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  Terahertz parametric amplification as a reporter of exciton condensate dynamics

Haque, S. R. U., Michael, M. H., Zhu, J., Zhang, Y., Windgätter, L., Latini, S., et al. (2024). Terahertz parametric amplification as a reporter of exciton condensate dynamics. Nature Materials. doi:10.1038/s41563-023-01755-2.

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Item Permalink: https://hdl.handle.net/21.11116/0000-000D-018B-5 Version Permalink: https://hdl.handle.net/21.11116/0000-000E-1F51-5
Genre: Journal Article

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Supplementary information & Source data: Supplementary Information (pdf): Suppmentary Figs, 1–18, refs. 58–60 and sections on phonon squeezing in detail, telation between phonon squeezing and reflectivity enhancement, penetration depth mismatch analysis, thermal effect analysis, possibility of thermal phonon shift as an alternative interpretation, and oossibility of THz emission. | Reporting Summary (pdf) | Source data: Source Data Fig. 1-3 (xlsx); Source Data Extended Data Table. 1 (xlsx); Source Data Extended Data Fig. 1, 3-6 (xlsx)
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 Creators:
Haque, S. R. U.1, Author
Michael, M. H.2, Author
Zhu, J.3, Author
Zhang, Y.1, Author
Windgätter, L.4, Author           
Latini, S.4, Author           
Wakefield, J. P.3, Author
Zhang, G.-F.1, Author
Zhang, J.1, 5, Author
Rubio, A.4, 6, Author           
Checkelsky, J. G.3, Author
Demler, E.2, 7, Author
Averitt, R. D.1, Author
Affiliations:
1Department of Physics, University of California San Diego, ou_persistent22              
2Department of Physics, Harvard University, ou_persistent22              
3Department of Physics, Massachusetts Institute of Technology, ou_persistent22              
4Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
5Department of Physics, The Hong Kong University of Science and Technology, ou_persistent22              
6Center for Computational Quantum Physics, The Flatiron Institute, ou_persistent22              
7Institute for Theoretical Physics, ETH Zürich, ou_persistent22              

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 Abstract: Condensates are a hallmark of emergence in quantum materials such as superconductors and charge density waves. Excitonic insulators are 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. Here we employ nonlinear terahertz spectroscopy to disentangle such obscurants through measurement of the quantum dynamics. We target Ta2NiSe5, a putative room-temperature excitonic insulator in which electron–lattice coupling dominates the structural transition (Tc = 326 K), hindering identification of excitonic correlations. A pronounced increase in the terahertz reflectivity manifests following photoexcitation and exhibits a Bose–Einstein condensation-like temperature dependence well below the Tc, suggesting an approach to monitor the exciton condensate dynamics. Nonetheless, dynamic condensate–phonon coupling remains as evidenced by peaks in the enhanced reflectivity spectrum at select infrared-active phonon frequencies, indicating that parametric reflectivity enhancement arises from phonon squeezing. Our results highlight that coherent dynamics can drive parametric stimulated emission.

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Language(s): eng - English
 Dates: 2022-06-272023-11-062024-01-032024
 Publication Status: Issued
 Pages: -
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: arXiv: 2304.09249
DOI: 10.1038/s41563-023-01755-2
 Degree: -

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Project name : We thank D. Hsieh, P. Narang, M. K. Liu and A. Kogar for fruitful discussions. S.R.U.H., M.H.M., J. Zhu, Y.Z., J.P.W., G.-F.Z., J. Zhang, J.G.C., E.D. and R.D.A. acknowledge support from the DARPA ‘Driven Nonequilibrium Quantum Systems’ (DRINQS) programme under award number D18AC00014. E.D. acknowledges support from SNSF project 200021_212899 and ARO grant number W911NF-21-1-0184. L.W., S.L. and A.R. acknowledge support from the European Research Council (ERC-2015-AdG694097), the Cluster of Excellence ‘Advanced Imaging of Matter’ (AIM), Grupos Consolidados (IT1249-19) and Deutsche Forschungsgemeinschaft (DFG) – SFB-925 – project 170620586. A.R. also thanks the Flatiron Institute, a division of the Simons Foundation.
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Title: Nature Materials
  Abbreviation : Nat. Mater.
Source Genre: Journal
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Publ. Info: London, UK : Nature Pub. Group
Pages: - Volume / Issue: - Sequence Number: - Start / End Page: - Identifier: ISSN: 1476-1122
CoNE: https://pure.mpg.de/cone/journals/resource/111054835734000