skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Effects of self-phase modulation (SPM) on femtosecond coherent anti-Stokes Raman scattering spectroscopy

Abstract

The effects of self-phase modulation (SPM) on the power spectra of femtosecond (fs) pulses and the consequent impact on N2 chirped-probe-pulse (CPP) fs coherent anti-Stokes Raman scattering (CARS) spectra are discussed in this paper. We investigated the pressure dependence of CPP fs CARS for N2 in a room-temperature gas cell at pressures ranging from 1 to 10 bar, and in our initial experiments the CPP fs CARS spectrum changed drastically as the pressure increased. We found that the spectra of the near-Fourier-transform-limited, 60-fs pump and Stokes pulses at the exit of the gas cell changed drastically as the pressure increased due to self-phase-modulation (SPM). This effect was examined in detail in further experiments where the pulse energies of the pump and Stokes pulses were controlled using a combination of a half-wave plate and a linear polarizer. Along with the generated CARS spectrum, the spectra of pump and Stokes pulses were measured at the entrance and exit of the gas cell. The extent of SPM effects for a particular spectrum was characterized by the least squares difference between that spectrum and a spectrum recorded at low enough pressure and laser intensities that SPM was negligible. SPM effects were investigated for N2,more » O2, CO2, and CH4, for pressures ranging from 1 to 10 bar, and for pump and Stokes pulse energies ranging from 10 to 60 μJ. We found that SPM effects in N2 were much weaker than for O2, CO2 and CH4.« less

Authors:
; ;
Publication Date:
Research Org.:
Purdue Univ., West Lafayette, IN (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1573297
Alternate Identifier(s):
OSTI ID: 1594855
Grant/Contract Number:  
FG02-03ER15391
Resource Type:
Published Article
Journal Name:
Optics Express
Additional Journal Information:
Journal Name: Optics Express Journal Volume: 27 Journal Issue: 23; Journal ID: ISSN 1094-4087
Publisher:
Optical Society of America
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Gu, Mingming, Satija, Aman, and Lucht, Robert P. Effects of self-phase modulation (SPM) on femtosecond coherent anti-Stokes Raman scattering spectroscopy. United States: N. p., 2019. Web. doi:10.1364/OE.27.033954.
Gu, Mingming, Satija, Aman, & Lucht, Robert P. Effects of self-phase modulation (SPM) on femtosecond coherent anti-Stokes Raman scattering spectroscopy. United States. doi:10.1364/OE.27.033954.
Gu, Mingming, Satija, Aman, and Lucht, Robert P. Wed . "Effects of self-phase modulation (SPM) on femtosecond coherent anti-Stokes Raman scattering spectroscopy". United States. doi:10.1364/OE.27.033954.
@article{osti_1573297,
title = {Effects of self-phase modulation (SPM) on femtosecond coherent anti-Stokes Raman scattering spectroscopy},
author = {Gu, Mingming and Satija, Aman and Lucht, Robert P.},
abstractNote = {The effects of self-phase modulation (SPM) on the power spectra of femtosecond (fs) pulses and the consequent impact on N2 chirped-probe-pulse (CPP) fs coherent anti-Stokes Raman scattering (CARS) spectra are discussed in this paper. We investigated the pressure dependence of CPP fs CARS for N2 in a room-temperature gas cell at pressures ranging from 1 to 10 bar, and in our initial experiments the CPP fs CARS spectrum changed drastically as the pressure increased. We found that the spectra of the near-Fourier-transform-limited, 60-fs pump and Stokes pulses at the exit of the gas cell changed drastically as the pressure increased due to self-phase-modulation (SPM). This effect was examined in detail in further experiments where the pulse energies of the pump and Stokes pulses were controlled using a combination of a half-wave plate and a linear polarizer. Along with the generated CARS spectrum, the spectra of pump and Stokes pulses were measured at the entrance and exit of the gas cell. The extent of SPM effects for a particular spectrum was characterized by the least squares difference between that spectrum and a spectrum recorded at low enough pressure and laser intensities that SPM was negligible. SPM effects were investigated for N2, O2, CO2, and CH4, for pressures ranging from 1 to 10 bar, and for pump and Stokes pulse energies ranging from 10 to 60 μJ. We found that SPM effects in N2 were much weaker than for O2, CO2 and CH4.},
doi = {10.1364/OE.27.033954},
journal = {Optics Express},
number = 23,
volume = 27,
place = {United States},
year = {2019},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1364/OE.27.033954

Save / Share:

Works referenced in this record:

Time- and frequency-dependent model of time-resolved coherent anti-Stokes Raman scattering (CARS) with a picosecond-duration probe pulse
journal, January 2014

  • Stauffer, Hans U.; Miller, Joseph D.; Slipchenko, Mikhail N.
  • The Journal of Chemical Physics, Vol. 140, Issue 2
  • DOI: 10.1063/1.4860475

Indices governing optical self-focusing and self-induced changes in the state of polarization in N 2 , O 2 , H 2 , and Ar gases
journal, March 1990

  • Hellwarth, R. W.; Pennington, D. M.; Henesian, M. A.
  • Physical Review A, Vol. 41, Issue 5
  • DOI: 10.1103/PhysRevA.41.2766

BOXCARS: Crossed‐beam phase‐matched CARS generation in gases
journal, April 1978

  • Eckbreth, Alan C.
  • Applied Physics Letters, Vol. 32, Issue 7
  • DOI: 10.1063/1.90070

Time-resolved femtosecond CARS from 10 to 50 Bar: collisional sensitivity: Time-resolved femtosecond CARS
journal, March 2013

  • Wrzesinski, Paul J.; Stauffer, Hans U.; Kulatilaka, Waruna D.
  • Journal of Raman Spectroscopy, Vol. 44, Issue 10
  • DOI: 10.1002/jrs.4287

Measurement of high order Kerr refractive index of major air components
journal, January 2009

  • Loriot, Vincent; Hertz, Edouard; Faucher, Olivier
  • Optics Express, Vol. 17, Issue 16
  • DOI: 10.1364/OE.17.013429

Raman Scattering Cross Sections
journal, February 1972

  • Penney, C. M.; Goldman, L. M.; Lapp, M.
  • Nature Physical Science, Vol. 235, Issue 58
  • DOI: 10.1038/physci235110b0

Interference-free hybrid fs/ps vibrational CARS thermometry in high-pressure flames
journal, January 2018

  • Stauffer, Hans U.; Rahman, K. Arafat; Slipchenko, Mikhail N.
  • Optics Letters, Vol. 43, Issue 20
  • DOI: 10.1364/OL.43.004911

Measurement of pressure dependent nonlinear refractive index of inert gases
journal, January 2010

  • Börzsönyi, Á.; Heiner, Z.; Kovács, A. P.
  • Optics Express, Vol. 18, Issue 25
  • DOI: 10.1364/OE.18.025847

Ultra-broadband two beam CARS using femtosecond laser pulses
journal, July 2016


Femtosecond Raman-induced polarization spectroscopy studies of rotational coherence in O2, N2 and CO2
journal, June 1993


Technique developments and performance analysis of chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering combustion thermometry
journal, January 2017

  • Thomas, Levi M.; Satija, Aman; Lucht, Robert P.
  • Applied Optics, Vol. 56, Issue 31
  • DOI: 10.1364/AO.56.008797

Two-beam femtosecond coherent anti-Stokes Raman scattering for thermometry on CO 2
journal, January 2017

  • Kerstan, M.; Makos, I.; Nolte, S.
  • Applied Physics Letters, Vol. 110, Issue 2
  • DOI: 10.1063/1.4974030

Determination of the inertial contribution to the nonlinear refractive index of air, N_2, and O_2 by use of unfocused high-intensity femtosecond laser pulses
journal, January 1997

  • Nibbering, E. T. J.; Grillon, G.; Franco, M. A.
  • Journal of the Optical Society of America B, Vol. 14, Issue 3
  • DOI: 10.1364/JOSAB.14.000650

Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence
journal, December 2006

  • Lucht, Robert P.; Roy, Sukesh; Meyer, Terrence R.
  • Applied Physics Letters, Vol. 89, Issue 25
  • DOI: 10.1063/1.2410237

Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering for high-speed CH 4 /N 2 measurements in binary gas mixtures : Hybrid fs/ps CARS for high-speed CH
journal, February 2013

  • Engel, Sascha R.; Miller, Joseph D.; Dedic, Chloe E.
  • Journal of Raman Spectroscopy, Vol. 44, Issue 10
  • DOI: 10.1002/jrs.4261

One-dimensional single-shot thermometry in flames using femtosecond-CARS line imaging
journal, January 2011

  • Kulatilaka, W. D.; Stauffer, H. U.; Gord, J. R.
  • Optics Letters, Vol. 36, Issue 21
  • DOI: 10.1364/OL.36.004182

Determination of molecular contributions to the nonlinear refractive index of air for mid-infrared femtosecond laser-pulse excitation
journal, June 2019


Pressure measurements using hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering
journal, January 2015


Sensitivity of propagation and energy deposition in femtosecond filamentation to the nonlinear refractive index
journal, April 2015

  • Rosenthal, E. W.; Palastro, J. P.; Jhajj, N.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 48, Issue 9
  • DOI: 10.1088/0953-4075/48/9/094011

Absolute rotational Raman cross sections for N_2, O_2, and CO_2
journal, January 1974

  • Penney, C. M.; St. Peters, R. L.; Lapp, M.
  • Journal of the Optical Society of America, Vol. 64, Issue 5
  • DOI: 10.1364/JOSA.64.000712

Absolute measurement of the transient optical nonlinearity in N 2 , O 2 , N 2 O, and Ar
journal, April 2012


Optical Refractive Index of Air: Dependence on Pressure, Temperature and Composition
journal, January 1967


Measurement of the nonlinear refractive index of air and other gases at 248 nm
journal, November 1993


Quantitative one-dimensional imaging using picosecond dual-broadband pure-rotational coherent anti-Stokes Raman spectroscopy
journal, January 2011

  • Kliewer, Christopher J.; Gao, Yi; Seeger, Thomas
  • Applied Optics, Vol. 50, Issue 12
  • DOI: 10.1364/AO.50.001770

Propagation of intense short laser pulses in the atmosphere
journal, October 2002


Theoretical modeling of single-laser-shot, chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering thermometry
journal, April 2011