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Journal Article

Ultrafast Doublon Dynamics in Photoexcited 1T-TaS2


Eckstein,  M.
Theory of Correlated Systems out of Equilibrium, Condensed Matter Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
University of Hamburg-CFEL;

Fulltext (public)

(Preprint), 807KB

Supplementary Material (public)

Ligges, M., Avigo, I., Golež, D., Strand, H., Beyazit, Y., Hanff, K., et al. (2018). Ultrafast Doublon Dynamics in Photoexcited 1T-TaS2. Physical Review Letters, 120(16): 166401. doi:10.1103/PhysRevLett.120.166401.

Cite as: http://hdl.handle.net/21.11116/0000-0002-1514-0
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-TaS2, 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.