Pressure Tuning of the Low-Frequency Raman Response in Spin-Crossover Networks
that shows an unusual red shift through the pressure-induced SCO. Angle-dependent Raman measurements in the LF, fingerprint and C≡N stretching regions of the spectrum also show strong polarization sensitivity. First-principles modeling of the IR- and Raman-active phonon modes in both ambient and high-pressure structures reliably reproduces the THz absorption and angle-dependent Raman spectra, allowing assignment of the spectral features to the underlying atomic motion. This work establishes pressure tuning of the LF phonon modes and spin states in molecular SCO materials as a novel approach to modulating THz light and hence provides new avenues for the design of tunable THz absorbers for advanced photonics applications.
Authors
- Kazuki Nakamura (ORCID: https://orcid.org/0000-0003-1556-3263)
- Joseph M. Flitcroft (ORCID: https://orcid.org/0000-0001-8373-0233)
- Kenta Imoto (ORCID: https://orcid.org/0000-0002-6764-2484)
- Nico Giordano (ORCID: https://orcid.org/0000-0001-9518-1251)
- Lulu Xiong
- Koji Nakabayashi (ORCID: https://orcid.org/0000-0002-5946-944X)
- Guanping Li (ORCID: https://orcid.org/0000-0001-5168-7998)
- Nicholas F. Chilton (ORCID: https://orcid.org/0000-0002-8604-0171)
- Olaf Stefańczyk (ORCID: https://orcid.org/0000-0003-0955-5646)
- Tomu Otake
- Simon Parsons
- Calum S. Sangster (ORCID: https://orcid.org/0009-0006-6721-4398)
- Jonathan M. Skelton (ORCID: https://orcid.org/0000-0002-0395-1202)
- Euan K. Brechin
- Shin-ichi Ohkoshi (ORCID: https://orcid.org/0000-0001-9359-5928)
Institutions
- Australian National University (AU)
- Centre National de la Recherche Scientifique (FR)
- University of Macau (MO)
- Deutsches Elektronen-Synchrotron DESY (DE)
- University of Manchester (GB)
- Joint Laboratory for Extreme Conditions Matter Properties (CN)
- Institut de Physique de Rennes (FR)
- The University of Tokyo (JP)
- University of Edinburgh (GB)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2026-05-22
- DOI
- https://doi.org/10.1021/jacs.6c03325
- Primary Topic
- Magnetism in coordination complexes
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- UK Research and Innovation
- Leverhulme Trust
- University of Manchester
- Australian National University
- Iketani Science and Technology Foundation
- Engineering and Physical Sciences Research Council
- Deutsches Elektronen-Synchrotron
- Japan Society for the Promotion of Science
- Japan Science and Technology Agency