Quantum unidirectional rotation directly imaged with molecules

Mizuse, Kenta; Kitano, Koji; Hasegawa, H.; Ohshima, Yasuhiro

doi:10.1126/sciadv.1400185

Cited by 56 publications

(42 citation statements)

References 41 publications

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“…The later approach was theoretically suggested in [22], based on quantum mechanical arguments and it relied on exciting unidirectional rotation (UDR) of molecules with the help of a pair of nonresonant, delayed cross-polarized laser pulses. This excitation technique had been suggested in [23,24], further experimentally demonstrated in [25][26][27], investigated in detail, both from the quantum and classical perspectives in [28] and generalized to chiral trains of multiple pulses in [29,30]. In a recent paper [31] we showed that linearly polarized laser fields whose polarization axis twists with time in some plane are able to orient generic asymmetric molecules.…”

Section: Introductionmentioning

confidence: 96%

Selective Orientation of Chiral Molecules by Laser Fields with Twisted Polarization

Tutunnikov

Gershnabel

Gold

et al. 2018

J. Phys. Chem. Lett.

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We explore a pure optical method for enantioselective orientation of chiral molecules by means of laser fields with twisted polarization. Several field implementations are considered, including a pair of delayed, cross-polarized laser pulses, an optical centrifuge, and polarization-shaped pulses. We show that these schemes lead to out-of-phase time-dependent dipole signals for different enantiomers, and we also predict a substantial permanent molecular orientation persisting long after the laser fields are over. The underlying classical orientation mechanism common to all of these fields is discussed, and its operation is demonstrated for a range of chiral molecules of various complexity: hydrogen thioperoxide (HSOH), propylene oxide (CHCHCHO), and ethyl oxirane (CHCHCHCHO). The presented results demonstrate generality, versatility, and robustness of this optical method for manipulating molecular enantiomers in the gas phase.

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Section: Introductionmentioning

confidence: 96%

Selective Orientation of Chiral Molecules by Laser Fields with Twisted Polarization

Tutunnikov

Gershnabel

Gold

et al. 2018

J. Phys. Chem. Lett.

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“…Recent progress in creating and detecting unidirectional rotation of molecules [7][8][9][10][11]18] revived the interest in controlling molecular rotation with external magnetic fields. Magnetic effects could further broaden the controllability provided by tunable rotational excitation, including control of molecular collisions [12,13] and scattering of molecules at gas-solid interfaces [14], molecular trajectories [15] and formation of gas vortices [16], optical [5, 17] and acoustic [19,20] properties of a gas of rotating molecules.…”

Section: Pacs Numbersmentioning

confidence: 99%

Dynamics of molecular superrotors in an external magnetic field

Korobenko

Milner

2015

J. Phys. B: At. Mol. Opt. Phys.

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We excite diatomic oxygen and nitrogen to high rotational states with an optical centrifuge and study their dynamics in external magnetic field. Ion imaging is employed to directly visualize, and follow in time, the rotation plane of molecular superrotors. The two different mechanisms of interaction between the magnetic field and the molecular angular momentum in paramagnetic oxygen and non-magnetic nitrogen lead to the qualitatively different behaviour. In nitrogen, we observe the precession of the molecular angular momentum around the field vector. In oxygen, strong spin-rotation coupling results in faster and richer dynamics, encompassing the splitting of the rotation plane in three separate components. As the centrifuged molecules evolve with no significant dispersion of the molecular wave function, the observed magnetic interaction presents an efficient mechanism for controlling the plane of molecular rotation. PACS numbers:Magnetic field is one of the most powerful tools for controlling atomic and molecular dynamics. Both translational and rotational degrees of freedom of molecules have been successfully manipulated via various types of magnetic interaction. Alignment of molecular axes has been accomplished by creating pendular states in paramagnetic molecules at low temperature [1,2]. Gyroscopic precession along the direction of the applied magnetic field has been suggested for non-magnetic molecules in dispersionless "cogwheel" states [3,4]. Spin-rotational coupling has been recently utilized for converting unidirectional molecular rotation into axial alignment, manifested through magneto-rotational optical birefringence under ambient conditions [5,6].Recent progress in creating and detecting unidirectional rotation of molecules [7][8][9][10][11]18] revived the interest in controlling molecular rotation with external magnetic fields. Magnetic effects could further broaden the controllability provided by tunable rotational excitation, including control of molecular collisions [12,13] and scattering of molecules at gas-solid interfaces [14], molecular trajectories [15] and formation of gas vortices [16], optical [5, 17] and acoustic [19,20] properties of a gas of rotating molecules.With the invention of the optical centrifuge technique [21,22], a very flexible control over the degree of rotational excitation became available. The technique proved capable of producing synchronously rotating molecules with narrow rotational state distribution in a wide variety of species up to extremely high angular frequencies [5,23]. However, the spatial orientation of the induced angular momentum is often defined by the propagation direction of the excitation laser beam, and is therefore not easy to manipulate.Here we demonstrate how an applied magnetic field can be used to rotate the plane of molecular rotation. The described method is applicable to a wide variety of molecules and relies on the coupling between the rotation of a molecule and its magnetic moment. An applied magnetic field causes this moment to precess, "...

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“…6(b), the energy of the 9th harmonic photon differs from the expected value, which is nine times the energy of the fundamental photon. This shift can be interpreted as a manifestation of the rotational Doppler effect observed recently in molecular rotors probed through linear [27][28][29][30] and nonlinear 31 optical interactions. A closer inspection to the quantum state excited by the aligning pulse in Fig.…”

Section: Discussionmentioning

confidence: 51%

Polarization shaping of high-order harmonics in laser-aligned molecules

Skantzakis

Chatziathanasiou

Carpeggiani

et al. 2016

Sci Rep

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The present work reports on the generation of short-pulse coherent extreme ultraviolet radiation of controlled polarization. The proposed strategy is based on high-order harmonics generated in pre-aligned molecules. Field-free molecular alignment produced by a short linearly-polarized infrared laser pulse is used to break the isotropy of a gas medium. Driving the aligned molecules by a circularly-polarized infrared pulse allows to transfer the anisotropy of the medium to the polarization of the generated harmonic light. The ellipticity of the latter is controlled by adjusting the angular distribution of the molecules at the time they interact with the driving pulse. Extreme ultraviolet radiation produced with high degree of ellipticity (close to circular) is demonstrated.

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Quantum unidirectional rotation directly imaged with molecules

Abstract: High resolution imaging fully characterizes quantum-mechanical signatures of direction-controlled molecular rotational dynamics.

Cited by 56 publications

References 41 publications

Selective Orientation of Chiral Molecules by Laser Fields with Twisted Polarization

Selective Orientation of Chiral Molecules by Laser Fields with Twisted Polarization

Dynamics of molecular superrotors in an external magnetic field

Polarization shaping of high-order harmonics in laser-aligned molecules

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