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Optics Letters

Observation of molecular vibrations in the time domain with incoherent laser pulses

Zhi-Quan Huang, Yanxia Xie, Guolin Huang, Hoi Sing Kwok

Published May 1, 1990• 8 citations
Publisher

Abstract

With the method of self-diffraction of incoherent light, molecular vibrations were observed in real time in various dye molecules pumped near the absorption edge. In Rhodamine 560, 35-fsec oscillations in the signal were measured, which corresponds to a vibrational frequency of 1000 cm(-1). Simultaneously, this technique can be used to deduce the ultrafast dephasing times in the molecular vibrational quasi-continuum. Dephasing times of 20 and 150 fsec were observed in Rhodamine 590 and Rhodamine 560, respectively.

DOI
10.1364/ol.15.000501

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With the method of self-diffraction of incoherent light, molecular vibrations were observed in real time in various dye molecules pumped near the absorption edge. In Rhodamine 560, 35-fsec oscillations in the signal were measured, which corresponds to a vibrational frequency of 1000 cm(-1). Simultaneously, this technique can be used to deduce the ultrafast dephasing times in the molecular vibrational quasi-continuum. Dephasing times of 20 and 150 fsec were observed in Rhodamine 590 and Rhodamine 560, respectively.
Forced light scattering using broad-bandwidth incoherent pump light (${\ensuremath{\lambda}}_{\mathit{B}}$=508 nm, full width at half maximum \ensuremath{\Delta}${\ensuremath{\lambda}}_{\mathit{B}}$=13.8 nm), and narrow-bandwidth probe light is investigated experimentally and compared with self-diffraction. Forced light scattering improves the dynamic range of measurement by an order of magnitude compared to self-diffraction. A theoretical analysis of this scheme is presented. The technique is used to measure the dephasing kinetics of solutions of crystal violet and bis-(dimethylamino)heptamethine. Resulting from the relatively large autocorrelation time of 40 fs, the experimental signals show no influence from inhomogeneous broadening of the absorption bands; the dephasing kinetics can be characterized by a dephasing time T2{\mathit{T}}_{2}T2​\ensuremath{\approxeq}10 fs and an intrinsic correlation time ${\mathrm{\ensuremath{\tau}}}_{\mathit{C}}$\ensuremath{\approxeq}30 fs with a weak modulation (center frequencies ranging from 800 to 1200 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$), which is attributed to a coherent motion of the molecule (vibration). The dephasing kinetics of crystal violet shows a close agreement with the dephasing kinetics of malachite green previously reported for two-pulse photon echoes with ultrashort pulses [P. C. Becker et al., Phys. Rev. Lett. 63, 505 (1989)].
A new method to measure picosecond or subpicosecond vibrational-dephasing dynamics with the use of incoherent or broadband light is presented theoretically and experimentally. It is based on a transient coherent Raman process with three beams. In our experimental scheme, two of them are incoherent light from a single source, and a delay time between the two is variable. A third beam has a higher frequency than the incoherent light by a vibrational energy in a molecule of interest, and is coherent in the delay-time range of the measurement. The delay-time dependence of coherent Stokes Raman scattering (CSRS) intensity offers the information about the coherence dynamics of the vibrational transition with a resolution time determined only by the correlation time of the incoherent light. For the theoretical calculation, a three-level model of the molecular system with homogeneous broadening is used, and delay-time dependences of the CSRS signal are calculated for off-resonance and resonance cases. Dephasing dynamics of the 2915-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ mode in dimethylsulfoxide was observed experimentally by the new method with the use of nanosecond laser pulses, and the result agrees well with that obtained with picosecond pulses.
Recent advances in the development of synchronously mode-locked dye-laser systems have permitted the first low-power measurement of the time-resolved dephasing dynamics of a Raman active molecular vibration. Excitation and delayed probing of the coherent ensemble of vibrators is accomplished with the help of synchronized picosecond pulse trains from two independently tunable mode-locked dye lasers. A new probe technique, based on a gain measurement, is employed that provides a signal that scales linearly with the coherent vibrational amplitude. We demonstrate this technique with the first measurement of the dephasing dynamics of the normal mode (656.5 cm−1) of CS2 in the liquid state. An exponential decay with time constant 20±1 psec is obtained for the isotropic component of the coherent scattering.
The dependence of the electronic absorption spectrum of a dye molecule on the time of delay between the excitation of the molecule by a pump-laser pulse and the probing of the absorption by a test-laser pulse is studied. The effect of dephasing of the molecular transition arising from the interaction with dissipative systems is described by a stochastic modulation of the electronic transition frequency. It is shown that in the case when the two laser pulses are short compared with the correlation time of the frequency modulation and when the spectral linewidth of the pump-laser light is smaller than the bandwidth of the equilibrium absorption spectrum, hole burning appears although the molecules have equal mean transition frequencies. This effect arises from non-Markovian correlations between the dephasings of the molecule during the actions of the pump- and the test-laser pulse. With increasing delay time the holes are smoothed out and disappear when the delay time exceeds the correlation time. Such effects were found in recent femtosecond absorption experiments by Shank et al. [in Ultrafast Phenomena V, dited by G. R. Fleming and A. E. Siegman (Springer, Berlin, 1986), p. 179].
Subpicosecond photon echo quantum beats were studied in a dye, Rhodamine 800, doped in a polymer (polyvinyl alcohol) by using an incoherent photon echo technique. At the long-wavelength tail of absorption, photon echo quantum beats were observed as the sinusoidal modulation with the frequency of about 100 cm-1, which resulted from the interference between a single vibronic line and the zero-phonon line. The dephasing time of the vibronic line and its temperature dependence were briefly studied. At nearly the peak of absorption, the quantum beats appeared as more complicated modulation, indicating the contribution from multiple vibronic lines.