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International Symposium on Molecular Spectroscopy (ISMS)

LASER COOLING THE DIATOMIC MOLECULE CaH

III, Velasquez, Michael D. Di Rosa

Published Jun 19, 2014• 2 citations
Publisher

Abstract

To laser-cool a species, a closed (or nearly closed) cycle is required to dissipate translational energy through many directed laser-photon absorption and subsequent randomly-directed spontaneous emission events. Many atoms lend themselves to such a closed-loop cooling cycle. Attaining laser-cooled molecular species is challenging because of their inherently complex internal structure, yet laser-cooling molecules could lead to studies in interesting chemical dynamics among other applications. Typically, laser-cooled atoms are assembled into molecules through photoassociation or Feschbach resonance. CaH is one of a few molecules whose internal structure is quite atom-like, allowing a nearly closed cycle without the need for many repumping lasers. We will also present our work-to-date on laser cooling this molecule. We employ traditional pulsed atomic/molecular beam techniques with a laser vaporization source to generate species with well-defined translational energies over a narrow range of velocity. In this way, we can apply laser-cooling to most species in the beam along a single dimension (the beam’s axis). This project is funded by the LDRD program of the Los Alamos National Laboratory.

DOI
10.15278/isms.2014.rh07

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To laser-cool a species, a closed (or nearly closed) cycle is required to dissipate translational energy through many directed laser-photon absorption and subsequent randomly-directed spontaneous emission events. Many atoms lend themselves to such a closed-loop cooling cycle. Attaining laser-cooled molecular species is challenging because of their inherently complex internal structure, yet laser-cooling molecules could lead to studies in interesting chemical dynamics among other applications. Typically, laser-cooled atoms are assembled into molecules through photoassociation or Feschbach resonance. CaH is one of a few molecules whose internal structure is quite atom-like, allowing a nearly closed cycle without the need for many repumping lasers. We will also present our work-to-date on laser cooling this molecule. We employ traditional pulsed atomic/molecular beam techniques with a laser vaporization source to generate species with well-defined translational energies over a narrow range of velocity. In this way, we can apply laser-cooling to most species in the beam along a single dimension (the beam’s axis). This project is funded by the LDRD program of the Los Alamos National Laboratory.
A novel scheme is proposed for sequential cooling of rotation, translation, and vibration of molecules. More generally, this scheme manipulates and controls the states and energies of molecules. The scheme, while somewhat complex, is simpler and more feasible than simply providing a large number of synchronously but independently tunable lasers. The key component is a multiple single frequency laser (MSFL) in which a single narrow band pump laser generates an ensemble of resonant ‘‘stimulated Raman’’ (RSR) sidebands (subsequently amplified and selected) in a sample of the molecules to be cooled. Starting with a relatively cold molecular sample (e.g., a supersonic beam of Cs2), the rotation of molecules is cooled by sequential application of P branch electronic transition frequencies transverse to the molecular beam beginning at higher rotational angular momentum J. Then translation of molecules is cooled by application of multiple low J, P, and R branch transition frequencies which counterpropagate with the molecular beam and are synchronously chirped over their Doppler profiles. Finally, vibration of molecules is cooled by blocking the R(0) line of the 0–0 band. Only this specific order of rotation–translation–vibration appears feasible (using molecules produced by photoassociation of ultracold atoms avoids the requirement for translational cooling). Each step employs true dissipative cooling (i.e., reduction of system entropy in three degrees of freedom) by spontaneous emission and should yield a large translationally cold sample of molecules in the lowest (v=0, J=0) level of the ground electronic state, suitable for studies such as molecule trapping, ‘‘molecule optics,’’ or long range intermolecular states.
Laser cooling and trapping are central to modern atomic physics. It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields and a number of Nobel prizes. Prior to the work presented in this thesis, laser cooling had not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for a wide range of applications. The first direct laser cooling of a molecule and further results we present here provide a new route to ultracold temperatures for molecules. In particular, these methods bridge the gap between ultracold temperatures and the approximately 1 kelvin temperatures attainable with directly cooled molecules (e.g. with cryogenic buffer gas cooling or decelerated supersonic beams). Using the carefully chosen molecule strontium monofluoride (SrF), decays to unwanted vibrational states are suppressed. Driving a transition with rotational quantum number R=1 to an excited state with R'=0 eliminates decays to unwanted rotational states. The dark ground-state Zeeman sublevels present in this specific scheme are remixed via a static magnetic field. Using three lasers for this scheme, a given molecule should undergo an average of approximately 100,000 photon absorption/emission cycles before being lost via unwanted decays. This number of cycles should be sufficient to load a magneto-optical trap (MOT) of molecules. In this thesis, we demonstrate transverse cooling of an SrF beam, in both Doppler and a Sisyphus-type cooling regimes. We also realize longitudinal slowing of an SrF beam. Finally, we detail current progress towards trapping SrF in a MOT. Ultimately, this technique should enable the production of large samples of molecules at ultracold temperatures for molecules chemically distinct from competing methods.
Abstract We demonstrate optical cycling and 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. Furthermore, we measure that repeated photon scattering via the A ← X transition is achievable at a rate of ∼ 1.6 × 1 0 6 photons s−1 and demonstrate interaction-time limited scattering of ∼ 200 photons by repumping the largest vibrational decay channel. We also demonstrate a sub-Doppler cooling technique, namely the magnetically assisted Sisyphus effect, and use it to cool the transverse temperature of a molecular beam of CaH. Using a standing wave of light, we lower the transverse temperature from 12.2(1.2) mK to 5.7(1.1) mK. We compare these results to a model that uses 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.
Only bosonic molecular species have been directly laser cooled to date, primarily due to an abundance of bosonic isotopes in nature and to their simpler hyperfine structure. Fermionic molecules provide new opportunities for ultracold chemistry, quantum simulation, and precision measurements. Here we report direct laser cooling of a fermionic molecular isotopologue, calcium monodeuteride (CaD). With a nuclear spin I = 1 , only 5 hyperfine states need to be addressed for rotational closure in optical cycling. These hyperfine states are unresolved for typical experimental linewidths. We present a method for efficiently producing alkaline-earth metal hydrides and deuterides. We demonstrate rotational closure and show magnetically assisted Sisyphus cooling in one dimension for a beam of CaD molecules. Our results indicate that the experimental complexity for laser cooling CaD is similar to that of calcium monohydride (CaH). Laser cooling of CaD is a promising first step for production of ultracold and trapped atomic deuterium. Published by the American Physical Society 2024
Abstract The extension of laser cooling and trapping techniques from atoms to molecules is currently the subject of intense and growing interest. Molecular laser cooling and trapping offers a general technique applicable to a variety of molecules with different properties and internal structures and is well-suited to the growing list of proposed applications for ultracold molecules. The recent development of optical cycling schemes for specific molecular species now allow each molecule to scatter up to ∼10 6 photons. This has proven sufficient for multiple groups to laser cool and slow molecular beams and, notably, capture molecules in magneto-optical traps (MOTs) and cool them to ultracold temperatures. MOTs are the workhorse technique for atomic physics in the ultracold regime and today’s molecular MOTs represent a powerful starting point for the study and manipulation of ultracold molecular gases. This Topical Review presents a summary of the progress made in this new and emerging field.
Despite the prominent role of laser cooling in modern atomic physics, with applications ranging from quantum sensors to high-precision spectroscopy and ultracold chemistry, laser cooling techniques are still limited to atoms with simple energy level structure and closed transitions that are accessible by currently available continuous wave (cw) laser sources. Two main obstacles prevent the extension of laser cooling techniques to a variety of atomic species and molecules. The first is associated with technical difficulties in creating cw laser light in the vacuum ultraviolet (VUV) spectral range - the absence of those laser sources prevents laser cooling of simple atoms such as hydrogen, deuterium, and antihydrogen. The second obstacle is associated with complex energy level structure of many atoms and almost all molecules - it permits decay of an excited state into a number of lower-lying states that can be widely separated in energy, which makes laser cooling of such species inefficient and experimentally very challenging.