Beams of atoms and molecules are stalwart tools for spectroscopy and studies of collisional processes. The supersonic expansion technique can create cold beams of many species of atoms and molecules. However, the resulting beam is typically moving at a speed of 300-600 m/s in the lab frame, and for a large class of species has insufficient flux (i.e. brightness) for important applications. In contrast, buffer gas beams can be a superior method in many cases, producing cold and relatively slow molecules in the lab frame with high brightness and great versatility. There are basic differences between supersonic and buffer gas cooled beams regarding particular technological advantages and constraints. At present, it is clear that not all of the possible variations on the buffer gas method have been studied. In this review, we will present a survey of the current state of the art in buffer gas beams, and explore some of the possible future directions that these new methods might take.
Experiments with cold molecules usually begin with a molecular source. We describe the construction and characteristics of a cryogenic buffer gas source of CaF molecules. The source emits pulses with a typical duration of 240 $μ$s, a mean speed of about 150 m/s, and a flux of $5\times 10^{10}$ molecules per steradian per pulse in a single rotational state.
We realize a continuous guided beam of cold deuterated ammonia with a flux of 3e11 ND3 molecules/s and a continuous free-space beam of cold potassium with a flux of 1e16 K atoms/s. A novel feature of the buffer gas source used to produce these beams is cold neon, which, due to intermediate Knudsen number beam dynamics, produces a forward velocity 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. This source has properti…
We produce cold and dense clouds of atomic ions (Ca$^+$, Dy$^+$) by laser ablation of metal targets and cryogenic buffer gas cooling of the resulting plasma. We measure the temperature and density of the ion clouds using laser absorption spectroscopy. We find that large ion densities can be obtained at temperatures as low as 6 K. Our method opens up new ways to study cold neutral plasmas, and to perform survey spectroscopy of ions that cannot be laser-cooled easily.
Cryogenic buffer-gas beams are a promising method for producing bright sources of cold molecular radicals for cold collision and chemical reaction experiments. In order to use these beams in studies of reactions with controlled collision energies, or in trapping experiments, one needs a method of controlling the forward velocity of the beam. A Stark decelerator can be an effective tool for controlling the mean speed of molecules produced by supersonic jets, but efficient deceleration of buffer-gas beams presents new challenges due to longer pulse lengths. Traveling-wave decelerators are unique…
We reported a detailed experimental study of the cold collision of Barium monofluoride (BaF) with buffer gas and the high-resolution spectroscopy relevant with direct laser cooling. BaF molecules are efficiently produced with laser ablation and buffer-gas cooled in a cryogenic apparatus. The laser cooling relevant transition $|X^2Σ, v=0, N=1\rangle$ to $|A^2Π, v'=0, J'=1/2\rangle$ is identified. The collision cross section with buffer gas is measured to be $1.4(7)\times10^{-14} cm^{-2}$, which is very suitable for buffer gas cooling. Both rotational and vibrational temperatures are effectively…
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 applicatio…
A novel two-stage helium buffer gas cooled beam source is introduced. The properties of the molecular beams produced from this source are investigated theoretically using the CaF as a test molecule. The gas-phase molecules are first produced inside a 3~K helium buffer gas cell by laser ablation and subsequently cooled down to 3~K by collisions with buffer gas atoms. The precooled molecules are then extracted into the 0.5~K helium buffer gas cell where they are cooled further down to 0.5~K by collisions with cold helium atoms. Finally, the cold molecules are extracted out into the high vacuum t…
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 $2\times 10^{12}$ 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. Th…
Cooling molecules in the gas phase is important for precision spectroscopy, cold molecule physics, and physical chemistry. Measurements of conformational relaxation cross sections shed important light on potential energy surfaces and energy flow within a molecule. However, gas-phase conformational cooling has not been previously observed directly. In this work, we directly observe conformational dynamics of 1,2-propanediol in cold (6K) collisions with atomic helium using microwave spectroscopy and buffer-gas cooling. Precise knowledge and control of the collisional environment in the buffer-ga…
The cryogenic buffer gas beam (CBGB) is an important tool in the study of cold and ultracold molecules. While there are known techniques to enhance desired beam properties, such as high flux, low velocity, or reduced divergence, they have generally not undergone detailed numerical optimization. Numerical simulation of buffer gas beams is challenging, as the relevant dynamics occur in regions where the density varies by orders of magnitude, rendering standard numerical methods unreliable or intractable. Here, we present a hybrid approach to simulating CBGBs that combines gas dynamics methods wi…
We demonstrate an intense, continuous cold atom beam generated via post nozzle seeding of a supersonic helium jet with $^7$Li atoms. The nozzle is cooled to about 4.4 K to reduce the forward velocity of the atoms. The atomic beam is brought to a focus 175 cm from the nozzle by a 10 cm bore diameter magnetic hexapole lens. Absorption and fluorescence imaging of the focus show a flux of $2.3(4) \times 10^{12}$ atoms/s, brightness of $4.1(7)\times 10^{19}$ $\textrm{m}^{-2}\textrm{s}^{-1}\textrm{sr}^{-1}$, forward velocity of 211(2) m/s, and longitudinal temperature of 7(3) mK. Results agree with …
We produce YbF molecules with a density of 10^18 m^-3 using laser ablation inside a cryogenically-cooled cell filled with a helium buffer gas. Using absorption imaging and absorption spectroscopy we study the formation, diffusion, thermalization and optical pumping of the molecules. The absorption images show an initial rapid expansion of molecules away from the ablation target followed by a much slower diffusion to the cell walls. We study how the time constant for diffusion depends on the helium density and temperature, and obtain values for the YbF-He diffusion cross-section at two differen…
We present a generalization of the diagrammatic pump-probe approach to coherent backscattering (CBS) of intense laser light for atoms with degenerate energy levels. We employ this approach for a characterization of the double scattering signal from optically pumped atoms with the transition $J_g\rightarrow J_e=J_g+1$ in the helicity preserving polarization channel. We show that, in the saturation regime, the internal degeneracy becomes manifest for atoms with $J_g\geq 1$, leading to a faster decrease of the CBS enhancement factor with increasing saturation parameter than in the non-degenerate …
We present a 2D-MOT setup for the production of a continuous collimated beam of cold 87-Rb atoms out of a vapor cell. The underlying physics is purely two-dimensional cooling and trapping, which allows for a high flux of up to 6*10^(10) atoms/s and a small divergence of the resulting beam. We analyze the velocity distribution of the 2D-MOT. The longitudinal velocity distribution of the atomic beam shows a broad feature(FWHM=75m/s), centered around 50m/s. The dependence of the flux on laser intensity, geometry of the trapping volume and on pressure in the vapor cell was investigated in detail. …
Cryogenic buffer gas beams are important sources of cold molecules. In this work we explore the use of a converging-diverging nozzle with a buffer-gas beam. We find that, under appropriate circumstances, the use of a nozzle can produce a beam with improved collimation, lower transverse temperatures, and higher fluxes per solid angle.
We report our studies on an intense source of cold cesium atoms based on a two-dimensional magneto-optical trap with independent axial cooling and pushing. The new-designed source, proposed as 2D-HP MOT, uses hollow laser beams for axial cooling and a thin pushing laser beam for cold atomic beam extraction. Regulated independently by the pushing beam, the atomic flux can be substantially optimized. The atomic flux maximum obtained in the 2D-HP MOT is $4.02\times 10^{10}$ atoms/s, increased by 60 percent compared to the traditional 2D$^+$ MOT in our experiment. Moreover, with the pushing power …
We use narrow-band laser excitation of Yb 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 $^3$P$_1$ 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 statistic…
Using frequency-chirped radiation pressure slowing, we precisely control the velocity of a pulsed CaF molecular beam down to a few m/s, compressing its velocity spread by a factor of 10 while retaining high intensity: at a velocity of 15~m/s the flux, measured 1.3~m from the source, is 7$\times$10$^{5}$ molecules per cm$^{2}$ per shot in a single rovibrational state. The beam is suitable for loading a magneto-optical trap or, when combined with transverse laser cooling, improving the precision of spectroscopic measurements that test fundamental physics. We compare the frequency-chirped slowing…
We have used laser ablation and helium buffer-gas cooling to produce the titanium-helium van der Waals molecule at cryogenic temperatures. The molecules were detected through laser-induced fluorescence spectroscopy. Ground-state Ti-He binding energies were determined for the ground and first rotationally excited states from studying equilibrium thermodynamic properties, and found to agree well with theoretical calculations based on newly calculated ab initio Ti-He interaction potentials, opening up novel possibilities for studying the formation, dynamics, and non-universal chemistry of van der…
We employ laser cooling to intensify and cool an atomic beam of metastable Ne(3s) atoms. Using several collimators, a slower and a compressor we achieve a ^{20}Ne^* flux of 6 10^{10} atoms/s in an 0.7 mm diameter beam traveling at 100 m/s, and having longitudinal and transverse temperatures of 25mK and 300microK, respectively. This constitutes the highest flux in a concentrated beam achieved to date with metastable rare gas atoms. We characterize the action of the various cooling stages in terms of their influence on the flux, diameter and divergence of the atomic beam. The brightness and bril…
We demonstrate buffer-gas cooling, high-resolution spectroscopy and cycling fluorescence of cold barium monofluoride (BaF) molecules. Our source produces an intense and internally cold molecular beam containing the different BaF isotopologues with a mean forward velocity of 190 m/s. For a well-collimated beam of 138BaF we observe a flux of more than 1e10 molecules/sr/pulse in the X2Sigma, N=1 state in our downstream detection region. Studying the absorption line strength of the intermediate A'Delta state we infer a lifetime of 790+\-346 ns, significantly longer than previously estimated. Final…
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 $5\times10^{12}~$molecules per steradian per second in the $X^{2}Σ(v=0, N=1)$ state with a rotational temperature of $1.0(2)~$K and a forward velocity of $…
Kinetic modeling of molecular beam formation in a cryogenic buffer-gas cell
Vienna Center for Quantum Science and Technology, Atominstitut, TU Wien（维也纳量子科学与技术中心，原子研究所，维也纳工业大学）；LSS, Faculty of Engineering, Friedrich-Alexander-Universität Erlangen-Nürnberg（埃尔朗根-纽伦堡大学工程学院）；Institute of Space Systems, University of Stuttgart（斯图加特大学空间系统研究所）
We present a brief review of our progress towards measuring parity violation in heavy-metal chiral complexes using mid-infrared Ramsey interferometry. We discuss our progress addressing the main challenges, including the development of buffer-gas sources of slow, cold polyatomic molecules, and the frequency-stabilisation of quantum cascade lasers calibrated using primary frequency standards. We report investigations on achiral test species of which promising chiral derivatives have been synthesized.
We show that a large class of helium-containing cold polar molecules form readily in a cryogenic buffer gas, achieving densities as high as 10^12 cm^-3. We explore the spin relaxation of these molecules in buffer gas loaded magnetic traps, and identify a loss mechanism based on Landau-Zener transitions arising from the anisotropic hyperfine interaction. Our results show that the recently observed strong T^6 thermal dependence of spin change in buffer gas trapped silver (Ag) is accounted for by the formation and spin change of AgHe, thus providing evidence for molecular formation in a buffer ga…
We demonstrate Doppler-free saturated absorption spectroscopy of cold molecular radicals formed by laser ablation inside a cryogenic buffer gas cell. By lowering the temperature, congested regions of the spectrum can be simplified, and by using different temperatures for different regions of the spectrum a wide range of rotational states can be studied optimally. We use the technique to study the optical spectrum of YbF radicals with a resolution of 30 MHz, measuring the magnetic hyperfine parameters of the electronic ground state. The method is suitable for high resolution spectroscopy of a g…
We report on calculations of the elastic cross section and thermalization rate for collision between two maximally spin-polarized chromium atoms in the cold and ultracold regimes, relevant to buffer-gas and magneto-optical cooling of chromium atoms. We calculate ab initio potential energy curves for Cr2 and the van der Waals coefficient C6, and construct interaction potentials between two colliding Cr atoms. We explore the effect of shape resonances on elastic cross section, and find that they dramatically affect the thermalization rate. Our calculated value for the s-wave scattering length is…
We ask and answer a basic question about the length scales involved in quantum decoherence: how far apart in space do two parts of a quantum system have to be, before a common quantum environment decoheres them as if they were entirely separate? We frame this question specifically in a cold atom context. How far apart do two populations of bosons have to be, before an environment of thermal atoms of a different species (`buffer gas') responds to their two particle numbers separately? An initial guess for this length scale is the thermal coherence length of the buffer gas; we show that a standa…
Multipole radiofrequency ion traps are a highly versatile tool to study molecular ions and their interactions in a well-controllable environment. In particular the cryogenic 22-pole ion trap configuration is used to study ion-molecule reactions and complex molecular spectroscopy at temperatures between few Kelvin and room temperatures. This article presents a tutorial on radiofrequency ion trapping in multipole electrode configurations. Stable trapping conditions and buffer gas cooling, as well as important heating mechanisms, are discussed. In addition, selected experimental studies on cation…
Design and Performance of a Heated Gas Injector for Producing Cold Molecular Beams
Harvard/MIT Center for Ultracold Atoms（哈佛/麻省理工超冷原子中心）；Department of Physics, Harvard University（哈佛大学物理系）；Division of Engineering Science, University of Toronto（多伦多大学工程科学部）；Department of Physics, Massachusetts Institute of Technology（麻省理工学院物理系）
We discuss the possibility of non-exponential tunneling ionization of atoms irradiated by intense laser field. This effect can occur at times, which are greater than the lifetime of a system under consideration. The mechanism for non-exponential depletion of an initial quasi-stationary state is the cutting of the energy spectrum of final continuous states at long times. We first consider the known examples of cold emission of electrons from metal, tunneling alpha-decay of atomic nuclei, spontaneous decay in two-level systems and the single-photon atomic ionization by a weak electromagnetic fie…
Intense beams of cold and slow molecules are produced by supersonic expansion out of a rapidly rotating nozzle, as first demonstrated by Gupta and Herschbach. An improved setup is presented that allows to accelerate or decelerate cold atomic and molecular beams by up to 500 m/s. Technical improvements are discussed and beam parameters are characterized by detailed analysis of time of flight density distributions. The possibility of combining this beam source with electrostatic fields for guiding polar molecules is demonstrated.
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 ab…
We present the first experimental observation of cold collisions between two different species of neutral polar molecules, each prepared in a single internal quantum state. Combining for the first time the techniques of Stark deceleration, magnetic trapping, and cryogenic buffer gas cooling allows the enhancement of molecular interaction time by 10$^5$. This has enabled an absolute measurement of the total trap loss cross sections between OH and ND$_3$ at a mean collision energy of 3.6 cm$^{-1}$ (5 K). Due to the dipolar interaction, the total cross section increases upon application of an ext…
Employing a two-stage cryogenic buffer gas cell, we produce a cold, hydrodynamically extracted beam of calcium monohydride molecules with a near effusive velocity distribution. Beam dynamics, thermalization and slowing are studied using laser spectroscopy. The key to this hybrid, effusive-like beam source is a "slowing cell" placed immediately after a hydrodynamic, cryogenic source [Patterson et al., J. Chem. Phys., 2007, 126, 154307]. The resulting CaH beams are created in two regimes. One modestly boosted beam has a forward velocity of vf = 65 m/s, a narrow velocity spread, and a flux of 10^…
We report the observation of the optomechanical strain applied to thermal and to quantum degenerate $^{87}\text{Rb}$ atomic clouds when illuminated by an intense, far detuned homogenous laser beam. In this regime the atomic cloud acts as a lens which focuses the laser beam. As a back action, the atoms experience a force opposite to the beam deflection, which depends on the atomic cloud density profile. We experimentally demonstrate the basic features of this force, distinguishing it from the well-established scattering and dipole forces. The observed strain saturates, ultimately limiting the m…
We demonstrate an atom trap geometry for 87Rb which is capable of producing ultra high atom densities. Reradiation forces, which usually limit high densities, can be avoided in dark spontaneous-force optical traps (dark SPOTs) by sheltering atoms from intense trapping light. Here we demonstrate a dynamic implementation of a dark SPOT, resulting in an increase in atom density by almost two orders of magnitude up to 1.3x10^12cm-3. Holographic control of the trapping beams and dynamic switching between MOT and dark SPOT configuration allows us to optimise the trapping geometry. We have identified…
Ultrathin optical fibres integrated into cold atom setups are proving to be ideal building blocks for atom-photon hybrid quantum networks. Such optical nanofibres (ONF) can be used for the demonstration of nonlinear optics and quantum interference phenomena in atomic media. Here, we report on the observation of multilevel cascaded electromagnetically induced transparency (EIT) using an optical nanofibre to interface cold $^{87}$Rb atoms through the intense evanescent fields that can be achieved at ultralow probe and coupling powers. Both the probe (at 780 nm) and the coupling (at 776 nm) beams…
The correlation spectroscopy has been successfully employed in the measurement of the intrinsic linewidth of electromagnetically induced transparency (EIT) in time and frequency domain. We study the role of the sidebands of the intense fields in the measured spectra, analyzing the information that can be recovered working with different analysis frequencies. In this case, the non-zero one-photon detuning appears as a necessary condition for spectrally resolving the sideband resonances in the correlation coefficient. Our experimental findings are supported by the perturbative model defined in t…
We have measured the ratio of the diffusion cross-section to the angular momentum reorientation cross-section in the colliding Fe-3He and Ni-3He systems. Nickel (Ni) and iron (Fe) atoms are introduced via laser ablation into a cryogenically cooled experimental cell containing cold (< 1 K) 3He buffer gas. Elastic collisions rapidly cool the translational temperature of the ablated atoms to the helium temperature. The cross-section ratio is extracted by measuring the decays of the atomic Zeeman sublevels. For our experimental conditions, thermal energy is comparable to the Zeeman splitting. As a…
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) K, 5.9(0.5) K 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} Σ^{+} (v=0, J=0). With a single 7 ns ablation pulse, the number of molecules in the ground state is 4.5(1.8)*10^{7} molecules per steradian. A second, d…
Production and spectroscopy of cold radioactive molecules
California Institute of Technology（加州理工学院）；Yale University（耶鲁大学）；Johns Hopkins University（约翰斯·霍普金斯大学）；Massachusetts Institute of Technology（麻省理工学院）；Michigan State University（密歇根州立大学）
We report a combined experimental and theoretical study of collision-induced dipolar relaxation in a cold spin-polarized gas of atomic nitrogen (N). We use buffer gas cooling to create trapped samples of 14N and 15N atoms with densities 5+/-2 x 10^{12} cm-3 and measure their magnetic relaxation rates at milli-Kelvin temperatures. Rigorous quantum scattering calculations based on accurate ab initio interaction potentials for the 7Sigma_u electronic state of N2 demonstrate that dipolar relaxation in N + N collisions occurs at a slow rate of ~10^{-13} cm3/s over a wide range of temperatures (1 mK…
We present a rigorous theoretical study of low-temperature collisions of polyatomic molecular radicals with ^1S_0 atoms in the presence of an external magnetic field. Accurate quantum scattering calculations based on ab initio and scaled interaction potentials show that collision-induced spin relaxation of the prototypical organic molecule CH_2(X^3B_1) (methylene) and nine other triatomic radicals in cold 3He gas occurs at a slow rate, demonstrating that cryogenic buffer-gas cooling and magnetic trapping of these molecules is feasible with current technology. Our calculations further suggest t…
We perform numerical simulations of trapped $^{171}$Yb$^+$ ions that are buffer gas cooled by a cold cloud of $^6$Li atoms. This species combination has been suggested to be the most promising for reaching the quantum regime of interacting atoms and ions in a Paul trap. Treating the atoms and ions classically, we compute that the collision energy indeed reaches below the quantum limit for a perfect linear Paul trap. We analyze the effect of imperfections in the ion trap that cause excess micromotion. We find that the suppression of excess micromotion required to reach the quantum limit should …
The current best upper limit for electron electric dipole moment (EDM), $|d_e|<1.1\times10^{-29}\,$e$\cdot$cm ($90$% confidence), was set by the ACME collaboration in 2018. The ACME experiment uses a spin-precession measurement in a cold beam of ThO molecules to detect $d_e$. An improvement in statistical uncertainty would be possible with more efficient use of molecules from the cryogenic buffer gas beam source. Here, we demonstrate electrostatic focusing of the ThO beam with a hexapole lens. This results in a factor of $16$ enhancement in the molecular flux detectable downstream, in a beamli…
We present a theoretical analysis of optical pathways for formation of cold Ca($^1$S)Na$^+$($^1$S) molecular ions via an intermediate state. The formation schemes are based on ab initio potential energy curves and transition dipole moments calculated using effective-core-potential methods of quantum chemistry. In the proposed approach, starting from a mixture of cold trapped Ca$^+$ ions immersed into an ultracold gas of Na atoms, (NaCa)$^+$ molecular ions are photoassociated in the excited E$^{1}Σ^+$ electronic state and allowed to spontaneously decay either to the ground electronic state or a…
Laser cooled atoms are central to modern precision measurements. They are also increasingly important as an enabling technology for experimental cavity quantum electrodynamics, quantum information processing and matter wave interferometry. Although significant progress has been made in miniaturising atomic metrological devices, these are limited in accuracy by their use of hot atomic ensembles and buffer gases. Advances have also been made in producing portable apparatus that benefit from the advantages of atoms in the microKelvin regime. However, simplifying atomic cooling and loading using m…
