbital filling, in governing the lattice anharmonicitiy. This microscopic understanding can be used to increase the nonlinear coupling coefficient to facilitate more facile access of nonequilibrium structures and properties through ionic Raman scattering processes.

Research Organization:
Pennsylvania State Univ., University Park, PA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012375; AC02-06CH11357
OSTI ID:
1535821
Alternate ID(s):
OSTI ID: 1339007
Journal Information:
Physical Review. B, Vol. 95, Issue 2; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science

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Cited By (5)

Coupled Raman-Raman modes in the ionic Raman scattering process journal September 2018
Sum-frequency ionic Raman scattering journal May 2018
Nonlinear phononic control and emergent magnetism in Mott insulating titanates journal July 2018
Low-frequency and Moiré–Floquet engineering: A review journal March 2021
Comparison of coherent phonon generation by electronic and ionic Raman scattering in LaAlO3 text January 2021

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75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Materials Science
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