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Register a new userLifetimes of ultralong-range Rydberg molecules in vibrational ground and excited state
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Since their first experimental observation, ultralong-range Rydberg molecules consisting of a highly excited Rydberg atom and a ground state atom have attracted the interest in the field of ultracold chemistry. Especially the intriguing properties like size, polarizability and type of binding they inherit from the Rydberg atom are of interest. An open question in the field is the reduced lifetime of the molecules compared to the corresponding atomic Rydberg states. In this letter we present an experimental study on the lifetimes of the ^3Sigma (5s-35s) molecule in its vibrational ground state and in an excited state. We show that the lifetimes depends on the density of ground state atoms and that this can be described in the frame of a classical scattering between the molecules and ground state atoms. We also find that the excited molecular state has an even more reduced lifetime compared to the ground state which can be attributed to an inward penetration of the bound atomic pair due to imperfect quantum reflection that takes place in the special shape of the molecular potential.
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We predict that ultralong-range Rydberg bi-molecules form in collisions between polar molecules in cold and ultracold settings. The collision of $Lambda$-doublet nitric oxide (NO) with long-lived Rydberg NO($nf$, $ng$) molecules forms ultralong-range Rydberg bi-molecules with GHz energies and kilo-Debye permanent electric dipole moments. The Hamiltonian includes both the anisotropic charge-molecular dipole interaction and the electron-NO scattering. The rotational constant for the Rydberg bi-molecules is in the MHz range, allowing for microwave spectroscopy of rotational transitions in Rydberg bi-molecules. Considerable orientation of NO dipole can be achieved. The Rydberg molecules described here hold promise for studies of a special class of long-range bi-molecular interactions.
The lifetimes and decay channels of ultralong-range Rydberg molecules created in a dense BEC are examined by monitoring the time evolution of the Rydberg population using field ionization. Studies of molecules with values of principal quantum number, $n$, in the range $n=49$ to $n=72$ that contain tens to hundreds of ground state atoms within the Rydberg electron orbit show that their presence leads to marked changes in the field ionization characteristics. The Rydberg molecules have lifetimes of $sim1-5,mu$s, their destruction being attributed to two main processes: formation of Sr$^+_2$ ions through associative ionization, and dissociation induced through $L$-changing collisions. The observed loss rates are consistent with a reaction model that emphasizes the interaction between the Rydberg core ion and its nearest neighbor ground-state atom. The measured lifetimes place strict limits on the time scales over which studies involving Rydberg species in cold, dense atomic gases can be undertaken and limit the coherence times for such measurements.
We have calculated the isotropic $C_6$ coefficients characterizing the long-range van der Waals interaction between two identical heteronuclear alkali-metal diatomic molecules in the same arbitrary vibrational level of their ground electronic state $X^1Sigma^+$. We consider the ten species made up of $^7$Li, $^{23}$Na, $^{39}$K, $^{87}$Rb and $^{133}$Cs. Following our previous work [M.~Lepers textit{et.~al.}, Phys.~Rev.~A textbf{88}, 032709 (2013)] we use the sum-over-state formula inherent to the second-order perturbation theory, composed of the contributions from the transitions within the ground state levels, from the transition between ground-state and excited state levels, and from a crossed term. These calculations involve a combination of experimental and quantum-chemical data for potential energy curves and transition dipole moments. We also investigate the case where the two molecules are in different vibrational levels and we show that the Moelwyn-Hughes approximation is valid provided that it is applied for each of the three contributions to the sum-over-state formula. Our results are particularly relevant in the context of inelastic and reactive collisions between ultracold bialkali molecules, in deeply bound or in Feshbach levels.
Photoexcitation rates for creation of ultralong-range Rydberg molecules (ULRM) with 31$lesssim n lesssim41$ in both ground and excited vibrational levels in cold ($Tsim900$~nK) gases of polarized and unpolarized $^{87}$Sr are presented. The measured production rates of the $ u=0, 1$ and 2 vibrational levels reveal rather different $n$ dependences which are analyzed by evaluating the Franck-Condon factors associated with excitation of the different vibrational levels and molecular rotational states. In particular, for gases of spin-polarized fermions, only Rydberg dimers with odd rotational quantum numbers are excited due to the requirement that their wavefunctions be anti-symmetric with respect to exchange. The data also demonstrate that measurements of the formation of vibrationally-excited $ u=1$ molecules can furnish a probe of pair correlations over intermediate length scales extending from $sim20$~nm to greater than 250~nm.
The lifetimes of the lower-lying vibrational states of ultralong-range strontium Rydberg molecules comprising one ground-state 5s2 1S0 atom and one Rydberg atom in the 5s38s 3S1 state are reported. The molecules are created in an ultracold gas held in an optical dipole trap and their numbers determined using field ionization, the product electrons being detected by a microchannel plate. The measurements show that, in marked contrast to earlier measurements involving rubidium Rydberg molecules, the lifetimes of the low-lying molecular vibrational states are very similar to those of the parent Rydberg atoms. This results because the strong p-wave resonance in low-energy electronrubidium scattering, which plays an important role in determining the molecular lifetimes, is not present for strontium. The absence of this resonance offers advantages for experiments involving strontium Rydberg atoms as impurities in quantum gases and for testing theories of molecular formation and decay.
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