Disentangling Electronic and Ionic Nonlinear Polarization Effects in Bulk THz Kerr Response

Terahertz (THz) spectroscopy is a powerful probe of low-energy excitations in complex materials. Extending it into the nonlinear regime broadens its scope and can provide valuable insight into interactions among these modes. However, interpreting nonlinear spectra is challenging because resonant features in this case do not always reflect intrinsic material dynamics. Here, we study nonlinear THz-induced Kerr effect in a generic material LaAlO_{3}. After detailed analysis of temporal oscillations of the Kerr signal, we identify an E_{g} Raman mode at 1.1 THz excited through a two-photon process, while two additional peaks (0.86 and 0.36 THz) arise from phase matching of the near-infrared probe beam with co- and counterpropagating THz pump fields, mediated by off-resonant electronic hyperpolarizability. These results demonstrate the crucial role of kinematic effects in shaping THz-induced Kerr response and establish a framework for interpreting nonlinear spectroscopies in complex materials.

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Publication Details

Journal
Physical Review Letters
Published
2026-02-03
DOI
https://doi.org/10.1103/1c5k-9z82
Primary Topic
Terahertz technology and applications
Type
article
Field-Weighted Citation Impact
0.00
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article

Disentangling Electronic and Ionic Nonlinear Polarization Effects in Bulk THz Kerr Response

Sebastian F. Maehrlein, Maximilian Frenzel, Zhanybek Alpichshev
Physical Review Letters
Terahertz technology and applications
article

Disentangling Electronic and Ionic Nonlinear Polarization Effects in Bulk THz Kerr Response

Sebastian F. Maehrlein, Maximilian Frenzel, Zhanybek Alpichshev
article en

Abstract

Terahertz (THz) spectroscopy is a powerful probe of low-energy excitations in complex materials. Extending it into the nonlinear regime broadens its scope and can provide valuable insight into interactions among these modes. However, interpreting nonlinear spectra is challenging because resonant features in this case do not always reflect intrinsic material dynamics. Here, we study nonlinear THz-induced Kerr effect in a generic material LaAlO_{3}. After detailed analysis of temporal oscillations of the Kerr signal, we identify an E_{g} Raman mode at 1.1 THz excited through a two-photon process, while two additional peaks (0.86 and 0.36 THz) arise from phase matching of the near-infrared probe beam with co- and counterpropagating THz pump fields, mediated by off-resonant electronic hyperpolarizability. These results demonstrate the crucial role of kinematic effects in shaping THz-induced Kerr response and establish a framework for interpreting nonlinear spectroscopies in complex materials.

Physical Review LettersVol. 136(10)
Institute of Science and Technology Austria (AT), Fritz Haber Institute of the Max Planck Society (DE), Helmholtz-Zentrum Dresden-Rossendorf (DE)
Openalex Percentile: Top 68%
Terahertz technology and applications
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Disentangling Electronic and Ionic Nonlinear Polarization Effects in Bulk THz Kerr Response — Sebastian F. Maehrlein, Maximilian Frenzel, et al. · Physical Review Letters (2026) | TGRS Research Map | TGRS