We demonstrate optical cycling and sub-Doppler laser cooling of a cryogenic buffer-gas beam of calcium monohydride (CaH) molecules. We measure vibrational branching ratios for laser cooling transitions for both excited electronic states A and B. We measure further that repeated photon scattering via the $A\leftarrow X$ transition is achievable at a rate of $\sim$ $1.6\times10^6$ photons/s and demonstrate the interaction-time limited scattering of $\sim$ $200$ photons by repumping the largest vibrational decay channel. We also demonstrate the ability to sub-Doppler cool a molecular beam of CaH through the magnetically assisted Sisyphus effect. Using a standing wave of light, we lower the molecular beam's transverse temperature from $12.2(1.2)$ mK to $5.7(1.1)$ mK. We compare these results to sub-Doppler forces modeled using optical Bloch equations and Monte Carlo simulations of the molecular beam trajectories. This work establishes a clear pathway for creating a magneto-optical trap (MOT) of CaH molecules. Such a MOT could serve as a starting point for production of ultracold hydrogen gas via dissociation of a trapped CaH cloud.
New molecular line lists for calcium monohydride ($^{40}$Ca$^{1}$H) and magnesium monohydride ($^{24}$Mg$^{1}$H) and its minor isotopologues ($^{25}$Mg$^{1}$H and $^{26}$Mg$^{1}$H) are presented. The rotation-vibration-electronic (rovibronic) line lists, named \texttt{XAB}, consider transitions involving the \X, \A, and \BBp\ electronic states in the 0--30\,000~cm$^{-1}$ region (wavelengths $λ> 0.33$~$μ$m) and are suitable for temperatures up to 5000 K. A comprehensive analysis of the published spectroscopic literature on CaH and MgH is used to obtain new extensive datasets of accurate rovibro…
We present the first experimental demonstration of radiation pressure force deflection and direct laser cooling for barium monohydride (BaH) molecules resulting from multiple photon scattering. Despite a small recoil velocity (2.7 mm/s) and a long excited state lifetime (137 ns), we use 1060 nm laser light exciting the $X\rightarrow A$ electronic transition of BaH to deflect a cryogenic buffer-gas beam and reduce its transverse velocity spread. Multiple experimental methods are employed to characterize the optical cycling dynamics and benchmark theoretical estimates based on rate equation mode…
Laser cooling by collisional redistribution of radiation has been successfully applied in the past for cooling dense atomic gases. Here we report on progress of work aiming at the demonstration of redistribution laser cooling in a molecular gas. The candidate molecule strontium monohydride is produced by laser ablation of strontium dihydride in a pressurized noble gas atmosphere. The composition of the ablation plasma plume is analyzed by measuring its emission spectrum. The dynamics of SrH molecular density following the ablation laser pulse is studied as a function of the buffer gas pressure…
We describe a simple experimental apparatus for laser ablation of barium monohydride (BaH) molecules and the study of their rovibrational spectra that are relevant to direct laser cooling. We present a detailed analysis of the properties of ablation plumes that can improve the understanding of surface ablation and deposition technologies. A range of absorption spectroscopy and collisional thermalization regimes has been studied. We directly measured the Franck-Condon factor of the $\mathrm{B}^2Σ^+(v'=0)\leftarrow\mathrm{X}^2Σ^+(v"=1)$ transition. Prospects for production of a high luminosity c…
Ultracold molecular gases are promising as an avenue to rich many-body physics, quantum chemistry, quantum information, and precision measurements. This richness, which flows from the complex internal structure of molecules, makes the creation of ultracold molecular gases using traditional methods (laser plus evaporative cooling) a challenge, in particular due to the spontaneous decay of molecules into dark states. We propose a way to circumvent this key bottleneck using an all-optical method for decelerating molecules using stimulated absorption and emission with a single ultrafast laser. We …
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 present a new method for the generation of rotationally and vibrationally state-selected, translationally cold molecular ions in ion traps. Our technique is based on the state-selective threshold photoionization of neutral molecules followed by sympathetic cooling of the resulting ions with laser-cooled calcium ions. Using N$_2^+$ ions as a test system, we achieve > 90 % selectivity in the preparation of the ground rovibrational level and state lifetimes on the order of 15 minutes limited by collisions with background-gas molecules. The technique can be employed to produce a wide range of a…
We report direct laser cooling of a symmetric top molecule, reducing the transverse temperature of a beam of calcium monomethoxide (CaOCH$_3$) to $1.8\pm0.7$ mK while addressing two distinct nuclear spin isomers. These results open a path to efficient production of ultracold chiral molecules and conclusively demonstrate that by using proper rovibronic optical transitions, both photon cycling and laser cooling of complex molecules can be as efficient as for much simpler linear species.
Calcium monofluoride (CaF) molecules are loaded into an optical dipole trap (ODT) and subsequently laser cooled within the trap. Starting with magneto-optical trapping, we sub-Doppler cool CaF and then load $150(30)$ CaF molecules into an ODT. Enhanced loading by a factor of five is obtained when sub-Doppler cooling light and trapping light are on simultaneously. For trapped molecules, we directly observe efficient sub-Doppler cooling to a temperature of $60(5)$ $μ\text{K}$. The trapped molecular density of $8(2)\times10^7$ cm$^{-3}$ is an order of magnitude greater than in the initial sub-Dop…
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 have characterized the molecular tellurium (Te$_2$) spectrum in the vicinity of the 423nm $^1S_0-^1P_1$ and the 431nm $^3P_1-^3P_0$ transitions in neutral calcium. These transitions are relevant to optical clocks for atomic-beam characterization and cooling (423nm) and enhanced detection (431nm). The use of a Te$_2$ vapor cell as a frequency reference has many advantages over other laser stabilization techniques, and we discuss an application to measuring the instability due to the second-order Doppler shift in a calcium beam clock.
Charge Exchange Dynamics in Cold Collisions of $^{40}$CaH$^+$ and $^{39}$K
Lawrence Berkeley National Lab（劳伦斯伯克利国家实验室）；Duke Quantum Center, Duke University（杜克大学量子中心）；Department of Physics, Duke University（杜克大学物理系）；Faculty of Physics, University of Warsaw（华沙大学物理学院）；IonQ Inc（IonQ公司）；Department of Electrical and Computer Engineering, Duke University（杜克大学电气与计算机工程系）；Department of Chemistry, Duke University（杜克大学化学系）
We present studies of resonance-enhanced photo-ionization for isotope-selective loading of Ca+ into a Paul trap. The 4s^2 ^1S_0 <-> 4s4p ^1P_1 transition of neutral calcium is driven by a 423nm laser and the atoms are photo-ionized by a second laser at 389nm. Isotope-selectivity is achieved by using crossed atomic and laser beams to reduce the Doppler width significantly below the isotope shifts in the 423nm transition. The loading rate of ions into the trap is studied under a range of experimental parameters for the abundant isotope 40Ca+. Using the fluorescence of the atomic beam at 423nm as…
We present a high-resolution laser spectroscopic study of the $\tilde{A}\,^2B_2- \tilde{X}\,^2A_1$ and $\tilde{B}\,^2B_1- \tilde{X}\,^2A_1$ transitions of calcium (I) phenoxide, CaOPh (CaOC$_6$H$_5$). The rotationally resolved band systems are analyzed using an effective Hamiltonian model and are accurately modeled as independent perpendicular ($b$- or $c$-type) transitions. The structure of calcium monophenoxide is compared to previously observed Ca-containing radicals and implications for direct laser cooling are discussed. This work demonstrates that functionalization of aromatic molecules …
The calcium monohydroxide radical (CaOH) is an important astrophysical molecule relevant to cool stars and rocky exoplanets, amongst other astronomical environments. Here, we present a consistent set of highly accurate rovibronic (rotation-vibration-electronic) energy levels for the five lowest electronic states ($\tilde{X}\,^2Σ^+$, $\tilde{A}\,^2Π$, $\tilde{B}\,^2Σ^+$, $\tilde{C}\,^2Δ$, $\tilde{D}\,^2Σ^+$) of CaOH. A comprehensive analysis of the published spectroscopic literature on this system has allowed 1955 energy levels to be determined from 3204 rovibronic experimental transitions, all…
A new possibility of laser cooling of alkaline-earth-metal and Ytterbium atoms using a two-photon transition is analyzed. We consider a $^{1}S_{0}$ - $^{1}S_{0}$ transition, with excitation in near resonance with the $^{1}P_{1}$ level. This greatly increases the two-photon transition rate, allowing an effective transfer of momentum. The experimental implementation of this technique is discussed and we show that for Calcium, for example, two-photon cooling can be used to achieve a Doppler limit of 123 microKelvin. The efficiency of this cooling scheme and the main loss mechanisms are analyzed.
We report magneto-optical trapping (MOT) of a polyatomic molecule, calcium monohydroxide (CaOH). The MOT contains $2.0(5)\times 10^4$ CaOH molecules at a peak density of $3.0(8)\times10^{6}$ cm$^{-3}$. CaOH molecules are further sub-Doppler laser cooled in an optical molasses, to a temperature of 110(4) $μ$K. The temperatures and densities achieved here make CaOH a viable candidate for a wide variety of quantum science applications, including the creation of optical tweezer arrays of CaOH molecules. This work also suggests that laser cooling and magneto-optical trapping of many other polyatomi…
We report non-destructive imaging of optically trapped calcium monofluoride (CaF) molecules using in-situ $Λ$-enhanced gray molasses cooling. $200$ times more fluorescence is obtained compared to destructive on-resonance imaging, and the trapped molecules remain at a temperature of $20\,μ\text{K}$. The achieved number of scattered photons makes possible non-destructive single-shot detection of single molecules with high fidelity.
Photon Cycling and Laser Cooling of an Asymmetric Top Molecule
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）；Korea University（高丽大学）；Massachusetts Institute of Technology（麻省理工学院）；University of California, Berkeley（加州大学伯克利分校）；Michigan State University（密歇根州立大学）；University of Southern California（南加州大学）
We demonstrate a 1D magneto-optical trap of the polar free radical calcium monohydroxide (CaOH). A quasi-closed cycling transition is established to scatter $\sim 10^3$ photons per molecule, predominantly limited by interaction time. This enables radiative laser cooling of CaOH while compressing the molecular beam, leading to a significant increase in on-axis beam brightness and reduction in temperature from 8.4 mK to 1.4 mK.
Calcium monofluoride (CaF) is magnetically slowed and trapped using optical pumping. Starting from a collisionally cooled slow beam, CaF with an initial velocity of ~ 30 m/s is slowed via magnetic forces as it enters a 800 mK deep magnetic trap. Employing two-stage optical pumping, CaF is irreversibly loaded into the trap via two scattered photons. We observe a trap lifetime exceeding 500 ms, limited by background collisions. This method paves the way for cooling and magnetic trapping of chemically diverse molecules without closed cycling transitions.
This paper presents one of the case studies of the Gamma Factory initiative -- a proposal of a new operation scheme of ion beams in the CERN accelerator complex. Its goal is to extend the scope and precision of the LHC-based research by complementing the proton-proton collision programme with the high-luminosity nucleus-nucleus one. Its numerous physics highlights include studies of the exclusive Higgs-boson production in photon-photon collisions and precision measurements of the electroweak (EW) parameters. There are two principal ways to increase the LHC luminosity which do not require an up…
We study optical cycling in the polar free radical calcium monohydroxide (CaOH) and establish an experimental path towards scattering $\sim$$10^4$ photons. We report rovibronic branching ratio measurements with precision at the $\sim10^{-4}$ level and observe weak symmetry-forbidden decays to bending modes with non-zero vibrational angular momentum. Calculations are in excellent agreement with these measurements and predict additional decay pathways. Additionally, we perform high-resolution spectroscopy of the $\widetilde{\text{X}}\,^2Σ^+(12^00)$ and $\widetilde{\text{X}}\,^2Σ^+(12^20)$ hybrid…
We study theoretically the behavior of laser-cooled calcium monofluoride (CaF) molecules in an optical molasses and magneto-optical trap (MOT), and compare our results to recent experiments. We use multi-level optical Bloch equations to estimate the force and the diffusion constant, followed by a Fokker-Planck-Kramers equation to calculate the time-evolution of the velocity distribution. The calculations are done in three-dimensions, and we include all the relevant energy levels of the molecule and all the relevant frequency components of the light. Similar to simpler model systems, the veloci…
We examine the prospects for utilizing the optical bichromatic force (BCF) to greatly enhance laser deceleration and cooling for near-cycling transitions in small molecules. We discuss the expected behavior of the BCF in near-cycling transitions with internal degeneracies, then consider the specific example of decelerating a beam of calcium monofluoride molecules. We have selected CaF as a prototype molecule both because it has an easily-accessible near-cycling transition, and because it is well-suited to studies of ultracold molecular physics and chemistry. We also report experimental verific…
Optically trapped laser-cooled polar molecules hold promise for new science and technology in quantum information and quantum simulation. Large numerical aperture optical access and long trap lifetimes are needed for many studies, but these requirements are challenging to achieve in a magneto-optical trap (MOT) vacuum chamber that is connected to a cryogenic buffer gas beam source, as is the case for all molecule laser cooling experiments so far. Long distance transport of molecules greatly eases fulfilling these requirements as molecules are placed into a region separate from the MOT chamber.…
