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Charge-transfer properties and electron dynamics in ferromagnetic CoS2
Department of Applied Physics and Astronomy, University of Sharjah, P. O. Box 27272 Sharjah, United Arab Emirates, P. O. Box 27272; Center for Advanced Materials Research, Research Institute of Sciences and Engineering, University of Sharjah, Sharjah 27272, United Arab Emirates; Department of Physics, Faculty of Science, Fayoum University, Fayoum 63514, Egypt.
Institute Methods and Instrumentation for Synchrotron Radiation Research PS-ISRR, Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Straße 15, 12489 Berlin, Germany; Institut für Physik und Astronomie, Universität Potsdam, Karl-Liebknecht-Strasse 24-25, 14476 Potsdam, Germany; Present address: Department of Physics, Uppsala University, Box 516, SE-75121 Uppsala, Sweden.
Homi Bhabha National Institute, Anushaktinagar, Mumbai 400094, India.
Department of Physics and Astronomy, Uppsala University, Box 516, SE-75121 Uppsala, Sweden.
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2025 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 112, no 16, article id 165115Article in journal (Refereed) Published
Abstract [en]

We investigated the element-specific electronic structure and charge-carrier dynamics of a single-crystal ferromagnet CoS2 with complementary x-ray spectroscopy techniques. Hard x-ray photoemission (HAXPES) is used to provide crucial information on the bulk electronic structure and chemical bonding in CoS2 that is compared against the isoelectronic paramagnet CoSe2. The Co 1⁢𝑠 core-level line shows several satellite features for CoS2, showing explicit charge-transfer processes and local screening of the core hole by S ligands, whereas no such features are observed in CoSe2. The satellite structures indicate the electronic configuration of divalent Co2+ as a combination of 𝑑8⁢Ḻ and 𝑑9⁢Ḻ2 in addition to the nominal ionic 𝑑7 state, where Ḻ represents an S 3⁢𝑝 hole. We employ resonant Auger spectroscopy across the S 𝐾-edge for CoS2 to obtain electron delocalization times to adjacent Co atomic sites. The fast carrier dynamics are attributed to strongly screened Coulomb interactions and hence a facile carrier delocalization. The strong hybridization formed between the Co 3⁢𝑑 and S 3⁢𝑝 states with pronounced charge-transfer character reflects a self-doped system with a finite density 𝑛 of holes at the sulfur site (Ḻ𝑛), in line with recent models that indicate a negative charge-transfer energy for CoS2. In addition to HAXPES data, we also report on experimental and theoretical 𝐿-edge x-ray absorption and x-ray magnetic circular dichroism data for CoS2 that demonstrate multiconfiguration effects in the excitation process. To enable a direct comparison of the experimental spectra, we used density functional theory calculations to obtain the projected density of states to describe the ground-state electronic structure. The existence of fast carrier dynamics and strong charge-transfer properties, demonstrated in this study, highlights the unique nature of CoS2 with a wide potential in topological spintronics applications and integration in energy-related device platforms.

Place, publisher, year, edition, pages
American Physical Society (APS) , 2025. Vol. 112, no 16, article id 165115
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Condensed Matter Physics Theoretical Chemistry
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URN: urn:nbn:se:kth:diva-373244DOI: 10.1103/vg4c-h785ISI: 001596938000001Scopus ID: 2-s2.0-105020662149OAI: oai:DiVA.org:kth-373244DiVA, id: diva2:2016282
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QC 20251125

Available from: 2025-11-25 Created: 2025-11-25 Last updated: 2025-11-25Bibliographically approved

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Edström, AlexanderDelin, AnnaPhuyal, Dibya

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