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Register a new userObservation of persistent orientation of chiral molecules by laser field with twisted polarization
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Molecular chirality is an omnipresent phenomenon of fundamental significance in physics, chemistry and biology. For this reason, search for novel techniques for enantioselective control, detection and separation of chiral molecules is of particular importance. It has been recently predicted that laser fields with twisted polarization may induce persistent enantioselective field-free orientation of chiral molecules. Here we report the first experimental observation of this phenomenon using propylene oxide molecules ($mathrm{CH_{3}CHCH_{2}O}$, or PPO) spun by an optical centrifuge - a laser pulse, whose linear polarization undergoes an accelerated rotation around its propagation direction. We show that PPO molecules remain oriented on a time scale exceeding the duration of the centrifuge pulse by several orders of magnitude. The demonstrated long-time field-free enantioselective orientation opens new avenues for optical manipulation, discrimination, and, potentially, separation of molecular enantiomers.
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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. The underlying classical orientation mechanism common for all these fields is discussed, and its operation is demonstrated for a range of chiral molecules of various complexity: hydrogen thioperoxide (${rm HSOH}$), propylene oxide (${rm CH_{3}CHCH_{2}O}$) and ethyl oxirane (${rm CH_{3}CH_{2}CHCH_{2}O}$). The presented results demonstrate generality, versatility and robustness of this optical method for manipulating molecular enantiomers in the gas phase.
We study interaction of generic asymmetric molecules with a pair of strong time-delayed short laser pulses with crossed linear polarizations. We show that such an excitation not only provides unidirectional rotation of the most polarizable molecular axis, but also induces a directed torque along this axis, which results in the transient orientation of the molecules. The asymmetric molecules are chiral in nature and different molecular enantiomers experience the orienting action in opposite directions causing out-of-phase oscillation of their dipole moments. The resulting microwave radiation was recently suggested to be used for analysis/discrimination of chiral molecular mixtures. We reveal the mechanism behind this laser induced orientation effect, show that it is classical in nature, and envision further applications of light with skewed polarization.
We report the first experimental observation of non-adiabatic field-free orientation of a heteronuclear diatomic molecule (CO) induced by an intense two-color (800 and 400 nm) femtosecond laser field. We monitor orientation by measuring fragment ion angular distributions after Coulomb explosion with an 800 nm pulse. The orientation of the molecules is controlled by the relative phase of the two-color field. The results are compared to quantum mechanical rigid rotor calculations. The demonstrated method can be applied to study molecular frame dynamics under field-free conditions in conjunction with a variety of spectroscopy methods, such as high-harmonic generation, electron diffraction and molecular frame photoemission.
Alignment and orientation of molecules by intense, ultrashort laser fields are crucial for a variety of applications in physics and chemistry. These include control of high harmonics generation, molecular orbitals tomography, control of molecular photoionization and dissociation processes, production of molecular movies with the help of X-ray free-electron laser sources and ultrafast electron diffraction of relativistic electrons. While the dynamics of laser-induced molecular alignment has been extensively studied and demonstrated, molecular orientation is a much more challenging task, especially for asymmetric-top molecules. Here we report the first experimental demonstration of a field-free, all-optical three-dimensional orientation of asymmetric-top molecules by means of phase-locked cross-polarized two-color laser pulses. In addition to the conventional integrated orientation factor, we report the differential degree of orientation which is not amenable to optical measurements, but is readily accessible in our angle-resolved imaging technique. Our scheme applies to a wide class of asymmetric molecules and opens new ways towards controlling their orientation, eventually leading to direct imaging of structure of gas-phase molecules using advanced free electron laser beams with extremely high spatiotemporal resolution.
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.
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