Long-Lasting Molecular Orientation Induced by a Single Terahertz Pulse

Xu, Long; Tutunnikov, Ilia; Gershnabel, E.; Prior, Yehiam; Averbukh, Ilya Sh.

doi:10.1103/physrevlett.125.013201

Cited by 36 publications

(39 citation statements)

References 43 publications

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“…2(a) and 2(b), which are before and after 0 ps, respectively]. This transient orientation induced by single THz pulses is expected and has been observed before [41][42][43][44][45][46][47][48].…”

Section: Resultsmentioning

confidence: 56%

“…Notice, the persistent orientation appearing in the directions of each of the pulses (along the X and Y axes) does not rely on chirality. It was recently shown that single THz pulses applied to symmetric-and asymmetrictop molecules also induce persistent orientation [48]. In contrast, both the appearance and permanency of the orientation along the propagation direction which is perpendicular to both the X and Y axes depend on the chirality of the molecule.…”

Section: Resultsmentioning

confidence: 99%

“…Although transient orientation revival spikes may periodically appear on long time scales, the orientation signature generally rides on a zero baseline and its time average is exactly zero. Recently, it was shown that a single linearly polarized THz pulse induces persistent orientation in symmetric-and asymmetric-top molecules, including chiral molecules [48]. In contrast to the transient signal, persistent orientation means that the time-averaged post-pulse orientation degree differs from zero on a long time scale, in the case discussed in this paper -exceeding the duration of the THz pulse by several orders of magnitude.…”

Section: Introductionmentioning

confidence: 85%

“…c are the rotational constants (A > B > C), and I a < I b < I c are the molecular moments of inertia. The time-dependent Schrödinger equation i ∂ t |Ψ(t) =Ĥ(t)|Ψ(t) is solved by numerical exponentiation of the Hamiltonian matrix (see Expokit [52]), and a detailed description of our numerical scheme can be found in [48]. In our simulations, the computational basis included all the rotational states with an angular momentum J ≤ 44.…”

Section: Methodsmentioning

confidence: 99%

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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: Resultsmentioning

confidence: 56%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 85%

Section: Methodsmentioning

confidence: 99%

See 2 more Smart Citations

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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“…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%

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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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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Long-Lasting Molecular Orientation Induced by a Single Terahertz Pulse

Cited by 36 publications

References 43 publications

Selective Orientation of Chiral Molecules by Laser Fields with Twisted Polarization

Selective Orientation of Chiral Molecules by Laser Fields with Twisted Polarization

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

Controlling molecular orientation by laser pulses with two different envelope shapes

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