Laser‐Induced Cooperative Transition in Molecular Electronic Crystal
Abstract
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.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Aug 16, 2021
- Source ID
- 10.1002/adma.202103000
Entities
People
- Ahmed H. Ali
- Andrew K. Tan
- Chuankun Huang
- Dasharath Adhikari
- Elliot Snider
- Eva Zurek
- Feng Hu
- Ganapathy Sambandamurthy
- Hans A. Bechtel
- Ian Neuhart
- Jason B Benedict
- Jason N. Armstrong
- Jeffrey Grossman
- Jiawei Zhang
- Jigang Wang
- Mengkun Liu
- Michael C Martin
- Nathan Dasenbrock‐gammon
- Pengpeng Zhang
- Ranga P. Dias
- Richard Kim
- Shenqiang Ren
- Stephanie N. Gilbert Corder
- Taishan Zhu
- Travis Mitchell
- Xi Dong
- Xiaoyu Wang
- Yong Hu
- Yulong Huang
- Zheng Li
- Ziheng Yao
Organizations
- Army Research Office
- Iowa State University
- Lawrence Berkeley National Laboratory
- Massachusetts Institute of Technology
- Michigan State University
- National Science Foundation
- National Science Foundation Directorate for Mathematical & Physical Sciences
- Office of Basic Energy Sciences
- Office of Science
- Stony Brook University
- United States Department of Energy
- University at Buffalo
- University of Rochester