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Observation of energy level shifts of Rydberg atoms due to thermal fields. Final report

Leo W. Hollberg, J. L. Hall

Published Oct 1, 1983• 0 citations
OpenAlex

Abstract

The authors report the first observation of level shifts of Rydberg states due to their coupling with thermal radiation fields. The Rydberg level positions were measured relative to the atomic ground state using two photon optical Ramsey fringe techniques in an atomic beam apparatus. The level shifts were isolated by chopping the blackbody radiation source. The runs analyzed are consistent with the expected T sup 2 dependence and much data remains to be analyzed.

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The authors report the first observation of level shifts of Rydberg states due to their coupling with thermal radiation fields. The Rydberg level positions were measured relative to the atomic ground state using two photon optical Ramsey fringe techniques in an atomic beam apparatus. The level shifts were isolated by chopping the blackbody radiation source. The runs analyzed are consistent with the expected T sup 2 dependence and much data remains to be analyzed.
Blackbody radiation is expected to produce a temperature-dependent Stark shift in atomic Rydberg states. Unfortunately, in "one-electron" atoms, all the Rydberg levels experience the same shift, and the effect is only observable on an optical transition from the ground state. However, in a many-electron atom the presence of valence-state perturbers leads to unequal shifts of the Rydberg levels. This should make it possible to observe the frequency shift of a transition between two neighboring Rydberg states at a frequency in the radio-frequency range. This eliminates the need for a very stable visible laser, which so far has been the major technical obstacle to the observation and utilization of the effect. We present as an example a specific case in Ba.
Lying ≥4 eV above the ground state, Rydberg states are not populated thermally, except at very high temperatures. Accordingly, it is natural to assume that thermal effects are negligible in dealing with Rydberg atoms. However, Rydberg atoms are strongly affected by black body radiation, even at room temperature. The dramatic effect of thermal radiation is due to two facts. First, the energy spacings Δ W between Rydberg levels are small, so that Δ W < kT at 300 K. Second, the dipole matrix elements of transitions between Rydberg states are large, providing excellent coupling of the atoms to the thermal radiation. The result of the strong coupling between Rydberg atoms and the thermal radiation is that population initially put into one state, by laser excitation for example, rapidly diffuses to other energetically nearby states by black body radiation induced dipole transitions. Both the redistribution of population and the implicit increase in the radiative decay rates are readily observed. Although the above mentioned effects on level populations are the most obvious effects, the fact that a Rydberg atom is immersed in the thermal radiation field increases its energy by a small amount, 2 kHz at 300 K. While the radiation intensity is vastly different in the two cases, this effect is the same as the ponderomotive shift of the ionization limit in high intensity laser experiments.
We have excited helium atoms from their metastable 2 3S{}^{3}\phantom{\rule{-0.16em}{0ex}}S3S state to Rydberg states in the range 13<n<5013<n<5013<n<50 in a two-step process via the 3 3P{}^{3}\phantom{\rule{-0.16em}{0ex}}P3P state using light at $\ensuremath{\lambda}=389$ nm and 785--815 nm. Atoms in a thermal beam (100 K) cross partially overlapping laser beams of the appropriate frequencies in the counterintuitive order to exploit the high efficiency of stimulated rapid adiabatic passage. The interaction region is between two plates that can be used for Stark tuning in a few V/cm field or for field ionization. At fields much too low for field ionization, we observe signals attributed to ionization by blackbody radiation. Multiple tests confirm this attribution as the cause of ionization. For example, by heating the plates we observe the expected signal increases. Our experiments reinforce previous work where the interaction between Rydberg atoms and room temperature blackbody radiation is important for experiments.
Using state-resolved field ionization we have studied the time evolution of sodium Rydberg states, in a thermal atomic beams initially excited to 28s. The velocities of the detected Rydberg atoms were selected using the time-of-flight technique. With this selection we were able to study the time evolution of atoms with average velocities v{sub r} different from v{sub b}, the average velocity of the ground state atoms of the beam. We observe that for v{sub r}{approximately}v{sub b} the time evolution is dominated by blackbody radiation induced transitions to neighboring levels. However, as v{sub r}>>v{sub b} collisional transfers become important. For v{sub r}>>v{sub b} the time evolution is dominated by collisional transfer. The data shows evidence of both n{sup -} and l{sup -} changing collisions. We will compare a modeled theory with the data.
Effects due to the interaction of 300 K background radiation with Xe(nf)\mathrm{Xe}(\mathrm{nf})Xe(nf) Rydberg atoms are reported. Transitions to nearby ddd and ggg levels are observed. When the ambient photon density is reduced to that appropriate to liquid-nitrogen temperature by cooling the apparatus, a corresponding reduction in the transition rates to these levels is observed. The transition rates are found to be consistent with those predicted by use of quantum-defect theory.