Femtosecond coherent Raman spectroscopy

Femtosecond time-resolved CARS spectroscopy is applied in order to prepare and monitor coherent states of different samples mainly in its electronic ground but also excited states. The time evolution prepared by such methods give information on the dynamics of molecular vibrations. In a first example, the fs CARS transients of iodine are investigated. Depending on the timing of the laser pulses different dynamics are reflected in the transient CARS signal. Second, we report on selective excitation of the vibrational modes in the electronic ground state of polymers of diacetylene by means of a femtosecond time-resolved CARS scheme. Control is achieved by varying the timing and the phase shape of the exciting laser pulses. Finally the electronic ground state dynamics of biologically relevant porphyrine molecules are studied with transient CARS spectroscopy.

[1]  Xiaoyuan Li,et al.  Consistent porphyrin force field. 1. Normal-mode analysis for nickel porphine and nickel tetraphenylporphine from resonance Raman and infrared spectra and isotope shifts , 1990 .

[2]  T. Joo,et al.  Time-resolved coherent Stokes Raman spectroscopy (CSRS ) of benzene , 1991 .

[3]  K. Yoshihara,et al.  Femtosecond time-resolved coherent Raman scattering from β-carotene in solution. Ultrahigh frequency (11 THz) beating phenomenon and sub-picosecond vibrational relaxation , 1991 .

[4]  A. Laubereau,et al.  Polarization interference in femtosecond CARS , 1992 .

[5]  R. Vivie-Riedle,et al.  Femtosecond Study of Multiphoton Ionization Processes in K2: From Pump−Probe to Control# , 1996 .

[6]  D. Chandler,et al.  Femtosecond time‐resolved studies of coherent vibrational Raman scattering in large gas‐phase molecules , 1995 .

[7]  R. Leonhardt,et al.  Terahertz quantum beats in molecular liquids , 1987 .

[8]  K. Yoshihara,et al.  Femtosecond time-resolved coherent Raman scattering under various polarization and resonance conditions , 1990 .

[9]  M. Schmitt,et al.  The Application of Femtosecond Time-Resolved Coherent Anti-Stokes Raman Scattering for the Investigation of Ground and Excited State Molecular Dynamics of Molecules in the Gas Phase , 1998 .

[10]  R. de Vivie-Riedle,et al.  Ultrafast detection and control of molecular dynamics. , 1999, Proceedings of the National Academy of Sciences of the United States of America.

[11]  V. Sundström,et al.  Femtochemistry and femtobiology : ultrafast reaction dynamics at atomic-scale resolution : Nobel Symposium 101, Björkborn, Sweden, September 9-12, 1996 , 1997 .

[12]  Ahmed H. Zewail,et al.  Femtochemistry: Ultrafast Dynamics of the Chemical Bond , 1994 .

[13]  Y. Adachi,et al.  Condensed phase CARS , 1988 .

[14]  T. Baumert,et al.  Femtosecond two-photon ionization spectroscopy of the B state of Na3 clusters , 1993 .

[15]  A. Laubereau,et al.  High‐precision femtosecond CARS of simple liquids , 1990 .

[16]  K. Yoshihara,et al.  Femtosecond time-resolved polarized coherent anti-Stokes Raman studies on reorientational relaxation in benzonitrile , 1993 .

[17]  R. Leonhardt,et al.  Fast dephasing processes studied with a femtosecond coherent Raman system , 1988 .

[18]  A. Laubereau,et al.  Resonant vibrational dephasing investigated by high-precision femtosecond CARS , 1992 .

[19]  M. Nissum,et al.  Polarization-sensitive resonance CARS spectroscopy of magnesium octaethylporphine , 1999 .

[20]  Uwe Stamm,et al.  Relaxation dynamics of photoexcitations in polydiacetylenes and polythiophene , 1990 .

[21]  Christopher J. Bardeen,et al.  Selective Excitation of Wavepacket Motion in the Condensed Phase Using Chirped Pulses , 1996 .

[22]  Mehta,et al.  New nonequilibrium phonon state. , 1989, Physical Review Letters.

[23]  Stuart A. Rice,et al.  Control of selectivity of chemical reaction via control of wave packet evolution , 1985 .

[24]  K. Kompa,et al.  Femtosecond CARS on H2 , 1999 .

[25]  Tzyy‐Schiuan Yang,et al.  Femtosecond electronic dynamics by time-delayed four-wave mixing with incoherent light: iodine and azulene , 1994, Ultrafast Phenomena.

[26]  G. Wegner.  Topochemical reactions of monomers with conjugated triple bonds. III. Solid-state reactivity of derivatives of diphenyldiacetylene , 1971 .

[27]  E. Schreiber.  Femtosecond real-time spectroscopy of small molecules and clusters , 1998 .

[28]  Haw Yang,et al.  Femtosecond Infrared Studies of the Dissociation and Dynamics of Transition Metal Carbonyls in Solution , 1996 .

[29]  G. Knopp,et al.  Femtosecond time-resolved coherent anti-Stokes Raman scattering for the simultaneous study of ultrafast ground and excited state dynamics: iodine vapour , 1997 .

[30]  Gustav Gerber,et al.  High laser field effects in multiphoton ionization of Na2. Experiment and quantum calculations , 1992 .

[31]  H. Schwoerer,et al.  Selective generation and control of excited vibrational wave packets in the electronic ground state of K2 , 1999 .