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

TL;DR

This study shows that linearly polarized light can induce orbital polarization in RNiO$_3$, leading to Jahn-Teller distortions and enabling ultrafast control of electronic and structural phases.

Contribution

It demonstrates that optical excitation can selectively manipulate orbital populations and trigger Jahn-Teller distortions in rare-earth nickelates.

Findings

Photoinduced $d$-$d$ transitions reduce local magnetic moments.

Tuning light polarization controls orbital imbalance.

Induced states become unstable toward Jahn-Teller distortions.

Abstract

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.