Ultrafast coupled charge and spin dynamics in strongly correlated NiO

Konrad Gillmeister, Denis Golež, Cheng-Tien Chiang, Nikolaj Bittner, Yaroslav Pavlyukh, Jamal Berakdar, Philipp Werner () and Wolf Widdra ()
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Konrad Gillmeister: Martin-Luther-Universität Halle-Wittenberg
Denis Golež: Flatiron Institute
Cheng-Tien Chiang: Martin-Luther-Universität Halle-Wittenberg
Nikolaj Bittner: University of Fribourg
Yaroslav Pavlyukh: Technische Universität Kaiserslautern
Jamal Berakdar: Martin-Luther-Universität Halle-Wittenberg
Philipp Werner: University of Fribourg
Wolf Widdra: Martin-Luther-Universität Halle-Wittenberg

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Charge excitations across an electronic band gap play an important role in opto-electronics and light harvesting. In contrast to conventional semiconductors, studies of above-band-gap photoexcitations in strongly correlated materials are still in their infancy. Here we reveal the ultrafast dynamics controlled by Hund’s physics in strongly correlated photoexcited NiO. By combining time-resolved two-photon photoemission experiments with state-of-the-art numerical calculations, an ultrafast (≲10 fs) relaxation due to Hund excitations and related photo-induced in-gap states are identified. Remarkably, the weight of these in-gap states displays long-lived coherent THz oscillations up to 2 ps at low temperature. The frequency of these oscillations corresponds to the strength of the antiferromagnetic superexchange interaction in NiO and their lifetime vanishes slightly above the Néel temperature. Numerical simulations of a two-band t-J model reveal that the THz oscillations originate from the interplay between local many-body excitations and antiferromagnetic spin correlations.

Date: 2020
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DOI: 10.1038/s41467-020-17925-8

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