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Ultrafast doublon dynamics in photo-excited 1T-TaS$_2$

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arxiv 1702.05300 v2 pith:X5GLOLVF submitted 2017-02-17 cond-mat.str-el

classification cond-mat.str-el
keywords dynamicscorrelateddoublonelectronicstronglyt-tasultrafastagreement
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abstract

Strongly correlated systems exhibit intriguing properties caused by intertwined microscopic in- teractions that are hard to disentangle in equilibrium. Employing non-equilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1T-TaS$_2$, we identify a spectroscopic signature of double occupied sites (doublons) that are reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on time scales of one electronic hopping cycle $\hbar/J\approx$ 14 fs. Despite strong electron-phonon coupling the dynamics can be explained by purely electronic effects captured by the single band Hubbard model, where thermalization is fast in the small-gap regime. Qualitative agreement with the experimental results however requires the assumption of an intrinsic hole-doping. The sensitivity of the doublon dynamics on the doping level provides a way to control ultrafast processes in such strongly correlated materials.

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