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arXiv:1404.5677 · Physical Review Letters

Effects of Ultrafast Molecular Rotation on Collisional Decoherence

A. Milner, Aleksey Korobenko, John W. Hepburn, Valery Milner

Published Jul 25, 2014• 61 citations
arXivHTMLPDF

Abstract

Using an optical centrifuge to control molecular rotation in an extremely broad range of angular momenta, we study coherent rotational dynamics of nitrogen molecules in the presence of collisions. We cover the range of rotational quantum numbers between J=8 and J=66 at room temperature and study a crossover between the adiabatic and nonadiabatic regimes of rotational relaxation, which cannot be easily accessed by thermal means. We demonstrate that the rate of rotational decoherence changes by more than an order of magnitude in this range of J values and show that its dependence on J can be described by a simplified scaling law.

DOI
10.1103/physrevlett.113.043005

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Using an optical centrifuge to control molecular rotation in an extremely broad range of angular momenta, we study coherent rotational dynamics of nitrogen molecules in the presence of collisions. We cover the range of rotational quantum numbers between J=8 and J=66 at room temperature and study a crossover between the adiabatic and nonadiabatic regimes of rotational relaxation, which cannot be easily accessed by thermal means. We demonstrate that the rate of rotational decoherence changes by more than an order of magnitude in this range of J values and show that its dependence on J can be described by a simplified scaling law.
Abstract Quantum coherence plays an essential role in diverse natural phenomena and technological applications. The unavoidable coupling of the quantum system to an uncontrolled environment incurs dissipation that is often described using the secular approximation. Here we probe the limit of this approximation in the rotational relaxation of molecules due to thermal collisions by using the laser-kicked molecular rotor as a model system. Specifically, rotational coherences in N2O gas (diluted in He) are created by two successive nonresonant short and intense laser pulses and probed by studying the change of amplitude of the rotational alignment echo with the gas density. By interrogating the system at the early stage of its collisional relaxation, we observe a significant variation of the dissipative influence of collisions with the time of appearance of the echo, featuring a decoherence process that is well reproduced by the nonsecular quantum master equation for modeling molecular collisions.
The control of ultrafast molecular rotational motion has benefited from the development of innovative techniques in strong-field laser physics. Here, we theoretically demonstrate a novel type of coherent control by inducing rotation of an asymmetric-top molecule about two different molecular axes. An optical centrifuge is applied to the hydrogen sulfide (H 2 S) molecule to create a molecular superrotor, an object performing ultrafast rotation about a well-defined axis. Using two distinct pulse envelopes for the optical centrifuge, we show that H 2 S can be excited along separate pathways of rotational states. This leads to stable rotation about two entirely different molecular axes while ensuring rotation is about the propagation direction of the centrifuge, i.e., the laboratory-fixed Z -axis. The presented scheme to control the angular momentum alignment of a molecule will, for instance, be useful in studies of molecule–molecule or molecule–surface scattering, especially due to the large amounts of energy associated with superrotors, which can even be controlled by changing the duration of the optical centrifuge pulse.
Abstract Quantum coherence plays an essential role in diverse natural phenomena and technological applications. The unavoidable coupling of the quantum system to an uncontrolled environment incurs dissipation that is often described using the secular approximation. Here we probe the limit of this approximation in the rotational relaxation of molecules due to thermal collisions by using the laser-kicked molecular rotor as a model system. Specifically, rotational coherences in N2O gas (diluted in He) are created by two successive nonresonant short and intense laser pulses and probed by studying the change of amplitude of the rotational alignment echo with the gas density. By interrogating the system at the early stage of its collisional relaxation, we observe a significant variation of the dissipative influence of collisions with the time of appearance of the echo, featuring a decoherence process that is well reproduced by the nonsecular quantum master equation for modeling molecular collisions.
We experimentally demonstrate that the rotation of molecules embedded in helium nanodroplets can be controlled with an optical centrifuge, allowing for the study of molecular dynamics inside the strongly interacting many-body environment of superfluid helium at variable levels of rotational excitation. By doping the droplets with dimers of nitric oxide, (NO)_{2}, and measuring the degree of their centrifuge-induced alignment as a function of time, we show both the forced in-field rotation of molecules in a continuous range of frequencies, as well as the field-free resonant rotation with a long nanosecond-scale decay. The ability to control and monitor the rotational dynamics of molecular rotors inside the superfluid medium may shed new light on superfluidity and the interaction of superfluids with defects at the atomic level.
Laser control of molecular rotation is an area of active research. A number of recent studies has aimed at expanding the reach of rotational control to extreme, previously inaccessible rotational states, as well as controlling the directionality of molecular rotation. Dense ensembles of molecules undergoing ultrafast uni-directional rotation, known as molecular superrotors, are anticipated to exhibit unique properties, from spatially anisotropic diffusion and vortex formation to the creation of powerful acoustic waves and tuneable THz radiation. Here we describe our recent progress in controlling molecular rotation in the regime of high rotational excitation. We review two experimental techniques of producing uni-directional rotational wave packets with a "chiral train" of femtosecond pulses and an "optical centrifuge". Three complementary detection methods, enabling the direct observation, characterization and control of the superrotor states, are outlined: the one based on coherent Raman scattering, and two other methods employing both resonant and non-resonant multi-photon ionization. The capabilities of the described excitation and detection techniques are demonstrated with a few examples. The paper is concluded with an outlook for future developments.
A macroscopic manifestation of superfluidity is that objects moving through liquid helium experience negligible friction below the Landau critical velocity. How this frictionless motion breaks down at the nanoscale remains an open question. Molecules embedded in helium nanodroplets represent a well-controlled system for studying this breakdown, yet none has reached the regime of strong dissipative coupling, when energy transfer from the molecule to the superfluid dominates the observed dynamics. Molecular rotation, induced by short laser pulses, offer a suitable probe to reach rotational energies in the range of the roton gap, where superfluid helium supports a large number of elementary excitations. However, the solvation shell around a rotating molecule caps the energy reachable by a free rotor after impulsive excitation well below the roton excitation energy. Here we show that continuous driving with an ultraslow optical centrifuge overcomes this limitation: the strong field dresses the molecule into pendular states whose energies fall within the spectrum of the collective excitations of the superfluid, placing the system in the strong-dissipation regime. The resulting rapid thermalization locks the molecule to the rotating field until the rotation-induced level splittings overtake the thermalization rate, beyond which the molecular alignment is progressively lost. Our approach offers a direct measurement of the molecule-bath coupling in a quantum fluid.