Laser Scheme for Doppler Cooling of the Hydroxyl Cation (OH+^+)

We report on a cycling scheme for Doppler cooling of trapped OH$^+$ ions using transitions between the electronic ground state $X^3\Sigma^-$ and the first excited triplet state $A^3\Pi$. We have identified relevant transitions for photon cycling and repumping, have found that coupling into other electronic states is strongly suppressed, and have calculated the number of photon scatterings required to cool OH$^+$ to a temperature where Raman sideband cooling can take over. In contrast to the standard approach, where molecular ions are sympathetically cooled, our scheme does not require co-trapping of another species and opens the door to the creation of pure samples of cold molecular ions with potential applications in quantum information, quantum chemistry, and astrochemistry. The laser cooling scheme identified for OH$^+$ is efficient despite the absence of near-diagonal Franck-Condon factors, suggesting that broader classes of molecules and molecular ions are amenable to laser cooling than commonly assumed.Comment: 6 pages, 3 figure

Automated detection of laser cooling schemes for ultracold molecules

One of the demanding frontiers in ultracold science is identifying laser cooling schemes for complex atoms and molecules, out of their vast spectra of internal states. Motivated by a need to expand the set of available ultracold molecules for applications in fundamental physics, chemistry, astrochemistry, and quantum simulation, we propose and demonstrate an automated graph-based search approach for viable laser cooling schemes. The method is time efficient and the outcomes greatly surpass the results of manual searches used so far. We discover new laser cooling schemes for C$_2$, OH$^+$, CN, YO, and CO$_2$ that can be viewed as surprising or counterintuitive compared to previously identified laser cooling schemes. In addition, a central insight of this work is that the reinterpretation of quantum states and transitions between them as a graph can dramatically enhance our ability to identify new quantum control schemes for complex quantum systems. As such, this approach will also be applicable to complex atoms and, in fact, any complex many-body quantum system with a discrete spectrum of internal states.Comment: 10 pages and 5 figures in the main text + 11 pages and 7 figures in appendices. Comments and feedback are very welcome. Code is available at https://github.com/Shmoo137/Detection-Of-Laser-Cooled-Molecule

Laser cooling scheme for the carbon dimer (12C2)

We report on a scheme for laser cooling of 12 C 2 . We have calculated the branching ratios for cycling and repumping transitions and calculated the number of photon scatterings required to achieve deflection and laser cooling of a beam of C 2 molecules under realistic experimental conditions. Our results demonstrate that C 2 cooling using the Swan ( d 3 Π g ↔ a 3 Π u ) and so-called Duck ( d 3 Π g ↔ c 3 Σ + u ) bands is achievable via techniques similar to state-of-the-art molecular cooling experiments. The Phillips ( A 1 Π u ↔ X 1 Σ + g ) and Ballik-Ramsay ( b 3 Σ − g ↔ a 3 Π u ) bands offer the potential for narrow-line cooling. This work opens up a path to cooling of molecules with carbon-carbon bonds and may pave the way toward quantum control of organic molecules

Collisionally Stable Gas of Bosonic Dipolar Ground State Molecules

Stable ultracold ensembles of dipolar molecules hold great promise for many-body quantum physics, but high inelastic loss rates have been a long-standing challenge. Recently, it was shown that gases of fermionic molecules can be effectively stabilized through external fields. However, many quantum applications will benefit from molecular ensembles with bosonic statistics. Here, we stabilize a bosonic gas of strongly dipolar NaCs molecules against inelastic losses via microwave shielding, decreasing losses by more than a factor of 200 and reaching lifetimes on the scale of 1 second. We also measure high elastic scattering rates, a result of strong dipolar interactions, and observe the anisotropic nature of dipolar collisions. Finally, we demonstrate evaporative cooling of a bosonic molecular gas to a temperature of 36(5) nK, increasing its phase-space density by a factor of 20. This work is a critical step towards the creation of a Bose-Einstein condensate of dipolar molecules.Comment: 13 pages, 10 figure

Ultracold Gas of Dipolar NaCs Ground State Molecules

We report on the creation of bosonic NaCs molecules in their absolute rovibrational ground state via stimulated Raman adiabatic passage. We create ultracold gases with up to 22,000 dipolar NaCs molecules at a temperature of 300(50) nK and a peak density of $1.0(4) \times 10^{12}$ cm$^{-3}$. We demonstrate comprehensive quantum state control by preparing the molecules in a specific electronic, vibrational, rotational, and hyperfine state. Employing the tunability and strength of the permanent electric dipole moment of NaCs, we induce dipole moments of up to 2.6 D. Dipolar systems of NaCs molecules are uniquely suited to explore strongly interacting phases in dipolar quantum matter.Comment: 6 pages, 5 figure

Efficient Pathway to NaCs Ground State Molecules

We present a study of two-photon pathways for the transfer of NaCs molecules to their rovibrational ground state. Starting from NaCs Feshbach molecules, we perform bound-bound excited state spectroscopy in the wavelength range from 900~nm to 940~nm, covering more than 30 vibrational states of the c \, ^3\Sigma^+, b \, ^3\Pi, and B \, ^1\Pi electronic states. Analyzing the rotational substructure, we identify the highly mixed c \, ^3\Sigma^+_1 \, |v=22 \rangle \sim b \, ^3\Pi_1 \, | v=54\rangle state as an efficient bridge for stimulated Raman adiabatic passage (STIRAP). We demonstrate transfer into the NaCs ground state with an efficiency of up to 88(4)\%. Highly efficient transfer is critical for the realization of many-body quantum phases of strongly dipolar NaCs molecules and high fidelity detection of single molecules, for example, in spin physics experiments in optical lattices and quantum information experiments in optical tweezer arrays.Comment: 17 pages, 8 figure

A High Phase-Space Density Gas of NaCs Feshbach Molecules

We report on the creation of ultracold gases of bosonic Feshbach molecules of NaCs. The molecules are associated from overlapping gases of Na and Cs using a Feshbach resonance at 864.12(5) G. We characterize the Feshbach resonance using bound state spectroscopy, in conjunction with a coupled-channel calculation. By varying the temperature and atom numbers of the initial atomic mixtures, we demonstrate the association of NaCs gases over a wide dynamic range of molecule numbers and temperatures, reaching 70 nK for our coldest systems and a phase-space density (PSD) near 0.1. This is an important stepping-stone for the creation of degenerate gases of strongly dipolar NaCs molecules in their absolute ground state.Comment: 6 pages, 5 figures, supplemental materia

Reaching the Bose-Einstein Condensation of Dipolar Molecules: a Journey from Ultracold Atoms to Molecular Quantum Control

Achieving the quantum control of ever more complex systems has been a driving force of atomic, molecular, and optical physics. This goal has materialized in the harnessing of systems with increasingly rich structures and interactions: the more sophisticated the system, the more faceted and fascinating its application to fields as varied as quantum simulation, quantum information, many body physics, metrology, and quantum chemistry. One of the current frontiers of quantum control is ultracold dipolar molecules. They present rich internal structures and long-range, anisotropic dipole-dipole interactions which promise to revolutionize AMO physics, for example by realizing realistic Hamiltonians in quantum simulation, by providing a new platform for quantum information, and by achieving a novel kind of quantum liquid. Despite its promises, the full quantum control of dipolar molecules has been over a decade in the making. The difficulties in either directly laser cooling molecules or in collisionally stabilizing their bulk samples have been major roadblocks that have hampered the development of this quantum system. The realization of a Bose-Einstein condensate of dipolar molecules has been a particularly elusive milestone. In this thesis, I report on the first observation of this quantum state of matter. The work that brought us to this achievement parallels the historical evolution of AMO physics in the last thirty years. To reach a BEC of molecules, we initially constructed a dual species experiment capable of realizing the simultaneous Bose-Einstein condensation of atomic sodium (Na) and cesium (Cs). Individual BECs of sodium and cesium were first reported in 1995 and 2003 respectively, while our experiment was the first instance of their concurrent condensation. The study of the Na-Cs interatomic scattering properties in an homogeneous magnetic field showed us the path to the Feshbach association of loosely-bound sodium-cesium (NaCs) molecules, a technique first demonstrated in 2006 for heteronuclear molecules but never attempted on our species. Following the Feschbach association, we determined a novel pathway to the molecular electronic, vibrational and rotational ground state using STIRAP. From this point, we found ourselves at the forefront of the field: bulk samples of bosonic molecules such as NaCs had neither been stabilized against collisional losses nor evaporatively cooled. At first, we successfully applied a single-frequency microwave shielding approach to decrease in-bulk losses by a factor of 200 and reach lifetimes on the order of 2 s, allowing us to measure high elastic scattering rates and characterize their dipolar anisotropy. Moreover, we demonstrated the first evaporative cooling of a bosonic molecular gas by increasing its phase-spacedensity by a factor of 20 and reaching a temperature of 36(5) nK. Since this proved insufficient to achieve Bose-Einstein condensation due to unexpected three-body losses, we introduced an enhanced microwave shielding technique, double microwave shielding. This further decreased loss rates enabling efficient evaporative cooling of our sample to a long-lived Bose-Einstein condensate of dipolar molecules. This new double microwave shielding technique also allows the tunability of the strength of dipole-dipole interaction, establishing ultracold bosonic dipolar molecules as a new quantum liquid for the exploration of many body physics. In addition to the experimental work on dipolar NaCs, we have theoretically explored the field of direct molecular laser cooling. Our aim was twofold: we aimed to expand the category of molecules that can be laser cooled and to simplify the identification of laser cycling schemes. For the former goal, we lifted the widespread assumption that only molecules with diagonal Franck-Condon factors could be laser cooled. For the latter, we decided to employ publicly available repositories of molecular transitions. A second consequence of the use of these databases is that they contain data on molecules of interest to other scientific fields, further establishing direct laser cooling as a technique that could be of interest beyond AMO physics. Our work was successful in that we identified laser cycling schemes for C₂ and OH+. To simplify the determination of laser cycling schemes, we developed a graph-based algorithm form their identification starting from spectroscopic data

Laser Cooling Scheme for the Carbon Dimer (12^{12}C2_2)

We report on a scheme for laser cooling of $^{12}$C$_2$. We have calculated the branching ratios for cycling and repumping transitions and calculated the number of photon scatterings required to achieve deflection and laser cooling of a beam of $C_2$ molecules under realistic experimental conditions. Our results demonstrate that C$_2$ cooling using the Swan ($d^3\Pi_\text{g} \leftrightarrow a^3\Pi_\text{u}$) and Duck ($d^3\Pi_\text{g} \leftrightarrow c^3\Sigma_\text{u}^+$) bands is achievable via techniques similar to state-of-the-art molecular cooling experiments. The Phillips ($A^1\Pi_\text{u} \leftrightarrow X^1\Sigma_\text{g}^+$) and Ballik-Ramsay ($b^3\Sigma_\text{g}^- \leftrightarrow a^3\Pi_\text{u}$) bands offer the potential for narrow-line cooling. This work opens up a path to cooling of molecules with carbon-carbon bonds and may pave the way toward quantum control of organic molecules.Comment: 7 pages, 5 figure