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Physical Review A

Nonadiabatic molecular orientation by polarization-gated ultrashort laser pulses

Cheng Chen, Jian Wu, Heping Zeng

Published Sep 13, 2010• 17 citations
Publisher

Abstract

We show that the nonadiabatic orientation of diatomic polar molecules can be controlled by polarization-gated ultrashort laser pulses. By finely adjusting the time interval between two circularly polarized pulses of different wavelengths but the same helicity, the orientation direction of the molecules can be twirled. A cloverlike potential is created by using two circularly polarized laser pulses of different wavelengths and opposite helicity, leading to multidirectional molecular orientation along the potential wells, which can be well revealed by a high-order statistics metric of $\ensuremath{\langle}\ensuremath{\langle}\mathrm{cos}{}^{3}{\ensuremath{\theta}}_{d}\ensuremath{\rangle}\ensuremath{\rangle}$.

DOI
10.1103/physreva.82.033409

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We show that the nonadiabatic orientation of diatomic polar molecules can be controlled by polarization-gated ultrashort laser pulses. By finely adjusting the time interval between two circularly polarized pulses of different wavelengths but the same helicity, the orientation direction of the molecules can be twirled. A cloverlike potential is created by using two circularly polarized laser pulses of different wavelengths and opposite helicity, leading to multidirectional molecular orientation along the potential wells, which can be well revealed by a high-order statistics metric of \ensuremath⟨\ensuremath⟨cos3\ensuremathθd\ensuremath⟩\ensuremath⟩\ensuremath{\langle}\ensuremath{\langle}\mathrm{cos}{}^{3}{\ensuremath{\theta}}_{d}\ensuremath{\rangle}\ensuremath{\rangle}\ensuremath⟨\ensuremath⟨cos3\ensuremathθd​\ensuremath⟩\ensuremath⟩.
We present an analysis of two experimental approaches to controlling the directionality of molecular rotation with ultrashort laser pulses. The two methods are based on the molecular interaction with either a pair of pulses (a ``double-kick'' scheme) or a longer pulse sequence (a ``chiral-pulse-train'' scheme). In both cases, rotational control is achieved by varying the polarization of and the time delay between the consecutive laser pulses. Using the technique of polarization-sensitive resonance-enhanced multiphoton ionization, we show that both methods produce significant rotational directionality. We demonstrate that increasing the number of excitation pulses supplements the ability to control the sense of molecular rotation with quantum-state selectivity, i.e., predominant excitation of a single rotational state. We also demonstrate the ability of both techniques to generate counterrotation of molecular nuclear-spin isomers (here, ortho- and para-nitrogen) and molecular isotopologs (here, 14{}^{14}14N2{}_{2}2​ and 15{}^{15}15N2{}_{2}2​).
We propose a scheme to coherently control the field-free orientation of NO molecule whose rotational temperature is above 0 K. It is found that the maximum molecular orientation is affected by two factors: one is the sum of the population of M = 0 rotational states and the other is their distribution, however, their distribution plays a much more significant role in molecular orientation than the sum of their population. By adopting a series of linearly polarized pulses resonant with the rotational states, the distribution of M = 0 rotational states is well rearranged. Though the number of pulses used is small, a relatively high orientation degree can be obtained. This scheme provides a promising approach to the achievement of a good orientation effect.
We present a scheme to prepare a single rotational state with high probability from an arbitrary superposition state. The NO molecule is used as a computational example. By using a series of linearly and circularly polarized laser pulses and adjusting their parameters, a ground rotational state with probability of 99.982% can be obtained. Starting from the ground rotational state prepared, we can prepare any desired single rotational state with high probability and some rotational superposition states. On this basis, the molecular orientation with initial thermal distribution can be considerably enhanced and well controlled.
We introduce a new scheme for controlling the sense of molecular rotation. By varying the polarization and the delay between two ultrashort laser pulses, we induce unidirectional molecular rotation, thereby forcing the molecules to rotate clockwise/counterclockwise under field-free conditions. We show that unidirectionally rotating molecules are confined to the plane defined by the two polarization vectors of the pulses, which leads to a permanent anisotropy in the molecular angular distribution. The latter may be useful for controlling collisional cross-sections and optical and kinetic processes in molecular gases. We discuss the application of this control scheme to individual components within a molecular mixture in a selective manner.
Atomic and molecular free electron vortices (FEVs), characterized by their spiral-shaped momentum distribution, have recently attracted a great deal of attention due to their varied shapes and their unusual topological properties. Shortly after their theoretical prediction by the single-photon ionization (SPI) of He atoms using pairs of counterrotating circularly polarized attosecond pulses, FEVs have been demonstrated experimentally by the multiphoton ionization (MPI) of alkali atoms using single-color and bichromatic circularly polarized femtosecond pulse sequences. Recently, we reported on the analysis of the experimental results employing a numerical model based on the ab initio solution of the time-dependent Schrödinger equation (TDSE) for a two-dimensional (2D) atom interacting with a polarization-shaped ultrashort laser field. Here, we apply the 2D TDSE model to study molecular FEVs created by SPI and MPI of a diatomic molecule using polarization-tailored single-color and bichromatic femtosecond pulse sequences. We investigate the influence of the coupled electron-nuclear dynamics on the vortex formation dynamics and discuss the effect of CEP- and rotational averaging on the photoelectron momentum distribution. By analyzing how the molecular structure and dynamics is imprinted in the photoelectron spirals, we explore the potential of molecular FEVs for ultrafast spectroscopy.