Title: Laser-Induced Cooperative Transition in Molecular Electronic Crystal

Journal Article · · Advanced Materials
 [1];  [2];  [3];  [3];  [4];  [2];  [2];  [2];  [5];  [6];  [6];  [6];  [7];  [7];  [3];  [2];  [8];  [9];  [9];  [9] more »;  [2];  [2];  [2];  [7];  [8];  [2];  [2];  [2];  [4];  [3];  [2] « less
  1. State Univ. of New York (SUNY), Buffalo, NY (United States); University at Buffalo
  2. State Univ. of New York (SUNY), Buffalo, NY (United States)
  3. Michigan State Univ., East Lansing, MI (United States)
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  5. Stony Brook Univ., NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  6. Univ. of Rochester, NY (United States)
  7. Ames Lab., and Iowa State Univ., Ames, IA (United States)
  8. Stony Brook Univ., NY (United States)
  9. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
+ Show Author Affiliations

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. Finally, 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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. at Buffalo, NY (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division (SC-22.3 ); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
Grant/Contract Number:
AC02-05CH11231; AC02-07CH11358; SC0018631; SC0019120
OSTI ID:
1830685
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 39 Vol. 33; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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