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Journal of Physics B Atomic Molecular and Optical Physics

Barrier-discharge source of cold hydrogen atoms in supersonic beams: Stark effect in the 1s–2s transition

Simon Scheidegger, David Schlander, Josef A. Agner, Hansjürg Schmutz, Paul Jansen, Frédéric Merkt

Published Jun 2, 2022• 6 citations
Publisher

Abstract

Abstract An intense source of cold hydrogen atoms in a supersonic beam is presented. H and D atoms are produced from pure samples of H2 and D2 using a barrier discharge near the orifice of a cryogenic pulsed valve. The atoms are entrained in the supersonic expansion of the precursor molecules and cool down to translational temperatures as low as ∼ 15 mK. The H-atom density at a distance of 1.2 m from the valve orifice is estimated to be around 108 cm−3. The mean velocity of the supersonic beam containing the H (D) atoms can be adjusted between 2600 and 1200 m s−1 (between 1850 and 820 m s−1). The barrier discharge also produces H n + and D n + ions with n ranging from 2 to 8, which can be deflected off the beam by electric fields. The use of this H-atom source in spectroscopic measurements is demonstrated by an investigation of the Stark effect in the 1s–2s two-photon transition of H and D. A near-Fourier-transform-limited pulsed laser generating pulses of UV radiation of adjustable pulse length between 10 and 200 ns near 243 nm is used to record spectra with full resolution of the hyperfine structure in the s states, providing a textbook example of the Stark effect in the simplest set of near-degenerate states of one-electron atoms.

DOI
10.1088/1361-6455/ac7598

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arXiv:physics/0612163•The Journal of Chemical Physics•Mar 28, 2007•18 citations
Abstract An intense source of cold hydrogen atoms in a supersonic beam is presented. H and D atoms are produced from pure samples of H2 and D2 using a barrier discharge near the orifice of a cryogenic pulsed valve. The atoms are entrained in the supersonic expansion of the precursor molecules and cool down to translational temperatures as low as ∼ 15 mK. The H-atom density at a distance of 1.2 m from the valve orifice is estimated to be around 108 cm−3. The mean velocity of the supersonic beam containing the H (D) atoms can be adjusted between 2600 and 1200 m s−1 (between 1850 and 820 m s−1). The barrier discharge also produces H n + and D n + ions with n ranging from 2 to 8, which can be deflected off the beam by electric fields. The use of this H-atom source in spectroscopic measurements is demonstrated by an investigation of the Stark effect in the 1s–2s two-photon transition of H and D. A near-Fourier-transform-limited pulsed laser generating pulses of UV radiation of adjustable pulse length between 10 and 200 ns near 243 nm is used to record spectra with full resolution of the hyperfine structure in the s states, providing a textbook example of the Stark effect in the simplest set of near-degenerate states of one-electron atoms.
Second harmonic generation (SHG) in free atoms is one of the unsolved problems in nonlinear optics. The most probable mechanism is due to Stark mixing between nearby excited states through an electric field caused by charge separation through the process of three-photon ionization. To test the mechanism, atomic hydrogen appears to be the best candidate because of its well-known electronic structure and large dipole moments of its excited states. In this work we report on the observation of SHG in atomic hydrogen in the Lyman-α region. Pulsed dye laser radiation was doubled and tuned to 243 nm for excitation of the 2s ← 1s transition at 121.6 nm by a two-photon resonance process. A cw atomic beam was used with hydrogen atoms generated in a dc discharge of H2 gas. The laser beam was focused ~1 mm below the nozzle where the hydrogen atom density was estimated to be 1013 cm−3. The second harmonic radiation was strongly enhanced by adding an external dc field of up to 10 kV/cm. Stark splitting was clearly observed at higher fields.
This dissertation describes a general approach of generating a high flux of cold atoms that can be confined in a magneto-optical trap. As an alternative to the state-of-the-art laser cooling method, this approach widens our ability to cool and control atoms without relying on a specific atomic transition and availability of laser. In this dissertation I will discuss the design, construction of the experiment and characterization of a pulsed cold atom source in detail. This work is based on a new paradigm: entrainment of atoms in the carrier gas of a supersonic beam, followed by the magnetic deceleration and trapping. Our methodology is based on the supersonic beam created by the expansion of a dense carrier gas from a pulsed release of gas through a small aperture. Cold noble gas emerging from this pulsed high pressure supersonic nozzle acts as a carrier, into which atoms of interest are then entrained. In our studies with the lithium atoms, up to 10¹¹ atoms per pulse could be entrained into a supersonic beam of helium at a translation temperature of below 100 mK. The supersonic valve is typically operated at a rate of below 1 Hz in the experiment. A much larger flux can be achieved at a higher repetition rate. These atoms are moving at a speed of 500 ms⁻¹ and need to be decelerated almost to a complete stop, in order to be trapped and cooled to quantum degeneracy. A 2.5-meter long moving-trap magnetic decelerator with 480 coil pairs was built and characterized. Atoms moving at a speed around 500 ms⁻¹ were trapped and decelerated to various final velocities ranging from 400 ms⁻¹ to 50 ms⁻¹, at a resulting temperature of 30 mK and a flux of 10⁸ ~ 10⁹ atoms per pulse. This whole process takes place within only 10 ms, at a repetition rate of 100 Hz 10¹⁰ ~ 10¹¹ atoms can be delivered per second. This approach is very general compared to the laser cooling, since most atoms in the periodic table have a magnetic moment in their ground state or can be optically pumped to a long-lived para-magnetic metastable state. In this dissertation, I show the working principle of each component of our experiment and characterize the atom beam at multiple stages. I describe in detail the construction and optimization of our magnetic decelerator, and demonstrate the control and monitoring system with the experiment results. Also implemented in this work is a flexible laser system that is composed of a reference diode laser and two tapered amplifiers to control and probe the internal states of atoms, as well as provide the trapping force. I also explore the optical molasses and chirped cooling techniques which help load the atoms into a magneto-optical trap. The successful demonstration of this method of creating a cold atom source leads us to believe that the magnetically decelerated supersonic atoms will play an important role in the area of cold atom physics
The authors report the observation of the 1S-2S two-photon transition in atomic hydrogen in an atomic beam, excited by light from a narrow-band continuous-wave laser. The excitation takes place in a collision-free environment and detection of the resonance is carried out by Stark-quenching the metastable atoms some distance from the interaction region. This approach removes the limitations of cell excitation employed in previous experiments with continuous-wave lasers, and should allow the full precision of modern tunable laser techniques to be applied to the 1S-2S transition. It also gives a new method for producing a collimated beam of metastable atoms which has particular applications to a variety of future experiments with cold hydrogen.
Atomic hydrogen has been loaded into a 1-K deep magnetic trap through the use of a dilution refrigerator. Evaporative cooling has been used to cool the trapped hydrogen into the submillikelvin temperature regime. These techniques have produced a sample with density of 8 × 1013 cm-3 at a temperature of 100 μK. At this density a transition to a Bose-Einstein condensate is predicted to occur at a temperature of 30 μK. These results have been obtained with a magnetic trap that has been constructed to accommodate upcoming experiments based on laser spectroscopy of the 1S-2S two photon transition in the trapped hydrogen. A frequency doubled narrow linewidth cw dye laser system has been constructed to excite the 1S-2S transition. The excitation will be detected by the observation of electric field-induced Lyman-alpha fluorescence. The optical detection system should yield improved sample density and temperature diagnostic capabilities that will facilitate a closer approach to the quantum degenerate regime. Additionally the cold, confined hydrogen gas offers the possibility of improving the level of resolution of Doppler-free hydrogen 1S-2S laser spectroscopy by several orders of magnitude.
A pinhole discharge unit as well as a dielectric barrier discharge (DBD) head were developed for the Nijmegen pulsed valve (NPV) and the molecular beam properties accessible from each source were characterised and compared. The discharge conditions were optimised for maximum hydroxyl radical density. It was found that the DBD source yields colder OH radicals, whereas the pinhole discharge source provides a threefold larger radical density compared to the DBD discharge head. \n \nTranslationally cold packages of hydroxyl radicals (Ttrans > 1mK) were produced by means of Stark deceleration and a 124-stage Stark decelerator was set up in the laboratory. The decelerator was conditioned, characterised and optimised for operation at low final velocities (v < 40 m/s). The performance of the decelerator was assessed by determining the density of OH radicals available after the deceleration process. \n \nIn a final step, a translationally cold OH package was loaded into a cryogenic magnetic trap. The trap design, the coupling of the magnetic trap to the Stark decelerator and the loading efficiency were numerically optimised employing a direct search algorithm on Monte-Carlo trajectory simulations. The cryogenic environment efficiently prevents black-body radiation from pumping OH radicals out of trappable states and the background pressure improved significantly. Under cryogenic conditions the 1/e trap lifetime improved by a factor of 30 compared to room temperature. The magnetic trap forms part of a hybrid trapping scheme for neutral molecules and ionic species. This novel type of trap represents a versatile environment for investigating ion-neutral molecule reactions in the cold regime, while offering full control over the contributing quantum states.
We have developed a source of cold LiH molecules for Stark deceleration and trapping experiments. Lithium metal is ablated from a solid target into a supersonically expanding carrier gas. The translational, rotational, and vibrational temperatures are 0.9+/-0.1, 5.9+/-0.5, and 468+/-17 K, respectively. Although they have not reached thermal equilibrium with the carrier gas, we estimate that 90% of the LiH molecules are in the ground state, X (1)Sigma(+)(v=0,J=0). With a single 7 ns ablation pulse, the number of molecules in the ground state is 4.5+/-1.8 x 10(7) molecules/sr. A second, delayed, ablation pulse produces another LiH beam in a different part of the same gas pulse, thereby almost doubling the signal. A long pulse, lasting 150 micros, can make the beam up to 15 times more intense.