Ultrafast Doublon Dynamics in Photoexcited 1T-TaS_{2}

Physical Review Letters
M LiggesU Bovensiepen

Abstract

Strongly correlated materials exhibit intriguing properties caused by intertwined microscopic interactions that are hard to disentangle in equilibrium. Employing nonequilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1T-TaS_{2}, we identify a spectroscopic signature of doubly occupied sites (doublons) that reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on timescales of electronic hopping ℏ/J≈14  fs. Despite strong electron-phonon coupling, the dynamics can be explained by purely electronic effects captured by the single-band Hubbard model under the assumption of weak hole doping, in agreement with our static sample characterization. This sensitive interplay of static doping and vicinity to the metal-insulator transition suggests a way to modify doublon relaxation on the few-femtosecond timescale.

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Citations

Apr 2, 2019·Physical Review Letters·Sung-Hoon LeeDoohee Cho
Jun 8, 2019·Physical Review Letters·Chen-Yen Lai, Jian-Xin Zhu
Aug 26, 2020·Nature Communications·Y D WangY Zhang
Mar 8, 2020·Nature Communications·Quirin StahlTobias Ritschel
Jan 13, 2019·Physical Review Letters·Karsten BalzerMichael Bonitz
Apr 21, 2021·Nature Communications·Jan RavnikDragan Mihailovic
May 29, 2021·Physical Review Letters·Jinwon LeeHan Woong Yeom
Nov 3, 2021·Journal of Chemical Theory and Computation·Xavier AndradeAlfredo A Correa

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