This thesis reports the application of static and ramped electric fields to the Rydberg states of NO. Chapter 1 introduces the history of Rydberg states, their exotic properties, decay mechanisms, and the effect of an applied electric field. Chapter 2 details the experimental set-up used for the experiments presented in this thesis. Chapter 3 describes the structure of NO and multiphoton excita...

New experiments and theory contributing to the understanding of the dynamics and control of molecular Rydberg wave packets are presented. An intuitive scheme for controlling the rotational quantum state of a Rydberg molecule is demonstrated experimentally. We determine the accumulated phase difference between the various components of a molecular electron wave packet, and then employ a sequence...

A method is presented for calculating the wave function and energy of Rydberg excited states of molecules. A good estimate of the Rydberg state orbital is obtained using ground state density functional theory including Perdew-Zunger self-interaction correction and an optimized effective potential. The total energy of the excited molecule is obtained using the Delta Self-Consistent Field method ...

Ultracold Rb atoms were used to demonstrate nondegenerate four-wave mixing through a Rydberg state. Continuous 5S-5P-nD two-photon excitation to the Rydberg state was combined with an nD-6P tuned laser in a phase-matched geometry. The angular dependence, spatial profile, and dependence on detuning were investigated, showing good agreement with theory. Under optimum conditions 50% of the radiati...

Articles you may be interested in Photodissociation dynamics of the A Σ 2 + state of SH and SD radicals Observation of the 5 p Rydberg states of sulfur difluoride radical by resonance-enhanced multiphoton ionization spectroscopy J. Resonance enhanced multiphoton ionization of the hydrogen halides: Rotational structure and anomalies in Rydberg and ion-pair states of HCl and HBr

In rubidium Rydberg states, the collision nD_(5/2)+nD_(5/2)-->(n-2)F_(7/2)+(n+2)P_(3/2) is nearly resonant in the vicinity of n=43. As a result, over a short range of n centered around n approximately 43 the Rydberg-Rydberg interaction potential is quite large and turns from repulsive to attractive [Phys. Rev. A 75, 032712 (2007)10.1103/PhysRevA.75.032712]. We use state-selective field ionizati...

The formation of high-n Rydberg atoms from the neutral dissociation of superexcited states of I(2) formed by resonant two-photon excitation of molecular iodine using an ArF laser has been investigated. The high-n Rydberg atoms I* are formed by predissociation of the optically excited molecular Rydberg states I*(2)[R(B (2)Sigma(g) (+))] converging on the I(2) (+)(B (2)Sigma(g) (+)) state of the ...

Articles you may be interested in Resonance enhanced multiphoton ionization spectroscopy of the NF molecule: 1,3Φ 3d and 4d Rydberg states J. Rotationally resolved photoelectron spectra in resonance enhanced multiphoton ionization of H2O via the C 1 B 1 Rydberg state

Rydberg spin-waves are optically excited in a quasi-one-dimensional atomic sample of Rb atoms. Pairwise spin-wave correlations are observed by a spatially selective transfer of the quantum state onto a light field and photoelectric correlation measurements of the light. The correlations are interpreted in terms of the dephasing of multiply excited spin-waves by long-range Rydberg interactions.

The first vacuum-ultraviolet absorption spectrum of pyridine-N-oxide has been obtained, and has led to the identification of nearly 30 Rydberg states. These states were identified by use of the vibrational envelope ("footprint") of the UV-photoelectron spectrum, and are based on the first to the third ionization energies (IE). The adiabatic IE order, central to the Rydberg state symmetry identi...