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Chemical Physics Letters

Femtosecond incoherent photon echo from rhodamine B in propylene glycol. Inhomogeneous broadening and spectral diffusion at room temperature

Ruihua Zhang, Tzyy‐Schiuan Yang, Anne B. Myers

Published Aug 1, 1993• 21 citations

Abstract

Two-pulse degenerate four-wave mixing (photon-echo) experiments using “incoherent” light are reported for rhodamine B in propylene glycol and ethanol at 295 K. The signal detected in a particular direction is strongly asymmetric with respect to the time delay between the two pulses, implying that the electronic spectrum is inhomogeneously broadened on the time scale of the “waiting time” between interactions of the material system with the second and third electric fields. Similar experiments on nile blue yield a symmetric signal response characteristic of a homogeneously broadened system. The effective waiting times in experimental configurations employing parallel and perpendicularly polarized excitation pulses are discussed.

DOI: 10.1016/0009-2614(93)80140-k

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Two-pulse degenerate four-wave mixing (photon-echo) experiments using “incoherent” light are reported for rhodamine B in propylene glycol and ethanol at 295 K. The signal detected in a particular direction is strongly asymmetric with respect to the time delay between the two pulses, implying that the electronic spectrum is inhomogeneously broadened on the time scale of the “waiting time” between interactions of the material system with the second and third electric fields. Similar experiments on nile blue yield a symmetric signal response characteristic of a homogeneously broadened system. The effective waiting times in experimental configurations employing parallel and perpendicularly polarized excitation pulses are discussed.

In this paper, our multi-level theory of time-delay four wave mixing with incoherent light (TDFWM-IL) developed previously for the case of homogeneous broadening system has been extended to a generally inhomogeneous broadening case. From the present theory, a general expression of signal intensity for absorption band with both homogeneous and inhomogeneous broadening is given as a function of mutual time delay τ between two pump beams. Photon echo with incoherent light under the condition of extremely inhomogeneous broadening is discussed, and the difference of results obtained scperately from multi-level and two-level theory is pointed out. It has been demonstrated that the experiment of TDFWM-IL can also be analysed approximately by using an effective two-level model when a weak effect of inhomogeneous broadening of absorption band exists. Finally, our experimental results of TDFWM-IL obtained at zero-phonon line of ruby and absorption edge of cresyl violet film in PMMA are also presented and compared with the theory mentioned above.

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.

Stimulated photon echoes (three-pulse echoes) produced by broadband (incoherent) light pulses are discussed. A switching time corresponding to the reciprocal inhomogeneous width is predicted for the echo signal when the time interval between the first two time-overlapping, mutually coherent pulses is scanned across 0. The effect is demonstrated in an experiment performed with cesium vapor. A new method for fast sampling of atomic or molecular velocity distribution is proposed with potential applications to photodissociation and photofragmentation studies.