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Register a new userCoulomb correlations intertwined with spin and orbital excitations in LaCoO$_3$
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We carried out temperature-dependent (20 - 550 K) measurements of resonant inelastic X-ray scattering on LaCoO$_3$ to investigate the evolution of its electronic structure across the spin-state crossover. In combination with charge-transfer multiplet calculations, we accurately quantized the renormalized crystal-field excitation energies and spin-state populations. We show that the screening of the on-site Coulomb interaction of 3d electrons is orbital selective and coupled to the spin-state crossover in LaCoO$_3$. The results establish that the gradual spin-state crossover is associated with a relative change of Coulomb energy versus bandwidth, leading to a Mott-type insulator-to-metal transition.
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Spin crossover is expected to enrich unusual physical states in various types of condensed matter. Through inelastic neutron scattering, we study the spin-state excitations in the canonical and advanced platform, LaCoO$_3$, and reveal that the spatial correlation robustly maintains the seven-Co-site size below 300 K and the internal Co-$d$ electrons are spatially delocalized. By combining theoretical calculations, this dynamical short-range order is identified as a new collective unit for describing spin-state with dual spin-state nature beyond the conventional one-Co-site classification.
The spin transition in LaCoO$_3$ has been investigated within the density-functional theory + dynamical mean-field theory formalism using continuous time quantum Monte Carlo. Calculations on the experimental rhombohedral atomic structure with two Co sites per unit cell show that an independent treatment of the Co atoms results in a ground state with strong charge fluctuations induced by electronic correlations. Each atom shows a contribution from either a $d^5$ or a $d^7$ state in addition to the main $d^6$ state. These states play a relevant role in the spin transition which can be understood as a low spin-high spin (LS-HS) transition with significant contributions ($sim$ $10$ %) to the LS and HS states of $d^5$ and $d^7$ states respectively. A thermodynamic analysis reveals a significant kinetic energy gain through introduction of charge fluctuations, which in addition to the potential energy reduction lowers the total energy of the system.
By means of neutron scattering we have determined new branches of magnetic excitations in orbitally active CoO (TN=290 K) up to 15 THz and for temperatures from 6 K to 450 K. Data were taken in the (111) direction in six single-crystal zones. From the dependence on temperature and Q we have identified several branches of magnetic excitation. We describe a model for the coupled orbital and spin states of Co2+ subject to a crystal field and tetragonal distortion.
The spin states of Co$^{3+}$ ions in perovskite-type LaCoO$_3$, governed by complex interplay between the electron-lattice interactions and the strong electron correlations, still remain controversial due to the lack of experimental techniques which can detect directly. In this letter, we revealed the tensile-strain dependence of spin states, $i. e.$ the ratio of the high- and low-spin states, in epitaxial thin films and a bulk crystal of LaCoO$_3$ via resonant inelastic soft x-ray scattering. The tensile-strain as small as 1.0% was found to realize different spin states from that in the bulk.
We study ferromagnetic ordering and microscopic inhomogeneity in tensile strained LaCoO$_3$ using numerical simulations. We argue that both phenomena originate from effective superexchange interactions between atoms in the high-spin (HS) state mediated by the intermediate-spin excitations. We derive a model of the HS excitation as a bare atomic state dressed by electron and electron-hole fluctuations on the neighbor atoms. We construct a series of approximations to account for electron correlation effects responsible for HS fluctuations and magnetic exchange. The obtained amplitudes and directional dependence of magnetic couplings between the dressed HS states show a qualitative agreement with experimental observations and provide a new physical picture of LaCoO$_3$ films.
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