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Conny Såthe

Publications and source records attributed to Conny Såthe.

2 recordsLinked to original sources

Electronic excitations in the Shastry-Sutherland compound SrCu$_2$(BO$_3$)$_2$

SrCu2(BO3)2 (SCBO) is a paradigmatic realization of the Shastry-Sutherland model, hosting geometrically frustrated spin dimers and a variety of quantum magnetic phases and phenomena. Although its magnetic properties have been extensively studied, the high-energy electronic excitations that determine the crystal-field environment and Cu-O hybridization have remained largely unexplored. Here we combine Cu L3-edge resonant inelastic x-ray scattering (RIXS), broadband optical spectroscopy, and electronic-structure calculations to determine the relevant local and interband excitation energy scales in SCBO. RIXS resolves a well-defined manifold of localized Cu2+ d-d excitations between 1.8 and 2.4 eV, whose energies and polarization dependence are well reproduced by multireference quantum-chemistry calculations. In contrast, optical spectroscopy identifies charge-transfer excitations with an absorption onset near 1.2-1.6 eV and a broader higher-energy structure around 4.5 eV, which are qualitatively captured by DFT+U calculations. Taken together, these results define the characteristic energy scales of d-d and CT excitations, offering quantitative benchmarks for computational frameworks and providing essential input for refining superexchange-based magnetic models of this prototypical frustrated quantum antiferromagnet.

cond-mat.str-el↗

Intermolecular Radiative Decay: A non-local decay mechanism providing an insider's view of the solvation shell

Aqueous solutions are crucial in chemistry, biology, environmental science, and technology. The chemistry of solutes is influenced by the surrounding solvation shell of water molecules, which have different chemical properties than bulk water due to their different electronic and geometric structure. It is an experimental challenge to selectively investigate this property-determining electronic and geometric structure. Here, we report experimental results on a novel non-local X-ray emission process, Intermolecular Radiative Decay (IRD), for the prototypical ions Na$^{+}$ and Mg$^{2+}$ in water. We show that, in IRD, an electron from the solvation shell fills a core hole in the solute, and the released energy is emitted as an X-ray photon. We analyze the underlying mechanism using theoretical calculations, and show how IRD will allow us to meet the challenge of chemically selective probing of solvation shells from within.

physics.chem-ph↗