Rotational coherence imaging and control for CN molecules through time-frequency resolved coherent anti-Stokes Raman scattering

Lindgren, Johan; Hulkko, Eero; Pettersson, Mika; Kiljunen, Toni

doi:doi:10.1063/1.3665934

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In lithium ion batteries, decomposition of the electrolyte and its associated passivation of the electrode surface occurs at low potentials, resulting in an electronically insulating, but Li-ion conducting, solid electrolyte interphase (SEI). The products of the SEI and their chemical constituents/properties play an important role in the long-term stability and performance of the battery. Reactivity and the sub-keV core binding energies of lithium, carbon, oxygen, and fluorine species in the SEI...

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Numerical wave packet simulations are performed for studying coherent anti-Stokes Raman scattering (CARS) for CN radicals. Electronic coherence is created by femtosecond laser pulses between the X ²Σ and B ²Σ states. Due to the large energy separation of vibrational states, the wave packets are superpositions of rotational states only. This allows for a specially detailed inspection of the second- and third-order coherences by a two-dimensional imaging approach. We present the time-frequency domain images to illustrate the intra- and intermolecular interferences, and discuss the procedure to rationally control and experimentally detect the interferograms in solid Xe environment.

Article Outline

INTRODUCTION
THEORY AND METHODS
1. Interferences
2. Detection methods
3. Implementation methods
RESULTS AND DISCUSSION
1. Interferometric imaging
2. Time-integrated spectrograms
3. Controlling the interferograms
CONCLUSIONS

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KEYWORDS and PACS

Keywords

carbon compounds, coherent antiStokes Raman scattering, free radicals, intermolecular mechanics, intramolecular mechanics, numerical analysis, rotational states, vibrational states

PACS

33.20.Fb

Raman and Rayleigh spectra (including optical scattering)
33.20.Sn

Rotational analysis
33.20.Tp

Vibrational analysis
34.20.Gj

Intermolecular and atom-molecule potentials and forces
33.15.Hp

Barrier heights (internal rotation, inversion, rotational isomerism, conformational dynamics)
31.15.xv

Molecular dynamics and other numerical methods

ARTICLE DATA

Digital Object Identifier

http://dx.doi.org/10.1063/1.3665934

PUBLICATION DATA

ISSN

0021-9606 (print)

1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef

American Institute of Physics

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