No Arabic abstract
The ultrafast response of the prototype Mott-Hubbard system (V1-xCrx)2O3 was systematically studied with fs pump-probe reflectivity, allowing us to clearly identify the effects of the metal-insulator transition on the transient response. The isostructural nature of the phase transition in this material made it possible to follow across the phase diagram the behaviour of the detected coherent acoustic wave, whose average value and lifetime depend on the thermodynamic phase and on the correlated electron density of states. It is also shown how coherent lattice oscillations can play an important role in some changes affecting the ultrafast electronic peak relaxation at the phase transition, changes which should not be mistakenly attributed to genuine electronic effects. These results clearly show that a thorough understanding of the ultrafast response of the material over several tenths of ps is necessary to correctly interpret its sub-ps excitation and relaxation regime, and appear to be of general interest also for other strongly correlated materials.
V2O3 is the prototype system for the Mott transition, one of the most fundamental phenomena of electronic correlation. Temperature, doping or pressure induce a metal to insulator transition (MIT) between a paramagnetic metal (PM) and a paramagnetic insulator (PI). This or related MITs have a high technological potential, among others for intelligent windows and field effect transistors. However the spatial scale on which such transitions develop is not known in spite of their importance for research and applications. Here we unveil for the first time the MIT in Cr-doped V2O3 with submicron lateral resolution: with decreasing temperature, microscopic domains become metallic and coexist with an insulating background. This explains why the associated PM phase is actually a poor metal. The phase separation can be associated with a thermodynamic instability near the transition. This instability is reduced by pressure which drives a genuine Mott transition to an eventually homogeneous metallic state.
The study of photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behavior, including non-thermal phases and photoinduced phase transitions. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states of matter inaccessible by quasi-adiabatic pathways. Here we present a study of the ultrafast non-equilibrium evolution of the prototype Mott-Hubbard material V2O3, which presents a transient non-thermal phase developing immediately after photoexcitation and lasting few picoseconds. For both the insulating and the metallic phase, the formation of the transient configuration is triggered by the excitation of electrons into the bonding a1g orbital, and is then stabilized by a lattice distortion characterized by a marked hardening of the A1g coherent phonon. This configuration is in stark contrast with the thermally accessible ones - the A1g phonon frequency actually softens when heating the material. Our results show the importance of selective electron-lattice interplay for the ultrafast control of material parameters, and are of particular relevance for the optical manipulation of strongly correlated systems, whose electronic and structural properties are often strongly intertwinned.
The combination of bandstructure theory in the local density approximation with dynamical mean field theory was recently successfully applied to V$_2$O$_3$ -- a material which undergoes the f amous Mott-Hubbard metal-insulator transition upon Cr doping. The aim of this sh ort paper is to emphasize two aspects of our recent results: (i) the filling of the Mott-Hubbard gap with increasing temperature, and (ii) the peculiarities of the Mott-Hubbard transition in this system which is not characterized by a diver gence of the effective mass for the $a_{1g}$-orbital.
The changes in the electronic structure of V2O3 across the metal-insulator transition induced by temperature, doping and pressure are identified using high resolution x-ray absorption spectroscopy at the V pre K-edge. Contrary to what has been taken for granted so far, the metallic phase reached under pressure is shown to differ from the one obtained by changing doping or temperature. Using a novel computational scheme, we relate this effect to the role and occupancy of the a1g orbitals. This finding unveils the inequivalence of different routes across the Mott transition in V2O3
We introduce the notion of superstructure Mottness to describe the Mott and Wigner-Mott transition in doped strongly correlated electron systems at commensurate filling fractions away from one electron per site. We show that superstructure Mottness emerges in an inhomogeneous electron system when the superstructure contains an odd number of electrons per supercell. We argue that superstructure Mottness exists even in the absence of translation symmetry breaking by a superlattice, provided that the extended or intersite Coulomb interaction is strong. In the latter case, superstructure Mottness offers a unifying framework for the Mott and Wigner physics and a nonperturbative, strong coupling description of the Wigner-Mott transition. We support our proposal by studying a minimal single-band ionic Hubbard $t$-$U$-$V$-$Delta$ model with nearest neighbor Coulomb repulsion $V$ and a two-sublattice ionic potential $Delta$. The model is mapped onto a Hubbard model with two effective ``orbitals representing the two sites within the supercell, the intra and interorbital Coulomb repulsion $U$ and $U^prime sim V$, and a crystal field splitting $Delta$. Charge order on the original lattice corresponds to orbital order. Developing a cluster Gutzwiller approximation, we study the effects and the interplay between $V$ and $Delta$ on the Mott and Wigner-Mott transitions at quarter-filling. We provide the mechanism by which the superlattice potential enhances the correlation effects and the tendency towards local moment formation, construct and elucidate the phase diagram in the unifying framework of superstructure Mottness.