Abstract
Collective excitations of bound electron-hole pairs—known as excitons—are ubiquitous in condensed matter, emerging in systems as diverse as band semiconductors, molecular crystals, and proteins. Recently, their existence in strongly correlated electron materials has attracted increasing interest due to the excitons’ unique coupling to spin and orbital degrees of freedom. The non-equilibrium driving of such dressed quasiparticles offers a promising platform for realizing unconventional many-body phenomena and phases beyond thermodynamic equilibrium. Here, we achieve this in the van der Waals correlated insulator NiPS3 by photoexciting its newly discovered spin–orbit-entangled excitons that arise from Zhang-Rice states. By monitoring the time evolution of the terahertz conductivity, we observe the coexistence of itinerant carriers produced by exciton dissociation and a long-wavelength antiferromagnetic magnon that coherently precesses in time. These results demonstrate the emergence of a transient metallic state that preserves long-range antiferromagnetism, a phase that cannot be reached by simply tuning the temperature. More broadly, our findings open an avenue toward the exciton-mediated optical manipulation of magnetism.
Original language | English |
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Article number | 4837 |
Journal | Nature communications |
Volume | 12 |
Issue number | 1 |
DOIs | |
Publication status | Published - 2021 Dec 1 |
Bibliographical note
Funding Information:We acknowledge useful discussions with Jonathan Pelliciari and Ki Hoon Lee. Work at MIT was supported by the US Department of Energy, BES DMSE (data taking and analysis), and by the Gordon and Betty Moore Foundation’s EPiQS Initiative grant GBMF9459 (instrumentation). C.A.B. and E.B. acknowledge additional support from the National Science Foundation Graduate Research Fellowship under Grant No. 1745302 and the Swiss National Science Foundation under fellowships P2ELP2-172290 and P400P2-183842, respectively. D.M. and T.S. are supported by a US Department of Energy grant DE-SC0008739, and T.S., in part, by a Simons Investigator award from the Simons Foundation. H.C.P. is supported by a Pappalardo Fellowship at MIT and a Croucher Foundation Fellowship. Work at IBS-CCES was supported by the Institute for Basic Science (IBS) in Korea (Grant No. IBS-R009-G1) and work at CQM was supported by the Leading Researcher Program of the National Research Foundation of Korea (Grant No. 2020R1A3B2079375). J.H.K. acknowledges support from the National Research Foundation of Korea (NRF) grants funded by the Ministry of Science, ICT, and Future Planning (MSIP) of Korea (NRL Program No. NRF-2019R1I1A2A01062306, SRC Program No. NRF-2017R1A5A1014862).
Publisher Copyright:
© 2021, The Author(s).
All Science Journal Classification (ASJC) codes
- Chemistry(all)
- Biochemistry, Genetics and Molecular Biology(all)
- General
- Physics and Astronomy(all)