Spectrally Resolving the Phase and Amplitude of Coherent Phonons in the Charge Density Wave State of 1T-TaSe2

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Abstract

The excitation and detection of coherent phonons have given unique insights into the condensed matter, in particular for materials with strong electron–phonon coupling. A study of coherent phonons is reported in the layered charge density wave (CDW) compound 1T-TaSe 2 performed using transient broadband reflectivity spectroscopy, in the photon energy range 1.75–2.65 eV. Several intense and long-lasting (>20 ps) oscillations, arising from the CDW superlattice reconstruction, are observed allowing for detailed analysis of the spectral dependence of their amplitude and phase. For energies above 2.4 eV, where transitions involve Ta d-bands, the CDW amplitude mode at 2.19 THz is found to dominate the coherent response. At lower energies, instead, beating arises between additional frequencies, with a particularly intense mode at 2.95 THz. Interestingly, the spectral analysis reveals a π phase shift at 2.4 eV. Results are discussed considering the selective coupling of specific modes to energy bands involved in the optical transitions seen in steady-state reflectivity. The work demonstrates how coherent phonon spectroscopy can distinguish and resolve optical states strongly coupled to the CDW order and provide additional information normally hidden in conventional steady-state techniques.

Original languageEnglish
Article number2200362
JournalAdvanced Optical Materials
Volume10
Issue number14
DOIs
Publication statusPublished - 18 Jul 2022

Keywords

  • TaSe
  • charge density waves
  • coherent phonons
  • transition metal dichalcogenides
  • ultrafast spectroscopy

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Atomic and Molecular Physics, and Optics

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