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Precision test of statistical dynamics with state-to-state ultracold chemistry

Yu Liu, Ming-Guang Hu, Matthew A. Nichols, Dongzheng Yang, Daiqian Xie, Hua Guo, Kang-Kuen Ni

Published Jan 1, 2021• 76 citations
OpenAlex

Abstract

Abstract Chemical reactions represent a class of quantum problems that challenge both the current theoretical understanding and computational capabilities1. Reactions that occur at ultralow temperatures provide an ideal testing ground for quantum chemistry and scattering theories, because they can be experimentally studied with unprecedented control2, yet display dynamics that are highly complex3. Here we report the full product state distribution for the reaction 2KRb → K2 + Rb2. Ultracold preparation of the reactants allows us complete control over their initial quantum degrees of freedom, whereas state-resolved, coincident detection of both products enables the probability of scattering into each of the 57 allowed rotational state-pairs to be measured. Our results show an overall agreement with a state-counting model based on statistical theory4–6, but also reveal several deviating state-pairs. In particular, we observe a strong suppression of population in the state-pair closest to the exoergicity limit as a result of the long-range potential inhibiting the escape of products. The completeness of our measurements provides a benchmark for quantum dynamics calculations beyond the current state of the art.

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Rapid progress in atomic, molecular, and optical (AMO) physics techniques enabled the creation of ultracold samples of molecular species and opened opportunities to explore chemistry in the ultralow temperature regime. In particular, both the external and internal quantum degrees of freedom of the reactant atoms and molecules are controlled, allowing studies that explored the role of the long-range potential in ultracold reactions. The kinetics of these reactions have typically been determined using the loss of reactants as proxies. To extend such studies into the short-range, we developed an experimental apparatus that combines the production of quantum-state-selected ultracold KRb molecules with ion mass and kinetic energy spectrometry, and directly observed KRb + KRb reaction intermediates and products [M.-G. Hu and Y. Liu, et al., Science, 2019, 366, 1111]. Here, we present the apparatus in detail. For future studies that aim for detecting the quantum states of the reaction products, we demonstrate a photodissociation based scheme to calibrate the ion kinetic energy spectrometer at low energies.

arXiv:1912.12741•Physical Chemistry Chemical Physics•Jan 1, 2020•23 citations
Abstract Chemical reactions represent a class of quantum problems that challenge both the current theoretical understanding and computational capabilities1. Reactions that occur at ultralow temperatures provide an ideal testing ground for quantum chemistry and scattering theories, because they can be experimentally studied with unprecedented control2, yet display dynamics that are highly complex3. Here we report the full product state distribution for the reaction 2KRb → K2 + Rb2. Ultracold preparation of the reactants allows us complete control over their initial quantum degrees of freedom, whereas state-resolved, coincident detection of both products enables the probability of scattering into each of the 57 allowed rotational state-pairs to be measured. Our results show an overall agreement with a state-counting model based on statistical theory4–6, but also reveal several deviating state-pairs. In particular, we observe a strong suppression of population in the state-pair closest to the exoergicity limit as a result of the long-range potential inhibiting the escape of products. The completeness of our measurements provides a benchmark for quantum dynamics calculations beyond the current state of the art.
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.
Studying ultracold chemical reactions with quantum state resolution reveals details of the reaction processes, especially with single quantum state preparation of the reactants and state-selective detection of reaction products. In this thesis, we investigate two main processes: KRb + KRb → K2 + Rb2 reactions, and Rb and KRb atom-molecule collisions. In the KRb bimolecular reaction, we demonstrate the preservation of quantum coherence in bimolecular reactions for the first time, which is surprising in a reaction considered to be largely chaotic. Additionally, we proposed a coherent control scheme to manipulate product yields across different product channels. These results represent a critical step toward probing quantum coherence and entanglement in the chemical reaction. In atom-molecule collisions between Rb and KRb, we discovered an exceptionally long-lived intermediate complex, KRb2, which can be photo-excited by trapping light. The observed complex lifetime was orders of magnitude longer than theoretical predictions, underscoring the limitations of the current theory. We further explored the dependence of complex lifetimes on the initial quantum states and external electric and magnetic fields, providing additional experimental benchmarks to guide future theoretical work. Separately, we found that inelastic collisions between hyperfine-excited Rb atoms and KRb molecules can lead to rotation excitation of KRb post-collision. By probing the product state distribution, the result suggests that mechanical angular momentum is coupled to the spins. Such couplings are too weak in the current theory models to explain the result. Moreover, our result contradicts state-of-the-art coupled-channel calculations. These suggest that some subtle effects, such as molecular vibration and conical intersections, play a critical role in the reaction dynamics. The final piece of the thesis describes the observation of resonant interaction between a Rydberg atom and an ensemble of polar molecules. Such hybrid quantum systems have been proposed for a wide range of applications. Our work provides an experimental demonstration of resonant dipolar interactions between Rydberg atoms and ultracold polar molecules, paving the way for the realization of hybrid systems for quantum computation and simulation.
Coherent superpositions and entanglement are hallmarks of quantum mechanics, but they are fragile and can easily be perturbed by their environment. Selected isolated physical systems can maintain coherence and generate entanglement using well-controlled interactions. Chemical reactions, where bonds break and form, are highly dynamic quantum processes. A fundamental question is whether coherence can be preserved in chemical reactions and then harnessed to generate entangled products. Here we investigate this question by studying the 2KRb →\rightarrow→ K2_22​ + Rb2_22​ reaction at 500 nK, focusing on the the nuclear spin degrees of freedom. We prepare the initial nuclear spins in KRb in an entangled state and characterize the preserved coherence in nuclear spin wavefunction after the reaction. The data are consistent with full coherence at the end of the reaction. This suggests that entanglement can be prepared within the reactants, followed by a chemical reaction that produces separate, entangled molecules. We additionally demonstrate control of the reaction product state distribution by deliberately decohering the reactants.
A full-dimensional global potential energy surface (PES) for the KRb + KRb → K 2 Rb 2 * → K 2 + Rb 2 reaction is reported based on high-level ab initio calculations. The short-range part of the PES is fit with the permutationally invariant polynomial-neural network method, while the long-range parts of the PES in both the reactant and product asymptotes are represented by an asymptotically correct form. The long- and short-range parts are connected with intermediate-range parts to make them smooth. Within a statistical quantum model, this PES reproduces both the measured loss rates of ultracold KRb molecules and the K 2 and Rb 2 product state distributions, underscoring the important role of tunneling in ultracold chemistry. The PES also correctly predicts the lifetime of the K 2 Rb 2 * intermediate complex within the Rice–Ramsperger–Kassel–Marcus limit. It thus provides a reliable platform for future dynamical studies of the prototypical reaction.
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.
Rapid progress in atomic, molecular, and optical (AMO) physics techniques enabled the creation of ultracold samples of molecular species and opened opportunities to explore chemistry in the ultralow temperature regime. In particular, both the external and internal quantum degrees of freedom of the reactant atoms and molecules are controlled, allowing studies that explored the role of the long-range potential in ultracold reactions. The kinetics of these reactions have typically been determined using the loss of reactants as proxies. To extend such studies into the short-range, we developed an experimental apparatus that combines the production of quantum-state-selected ultracold KRb molecules with ion mass and kinetic energy spectrometry, and directly observed KRb + KRb reaction intermediates and products [M.-G. Hu and Y. Liu, et al., Science, 2019, 366, 1111]. Here, we present the apparatus in detail. For future studies that aim for detecting the quantum states of the reaction products, we demonstrate a photodissociation based scheme to calibrate the ion kinetic energy spectrometer at low energies.