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arXiv:2103.00510 · Physical Review Letters

Probing Photoinduced Two-Body Loss of Ultracold Nonreactive Bosonic Na 23 Rb 87 and Na 23 K 39 Molecules

Philipp Gersema, Kai K. Voges, Mara Meyer zum Alten Borgloh, Leon Koch, Torsten Hartmann, Alessandro Zenesini, Silke Ospelkaus, Junyu Lin, J. He, Dajun Wang

Published Oct 11, 2021• 71 citations
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Abstract

We probe photoinduced loss for chemically stable bosonic ^{23}Na^{87}Rb and ^{23}Na^{39}K molecules in chopped optical dipole traps, where the molecules spend a significant time in the dark. We expect the effective two-body decay to be significantly suppressed due to the small expected complex lifetimes of about 13 and 6 μs for ^{23}Na^{87}Rb and ^{23}Na^{39}K, respectively. However, instead we do not observe any suppression of the two-body loss in parameter ranges where large loss suppressions are expected. We believe these unexpected results are most probably due to drastic underestimation of the complex lifetime by at least 1-2 orders of magnitude.

DOI
10.1103/physrevlett.127.163401

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We probe photoinduced loss for chemically stable bosonic ^{23}Na^{87}Rb and ^{23}Na^{39}K molecules in chopped optical dipole traps, where the molecules spend a significant time in the dark. We expect the effective two-body decay to be significantly suppressed due to the small expected complex lifetimes of about 13 and 6 μs for ^{23}Na^{87}Rb and ^{23}Na^{39}K, respectively. However, instead we do not observe any suppression of the two-body loss in parameter ranges where large loss suppressions are expected. We believe these unexpected results are most probably due to drastic underestimation of the complex lifetime by at least 1-2 orders of magnitude.
We show that the lifetime of ultracold ground-state ^{87}Rb^{133}Cs molecules in an optical trap is limited by fast optical excitation of long-lived two-body collision complexes. We partially suppress this loss mechanism by applying square-wave modulation to the trap intensity, such that the molecules spend 75% of each modulation cycle in the dark. By varying the modulation frequency, we show that the lifetime of the collision complex is 0.53±0.06 ms in the dark. We find that the rate of optical excitation of the collision complex is 3_{-2}^{+4}×10^{3} W^{-1} cm^{2} s^{-1} for λ=1550 nm, leading to a lifetime of <100 ns for typical trap intensities. These results explain the two-body loss observed in experiments on nonreactive bialkali molecules.
The lifetime of nonreactive ultracold bialkali gases was conjectured to be limited by sticky collisions amplifying three-body loss. We show that the sticking times were previously overestimated and do not support this hypothesis. We find that electronic excitation of NaK+NaK collision complexes by the trapping laser leads to the experimentally observed two-body loss. We calculate the excitation rate with a quasiclassical, statistical model employing ab initio potentials and transition dipole moments. Using longer laser wavelengths or repulsive box potentials may suppress the losses.
Abstract Understanding ultracold collisions involving molecules is of fundamental importance for current experiments, where inelastic collisions typically limit the lifetime of molecular ensembles in optical traps. Here we present a broad study of optically trapped ultracold RbCs molecules in collisions with one another, in reactive collisions with Rb atoms, and in nonreactive collisions with Cs atoms. For experiments with RbCs alone, we show that by modulating the intensity of the optical trap, such that the molecules spend 75% of each modulation cycle in the dark, we partially suppress collisional loss of the molecules. This is evidence for optical excitation of molecule pairs mediated via sticky collisions. We find that the suppression is less effective for molecules not prepared in the spin-stretched hyperfine ground state. This may be due either to longer lifetimes for complexes in the dark or to laser-free decay pathways. For atom–molecule mixtures, RbCs + Rb and RbCs + Cs, we demonstrate that the rate of collisional loss of molecules scales linearly with the density of atoms. This indicates that, in both cases, the loss of molecules is rate-limited by two-body atom–molecule processes. For both mixtures, we measure loss rates that are below the thermally averaged universal limit.
Understanding collisions between ultracold molecules is crucial for making stable molecular quantum gases and harnessing their rich internal degrees of freedom for quantum engineering. Transient complexes can strongly influence collisional physics, but in the ultracold regime, key aspects of their behavior have remained unknown. To explain experimentally observed loss of ground-state molecules from optical dipole traps, it was recently proposed that molecular complexes can be lost due to photoexcitation. By trapping molecules in a repulsive box potential using laser light near a narrow molecular transition, we are able to test this hypothesis with light intensities three orders of magnitude lower than what is typical in red-detuned dipole traps. This allows us to investigate light-induced collisional loss in a gas of nonreactive fermionic 23Na40K^{23}\mathrm{Na}^{40}\mathrm{K}23Na40K molecules. Even for the lowest intensities available in our experiment, our results are consistent with universal loss, meaning unit loss probability inside the short-range interaction potential. Our findings disagree by at least two orders of magnitude with latest theoretical predictions, showing that crucial aspects of molecular collisions are not yet understood and provide a benchmark for the development of new theories.
We propose a method to suppress the chemical reactions between ultracold bosonic ground-state ^{23}Na^{87}Rb molecules based on optical shielding. By applying a laser with a frequency blue-detuned from the transition between the lowest rovibrational level of the electronic ground state X^{1}Σ^{+}(v_{X}=0,j_{X}=0), and the long-lived excited level b^{3}Π_{0}(v_{b}=0,j_{b}=1), the long-range dipole-dipole interaction between the colliding molecules can be engineered, leading to a dramatic suppression of reactive and photoinduced inelastic collisions, for both linear and circular laser polarizations. We demonstrate that the spontaneous emission from b^{3}Π_{0}(v_{b}=0,j_{b}=1) does not deteriorate the shielding process. This opens the possibility for a strong increase of the lifetime of cold molecule traps and for an efficient evaporative cooling. We also anticipate that the proposed mechanism is valid for alkali-metal diatomics with sufficiently large dipole-dipole interactions.
Recent years have witnessed tremendous progress in creating and manipulating ground-state ultracold polar molecules.However, the two-body loss regardless of the chemical reactivities is still a hurdle for many future explorations.Here, we investigate the loss suppression of nonreactive bosonic 23 Na 87 Rb molecules with a circularly polarized microwave blue detuned to the rotational transition.We achieve suppression of the loss by 2 orders of magnitude with the lowest two-body loss rate coefficient reduced to 3 × 10 -12 cm 3 =s.Meanwhile, the elastic collision rate coefficient is increased to the 10 -8 cm 3 =s level.The large good-to-bad collision ratio has allowed us to carry out evaporative cooling of 23 Na 87 Rb with an efficiency of 1.7(2), increasing the phase-space density by a factor of 10.With further improvements, this technique holds great promises for creating a Bose-Einstein condensate of ultracold polar molecules.