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Possible observation of parametrically amplified coherent phasons in K0.3MoO3 using time-resolved extreme-ultraviolet angle-resolved photoemission spectroscopy

H. Y. Liu, I. Gierz, J. C. Petersen, S. Kaiser, A. Simoncig, A. L. Cavalieri, C. Cacho, I. C. E. Turcu, E. Springate, F. Frassetto, L. Poletto, S. S. Dhesi, Z.-A. Xu, T. Cuk, R. Merlin, and A. Cavalleri
Phys. Rev. B 88, 045104 – Published 2 July 2013

Abstract

We use time- and angle-resolved photoemission spectroscopy in the extreme ultraviolet to measure the time- and momentum-dependent electronic structures of photoexcited K0.3MoO3. Prompt depletion of the charge-density wave condensate launches coherent oscillations of the amplitude mode, observed as a 1.7-THz-frequency modulation of the bonding band position. In contrast, the antibonding band oscillates at about half this frequency. We attribute these oscillations to coherent excitation of phasons via parametric amplification of phase fluctuations.

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  • Received 25 June 2012

DOI:https://doi.org/10.1103/PhysRevB.88.045104

©2013 American Physical Society

Authors & Affiliations

H. Y. Liu1,*, I. Gierz1, J. C. Petersen1,2, S. Kaiser1, A. Simoncig1, A. L. Cavalieri1, C. Cacho3, I. C. E. Turcu3, E. Springate3, F. Frassetto4, L. Poletto4, S. S. Dhesi5, Z.-A. Xu6, T. Cuk7, R. Merlin8, and A. Cavalleri1,2,†

  • 1Max Planck Department for Structural Dynamics, CFEL, Hamburg, Germany
  • 2Department of Physics, Clarendon Laboratory, University of Oxford, United Kingdom
  • 3Central Laser Facility, STFC Rutherford Appleton Laboratory, United Kingdom
  • 4CNR-Institute for Photonics and Nanotechnologies, Padova, Italy
  • 5Diamond Light Source Ltd., Chilton, United Kingdom
  • 6Department of Physics, Zhejiang University, Hangzhou, China
  • 7Materials Sciences Division and Physical Biosciences Division, Lawrence Berkeley National Laboratory, University of California, Berkeley, California 94720-1460, USA
  • 8Department of Physics, University of Michigan, Ann Arbor, Michigan 48109-1040, USA

  • *haiyun.liu@mpsd.cfel.de
  • andrea.cavalleri@mpsd.cfel.de

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Vol. 88, Iss. 4 — 15 July 2013

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Images

  • Figure 1
    Figure 1
    Crystal structure and static band properties of K0.3MoO3. (a) Linear chains of MoO6 octahedra form slabs, which make up the b-d cleavage plane. (b) Upper panel: static ARPES intensity map at t = −50 fs and 20 K as a function of binding energy and momentum. To bring out the underlying band structure, we also plot 2I/E2 (lower panel). The dashed blue and red lines locate the antibonding (A1 and A2) and bonding (B1 and B2) bands. Vertical arrows mark the different Fermi wave vectors. The photoelectron momentum is measured along the cut direction indicated on the zone map shown in the inset. (c) Individual EDCs used to produce the intensity map. EDCs at the Fermi momenta are highlighted and are labeled.Reuse & Permissions
  • Figure 2
    Figure 2
    Response to impulsive excitation by a femtosecond laser pulse. (a) Photoemission intensity maps at 50 and 250 fs, shown on the same color scale. The arrows mark the centers of increased intensity above EF. (b) Photoinduced changes in the EDCs at kF(B1) and kF(A2) with intensity transferred from the valence bands to EF as the CDW phase melts in response to the excitation pulse.Reuse & Permissions
  • Figure 3
    Figure 3
    Time evolution of the electronic structure near the gap edge for each Fermi wave vector as labeled. Symbols: intensity near EF, integrated from 50 to +100 meV. Solid lines: fits to the integrated intensity. The model contains an exponential decay plus a sine function with frequencies of 1.7 THz (a), 0.8 THz (b), or both (c and d).Reuse & Permissions
  • Figure 4
    Figure 4
    Collective excitations of the CDW state. (a) Free energy of the ground state (blue) and the excited state (red) as a function of amplitude |Δ| and phase Φ of the complex order parameter. As the minimum of the free energy in the excited state is located at a different |Δ|'s compared to the ground state, amplitude oscillations are excited (yellow arrows). (b) Idealized dispersion and snapshots of the charge density of an amplitude mode (red) and phase mode (blue). Arrows indicate a parametric generation process from ωA(0) to ωP(±qP)=ωA(0)/2. (c) Coherent phase-mode oscillations obtained by solving the coupled differential equations given in the text for different ratios of ωA/ωP. (d) Dispersion (red curves) and Fermi-surface nesting (green arrow) in the presence of a time-dependent phase.Reuse & Permissions
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