Excitations across the equilibrium and photoinduced `hidden' states of magnetoresistive manganites

TL;DR

This study investigates the excitations and phases of photoinduced hidden states in manganites using ultrafast spectroscopy and x-ray techniques, revealing unique long-lived states with distinct polaron and lattice dynamics.

Contribution

It combines ultrafast photo-excitation with in situ x-ray and transport measurements to characterize the excitations of photo-induced hidden phases in manganites, revealing their unique properties.

Findings

Long-lived photo-induced phase shows softened polaron excitations.

Partial suppression of Jahn-Teller distortion in the photo-excited state.

Constructed a polaron phase diagram varying temperature, strain, and fluence.

Abstract

"Hidden" phases, generated using ultrafast laser pulses (few hundred femtoseconds), with properties distinct from thermodynamic equilibrium, are appealing for technologies because they can be long-lived, with lifetimes of hours or weeks, and reversible with temperature sweeping or extra pulses. In this regard, La$_{2/3}$Ca$_{1/3}$MnO$_3$ (LCMO) stands out due to its tunability through epitaxial strain, which can drive the bulk ferromagnetic metal (FMM) into an antiferromagnetic insulator (AFI), and its susceptibility to photo-induced transitions. Indeed, AFI LCMO displays a long-lived photo-induced transition into a putative 'hidden' phase whose exact nature and excitations are still largely unknown. Here, we combine ultrafast photo-excitation in the near infrared with in situ transport, x-ray absorption (XAS), and Resonant Inelastic X-ray Scattering (RIXS) to investigate the excitations (polarons, phonons, and orbital) of the photo-excited phase of LCMO and contrast them with the thermodynamic phases achieved through strain and temperature. In the thermodynamic regime, we establish the correlation between polarons and transport, placing them in the 'strong coupling' regime of the Holstein model. Upon photo-excitation of LCMO-AFI, we uncover a long-lived phase characterized by the softening of the polaron excitations, the partial suppression of the Jahn-Teller distortion, and nearly unchanged phonons, showing the emergence of a photo-excited state absent in the equilibrium phase diagram. Finally, by varying temperature, epitaxial strain, and photo-excitation fluence, we construct a polaron phase diagram and identify the key spectroscopic signatures of each phase. Our laser-RIXS approach establishes a versatile platform for exploring photo-induced 'hidden' phases in quantum materials in non-stroboscopic conditions.