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arXiv:1909.00777 · Physical Review Letters

Hyperfine Magnetic Substate Resolved State-to-State Chemistry

Joschka Wolf, Markus Deiß, Johannes Hecker Denschlag

Published Dec 19, 2019• 14 citations
arXivHTMLPDF

Abstract

We extend state-to-state chemistry to a realm where besides vibrational, rotational, and hyperfine quantum states magnetic quantum numbers are also resolved. For this, we make use of the Zeeman effect, which energetically splits levels of different magnetic quantum numbers. The chemical reaction which we choose to study is three-body recombination in an ultracold quantum gas of ^{87}Rb atoms forming weakly bound Rb_{2} molecules. Here, we find the propensity rule that the total m_{F} quantum number of the two atoms forming the molecule is conserved. Our method can be employed for many other reactions and inelastic collisions and will allow for novel insights into few-body processes.

DOI
10.1103/physrevlett.123.253401

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We extend state-to-state chemistry to a realm where besides vibrational, rotational, and hyperfine quantum states magnetic quantum numbers are also resolved. For this, we make use of the Zeeman effect, which energetically splits levels of different magnetic quantum numbers. The chemical reaction which we choose to study is three-body recombination in an ultracold quantum gas of ^{87}Rb atoms forming weakly bound Rb_{2} molecules. Here, we find the propensity rule that the total m_{F} quantum number of the two atoms forming the molecule is conserved. Our method can be employed for many other reactions and inelastic collisions and will allow for novel insights into few-body processes.
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.
In this thesis, I report on experiments on the detection and the production of molecules in an ultracold atomic gas. These experiments can be divided into two main parts. The first part is about state-to-state experiments where chemical reaction products are detected in a quantum state resolved way. The second part is about Rydberg molecules. In the first part, I investigate three-body recombination of neutral Rb, which is a chemical reaction leading to the formation of Rb2 dimers. The quantum states of the three-body recombination product molecules are investigated for different initial atomic samples. This includes different atomic hyperfine states and different atomic magnetic sub states that are prepared. The molecular reaction product is state-selectively ionized and detected afterwards. The detection scheme resolves total electron spin, the vibrational, the rotational, the hyperfine and even the magnetic sub state of the product molecules. We determine the population distribution of the product molecules covering the majority of all produced molecules. The insights gained enable us to formulate various propensity rules for the three-body recombination of 87Rb. The second part is furthermore divided into two parts: the investigations of charged and uncharged Rydberg molecules. The investigations of charged Rydberg molecules are the first step towards one of our goals, the photoassociation of BaRb+ or Rb2+ Rydberg molecules. For this work, we have developed a novel method to measure Stark spectra within an ion trap. In experiments with neutral Rb2 Rydberg molecules we observe a complex spin structure of the molecular states. The substructure emerges partially due to a novel, recently predicted spin-orbit interaction of the Rydberg electron and the perturber atom, which we prove for the first time.
molecule. The measured product distribution covers about 90% of the final products, and we are able to discriminate between product states with a level splitting as small as 20 megahertz multiplied by Planck's constant. Furthermore, we formulate propensity rules for the distribution of products, and we develop a theoretical model that predicts many of our experimental observations. The scheme can readily be adapted to other species and opens a door to detailed investigations of inelastic or reactive processes.
We explore the physical origin and the general validity of a propensity rule for the conservation of the hyperfine spin state in three-body recombination. This rule was recently discovered for the special case of ^{87}Rb with its nearly equal singlet and triplet scattering lengths. Here, we test the propensity rule for ^{85}Rb for which the scattering properties are very different from ^{87}Rb. The Rb_{2} molecular product distribution is mapped out in a state-to-state fashion using resonance-enhanced multiphoton ionization detection schemes which fully cover all possible molecular spin states. Interestingly, for the experimentally investigated range of binding energies from zero to ∼13 GHz×h we observe that the spin-conservation propensity rule also holds for ^{85}Rb. From these observations and a theoretical analysis we derive an understanding for the conservation of the hyperfine spin state. We identify several criteria to judge whether the propensity rule will also hold for other elements and collision channels.
We employ collisions of individual atomic cesium (Cs) impurities with an ultracold rubidium (Rb) gas to probe atomic interaction with hyperfine- and Zeeman-state sensitivity. Controlling the Rb bath's internal state yields access to novel phenomena observed in interatomic spin exchange. These can be tailored at ultralow energies, owing to the excellent experimental control over all relevant energy scales. First, detecting spin-exchange dynamics in the Cs hyperfine-state manifold, we resolve a series of previously unreported Feshbach resonances at magnetic fields below 300 mG, separated by energies as low as h×15 kHz. The series originates from a coupling to molecular states with binding energies below h×1 kHz and wave function extensions in the micrometer range. Second, at magnetic fields below ≈100 mG, we observe the emergence of a new reaction path for alkali atoms, where in a single, direct collision between two atoms two quanta of angular momentum can be transferred. This path originates from the hyperfine analog of dipolar spin-spin relaxation. Our work yields control of subtle ultralow-energy features of atomic collision dynamics, opening new routes for advanced state-to-state chemistry, for controlling spin exchange in quantum many-body systems for solid-state simulations, or for determination of high-precision molecular potentials.
We demonstrate that it is possible to efficiently control ultracold chemical reactions of alkali-metal atoms colliding with open-shell alkali-metal dimers in their metastable triplet states by choosing the internal hyperfine and rovibrational states of the reactants as well as by inducing magnetic Feshbach resonances with an external magnetic field. We base these conclusions on coupled-channel statistical calculations that include the effects of hyperfine contact and magnetic-field-induced Zeeman interactions on ultracold chemical reactions of hyperfine-resolved ground-state Na and the triplet NaLi(a^{3}Σ^{+}) producing singlet Na_{2}(^{1}Σ_{g}^{+}) and a Li atom. We find that the reaction rates are sensitive to the initial hyperfine states of the reactants. The chemical reaction of fully spin-polarized, high-spin states of rotationless NaLi(a^{3}Σ^{+},v=0,N=0) molecules with fully spin-polarized Na is suppressed by a factor of 10-100 compared to that of unpolarized reactants. We interpret these findings within the adiabatic state model, which treats the reaction as a sequence of nonadiabatic transitions between the initial nonreactive high-spin state and the final low-spin states of the reaction complex. In addition, we show that magnetic Feshbach resonances can similarly change reaction rate coefficients by several orders of magnitude. Some of these resonances are due to resonant trimer bound states dissociating to the N=2 rotational state of NaLi(a^{3}Σ^{+},v=0) and would thus exist in systems without hyperfine interactions.