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Le Journal de Physique Colloques

ULTRAFAST DEPHASING TIME MEASUREMENT IN CRESYL FAST VIOLET DOPED CELLULOSE BY PHOTON ECHOES WITH TEMPORALLY INCOHERENT LIGHT

Hiroki Nakatsuka, Masahiro Fujiwara, R. Kuroda

Published Oct 1, 1985• 0 citations
Publisher

Abstract

Photon echoes with broad spectrum nanosecond laser pulses have been used to measure a femtosecond dephasing time (homogeneous transverse relaxation time) T2 of the S0↔1 transition of Cresyl Fast Violet molecules in a cellulose film. The measured T2 was much shorter at a shorter wavelength 5940A than that at a longer wavelength 6250A near the band edge.

DOI
10.1051/jphyscol:1985791

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Measurement of ultrafast dephasing time of Cresyl Fast Violet in cellulose by photon echoes with incoherent light

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Ultrafast homogeneous transverse relaxation time (dephasing time) T2 of Cresyl Fast Violet in cellulose has been measured in the S0 ↔ S1 transition by photon echoes with temporally incoherent nanosecond laser pulses. At 10 K, T2 was 0.7 psec when the sample was excited 6250 Å near the long-wavelength edge of the absorption band, but it was several tens of femtoseconds at 5940 Å. The fact that T2 is shorter at shorter wavelengths can attributed to the intramolecular relaxation of Cresyl Fast Violet molecules. T2 was measured also at 80 and 300 K. At 10 K persistent nonphotochemical holes (PNPH’s) were observed, and the relations between T2 and the shapes of the PNPH’s have been considered.

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Chemical Physics Letters•Nov 1, 1988•49 citations
Photon echoes with broad spectrum nanosecond laser pulses have been used to measure a femtosecond dephasing time (homogeneous transverse relaxation time) T2 of the S0↔1 transition of Cresyl Fast Violet molecules in a cellulose film. The measured T2 was much shorter at a shorter wavelength 5940A than that at a longer wavelength 6250A near the band edge.
Ultrafast homogeneous transverse relaxation time (dephasing time) T2 of Cresyl Fast Violet in cellulose has been measured in the S0 ↔ S1 transition by photon echoes with temporally incoherent nanosecond laser pulses. At 10 K, T2 was 0.7 psec when the sample was excited 6250 Å near the long-wavelength edge of the absorption band, but it was several tens of femtoseconds at 5940 Å. The fact that T2 is shorter at shorter wavelengths can attributed to the intramolecular relaxation of Cresyl Fast Violet molecules. T2 was measured also at 80 and 300 K. At 10 K persistent nonphotochemical holes (PNPH’s) were observed, and the relations between T2 and the shapes of the PNPH’s have been considered.
Incoherent light photon echoes were observed in organic amorphous systems (cresyl violet in polyvinyl alcohol and 1,4-dihydroxyanthraquinone in polymethacrylic acid) by using temporally-incoherent nanosecond laser pulses. It was found that an echo decay curve of an organic amorphous system is composed of a sharp peak which decays very rapidly and a slowly decaying wing at the tail. We show that the persistent hole burning (PHB) spectra were reproduced by the Fourier-cosine transforms of the echo decay curves. We claim that in general, we must take into account the multi-level feature of the system in order to explain ultrafast dephasing at very low temperatures.
It has been recently pointed out that incoherent light can be used to generate coherent optical transients and that there are decided advantages in using such broad-band non-laser source to achieve very high time resolution {1,2}. When a light pulse and its time-delayed replica interact with a sample to produce the non-linear optical response, the ultimate time resolution should identify with the correlation time τC of the light field rather than with the pulse duration τL. The situation where τC ≪ τL is easily obtained with broad-band incoherent light sources. Time resolution in the femtosecond range is then attainable using nanosecond light pulses. This has been recently demonstrated through the observation of the relaxation of photon echoes in Nd3+-doped silicate glass {1,2}. In these cases, attention is focused on the measurement of fast homogeneous decay rates and the inhomogeneous broadening ΩD is assumed to be much larger than the spectral width of the excitation light.
Photon echo and non-photochemical hole burning experiments on cresyl violet in ethanol glass are reported. At 1.5 K the optical dephasing time measured by the picosecond echo is eight times longer than the time measured by hole burning because of the difference in the time scales associated with the measurements. The observed temperature dependence arises from the glass's two-level systems and from a pseudolocal phonon mode at higher temperatures. Comparing the ratios of the echo to hole burning dephasing times for cresyl violet and resornfin, suggests that their dephasing is influenced by the nature of their ethanol solvation shells in addition to the dynamics of the bulk ethanol.