Photo-generated charge-transfer excitons in NiO revealed by ultrafast time-resolved resonant inelastic x-ray scattering

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Auteurs principaux: Merzoni, Giacomo, Martinelli, Leonardo, Parchenko, Sergii, TenHuisen, Sophia F. R., Lebedev, Vasily, Adriano, Luigi, Carley, Robert, Gerasimova, Natalia, Mercadier, Laurent, Teichmann, Martin, van Kuiken, Benjamin E., Yin, Zhong, Alic, Amina, Baykusheva, Denitsa R., Chiuzbaian, Sorin G., Conte, Stefano Dal, Dogadov, Oleg, Föhlisch, Alexander, Haverkort, Maurits W., Kusch, Maximilian, Laarmann, Tim, Lee, Wei Sheng, Sala, Marco Moretti, Peng, Ying Ying, Qiu, Qing Zheng, Schmitt, Thorsten, Lalithambika, Sreeju Sreekantan Nair, Techert, Simone, Cerullo, Giulio, Först, Michael, Mitrano, Matteo, Dean, Mark P. M., Schlappa, Justine, Scherz, Andreas, Ghiringhelli, Giacomo
Format: Preprint
Publié: 2025
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author Merzoni, Giacomo
Martinelli, Leonardo
Parchenko, Sergii
TenHuisen, Sophia F. R.
Lebedev, Vasily
Adriano, Luigi
Carley, Robert
Gerasimova, Natalia
Mercadier, Laurent
Teichmann, Martin
van Kuiken, Benjamin E.
Yin, Zhong
Alic, Amina
Baykusheva, Denitsa R.
Chiuzbaian, Sorin G.
Conte, Stefano Dal
Dogadov, Oleg
Föhlisch, Alexander
Haverkort, Maurits W.
Kusch, Maximilian
Laarmann, Tim
Lee, Wei Sheng
Sala, Marco Moretti
Peng, Ying Ying
Qiu, Qing Zheng
Schmitt, Thorsten
Lalithambika, Sreeju Sreekantan Nair
Techert, Simone
Cerullo, Giulio
Först, Michael
Mitrano, Matteo
Dean, Mark P. M.
Schlappa, Justine
Scherz, Andreas
Ghiringhelli, Giacomo
author_facet Merzoni, Giacomo
Martinelli, Leonardo
Parchenko, Sergii
TenHuisen, Sophia F. R.
Lebedev, Vasily
Adriano, Luigi
Carley, Robert
Gerasimova, Natalia
Mercadier, Laurent
Teichmann, Martin
van Kuiken, Benjamin E.
Yin, Zhong
Alic, Amina
Baykusheva, Denitsa R.
Chiuzbaian, Sorin G.
Conte, Stefano Dal
Dogadov, Oleg
Föhlisch, Alexander
Haverkort, Maurits W.
Kusch, Maximilian
Laarmann, Tim
Lee, Wei Sheng
Sala, Marco Moretti
Peng, Ying Ying
Qiu, Qing Zheng
Schmitt, Thorsten
Lalithambika, Sreeju Sreekantan Nair
Techert, Simone
Cerullo, Giulio
Först, Michael
Mitrano, Matteo
Dean, Mark P. M.
Schlappa, Justine
Scherz, Andreas
Ghiringhelli, Giacomo
contents Strong electronic correlation can lead to insulating behavior and to the opening of large optical gaps, even in materials with partly filled valence shells. Although the non-equilibrium optical response encodes both local (quasi atomic) and collective (long range) responses, optical spectroscopy is usually more sensitive to the latter. Resonant x-ray techniques are better suited to investigate the quasi-atomic properties of correlated solids. Using time-resolved resonant inelastic x-ray scattering (RIXS), here we study the ultrafast non-equilibrium processes in NiO following photo-excitation by ultraviolet photons with energy exceeding the optical gap. We observe the creation of charge-transfer excitons that decay with a time constant of about 2\,ps, while itinerant photo-doping persists for tens of picoseconds. Following our discovery, which establishes time-resolved high-resolution RIXS as a powerful tool for the study of transient phenomena in condensed matter, the possible presence of charge-transfer excitons will need to be considered when interpreting optical pump-probe experiments on correlated quantum materials.
format Preprint
id arxiv_https___arxiv_org_abs_2504_16653
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Photo-generated charge-transfer excitons in NiO revealed by ultrafast time-resolved resonant inelastic x-ray scattering
Merzoni, Giacomo
Martinelli, Leonardo
Parchenko, Sergii
TenHuisen, Sophia F. R.
Lebedev, Vasily
Adriano, Luigi
Carley, Robert
Gerasimova, Natalia
Mercadier, Laurent
Teichmann, Martin
van Kuiken, Benjamin E.
Yin, Zhong
Alic, Amina
Baykusheva, Denitsa R.
Chiuzbaian, Sorin G.
Conte, Stefano Dal
Dogadov, Oleg
Föhlisch, Alexander
Haverkort, Maurits W.
Kusch, Maximilian
Laarmann, Tim
Lee, Wei Sheng
Sala, Marco Moretti
Peng, Ying Ying
Qiu, Qing Zheng
Schmitt, Thorsten
Lalithambika, Sreeju Sreekantan Nair
Techert, Simone
Cerullo, Giulio
Först, Michael
Mitrano, Matteo
Dean, Mark P. M.
Schlappa, Justine
Scherz, Andreas
Ghiringhelli, Giacomo
Strongly Correlated Electrons
Strong electronic correlation can lead to insulating behavior and to the opening of large optical gaps, even in materials with partly filled valence shells. Although the non-equilibrium optical response encodes both local (quasi atomic) and collective (long range) responses, optical spectroscopy is usually more sensitive to the latter. Resonant x-ray techniques are better suited to investigate the quasi-atomic properties of correlated solids. Using time-resolved resonant inelastic x-ray scattering (RIXS), here we study the ultrafast non-equilibrium processes in NiO following photo-excitation by ultraviolet photons with energy exceeding the optical gap. We observe the creation of charge-transfer excitons that decay with a time constant of about 2\,ps, while itinerant photo-doping persists for tens of picoseconds. Following our discovery, which establishes time-resolved high-resolution RIXS as a powerful tool for the study of transient phenomena in condensed matter, the possible presence of charge-transfer excitons will need to be considered when interpreting optical pump-probe experiments on correlated quantum materials.
title Photo-generated charge-transfer excitons in NiO revealed by ultrafast time-resolved resonant inelastic x-ray scattering
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2504.16653