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Physical Review A

Lowest quartet states of heteronuclear alkali-metal trimers

Pavel Soldán

Published Sep 2, 2010• 18 citations
Publisher

Abstract

We analyze three-body nonadditive interactions and characterize critical points on potential energy surfaces of the lowest ${A}_{2}B$ ($A,B=\mathrm{Li},\mathrm{Na},\mathrm{K},\mathrm{Rb},\mathrm{Cs}$) quartet states using high-level ab initio calculations. Our calculations indicate that near equilibrium geometries, large nonadditive effects are stabilizing the systems. We also show that trimer formation reactions are always energetically allowed even for low-lying rovibrational states of heteronuclear triplet-$\ensuremath{\Sigma}$ dimers.

DOI
10.1103/physreva.82.034701

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We analyze three-body nonadditive interactions and characterize critical points on potential energy surfaces of the lowest A2B{A}_{2}BA2​B (A,B=Li,Na,K,Rb,CsA,B=\mathrm{Li},\mathrm{Na},\mathrm{K},\mathrm{Rb},\mathrm{Cs}A,B=Li,Na,K,Rb,Cs) quartet states using high-level ab initio calculations. Our calculations indicate that near equilibrium geometries, large nonadditive effects are stabilizing the systems. We also show that trimer formation reactions are always energetically allowed even for low-lying rovibrational states of heteronuclear triplet-\ensuremathΣ\ensuremath{\Sigma}\ensuremathΣ dimers.
We investigate the energetics of reactions involving pairs of alkali-metal dimers. Atom exchange reactions to form homonuclear dimers are energetically allowed for some but not all of the heteronuclear dimers. We carry out high-level electronic structure calculations on the potential energy surfaces of all the heteronuclear alkali-metal trimers and show that trimer formation reactions are always energetically forbidden for low-lying singlet states of the dimers. The results have important implications for the stability of quantum gases of alkali-metal dimers.
Three-body nonadditive forces in systems of three spin-polarized alkali-metal atoms (Li, Na, K, Rb, and Cs) are investigated using high-level ab initio calculations. The nonadditive forces are found to be large, especially near the equilateral equilibrium geometries. For Li, they increase the three-atom potential well depth by a factor of 4 and reduce the equilibrium interatomic distance by 1.07A˚.1.07\mathrm{\AA{}}.1.07A˚. The nonadditive forces originate principally from chemical bonding arising from sp\mathrm{sp}sp mixing effects.
The electronic excitation spectra of all possible homo- and heteronuclear high-spin (quartet) trimers of K and Rb (KxRb(3-x), x=0...3) assembled on the surface of superfluid helium droplets, are measured in the spectral range from 10,600 to 17,400 cm(-1). A regular series of corresponding bands is observed, reflecting the similar electronic structure of all these trimers. For the assignment and separation of overlapping bands, we determine x directly, with mass-selected beam depletion, and indirectly with a V-type double-resonance scheme. The assignment is confirmed by high-level ab initio calculations of the electronic structure of the bare trimers. The level structure is rationalized in terms of harmonic-oscillator states of the three valence electrons in a quantum-dot-like confining potential. We predict that three should be a magic number for high-spin alkali clusters.
We show that the interaction of polar alkali-metal dimers in the quintet spin state leads to the formation of a deeply bound reaction complex. The reaction complex can decompose adiabatically into homonuclear alkali-metal dimers (for all molecules except KRb) and into alkali-metal trimers (for all molecules). We show that there are no barriers for these chemical reactions. This means that all alkali-metal dimers in the ${a}^{3}{\ensuremath{\Sigma}}^{+}$ state are chemically unstable at ultracold temperature, and the use of an optical lattice to segregate the molecules and suppress losses may be necessary. In addition, we calculate the minimum-energy path for the chemical reactions of alkali-metal hydrides. We find that the reaction of two molecules is accelerated by a strong attraction between the alkali-metal atoms, leading to a barrierless process that produces hydrogen atoms with large kinetic energy. We discuss the unique features of the chemical reactions of ultracold alkali-metal dimers in the ${a}^{3}{\ensuremath{\Sigma}}^{+}$ electronic state.