Enantioselective orientation of chiral molecules induced by terahertz pulses with twisted polarization

Tutunnikov, Ilia; Xu, Long; Field, Robert W.; Nelson, Keith A.; Prior, Yehiam; Averbukh, Ilya Sh.

doi:10.1103/physrevresearch.3.013249

Cited by 29 publications

(35 citation statements)

References 68 publications

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“…The long-lasting orientation induced by a two-color pulse has an intricate dependence on both the molecular polarizability and hyperpolarizability. Related effects have been recently observed in chiral molecules excited by one-color laser pulses with twisted polarization [30,32] and investigated in non-linear molecules excited by THz pulses [23,33].…”

Section: Introductionmentioning

confidence: 91%

“…There are several laser-based strategies for achieving molecular orientation in the gas phase, including using a combination of intense non-resonant laser and weak electrostatic fields [7][8][9][10][11][12][13][14][15], and using strong single-cycle terahertz (THz) pulses [16][17][18][19][20][21][22][23], alone or together with optical pulses [24][25][26]. In addition, laser and THz pulses with twisted polarization were shown to be effective for inducing enantioselective orientation of chiral molecules [27][28][29][30][31][32][33].…”

Section: Introductionmentioning

confidence: 99%

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Long-Lasting Orientation of Symmetric-Top Molecules Excited by Two-Color Femtosecond Pulses

Tutunnikov

Prior

et al. 2021

Front. Phys.

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Impulsive orientation of symmetric-top molecules excited by two-color femtosecond pulses is considered. In addition to the well-known transient orientation appearing immediately after the pulse and then reemerging periodically due to quantum revivals, we report the phenomenon of field-free long-lasting orientation. Long-lasting means that the time averaged orientation remains non-zero until destroyed by other physical effects, e.g., intermolecular collisions. The effect is caused by the combined action of the field-polarizability and field-hyperpolarizability interactions. The dependence of degree of long-lasting orientation on temperature and pulse parameters is considered. The effect can be measured by means of second (or higher-order) harmonic generation, and may be used to control the deflection of molecules traveling through inhomogeneous electrostatic fields.

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Section: Introductionmentioning

confidence: 91%

Section: Introductionmentioning

confidence: 99%

Long-Lasting Orientation of Symmetric-Top Molecules Excited by Two-Color Femtosecond Pulses

Tutunnikov

Prior

et al. 2021

Front. Phys.

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“…By taking advantage of the sign difference property of optical rotations, it has become promising to select enantiomers by designing coherent quantum optical schemes [9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26]. The concept of the adiabatic passage techniques, such as stimulated Raman adiabatic passages [27,28] and shortcuts to adiabaticity [29,30], was proposed to generate efficient and robust detection and separation of chiral molecules [31][32][33][34][35][36].…”

Section: Introductionmentioning

confidence: 99%

Cyclic three-level-pulse-area theorem for enantioselective state transfer of chiral molecules

Guo,

Gong,

et al. 2021

Preprint

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We derive a pulse-area theorem for a cyclic three-level system, an archetypal model for exploring enantioselective state transfer (ESST) in chiral molecules driven by three linearly polarized microwave pulses.By dividing the closed-loop excitation into two separate stages, we obtain both amplitude and phase conditions of three control fields to generate high fidelity of ESST. As a proof of principle, we apply this pulse-area theorem to the cyclohexylmethanol molecules (C 7 H 14 O), for which three rotational states are connected by the a-type, b-type, and c-type components of the transition dipole moments in both centerfrequency resonant and detuned conditions. Our results show that two enantiomers with opposite handedness can be transferred to different target states by designing three microwave pulses that satisfy the amplitude and phase conditions at the transition frequencies. The corresponding control schemes are robust against the time delays between the two stages. We suggest that the two control fields used in the second stage should be applied simultaneously for practical applications. This work contributes an alternative pulse-area theorem to the field of quantum control, which has the potential to determine the chirality of enantiomers in a mixture.

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“…Daems et al [47] and Yu et al [48] obtained an efficient and long-lived orientation of the molecule. In a recent study, the enantioselective orientation of chiral molecules was achieved by terahertz pulses with twisted polarization, and the orientation persists for a long time [49].…”

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confidence: 99%

Controlling molecular orientation by laser pulses with two different envelope shapes

Guo

Zhou

Chai

et al. 2021

Int J of Quantum Chemistry

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We use density matrix theory to numerically simulate the orientation of LiH molecules induced by laser pulses with two different envelope shapes. The results show that the envelope shape of the terahertz single-cycle laser pulse (SCP) has significant effects on molecular orientation degree and duration. When a SCP with adjusted laser field amplitude and carrier envelope phase is used to steer the molecular orientation, a larger orientation degree can be obtained by the Gaussian-shaped SCP, while a longer orientation duration can be realized by the sin 2 -shaped SCP.When combined with the two-color femtosecond laser pulse, the sin 2 -shaped SCP is better than Gaussian-shaped SCP, either in improving orientation degree and duration or in stability and controllability shown with increasing temperature. The optimal molecular orientation can be realized under the combination of the two-color femtosecond laser pulse and sin 2 -shaped SCP which has the appropriate delay time: the maximal orientation degree reaches 0.801 at 0 K and 0.450 at 20 K, the maximal orientation duration is 31.3% of the rotational period at 0 K.

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Enantioselective orientation of chiral molecules induced by terahertz pulses with twisted polarization

Cited by 29 publications

References 68 publications

Long-Lasting Orientation of Symmetric-Top Molecules Excited by Two-Color Femtosecond Pulses

Long-Lasting Orientation of Symmetric-Top Molecules Excited by Two-Color Femtosecond Pulses

Cyclic three-level-pulse-area theorem for enantioselective state transfer of chiral molecules

Controlling molecular orientation by laser pulses with two different envelope shapes

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