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Register a new userPhoto-induced two-body loss of ultracold molecules
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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.
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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 $0.53pm0.06$ ms in the dark. We find that the rate of optical excitation of the collision complex is $3^{+4}_{-2}times10^{3}$ W$^{-1}$ cm$^2$ s$^{-1}$ for $lambda = 1550$ 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.
We probe photo-induced 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 largely suppressed in chopped traps due to the small expected complex lifetimes of about $13mu$s and $6mu$s for $^{23}$Na$^{87}$Rb and $^{23}$Na$^{39}$K respectively. However, instead we do observe near-universal loss even at the lowest chopping frequencies we can probe. Our data thus either suggest a so far unknown loss mechanism or a drastic underestimation of the complex lifetime by at least one to two orders of magnitude.
Femtochemistry techniques have been instrumental in accessing the short time scales necessary to probe transient intermediates in chemical reactions. Here we take the contrasting approach of prolonging the lifetime of an intermediate by preparing reactant molecules in their lowest ro-vibronic quantum state at ultralow temperatures, thereby drastically reducing the number of exit channels accessible upon their mutual collision. Using ionization spectroscopy and velocity-map imaging of a trapped gas of potassium-rubidium molecules at a temperature of 500~nK, we directly observe reactants, intermediates, and products of the reaction $^{40}$K$^{87}$Rb + $^{40}$K$^{87}$Rb $rightarrow$ K$_2$Rb$^*_2$ $rightarrow$ K$_2$ + Rb$_2$. Beyond observation of a long-lived energy-rich intermediate complex, this technique opens the door to further studies of quantum-state resolved reaction dynamics in the ultracold regime.
How does a chemical reaction proceed at ultralow temperatures? Can simple quantum mechanical rules such as quantum statistics, single scattering partial waves, and quantum threshold laws provide a clear understanding for the molecular reactivity under a vanishing collision energy? Starting with an optically trapped near quantum degenerate gas of polar $^{40}$K$^{87}$Rb molecules prepared in their absolute ground state, we report experimental evidence for exothermic atom-exchange chemical reactions. When these fermionic molecules are prepared in a single quantum state at a temperature of a few hundreds of nanoKelvins, we observe p-wave-dominated quantum threshold collisions arising from tunneling through an angular momentum barrier followed by a near-unity probability short-range chemical reaction. When these molecules are prepared in two different internal states or when molecules and atoms are brought together, the reaction rates are enhanced by a factor of 10 to 100 due to s-wave scattering, which does not have a centrifugal barrier. The measured rates agree with predicted universal loss rates related to the two-body van der Waals length.
We report the measurement of the anisotropic AC polarizability of ultracold polar $^{40}$K$^{87}$Rb molecules in the ground and first rotationally excited states. Theoretical analysis of the polarizability agrees well with experimental findings. Although the polarizability can vary by more than 30%, a magic angle between the laser polarization and the quantization axis is found where the polarizability of the $|N=0,m_N=0>$ and the $|N=1,m_N=0>$ states match. At this angle, rotational decoherence due to the mismatch in trapping potentials is eliminated, and we observe a sharp increase in the coherence time. This paves the way for precise spectroscopic measurements and coherent manipulations of rotational states as a tool in the creation and probing of novel quantum many-body states of polar molecules.
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