Polarization of photoluminescence by optically driven orbital reconstruction in magnetically ordered CrCl3

Lanqing Zhou; Marjana Ležaić; Yuriy Mokrousov; Minh N. Bui; Renu Rani; Govind Ummethala; Amir H. Tavabi; Tatiana E. Gorelik; Rafal E. Dunin-Borkowski; Detlev Grützmacher; Beata E. Kardynał

arXiv · 2502.16285

Polarization of photoluminescence by optically driven orbital reconstruction in magnetically ordered CrCl3

Lanqing Zhou·Marjana Ležaić·Yuriy Mokrousov·Minh N. Bui·Renu Rani·Govind Ummethala·Amir H. Tavabi·Tatiana E. Gorelik·Rafal E. Dunin-Borkowski·Detlev Grützmacher·Beata E. Kardynał

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Abstract

Control of magnetic order through optical manipulation of orbital states can be realized in a wide range of materials, including insulators. In the latter case, electrons are excited into different electronic states, whose character may be a complex result of spin-orbit-lattice coupling. Here, we use a combination of polarization-resolved photoluminescence spectroscopy and density functional theory calculations to study excited Cr3+ ions in bulk, insulating antiferromagnetic CrCl3. Our results demonstrate a temperature-dependent preferential polarization direction below ~17 K, which reorients in the presence of an applied in-plane magnetic field. Density functional theory calculations reveal a local distortion of the ligand field and the generation of out-of-plane spin and orbital moments, following Cr3+ ion excitation. These changes link the photoluminescence polarization to the magnetic state of CrCl3. Our findings provide insight into the excited-state electronic structure of Cr3+ ions and suggest that CrCl3 is a promising candidate for opto-orbitronic applications.

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Lanqing Zhou, Marjana Ležaić, Yuriy Mokrousov, Minh N. Bui, Renu Rani, Govind Ummethala, Amir H. Tavabi, Tatiana E. Gorelik, Rafal E. Dunin-Borkowski, Detlev Grützmacher, Beata E. Kardynał. 2025-02-22. Polarization of photoluminescence by optically driven orbital reconstruction in magnetically ordered CrCl3. https://arxiv.org/abs/2502.16285

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