Laser Control of Ultrafast Molecular Rotation

Milner, Valery; Hepburn, J. W.

doi:10.1002/9781119096276.ch10

Cited by 10 publications

(13 citation statements)

References 43 publications

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“…The preparation of molecules in highly excited rotational states has seen a range of innovative methods developed in recent years. 42,43 One of these is the optical centrifuge, 44,45 which is a non-resonant, linearly polarized laser pulse that undergoes accelerated rotation along the direction of propagation (see Fig. 2).…”

Section: Rotational Excitation With An Optical Centrifugementioning

confidence: 99%

RichMol: A general variational approach for rovibrational molecular dynamics in external electric fields

Owens

Yachmenev

2018

The Journal of Chemical Physics

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In this paper, a general variational approach for computing the rovibrational dynamics of polyatomic molecules in the presence of external electric fields is presented. Highly accurate, full-dimensional variational calculations provide a basis of field-free rovibrational states for evaluating the rovibrational matrix elements of high-rank Cartesian tensor operators and for solving the time-dependent Schrödinger equation. The effect of the external electric field is treated as a multipole moment expansion truncated at the second hyperpolarizability interaction term. Our fully numerical and computationally efficient method has been implemented in a new program, RichMol, which can simulate the effects of multiple external fields of arbitrary strength, polarization, pulse shape, and duration. Illustrative calculations of two-color orientation and rotational excitation with an optical centrifuge of NH are discussed.

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Section: Rotational Excitation With An Optical Centrifugementioning

confidence: 99%

RichMol: A general variational approach for rovibrational molecular dynamics in external electric fields

Owens

Yachmenev

2018

The Journal of Chemical Physics

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“…Characteristic value of the chirp rate β in these setups is 1ps −2 (see, for example, [34,35]). With this value of β, and the molecules already in use in OC experiments [8,35,36], parameter P 2 (see Eq. 2) varies from 11.2 (for Cl 2 ) through 0.73 (N 2 ) to 0.09 (D 2 ).…”

Section: Relevance To Existing Experimentsmentioning

confidence: 99%

“…[36]. The experiment involved N 2 molecules (P 2 = 0.73) and the OC laser pulse had a varying amplitude of a Gaussian form,…”

Section: Relevance To Existing Experimentsmentioning

confidence: 99%

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Quantum versus classical dynamics in the optical centrifuge

Armon

Frièdland

2017

Phys. Rev. A

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The interplay between classical and quantum mechanical evolution in the optical centrifuge (OC) is discussed. The analysis is based on the quantum mechanical formalism starting from either the ground state or a thermal ensemble. Two resonant mechanisms are identified, i.e. the classical autoresonance and the quantum mechanical ladder-climbing, yielding different dynamics and rotational excitation efficiencies. The rotating wave approximation is used to analyze the two resonant regimes in the associated dimensionless two-parameter space and calculate the OC excitation efficiency. The results show good agreement between numerical simulations and theory and are relevant to existing experimental setups.

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“…The main obstacle to overcome when generating large amounts of rotational excitation is that selection rules permit only small changes in the overall angular momentum J. With the development of clever adiabatic and non-adiabatic approaches [5,6], this is now far less challenging and it is possible to efficiently create rotational wavepackets with a narrow and well-defined distribution of states. Molecular superrotors, as they are known in the literature, display novel behavior.…”

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confidence: 99%

Climbing the Rotational Ladder to Chirality

et al. 2018

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Molecular chirality is conventionally understood as space-inversion-symmetry breaking in the equilibrium structure of molecules. Less well known is that achiral molecules can be made chiral through extreme rotational excitation. Here, we theoretically demonstrate a clear strategy for generating rotationally-induced chirality (RIC): An optical centrifuge rotationally excites the phosphine molecule (PH3) into chiral cluster states that correspond to clockwise (R-enantiomer) or anticlockwise (Lenantiomer) rotation about axes almost coinciding with single P-H bonds. Application of a strong dc electric field during the centrifuge pulse favors the production of one rotating enantiomeric form over the other, creating dynamically chiral molecules with permanently oriented rotational angular momentum. This essential step toward characterizing RIC promises a fresh perspective on chirality as a fundamental aspect of nature.

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Laser Control of Ultrafast Molecular Rotation

Cited by 10 publications

References 43 publications

RichMol: A general variational approach for rovibrational molecular dynamics in external electric fields

RichMol: A general variational approach for rovibrational molecular dynamics in external electric fields

Quantum versus classical dynamics in the optical centrifuge

Climbing the Rotational Ladder to Chirality

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