---
_id: '66942'
abstract:
- lang: eng
  text: Raman imaging, based on incoherent spontaneous Raman scattering (SR) or coherent
    techniques such as broadband coherent anti-Stokes Raman spectroscopy (BCARS),
    is a powerful tool for visualizing local lattice distortions. It can thus be employed,
    e.g., to identify and visualize ferroelectric (FE) domain walls (DWs). While SR-based
    DW imaging relies on small changes in the intensity or position of Raman peaks
    at the DW, BCARS measurements may detect DW signatures with a drastically increased
    contrast and orders of magnitude faster imaging speed. However, while SR-based
    contrasts can be predicted from existing models, the increased DW contrasts in
    BCARS remain poorly understood. In this work, we develop a first-principles approach
    for the simulation of CARS spectra to investigate the origin of this BCARS signal
    contrast at periodically poled stoichiometric lithium niobate (sPPLN) DWs. Combining
    these atomistic simulations with strain modeling allows us to explore how strain
    affects the CARS signal generation at FE DWs. We then apply polarization-sensitive
    BCARS to image sPPLN DWs for different polarization configurations. Our results
    reveal additional Raman peaks specific to the DWs across all investigated polarization
    combinations, yielding a strong DW-to-bulk contrast that enables in situ identification
    and localization of DWs in two-dimensional BCARS maps. This study demonstrates
    the practical utility of polarization-sensitive BCARS for fast DW imaging and
    provides fundamental insights into the BCARS contrast mechanism in FE materials,
    both in strained regions and in the unstrained bulk.
article_number: '034104'
article_type: original
author:
- first_name: Robin
  full_name: Buschbeck, Robin
  last_name: Buschbeck
- first_name: Mike N.
  full_name: Pionteck, Mike N.
  last_name: Pionteck
- first_name: Naomi
  full_name: Herrmann, Naomi
  last_name: Herrmann
- first_name: Michael
  full_name: Rüsing, Michael
  id: '22501'
  last_name: Rüsing
  orcid: 0000-0003-4682-4577
- first_name: Susanne C.
  full_name: Kehr, Susanne C.
  last_name: Kehr
- first_name: Simone
  full_name: Sanna, Simone
  last_name: Sanna
- first_name: Lukas M.
  full_name: Eng, Lukas M.
  last_name: Eng
citation:
  ama: 'Buschbeck R, Pionteck MN, Herrmann N, et al. Ab initio modeling and experimental
    analysis of contrast in broadband coherent anti-Stokes Raman spectroscopy: A case
    study on ferroelectric domain walls. <i>Physical Review B</i>. 2026;114(3). doi:<a
    href="https://doi.org/10.1103/m1xq-rlft">10.1103/m1xq-rlft</a>'
  apa: 'Buschbeck, R., Pionteck, M. N., Herrmann, N., Rüsing, M., Kehr, S. C., Sanna,
    S., &#38; Eng, L. M. (2026). Ab initio modeling and experimental analysis of contrast
    in broadband coherent anti-Stokes Raman spectroscopy: A case study on ferroelectric
    domain walls. <i>Physical Review B</i>, <i>114</i>(3), Article 034104. <a href="https://doi.org/10.1103/m1xq-rlft">https://doi.org/10.1103/m1xq-rlft</a>'
  bibtex: '@article{Buschbeck_Pionteck_Herrmann_Rüsing_Kehr_Sanna_Eng_2026, title={Ab
    initio modeling and experimental analysis of contrast in broadband coherent anti-Stokes
    Raman spectroscopy: A case study on ferroelectric domain walls}, volume={114},
    DOI={<a href="https://doi.org/10.1103/m1xq-rlft">10.1103/m1xq-rlft</a>}, number={3034104},
    journal={Physical Review B}, publisher={American Physical Society (APS)}, author={Buschbeck,
    Robin and Pionteck, Mike N. and Herrmann, Naomi and Rüsing, Michael and Kehr,
    Susanne C. and Sanna, Simone and Eng, Lukas M.}, year={2026} }'
  chicago: 'Buschbeck, Robin, Mike N. Pionteck, Naomi Herrmann, Michael Rüsing, Susanne
    C. Kehr, Simone Sanna, and Lukas M. Eng. “Ab Initio Modeling and Experimental
    Analysis of Contrast in Broadband Coherent Anti-Stokes Raman Spectroscopy: A Case
    Study on Ferroelectric Domain Walls.” <i>Physical Review B</i> 114, no. 3 (2026).
    <a href="https://doi.org/10.1103/m1xq-rlft">https://doi.org/10.1103/m1xq-rlft</a>.'
  ieee: 'R. Buschbeck <i>et al.</i>, “Ab initio modeling and experimental analysis
    of contrast in broadband coherent anti-Stokes Raman spectroscopy: A case study
    on ferroelectric domain walls,” <i>Physical Review B</i>, vol. 114, no. 3, Art.
    no. 034104, 2026, doi: <a href="https://doi.org/10.1103/m1xq-rlft">10.1103/m1xq-rlft</a>.'
  mla: 'Buschbeck, Robin, et al. “Ab Initio Modeling and Experimental Analysis of
    Contrast in Broadband Coherent Anti-Stokes Raman Spectroscopy: A Case Study on
    Ferroelectric Domain Walls.” <i>Physical Review B</i>, vol. 114, no. 3, 034104,
    American Physical Society (APS), 2026, doi:<a href="https://doi.org/10.1103/m1xq-rlft">10.1103/m1xq-rlft</a>.'
  short: R. Buschbeck, M.N. Pionteck, N. Herrmann, M. Rüsing, S.C. Kehr, S. Sanna,
    L.M. Eng, Physical Review B 114 (2026).
date_created: 2026-09-02T12:04:02Z
date_updated: 2026-09-02T12:06:24Z
department:
- _id: '15'
- _id: '288'
- _id: '623'
doi: 10.1103/m1xq-rlft
intvolume: '       114'
issue: '3'
language:
- iso: eng
publication: Physical Review B
publication_identifier:
  issn:
  - 2469-9950
  - 2469-9969
publication_status: published
publisher: American Physical Society (APS)
quality_controlled: '1'
status: public
title: 'Ab initio modeling and experimental analysis of contrast in broadband coherent
  anti-Stokes Raman spectroscopy: A case study on ferroelectric domain walls'
type: journal_article
user_id: '22501'
volume: 114
year: '2026'
...