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arXiv:1101.4217 · Physical Chemistry Chemical Physics

A cryogenic beam of refractory, chemically reactive molecules with expansion cooling

Nicholas R. Hutzler, Maxwell F. Parsons, Yulia V. Gurevich, Paul W. Hess, Elizabeth Petrik, Ben Spaun, Amar C. Vutha, David DeMille, Gerald Gabrielse, John M. Doyle

Published Jan 1, 2011• 78 citations
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Abstract

Cryogenically cooled buffer gas beam sources of the molecule thorium monoxide (ThO) are optimized and characterized. Both helium and neon buffer gas sources are shown to produce ThO beams with high flux, low divergence, low forward velocity, and cold internal temperature for a variety of stagnation densities and nozzle diameters. The beam operates with a buffer gas stagnation density of ∼10(15)-10(16) cm(-3) (Reynolds number ∼1-100), resulting in expansion cooling of the internal temperature of the ThO to as low as 2 K. For the neon (helium) based source, this represents cooling by a factor of about 10 (2) from the initial nozzle temperature of about 20 K (4 K). These sources deliver ∼10(11) ThO molecules in a single quantum state within a 1-3 ms long pulse at 10 Hz repetition rate. Under conditions optimized for a future precision spectroscopy application [A. C. Vutha et al., J. Phys. B: At., Mol. Opt. Phys., 2010, 43, 074007], the neon-based beam has the following characteristics: forward velocity of 170 m s(-1), internal temperature of 3.4 K, and brightness of 3 × 10(11) ground state molecules per steradian per pulse. Compared to typical supersonic sources, the relatively low stagnation density of this source and the fact that the cooling mechanism relies only on collisions with an inert buffer gas make it widely applicable to many atomic and molecular species, including those which are chemically reactive, such as ThO.

DOI
10.1039/c1cp20901a

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Bulletin of the American Physical Society•May 20, 2005•0 citations
Cryogenically cooled buffer gas beam sources of the molecule thorium monoxide (ThO) are optimized and characterized. Both helium and neon buffer gas sources are shown to produce ThO beams with high flux, low divergence, low forward velocity, and cold internal temperature for a variety of stagnation densities and nozzle diameters. The beam operates with a buffer gas stagnation density of ∼10(15)-10(16) cm(-3) (Reynolds number ∼1-100), resulting in expansion cooling of the internal temperature of the ThO to as low as 2 K. For the neon (helium) based source, this represents cooling by a factor of about 10 (2) from the initial nozzle temperature of about 20 K (4 K). These sources deliver ∼10(11) ThO molecules in a single quantum state within a 1-3 ms long pulse at 10 Hz repetition rate. Under conditions optimized for a future precision spectroscopy application [A. C. Vutha et al., J. Phys. B: At., Mol. Opt. Phys., 2010, 43, 074007], the neon-based beam has the following characteristics: forward velocity of 170 m s(-1), internal temperature of 3.4 K, and brightness of 3 × 10(11) ground state molecules per steradian per pulse. Compared to typical supersonic sources, the relatively low stagnation density of this source and the fact that the cooling mechanism relies only on collisions with an inert buffer gas make it widely applicable to many atomic and molecular species, including those which are chemically reactive, such as ThO.
Cryogenically cooled buffer gas beam sources of the molecule thorium monoxide (ThO) are optimized and characterized. Both helium and neon buffer gas sources are shown to produce ThO beams with high flux, low divergence, low forward velocity, and cold internal temperature for a variety of stagnation densities and nozzle diameters. The beam operates with a buffer gas stagnation density of \\(\\sim 10^{15}-10^{16}\\) cm\\(^{-3}\\) (Reynolds number \\(\\sim 1-100\\)), resulting in expansion cooling of the internal temperature of the ThO to as low as 2 K. For the neon (helium) based source, this represents cooling by a factor of about 10 (2) from the initial nozzle temperature of about 20 K (4 K). These sources deliver \\(\\sim 10^{11}\\) ThO molecules in a single quantum state within a 1-3 ms long pulse at 10 Hz repetition rate. Under conditions optimized for a future precision spectroscopy application [A C Vutha et al 2010 J. Phys. B: At. Mol. Opt. Phys. 43 074007], the neon-based beam has the following characteristics: forward velocity of 170 m/s, internal temperature of 3.4 K, and brightness of \\(3 \\times 10^{11}\\) ground state molecules per steradian per pulse. Compared to typical supersonic sources, the relatively low stagnation density of this source, and the fact that the cooling mechanism relies only on collisions with an inert buffer gas, make it widely applicable to many atomic and molecular species, including those which are chemically reactive, such as ThO.
We realize a continuous, intense, cold molecular and atomic beam source based on buffer-gas cooling. Hot vapor (up to 600 K) from an oven is mixed with cold (15 K) neon buffer gas, and then emitted into a high-flux beam. The novel use of cold neon as a buffer gas produces a forward velocity distribution and low-energy tail that is comparable to much colder helium-based sources. We expect this source to be trivially generalizable to a very wide range of atomic and molecular species with significant vapor pressure below 1000 K. The source has properties that make it a good starting point for laser cooling of molecules or atoms, cold collision studies, trapping, or nonlinear optics in buffer-gas-cooled atomic or molecular gases. A continuous guided beam of cold deuterated ammonia with a flux of 3×10\\(^{11}\\) ND\\(_{3}\\) molecules s\\(^{−1}\\) and a continuous free-space beam of cold potassium with a flux of 1×10\\(^{16}\\) K atoms s\\(^{−1}\\) are realized.
We realize a continuous, intense, cold molecular and atomic beam source based on buffer-gas cooling. Hot vapor (up to 600 K) from an oven is mixed with cold (15 K) neon buffer gas, and then emitted into a high-flux beam. The novel use of cold neon as a buffer gas produces a forward velocity distribution and low-energy tail that is comparable to much colder helium-based sources. We expect this source to be trivially generalizable to a very wide range of atomic and molecular species with significant vapor pressure below 1000 K. The source has properties that make it a good starting point for laser cooling of molecules or atoms, cold collision studies, trapping, or nonlinear optics in buffer-gas-cooled atomic or molecular gases. A continuous guided beam of cold deuterated ammonia with a flux of 3 × 10 11 ND 3 molecules s −1 and a continuous free-space beam of cold potassium with a flux of 1 × 10 16 K atoms s −1 are realized.
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.
We demonstrate and characterize a cryogenic buffer gas-cooled molecular beam source capable of producing bright beams of free radicals and refractory species. Details of the beam properties (brightness, forward velocity distribution, transverse velocity spread, rotational and vibrational temperatures) are measured under varying conditions for the molecular species SrF. Under typical conditions we produce a beam of brightness 1.2 × 10(11) molecules/sr/pulse in the X(2)Σ(+)(v = 0, N(rot) = 0) state, with 140(m/s) forward velocity and a rotational temperature of ≈ 1 K. This source compares favorably to other methods for producing beams of free radicals and refractory species for many types of experiments. We provide details of construction that may be helpful for others attempting to use this method.
We demonstrate and characterize a high-flux beam source for cold, slow atoms or molecules. The desired species is vaporized using laser ablation, then cooled by thermalization in a cryogenic cell of buffer gas. The beam is formed by particles exiting a hole in the buffer gas cell. We characterize the properties of the beam (flux, forward velocity, temperature) for both an atom (Na) and a molecule (PbO) under varying buffer gas density, and discuss conditions for optimizing these beam parameters. Our source compares favorably to existing techniques of beam formation, for a variety of applications.