Universität zu Köln

Wagner, Julian ORCID: 0000-0001-8325-9373, Sahasrabudhe, Anuja, Versteeg, Rolf, Wang, Zhe ORCID: 0000-0001-7464-5408, Tsurkan, Vladimir, Loidl, Alois ORCID: 0000-0002-5579-0746, Hedayat, Hamoon and van Loosdrecht, Paul H. M. (2022). Nonequilibrium dynamics of alpha-RuCl3 - a time-resolved magneto-optical spectroscopy study. Faraday Discuss., 237. S. 237 - 259. CAMBRIDGE: ROYAL SOC CHEMISTRY. ISSN 1364-5498

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Abstract

We present time-resolved magneto-optical spectroscopy on the magnetic Mott-Hubbard-insulating Kitaev spin liquid candidate alpha-RuCl3 to investigate the nonequilibrium dynamics of its antiferromagnetically ordered zigzag groundstate after photoexcitation. A systematic study of the transient magnetic linear dichroism under different experimental conditions (temperature, external magnetic field, photoexcitation density) gives direct access to the dynamical interplay of charge excitations with the zigzag ordered state on ultrashort time scales. We observe a rather slow initial demagnetization (few to 10s of ps) followed by a long-lived non-thermal antiferromagnetic spin-disordered state (100-1000s of ps), which can be understood in terms of holons and doublons disordering the antiferromagnetic background after photoexcitation. Varying temperature and fluence in the presence of an external magnetic field reveals two distinct photoinduced dynamics associated with the zigzag and quantum paramagnetic disordered phases. The photo-induced non-thermal spin-disordered state shows universal compressed-exponential recovery dynamics related to the growth and propagation of zigzag domains on nanosecond time scales, which is interpreted within the framework of the Fatuzzo-Labrune model for magnetization reversal. The study of nonequilibrium states in strongly correlated materials is a relatively unexplored topic, but our results are expected to be extendable to a large class of Mott-Hubbard insulator materials with strong spin-orbit coupling.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Wagner, Julian UNSPECIFIED orcid.org/0000-0001-8325-9373 UNSPECIFIED Sahasrabudhe, Anuja UNSPECIFIED UNSPECIFIED UNSPECIFIED Versteeg, Rolf UNSPECIFIED UNSPECIFIED UNSPECIFIED Wang, Zhe UNSPECIFIED orcid.org/0000-0001-7464-5408 UNSPECIFIED Tsurkan, Vladimir UNSPECIFIED UNSPECIFIED UNSPECIFIED Loidl, Alois UNSPECIFIED orcid.org/0000-0002-5579-0746 UNSPECIFIED Hedayat, Hamoon UNSPECIFIED UNSPECIFIED UNSPECIFIED van Loosdrecht, Paul H. M. UNSPECIFIED UNSPECIFIED UNSPECIFIED
URN:	urn:nbn:de:hbz:38-678913
DOI:	10.1039/d2fd00006g
Journal or Publication Title:	Faraday Discuss.
Volume:	237
Number:	0
Page Range:	S. 237 - 259
Date:	2022
Publisher:	ROYAL SOC CHEMISTRY
Place of Publication:	CAMBRIDGE
ISSN:	1364-5498
Language:	English
Faculty:	Unspecified
Divisions:	Unspecified
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language Chemistry, Physical Multiple languages
URI:	http://kups.ub.uni-koeln.de/id/eprint/67891