The electron-phonon coupling and the corresponding energy exchange are investigated experimentally and by ab initio theory in nonequilibrium states of the free-electron metal aluminium. The temporal evolution of the atomic mean-squared displacement in laser-excited thin freestanding films is monitored by femtosecond electron diffraction. The electron-phonon coupling strength is obtained for a range of electronic and lattice temperatures from density functional theory molecular dynamics simulations. The electron-phonon coupling parameter extracted from the experimental data in the framework of a two-temperature model (TTM) deviates significantly from the ab initio values. We introduce a nonthermal lattice model (NLM) for describing nonthermal phonon distributions as a sum of thermal distributions of the three phonon branches. The contributions of individual phonon branches to the electron-phonon coupling are considered independently and found to be dominated by longitudinal acoustic phonons. Using all material parameters from first-principles calculations except the phonon-phonon coupling strength, the prediction of the energy transfer from electrons to phonons by the NLM is in excellent agreement with time-resolved diffraction data. Our results suggest that the TTM is insufficient for describing the microscopic energy flow even for simple metals like aluminium and that the determination of the electron-phonon coupling constant from time-resolved experiments by means of the TTM leads to incorrect values. In contrast, the NLM describing transient phonon populations by three parameters appears to be a sufficient model for quantitatively describing electron-lattice equilibration in aluminium. We discuss the general applicability of the NLM and provide a criterion for the suitability of the two-temperature approximation for other metals

We study the basic mechanisms allowing light to photoswitch at the molecular scale a spin-crossover material from a low- to a high-spin state. Combined femtosecond x-ray absorption performed at LCLS X-FEL and optical spectroscopy reveal that the structural stabilization of the photoinduced high-spin state results from a two step structural trapping. Molecular breathing vibrations are first activated and rapidly damped as part of the energy is sequentially transferred to molecular bending vibrations. During the photoswitching, the system follows a curved trajectory on the potential energy surface.

International audiencePhotoinduced phase transformations [1,2] occur when a laser pulse impacts a material, thereby transforming its electronic and/or structural orders, consequently directing the functionalities [3,4,5,6,7]. The transient nature of photoinduced states has thus far severely limited the application scope. It is of paramount importance to explore whether structural feedback during the solid deformation has capacity to amplify and stabilize photoinduced transformations. Contrary to coherent optical phonons long under scrutiny [8,9,10] , coherently propagating cell deformations over acoustic timescale [11,12,13,14] have not been explored to similar degree, particularly in light of cooperative elastic interactions. Herein we demonstrate experimentally and theoretically a self-amplified responsiveness in a spin-crossover material [15] during its delayed volume expansion. The cooperative response at material scale prevails above a threshold excitation, significantly extending the lifetime of photoinduced states. Such elastically-driven cooperativity triggered by a light pulse offers a new efficient route to the generation and stabilization of photoinduced phases in many volume-changing materials