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Physical Review Letters

Rotational-State-Dependent Dispersion of Molecules by Pulsed Optical Standing Waves

Xing Nan Sun, Lee Yeong Kim, Bum Suk Zhao, Doo Soo Chung

Published Nov 24, 2015• 6 citations
Publisher

Abstract

We report on the rotational-state-dependent, transverse acceleration of CS_{2} molecules affected by pulsed optical standing waves. The steep gradient of the standing wave potential imparts far stronger dipole forces on the molecules than propagating pulses do. Moreover, large changes in the transverse velocities (i.e., up to 80 m/s) obtained with the standing waves are well reproduced in numerical simulations using the effective polarizability that depends on the molecular rotational states. Our analysis based on the rotational-state-dependent effective polarizability can therefore serve as a basis for developing a new technique of state selection for both polar and nonpolar molecules.

DOI
10.1103/physrevlett.115.223001

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We report on the rotational-state-dependent, transverse acceleration of CS_{2} molecules affected by pulsed optical standing waves. The steep gradient of the standing wave potential imparts far stronger dipole forces on the molecules than propagating pulses do. Moreover, large changes in the transverse velocities (i.e., up to 80 m/s) obtained with the standing waves are well reproduced in numerical simulations using the effective polarizability that depends on the molecular rotational states. Our analysis based on the rotational-state-dependent effective polarizability can therefore serve as a basis for developing a new technique of state selection for both polar and nonpolar molecules.
molecules in their lowest few rotational states are adiabatically aligned and transversely accelerated by a nonresonant optical standing wave. The width of the measured transverse velocity distribution increases to 160 m/s with the field intensity, while its central peak position moves from 10 to -10 m/s. These changes are well reproduced by numerical simulations based on the rotational state-dependent alignment but cannot be modeled when ignoring these effects. Moreover, the molecular scattering by an off-resonant optical field amounts to manipulating the translational motion of molecules in a rotational state-specific way. Conversely, our results demonstrate that scattering from a nonresonant optical standing wave is a viable method for rotational state selection of nonpolar molecules.
The properties of molecule-optical elements such as lenses or prisms based on the interaction of molecules with optical fields depend in a crucial way on the molecular quantum state and its alignment created by the optical field. Herein, we consider the effects of state-dependent alignment in estimating the optical dipole force acting on the molecules and, to this end, introduce an effective polarizability which takes proper account of molecular alignment and is directly related to the alignment-dependent optical dipole force. We illustrate the significance of including molecular alignment in the optical dipole force by a trajectory study that compares previously used approximations with the present approach. The trajectory simulations were carried out for an ensemble of linear molecules subject to either propagating or standing-wave optical fields for a range of temperatures and laser intensities. The results demonstrate that the alignment-dependent effective polarizability can serve to provide correct estimates of the optical dipole force, on which a state-selection method applicable to nonpolar molecules could be based. We note that an analogous analysis of the forces acting on polar molecules subject to an inhomogeneous static electric field reveals a similarly strong dependence on molecular orientation.
Abstract The optical dipole force acting on molecules is enhanced by decreasing the rotational temperature of the molecule and aligning the molecular axis with a linearly polarized nonresonant laser beam. The rotational temperature is decreased by increasing the source pressure from 2 to 81 bar. By using the effective polarizability directly pertaining to the optical dipole force, the force and the resulting change in the velocity of the molecules can be evaluated. Theoretical calculations are compared with measurements based on velocity map imaging techniques. If the rotational temperature is reduced from 295 to 1 K, the maximum alignment is increased from <cos2θ>=0.33 to 0.92, and the average optical force is enhanced by 74 %.
The absolute laser phase dependence of the time-dependent populations of the molecular states, including the steady-state (long time) populations of the states, associated with the interaction of a molecule with a pulsed laser is investigated using illustrative two-level examples. One-photon transitions, including the effects of permanent dipoles, are discussed as a function of the pulse duration, intensity, and (absolute) laser phase, for selected laser frequencies. The effects of laser phase can be large, depending on the values of the pulse duration for a given frequency and intensity. The effects of permanent dipoles, relative to no permanent dipoles, are significant for large laser field strengths ε0. When the laser-molecule coupling parameter b=μ12ε0/E21⩾0.2, where μ12 and E21 are the transition dipole and energy difference between the ground and excited states, respectively, the dynamics of the pulse-molecule interaction are (strongly) phase dependent, independent of pulse duration, whereas the corresponding steady-state populations of the molecular states may or may not be phase-dependent depending on the pulse duration. Analytical rotating wave approximations for pulsed laser-molecule interactions are useful for interpreting the dynamics and the steady-state results as a function of field strength and pulse duration, including the effects of permanent dipole moments. The results reported in this paper are based on molecular parameters associated with an S0→S1 electronic transition in a dipolar molecule. However, they are presented in reduced form and therefore can be scaled to other regions of the electromagnetic spectrum. Short, intense pulses at or beyond the limits of current laser technology will often be required for the types of absolute laser phase effects of this paper to be appreciable for electronic excitations. The discussion, in the UV-VIS, also suffers from the use of a two-level model and from the requirement of field intensities that can be beyond the Keldysh limit. For other spectral regions, these absolute laser phase effects will be much more readily applicable.
Summary form only given. Acceleration of molecules within a time varying electric field produced by an optical traveling wave has been proposed as a means to accelerate neutral particles to high velocity. This technique is attractive because extremely large Stark forces can be produced by the high electric field gradients that can be created within an optical traveling wave. The electrodeless electric field gradient produced by focused laser beams can be orders of magnitude greater than electrostatic gradients, allowing acceleration of polar as well as polarizable molecules and atoms. This concept has already been used to accelerate ultracold atoms in a very weak optical periodic potentials, or lattices, and acceleration up to the velocities in the m/s velocity was observed. We report on the study of acceleration of polarizable particles to velocities in excess of 10 km/s range in an accelerated optical lattice, using high intensity pulsed fields.
We measure the role of field-induced alignment on the dipole force for molecules using a single focused nonresonant laser beam. We show that through the alignment process we can modify the effective polarizability by field polarization and thus control the center-of-mass motion of the molecule. We observe a maximum change of 2020%20 in the dipole force on CS2{}_{2}2​ molecules when changing from linearly to circularly polarized light. Additionally, the effect of the dipole force on different vibrational states is also studied.