Itinerant type many-body theories for photo-induced structural phase transitions

Abstract

Itinerant type quantum many-body theories for photo-induced structural phase transitions (PSPTs) are reviewed in close connection with various recent experimental results related to this new optical phenomenon. There are two key concepts: the hidden multi-stability of the ground state, and the proliferations of optically excited states. Taking the ionic (I) → neutral (N) phase transition in the organic charge transfer (CT) crystal, TTF–CA, as a typical example for this type of transition, we, at first, theoretically show an adiabatic path which starts from CT excitons in the I-phase, but finally reaches an N-domain with a macroscopic size. In connection with this I–N transition, the concept of the initial condition sensitivity is also developed so as to clarify experimentally observed nonlinear characteristics of this material.In the next, using a more simplified model for the many-exciton system, we theoretically study the early time quantum dynamics of the exciton proliferation, which finally results in the formation of a domain with a large number of excitons. For this purpose, we derive a stepwise iterative equation to describe the exciton proliferation, and clarify the origin of the initial condition sensitivity.Possible differences between a photo-induced nonequilibrium phase and an equilibrium phase at high temperatures are also clarified from general and conceptional points of view, in connection with recent experiments on the photo-induced phase transition in an organo-metallic complex crystal. It will be shown that the photo-induced phase can make a new interaction appear as a broken symmetry only in this phase, even when this interaction is almost completely hidden in all the equilibrium phases, such as the ground state and other high-temperature phases. The relation between the photo-induced nonequilibrium phase and the hysteresis induced nonequilibrium one is also qualitatively discussed.We will be concerned with a macroscopic parity violation and a ferro- (or super-para-) electricity, induced by a photogenerated electron in the perovskite type quantum dielectric SrTiO3. The photogenerated electron in the 3d band of Ti is assumed to couple weakly, but quadratically, with soft-anharmonic T1u phonons, and strongly but linearly to the breathing (A1g) type high energy phonons. These two types of electron–phonon coupling result in two types of polarons, a super-para-electric (SPE) large polaron with a quasi-global parity violation, and an off-centre type self-trapped polaron with only a local parity violation. This SPE large polaron, being equal to a charged and conductive ferroelectric domain, greatly enhances both the quasi-static electric susceptibility and the electronic conductivity.We also briefly review recent successes to observe the PSPTs more directly by using x-ray measurements.