Laser-Induced Cooperative Transition in Molecular Electronic Crystal

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2021-08-16
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Hu, Yong
Huang, C.
Kim, R.
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Iowa State University Digital Repository, Ames IA (United States)
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Wang, Jigang
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Ames National Laboratory

Ames National Laboratory is a government-owned, contractor-operated national laboratory of the U.S. Department of Energy (DOE), operated by and located on the campus of Iowa State University in Ames, Iowa.

For more than 70 years, the Ames National Laboratory has successfully partnered with Iowa State University, and is unique among the 17 DOE laboratories in that it is physically located on the campus of a major research university. Many of the scientists and administrators at the Laboratory also hold faculty positions at the University and the Laboratory has access to both undergraduate and graduate student talent.

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Physics and Astronomy
Physics and astronomy are basic natural sciences which attempt to describe and provide an understanding of both our world and our universe. Physics serves as the underpinning of many different disciplines including the other natural sciences and technological areas.
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The competing and non-equilibrium phase transitions, involving dynamic tunability of cooperative electronic and magnetic states in strongly correlated materials, show great promise in quantum sensing and information technology. To date, the stabilization of transient states is still in the preliminary stage, particularly with respect to molecular electronic solids. Here, a dynamic and cooperative phase in potassium-7,7,8,8-tetracyanoquinodimethane (K-TCNQ) with the control of pulsed electromagnetic excitation is demonstrated. Simultaneous dynamic and coherent lattice perturbation with 8 ns pulsed laser (532 nm, 15 MW cm−2, 10 Hz) in such a molecular electronic crystal initiates a stable long-lived (over 400 days) conducting paramagnetic state (≈42 Ωcm), showing the charge–spin bistability over a broad temperature range from 2 to 360 K. Comprehensive noise spectroscopy, in situ high-pressure measurements, electron spin resonance (ESR), theoretical model, and scanning tunneling microscopy/spectroscopy (STM/STS) studies provide further evidence that such a transition is cooperative, requiring a dedicated charge–spin–lattice decoupling to activate and subsequently stabilize nonequilibrium phase. The cooperativity triggered by ultrahigh-strain-rate (above 106 s−1) pulsed excitation offers a collective control toward the generation and stabilization of strongly correlated electronic and magnetic orders in molecular electronic solids and offers unique electro-magnetic phases with technological promises.
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This is a manuscript of an article published as Hu, Yong, Dasharath Adhikari, Andrew Tan, Xi Dong, Taishan Zhu, Xiaoyu Wang, Yulong Huang et al. "Laser‐Induced Cooperative Transition in Molecular Electronic Crystal." Advanced Materials 33, no. 39 (2021): 2103000. DOI: 10.1002/adma.202103000. Copyright 2021 Wiley-VCH GmbH. Posted with permission. DOE Contract Number(s): SC0018631; SC0019120; AC02-07CH11358; AC02-05CH11231.
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