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arXiv:2005.07861 · Science Advances

Universal relations for ultracold reactive molecules

Mingyuan He, Chenwei Lv, Hai‐Qing Lin, Qi Zhou

Published Dec 18, 2020• 31 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1126/sciadv.abd4699

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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.
Abstract Recent experimental developments have allowed physicists to freeze molecules' motion down to an ultracold temperature regime where quantum effects become profound. Furthermore, each molecule can be precisely prepared at chosen internal states and the mutual interactions between molecules are also highly tunable. As such, ultracold molecules have emerged as a powerful platform in multiple disciplines across physics and chemistry. Meanwhile, a grand challenge exists as to how losses of molecules depend on a quantum many‐body environment. In this article, the recent experimental and theoretical progress of exploring losses of ultracold molecules is reviewed. Since the conventional theoretical scheme of treating isolated pairs of molecules is no longer applicable to the quantum degenerate regime that has been reached in recent experiments, an alternative framework of universal relations between two‐body losses and many‐body correlations has been established. Regardless of microscopic parameters ranging from the temperature and the particle number to the interaction strength, these universal relations always hold. This approach unfolds a simple universality behind complex loss processes of many‐body systems and provides physicists and chemists with a new tool to explore ultracold molecules.
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.
Ultracold molecules offer unprecedented opportunities for the controlled interrogation of molecular events, including chemical reactivity in the ultimate quantum regime. The proliferation of methods to create, cool, and confine them has allowed the investigation of a diverse array of molecular systems and chemical reactions at temperatures where only a single partial wave contributes. Here we present a brief account of recent progress on the experimental and theoretical fronts on cold and ultracold molecules and the opportunities and challenges they provide for a fundamental understanding of bimolecular chemical reaction dynamics.
Physical systems in reduced dimensions exhibit intriguing properties. For instance, the dependences of two-body and many-body physics on scattering lengths are distinct from their counterparts in three dimensions. Whereas many studies of ultracold atoms and molecules in reduced dimensions have been focusing on closed systems, two-body losses may occur in such systems. Here, we show that the two-body inelastic loss rate in reduced dimensions can be expressed in universal relations that are governed by contacts. These universal relations correlate the two-body decay rate with other physical observables at zero and finite temperatures and generic interaction strengths. Our results will provide experimentalists with a new protocol to study inelastic scatterings in both few- and many-body systems in reduced dimensions.
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.
We propose a platform for observing and controlling the interactions between atomic ions and a quantum gas of polar molecules in the ultracold regime. This approach is based on the combination of several recently developed methods in two so-far complementary research domains: ion-atom collisions and studies of ultracold polar molecules. In contrast to collisions between ions and ground-state atoms, which are dominated by losses due to three-body recombination (TBR) already at densities far below those typical for quantum degenerate ensembles, our proposal makes use of polar molecules, their rich level structure, and sensitivity to electric fields to design effective interaction potentials where ion-neutral TBR losses and molecule-molecule losses due to sticky collisions could be strongly suppressed. This may open a broad range of applications including precise control of collisional properties in molecular ensembles using ions, quantum simulations, and cold quantum chemistry between polyatomic molecules.