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Tuning out vibrational levels in molecular electron energy-loss spectra




Heays, Alan
Lewis, Brenton
Gibson, Stephen
Malone, C.P.
Johnson, P V
Kanik, Isik
Khakoo, M.A.

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American Physical Society


The phenomenon whereby features associated with certain vibrational levels in molecular states of mixed electronic character disappear under specific scattering conditions in electron energy-loss spectra is investigated. In particular, using a combination of experimental measurements and coupled-channel calculations, anomalous vibrational intensities in the mixed valence-Rydberg 1Π u←X1Σg+ transition of N 2 are explained. A single parameter, i.e., the ratio of the generalized electronic transition moments to the diabatic valence and Rydberg components of the mixed states, dependent on the experimental scattering conditions, is found to be essentially capable of describing all observed relative vibrational intensities, including the near disappearance of the b1Π u(v=5) feature for momentum-transfer-squared values K2 ≈ 0.3 a.u. This result highlights the interesting possibility of experimental control of molecular quantum-interference effects in electron energy-loss spectra, something that is not possible in optical spectra.



Keywords: Coupled-channel calculations; Diabatic; Electron energy-loss spectra; Electronic transition moments; Experimental control; Experimental measurements; Mixed state; Molecular electrons; Molecular state; Optical spectra; Quantum-interference effects; Rydberg



Physical Review A: Atomic, Molecular and Optical Physics


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Open Access

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