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Communication: Time-domain measurement of high-pressure N2 and O2 self-broadened linewidths using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering
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Figures

Image of FIG. 1.

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FIG. 1.

Spectrally resolved hybrid fs/ps RCARS signals from J = 4 and 14 for N2 at (a) 1 atm, (b) 10 atm, and (c) 20 atm and N = 5 and 15 for O2 at (d) 1 atm, (e) 10 atm, and (f) 20 atm. Solid lines are exponential fits to signal decay.

Image of FIG. 2.

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FIG. 2.

Measured (a) N2 and (b) O2 self-broadened linewidths as a function of initial rotational state at pressures of 1, 10, and 20 atm. Solid lines are MEG linewidths using S-branch approximation. Bars represent calculated uncertainty.

Image of FIG. 3.

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FIG. 3.

Decay of N = 1 and 3 rotational lines of O2. Solid lines show measured oscillations due to triplet ground state with periods of 16.8 ps and 16.9 ps, respectively.

Tables

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Table I.

Experimental N2 self-broadened linewidths, FWHM (cm−1).

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Table II.

Experimental O2 self-broadened linewidths, FWHM (cm−1).

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/content/aip/journal/jcp/135/20/10.1063/1.3665932
2011-11-28
2014-04-20

Abstract

The direct measurement of self-broadened linewidths using the time decay of pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps RCARS) signals is demonstrated in gas-phase N2 and O2 from 1–20 atm. Using fs pump and Stokes pulses and a spectrally narrowed ps probe pulse, collisional dephasing rates with time constants as short as 2.5 ps are captured with high accuracy for individual rotational transitions. S-branch linewidths of N2 and O2 from ∼0.06 to 2.2 cm−1 and the line separation of O2 triplet states are obtained from the measureddephasing rates and compared with high-resolution, frequency-domain measurements and S-branch approximations using the modified exponential gap model. The accuracy of the current measurements suggests that the fs/ps RCARS approach is well suited for tracking the collisional dynamics of gas-phase mixtures over a wide range of pressures.

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Scitation: Communication: Time-domain measurement of high-pressure N2 and O2 self-broadened linewidths using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering
http://aip.metastore.ingenta.com/content/aip/journal/jcp/135/20/10.1063/1.3665932
10.1063/1.3665932
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