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Experimental and Theoretical Study of the Ultrafast Dynamics of a Ni$_2$Dy$_2$-Compound in DMF After UV/Vis Photoexcitation

Sold, S.; Mummaneni, B. C.; Michenfelder, N. C.; Peng, Y.; Powell, A. K.; Unterreiner, A.-N. ORCID iD icon; Lefkidis, G.; Hübner, W.


We present a combined experimental and theoretical study of the ultrafast transient absorption spectroscopy results of a {Ni$_{2}$Dy$_{2}$}-compound in DMF, which can be considered as a prototypic molecule for single molecule magnets. We apply state-of-the-art ab initio quantum chemistry to quantitatively describe the optical properties of an inorganic complex system comprising ten atoms to form the chromophoric unit, which is further stabilized by surrounding ligands. Two different basis sets are used for the calculations to specifically identify two dominant peaks in the ground state. Furthermore, we theoretically propagate the compound's correlated many-body wavefunction under the influence of a laser pulse as well as relaxation processes and compare against the time-resolved absorption spectra. The experimental data can be described with a time constant of several hundreds of femtoseconds attributed to vibrational relaxation and trapping into states localized within the band gap. A second time constant is ascribed to the excited state while trap states show lifetimes on a longer timescale. The theoretical propagation is performed with the density-matrix formalism and the Lindblad superoperator, which couples the system to a thermal bath, allowing us to extract relaxation times from first principles.

Verlagsausgabe §
DOI: 10.5445/IR/1000141580
Veröffentlicht am 03.01.2022
DOI: 10.1002/open.202100153
Zitationen: 1
Web of Science
Zitationen: 2
Zitationen: 1
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Nanotechnologie (INT)
Institut für Physikalische Chemie (IPC)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2021
Sprache Englisch
Identifikator ISSN: 2191-1363, 2191-1355
KITopen-ID: 1000141580
HGF-Programm 43.32.01 (POF IV, LK 01) Molecular Materials Basis for Optics & Photonics
Erschienen in ChemistryOpen
Verlag Wiley-VCH Verlag
Band 11
Heft 5
Seiten e202100153
Vorab online veröffentlicht am 20.12.2021
Nachgewiesen in Dimensions
Web of Science
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