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Strongly Coupled Coherent Phonons in Single-Layer MoS <sub/>2</sub>

DOI:10.1021/acsnano.0c00309 期刊:ACS Nano 出版年份:2020 更新时间:2025-09-23 15:21:01
摘要: We present a transient absorption setup combining broadband detection over the visible-UV range with high temporal resolution (~20fs) which is ideally suited to trigger and detect vibrational coherences in different classes of materials. We generate and detect coherent phonons (CPs) in single layer (1L) MoS2, as a representative semiconducting 1L-Transition Metal Dichalcogenide (TMD), where the confined dynamical interaction between excitons and phonons is unexplored. The coherent oscillatory motion of the out-of-plane A'1 phonons, triggered by the ultrashort laser pulses, dynamically modulates the excitonic resonances on a timescale of few tens fs. We observe an enhancement by almost two orders of magnitude of the CP amplitude when detected in resonance with the C exciton peak, combined with a resonant enhancement of CP generation efficiency. Ab Initio calculations of the change in 1L-MoS2 band structure induced by the A'1 phonon displacement confirm a strong coupling with the C exciton. The resonant behavior of the CP amplitude follows the same spectral profile of the calculated Raman susceptibility tensor. These results explain the CP generation process in 1L-TMDs and demonstrates that CP excitation in 1L-MoS2 can be described as a Raman-like scattering process.
作者: Chiara Trovatello,Henrique P.C. Miranda,Alejandro Molina-Sanchez,Rocio Borrego-Varillas,Cristian Manzoni,Luca Moretti,Lucia Ganzer,Margherita Maiuri,Junjia Wang,Dumitru Dumcenco,Andras Kis,Ludger Wirtz,Andrea Marini,Giancarlo Soavi,Andrea C Ferrari,Giulio Cerullo,Davide Sangalli,Stefano Dal Conte
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To understand the mechanism underlying the coherent phonon (CP) generation process and to identify the physical parameters (such as the pump pulse photon energy) that allow their efficient excitation in single-layer MoS2.

The study demonstrated that A'1 optical phonon modes strongly couple with the C exciton, giving rise to a temporal modulation of the TA response over a broad energy range around this excitonic peak. The excitation profile of such coherent oscillations follows the energy dependence of the Raman tensor, proving that the lattice coherence in 1L-MoS2 can be described as a Raman-like excitation mechanism. Ab Initio calculations of the band structure for displaced atoms configuration confirm the strong coupling between C exciton and A'1 phonons.

The study was restricted to a narrow energy range (~100meV) around the A exciton, making it difficult to gain information on how CP excitation affects the whole band structure. The phonon dephasing time τdeph=1.7±0.2ps is almost three times smaller than that measured at the same temperature for CP in exfoliated 1L-WSe2, possibly due to different defect concentration in exfoliated and CVD-grown 1L-TMDs.

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