Capturing the photo-induced dynamics of nano-molecules by X-ray free electron laser induced Coulomb explosion

We performed reaction dynamics simulations to demonstrate that the vibrational dynamics of C₆₀ induced by infrared (IR) pulses can be traced by triggering Coulomb explosion with intense femtosecond X-ray free electron laser (XFEL) probe pulses. The time series of the angular anisotropy β(t) of fast C⁺ and C²⁺ fragments of C₆₀⁶⁰⁺ produced by such an XFEL pulse reflects the instantaneous structure of C₆₀ vibrationally excited by IR pulses. The phases and amplitudes of excited vibrational modes and the coupling between excited modes can be successfully extracted from the expansion of β(t) in terms of vibrational modes. This proof-of-principle simulation clearly demonstrates that various information of the structures and reaction dynamics of large clusters or biomolecules can be retrieved by decomposing the experimentally determined β(t) into vibrational modes.