Photo-induced charge-transfer renormalization in NiO
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arXiv
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2023
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| author | Lojewski, Tobias Golez, Denis Ollefs, Katharina Guyader, Loïc Le Kämmerer, Lea Rothenbach, Nico Engel, Robin Y. Miedema, Piter S. Beye, Martin Chiuzbăian, Gheorghe S. Carley, Robert Gort, Rafael Van Kuiken, Benjamin E. Mercurio, Giuseppe Schlappa, Justina Yaroslavtsev, Alexander Scherz, Andreas Döring, Florian David, Christian Wende, Heiko Bovensiepen, Uwe Eckstein, Martin Werner, Philipp Eschenlohr, Andrea |
| author_facet | Lojewski, Tobias Golez, Denis Ollefs, Katharina Guyader, Loïc Le Kämmerer, Lea Rothenbach, Nico Engel, Robin Y. Miedema, Piter S. Beye, Martin Chiuzbăian, Gheorghe S. Carley, Robert Gort, Rafael Van Kuiken, Benjamin E. Mercurio, Giuseppe Schlappa, Justina Yaroslavtsev, Alexander Scherz, Andreas Döring, Florian David, Christian Wende, Heiko Bovensiepen, Uwe Eckstein, Martin Werner, Philipp Eschenlohr, Andrea |
| contents | Photo-doped states in strongly correlated charge transfer insulators are characterized by $d$-$d$ and $d$-$p$ interactions and the resulting intertwined dynamics of charge excitations and local multiplets. Here we use femtosecond x-ray absorption spectroscopy in combination with dynamical mean-field theory to disentangle these contributions in NiO. Upon resonant optical excitation across the charge transfer gap, the Ni $L_3$ and O $K$ absorption edges red-shift for $>10$ ps, associated with photo-induced changes in the screening environment. An additional signature below the Ni $L_3$ edge is identified for $<1$ ps, reflecting a transient nonthermal population of local many-body multiplets. We employ a nonthermal generalization of the multiplet ligand field theory to show that the feature originates from $d$-$d$ transitions. Overall, the photo-doped state differs significantly from a chemically doped state. Our results demonstrate the ability to reveal excitation pathways in correlated materials by x-ray spectroscopies, which is relevant for ultrafast materials design. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2305_10145 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | Photo-induced charge-transfer renormalization in NiO Lojewski, Tobias Golez, Denis Ollefs, Katharina Guyader, Loïc Le Kämmerer, Lea Rothenbach, Nico Engel, Robin Y. Miedema, Piter S. Beye, Martin Chiuzbăian, Gheorghe S. Carley, Robert Gort, Rafael Van Kuiken, Benjamin E. Mercurio, Giuseppe Schlappa, Justina Yaroslavtsev, Alexander Scherz, Andreas Döring, Florian David, Christian Wende, Heiko Bovensiepen, Uwe Eckstein, Martin Werner, Philipp Eschenlohr, Andrea Strongly Correlated Electrons Photo-doped states in strongly correlated charge transfer insulators are characterized by $d$-$d$ and $d$-$p$ interactions and the resulting intertwined dynamics of charge excitations and local multiplets. Here we use femtosecond x-ray absorption spectroscopy in combination with dynamical mean-field theory to disentangle these contributions in NiO. Upon resonant optical excitation across the charge transfer gap, the Ni $L_3$ and O $K$ absorption edges red-shift for $>10$ ps, associated with photo-induced changes in the screening environment. An additional signature below the Ni $L_3$ edge is identified for $<1$ ps, reflecting a transient nonthermal population of local many-body multiplets. We employ a nonthermal generalization of the multiplet ligand field theory to show that the feature originates from $d$-$d$ transitions. Overall, the photo-doped state differs significantly from a chemically doped state. Our results demonstrate the ability to reveal excitation pathways in correlated materials by x-ray spectroscopies, which is relevant for ultrafast materials design. |
| title | Photo-induced charge-transfer renormalization in NiO |
| topic | Strongly Correlated Electrons |
| url | https://arxiv.org/abs/2305.10145 |