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arXiv:2501.05613 · The Journal of Physical Chemistry Letters

Chemistry in a Cryogenic Buffer Gas Cell

Qi Sun, Jinyu Dai, Rian Koots, Benjamin C. Riley, Jesús Pérez‐Ríos, Debayan Mitra, Tanya Zelevinsky

Published Dec 26, 2025• 2 citations
arXivHTMLPDF

Abstract

Cryogenic buffer gas sources are ubiquitous for producing cold, collimated molecular beams for quantum science, chemistry, and precision measurements. The molecules are typically produced by laser ablating a metal target in the presence of a donor gas. The radical of interest emerges due to a barrier-free reaction or under thermal or optical excitation. High-barrier reactions, such as between Ca and H 2, should be precluded. We study chemical reactions between Ca and three hydrogen isotopologues (H 2, D 2, and HD) in a cryogenic cell with helium buffer gas. We observe that H 2 can serve as both a reactant and a buffer gas, outperforming D 2 and HD. We use a reaction network model to describe the chemical dynamics and find that the enhanced molecular yield can be attributed to rapid vibrational excitations of the reactant gas. Our results demonstrate a robust method for generating bright cold beams of alkaline-earth-metal hydrides for laser cooling and trapping.

DOI
10.1021/acs.jpclett.5c02840

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Cryogenic buffer gas sources are ubiquitous for producing cold, collimated molecular beams for quantum science, chemistry, and precision measurements. The molecules are typically produced by laser ablating a metal target in the presence of a donor gas. The radical of interest emerges due to a barrier-free reaction or under thermal or optical excitation. High-barrier reactions, such as between Ca and H 2, should be precluded. We study chemical reactions between Ca and three hydrogen isotopologues (H 2, D 2, and HD) in a cryogenic cell with helium buffer gas. We observe that H 2 can serve as both a reactant and a buffer gas, outperforming D 2 and HD. We use a reaction network model to describe the chemical dynamics and find that the enhanced molecular yield can be attributed to rapid vibrational excitations of the reactant gas. Our results demonstrate a robust method for generating bright cold beams of alkaline-earth-metal hydrides for laser cooling and trapping.
Cryogenic buffer gas beams are central to many cold molecule experiments. Here, we use absorption and fluorescence spectroscopy to directly compare molecular beams of AlF, CaF, MgF and YbF molecules, produced by chemical reaction of laser ablated atoms with fluorine rich reagents. The beam brightness for AlF is measured as 2×1012 molecules per steradian per pulse in a single rotational state, comparable to an Al atomic beam produced in the same setup. The CaF, MgF and YbF beams show an order of magnitude lower brightness than AlF and far below the brightness of Ca and Yb beams. The addition of either NF3 or SF6 to the cell extinguishes the Al atomic beam, but has a minimal effect on the Ca and Yb beams. NF3 reacts more efficiently than SF6, as a significantly lower flow rate is required to maximise the molecule production, which is particularly beneficial for long-term stability of the AlF beam. We use NO as a proxy for the reactant gas as it can be optically detected. We demonstrate that a cold, rotationally pure NO beam can be generated by laser desorption, thereby gaining insight into the dynamics of the reactant gas inside the buffer gas cell.
We demonstrate a cryogenic buffer gas-cooled molecular beam source capable of producing bright, continuous beams of cold and slow free radicals via laser ablation over durations of up to 60 seconds. The source design uses a closed liquid helium reservoir as a large thermal mass to minimize heating and ensure reproducible beam properties during operation. Under typical conditions, the source produces beams of our test species SrF, containing $5\ifmmode\times\else\texttimes\fi{}{10}^{12}$ molecules per steradian per second in the $X{\phantom{\rule{0.16em}{0ex}}}^{2}\mathrm{\ensuremath{\Sigma}}(v=0,N=1)$ state with a rotational temperature of 1.0(2) K and a forward velocity of 140m/s140\phantom{\rule{0.28em}{0ex}}\mathrm{m}/\mathrm{s}140m/s. The beam properties are robust and unchanged for multiple cell exit geometries, but depend critically on the helium buffer gas flow rate, which must be $\ensuremath{\ge}10$ standard cubic centimeters per minute to produce bright, continuous beams of molecules for an ablation repetition rate of 55 Hz.
Abstract We use narrow-band laser excitation of Yb atoms to substantially enhance the brightness of a cold beam of YbOH, a polyatomic molecule with high sensitivity to physics beyond the standard model (BSM). By exciting atomic Yb to the metastable 3P1 state in a cryogenic environment, we significantly increase the chemical reaction cross-section for collisions of Yb with reactants. We characterize the dependence of the enhancement on the properties of the laser light, and study the final state distribution of the YbOH products. The resulting bright, cold YbOH beam can be used to increase the statistical sensitivity in searches for new physics utilizing YbOH, such as electron electric dipole moment and nuclear magnetic quadrupole moment experiments. We also perform new quantum chemical calculations that confirm the enhanced reactivity observed in our experiment and compare reaction pathways of Yb(3P) with the reactants H2O and H2O2. More generally, our work presents a broad approach for improving experiments that use cryogenic molecular beams for laser cooling and precision measurement searches of BSM physics.
In this paper we report on the production and characterization of a cold beam of BaOH molecules using a cryogenic buffer-gas beam source. BaOH is a highly suitable molecule for studies of the violation of fundamental symmetries, such as the search for the electron's electric dipole moment. BaOH molecules are synthesised inside the cold source through laser ablation of a barium metal target while water vapor is seeded into the neon buffer gas. The BaOH flux is significantly enhanced ($\sim$11 times) when laser-exciting the barium atoms inside the buffer-gas cell on the 1S0−3P1^1\mathrm S_0 - ^3\mathrm P_11S0​−3P1​ transition. A similar enhancement has been reported for other alkaline-earth(-like) monohydroxides. For typical source conditions, the molecular beam has an average velocity of ≈180\approx180≈180 m/s and an intensity of ∼109\sim 10^{9}∼109 molecules s−1^{-1}−1 in N=1N=1N=1, which is comparable to that of cryogenic BaF beams.
Abstract In this paper we report on the production and characterization of a cold beam of BaOH molecules using a cryogenic buffer-gas beam source. BaOH is a highly suitable molecule for studies of the violation of fundamental symmetries, such as the search for the electron’s electric dipole moment. BaOH molecules are synthesized inside the cold source through laser ablation of a barium metal target while water vapor is seeded into the neon buffer gas. The BaOH flux is significantly enhanced (∼11 times) when laser-exciting the barium atoms inside the buffer-gas cell on the 1 S 0 – 3 P 1 transition. A similar enhancement has been reported for other alkaline-earth(-like) monohydroxides. For typical source conditions, the molecular beam has an average velocity of ≈ 180 m s −1 and an intensity of ∼ 10 9 molecules s −1 in N = 1, which is comparable to that of cryogenic BaF beams.
We study the properties of a cryogenic buffer gas source that uses a low-temperature two-stage buffer gas cell to produce very slow beams of ytterbium monofluoride molecules. The molecules are produced by laser ablation inside the cell and extracted into a beam by a flow of cold helium. We measure the flux and velocity distribution of the beam as a function of ablation energy, helium flow rate, cell temperature, and the size of the gap between the first and second stages of the cell. We also compare the velocity distributions from one-stage and two-stage cells. The one-stage cell emits a beam with a speed of about 82 m s − 1 and a translational temperature of 0.63 K. The slowest beams are obtained using the two-stage cell at the lowest achievable cell temperature of 1.8 K. This beam has a peak velocity of 56 m s − 1 and a flux of 9 × 10 9 ground-state molecules per steradian per pulse, with a substantial fraction at speeds below 40 m s − 1 . These slow molecules can be decelerated further by radiation pressure slowing and then captured in a magneto-optical trap. Published by the American Physical Society 2024