Direct detection of Rydberg–Rydberg millimeter-wave transitions in a buffer gas cooled molecular beam
Author(s)
Patterson, David; Muenter, John S.; Zhou, Yan; Grimes, David Darrah; Barnum, Timothy James; Coy, Stephen; Klein, Ethan A.; Field, Robert W; ... Show more Show less
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Millimeter-wave transitions between molecular Rydberg states (n ∼ 35) of barium monofluoride are directly detected via Free Induction Decay (FID). Two powerful technologies are used in combination: Chirped-Pulse millimeter-Wave (CPmmW) spectroscopy and a buffer gas cooled molecular beam photoablation source. Hundreds of Rydberg–Rydberg transitions are recorded in 1 h with >10:1 signal:noise ratio and ∼150 kHz resolution. This high resolution, high spectral velocity experiment promises new strategies for rapid measurements of structural and dynamical information, such as the electric structure (multipole moments and polarizabilities) of the molecular ion-core and the strengths and mechanisms of resonances between Rydberg electron and ion-core motions. Direct measurements of Rydberg–Rydberg transitions with kilo-Debye dipole moments support efficient and definitive spectral analysis techniques, such as the Stark demolition and polarization diagnostics, which enable semi-automatic assignments of core-nonpenetrating Rydberg states. In addition, extremely strong radiation-mediated collective effects (superradiance) in a dense Rydberg gas of barium atoms are observed.
Date issued
2015-10Department
Massachusetts Institute of Technology. Department of ChemistryJournal
Chemical Physics Letters
Publisher
Elsevier
Citation
Zhou, Yan, David D. Grimes, Timothy J. Barnum, David Patterson, Stephen L. Coy, Ethan Klein, John S. Muenter, and Robert W. Field. “Direct Detection of Rydberg–Rydberg Millimeter-Wave Transitions in a Buffer Gas Cooled Molecular Beam.” Chemical Physics Letters 640 (November 2015): 124–136.
Version: Author's final manuscript
ISSN
00092614