Quantum resonances in selective rotational excitation of molecules with a sequence of ultrashort laser pulses

Abstract

We investigate experimentally the effect of quantum resonance in the rotational excitation of the simplest quantum rotor - a diatomic molecule. By using the techniques of high-resolution femtosecond pulse shaping and rotational state-resolved detection, we measure directly the amount of energy absorbed by molecules interacting with a periodic train of laser pulses, and study its dependence on the train period. We show that the energy transfer is significantly enhanced at quantum resonance, and use this effect for demonstrating selective rotational excitation of two nitrogen isotopologues, ${}^{14}{N}_2$ and ${}^{15}{N}_2$. Moreover, by tuning the period of the pulse train in the vicinity of a fractional quantum resonance, we achieve spin-selective rotational excitation of para- and ortho-isomers of ${}^{15}{N}_2$.

5 pages, 4 figures

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• Experimental demonstration of coherent control in quantum chaotic systems
• Observation of nondispersing classical-like molecular rotation
• Field-free long-lived alignment of molecules in extreme rotational states
• Control of quantum localization and classical diffusion in laser-kicked molecular rotors
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• Unified parameter for localization in isotope-selective rotational excitation of diatomic molecules using a train of optical pulses
• Topological charges of periodically kicked molecules
• Isotopologue-selective laser cooling of molecules
• Symmetry and dynamics universality of supermetal in quantum chaos
• State- and molecule-selective rotational control in gas mixtures with a shaped optical centrifuge
• Impact of Boundary Conditions on the Double-Kicked Quantum Rotor