No Arabic abstract
The decay of Rydberg-atom-ion molecules (RAIMs) due to non-adiabatic couplings between electronic potential energy surfaces is investigated. We employ the Born-Huang representation and perform numerical simulations using a Crank-Nicolson algorithm. The non-adiabatic lifetimes of rubidium RAIMs for the lowest ten vibrational states, $ u$, are computed for selected Rydberg principal quantum numbers, $n$. The non-adiabatic lifetimes are found to generally exceed the radiative Rydberg-atom lifetimes. We observe and explain a trend of the lifetimes as a function of $ u$ and $n$, and attribute irregularities to quantum interference arising from a shallow potential well in an inner potential surface. Our results will be useful for future spectroscopic studies of RAIMs.
We propose a novel type of Rydberg dimer, consisting of a Rydberg-state atom bound to a distant positive ion. The molecule is formed through long-range electric-multipole interaction between the Rydberg atom and the point-like ion. We present potential energy curves (PECs) that are asymptotically connected with Rydberg $nP$- or $nD$-states of rubidium or cesium. The PECs exhibit deep, long-range wells which support many vibrational states of Rydberg-atom-ion molecules (RAIMs). We consider photo-association of RAIMs in both the weak and the strong optical-coupling regimes between initial and Rydberg states of the neutral atom. Experimental considerations for the realization of RAIMs are discussed.
We report the creation of heteronuclear ultralong-range Rydberg-molecule dimers by excitation of minority $^{88}text{Sr}$ atoms to $5sns,^3S_1$ Rydberg states ($n=31-39$) in a dense background of $^{84}text{Sr}$. We observe an isotope shift of the $ u=0$ vibrational state over this range of $n$ and compare our measurements with a theoretical prediction and a simple scaling argument. With the appropriate choice of principal quantum number the isotope shift is sufficiently large to produce heteronuclear dimers with almost perfect fidelity. When the spectral selectivity is limited, we obtain a lower bound on the ratio of heteronuclear to homonuclear excitation probability of 30 to 1 by measuring the scaling of the molecular excitation rate with varying relative densities of $^{88}text{Sr}$ and $^{84}text{Sr}$ in the ultracold mixture.
In this work we discuss the rotational structure of Rydberg molecules. We calculate the complete wave function in a laboratory fixed frame and derive the transition matrix elements for the pho- toassociation of free ground state atoms. We discuss the implications for the excitation of different rotational states as well as the shape of the angular nuclear wave function. We find a rather com- plex shape and unintuitive coupling strengths, depending on the angular momenta coupling that are relevant for the states. This work explains the different steps to calculate the wave functions and the transition matrix elements in a way, that they can be directly transferred to different molecular states, atomic species or molecular coupling cases.
Polar molecules in selected quantum states can be guided, decelerated and trapped using electric fields created by microstructured electrodes on a chip. Here we explore how non-adiabatic transitions between levels in which the molecules are trapped and levels in which the molecules are not trapped can be suppressed. We use 12-CO and 13-CO (a 3-Pi(1), v=0) molecules, prepared in the upper Lambda-doublet component of the J=1 rotational level, and study the trap loss as a function of an offset magnetic field. The experimentally observed suppression (enhancement) of the non-adiabatic transitions for 12-CO (13-CO) with increasing magnetic field is quantitatively explained.
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.