Phonon spectrum in the spin-Peierls phase of <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mi>CuGeO</mml:mi> <mml:mn>3</mml:mn> </mml:msub> </mml:math>
<a:math xmlns:a="http://www.w3.org/1998/Math/MathML"> <a:msub> <a:mi>CuGeO</a:mi> <a:mn>3</a:mn> </a:msub> </a:math> has long been studied as a prototypical example of the spin-Peierls transition in a <b:math xmlns:b="http://www.w3.org/1998/Math/MathML"> <b:mrow> <b:mi>S</b:mi> <b:mo>=</b:mo> <b:mn>1</b:mn> <b:mo>/</b:mo> <b:mn>2</b:mn> </b:mrow> </b:math> Heisenberg chain. Despite intensive investigation of this quasi-one-dimensional material, systematic measurements and calculations of the phonon excitations in the dimerized phase have not to date been possible, leaving certain aspects of the spin-Peierls phenomenon unresolved. We perform state-of-the-art density functional theory (DFT) calculations to compute the electronic structure and phonon dynamics in the low-temperature dimerized phase. We also perform high-resolution neutron spectroscopy to measure the full phonon spectrum over multiple Brillouin zones. We find excellent agreement between our numerical and experimental results that extend to all measurement temperatures. Notable features of our phonon spectra include a number of steeply dispersive modes, nonmonotonic dispersion features, and specific phonon anticrossings, which we relate to the mode eigenvectors. By calculating the magnetic interactions within DFT and studying the effects of different phonon modes on the superexchange paths, we discuss the possibility of observing spin-phonon hybridization effects in experiments performed both in and out of equilibrium.
Authors
- Aleksandar Razpopov (ORCID: https://orcid.org/0009-0009-6935-3297)
- Christian Rüegg (ORCID: https://orcid.org/0000-0003-0139-7786)
- M. Fujita (ORCID: https://orcid.org/0000-0001-8330-8040)
- B. Normand (ORCID: https://orcid.org/0000-0002-1060-2238)
- С. Е. Никитин (ORCID: https://orcid.org/0000-0001-8495-1038)
- Martin Mourigal (ORCID: https://orcid.org/0000-0003-2772-8440)
- Leonie Spitz (ORCID: https://orcid.org/0000-0002-1028-3548)
- Kazuki Iida (ORCID: https://orcid.org/0000-0001-9989-9965)
- Ryoichi Kajimoto (ORCID: https://orcid.org/0000-0003-4845-5947)
- Sananda Biswas (ORCID: https://orcid.org/0000-0002-3323-2057)
- Roser Valentí (ORCID: https://orcid.org/0000-0003-0497-1165)
- H. Lane (ORCID: https://orcid.org/0009-0005-0391-4750)
- Masatoshi Arai (ORCID: https://orcid.org/0000-0001-8688-4238)
Institutions
- Goethe University Frankfurt (DE)
- University of Geneva (CH)
- Japan Atomic Energy Agency (JP)
- Georgia Institute of Technology (US)
- University of St Andrews (GB)
- European Spallation Source (SE)
- Paul Scherrer Institute (CH)
- University of Manchester (GB)
- ETH Zurich (CH)
- Comprehensive Research Organization for Science and Society (JP)
- Institute for Materials Research, Tohoku University
- École Polytechnique Fédérale de Lausanne (CH)
Publication Details
- Journal
- Physical review. B./Physical review. B
- Published
- 2025-09-29
- DOI
- https://doi.org/10.1103/jz36-8kz9
- Citations
- 1
- Primary Topic
- Physics of Superconductivity and Magnetism
- Type
- article
- Field-Weighted Citation Impact
- 1.26