Resonance-induced anomalies in temperature-dependent Raman scattering of PdSe2

Omar Abdul-Aziz, Daniel Wolverson, Charles J. Sayers, Ettore Carpene, Fulvio Parmigiani, Hamoon Hedayat, Paul H.M. van Loosdrecht

Research output: Contribution to journalArticlepeer-review

Abstract

We report a comprehensive Raman study of the phonon behavior in PdSe2 in the temperature range of 5 K to 300 K. A remarkable change in the Raman spectrum is observed at 120 K: a significant enhancement of the out-of-plane phonon A1g mode, accompanied by a suppression of the in-plane A2g and B21g modes. This intriguing behavior is attributed to a temperature-dependent resonant excitation effect. The results are supported by density functional theory (DFT) calculations, which demonstrate that the electron-phonon coupling for the phonon modes varies and is strongly associated with the relevant electronic states. Furthermore, nonlinear frequency shifts are identified in all modes, indicating the decay of an optical phonon into multiple acoustic phonons. The study of Raman emission reported here, complemented by linear optical spectroscopy, reveals an unexpected scenario for the vibrational properties of PdSe2 that holds substantial promise for future applications in PdSe2-based optoelectronics.

Original languageEnglish
Pages (from-to)11402-11411
Number of pages10
JournalJournal of Materials Chemistry C
Volume12
Issue number30
Early online date24 Jun 2024
DOIs
Publication statusPublished - 14 Aug 2024

Data Availability Statement

The experimental data are accessible through: https://doi.org/10.5281/zenodo.10424154. Inputs to the computational codes are available free of charge at https://doi.org/10.15125/BATH-01356.

Funding

The authors acknowledge financial support by the Deutsche Forschungsgemeinschaft (DFG) through project German Research Foundation via project No. 277146847 \u2013 CRC 1238: Control and Dynamics of quantum Materials. Computational work was performed on the University of Bath's High Performance Computing Facility and was supported by the EU Horizon 2020 OCRE/GEANT project \u201CCloud funding for research\u201D. We acknowledge the financial support from the Italian Ministry of University and Research (Grant No. PRIN 2017BZPKSZ).

FundersFunder number
GEANT
Deutsche Forschungsgemeinschaft
EU Horizon 2020 OCRE
Deutsche Forschungsgemeinschaft (DFG)277146847 – CRC 1238
Ministero dell’Istruzione, dell’Università e della RicercaPRIN 2017BZPKSZ
Ministero dell’Istruzione, dell’Università e della Ricerca

    ASJC Scopus subject areas

    • General Chemistry
    • Materials Chemistry

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    • Cloud funding for Research

      Wolverson, D. (PI)

      25/01/2212/10/28

      Project: Research-related funding

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