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arXiv:1407.4502 · Physical Review A

Statistical product distributions for ultracold reactions in external fields

Maykel Leonardo González-Martínez, Olivier Dulieu, P. Larrégaray, Laurent Bonnet

Published Nov 18, 2014• 33 citations
arXivHTMLPDF

Abstract

The main limitation of most ultracold chemistry studies to date is the lack of an analysis of reaction products. Here, we discuss a generally tractable, rigorous theoretical framework for computing statistical product-state distributions for ultracold reactions in external fields. We show that fields have two main effects on the products of a statistical reaction, by (1) modifying the product energy levels and thus potentially reshaping the product distributions and/or (2) adding or removing product states by changing the reaction exothermicity. By analyzing these effects and the strength of the formalism to distinguish between different reaction mechanisms in benchmark reactions involving $^{40}\mathrm{K}$ and $^{87}\mathrm{Rb}$ species, we argue that statistical predictions will help understanding product formation and control, and lead developments to realize the full potential of ultracold chemistry.

DOI
10.1103/physreva.90.052716

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Advances in atomic, molecular, and optical physics techniques allowed the cooling of simple molecules down to the ultracold regime ([Formula: see text]1 mK) and opened opportunities to study chemical reactions with unprecedented levels of control. This review covers recent developments in studying bimolecular chemistry at ultralow temperatures. We begin with a brief overview of methods for producing, manipulating, and detecting ultracold molecules. We then survey experimental works that exploit the controllability of ultracold molecules to probe and modify their long-range interactions. Further combining the use of physical chemistry techniques such as mass spectrometry and ion imaging significantly improved the detection of ultracold reactions and enabled explorations of their dynamics in the short range. We discuss a series of studies on the reaction KRb + KRb → K 2 + Rb 2 initiated below 1 μK, including the direct observation of a long-lived complex, the demonstration of product rotational state control via conserved nuclear spins, and a test of the statistical model using the complete quantum state distribution of the products.
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Fully understanding a chemical reaction on the quantum level is a long-standing goal in physics and chemistry. Experimental investigation of such state-to-state chemistry requires both the preparation of the reactants and the detection of the products in a quantum state resolved way, which has been a long term challenge. Using the high level control in the ultracold domain, we prepare a few-body quantum state of reactants and demonstrate state-to-state chemistry with unprecedented resolution. We present measurements and accompanying theoretical analysis for the recombination of three spin-polarized ultracold Rb atoms forming a weakly bound Rb2_22​ dimer. Detailed insights of the reaction process are obtained that suggest propensity rules for the distribution of reaction products. The scheme can readily be adapted to other species and opens a door to detailed investigations of inelastic or reactive processes in domains never before accessible.