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

Please always quote using this URN: urn:nbn:de:bvb:29-opus-38072
  • 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 measured dephasing rates and compared with high-resolution, frequency-domain measurements and S-branch approximations usingThe 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 measured dephasing 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.show moreshow less

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Metadaten
Author:Joseph D. Miller, Sukesh Roy, James R. Gord, Terrence R. Meyer
URN:urn:nbn:de:bvb:29-opus-38072
Document Type:Article
Language:English
Year of Completion:2011
Publishing Institution:Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU)
Release Date:2012/11/07
Tag:coherent antiStokes Raman scattering; high-speed optical techniques; nitrogen; oxygen; rotational states
SWD-Keyword:-
Original publication:Journal of Chemical Physics 135.20 (2011): 06.11.2012 <http://jcp.aip.org/resource/1/jcpsa6/v135/i20/p201104_s1>
Institutes:Technische Fakultät / Technische Fakultät -ohne weitere Spezifikation-
Dewey Decimal Classification:Technik, Medizin, angewandte Wissenschaften / Technik / Technik, Technologie
PACS-Classification:30.00.00 ATOMIC AND MOLECULAR PHYSICS / 33.00.00 Molecular properties and interactions with photons / 33.15.-e Properties of molecules (see also section 31, Electronic structure of atoms and molecules: theory; for molecules of interest in astrophysics, see 95.30.Ky; for structure and properties of biomolecules, see 87.15.-v) / 33.15.Mt Rotation, vibration, and vibration-rotation constants
30.00.00 ATOMIC AND MOLECULAR PHYSICS / 33.00.00 Molecular properties and interactions with photons / 33.20.-t Molecular spectra (see also 78.47.J- Ultrafast pump/probe spectroscopy in condensed matter and 82.53.Kp Coherent spectroscopy of atoms and molecules; for chemical analytical methods using spectroscopy, see 82.80.Dx, Gk, Ha in physical chemistry; 87.64.-t / 33.20.Fb Raman and Rayleigh spectra (including optical scattering)
30.00.00 ATOMIC AND MOLECULAR PHYSICS / 33.00.00 Molecular properties and interactions with photons / 33.70.-w Intensities and shapes of molecular spectral lines and bands / 33.70.Jg Line and band widths, shapes, and shifts
open_access (DINI-Set):open_access
Collections:Universität Erlangen-Nürnberg / Allianzlizenzen: Alle Beiträge sind mit Zustimmung der Rechteinhaber aufgrund einer DFG-geförderten Allianzlizenz frei zugänglich. / Allianzlizenzen 2011