Photoinduced orbital polarization and Jahn-Teller effect in RNiO$_3$

Fuente: arXiv
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Main Authors: Rajpurohit, Sangeeta, Haque, Sheikh Rubaiat Ul, Lindenberg, Aaron M., Blöchl, Peter E., Ogitsu, Tadashi
Format: Preprint
Published: 2026
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_version_ 1866911610722844672
author Rajpurohit, Sangeeta
Haque, Sheikh Rubaiat Ul
Lindenberg, Aaron M.
Blöchl, Peter E.
Ogitsu, Tadashi
author_facet Rajpurohit, Sangeeta
Haque, Sheikh Rubaiat Ul
Lindenberg, Aaron M.
Blöchl, Peter E.
Ogitsu, Tadashi
contents The orbital degree of freedom in rare-earth nickelates is typically inactive across the temperature-driven metal-insulator transition, where the system develops two inequivalent Ni sites associated with Ni-O bond disproportionation and breathing-mode distortions of NiO$_6$ octahedra. Here, we show that orbital polarization can be induced by optical excitation with linearly polarized light. Using an interacting multiband tight-binding model combined with real-time simulations of coupled electron-ion-spin dynamics, we find that photoinduced $d$-$d$ transitions reduce the local magnetic moments at Ni sites and effectively suppress Hund's coupling $J$ in the excited state. Importantly, these transitions can be made strongly orbital-selective by tuning the light polarization, leading to an imbalance in $e_g$ orbital occupancies. The resulting nonequilibrium state, characterized by reduced effective $J$ and unequal orbital populations, becomes unstable toward Jahn-Teller (JT) distortions, driving structural relaxation along coherently excited JT modes. Our results demonstrate that polarization-controlled optical excitation provides a pathway to access hidden nonthermal phases with emergent orbital order, enabling coherent control of coupled charge, spin, and lattice degrees of freedom on ultrafast timescales.
format Preprint
id arxiv_https___arxiv_org_abs_2604_18524
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Photoinduced orbital polarization and Jahn-Teller effect in RNiO$_3$
Rajpurohit, Sangeeta
Haque, Sheikh Rubaiat Ul
Lindenberg, Aaron M.
Blöchl, Peter E.
Ogitsu, Tadashi
Strongly Correlated Electrons
The orbital degree of freedom in rare-earth nickelates is typically inactive across the temperature-driven metal-insulator transition, where the system develops two inequivalent Ni sites associated with Ni-O bond disproportionation and breathing-mode distortions of NiO$_6$ octahedra. Here, we show that orbital polarization can be induced by optical excitation with linearly polarized light. Using an interacting multiband tight-binding model combined with real-time simulations of coupled electron-ion-spin dynamics, we find that photoinduced $d$-$d$ transitions reduce the local magnetic moments at Ni sites and effectively suppress Hund's coupling $J$ in the excited state. Importantly, these transitions can be made strongly orbital-selective by tuning the light polarization, leading to an imbalance in $e_g$ orbital occupancies. The resulting nonequilibrium state, characterized by reduced effective $J$ and unequal orbital populations, becomes unstable toward Jahn-Teller (JT) distortions, driving structural relaxation along coherently excited JT modes. Our results demonstrate that polarization-controlled optical excitation provides a pathway to access hidden nonthermal phases with emergent orbital order, enabling coherent control of coupled charge, spin, and lattice degrees of freedom on ultrafast timescales.
title Photoinduced orbital polarization and Jahn-Teller effect in RNiO$_3$
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2604.18524