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Title: Terahertz parametric amplification as a reporter of exciton condensate dynamics

Journal Article · · Nature Materials
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [5]; ORCiD logo [5]; ORCiD logo [3];  [4]; ORCiD logo [6];  [7]; ORCiD logo [3];  [8]; ORCiD logo [4]
  1. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Univ. of San Diego, La Jolla, CA (United States); SLAC
  2. Harvard Univ., Cambridge, MA (United States)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  4. Univ. of San Diego, La Jolla, CA (United States)
  5. Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany)
  6. Univ. of San Diego, La Jolla, CA (United States); Hong Kong University of Science and Technology (HKUST) (Hong Kong)
  7. Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany); Flatiron Institute, New York, NY (United States)
  8. Harvard Univ., Cambridge, MA (United States); Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)
+ Show Author Affiliations

Condensates are a hallmark of emergence in quantum materials with superconductors and charge density wave as prominent examples. An excitonic insulator (EI) is an intriguing addition to this library, exhibiting spontaneous condensation of electron-hole pairs. However, condensate observables can be obscured through parasitic coupling to the lattice. Time-resolved terahertz (THz) spectroscopy can disentangle such obscurants through measurement of the quantum dynamics. We target Ta2NiSe5, a putative room-temperature EI where electron-lattice coupling dominates the structural transition (Tc = 326 K), hindering identification of excitonic correlations. A pronounced increase in the THz reflectivity manifests following photoexcitation and exhibits a BEC-like temperature dependence. This occurs well below the Tc, suggesting a novel approach to monitor exciton condensate dynamics. Nonetheless, dynamic condensate-phonon coupling remains as evidenced by peaks in the enhanced reflectivity spectrum at select infrared-active phonon frequencies. This indicates that parametric reflectivity enhancement arises from phonon squeezing, validated using Fresnel-Floquet theory and density functional calculations. In conclusion, our results highlight that coherent dynamics can drive parametric stimulated emission with concomitant possibilities, including entangled THz photon generation.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC); European Research Council (ERC)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
2323401
Journal Information:
Nature Materials, Journal Name: Nature Materials Vol. 23; ISSN 1476-1122
Publisher:
Springer NatureCopyright Statement
Country of Publication:
United States
Language:
English

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