Raman scattering coherent

J) TIME RESOLVED COHERENT RAMAN SCATTERING (TRCRS)... 

With the advent of short pulsed lasers, investigators were able to perfonn time resolved coherent Raman scattering. In contrast to using femtosecond pulses whose spectral widtii provides the two colours needed to produce Raman coherences, discussed above, here we consider pulses having two distinct centre frequencies whose difference drives the coherence. Since the 1970s, picosecond lasers have been employed for this purpose [113. 114], and since the late 1980s femtosecond pulses have also been used [115]. Flere we shall briefly focus on the two-colour femtosecond pulsed experiments since they and the picosecond experiments are very similar in concept. 

Ulness D J, Stimson M J, Kirkwood J C and Albrecht A C 1997 Interferometric downconversion of high frequency molecular vibrations with time-frequency-resolved coherent Raman scattering using quasi-cw noisy laser light C-H stretching modes of chloroform and benzene J. Rhys. Chem. A 101 4587-91... 

Ulness D J and Albrecht A C 1997 A theory of time resolved coherent Raman scattering with spectrally tailored noisy light J. Raman Spectrosc. 28 571-8... 

Ulness D J, Kirkwood J C, Stimson M J and Albrecht A C 1997 Theory of coherent Raman scattering with... 

Okamoto H and Yoshihara K 1990 Femtosecond time-resolved coherent Raman scattering under various polarization and resonance conditions J. Opt. Soc. B7 1702-8... 

Okamoto H and Yoshihara K 1991 Femtosecond time-resolved coherent Raman scattering from p-carotene in solution. Ultrahigh frequency (11 THz) beating phenomenon and sub-picosecond vibrational relaxation Chem. Phys. Lett. 177 568-71... 

Chang T-C and DIott D D 1988 Picosecond vibrational cooling in mixed molecular crystals studied with a new coherent Raman scattering technique Chem. Phys. Lett. 147 18-24... 

Fourth-Order Coherent Raman Scattering at Buried Interfaces... 

Raman excitation. and I2s are the high-frequency and low-frequency components of the pump light pulse. A probe pulse of frequency 12 interacts with the coherence to present the optical response of the fundamental frequency 12 + C0fsl2. (c) Fourth-order coherent Raman scattering, the optical response of the second harmonic frequency 212 + co 2I2 is modulated by the vibrational coherence. 

Successful applications of fourth-order coherent Raman scattering are presented. Interface-selective detection of Raman-active vibrations is now definitely possible at buried interfaces. It can be recognized as a Raman spectroscopy with interface selectivity. Vibrational sum-frequency spectroscopy provides an interface-selective IR spectroscopy in which the vibrational coherence is created in the IR resonant transition. The two interface-selective methods are complementary, as has been experienced with Raman and IR spectroscopy in the bulk. 

I. Is it possible to observe a shift in coherent Raman scattering in the three-level system with A-type coupling We have done an experiment to obtain a femtosecond Raman gain spectrum in polydiacetylenes. The Raman spectrum is shifted to the red under increased pump (to i) intensity. By changing o>2> the amplification peak signal is to be shifted to lower frequency. If the optical Stark effect is observed, then, in principle, it should be possible to observe the effect of a high field on the coherent Raman spectrum (see Fig. 1). 

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