Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

International Conference on Ultrafast Phenomena

High-Yield Picosecond Photon Echoes by Photochemical Hole-Burning

Rein K. Kaarli, Alexander Rebane, Peeter Saari

Published Jan 1, 1984• 0 citations
Publisher

Abstract

The phenomenon of stimulated photon echo [1] has already been investigated in a variety of molecular systems but in all cases the magnitude of echo signals has been limited to a small fraction of the pumping pulses intensity. The main reason for that lies in a rapid relaxation of nonequilibrium population of molecular states, which hinder the formation of spectral population gratings responsible for the stimulation of retarded optical pulses.

DOI
10.1364/up.1984.the12

Related papers

Frequency - Domain Measurements of Spectral Hole Patterns Burned with Phase - Coherent Pulses

C. Michael Jefferson, Alfred Johann Meixner

Several investigations have shown that in some systems stimulated photon echoes may be obtained over times much longer than the excited state relaxation time T11,2. It has been claimed that the mechanism for this anomalously long storage time is the formation of a frequency dependent modulation of the ground state population which persists because of spectral hole-burning1. Such a population grating produced by coherent multipulse excitation and spectral hole-burning has been measured only in a few cases3.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1991•0 citations

Picosecond two-color photon echoes in doped molecular solids

Douwe A. Wiersma, D. P. Weitekamp, Koos Duppen

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.

International Conference on Ultrafast Phenomena•Jan 1, 1984•0 citations

Persistent Photochemical Hole Burning and Subpicosecond Photon Echoes by Using Diode Laser : FUTURE TECHNOLOGY

Hiroki Nakatsuka, Kazuki Inouye, Sadao Uemura +2 more

Japanese Journal of Applied Physics•Dec 25, 1989•0 citations

Dynamics of broadband accumulated spectral gratings in Tm ^3+ :YAG

Ming Tian, Jun Zhao, Zachary Cole +2 more

High-bandwidth accumulated spectral gratings are experimentally studied in Tm3+:YAG by the stimulated-photon-echo technique with a mode-locked picosecond Ti:sapphire laser system. The experimental results show that the spectral grating builds up and decays on the time scale of the metastable-state lifetime (∼10 ms), provided that the time interval of accumulating shots is of the order of the excited-state lifetime (800 µs). An echo efficiency of the order of 0.1% was achieved with pulse intensities 2 orders of magnitude less than those needed for a single-shot process. These results fit well an analytic solution of the Bloch equations and a three-level system relaxation model.

Journal of the Optical Society of America B•May 1, 2001•15 citations

Formation of stimulated photon echo by nonresonant laser pulses

L. A. Nefedev, É. I. Khakimzyanova, Guzel I. Garnaeva

Journal of Applied Spectroscopy•Jan 1, 2013•0 citations

Picosecond Two-Color Photon Echoes in Doped Molecular Solids

D. A. Wiersma, D. P. Weitekamp, Koos Duppen

Springer series in chemical physics•Jan 1, 1984•0 citations
The phenomenon of stimulated photon echo [1] has already been investigated in a variety of molecular systems but in all cases the magnitude of echo signals has been limited to a small fraction of the pumping pulses intensity. The main reason for that lies in a rapid relaxation of nonequilibrium population of molecular states, which hinder the formation of spectral population gratings responsible for the stimulation of retarded optical pulses.
Several investigations have shown that in some systems stimulated photon echoes may be obtained over times much longer than the excited state relaxation time T11,2. It has been claimed that the mechanism for this anomalously long storage time is the formation of a frequency dependent modulation of the ground state population which persists because of spectral hole-burning1. Such a population grating produced by coherent multipulse excitation and spectral hole-burning has been measured only in a few cases3.
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.
High-bandwidth accumulated spectral gratings are experimentally studied in Tm3+:YAG by the stimulated-photon-echo technique with a mode-locked picosecond Ti:sapphire laser system. The experimental results show that the spectral grating builds up and decays on the time scale of the metastable-state lifetime (∼10 ms), provided that the time interval of accumulating shots is of the order of the excited-state lifetime (800 µs). An echo efficiency of the order of 0.1% was achieved with pulse intensities 2 orders of magnitude less than those needed for a single-shot process. These results fit well an analytic solution of the Bloch equations and a three-level system relaxation model.