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Ultrafast electron localization and screening in a transition metal dichalcogenide

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arxiv 2210.05465 v1 pith:27JHUMYU submitted 2022-10-11 cond-mat.mtrl-sci

classification cond-mat.mtrl-sci
keywords carrierstransitionatomicmetalprobedabsorptionactingbehavior
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abstract

The coupling of light to electrical charge carriers in semiconductors is the foundation of many technological applications. Attosecond transient absorption spectroscopy measures simultaneously how excited electrons and the vacancies they leave behind dynamically react to the applied optical fields. In compound semiconductors, these dynamics can be probed via any of their atomic constituents. Often, the atomic species forming the compound contribute comparably to the relevant electronic properties of the material. One therefore expects to observe similar dynamics, irrespective of the choice of atomic species via which it is probed. Here, we show in the two-dimensional transition metal dichalcogenide semiconductor $MoSe_2$, that through a selenium-based transition we observe charge carriers acting independently from each other, while when probed through molybdenum, the collective, many-body motion of the carriers dominates. Such unexpectedly contrasting behavior can be traced back to a strong localization of electrons around molybdenum atoms following absorption of light, which modifies the local fields acting on the carriers. We show that similar behavior in elemental titanium metal carries over to transition metal-containing compounds and is expected to play an essential role for a wide range of such materials. Knowledge of independent particle and collective response is essential for fully understanding these materials.

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  1. First-principles approach to ultrafast pump-probe spectroscopy in solids

    cond-mat.mtrl-sci 2025-09 conditional novelty 6.0 of 10

    A cDFT/RT-TDDFT + non-equilibrium BSE method reproduces transient absorption spectra in three solids and attributes the blue shift to Coulomb screening, the red shift to lattice expansion, with Pauli blocking minor.

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