Tracking the local order parameter through the Hubbard exciton decoherence time in the Mott-Hubbard insulator LaVO3
Year: 2026
Authors: Milloch A., Franceschini P., Villar-Arribi P., Chaluvadi SK., Orgiani P., Panaccione G., Rossi G., Liu Y., Schlom DG., Shen KM., Capone M., Giannetti C.
Autors Affiliation: Univ Cattolica Sacro Cuore, Dept Math & Phys, I-25133 Brescia, Italy; Univ Cattolica Sacro Cuore, ILAMP Interdisciplinary Labs Adv Mat Phys, I-25133 Brescia, Italy; Katholieke Univ Leuven, Dept Phys & Astron, B-3001 Leuven, Belgium; CNR, INO, Natl Inst Opt, Via Branze 45, I-25123 Brescia, Italy; Univ Brescia, Dept Informat Engn, I-25123 Brescia, Italy; Int Sch Adv Studies SISSA, Via Bonomea 265, I-34136 Trieste, Italy; CNR, IOM Ist Officina Mat, SS 14,Km 163-5, I-34149 Trieste, Italy; Univ Milan, Dipartimento Fis, Via Celoria 16, I-20133 Milan, Italy; Cornell Univ, Lab Atom & Solid State Phys, Ithaca, NY 14853 USA; Cornell Univ, Dept Mat Sci & Engn, Ithaca, NY 14853 USA; Kavli Inst, Cornell Nanoscale Sci, Ithaca, NY 14853 USA; Leibniz Inst Kristallzuchtung, Max Born Str 2, D-12489 Berlin, Germany; CNR, IOM, Ist Officina Mat, Via Bonomea 265, I-34136 Trieste, Italy.
Abstract: The prototypical Mott-Hubbard insulator LaVO3 undergoes a structural phase transition accompanied by the onset of spin and orbital ordering below 140 K. By combining ultrafast optical pump-probe spectroscopy and two-dimensional electronic spectroscopy, we investigate the interplay between fluctuations of the local spin and orbital order parameter and the lifetime of high-energy electron-hole excitations. Specifically, we demonstrate that the pump-induced perturbation of the order parameter leads to a change of the Hubbard exciton decoherence time and, consequently, of its homogeneous linewidth. Dynamical mean-field theory calculations confirm that the exciton scattering rate is crucially affected by the degree of order of the spin and orbital lattices in LaVO3. Our results demonstrate that multi-dimensional ultrafast optical spectroscopy can be used to track the dynamics of the order parameter, thus opening new routes in the study of correlated quantum materials characterized by intertwined orders.
Journal/Review: PHYSICAL REVIEW B
Volume: 113 (20) Pages from: 205146-1 to: 205146-12
More Information: A.M., P.F., and C.G. acknowledge financial support from MIUR through the PRIN 2017 (Prot. 20172H2SC4 005) and PRIN 2020 (Prot. 2020JLZ52N 003) programs and from the European Union-Next Generation EU through PRIN 2022 (Prof. 20228YCYY7 001). Y.L. and K.M.S. would like to acknowledge support from NSF DMR-2104427 and AFOSR FA9550-21-1-0168. This work made use of the thin-film facility of the Platform for the Accelerated Realization, Analysis, and Discovery of Interface Materials (PARADIM) , which is supported by the NSF under Cooperative Agreement No. DMR- 2039380. This work was in the frameworkof the NFFA facility supported by MUR under CUP number B91J12000310001 as the Activity of International Relevance NFFA [69].KeyWords: Transition; SpectroscopyDOI: 10.1103/9zzp-8gkz
