We present a combined experimental and theoretical study of beam formation from a cryogenic buffer gas cell. Atoms and molecules are loaded into the cell by laser ablation of a target, and are cooled and swept out of the cell by a flow of cold helium. We study the thermalization and flow dynamics inside the cell and measure how the speed, temperature, divergence and extraction efficiency of the beam are influenced by the helium flow. We use a finite element model to simulate the flow dynamics and use the predictions of this model to interpret our experimental results.
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 demonstrate the direct loading of a D$_2$ MOT of potassium-39 atoms from a cryogenic buffer gas beam source. We load $10^8$ atoms in a 10 ms pulse, with no degradation in performance up to a 10 Hz repetition rate. Observed densities reach $\sim10^{11}$ atoms/cm$^3$ in a single pulse, achieved with no sub-Doppler cooling or transverse compression. This system produces an ideal starting point for ultracold atom experiments where high experimental repetition rates are desirable and initial high densities are critical. Extension to other atomic species (e.g., refractory metals) that present tec…
A cryogenic buffer gas beam source with in-situ ablation target replacement
University of Chicago（芝加哥大学）；Harvard University（哈佛大学）；Harvard-MIT Center for Ultracold Atoms（哈佛-麻省理工学院超冷原子中心）；Northwestern University（西北大学）；Okayama University（冈山大学）；Michigan State University（密歇根州立大学）
We apply near-threshold laser photodetachment to characterize the rotational quantum level distribution of OH$^-$ ions stored in the cryogenic ion-beam storage ring, DESIREE, at Stockholm University. We find that the stored ions relax to a rotational temperature of 13.4$\pm$0.2 K with 94.9$\pm$0.3 % of the ions in the rotational ground state. This is consistent with the storage ring temperature of 13.5$\pm$0.5 K as measured with eight silicon diodes, but in contrast to all earlier studies in cryogenic traps and rings where the rotational temperatures were always much higher than those of the s…
Electrostatic quadrupole lens for focusing a cryogenic $^{205}$TlF molecular beam
Columbia University（哥伦比亚大学）；Argonne National Laboratory（阿贡国家实验室）；Johns Hopkins University（约翰斯·霍普金斯大学）；Yale University（耶鲁大学）；University of Massachusetts Amherst（马萨诸塞大学阿默斯特分校）；University of Chicago（芝加哥大学）
We demonstrate the deceleration of heavy polar molecules in low-field seeking states by combining a cryogenic source and a travelling-wave Stark decelerator. The cryogenic source provides a high intensity beam with low speed and temperature, and the travelling-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.
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 x 10^11 molecules/sr/pulse in the rovibrational ground state, with 140 m/s forward velocity and a rotational temperature of approximately 1 K. This source compares fav…
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 present a versatile and compact electron beam driven source for alkali metal atoms, which can be implemented in cryostats. With a heat load of less than 10mW, the heat dissipation normalized to the atoms loaded into the magneto-optical Trap (MOT), is about a factor 1000 smaller than for a typical alkali metal dispenser. The measured linear scaling of the MOT loading rate with electron current observed in the experiments, indicates that electron stimulated desorption is the corresponding mechanism to release the atoms.
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…
Barium monohydride (BaH) is an attractive candidate for extending laser cooling and trapping techniques to diatomic hydrides. The apparatus and high-resolution optical spectroscopy presented here demonstrate progress toward this goal. A cryogenic buffer-gas-cooled molecular beam of BaH was constructed and characterized. Pulsed laser ablation into cryogenic helium buffer gas delivers $\sim1\times10^{10}$ molecules/sr/pulse in the X$^2Σ^+$ ($v''=0,N''=1$) state of primary interest. More than $1\times10^7$ of these molecules per pulse enter the downstream science region with forward velocities be…
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）
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…
We have produced a cryogenic buffer-gas cooled beam of the diatomic molecular radical CH (methylidyne). This molecule is of interest for studying cold chemical reactions and fundamental physics measurements. Its light mass and ground-state structure make it a promising candidate for electrostatic guiding and Stark deceleration, which allows for control over its kinetic energy. This control can facilitate studies of reactions with tuneable collision energies and trapping for precise spectroscopic studies. Here, we have demonstrated electrostatic guiding of CH with fluxes up to $10^9$ molecules …
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 demonstrate cryogenic buffer-gas cooling of gas-phase methyltrioxorhenium (MTO). This molecule is closely related to chiral organometallic molecules where the parity-violating energy differences between enantiomers may be measurable. The molecules are produced with a rotational temperature of approximately 6~K by laser ablation of an MTO pellet inside a cryogenic helium buffer gas cell. Facilitated by the low temperature, we demonstrate absorption spectroscopy of the 10.2~$μ$m antisymmetric Re=O stretching mode of MTO with a resolution of 8~MHz and a frequency accuracy of 30~MHz. We partial…
We have systematically investigated the energy resolution of a magnetic micro-calorimeter (MMC) for atomic and molecular projectiles at impact energies ranging from $E\approx13$ to 150 keV. For atoms we obtained absolute energy resolutions down to $ΔE \approx 120$ eV and relative energy resolutions down to $ΔE/E\approx10^{-3}$. We also studied in detail the MMC energy-response function to molecular projectiles of up to mass 56 u. We have demonstrated the capability of identifying neutral fragmentation products of these molecules by calorimetric mass spectrometry. We have modeled the MMC energy…
Exchange of orbital angular momentum between Laguerre-Gaussian beam of light and center-of-mass motion of an atom or molecule is well known. We show that orbital angular momentum of light can also be transferred to the internal electronic or rotational motion of an atom or a molecule provided the internal and center-of-mass motions are coupled. However, this transfer does not happen directly to the internal motion, but via center-of-mass motion. If atoms or molecules are cooled down to recoil limit then an exchange of angular momentum between the quantized center-of-mass motion and the interna…
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^…
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…
We describe the generation and properties of a cryogenic beam of $^7$Li$_2$ dimers from sublimation of a neon matrix where lithium atoms have been implanted via laser ablation of solid precursors of metallic lithium or lithium hydride (LiH). Different sublimation regimes lead to pulsed molecular beams with different temperatures, densities and forward velocities. With laser absorption spectroscopy these parameters were measured using the molecular $^7$Li$_2$ (R) transitions A$^1Σ_u^+(v'=4,J'=J''+1)\leftarrow $X$^1Σ_g^+ (v''=0,J''=0,1,3)$. In a typical regime, sublimating a matrix at 16 K, tran…
We report on the deceleration of a beam of SrF molecules from 290 to 120~m/s. Following supersonic expansion, the molecules in the $X^2Σ$ ($v=0$, $N=1$) low-field seeking states are trapped by the moving potential wells of a traveling-wave Stark decelerator. With a deceleration strength of 9.6 km/s$^2$ we have demonstrated the removal of 85 % of the initial kinetic energy in a 4 meter long modular decelerator. The absolute amount of kinetic energy removed is a factor 1.5 higher compared to previous Stark deceleration experiments. The demonstrated decelerator provides a novel tool for the creat…
We demonstrate multiple photon cycling and radiative force deflection on the triatomic free radical strontium monohydroxide (SrOH). Optical cycling is achieved on SrOH in a cryogenic buffer-gas beam by employing the rotationally closed $P\left(N''=1\right)$ branch of the vibronic transition $\tilde{X}^{2}Σ^{+}\left(000\right)\leftrightarrow\tilde{A}^{2}Π_{1/2}\left(000\right)$. A single repumping laser excites the Sr-O stretching vibrational mode, and photon cycling of the molecule deflects the SrOH beam by an angle of $0.2^{\circ}$ via scattering of $\sim100$ photons per molecule. This approa…
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.
An electrostatic cryogenic storage ring, CSR, for beams of anions and cations with up to 300 keV kinetic energy per unit charge has been designed, constructed and put into operation. With a circumference of 35 m, the ion-beam vacuum chambers and all beam optics are in a cryostat and cooled by a closed-cycle liquid helium system. At temperatures as low as (5.5 $\pm$ 1) K inside the ring, storage time constants of several minutes up to almost an hour were observed for atomic and molecular, anion and cation beams at an energy of 60 keV. The ion-beam intensity, energy-dependent closed-orbit shifts…
We demonstrate the coherent optical bichromatic force on a molecule, the polar free radical strontium monohydroxide (SrOH). A dual-frequency retro-reflected laser beam addressing the $\tilde{X}^2Σ^+\leftrightarrow\tilde{A}^2Π_{1/2}$ electronic transition coherently imparts momentum onto a cryogenic beam of SrOH. This directional photon exchange creates a bichromatic force that transversely deflects the molecules. By adjusting the relative phase between the forward and counter propagating laser beams we reverse the direction of the applied force. A momentum transfer of $70\hbar k$ is achieved w…
In this communication, we present the results of the Five-fold Differential Cross Section (5DCS) and Triple Differential Cross Section (TDCS) for the (e,2e) process on molecular hydrogen ($H_2$) by the plane wave and the twisted electron beam impact. The formalism is developed within the first Born approximation using the plane wave and the twisted wave for the incident electron beam. We describe the plane wave, Heitler-London type wave function and Coulomb wave for the scattered electron, $H_2$ molecular state, and the ejected electron respectively. We compare the angular profiles of the 5DCS…
A cryogenic apparatus with a rotatable substrate for matrix isolation spectroscopy of BaF in neon crystals down to 3.2 K
Istituto Nazionale di Fisica Nucleare（意大利国家核物理研究所）；University of Ferrara（费拉拉大学）；University of Padua（帕多瓦大学）；National Quantum Science and Technology Institute（国家量子科学与技术研究所）
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.
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…
This paper theoretically treats the spontaneous resonant inelastic scattering of Laguerre-Gauss (LG) beams from the totally symmetric vibrations of complex polyatomic molecules within the semi-classical framework. We develop an interaction Hamiltonian that accounts for the position of the molecule within the excitation beam to derive the effective differential scattering cross-section of a classical LG beam from a molecule using the frequency domain third order nonlinear optical response function. To gain physical insight into this scattering process, we utilize a model vibronic molecule to st…
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 experimentally observe the action of multiple light pulses on the transverse motion of a continuous beam of fullerenes. The light potential is generated by non-resonant ultra-short laser pulses in perpendicular spatial overlap with the molecule beam. We observe a small but clear enhancement of the number of molecules in the center fraction of the molecular beam. Relatively low light intensity and short laser pulse duration prevent the molecule from fragmentation and ionization. Experimental results are confirmed by Monte Carlo trajectory simulations.
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 bet…
We have demonstrated a new, accessible and economical technique, dubbed photostop, for producing high densities of trappable molecules. Direct measurements are presented of NO molecules produced with a narrow velocity distribution centered at zero in the laboratory frame. NO2, initially cooled in a pulsed molecular beam, is photodissociated such that the recoil velocity of the NO photofragments cancels out the velocity of the beam. NO(X^2Pi_3/2, v=0, J=1.5) molecules are observed up to 10 mircoseconds after the dissociation event in the probe volume at an estimated density of 1E7 cm-3 per quan…
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 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 make use of an inhomogeneous electrostatic dipole field to impart a quantum-state-dependent deflection to a pulsed beam of OCS molecules, and show that those molecules residing in the absolute ground state, $X ^1Σ^+$, $\ket{00^00}$, J=0, can be separated out by selecting the most deflected part of the molecular beam. Past the deflector, we irradiate the molecular beam by a linearly polarized pulsed nonresonant laser beam that impulsively aligns the OCS molecules. Their alignment, monitored via velocity-map imaging, is measured as a function of time, and the time dependence of the alignment …
We study the dynamics of a supersonic molecular beam in a low-finesse optical cavity and demonstrate that most molecules in the beam can be decelerated to zero central velocity by the intracavity optical field in a process analogous to electrostatic Stark deceleration. We show that the rapid switching of the optical field for slowing the molecules is automatically generated by the cavity-induced dynamics. We further show that $\sim1\%$ of the molecules can be optically trapped at a few millikelvin in the same cavity.
Recently, we reported the commissioning of the new cryogenic ion storage ring RICE, which demonstrated potential capabilities for the precise studies of molecular structures and reaction dynamics. In the present article, we describe the status of experimental programs ongoing at RICE with a focus on the laser spectroscopy and merged-beam collision experiments.
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…
Helium atoms in Rydberg states have been manipulated coherently with microwave radiation pulses near a gold surface and near a superconducting NbTiN surface at a temperature of $3 \text{K}$. The experiments were carried out with a skimmed supersonic beam of metastable $(1\text{s})^1(2\text{s})^1\, {}^1\text{S}_0$ helium atoms excited with laser radiation to $n\text{p}$ Rydberg levels with principal quantum number $n$ between $30$ and $40$. The separation between the cold surface and the center of the collimated beam is adjustable down to $250 μ\text{m}$. Short-lived $n\text{p}$ Rydberg levels …
Electric deflection measurements on liquid helium nanodroplets doped with individual polar molecules demonstrate that the cold superfluid matrix enables full orientation of the molecular dipole along the external field. This translates into a deflection force which is increased enormously by comparison with typical deflection experiments, and it becomes possible to measurably deflect neutral doped droplets with masses of tens to hundreds of thousands of Daltons. This approach permits preparation and study of continuous fluxes of fully oriented polar molecules and is broadly and generally appli…
