Vibronic transitions to the 21A2(3py <-- pi) Rydberg state of CH2N2, CD2N2, and CHDN2 were recorded by 2 + 1 REMPI spectroscopy, and kinetic energy distributions (eKE) of photoelectrons from ionization of selected vibronic levels were determined by velocity map imaging. Normal-mode frequencies were obtained for the 21A2(3py) Rydberg state and for the cation. Mixed levels of the 21A2(3py) and 21...

We propose to apply atom-chip techniques to the trapping of a single atom in a circular Rydberg state. The small size of microfabricated structures will allow for trap geometries with microwave cut-off frequencies high enough to inhibit the spontaneous emission of the Rydberg atom, paving the way to complete control of both external and internal degrees of freedom over very long times. Trapping...

Full quantum-state resolved scattering of a highly excited Rydberg H atom with D2 has been carried out using the Rydberg H-atom time-of-flight method. A detailed analysis of the experimental results shows that both inelastic and reactive scatterings are significant in the Hn-D2 collisions, and nuclear spin is conserved in the inelastic scattering process. The differential cross sections for the...

Double resonance excitation of vibrationally autoionizing states of the water molecule has been performed for the first time. Tunable, coherent vacuum ultraviolet light was used to excite selected rotational levels of the C̃ B1 state with one quantum of symmetric stretch vibrational energy ~100!, from which ~100! Rydberg states were excited with a second dye laser. The Rydberg character of the C̃...

Realization of distributed quantum systems requires fast generation and long-term storage of quantum states. Ground atomic states enable memories with storage times in the range of a minute, however their relatively weak interactions do not allow fast creation of non-classical collective states. Rydberg atomic systems feature fast preparation of singly excited collective states and their effici...

During the funding period, our primary research efforts have focused on the exploration and control of coherent time-dependent electronic interactions within and between atoms. Specifically, we have examined the response of ensembles of Rydberg atoms to each other and to externally applied THz radiation. By definition, one or more electrons in a Rydberg atom are highly excited, and reside in a ...

Two nitrogen atoms and a flexible carbon skeleton make N,N,N0,N0-tetramethylethylenediamine (TMEDA) an important model system to study the interplay of conformeric motions and charge delocalization. Ionization of one of the nitrogen atoms generates a localized charge that may (partially) transfer to the other nitrogen. The structural motions, conformation dependent electron lone pair interactio...

We observe the formation of long-range Cs2 Rydberg molecules consisting of a Rydberg and a ground-state atom by photoassociation spectroscopy in an ultracold Cs gas near 6s1/2(F=3,4)→np3/2 resonances (n=26-34). The spectra reveal two types of molecular states recently predicted by D. A. Anderson, S. A. Miller, and G. Raithel [Phys. Rev. A 90, 062518 (2014)]: states bound purely by triplet s-wav...

We report on the formation of ultralong-range Rydberg D-state molecules via photoassociation in an ultracold cloud of rubidium atoms. By applying a magnetic offset field on the order of 10 G and high resolution spectroscopy, we are able to resolve individual rovibrational molecular states. A full theory, using a Fermi pseudopotential approach including s- and p-wave scattering terms, reproduces...