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Photoinduced charge transfer renormalization in NiO

Lojewski, Tobias ; GoleŽ, Denis ; Ollefs, Katharina ; Le Guyader, Loïc ; Kämmerer, Lea ; Rothenbach, Nico ; Engel, Robin Y. ; Miedema, Piter S. ; Beye, Martin and Chiuzbǎian, Gheorghe S. , et al. (2024) In Physical Review B 110(24).
Abstract

Photodoped 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 L3 and O K absorption edges red-shift for >10 ps, which we associate with photoinduced changes in the screening environment. An additional signature below the Ni L3 edge is identified for <1 ps, reflecting a transient nonthermal population of local many-body multiplets. We employ a nonthermal generalization of the multiplet... (More)

Photodoped 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 L3 and O K absorption edges red-shift for >10 ps, which we associate with photoinduced changes in the screening environment. An additional signature below the Ni L3 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 and argue that this feature originates from d-d transitions. Overall, the photodoped state differs significantly from a chemically doped state. Our results demonstrate that x-ray spectroscopies are helpful in revealing excitation pathways in correlated materials.

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publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review B
volume
110
issue
24
article number
245120
publisher
American Physical Society
external identifiers
  • scopus:85211972895
ISSN
2469-9950
DOI
10.1103/PhysRevB.110.245120
language
English
LU publication?
yes
id
b0452ee4-e094-4447-9805-ed8c45c31cc6
date added to LUP
2025-01-16 13:39:37
date last changed
2025-04-04 13:58:54
@article{b0452ee4-e094-4447-9805-ed8c45c31cc6,
  abstract     = {{<p>Photodoped 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 L3 and O K absorption edges red-shift for &gt;10 ps, which we associate with photoinduced changes in the screening environment. An additional signature below the Ni L3 edge is identified for &lt;1 ps, reflecting a transient nonthermal population of local many-body multiplets. We employ a nonthermal generalization of the multiplet ligand field theory and argue that this feature originates from d-d transitions. Overall, the photodoped state differs significantly from a chemically doped state. Our results demonstrate that x-ray spectroscopies are helpful in revealing excitation pathways in correlated materials.</p>}},
  author       = {{Lojewski, Tobias and GoleŽ, Denis and Ollefs, Katharina and Le Guyader, Loïc and Kämmerer, Lea and Rothenbach, Nico and Engel, Robin Y. and Miedema, Piter S. and Beye, Martin and Chiuzbǎian, Gheorghe S. and Carley, Robert and Gort, Rafael and Van Kuiken, Benjamin E. and Mercurio, Giuseppe and Schlappa, Justina and Yaroslavtsev, Alexander and Scherz, Andreas and Döring, Florian and David, Christian and Wende, Heiko and Bovensiepen, Uwe and Eckstein, Martin and Werner, Philipp and Eschenlohr, Andrea}},
  issn         = {{2469-9950}},
  language     = {{eng}},
  number       = {{24}},
  publisher    = {{American Physical Society}},
  series       = {{Physical Review B}},
  title        = {{Photoinduced charge transfer renormalization in NiO}},
  url          = {{http://dx.doi.org/10.1103/PhysRevB.110.245120}},
  doi          = {{10.1103/PhysRevB.110.245120}},
  volume       = {{110}},
  year         = {{2024}},
}