$χ^{(2)}$-Induced Artifact Overwhelming the Third-Order Signal in 2D Raman-THz Spectroscopy of Non-Centrosymmetric Materials

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Hauptverfasser: Mousavi, Seyyed Jabbar, Biggs, Megan F., Johnson, Jeremy A., Hamm, Peter, Shalit, Andrey
Format: Preprint
Veröffentlicht: 2024
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author Mousavi, Seyyed Jabbar
Biggs, Megan F.
Johnson, Jeremy A.
Hamm, Peter
Shalit, Andrey
author_facet Mousavi, Seyyed Jabbar
Biggs, Megan F.
Johnson, Jeremy A.
Hamm, Peter
Shalit, Andrey
contents Through comprehensive data analysis, we demonstrate that a $χ^{(2)}$-induced artifact, arising from imperfect balancing in the conventional electro-optic sampling (EOS) detection scheme, contributes significantly to the measured signal in 2D Raman-THz spectroscopy of non-centrosymmetric materials. The artifact is a product of two 1D responses, overwhelming the desired 2D response. We confirm that by analyzing the 2D Raman-THz response of a x-cut beta barium borate (BBO) crystal. We furthermore show that this artifact can be effectively suppressed by implementing a special detection scheme. We successfully isolate the desired third-order 2D Raman-THz response, revealing a distinct cross-peak feature, whose frequency position suggests the coupling between two crystal phonons.
format Preprint
id arxiv_https___arxiv_org_abs_2407_09243
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle $χ^{(2)}$-Induced Artifact Overwhelming the Third-Order Signal in 2D Raman-THz Spectroscopy of Non-Centrosymmetric Materials
Mousavi, Seyyed Jabbar
Biggs, Megan F.
Johnson, Jeremy A.
Hamm, Peter
Shalit, Andrey
Optics
Through comprehensive data analysis, we demonstrate that a $χ^{(2)}$-induced artifact, arising from imperfect balancing in the conventional electro-optic sampling (EOS) detection scheme, contributes significantly to the measured signal in 2D Raman-THz spectroscopy of non-centrosymmetric materials. The artifact is a product of two 1D responses, overwhelming the desired 2D response. We confirm that by analyzing the 2D Raman-THz response of a x-cut beta barium borate (BBO) crystal. We furthermore show that this artifact can be effectively suppressed by implementing a special detection scheme. We successfully isolate the desired third-order 2D Raman-THz response, revealing a distinct cross-peak feature, whose frequency position suggests the coupling between two crystal phonons.
title $χ^{(2)}$-Induced Artifact Overwhelming the Third-Order Signal in 2D Raman-THz Spectroscopy of Non-Centrosymmetric Materials
topic Optics
url https://arxiv.org/abs/2407.09243