Broadband coherent anti-Stokes Raman scattering for crystalline materials

Franz Hempel, Sven Reitzig, Michael Rüsing, and Lukas M. Eng
Phys. Rev. B 104, 224308 – Published 30 December 2021
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Abstract

Broadband coherent anti-Stokes Raman scattering (B-CARS) has emerged in recent years as a promising chemosensitive high-speed imaging technique. B-CARS allows for the detection of vibrational sample properties in analogy to spontaneous Raman spectroscopy, but also makes electronic sample environments accessible due to its resonant excitation mechanism. Nevertheless, this technique has only gained interest in the biomedical field so far, whereas CARS investigations on solid-state materials are rare and concentrate on layered, two-dimensional materials such as graphene and hexagonal boron nitride . In this work, we discuss the specific properties of this technique when applied to single-crystalline samples, with respect to signal generation, phase matching, and selection rules in the model systems lithium niobate and lithium tantalate. Via polarized B-CARS measurements and subsequent phase retrieval, we validate the predicted selection rules, unequivocally assign the phonons of the A1(TO), E(TO) and A1(LO) branches to the detected CARS peaks, and address differences in spontaneous Raman spectroscopy concerning peak frequencies and scattering efficiencies. We thus establish this technique for future investigations of solid-state materials, specifically in the field of ferroelectric single crystals.

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  • Received 5 October 2021
  • Accepted 9 December 2021

DOI:https://doi.org/10.1103/PhysRevB.104.224308

©2021 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Franz Hempel1,*,†, Sven Reitzig1,*,‡, Michael Rüsing1, and Lukas M. Eng1,2

  • 1Institut für Angewandte Physik, Technische Universität Dresden, 01062 Dresden, Germany
  • 2ct.qmat: Dresden-Würzburg Cluster of Excellence–EXC 2147, TU Dresden, 01062 Dresden, Germany

  • *These authors contributed equally to this paper.
  • franz.hempel@tu-dresden.de
  • sven.reitzig@tu-dresden.de

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Issue

Vol. 104, Iss. 22 — 1 December 2021

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