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arXiv:1505.03443 · Physical Review Letters

Energetics and Control of Ultracold Isotope-Exchange Reactions between Heteronuclear Dimers in External Fields

Michał Tomza

Published Aug 6, 2015• 32 citations
arXivHTMLPDF

Abstract

We show that isotope-exchange reactions between ground-state alkali-metal, alkaline-earth-metal, and lanthanide heteronuclear dimers consisting of two isotopes of the same atom are exothermic with an energy change in the range of 1-8000 MHz, thus resulting in cold or ultracold products. For these chemical reactions, there are only one rovibrational and at most several hyperfine possible product states. The number and energetics of open and closed reactive channels can be controlled by the laser and magnetic fields. We suggest a laser-induced isotope- and state-selective Stark shift control to tune the exothermic isotope-exchange reactions to become endothermic, thus providing the ground for testing models of the chemical reactivity. The present proposal opens the way for studying the state-to-state dynamics of ultracold chemical reactions beyond the universal limit with a meaningful control over the quantum states of both reactants and products.

DOI
10.1103/physrevlett.115.063201

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We show that isotope-exchange reactions between ground-state alkali-metal, alkaline-earth-metal, and lanthanide heteronuclear dimers consisting of two isotopes of the same atom are exothermic with an energy change in the range of 1-8000 MHz, thus resulting in cold or ultracold products. For these chemical reactions, there are only one rovibrational and at most several hyperfine possible product states. The number and energetics of open and closed reactive channels can be controlled by the laser and magnetic fields. We suggest a laser-induced isotope- and state-selective Stark shift control to tune the exothermic isotope-exchange reactions to become endothermic, thus providing the ground for testing models of the chemical reactivity. The present proposal opens the way for studying the state-to-state dynamics of ultracold chemical reactions beyond the universal limit with a meaningful control over the quantum states of both reactants and products.
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.
We consider ultracold, chemically reactive scattering collisions of the diatomic molecules KRb. When two such molecules collide in an ultracold gas, we find that they are energetically forbidden from reacting to form the trimer species K2Rb{\mathrm{K}}_{2}\mathrm{Rb}K2​Rb or Rb2K{\mathrm{Rb}}_{2}\mathrm{K}Rb2​K, and hence can only react via the bond-swapping reaction $2\mathrm{KRb}\ensuremath{\rightarrow}{\mathrm{K}}_{2}+{\mathrm{Rb}}_{2}$. Moreover, the tiny energy released in this reaction can in principle be set to zero by applying electric or microwave fields, implying a means of controlling the available reaction channels in a chemical reaction.
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We consider ultracold collisions of ground-state heteronuclear alkali-metal dimers that are susceptible to four-center chemical reactions $2AB\ensuremath{\rightarrow}{A}_{2}+{B}_{2}$ even at submicrokelvin temperatures. These reactions depend strongly on species, temperature, electric field, and confinement in an optical lattice. We calculate ab initio van der Waals coefficients for these interactions and use a quantum formalism to study the scattering properties of such molecules under an external electric field and optical lattice. We also apply a quantum threshold model to explore the dependence of reaction rates on the various parameters. We find that, among the heteronuclear alkali-metal fermionic species, LiNa is the least reactive, whereas LiCs is the most reactive. For the bosonic species, LiK is the most reactive in zero field, but all species considered, LiNa, LiK, LiRb, LiCs, and KRb, share a universal reaction rate once a sufficiently high electric field is applied. For indistinguishable bosons, the inelastic/reactive rate increases as d2{d}^{2}d2 in the quantum regime, where ddd is the dipole moment induced by the electric field. This is a weaker power-law dependence than for indistinguishable fermions, for which the rate behaves as d6{d}^{6}d6.
This paper develops a theoretical methodology to describe ultracold atom-diatom chemical reactions without a barrier in the presence of external magnetic fields and hyperfine interactions. The authors apply their method to the chemical reaction Li + CaH -> LiH + Ca and show good agreement with previous experimental work, as well as uncover the possibility of controlling ultracold barrierless chemical reactions by tuning selected hyperfine states of the reactants with an external magnetic field.