Single Crystal Vibronic Spectroscopy of [Yb(trensal)]
6 affiliations
- 1Department of Chemistry, University of Manchester, Oxford Road, Manchester, UK, M13 9PL
- 2Research School of Chemistry
- 3Australian National University
- 4Department of Chemistry
- 5University of Copenhagen
- 6National High Magnetic Field Laboratory
Abstract
Understanding vibronic coupling in molecular materials is crucial in the development of high performance molecule-based optical and quantum technologies. Vibronic coupling governs spin state lifetimes in these systems, and is additionally a source of decoherence. Hence, gaining detailed understanding of vibronic coupling will enable improvement of candidate materials. In this regard, magneto-spectroscopic techniques provide a direct probe of the vibronic coupling, which can be performed on polycrystalline and more recently single crystal samples. Single crystal magneto-spectroscopy offers a clear advantage due to its improved resolution and its ability to probe magnetic anisotropy, however, simulating the resulting spectra has proven difficult due to the simultaneous requirements of solid-state phonon calculations, embedded correlated electronic structure theory methods, and inclusion of large numbers of vibrational modes in the Hamiltonian to recreate experimental spectra. In this work we present single crystal far-infrared magneto-spectroscopy (FIRMS) and photo-luminescence magneto-spectroscopy (PLUMS) measurements on [Yb(trensal)] . We can experimentally verify previous assertions that most of the vibronic transitions in the FIRMS map are intra-Kramers doublet transitions and additionally elucidate the origin of the transitions observed in the PLUMS map. Crucially, to achieve this we have developed a new computational framework to perform robust and efficient simulations of magneto-spectroscopy incorporating hundreds of vibrational modes based on ab initio simulations in the solid state.
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BibTeX
@misc{morrillo2026single,
title = {{Single Crystal Vibronic Spectroscopy of [Yb(trensal)]}},
author = {William T. Morrillo and Benjamin E. Atkinson and Steen H. Hansen and Stergios Piligkos and Dmitry Smirnov and Mykhaylo Ozerov and Nicholas F. Chilton},
howpublished = {ChemRxiv},
year = {2026},
month = aug,
doi = {10.26434/chemrxiv.15008092/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008092/v1},
note = {CC BY},
}
RIS
TY - UNPB
TI - Single Crystal Vibronic Spectroscopy of [Yb(trensal)]
AU - William T. Morrillo
AU - Benjamin E. Atkinson
AU - Steen H. Hansen
AU - Stergios Piligkos
AU - Dmitry Smirnov
AU - Mykhaylo Ozerov
AU - Nicholas F. Chilton
PY - 2026
DA - 2026/08/31
PB - ChemRxiv
DO - 10.26434/chemrxiv.15008092/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008092/v1
AB - Understanding vibronic coupling in molecular materials is crucial in the development of high performance molecule-based optical and quantum technologies. Vibronic coupling governs spin state lifetimes in these systems, and is additionally a source of decoherence. Hence, gaining detailed understanding of vibronic coupling will enable improvement of candidate materials. In this regard, magneto-spectroscopic techniques provide a direct probe of the vibronic coupling, which can be performed on polycrystalline and more recently single crystal samples. Single crystal magneto-spectroscopy offers a clear advantage due to its improved resolution and its ability to probe magnetic anisotropy, however, simulating the resulting spectra has proven difficult due to the simultaneous requirements of solid-state phonon calculations, embedded correlated electronic structure theory methods, and inclusion of large numbers of vibrational modes in the Hamiltonian to recreate experimental spectra. In this work we present single crystal far-infrared magneto-spectroscopy (FIRMS) and photo-luminescence magneto-spectroscopy (PLUMS) measurements on [Yb(trensal)] . We can experimentally verify previous assertions that most of the vibronic transitions in the FIRMS map are intra-Kramers doublet transitions and additionally elucidate the origin of the transitions observed in the PLUMS map. Crucially, to achieve this we have developed a new computational framework to perform robust and efficient simulations of magneto-spectroscopy incorporating hundreds of vibrational modes based on ab initio simulations in the solid state.
ER -