Search

We present the results of experiments demonstrating the spectroscopic detection of Förster resonance energy transfer from NH3 in the X1A1 ground electronic state to helium atoms in 1sns 3S1 Rydberg levels, where n = 37 and n = 40. For these values of n, the 1sns 3S1 →1snp 3PJ transitions in helium lie close to resonance with the ground-state inversion transitions in NH3 and can be tuned through resonance using electric fields of less than 10 V/cm. In the experiments, energy transfer was detected by direct state-selective electric field ionization of the 3S1 and 3PJ Rydberg levels and by monitoring the population of the 3DJ levels following pulsed microwave transfer from the 3PJ levels. Detection by microwave spectroscopic methods represents a highly state selective, low-background approach to probing the collisional energy transfer process and the environment in which the atom-molecule interactions occur. The experimentally observed electric-field dependence of the resonant energy transfer process, probed both by direct electric field ionization and by microwave transfer, agrees well with the results of calculations performed using a simple theoretical model of the energy transfer process. For measurements performed in zero electric field with atoms prepared in the 1s40s 3S1 level, the transition from a regime in which a single energy transfer channel can be isolated for detection to one in which multiple collision channels begin to play a role has been identified as the NH3 density was increased. [ABSTRACT FROM AUTHOR]

Metastable (1s)(2s) helium atoms produced in a supersonic beam were excited to Rydberg-Stark states (with n in the 27–30 range) in a cryogenic environment and subsequently decelerated by, and trapped above, a surface-electrode decelerator. In the trapping experiments, the Rydberg atoms were brought to rest in 75 μs and over a distance of 33 mm and kept stationary for times in the 0–525 μs range, before being re-accelerated for detection by pulsed field ionisation. The use of a home-built valve producing short gas pulses with a duration of about 20 μs enabled the reduction of losses arising from collisions with atoms in the trailing part of the gas pulses. Cooling the decelerator to 4.7 K further suppressed losses by transitions induced by blackbody radiation and by collisions with atoms desorbing from the decelerator surface. The main contribution (60%) to the atom loss during deceleration is attributed to the escape out of the decelerator moving traps of atoms having energies higher than the trap saddle point, spontaneous emission and collisions with atoms in the trailing part of the gas pulses causing each only about 20% of the atom loss. At 4.7 K, the atom losses in the trapping phase of the experiments were found to be almost exclusively caused by spontaneous emission and the trap lifetimes were found to correspond to the natural lifetimes of the Rydberg-Stark states. Increasing the temperature to 100 K enhanced the trap losses by transitions stimulated by blackbody radiation. [ABSTRACT FROM AUTHOR]

Experimental and theoretical studies of the effects of weak radio-frequency electric fields on Rydberg–Stark states with electric dipole moments as large as 10,000 D are reported. High-resolution laser spectroscopic studies of Rydberg states with principal quantum numbern = 52 and 53 were performed in pulsed supersonic beams of metastable helium with the excited atoms detected by pulsed electric field ionisation. Experiments were carried out in the presence of sinusoidally oscillating electric fields with frequencies of 20 MHz, amplitudes of up to 120 mV/cm, and dc offsets of up to 4.4 V/cm. In weak fields, the experimentally recorded spectra are in excellent agreement with the results of calculations carried out using Floquet methods to account for electric dipole couplings in the oscillating fields. This highlights the validity of these techniques for the accurate calculation of the Stark energy level structure in such fields, and the limitations of the calculations in stronger fields wheren-mixing and higher order contributions become important. [ABSTRACT FROM AUTHOR]