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Physical Review A

Experimental and theoretical investigation of the Stark effect for manipulating cold molecules: Application to nitric oxide

Bryan J. Bichsel, Michael A. Morrison, Neil E. Shafer, E. R. I. Abraham

Published Feb 22, 2007• 16 citations

Abstract

As part of an ongoing investigation of cold-molecule collisions involving nitric oxide (NO), we here theoretically assess the first- and second-order perturbation-theory approximations to the Stark shifts; such approximations have been used almost exclusively in previous published research on NO in external electric fields. We perform this assessment by comparison to Stark shifts from the corresponding nonperturbative two-state model, considering field strengths from zero to values typical of current experimental studies of cold molecules. To facilitate the future use of this model, we give expressions for the Stark energies in a generic form that can trivially be applied to any molecules in the class under consideration. To provide insight into the validity of the two-state model, we also experimentally assess the two-state Stark shifts for NO.

DOI: 10.1103/physreva.75.023410

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As part of an ongoing investigation of cold-molecule collisions involving nitric oxide (NO), we here theoretically assess the first- and second-order perturbation-theory approximations to the Stark shifts; such approximations have been used almost exclusively in previous published research on NO in external electric fields. We perform this assessment by comparison to Stark shifts from the corresponding nonperturbative two-state model, considering field strengths from zero to values typical of current experimental studies of cold molecules. To facilitate the future use of this model, we give expressions for the Stark energies in a generic form that can trivially be applied to any molecules in the class under consideration. To provide insight into the validity of the two-state model, we also experimentally assess the two-state Stark shifts for NO.

One possible technique is the use of a modified straight Stark guide to filter the slow moving molecules from a thermal source. Here I present such a technique and the design of the necessary apparatus. Furthermore, I present experimental results for creating a molecular source of nitric oxide (NO) whose temperature is controlled. Results showing the effects of the guide on the lowest ro-vibrational states of NO and a new technique for measuring the speed distribution of a cold molecular sample are also discussed. Finally, the use of the guide to produce cold NO molecules at a temperature of 7 +/- 2 K is described.

We describe a device using the Stark effect to extract the cold fraction of nitric oxide molecules from a warmer thermal distribution. Room temperature NO is cryogenically cooled to 72-82 K and injected into a straight, hexapole guide that uses the Stark effect. By blocking line-of-sight trajectories from the input to the output, primarily the slowest molecules are guided around the obstruction and are transferred into a new chamber. We measure the temperature distribution using a field-stabilized Rydberg time-of-flight technique. A superposition of molecular Rydberg states is excited, sufficiently increasing the lifetime of the excited state for a time-of-flight measurement for cold molecular samples. We produce a continuous source of nitric oxide with temperatures ranging from 7 to 20 K in the lowest ro-vibrational state. The output temperature is controlled by the initial temperature distribution and the guide voltage.

Nitric oxide (NO) molecules in pulsed supersonic beams have been excited to long-lived Rydberg-Stark states in series converging to the lowest vibrational level in the ground electronic state of NO+ with rotational quantum numbers N+ = 2, 4, and 6. The molecules in these excited states were then guided, or decelerated and trapped in a chip-based Rydberg-Stark decelerator, and detected in situ by pulsed electric field ionization. Time constants, reflecting the decay of molecules in N+ = 2 Rydberg-Stark states, with principal quantum numbers n between 38 and 44, from the electrostatic traps were measured to be ∼300μs. Molecules in Rydberg-Stark states with N+ = 4 and 6, and the same range of values of n were too short-lived to be trapped, but their decay time constants could be determined from complementary sets of delayed pulsed electric field ionization measurements to be ∼100 and ∼25 μs, respectively.

Summary form only given. Use of the Stark shift in intense infrared laser fields to trap and align molecules has been proposed recently. For the ground state of a molecule the Stark shift in a low frequency laser field is negative. It increases in absolute value when the molecule approaches the center of the focal spot and peaks for molecular orientation parallel to the polarization of the electric field. We study the effect of Stark shift on the interaction of trapped molecules, in particular on the exchange reactions.

Nitric oxide (NO) molecules initially traveling at 795 m/s in pulsed supersonic beams have been photoexcited to long-lived hydrogenic Rydberg-Stark states, decelerated and electrostatically trapped in a cryogenically cooled, chip-based transmission-line Rydberg-Stark decelerator. The decelerated and trapped molecules were detected in situ by pulsed electric field ionization. The operation of the decelerator was validated by comparison of the experimental data with the results of numerical calculations of particle trajectories. Studies of the decay of the trapped molecules on timescales up to 1 ms provide new insights into the lifetimes of, and effects of blackbody radiation on, Rydberg states of NO.