Femtosecond Raman time-resolved molecular spectroscopy

Bruno Lavorel; Ha Tran; Edouard Hertz; Olivier Faucher; Pierre Joubert; Marcus Motzkus; Tiago Buckup; Tobias Lang; Hrvoje Skenderovi; Gregor Knopp; Paul Beaud; Hans M. Frey

doi:10.1016/j.crhy.2004.01.013

Femtosecond Raman time-resolved molecular spectroscopy
[Spectroscopie moléculaire Raman femtoseconde résolue en temps]

Présenté par : Guy Laval

Bruno Lavorel ¹ ; Ha Tran ^1,² ; Edouard Hertz ¹ ; Olivier Faucher ¹ ; Pierre Joubert ² ; Marcus Motzkus ³ ; Tiago Buckup ³ ; Tobias Lang ³ ; Hrvoje Skenderovi ³ ; Gregor Knopp ⁴ ; Paul Beaud ⁴ ; Hans M. Frey ⁵

¹ Laboratoire de physique de l'Université de Bourgogne, UMR CNRS 5027, BP 47 870, 21078 Dijon cedex, France
² Laboratoire de physique moléculaire, UMR CNRS 6624, 25030 Besançon cedex, France
³ Max-Planck-Institut für Quantenoptik, 85748 Garching, Germany
⁴ Paul Scherrer Institute, CH-5232 Villigen PSI, Switzerland
⁵ Department for Chemistry and Biochemistry, University of Bern, CH-3012 Bern, Switzerland

Comptes Rendus. Physique, Gas phase molecular spectroscopy, Volume 5 (2004) no. 2, pp. 215-229.

Résumé
Abstract

L'application de plusieurs techniques cohérentes non-linéaires femtosecondes résolues en temps comme la spectroscopie Raman de polarisation (RIPS), le mélange dégénéré à quatre ondes (DFWM), et la spectroscopie de diffusion Raman anti-Stokes cohérente (CARS), pour la spectroscopie moléculaire est présentée. Toutes les méthodes reposent sur l'excitation cohérente initiale d'états moléculaires produisant des paquets d'ondes dont l'évolution temporelle est ensuite mesurée. Dans les cas RIPS et DFWM, seuls des états rotationnels sont impliqués, alors qu'en CARS, des états vibrationnels peuvent être excités. En premier, la méthodologie des mesures de concentration et de température utilisant la technique RIPS dans des mélanges de gaz impliquant N₂, CO₂, O₂, et N₂O est présentée. Ensuite, plusieurs applications sont données pour les deux techniques proches DFWM et CARS. La technique DFWM est apte à extraire les constantes rotationnelles de molécules avec une grande précision comme il est démontré par des mesures sur CO₂ et la pyrimidine, qui est une unité moléculaire de construction biologique. La technique CARS peut aussi être utilisée pour étudier des constantes moléculaires d'ordre supérieur et pour mesurer avec sensibilité la température dans H₂ jusqu'à 2000 K. Finalement, la technique CARS est appliquée à l'investigation de modèles de forme de raie dépendant de la pression, qui sont importants pour la mesure de température à partir de données spectrales.

The applicability of several femtosecond time resolved non-linear coherent techniques such as Raman induced polarization spectroscopy (RIPS), degenerate four-wave mixing (DFWM) and coherent anti-Stokes Raman spectroscopy (CARS) for molecular spectroscopy is presented. All methods rely on the initial coherent excitation of molecular states producing wavepackets, whose time evolution is then measured. In the case of RIPS and DFWM only pure rotational transitions are involved, whereas in CARS vibrational states can be excited. First the methodology of concentration and temperature measurements using RIPS in gas mixtures involving N₂, CO₂, O₂, and N₂O is shown. In addition some applications are given for the two closely related techniques DFWM and CARS. DFWM is suitable to extract the rotational constants of molecules to a high accuracy as is demonstrated by measurements on CO₂ and pyrimidine, which is a biological building block. CARS can be used to study higher order molecular constants and to sensitively determine temperature in, e.g., H₂ up to 2000 K. Finally, CARS is applied for the investigation of pressure dependent lineshape models, which are important for the temperature evaluation from spectroscopic data.

Publié le : 2004-03-01

DOI : 10.1016/j.crhy.2004.01.013

Keywords: Femtosecond laser, Ultrafast phenomena, Non-linear coherent and time resolved spectroscopy, Rovibrational wavepacket, Pressure measurement, Thermometry
Mots-clés : Laser femtoseconde, Phénomènes ultra-rapides, Spectroscopie non-linéaire cohérente et résolue en temps, Paquet d'ondes rovibrationnel, Mesure de pression, Thermométrie

Affiliations des auteurs :

Bruno Lavorel ¹ ; Ha Tran ^{1, 2} ; Edouard Hertz ¹ ; Olivier Faucher ¹ ; Pierre Joubert ² ; Marcus Motzkus ³ ; Tiago Buckup ³ ; Tobias Lang ³ ; Hrvoje Skenderovi ³ ; Gregor Knopp ⁴ ; Paul Beaud ⁴ ; Hans M. Frey ⁵

¹ Laboratoire de physique de l'Université de Bourgogne, UMR CNRS 5027, BP 47 870, 21078 Dijon cedex, France
² Laboratoire de physique moléculaire, UMR CNRS 6624, 25030 Besançon cedex, France
³ Max-Planck-Institut für Quantenoptik, 85748 Garching, Germany
⁴ Paul Scherrer Institute, CH-5232 Villigen PSI, Switzerland
⁵ Department for Chemistry and Biochemistry, University of Bern, CH-3012 Bern, Switzerland

@article{CRPHYS_2004__5_2_215_0,
     author = {Bruno Lavorel and Ha Tran and Edouard Hertz and Olivier Faucher and Pierre Joubert and Marcus Motzkus and Tiago Buckup and Tobias Lang and Hrvoje Skenderovi and Gregor Knopp and Paul Beaud and Hans M. Frey},
     title = {Femtosecond {Raman} time-resolved molecular spectroscopy},
     journal = {Comptes Rendus. Physique},
     pages = {215--229},
     publisher = {Elsevier},
     volume = {5},
     number = {2},
     year = {2004},
     doi = {10.1016/j.crhy.2004.01.013},
     language = {en},
}

TY  - JOUR
AU  - Bruno Lavorel
AU  - Ha Tran
AU  - Edouard Hertz
AU  - Olivier Faucher
AU  - Pierre Joubert
AU  - Marcus Motzkus
AU  - Tiago Buckup
AU  - Tobias Lang
AU  - Hrvoje Skenderovi
AU  - Gregor Knopp
AU  - Paul Beaud
AU  - Hans M. Frey
TI  - Femtosecond Raman time-resolved molecular spectroscopy
JO  - Comptes Rendus. Physique
PY  - 2004
SP  - 215
EP  - 229
VL  - 5
IS  - 2
PB  - Elsevier
DO  - 10.1016/j.crhy.2004.01.013
LA  - en
ID  - CRPHYS_2004__5_2_215_0
ER  -

%0 Journal Article
%A Bruno Lavorel
%A Ha Tran
%A Edouard Hertz
%A Olivier Faucher
%A Pierre Joubert
%A Marcus Motzkus
%A Tiago Buckup
%A Tobias Lang
%A Hrvoje Skenderovi
%A Gregor Knopp
%A Paul Beaud
%A Hans M. Frey
%T Femtosecond Raman time-resolved molecular spectroscopy
%J Comptes Rendus. Physique
%D 2004
%P 215-229
%V 5
%N 2
%I Elsevier
%R 10.1016/j.crhy.2004.01.013
%G en
%F CRPHYS_2004__5_2_215_0

Bruno Lavorel; Ha Tran; Edouard Hertz; Olivier Faucher; Pierre Joubert; Marcus Motzkus; Tiago Buckup; Tobias Lang; Hrvoje Skenderovi; Gregor Knopp; Paul Beaud; Hans M. Frey. Femtosecond Raman time-resolved molecular spectroscopy. Comptes Rendus. Physique, Gas phase molecular spectroscopy, Volume 5 (2004) no. 2, pp. 215-229. doi : 10.1016/j.crhy.2004.01.013. https://comptes-rendus.academie-sciences.fr/physique/articles/10.1016/j.crhy.2004.01.013/

Bibliographie
Cité par

[1] M. Morgen; W. Price; L. Hunziker; P. Ludowise; M. Blackwell; Y. Chen Chem. Phys. Lett., 209 (1993), p. 1

[2] R. Leonhardt; W. Holzapfel; W. Zinth; W. Kaiser Chem. Phys. Lett., 133 (1987), p. 373

[3] W. Zinth; W. Kaiser, Topics Appl. Phys., vol. 60, Springer, Berlin, 1988, p. 235

[4] S. Mukamel Principles of Nonlinear Optical Spectroscopy, Oxford University Press, Oxford, 1995

[5] M. Motzkus; S. Pedersen; A.H. Zewail J. Phys. Chem., 100 (1996), p. 5620

[6] A.M. Zheltikov J. Raman Spectrosc., 31 (2000), p. 653

[7] P.M. Felker; A.H. Zewail (J. Manz; L. Wöste, eds.), Femtosecond Chemistry, vol. 1, VCH, Weinheim, 1995

[8] M. Fickenscher; H.G. Purucker; A. Laubereau Chem. Phys. Lett., 191 (1992), p. 182

[9] T. Chen; A. Vierheilig; P. Waltner; M. Heid; A. Materny Chem Phys. Lett., 325 (2000), p. 176

[10] M. Schmitt; G. Knopp; A. Materny; W. Kiefer Chem. Phys. Lett., 270 (1997), p. 9

[11] T. Lang; K.L. Kompa; M. Motzkus Chem. Phys. Lett., 310 (1999), p. 65

[12] G. Knopp; P. Beaud; P.P. Radi; M. Tulej; B. Bougie; D. Cannavo; T. Gerber J. Raman Spectrosc., 33 (2002), p. 861

[13] M. Morgen; W. Price; P. Ludowise; Y. Chen J. Chem. Phys., 102 (1995), p. 8780

[14] B. Lavorel; O. Faucher; M. Morgen; R. Chaux J. Raman Spectrosc., 31 (2000), p. 77

[15] H. Tran; B. Lavorel; O. Faucher; R. Saint Loup; P. Joubert J. Raman Spectrosc., 33 (2002), p. 872

[16] E. Hertz; B. Lavorel; O. Faucher; R. Chaux J. Chem. Phys., 113 (2000), p. 6629

[17] H.-M. Frey; P. Beaud; T. Gerber; B. Mischler; P.P. Radi; A.P. Tzannis Appl. Phys. B, 68 (1999), p. 735

[18] H.-M. Frey; P. Beaud; T. Gerber; B. Mischler; P.P. Radi; A.P. Tzannis J. Raman Spectrosc., 31 (2000), p. 71

[19] H.W. Schrötter; H.W. Klöckner, Topics Current Phys., vol. 11, Springer, Berlin, 1979 (p. 123)

[20] H. Frey, D. Kummli, S. Leutwyler, in preparation

[21] G. Herzberg Spectra of Diatomic Molecules, vol. 1, Molecular Spectra and Molecular Structure, Krieger, Florida, 1950

[22] M.L. Koszykowski; R.L. Farrow; R.E. Palmer Opt. Lett., 10 (1985), p. 478

[23] G. Knopp; P. Radi; M. Tulej; T. Gerber; P. Beaud J. Chem. Phys., 118 (2003), p. 8223

[24] A.E. DePristo; S.D. Augustin; R. Ramaswamy; H. Rabitz J. Chem. Phys., 71 (1979), p. 850

[25] A. Ben-Reuven Phys. Rev., 141 (1966), p. 34

[26] T.A. Brunner; R.D. Driver; N. Smith; D.E. Pritchard Phys. Rev. Lett., 41 (1978), p. 856

[27] J.C. Polanyi; K.B. Woodall J. Chem. Phys., 56 (1972), p. 1563

[28] I. Procaccia; R.D. Levine J. Chem. Phys., 64 (1976), p. 808

[29] P. Beaud; G. Knopp Chem. Phys. Lett., 371 (2003), p. 194

[30] P. Beaud; T. Gerber; P.P. Radi; M. Tulej; G. Knopp Chem. Phys. Lett., 373 (2003), p. 251

[31] V. Renard; M. Renard; S. Guerin; Y.T. Pashayan; B. Lavorel; O. Faucher; H.R. Jauslin Phys. Rev. Lett., 90 (2003), p. 153601

[32] S.A. Akhmanov; A.F. Bunkin; S.G. Ivanov; N.I. Koroteev Sov. Phys. JETP, 47 (1978), p. 667

[33] E. Hertz; R. Chaux; O. Faucher; B. Lavorel J. Chem. Phys., 115 (2001), p. 3598

[34] T. Lang; M. Motzkus; H.M. Frey; P. Beaud J. Chem. Phys., 115 (2001), p. 5418

[35] P. Beaud; H.M. Frey; T. Lang; M. Motzkus Chem. Phys. Lett., 344 (2001), p. 407

[36] L. Bonamy; J. Bonamy; D. Robert; B. Lavorel; R. Saint-Loup; R. Chaux; J. Santos; H. Berger J. Chem. Phys., 89 (1988), p. 5568

[37] L. Bonamy; J.V. Buldyreva Phys. Rev. A, 63 (2000), p. 012715

Francesco Mazza; Dirk van den Bekerom An ultrafast algorithm for ultrafast time-resolved coherent Raman spectroscopy, Communications Chemistry, Volume 8 (2025) no. 1 | DOI:10.1038/s42004-024-01397-8
Venkat Athmanathan; K. Arafat Rahman; Daniel K. Lauriola; James Braun; Guillermo Paniagua; Mikhail N. Slipchenko; Sukesh Roy; Terrence R. Meyer Femtosecond/picosecond rotational coherent anti-Stokes Raman scattering thermometry in the exhaust of a rotating detonation combustor, Combustion and Flame, Volume 231 (2021), p. 111504 | DOI:10.1016/j.combustflame.2021.111504
Paulette Vincent-Ruz What Does It Mean to Think Like a Chemist?, Integrating Professional Skills into Undergraduate Chemistry Curricula, Volume 1365 (2020), p. 57 | DOI:10.1021/bk-2020-1365.ch005
Mingming Gu; Aman Satija; Robert P. Lucht, AIAA Scitech 2019 Forum (2019) | DOI:10.2514/6.2019-1086
F. Chaussard; Th. Vieillard; F. Billard; O. Faucher; J.‐M. Hartmann; C. Boulet; B. Lavorel Dissipation of post‐pulse laser‐induced alignment of CO2 through collisions with Ar, Journal of Raman Spectroscopy, Volume 46 (2015) no. 8, p. 691 | DOI:10.1002/jrs.4646
Joseph D. Miller; Chloe E. Dedic; Terrence R. Meyer Vibrational femtosecond/picosecond coherent anti‐Stokes Raman scattering with enhanced temperature sensitivity for flame thermometry from 300 to 2400 K, Journal of Raman Spectroscopy, Volume 46 (2015) no. 8, p. 702 | DOI:10.1002/jrs.4725
A. Kouzov; P. Radi Line-space description of resonant four-wave mixing: Theory for isotropic molecular states, The Journal of Chemical Physics, Volume 140 (2014) no. 19 | DOI:10.1063/1.4874159
J. Lamouroux; J.-M. Hartmann; H. Tran; B. Lavorel; M. Snels; S. Stefani; G. Piccioni Molecular dynamics simulations for CO2 spectra. IV. Collisional line-mixing in infrared and Raman bands, The Journal of Chemical Physics, Volume 138 (2013) no. 24 | DOI:10.1063/1.4811518
Erin T. McCole; Johanan H. Odhner; Dmitri A. Romanov; Robert J. Levis Spectral-to-Temporal Amplitude Mapping Polarization Spectroscopy of Rotational Transients, The Journal of Physical Chemistry A, Volume 117 (2013) no. 29, p. 6354 | DOI:10.1021/jp402135t
Joseph D. Miller; Chloe E. Dedic; Sukesh Roy; James R. Gord; Terrence R. Meyer Interference-free gas-phase thermometry at elevated pressure using hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering, Optics Express, Volume 20 (2012) no. 5, p. 5003 | DOI:10.1364/oe.20.005003
J. H. Odhner; D. A. Romanov; E. T. McCole; J. K. Wahlstrand; H. M. Milchberg; R. J. Levis Ionization-Grating-Induced Nonlinear Phase Accumulation in Spectrally Resolved Transient Birefringence Measurements at 400 nm, Physical Review Letters, Volume 109 (2012) no. 6 | DOI:10.1103/physrevlett.109.065003
Sieghard Albert; Karen Keppler Albert; Martin Quack High‐Resolution Fourier Transform Infrared Spectroscopy, Handbook of High‐resolution Spectroscopy (2011) | DOI:10.1002/9780470749593.hrs042
Michele Marrocco CARS Spectroscopy, Handbook of Combustion (2010), p. 155 | DOI:10.1002/9783527628148.hoc026
Sukesh Roy; James R. Gord; Anil K. Patnaik Recent advances in coherent anti-Stokes Raman scattering spectroscopy: Fundamental developments and applications in reacting flows, Progress in Energy and Combustion Science, Volume 36 (2010) no. 2, p. 280 | DOI:10.1016/j.pecs.2009.11.001
Maxim F. Gelin; Christoph Riehn; Maksim Kunitski; Bernhard Brutschy Strong field effects in rotational femtosecond degenerate four-wave mixing, The Journal of Chemical Physics, Volume 132 (2010) no. 13 | DOI:10.1063/1.3367726
Ching-Yue Wang; Qi-Rong Xing; Yan-Feng Li; Ming-Lie Hu; Li Yang; Ji-Xian Gong; Wei Jia; Lu Chai Femtosecond Laser Applications in Micro/Nano Science and Technology: Nonlinear Effects in Photonic Crystal Fibers, Femtosecond Laser-Induced Forward Transfer, and Femtosecond Laser Manipulation System for Biology, Progress in Ultrafast Intense Laser Science, Volume 91 (2009), p. 233 | DOI:10.1007/978-3-540-69143-3_11
H. Tran; F. Chaussard; N. Le Cong; B. Lavorel; O. Faucher; P. Joubert Femtosecond time resolved coherent anti-Stokes Raman spectroscopy of H2–N2 mixtures in the Dicke regime: Experiments and modeling of velocity effects, The Journal of Chemical Physics, Volume 131 (2009) no. 17 | DOI:10.1063/1.3257640
T. Vieillard; F. Chaussard; D. Sugny; B. Lavorel; O. Faucher Field‐free molecular alignment of CO2 mixtures in presence of collisional relaxation, Journal of Raman Spectroscopy, Volume 39 (2008) no. 6, p. 694 | DOI:10.1002/jrs.1976
Takayoshi Kobayashi; Zhuan Wang Correlations of instantaneous transition energy and intensity of absorption peaks during molecular vibration: toward potential hyper-surface, New Journal of Physics, Volume 10 (2008) no. 6, p. 065015 | DOI:10.1088/1367-2630/10/6/065015
Sieghard Albert; Martin Quack High resolution rovibrational spectroscopy of pyrimidine: Analysis of the B1 modes ν10b and ν4 and B2 mode ν6b, Journal of Molecular Spectroscopy, Volume 243 (2007) no. 2, p. 280 | DOI:10.1016/j.jms.2007.04.009
A. M. Walser; P. Beaud; P. P. Radi; M. Tulej; T. Gerber; G. Knopp Time‐resolved investigation of the ν1 ro‐vibrational Raman band of H2CO with fs‐CARS, Journal of Raman Spectroscopy, Volume 38 (2007) no. 2, p. 147 | DOI:10.1002/jrs.1613
A. Rouzée; V. Renard; S. Guérin; O. Faucher; B. Lavorel Suppression of plasma contribution in femtosecond degenerate four‐wave mixing (fs‐DFWM) at high intensity, Journal of Raman Spectroscopy, Volume 38 (2007) no. 8, p. 969 | DOI:10.1002/jrs.1679
A. Rouzée; V. Renard; S. Guérin; O. Faucher; B. Lavorel Optical gratings induced by field-free alignment of molecules, Physical Review A, Volume 75 (2007) no. 1 | DOI:10.1103/physreva.75.013419
Yurii Loiko; Carles Serrat Coherent and phase-sensitive phenomena of ultrashort laser pulses propagating in three-levelΛ-type systems studied with the finite-difference time-domain method, Physical Review A, Volume 73 (2006) no. 6 | DOI:10.1103/physreva.73.063809
Matthew L. Costen; Kenneth G. McKendrick Orientation and alignment moments in two-color polarization spectroscopy, The Journal of Chemical Physics, Volume 122 (2005) no. 16 | DOI:10.1063/1.1883646

Cité par 25 documents. Sources : Crossref

Commentaires - Politique