Optimization of the double-laser-pulse scheme for enantioselective orientation of chiral molecules.

We present a comprehensive study of enantioselective orientation of chiral molecules excited by a pair of delayed cross-polarized femtosecond laser pulses. We show that by optimizing the pulses' parameters, a significant degree (∼10%) of enantioselective orientation can be achieved at 0 and 5 K rotational temperatures. This study suggests a set of reasonable experimental conditions for inducing and measuring strong enantioselective orientation. The strong enantioselective orientation and the wide availability of the femtosecond laser systems required for the proposed experiments may open new avenues for discriminating and separating molecular enantiomers.

Long-Lasting Molecular Orientation Induced by a Single Terahertz Pulse.

We present a novel, previously unreported phenomenon appearing in a thermal gas of nonlinear polar molecules excited by a single THz pulse. We find that the induced orientation lasts long after the excitation pulse is over. In the case of symmetric-top molecules, the time-averaged orientation remains indefinitely constant, whereas in the case of asymmetric-top molecules the orientation persists for a long time after the end of the pulse. We discuss the underlying mechanism, study its nonmonotonous temperature and amplitude dependencies, and show that there exist optimal parameters for maximal residual orientation. The persistent orientation implies a long-lasting macroscopic dipole moment, which may be probed by even harmonic generation and may enable deflection by inhomogeneous electrostatic fields.

Controlled Enantioselective Orientation of Chiral Molecules with an Optical Centrifuge.

We report on the first experimental demonstration of enantioselective rotational control of chiral molecules with a laser field. In our experiments, two enantiomers of propylene oxide are brought to accelerated unidirectional rotation by means of an optical centrifuge. Using Coulomb explosion imaging, we show that the centrifuged molecules acquire preferential orientation perpendicular to the plane of rotation, and that the direction of this orientation depends on the relative handedness of the enantiomer and the rotating centrifuge field. The observed effect is in agreement with theoretical predictions and is reproduced in numerical simulations of the centrifuge excitation followed by Coulomb explosion of the centrifuged molecules. The demonstrated technique opens new avenues in optical enantioselective control of chiral molecules with a plethora of potential applications in differentiation, separation, and purification of chiral mixtures.

Coherent Spatial Control of Wave Packet Dynamics on Quantum Lattices.

Quantum lattices are pivotal in the burgeoning fields of quantum materials and information science. Novel experimental techniques allow the preparation and monitoring of wave packet dynamics on quantum lattices with high spatiotemporal resolution. We present an analytical study of wave packet diffusivity and diffusion length on tight-binding quantum lattices subject to stochastic noise. Our analysis reveals the crucial role of spatial coherence and predicts a set of novel phenomena: (1) noise can enhance the transient diffusivity and diffusion length of spatially extended initial states; (2) standing or traveling initial states, with large momentum, spread faster than a localized initial state and exhibit a noise-induced peak in the transient diffusivity; (3) the differences in the diffusivity or diffusion length of extended and localized initial states have a universal dependence on initial width. These predictions suggest the possibility of controlling the wave packet dynamics by spatial manipulations, which will have implications for materials science and quantum technologies.

Selective Orientation of Chiral Molecules by Laser Fields with Twisted Polarization.

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 (CH3CHCH2O), and ethyl oxirane (CH3CH2CHCH2O). The presented results demonstrate generality, versatility, and robustness of this optical method for manipulating molecular enantiomers in the gas phase.

All-optical field-free three-dimensional orientation of asymmetric-top molecules.

Orientation and alignment of molecules by ultrashort laser pulses is crucial for a variety of applications and has long been of interest in physics and chemistry, with the special emphasis on stereodynamics in chemical reactions and molecular orbitals imaging. As compared to the laser-induced molecular alignment, which has been extensively studied and demonstrated, achieving molecular orientation is a much more challenging task, especially in the case of asymmetric-top molecules. Here, we report the experimental demonstration of all-optical field-free three-dimensional orientation of asymmetric-top molecules by means of phase-locked cross-polarized two-color laser pulse. This approach is based on nonlinear optical mixing process caused by the off-diagonal elements of the molecular hyperpolarizability tensor. It is demonstrated on SO2 molecules and is applicable to a variety of complex nonlinear molecules.