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Strongly Coupled Coherent Phonons in Single-Layer MoS2.

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  • 1Dipartimento di Fisica, Politecnico di Milano, Piazza L. da Vinci 32, I-20133 Milano, Italy.

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Summary

We developed a new setup to study vibrational coherences in materials. This system successfully generated and detected coherent phonons in single-layer molybdenum disulfide (MoS2), revealing strong exciton-phonon coupling.

Keywords:
ab initio calculationcoherent phononsexciton−phonon interactiontransient absorption spectroscopytransition metal dichalcogenides

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Spectroscopy

Background:

  • Understanding exciton-phonon interactions is crucial for exploring dynamical processes in low-dimensional materials.
  • Single-layer transition metal dichalcogenides (TMDs) exhibit unique optoelectronic properties influenced by coupled electron-lattice dynamics.
  • Previous studies have not fully explored the interplay between excitons and coherent phonons in semiconducting 1L-TMDs.

Purpose of the Study:

  • To investigate the generation and detection of coherent phonons (CPs) in single-layer molybdenum disulfide (1L-MoS2).
  • To explore the dynamical interaction between excitons and phonons in 1L-MoS2 using a high-temporal-resolution transient absorption setup.
  • To elucidate the mechanism of CP generation and its resonant enhancement in 1L-TMDs.

Main Methods:

  • Development of a transient absorption setup with broadband visible-UV detection and femtosecond temporal resolution (∼20 fs).
  • Generation and detection of coherent phonons (CPs) in single-layer MoS2 triggered by ultrashort laser pulses.
  • Utilizing ab initio calculations to study the band structure changes induced by A'1 phonon displacement and comparing with experimental Raman susceptibility.

Main Results:

  • Observed coherent oscillatory motion of out-of-plane A'1 phonons modulating excitonic resonances on a tens-of-femtoseconds timescale.
  • Demonstrated a significant enhancement (nearly 2 orders of magnitude) of the CP amplitude when detected in resonance with the C exciton peak.
  • Confirmed resonant enhancement of CP generation efficiency and strong coupling between the C exciton and A'1 phonon displacement via calculations.

Conclusions:

  • The study explains the CP generation process in 1L-TMDs, highlighting the significant role of exciton-phonon coupling.
  • CP excitation in 1L-MoS2 can be effectively described as a Raman-like scattering process.
  • The developed transient absorption setup is well-suited for probing vibrational coherences and exciton-phonon dynamics in various materials.