Laser‐Driven Transient Phase Oscillations in Individual Spin Crossover Particles

Abstract An unusual expansion dynamics of individual spin crossover nanoparticles is studied by ultrafast transmission electron microscopy. After exposure to nanosecond laser pulses, the particles exhibit considerable length oscillations during and after their expansion. The vibration period of 50–100 ns is of the same order of magnitude as the time that the particles need for a transition from the low‐spin to the high‐spin state. The observations are explained in Monte Carlo calculations using a model where elastic and thermal coupling between the molecules within a crystalline spin crossover particle govern the phase transition between the two spin states. The experimentally observed length oscillations are in agreement with the calculations, and it is shown that the system undergoes repeated transitions between the two spin states until relaxation in the high‐spin state occurs due to energy dissipation. Spin crossover particles are therefore a unique system where a resonant transition between two phases occurs in a phase transformation of first order.