Monitoring atomic cluster expansion by high-harmonic generation.

High-harmonic generation is shown to be capable of providing time-resolved information about the particle density of a complex system. As an example, we study numerically high-harmonic generation from expanding xenon clusters in a pump-probe laser scheme, where the pump laser pulse induces the cluster explosion and the probe pulse generates harmonics in the expanding cluster. We show that the high-harmonic spectra characterize the properties of the expanding cluster. Hence, measuring the dependence of the harmonic signal on the pump-probe delay suggests itself as an experimental tool to monitor many-particle dynamics with unique temporal resolution; based on optical measurements, this technique is naturally free from any spatial charge effects.