Two-photon-absorption line strengths for nitric oxide: Comparison of theory and sub-Doppler, laser-induced fluorescence measurements
Abstract
In this paper, we discuss the results of high-resolution, sub-Doppler two-photon-absorption laser-induced fluorescence (TPALIF) spectroscopy of nitric oxide at low pressure and room temperature. The measurements were performed using the single-longitudinal mode output of a diode-laser-seeded optical parametric generator (OPG) system with a measured frequency bandwidth of 220 MHz. The measurements were performed using a counter-propagating pump beam geometry, resulting in sub-Doppler TPALIF spectra of NO for various rotational transitions in the (0,0) vibrational band of the A2Σ+ - X2Π electronic transition. The experimental results are compared with the results of a perturbative treatment of the rotational line strengths for the 20 different rotational branches of the X2Π(v" = 0) → A2Σ+(v' = 0) two-photon absorption band. In the derivation of the expressions for the two-photon transition absorption strength, the closure relation is used for rotational states in the intermediate levels of the two-photon transition in analogy with the Placzek treatment of Raman transitions. The theoretical treatment of the effect of angular momentum coupling on the two-photon rotational line strengths features the use of irreducible spherical tensors and 3j symbols. The final results are expressed in terms of the Hund’s case (a) coupling coefficients aJ and bJ for the X2Π(v"more »
- Authors:
-
- Purdue Univ., West Lafayette, IN (United States). School of Mechanical Engineering
- Publication Date:
- Research Org.:
- Purdue Univ., West Lafayette, IN (United States). School of Mechanical Engineering
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1465956
- Grant/Contract Number:
- FG02-03ER15391
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 146; Journal Issue: 12; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Kulatilaka, Waruna D., and Lucht, Robert P. Two-photon-absorption line strengths for nitric oxide: Comparison of theory and sub-Doppler, laser-induced fluorescence measurements. United States: N. p., 2017.
Web. doi:10.1063/1.4978921.
Kulatilaka, Waruna D., & Lucht, Robert P. Two-photon-absorption line strengths for nitric oxide: Comparison of theory and sub-Doppler, laser-induced fluorescence measurements. United States. https://doi.org/10.1063/1.4978921
Kulatilaka, Waruna D., and Lucht, Robert P. Tue .
"Two-photon-absorption line strengths for nitric oxide: Comparison of theory and sub-Doppler, laser-induced fluorescence measurements". United States. https://doi.org/10.1063/1.4978921. https://www.osti.gov/servlets/purl/1465956.
@article{osti_1465956,
title = {Two-photon-absorption line strengths for nitric oxide: Comparison of theory and sub-Doppler, laser-induced fluorescence measurements},
author = {Kulatilaka, Waruna D. and Lucht, Robert P.},
abstractNote = {In this paper, we discuss the results of high-resolution, sub-Doppler two-photon-absorption laser-induced fluorescence (TPALIF) spectroscopy of nitric oxide at low pressure and room temperature. The measurements were performed using the single-longitudinal mode output of a diode-laser-seeded optical parametric generator (OPG) system with a measured frequency bandwidth of 220 MHz. The measurements were performed using a counter-propagating pump beam geometry, resulting in sub-Doppler TPALIF spectra of NO for various rotational transitions in the (0,0) vibrational band of the A2Σ+ - X2Π electronic transition. The experimental results are compared with the results of a perturbative treatment of the rotational line strengths for the 20 different rotational branches of the X2Π(v" = 0) → A2Σ+(v' = 0) two-photon absorption band. In the derivation of the expressions for the two-photon transition absorption strength, the closure relation is used for rotational states in the intermediate levels of the two-photon transition in analogy with the Placzek treatment of Raman transitions. The theoretical treatment of the effect of angular momentum coupling on the two-photon rotational line strengths features the use of irreducible spherical tensors and 3j symbols. The final results are expressed in terms of the Hund’s case (a) coupling coefficients aJ and bJ for the X2Π(v" = 0) rotational level wavefunctions, which are intermediate between Hund’s case (a) and case (b). Considerable physical insight is provided by this final form of the equations for the rotational line strengths. Corrections to the two-photon absorption rotational line strength for higher order effects such as centrifugal stretching can be included in a straightforward fashion in the analysis by incorporating higher order terms in these coupling coefficients aJ and bJ, although these corrections are essentially negligible for J < 50. The theoretical calculations of relative line intensities are in good agreement both with our experiment and with published experimental results. Furthermore, the calculated line shapes and relative intensities for closely spaced main branch and satellite transitions are in excellent agreement with our experimental measurements},
doi = {10.1063/1.4978921},
journal = {Journal of Chemical Physics},
number = 12,
volume = 146,
place = {United States},
year = {Tue Mar 28 00:00:00 EDT 2017},
month = {Tue Mar 28 00:00:00 EDT 2017}
}
Works referenced in this record:
Imaging laser-induced fluorescence of oxygen atoms in a flame
journal, January 1984
- Aldén, Marcus; Hertz, Hans M.; Svanberg, Sune
- Applied Optics, Vol. 23, Issue 19
Two-photon spectra of gases by three-wave mixing
journal, February 1978
- Hochstrasser, Robin M.; Meredith, G. R.; Trommsdorff, H. P.
- Chemical Physics Letters, Vol. 53, Issue 3
Detailed calculation of hydroxyl (OH) radical two-photon absorption via broadband ultrafast excitation
journal, December 2011
- Stauffer, Hans U.; Roy, Sukesh; Kulatilaka, Waruna D.
- Journal of the Optical Society of America B, Vol. 29, Issue 1
Honl-London Factors for Doublet Transitions in Diatomic Molecules
journal, January 1970
- Bennett, R. J. M.
- Monthly Notices of the Royal Astronomical Society, Vol. 147, Issue 1
Spectroscopie d'absorption multiphotonique sans effet Doppler
journal, January 1973
- Cagnac, B.; Grynberg, G.; Biraben, F.
- Journal de Physique, Vol. 34, Issue 10
ʌ-type doubling and spin-rotation splitting of NO, measured in simultaneous one- and two-photon laser spectroscopy
journal, June 1978
- Wallenstein, R.; Zacharias, H.
- Optics Communications, Vol. 25, Issue 3
Two-photon-excited fluorescence measurement of hydrogen atoms in flames
journal, January 1983
- Lucht, Robert P.; Salmon, Joseph T.; King, Galen B.
- Optics Letters, Vol. 8, Issue 7
Time-resolved two-photon-excited fluorescence detection of atomic hydrogen in flames
journal, January 1990
- Goldsmith, J. E. M.; Anderson, R. J. M.; Williams, L. R.
- Optics Letters, Vol. 15, Issue 1
Comparison of various two-photon excitation schemes for laser-induced fluorescence spectroscopy in atomic hydrogen
journal, January 1994
- Czarnetzki, U.; Miyazaki, K.; Kajiwara, T.
- Journal of the Optical Society of America B, Vol. 11, Issue 11
Über Elementarakte mit zwei Quantensprüngen
journal, January 1931
- Göppert-Mayer, Maria
- Annalen der Physik, Vol. 401, Issue 3
Doppler-free two-photon-excited fluorescence spectroscopy of atomic hydrogen in flames
journal, January 1990
- Goldsmith, J. E. M.; Rahn, L. A.
- Optics Letters, Vol. 15, Issue 14
Femtosecond two-photon LIF imaging of atomic species using a frequency-quadrupled Ti:sapphire laser
journal, April 2014
- Kulatilaka, Waruna D.; Gord, James R.; Roy, Sukesh
- Applied Physics B, Vol. 116, Issue 1
Nonperturbative modeling of two-photon absorption in a three-state system
journal, November 2004
- Lucht, Robert P.; Roy, Sukesh; Gord, James R.
- The Journal of Chemical Physics, Vol. 121, Issue 20
Single-laser two-step fluorescence detection of atomic hydrogen in flames
journal, January 1990
- Goldsmith, J. E. M.; Laurendeau, Normand M.
- Optics Letters, Vol. 15, Issue 10
Two‐photon spectroscopy of the A 2 Σ + – X 2 Π i system of OH
journal, November 1983
- Crosley, David R.; Smith, Gregory P.
- The Journal of Chemical Physics, Vol. 79, Issue 10
Determination of N-atom concentrations in low-pressure premixed H2/O2/N2 flames doped with NH3, HCN and (CN)2
journal, December 1990
- Lawitzki, Annette; Bittner, Jürgen; Kohse-Höinghaus, Katharina
- Chemical Physics Letters, Vol. 175, Issue 5
Doppler-free two-photon excitation of nitric oxide with frequency-stabilized cw dye laser radiation
journal, October 1981
- Timmermann, A.; Wallenstein, R.
- Optics Communications, Vol. 39, Issue 4
Two-photon excitation of nitric oxide fluorescence as a temperature indicator in unsteady gasdynamic processes
journal, January 1981
- McKenzie, R. L.; Gross, K. P.
- Applied Optics, Vol. 20, Issue 12
On the precise measurement of the frequency transition 1S–2S of the hydrogen atom
journal, November 1974
- Baklanov, E. V.; Chebotaev, V. P.
- Optics Communications, Vol. 12, Issue 3
Two-photon absorption by rotating diatomic molecules
journal, April 1976
- Bray, R. G.; Hochstrasser, R. M.
- Molecular Physics, Vol. 31, Issue 4
Doppler-Free Two-Photon Spectroscopy of Hydrogen
journal, February 1975
- Hänsch, T. W.; Lee, S. A.; Wallenstein, R.
- Physical Review Letters, Vol. 34, Issue 6
Rotational line strengths in two- and three-photon transitions in diatomic molecules
journal, January 1980
- Halpern, J. B.; Zacharias, H.; Wallenstein, R.
- Journal of Molecular Spectroscopy, Vol. 79, Issue 1
Carbon atom fluorescence and C2 emission detected in fuel-rich flames using a UV laser
journal, June 1991
- Westblom, U.; Bengtsson, P. -E.; Ald�n, M.
- Applied Physics B Photophysics and Laser Chemistry, Vol. 52, Issue 6
Two-step saturated fluorescence detection of atomic hydrogen in flames
journal, January 1985
- Goldsmith, J. E. M.
- Optics Letters, Vol. 10, Issue 3
High-resolution Doppler-free two-photon spectroscopic studies of molecules. I. The bands of F
journal, May 1976
- Bischel, William K.; Kelly, Patrick J.; Rhodes, Charles K.
- Physical Review A, Vol. 13, Issue 5
Corrections to two-photon Hönl-London factors
journal, June 1987
- Hornkohl, J. O.; Ruyten, W. M.
- Journal of Molecular Spectroscopy, Vol. 123, Issue 2
Theory of femtosecond coherent anti-Stokes Raman scattering spectroscopy of gas-phase transitions
journal, July 2007
- Lucht, Robert P.; Kinnius, Paul J.; Roy, Sukesh
- The Journal of Chemical Physics, Vol. 127, Issue 4
Concentration measurements of atomic hydrogen in subatmospheric premixed C2H4/O2/Ar flat flames
journal, December 1988
- Salmon, J. Thaddeus; Laurendeau, Normand M.
- Combustion and Flame, Vol. 74, Issue 3
A two-photon absorption cross section measurement in nitric oxide
journal, November 1983
- Burris, J.; McGee, T. J.; McIlrath, T. J.
- Chemical Physics Letters, Vol. 101, Issue 6
Three-photon-excited fluorescence detection of atomic hydrogen in an atmospheric-pressure flame
journal, January 1984
- Aldén, M.; Schawlow, A. L.; Svanberg, S.
- Optics Letters, Vol. 9, Issue 6
Photolytic-interference-free, femtosecond, two-photon laser-induced fluorescence imaging of atomic oxygen in flames
journal, January 2016
- Kulatilaka, Waruna D.; Roy, Sukesh; Jiang, Naibo
- Applied Physics B, Vol. 122, Issue 2
Detection of fluorescence from O and N atoms induced by two-photon absorption
journal, January 1982
- Bischel, William K.; Perry, Bryce E.; Crosley, David R.
- Applied Optics, Vol. 21, Issue 8
Development of injection-seeded, pulsed optical parametric generator/oscillator systems for high-resolution spectroscopy
journal, March 2005
- Kulatilaka, W. D.; Anderson, T. N.; Bougher, T. L.
- Applied Physics B, Vol. 80, Issue 6
Absolute determination of local ground-state densities of atomic hydrogen in nonlocal-thermodynamic-equilibrium environments by two-photon polarization spectroscopy
journal, February 1995
- Dux, R.; Grützmacher, K.; de la Rosa, M. I.
- Physical Review E, Vol. 51, Issue 2
The two‐photon absorptivity of rotational transitions in the A 2 Σ + ( v ′ = 0)– X 2 Π( v ′′ = 0) gamma band of nitric oxide
journal, June 1982
- Gross, K. P.; McKenzie, R. L.
- The Journal of Chemical Physics, Vol. 76, Issue 11
Applications of two-photon absorption for detection of CO in combustion gases
journal, April 1984
- Ald�n, M.; Wallin, S.; Wendt, W.
- Applied Physics B Photophysics and Laser Chemistry, Vol. 33, Issue 4
Investigation of simultaneous two-photon H and single photon OH excitation in flames using a single dye laser
journal, January 1990
- Goldsmith, John E. M.
- Applied Optics, Vol. 29, Issue 33
Doppler-Free Two-Photon Fluorescence Excitation Spectroscopy of the A ← X(1,0) Band of Nitric Oxide: Fine Structure Parameter for the (3sσ)A2Σ+(v = 1) Rydberg State of 14N16O
journal, May 1993
- Murphy, J. E.; Bushaw, B. A.; Miller, R. J.
- Journal of Molecular Spectroscopy, Vol. 159, Issue 1