Ultrafast Dynamics of Coherent Phonon Modes in Excitonic Insulator Ta$_2$NiSe$_5$

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Hauptverfasser: Arora, Vikas, Pal, Sukanya, Harnagea, Luminita, Muthu, D. V. S., Sood, A K
Format: Preprint
Veröffentlicht: 2024
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author Arora, Vikas
Pal, Sukanya
Harnagea, Luminita
Muthu, D. V. S.
Sood, A K
author_facet Arora, Vikas
Pal, Sukanya
Harnagea, Luminita
Muthu, D. V. S.
Sood, A K
contents The spontaneous condensation of excitons in the excitonic insulating phase has been reported in Ta$_2$NiSe$_5$ below 325 K. In this context, we present the temperature-dependent optical pump optical probe spectroscopy of Ta$_2$NiSe$_5$, with a focus on coherent phonon dynamics. In addition to the fast relaxation process involving excitonic recombination, we observe a systematic behavior for the slow relaxation process associated with the relaxation of hot phonons. The asymmetry parameter and cubic anharmonicity of the 3 THz mode demonstrate the structural transition across T$_C$=325 K, whereas the order parameter nature and asymmetry of 2 THz modes reveal its coupling with the excitonic phase of Ta$_2$NiSe$_5$. Coherent phonon modes display less anharmonicity compared to the corresponding Raman modes. Continuous Wavelet Transform (CWT) reveals that the peak time t$_{peak}$ of phonons is similar for all modes except the 3 THz mode. The temperature dependence of t$_{peak}$ for the M3 mode exhibits a possible role of excitonic condensate below T$_c$ in the formation of quasiparticle (phonon). CWT analysis supports the time-dependent asymmetry of the M3 mode caused by photoexcited carriers. This study illustrates the role of photoexcited carriers in depicting a structural transition and dressing of coherent phonons and, hence, demonstrating many-body effects.
format Preprint
id arxiv_https___arxiv_org_abs_2411_18839
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Ultrafast Dynamics of Coherent Phonon Modes in Excitonic Insulator Ta$_2$NiSe$_5$
Arora, Vikas
Pal, Sukanya
Harnagea, Luminita
Muthu, D. V. S.
Sood, A K
Materials Science
The spontaneous condensation of excitons in the excitonic insulating phase has been reported in Ta$_2$NiSe$_5$ below 325 K. In this context, we present the temperature-dependent optical pump optical probe spectroscopy of Ta$_2$NiSe$_5$, with a focus on coherent phonon dynamics. In addition to the fast relaxation process involving excitonic recombination, we observe a systematic behavior for the slow relaxation process associated with the relaxation of hot phonons. The asymmetry parameter and cubic anharmonicity of the 3 THz mode demonstrate the structural transition across T$_C$=325 K, whereas the order parameter nature and asymmetry of 2 THz modes reveal its coupling with the excitonic phase of Ta$_2$NiSe$_5$. Coherent phonon modes display less anharmonicity compared to the corresponding Raman modes. Continuous Wavelet Transform (CWT) reveals that the peak time t$_{peak}$ of phonons is similar for all modes except the 3 THz mode. The temperature dependence of t$_{peak}$ for the M3 mode exhibits a possible role of excitonic condensate below T$_c$ in the formation of quasiparticle (phonon). CWT analysis supports the time-dependent asymmetry of the M3 mode caused by photoexcited carriers. This study illustrates the role of photoexcited carriers in depicting a structural transition and dressing of coherent phonons and, hence, demonstrating many-body effects.
title Ultrafast Dynamics of Coherent Phonon Modes in Excitonic Insulator Ta$_2$NiSe$_5$
topic Materials Science
url https://arxiv.org/abs/2411.18839