Retrieval of the molecular orientation distribution from atom-pair angular distributions

Abstract

Imaging laser-induced rotational dynamics is an important and active field due to its applications in capturing reactions in the molecular frame and in molecular imaging. Experimental measurement of the molecular orientation distribution, as a function of the Euler angles, has only been demonstrated for special cases when the detectable signal is generated along the molecular symmetry axis. Here we developed the general theory that maps the probability density distribution of the molecular orientation to the atom-pair angular distributions for nonlinear molecules. With the theory, the molecular orientation distribution can be retrieved from the measured atom-pair angular distribution, which we demonstrate experimentally using ultrafast electron diffractive imaging of impulsively aligned trifluoro-iodomethane molecules. Here, the retrieved molecular orientation distribution is in good agreement with direct numerical simulations of the time-dependent Schrodinger equation using the experimental conditions. Unlike the existing retrieval methods, the retrieval method does not require solving Schrodinger equation, works for any alignment method, and is in principle applicable to asymmetric top molecules.