Ultrafast Science, Volume. 3, Issue 1, 0041(2023)

Nonlocal Probing of Amplitude Mode Dynamics in Charge-Density-Wave Phase of EuTe4

Ranjana Rathore1,2、*, Himanshu Singhal1,2, Vivek Dwij3,4, Mayanak K Gupta2,5, Abhishek Pathak3, Juzer Ali Chakera1,2, Ranjan Mittal2,5, Aditya Prasad Roy3, Arun Babu3, Ruta Kulkarni4, A Thamizhavel4, Ayman H Said6, and Dipanshu Bansal3,7、*
Author Affiliations
  • 1Laser Plasma Division, Raja Ramanna Centre for Advanced Technology, Indore, MP 452013, India.
  • 2Homi Bhabha National Institute, Training School Complex, Anushaktinagar, Mumbai, MH 400094, India.
  • 3Department of Mechanical Engineering, Indian Institute of Technology Bombay, Mumbai, MH 400076, India.
  • 4Department of Condensed Matter Physics & Materials Science, Tata Institute of Fundamental Research, Mumbai, MH 400005, India.
  • 5Solid State Physics Division, Bhabha Atomic Research Centre, Mumbai, MH 400085, India.
  • 6Advanced Photon Source, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, IL 60439, USA.
  • 7Center for Research in Nano Technology and Science, Indian Institute of Technology Bombay, Mumbai, MH 400076, India.
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    Amplitude mode is collective excitation emerging from frozen lattice distortions below the charge-density-wave (CDW) transition temperature TCDW and relates to the order parameter. Generally, the amplitude mode is non-polar (symmetry-even) and does not interact with incoming infrared photons. However, if the amplitude mode is polar (symmetry-odd), it can potentially couple with incoming photons, thus forming a coupled phonon–polariton quasiparticle that can travel with light-like speed beyond the optically excited region. Here, we present the amplitude mode dynamics far beyond the optically excited depth of ∼150 nm in the CDW phase of ∼10-μm-thick single-crystal EuTe4 using time-resolved x-ray diffraction. The observed oscillations of the CDW peak, triggered by photoexcitation, occur at the amplitude mode frequency ωAM. However, the underdamped oscillations and their propagation beyond the optically excited depth are at odds with the observation of the overdamped nature of the amplitude mode measured using meV-resolution inelastic x-ray scattering and polarized Raman scattering. The ωAM is found to decrease with increasing fluence owing to a rise in the sample temperature, which is independently confirmed using polarized Raman scattering and ab-initio molecular dynamics simulations. We rationalize the above observations by explicitly calculating two coupled quasiparticles—phonon–polariton and exciton–polariton. Our data and simulations cannot conclusively confirm or rule out the one but point toward the likely origin from propagating phonon–polariton. The observed non-local behavior of amplitude mode thus provides an opportunity to engineer material properties at a substantially faster time scale with optical pulses.

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    Ranjana Rathore, Himanshu Singhal, Vivek Dwij, Mayanak K Gupta, Abhishek Pathak, Juzer Ali Chakera, Ranjan Mittal, Aditya Prasad Roy, Arun Babu, Ruta Kulkarni, A Thamizhavel, Ayman H Said, Dipanshu Bansal. Nonlocal Probing of Amplitude Mode Dynamics in Charge-Density-Wave Phase of EuTe4[J]. Ultrafast Science, 2023, 3(1): 0041

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    Paper Information

    Category: Research Articles

    Received: Apr. 3, 2023

    Accepted: Aug. 1, 2023

    Published Online: Dec. 4, 2023

    The Author Email: Rathore Ranjana (ranjana@rrcat.gov.in), Bansal Dipanshu (dipanshu@iitb.ac.in)

    DOI:10.34133/ultrafastscience.0041

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