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Journal of Physics B Atomic Molecular and Optical Physics

Laser-assisted Stark deceleration of polar diatomic molecules in the Χ 1 Σ state

Yunxia Huang, Shuwu Xu, Xiaohua Yang

Published Jun 1, 2016• 6 citations
Publisher

Abstract

Abstract The traditional Stark deceleration method is difficult to apply in chemically stable polar diatomic molecules in their ground (Χ 1 Σ) state because the Χ 1 Σ state normally experiences little Stark shift and the rovibronic ground level is mostly high-field-seeking. To solve this problem, we propose a laser-assisted Stark deceleration scheme to decelerate such molecules in the present paper. Our results show that, owing to the transverse bunching effect of the applied red-detuning laser beam, the molecules of the high-field-seeking level | J = 0, M = 0〉 in the Χ 1 Σ state can be effectively decelerated. Furthermore, the present scheme is more effective because the interaction between the molecules and the combined fields can produce the pseudo-first-order Stark effect, and thus increase the depth of the effective potential. Compared to those molecules in the low-field-seeking state | J = 1, M Ω = −1〉 in the usual electrostatic Stark deceleration, a higher molecular density and lower velocity can be achieved under an equivalent initial phase angle.

DOI
10.1088/0953-4075/49/13/135101

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Physical Review A•Feb 1, 2006•71 citations
Abstract The traditional Stark deceleration method is difficult to apply in chemically stable polar diatomic molecules in their ground (Χ 1 Σ) state because the Χ 1 Σ state normally experiences little Stark shift and the rovibronic ground level is mostly high-field-seeking. To solve this problem, we propose a laser-assisted Stark deceleration scheme to decelerate such molecules in the present paper. Our results show that, owing to the transverse bunching effect of the applied red-detuning laser beam, the molecules of the high-field-seeking level | J = 0, M = 0〉 in the Χ 1 Σ state can be effectively decelerated. Furthermore, the present scheme is more effective because the interaction between the molecules and the combined fields can produce the pseudo-first-order Stark effect, and thus increase the depth of the effective potential. Compared to those molecules in the low-field-seeking state | J = 1, M Ω = −1〉 in the usual electrostatic Stark deceleration, a higher molecular density and lower velocity can be achieved under an equivalent initial phase angle.
A near-resonant, red-detuning laser-assisted Stark deceleration scheme is proposed to slow CaF in its high-field-seeking rovibronic ground state. The assisting Gaussian laser beam can confine CaF molecules transversely owing to the optical Stark effect. Simulations suggest that the present scheme is superior to previous Stark decelerators. Under typical experimental conditions, when the assisting laser frequency is red-detuned to the molecular transition ( λ ∼606.3 nm) by 5.0 GHz and the laser power is about 5.6 W, the proposed decelerator can achieve a total number at the order of 10 4 CaF molecules with a number density at the order of 10 8 cm −3 . The equivalent temperature of the obtained cold CaF molecules is 2.3 mK. Additionally, the desired assisting laser power can be as low as about 1.2 W if keeping the red-detuning value to be 1.0 GHz, which further suggests its experimental feasibility.
Cold molecules have great scientific significance in high-resolution spectroscopy, precision measurement of physical constants, cold collision, and cold chemistry. Supersonic expansion is a conventional and versatile method to produce cold molecules with high kinetic energies. We theoretically show here that fast-moving molecules from supersonic expansion can be effectively decelerated to any desired velocity with a rotating laser beam. The orbiting focus spot of the red-detuned laser serves as a two-dimensional potential well for the molecules. We analyze the dynamics of the molecules inside the decelerating potential well and investigate the dependence of their phase acceptance by the potential well on the tilting angle of the laser beam. ND 3 molecules are used in the test of the scheme and their trajectories under the impact of the decelerating potential well are numerically simulated using the Monte Carlo method. For instance, with a laser beam of 20 kW in power focused into a pot of in waist radius, ND 3 molecules of 250 m/s can be brought to a standstill by the decelerating potential well within a time interval of about 0.73 ms. The total angle covered by the rotating laser beam is about 5.24° with the distance travelled by the potential well being about 9.13 cm. In fact, the molecules can be decelerated to any desired velocity depending on the parameters adopted. This scheme is simple in structure and easy to be realized in experiment. In addition, it is applicable to decelerating both molecules and atoms.
We demonstrate the deceleration of heavy polar molecules in low-field-seeking states by combining a cryogenic source and a traveling-wave Stark decelerator. The cryogenic source provides a high-intensity beam with low speed and temperature, and the traveling-wave decelerator provides large deceleration forces and high phase-space acceptance. We prove these techniques using YbF molecules and find the experimental data to be in excellent agreement with numerical simulations. These methods extend the scope of Stark deceleration to a very wide range of molecules.
A Stark decelerator is an effective tool for controlling motional degrees of freedom of polar molecules. Due to technical limitations, many of the current Stark decelerators focus on molecules in low-field-seeking quantum states and are built based on a fixed electrode size and spacing (type-A architecture). Here, we present an alternative method based on a different architecture, so-called type-B, with microstructured electrodes and a simpler electric field pulse timing with the prospect of producing cold, quasi-CW molecular beams. We demonstrate with simulations the feasibility of this method and show that a 2 cm decelerator consisting of 100 stages can bring molecules from 200 m/s to a near standstill in about 150 microseconds. Subsequently, the molecules can be reaccelerated to 200 m/s in a phase-stable manner. Our simulations focus on the longitudinal transmission leaving the problem of a transverse confinement for a future study. This work points to a possible way of integrating polar molecule accelerators with solid-state electronics.
The Stark deceleration of OH radicals in both low-field-seeking and high-field-seeking levels of the rovibronic $^{2}\ensuremath{\Pi}_{3∕2}$, v=0v=0v=0, J=3∕2J=3∕2J=3∕2 ground state is demonstrated using a single experimental setup. Applying alternating-gradient focusing, OH radicals in their low-field-seeking $^{2}\ensuremath{\Pi}_{3∕2}$, v=0v=0v=0, J=3∕2J=3∕2J=3∕2, fff state have been decelerated from 345to239m∕s345\phantom{\rule{0.3em}{0ex}}\text{to}\phantom{\rule{0.3em}{0ex}}239\phantom{\rule{0.3em}{0ex}}\mathrm{m}∕\mathrm{s}345to239m∕s, removing 50% of the kinetic energy using only 27 deceleration stages. The alternating-gradient decelerator allows one to independently control longitudinal and transverse manipulation of the molecules. Optimized high-voltage switching sequences for the alternating-gradient deceleration are applied, in order to adjust the dynamic focusing strength in every deceleration stage to the changing velocity over the deceleration process. In addition we have also decelerated OH radicals in their high-field-seeking $^{2}\ensuremath{\Pi}_{3∕2}$, v=0v=0v=0, J=3∕2J=3∕2J=3∕2, eee state from 355to316m∕s355\phantom{\rule{0.3em}{0ex}}\text{to}\phantom{\rule{0.3em}{0ex}}316\phantom{\rule{0.3em}{0ex}}\mathrm{m}∕\mathrm{s}355to316m∕s. For the states involved, a real crossing of hyperfine levels occurs at 640V∕cm640\phantom{\rule{0.3em}{0ex}}\mathrm{V}∕\mathrm{cm}640V∕cm, which is examined by varying a bias voltage applied to the electrodes.
The concept of phase stability in a Stark decelerator ensures that polar molecules can be accelerated, guided, or decelerated without loss; molecules within a certain position and velocity interval are kept together throughout the deceleration process. In this paper the influence of the transverse motion on phase stability in a Stark decelerator is investigated. For typical deceleration experiments---i.e., for high values of the phase angle ${\ensuremath{\phi}}_{0}$---the transverse motion considerably enhances the region in phase space for which phase stable deceleration occurs. For low values of ${\ensuremath{\phi}}_{0}$, however, the transverse motion reduces the acceptance of a Stark decelerator and unstable regions in phase space appear. These effects are quantitatively explained in terms of a coupling between the longitudinal and transverse motion. The predicted longitudinal acceptance of a Stark decelerator is verified by measurements on a beam of OH $(X\phantom{\rule{0.2em}{0ex}}^{2}\ensuremath{\Pi}_{3∕2},J=3∕2)$ radicals passing through a Stark decelerator.