Ultrafast optical melting of trimer superstructure in layered 1T′-TaTe2

Siddiqui, Khalid M.; Durham, Daniel B.; Cropp, Frederick; Ophus, Colin; Rajpurohit, Sangeeta; Zhu, Yanglin; Carlström, Johan D.; Stavrakas, Camille; Mao, Zhiqiang; Raja, Archana; Musumeci, Pietro; Tan, Liang Z.; Minor, Andrew M.; Filippetto, Daniele; Kaindl, Robert A.

doi:10.1038/s42005-021-00650-z

Title: Ultrafast optical melting of trimer superstructure in layered 1T′-TaTe2

Journal Article · 01 July 2021 · Communications Physics

DOI: https://doi.org/10.1038/s42005-021-00650-z · OSTI ID:1805053

Siddiqui, Khalid M.;

;

; Rajpurohit, Sangeeta; Zhu, Yanglin; Carlström, Johan D.;

;

; Raja, Archana;

;

; Minor, Andrew M.;

;

Abstract Quasi-two-dimensional transition-metal dichalcogenides are a key platform for exploring emergent nanoscale phenomena arising from complex interactions. Access to the underlying degrees-of-freedom on their natural time scales motivates the use of advanced ultrafast probes sensitive to self-organised atomic-scale patterns. Here, we report the ultrafast investigation of TaTe ₂ , which exhibits unique charge and lattice trimer order characterised by a transition upon cooling from stripe-like chains into a (3 × 3) superstructure of trimer clusters. Utilising MeV-scale ultrafast electron diffraction, we capture the photo-induced TaTe ₂ structural dynamics – exposing a rapid ≈ 1.4 ps melting of its low-temperature ordered state followed by recovery via thermalisation into a hot cluster superstructure. Density-functional calculations indicate that the initial quench is triggered by intra-trimer Ta charge transfer which destabilises the clusters, unlike melting of charge density waves in other TaX ₂ compounds. Our work paves the way for further exploration and ultimately rapid optical and electronic manipulation of trimer superstructures.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1805053

Journal Information:: Communications Physics, Journal Name: Communications Physics Journal Issue: 1 Vol. 4; ISSN 2399-3650

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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