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 great variety of molecules at controlled temperature and pressure, and is particularly well-suited to those that are difficult to produce in the gas phase.
We demonstrate an improvement in short-term stability by a factor of 10 over a previous generation miniature buffer gas cooled trapped ion clock. We describe the enhancement to detection SNR that has enabled this improvement, the method of clock operation, and the measurement of clock short-term stability. Additionally, we numerically investigate the magnitude of the Dick effect in our pulsed ion clock.
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…
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…
We demonstrate one-dimensional Doppler cooling of a beam of buffer-gas cooled Barium monofluoride (BaF) molecules. The dependences of the cooling efficiency with the laser detuning, the bias filed and the laser intensity are carefully measured. We numerical simulate our experiment with a Monte Carlo method, and find the theoretic predictions consists with our experimental data. This result represents a key step towards further cooling and trapping of BaF molecules.
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…
Aluminum monochloride (AlCl) has been proposed as an excellent candidate for laser cooling. Here we present absorption spectroscopy measurements on the $A^1Π\leftarrow X^1Σ^+$ transition in AlCl inside a cryogenic helium buffer-gas beam cell. The high resolution absorption data enables a rigorous, quantitative comparison with our high-level ab initio calculations of the electronic and rovibronic energies, providing a comprehensive picture of the AlCl quantum structure. The combination of high resolution spectral data and theory permits the evaluation of spectroscopic constants and associated p…
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 report an experimental investigation on the Doppler-free saturated absorption spectroscopy of buffer-gas-cooled Barium monofluoride (BaF) molecules in a 4~K cryogenic cell. The obtained spectra with a resolution of 19~MHz, much smaller than previously observed in absorption spectroscopy, clearly resolve the hyperfine transitions. Moreover, we use these high-resolution spectra to fit the hyperfine splittings of excited $A(v=0)$ state and find the hyperfine splitting of the laser-cooling-relevant $A^2Π_{1/2}(v=0, J=1/2, +)$ state is about 18 MHz, much higher than the previous theoretically pr…
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…
Specular reflection of polar molecules from a simple multi-cylinder electrostatic mirror: a method for separating BaF molecules produced in a buffer-gas-cooled laser-ablation source from other ablation products
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 $…
An ion in a radiofrequency (rf) trap sympathetically cooled by a simultaneously trapped neutral buffer gas exhibits deviations from thermal statistics caused by collision-induced coupling of the rf field to the ion motion. For a uniform density distribution of the buffer gas, the energy distribution of the ion can be described by Tsallis statistics. Moreover, runaway heating of the ion occurs if the buffer gas particles are sufficiently heavy relative to the ion. In typical experiments, however, ultracold buffer gases are confined in traps resulting in localised, non-uniform density distributi…
We produce cold and dense clouds of atomic ions (Ca$^+$, Dy$^+$) by laser ablation of metal targets and cryogenic buffer gas cooling of the resulting plasma. We measure the temperature and density of the ion clouds using laser absorption spectroscopy. We find that large ion densities can be obtained at temperatures as low as 6 K. Our method opens up new ways to study cold neutral plasmas, and to perform survey spectroscopy of ions that cannot be laser-cooled easily.
In order to realize more sensitive eEDM measurement, it would be worthwhile to find some new laser-cooled molecules with larger internal effective electric field (E$_{eff}$), higher electric polarizability and longer lifetime of the eEDM measurement state. Here we explore the merits of mercuric monofluoride ($^{202}Hg^{19}F$, X$^ 2 Σ_{1/2}$) for its potential of laser cooling and eEDM measurement. We theoretically investigated the electronic, rovibrational and hyperfine structures and verified the highly diagonal Franck-Condon factors (FCFs) of the main transitions by the Rydberg-Klein-Rees in…
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 …
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…
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…
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 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 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 …
Ultracold CH radicals promise a fruitful testbed for probing quantum-state controllable organic chemistry. In this work, we calculate CH vibrational branching ratios (VBRs) and rotational branching ratios (RBRs) with ground state mixing. We subsequently use these values to inform optical cycling proposals and consider two possible radiative cooling schemes using the $X^{2}Π\leftarrow A^{2}Δ$ and $X^{2}Π\leftarrow B^{2}Σ^{-}$ transitions. As a first step towards laser cooled CH, we characterize the effective buffer gas cooling of this species and produce $\sim5\times10^{10}$ CH molecules per pu…
Trapping molecular ions that have been sympathetically cooled with laser-cooled atomic ions is a useful platform for exploring cold ion chemistry. We designed and characterized a new experimental apparatus for probing chemical reaction dynamics between molecular cations and neutral radicals at temperatures below 1 K. The ions are trapped in a linear quadrupole radio-frequency trap and sympathetically cooled by co-trapped, laser-cooled, atomic ions. The ion trap is coupled to a time-of-flight mass spectrometer to readily identify product ion species, as well as to accurately determine trapped i…
We show that weakly bound He-containing van der Waals molecules can be produced and magnetically trapped in buffer-gas cooling experiments, and provide a general model for the formation and dynamics of these molecules. Our analysis shows that, at typical experimental parameters, thermodynamics favors the formation of van der Waals complexes composed of a helium atom bound to most open-shell atoms and molecules, and that complex formation occurs quickly enough to ensure chemical equilibrium. For molecular pairs composed of a He atom and an S-state atom, the molecular spin is stable during forma…
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 demonstrate a quasi optical cycling for the $X(v=0)\to A(v'=0)$ transition and a radiative force induced deflection on the buffer-gas cooled BaF molecular beam. The laser induced fluorescence enhancement with additional sidebands and a polarization modulation scheme indicates that the hyperfine states and the Zeeman sublevels are closed. The quasi optical cycling by repumping the $X(v=1)\to A(v'=0)$ leads to a $\sim$ 0.8 mm deflection of the beam via scattering $\sim$ 150 photons per molecule, in good agreement with the predictions from our multi-level rate equation model. Further improveme…
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 describe measurements demonstrating laser cooling of an atomic gas by means of collisional redistribution of radiation. The experiment uses rubidium atoms in the presence of several hundred bar of argon buffer gas pressure. Frequent collisions in the dense gas transiently shift a far red detuned optical field into resonance, while spontaneous emission occurs close to the unperturbed atomic transition frequency. Evidence for the cooling is obtained both via thermographic imaging and via thermographic deflection spectroscopy. The cooled gas has a density above 10$^{21}$ atoms/cm$^3$, yielding…
Quantum state-resolved spectroscopy was recently achieved for C60 molecules when cooled by buffer gas collisions and probed with a midinfrared frequency comb. This rovibrational quantum state resolution for the largest molecule on record is facilitated by the remarkable symmetry and rigidity of C60, which also present new opportunities and challenges to explore energy transfer between quantum states in this many-atom system. Here we combine state-specific optical pumping, buffer gas collisions, and ultrasensitive intracavity nonlinear spectroscopy to initiate and probe the rotation-vibration e…
A prerequisite for laser cooling a molecular anion, which has not been achieved so far, is the precise knowledge of the relevant transition frequencies in the cooling scheme. To determine these frequencies we present a versatile method that uses one pump and one photodetachment light beam. We apply this approach to C$_{2}^{-}$ and study the laser cooling transitions between the electronic ground state and the second electronic excited state in their respective vibrational ground levels, $B ^{2} Σ_{u} ^{+}(v=0) \leftarrow X ^{2} Σ_{g} ^{+}(v=0) $. Measurements of the R(0), R(2), and P(2) transi…
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）
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）
The general idea that optical radiation may cool matter was put forward by Pringsheim already in 1929. Doppler cooling of dilute atomic gases is an extremely successful application of this concept, and more recently anti-Stokes cooling in multilevel systems has been explored, culminating in the optical refrigeration of solids. Collisional redistribution of radiation is a proposed different cooling mechanism that involves atomic two-level systems, though experimental investigations in gases with moderate density have so far not reached the cooling regime. Here we experimentally demonstrate lase…
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）
It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields. Unfortunately laser cooling has not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for many applications. For example, heteronuclear molecules possess permanent electric dipole moments which lead to long-range, tunable, anisotropic dipole-dipole interactions. The combination of the dipole-dipole interaction and the precise control over molecular degrees of freedom …
