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We demonstrate experimentally a method of all-optical selective rotational control in gas mixtures. Using an optical centrifuge - an intense laser pulse whose linear polarization rotates at an accelerated rate, we simultaneously excite two different molecular species to two different rotational frequencies of choice. The new level of control is achieved by shaping the centrifuge spectrum according to the rotational spectra of the centrifuged molecules. The shaped optical centrifuge releases one molecular species earlier than the other, therefore separating their target rotational frequencies and corresponding rotational states. The technique will expand the utility of rotational control in the studies of the effects of molecular rotation on collisions and chemical reactions.
We use an optical centrifuge to excite coherent rotational wave packets in N$_2$O, CS$_2$ and OCS molecules with rotational quantum numbers reaching up to J=465, 690 and 1186, respectively. Time-resolved rotational spectroscopy at such ultra-high lev
A proof-of-concept framework for identifying molecules of unknown elemental composition and structure using experimental rotational data and probabilistic deep learning is presented. Using a minimal set of input data determined experimentally, we des
Strong laser-induced magnetization of oxygen gas at room temperature and atmospheric pressure is achieved experimentally on the sub-nanosecond time scale. The method is based on controlling the electronic spin of paramagnetic molecules by means of ma
We report on the first experimental demonstration of enantioselective rotational control of chiral molecules with a laser field. In our experiments, two enantiomers of propylene oxide are brought to accelerated unidirectional rotation by means of an
Two-photon excitation (TPE) proceeds via a virtual pathway, which depends on the accessibility of one or more intermediate states, and, in the case of non-centrosymmetric molecules, an additional dipole pathway involving the off-resonance dipole-allo