Coherent ultrafast photoelectron spectroscopy in Br2: Analternative method for measuring Delta v=/0 transitions inRydberg-to-Rydberg excitations

Journal Article · Mon Feb 06 04:00:00 EST 2006 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.2190218· OSTI ID:927812

Stavros, V G; Lau, L; Strasser, D; Leone, S R

A two-state vibrational wave packet is prepared in a low-lying 4d[1/2]{sub 1 or 2} Rydberg state of jet cooled Br{sub 2} (4d, v{prime}=3 and v{prime}=4) by two-photon excitation with 266.5 nm pulses from an ultrafast laser. The wave packet is detected by autoionization following excitation with time-delayed 800 nm pulses to the n=8 (v{sup +}=4) and n=9 (v{sup +}=3) Rydberg states in the {sup 2}{Pi}{sub 1/2} angular momentum core state. Autoionization of each state occurs to the {sup 2}{Pi}{sub 3/2} state of the ion through spin-orbit ionization. Photoelectron spectroscopy is used to differentiate between the n=8 and n=9 ejected photoelectrons. Detection of the wave packet recurrences via the n=8 and n=9 Rydberg states reveals a {pi} phase-shift difference of the recurrences between the two final states. In each case, {Delta}v {ne} 0 transitions are observed since wave packet recurrences are detected. By fitting the observed phase change of the recurrences with a simple model for the overlap amplitudes and assumptions about the potentials, we estimate, within the context of the model, that approximately 0.6% of the transitions may be attributed to {Delta} v = {+-} 1 transitions between the initial Rydberg superposition state and the final Rydberg detection state.

• Research Organization: Ernest Orlando Lawrence Berkeley NationalLaboratory, Berkeley, CA (US)
• Sponsoring Organization: USDOE Director. Office of Science. Basic EnergySciences
• DOE Contract Number: AC02-05CH11231
• OSTI ID: 927812
• Report Number(s): LBNL--59817; BnR: KC0301020
• Journal Information: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 17 Vol. 124; ISSN JCPSA6; ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
AMPLITUDES
ANGULAR MOMENTUM
AUTOIONIZATION
DETECTION
EXCITATION
IONIZATION
PHASE SHIFT
PHOTOELECTRON SPECTROSCOPY
RYDBERG STATES
WAVE PACKETS