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Synopsis
SEVI is a variant of conventional anion photoelectron spectroscopy which combines a velocity-map imaging (VMI) detection scheme and tunable photodetachment energy. Anions are cryogenically cooled to temperatures as low as 5 K in a radiofrequency ion trap, then mass-selected and photodetached at energies 0.01-0.5 eV above threshold. The resulting photoelectrons are collected using relatively low extraction voltages, with the goal of selectively detecting slow electrons with high efficiency and enlarging their image on the detector. At each wavelength, one obtains a high resolution (up to 1 cm-1) photoelectron spectrum over a limited range of electron kinetic energy as well as the photoelectron angular distributions.
The SEVI spectra give the electronic and vibrational energy levels of the neutral molecule in high-resolution. In combination with ab initio electronic structure calculations and Franck-Condon simulations, the SEVI experiment yields information on the geometry, vibrational frequencies and electronic structure of both the anion and neutral states.
A recent review can be found here.
Molecules studied:
Vinylidene (H2CC)
Metal oxide clusters: FenO (n=1-5); VO2; SmO
Combustion-relevant radicals: methoxy (CH3O), t-butyl peroxy (C4H9OO), furanyl (C4H3O)
Transition state spectroscopy: F + CH3OH, CH4, H2
Project members:
Korina Vlahos
Astrid Zeng
Recent publications:
"Exploring vinylidene/acetylene isomerization by photoelectron spectroscopy of vibrationally excited vinylidene anions" M. DeWitt, D. Yang, J. A. Lau, K. Vlahos, H. Guo, D. M. Neumark, J. Phys. Chem. A, 129, 3682–3695 (2025). pdf
"High-resolution photoelectron spectroscopy of NO3− vibrationally excited along its ν3 mode" J. A. Lau, M. DeWitt, P. R. Franke, J. F. Stanton, D. M. Neumark, J. Phys. Chem. A, 129, 1634–1647 (2025). pdf
"High-resolution photoelectron spectroscopy of vibrationally excited vinoxide anions" J. A. Lau, M. DeWitt, M. A. Boyer, M. C. Babin, T. Solomis, M. Grellmann, K. R. Asmis, A. B. McCoy, D. M. Neumark, J. Phys. Chem. A, 127, 3133–3147 (2023). pdf
"Observation of resonances in the transition state region of the F + NH3 reaction using anion photoelectron spectroscopy" M. C. Babin, M. DeWitt, J. A. Lau, M. L. Weichman, J. B. Kim, H. Song, H. Guo, D. M. Neumark, Nat. Chem. (2022). pdf
"High Resolution Photoelectron Spectroscopy of the Acetyl Anion" M. DeWitt, M. C. Babin, J. A. Lau, T. Solomis, D. M. Neumark, J. Phys. Chem. A 126, 7962–7970 (2021). pdf
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