Real Time Quantum Dynamics of Spontaneous Translational Symmetry Breakage in the Early Stage of Photo-induced Structural Phase Transitions

Real time quantum dynamics of the spontaneous translational symmetry breakage in the early stage of photoinduced structural phase transitions is reviewed and supplementally explained, under the guide of the Toyozawa theory, which is exactly in compliance with the conservation laws of the total momentum and energy. At the Franck Condon state, an electronic excitation just created by a visible light, is in a plane wave state, extended all over the crystal. While, after the lattice relaxation having been completed, it is localized around a certain lattice site of the crystal, as a new excitation. Is there a sudden shrinkage of the excitation wave function, in between. The wave function never shrinks, but only the spatial, or inter lattice site quantum coherence, interference of the excitation disappears, as the lattice relaxation proceeds. This is nothing but the spontaneous breakage of translational symmetry.Comment: Applied Science 2018, MDP

Cooperative domain type interlayer sp3sp^3-bond formation in graphite

Using the classical molecular dynamics and the semiempirical Brenner's potential, we theoretically study the interlayer sigma bond formation, as cooperative and nonlinear phenomena induced by visible light excitations of a graphite crystal. We have found several cases, wherein the excitations of certain lattice sites result in new interlayer bonds even at non-excited sites. We have also found that, a new interlayer bond is easier to be formed around a bond, if it is already existing. As many more sites are going to be excited, the number of interlayer bonds increases nonlinearly with the number of excited sites. This nonlinearity shows 1.7 power of the total number of excited sites, corresponding to about three- or four-photon process.Comment: 7 pages, 8 figure

Coherent dynamics of photoinduced nucleation processes

We study the dynamics of initial nucleation processes of photoinduced structural change of molecular crystals. In order to describe the nonadiabatic transition in each molecule, we employ a model of localized electrons coupled with a fully quantized phonon mode, and the time-dependent Schr\"odinger equation for the model is numerically solved. We found a minimal model to describe the nucleation induced by injection of an excited state of a single molecule in which multiple types of intermolecular interactions are required. In this model coherently driven molecular distortion plays an important role in the successive conversion of electronic states which leads to photoinduced cooperative phenomena.Comment: 14 pages, 5 figure