Ultrafast melting and recovery of collective order in the excitonic insulator Ta2NiSe5

Hope M. Bretscher, Paolo Andrich (), Prachi Telang, Anupam Singh, Luminita Harnagea, A. K. Sood and Akshay Rao ()
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Hope M. Bretscher: University of Cambridge
Paolo Andrich: University of Cambridge
Prachi Telang: Indian Institute of Science Education and Research
Anupam Singh: Indian Institute of Science Education and Research
Luminita Harnagea: Indian Institute of Science Education and Research
A. K. Sood: Indian Institute of Science
Akshay Rao: University of Cambridge

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract The layered chalcogenide Ta2NiSe5 has been proposed to host an excitonic condensate in its ground state, a phase that could offer a unique platform to study and manipulate many-body states at room temperature. However, identifying the dominant microscopic contribution to the observed spontaneous symmetry breaking remains challenging, perpetuating the debate over the ground state properties. Here, using broadband ultrafast spectroscopy we investigate the out-of-equilibrium dynamics of Ta2NiSe5 and demonstrate that the transient reflectivity in the near-infrared range is connected to the system’s low-energy physics. We track the status of the ordered phase using this optical signature, establishing that high-fluence photoexcitations can suppress this order. From the sub-50 fs quenching timescale and the behaviour of the photoinduced coherent phonon modes, we conclude that electronic correlations provide a decisive contribution to the excitonic order formation. Our results pave the way towards the ultrafast control of an exciton condensate at room temperature.

Date: 2021
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DOI: 10.1038/s41467-021-21929-3

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