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arXiv:2008.05904 · Physical Review A

Exploring chemical reactions in a quantum degenerate gas of polar molecules via complex formation

Peiru He, Thomas Bilitewski, Chris H. Greene, Ana María Rey

Published Dec 18, 2020• 9 citations

Abstract

A recent experiment [L. De Marco, G. Valtolina, K. Matsuda, W. G. Tobias, J. P. Covey, and J. Ye, A degenerate Fermi gas of polar molecules, Science 363, 853 (2019)] reported for the first time the preparation of a Fermi degenerate gas of polar molecules and observed a suppression of their chemical reaction rate compared to the one expected from a treatment assuming classical Maxwell-Boltzmann statistics. While it was hypothesized that the suppression in the ultracold regime had its roots in the Fermi statistics of the molecules, this argument is inconsistent with the fact that the Fermi pressure should set a lower bound for the chemical reaction rate. Here we develop a simple model of chemical reactions that occur via the formation and decay of molecular complexes. We indeed find that pure two-body molecule losses are unable to explain the observed suppression. Instead we extend our description beyond two-body physics by including multibody complex-molecule interactions. Although our model is able to quantitatively reproduce recent experimental observations, it requires parameters physically unlikely for direct microscopic interactions. The underlying processes, however, might emerge effectively from many-body or medium effects. A detailed understanding of the direct microscopic mechanisms responsible for these higher-order interaction processes is therefore still pending.

DOI: 10.1103/physreva.102.063322

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The realization of ultracold polar molecules in laboratories has pushed physics and chemistry to new realms. In particular, these polar molecules offer scientists unprecedented opportunities to explore chemical reactions in the ultracold regime where quantum effects become profound. However, a key question about how two-body losses depend on quantum correlations in interacting many-body systems remains open so far. Here, we present a number of universal relations that directly connect two-body losses to other physical observables, including the momentum distribution and density correlation functions. These relations, which are valid for arbitrary microscopic parameters, such as the particle number, the temperature, and the interaction strength, unfold the critical role of contacts, a fundamental quantity of dilute quantum systems, in determining the reaction rate of quantum reactive molecules in a many-body environment. Our work opens the door to an unexplored area intertwining quantum chemistry; atomic, molecular, and optical physics; and condensed matter physics.

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We present a simple theoretical model used for describing the suppressing reactivity of an ultracold Fermi molecular gas in a degenerate regime via the statistical potential. The statistical potential originates from the symmetry properties of the wave function of identical particles, and is derived by using the density matrix. We use our theoretical model to well reproduce recent experimental results of a potassium-rubidium molecule gas in the deep quantum degenerate regime reported by De Marco et al. [Science 363, 853 (2019)]. The suppression of the chemical reaction rate observed in the experiment is quantitatively reproduced by using the

p

-wave scattering volume as an adjusting parameter. The strength of spatial correlation can be intuitively captured by the statistical potential.

Ultracold polar molecular gases promise new directions and exciting applications in collisions and chemical reactions at ultralow energies, precision measurements, novel quantum phase transitions, and quantum information science. Here we briefly discuss key experimental requirements for observing strong dipole-dipole interactions in an ultracold dipolar gas of molecules. We then survey current experimental progress in the field with a focus on our recent work creating a near quantum degenerate gas of KRb polar molecules [Ni et al., Science, 2008, 322, 231].

Ultracold polar molecular quantum gases promise to open new research directions ranging from the study of ultra-cold chemistry, precision measurements to novel quantum phase transitions. Based on the preparation of high-phase space density gases of polar KRb molecules [1–3], I will discuss the control of dipolar collisions and chemical reactions of polar molecules in a regime where quantum statistics, single scattering partial waves, and quantum threshold laws play a dominant role [4]. In particular, I will point out the crucial role of electric dipole-dipole interactions [5] and external confinement [6] in determining the chemical reaction rate. Finally, I will discuss prospects of reaching quantum degeneracy in bialkali samples of polar molecules and prospects for these systems as novel dipolar quantum many-body systems.