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International Conference on Ultrafast Phenomena

Two dimensional analysis of integrated three pulse photon echo

Yutaka Nagasawa, Kazushige Seike, Tadayuki Muromoto, Tadashi Okada

Published Jan 1, 2002• 0 citations
Publisher

Abstract

We have carried out two-dimensional measurement of integrated three-pulse photon echo signal of Nile blue doped in poly(methyl methacrylate) (PMMA) at various temperatures (30-230 K). Rephasing and echo formation were still clear even when the population period was extended to >100 ps, indicating that spectral diffusion is a minor process in the picosecond time scale for this sample. The intramolecular vibrational relaxation did not cause a sufficient spectral diffusion.

DOI
10.1364/up.2002.me27

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Two-Dimensional Analysis of Integrated Three-Pulse Photon Echo Signals of Nile Blue Doped in PMMA

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The integrated three-pulse photon echo signal of Nile blue doped in poly(methyl methacrylate) (PMMA) was measured two-dimensionally by varying the first coherence period and the subsequent population period. The electronic dephasing time was in the femtosecond time range even at low temperatures, whereas rephasing and echo formation were still possible even when the population period was extended to >100 ps. Oscillation was present in the echo signal even when population period was extended to longer values than the dephasing time of the vibrational coherence. Echo peak shift measurement indicated a presence of small spectral diffusion in the picosecond time range. A computer simulation was carried out from a model spectral density. The phonon mode of PMMA was represented by a Brownian oscillator centered at ∼116 cm -1, and it reproduced the temperature dependence of the echo signal surprisingly well.

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Chemical Physics Letters•Aug 1, 1993•21 citations
We have carried out two-dimensional measurement of integrated three-pulse photon echo signal of Nile blue doped in poly(methyl methacrylate) (PMMA) at various temperatures (30-230 K). Rephasing and echo formation were still clear even when the population period was extended to >100 ps, indicating that spectral diffusion is a minor process in the picosecond time scale for this sample. The intramolecular vibrational relaxation did not cause a sufficient spectral diffusion.
The integrated three-pulse photon echo signal of Nile blue doped in poly(methyl methacrylate) (PMMA) was measured two-dimensionally by varying the first coherence period and the subsequent population period. The electronic dephasing time was in the femtosecond time range even at low temperatures, whereas rephasing and echo formation were still possible even when the population period was extended to >100 ps. Oscillation was present in the echo signal even when population period was extended to longer values than the dephasing time of the vibrational coherence. Echo peak shift measurement indicated a presence of small spectral diffusion in the picosecond time range. A computer simulation was carried out from a model spectral density. The phonon mode of PMMA was represented by a Brownian oscillator centered at ∼116 cm -1, and it reproduced the temperature dependence of the echo signal surprisingly well.
An alternative experimental outline to measure homodyne detected three-pulse photon-echo data is presented. The novel experimental approach allowing for online monitoring and correction of experimental timing and stability is discussed in detail using the paradigm system of Nile blue in alcohol solution. It is shown that excellent signal-to-noise ratios together with high reproducibility of the data can be routinely achieved. We report in detail on the appearance of high-frequency intramolecular vibrations in the two-dimensional three-pulse photon-echo data and suggest that besides the conventionally discussed three-pulse photon-echo peak-shift the width of the integrated echo signal as a function of population time contains identical and easily accessible information on high-frequency intramolecular vibrations. A comparison of experimental data with theoretical modeling is performed showing that the observed echo-width oscillations are in line with predictions of the Brownian oscillator model.
The time-integrated three-pulse photon echo is discussed in terms of the line-shape functions which are shown to be directly related to the solvation dynamics. By using the short-time approximation to the line-shape function, an algebraic form of the three-pulse photon echo signal S PE (τ, T ) is obtained as a function of two delay times, τ and T, between pulses. On the basis of the approximate form of the photon echo signal, the echo peak shift with respect to the second delay time (population evolution period) is derived and found to be linearly proportional to the time-dependent fluorescence Stokes shift function for times greater than the bath correlation time, τ c . In the case of intermediate inhomogeneous broadening, the asymptotic echo peak shift magnitude is found to be useful in estimating the static inhomogeneous width. To illustrate the theoretical results, an analysis of the echo peak shift measurement of IR144 in a room temperature glass, PMMA, is presented.
The three pulse stimulated echo, long known in magnetic resonance (1), has more recently been demonstrated on optical transitions(2). An interesting way of looking at the stimulated-echo-formation relies on the fact that the first two excitation pulses create an "ordered" population as a function of detuning .This ordered population can also be looked upon as a " grating " in frequency space from which a probe pulse can "reflect" an echo. Since a grating in only one of the levels suffices, a corollary is that the echo may be stimulated at some entirely different frequency ω2 than the one ω1, at which the grating was prepared. We report the observation of such a connected two-color stimulated echo(C2CSE) in a solid and use it to confirm the relaxation out of the 747 cm−1 vibrational state of the S1 manifold of pentacene in naphthalene. It has also been realized (3) that after redistribution of the initially excited population grating, that the echo may be stimulated from any state into which the grating has relaxed. We report here the first observation of such a relaxed two-color stimulated echo(R2CSE) and note that this echo can be seen as the optical analogue of the cross-relaxation peak in a two-dimensional nmr spectrum. The rise and fall of this relaxed echo can be used as a probe for the vibrational deactivation pathway(s) subsequent to excitation of various vibrational levels in the S1 manifold. Prior to discussing briefly some of the results we note that from an analysis of this echo effect it is clear that a necessary prerequiste to observation of such two-color photon echoes is that the inhomogeneous broadening on the selected transitions is strongly correlated. Furthermore we note that in these echo effects interference with stimulated emission and super -fluorescence must be avoided by using small-angle excitation pulses. Some of the results are shown in Fig.1. In (A) the decay of the C2CSE is presented with the solid line being a fit to a population decay parameter of the 747 cm-1 level of 33 psec. In (B) the rise of the R2CSE is shown where the probe wavelength is at the pure electronic transition. The dashed line is the expected echo-intensity rise if the initially excited vibration would directly decay into the vibrationless state. The mismatch between the dashed curve and the experimental one shows that intermediate levels in the relaxation pathway must exist. The solid line in (B) is a fit to a model where one intermediate bottleneck level is assumed with a lifetime of 16±2 psec. Other examples will be presented at the meeting.
The long-lived stimulated photon echo is put forward as a powerful technique to probe structural dynamics in glasses and other amorphous solids. We present results of optical dephasing measurements on several doped organic glasses (deuterated ethanol, toluene, and triethylamine) and polymers (polystyrene, polyvinylbutyral, and polymethylmethacrylate). Using a stochastic analysis within the so-called two-level-system model, we can extract from these measurements the distribution function of fluctuation rates over a huge range of time scales, varying from picoseconds to hundreds of milliseconds. We show that the dynamics, which lies at the origin of spectral diffusion, is very dependent on the glass structure and can be described by two separate hyperbolic distribution functions of fluctuation rates. From longitudinal photon echo measurements in the population dimension, we find evidence for structural dynamics which is not accounted for in the standard two-level-system model and which is related to a spatially inhomogeneous distribution of fluctuation centers.
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.