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

IEEE Journal of Quantum Electronics

Spectral hole burning in dye solutions

Gerard A. Mourou

Published Jan 1, 1975• 45 citations
Publisher

Abstract

Using picopulses generated by a mode-locked ruby laser, we have measured the 3-8-Å bandwidth of a hole burned in the 0-0 transition of cryptocyanine in methanol and demonstrated the inhomogeneous chatacter of this transition. The population-rate equations are written for an inhomogeneous transition with two and four energy levels interacting with continuous or pulsed excitation. Using the numerical solutions of this model together with the experimental result we determine a transverse relaxation timeT_{2} = 0.6-1ps for cryptocyanine in methanol.

DOI
10.1109/jqe.1975.1068521

Related papers

Spectroscopic Hole Burning In Saturable Dyes

David L. Stockman

The results of frequency locking experiments with coupled ruby lasers are presented. The single axial mode characteristics of an individual saturable dye-switched laser can be understood without requiring spectroscopic hole burning in the dye. For coupled lasers in which frequency locking is observed, the existence of a spectroscopic hole seems necessary to explain the experimental results. The widths of the holes are inferred to be about 0.10 cm-1 using pyridine and 0.04 cm-1 using cyclohexanol as solvents. A relatively slow time dependent perturbation of the dye by thermal density fluctuations in the solvent yields a fluctuation in the transition energy of about 0.12 cm-1, which is in qualitative agreement with the inferred widths.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•May 17, 1969•0 citations

Saturation inhomogène des colorants dans le cas d'une excitation incohérente

Gerard A. Mourou, Marguerite-Marie Denariez

A theoretical model is developed here which describes the evolution of hole burning in solutions when the pulse duration is assumed to be longer than the transverse relaxation time T2. The double influence of T2 on the width of the initial hole and also on the transient nature of this hole is observed. A comparison of these results with some experimental measurements is performed.

Canadian Journal of Physics•Dec 1, 1974•3 citations

Persistent spectral hole-burning in electronic tranisitions of different types of lattice defects

T. Attenberger, Ilmo Sildos, Glynn D. Jones +2 more

With a ring dye laser persistent spectral hole-burning was measured by fluorescence excitation spectroscopy in the zero-phonon lines of the 2llg ↔ 2llu transition in KI:S2 − and of the 3H4 → 3P0 transition of a defect center with three D− ions in SrF2:Pr3+:D−and also in the zero-phonon line at 462.5 nm of a color center in neutron-irradiated and annealed α-Al2O3. In all three lines holes with a width in the order of 1 GHz could be obtained at 1.5 K with single frequency laser. With broad-band laser in KI:S2 − and SrF2:Pr3+:D− spectral redistribution within the full range of inhomogeneous broadening could be observed which are explained by a photophysical model based on barrier crossing in asymmetric double-well-potentials. In the case of sapphire a photobleaching process is dominant which is effective also for nonselective excitation, and the holes are thermoresistant up to 300 K.

Radiation effects and defects in solids•Nov 1, 1991•4 citations

Saturation of Depth and Polarization of Resonant and Satellite Spectral Holes Generated with Pulsed Laser Excitation

Wolfgang Drescher, Bernhard Dick

The authors consider photochem. hole burning of an inhomogeneous and isotropic ensemble of chromophores through excitation with a narrow-bandwidth source of polarized light. The authors derive expressions for the depth and anisotropy of resonant and vibronic satellite spectral holes with increasing fluence. A fit of these satn. curves to exptl. data yields the Debye-Waller factor of the system. A simple rate equation model predicts that the anisotropy of a spectral hole depends only on the angle between the transition dipoles of the burnt and the probed transitions. In expts. with pulsed lasers strong deviations from this ideal behavior are obsd. An extended theory including satn. gives a satisfactory description of this phenomenon and provides a new method for the detn. of photochem. quantum yields.

The Journal of Physical Chemistry•Mar 1, 1994•3 citations

The Shape of a Spectral Hole and Its Temporal Response at Short Burning Times in Two‐, Three,‐ and Four‐Level Systems

Inna Rebane

Abstract The shape of the spectral hole in an inhomogeneous distribution function of centres over the transition frequency is calculated for the case of a quasimonochromatic burning light pulse which characteristic duration time is comparable to the relaxation times of the excited electronic level. Two‐step spectral hole‐burning in the cases of three‐ and four‐level systems as well as one‐step processes are considered. The temporal responses of the spectral holes as spectral filters on δ‐pulse of light are found.

physica status solidi (b)•Sep 1, 1991•4 citations

Effects of spectral cross relaxation and collisional dephasing on the absorption of light by organic-dye solutions

David W. Vahey, Amnon Yariv

The nonlinear absorption of intense laser light is used to obtain information about the times required for spectral cross relaxation (${T}_{3}$) and collisional dephasing (${T}_{2}$) in organic-dye solutions. The steady-state transmission experiment of Huff and DeShazer indicates that ${T}_{2}$ is in the range 0.1-1 psec for cryptocyanine-methanol, while ${T}_{3}$ is in the range 1-10 psec. For DDI-glycerin (1, 1\ensuremath{'}-diethyl-2, 2\ensuremath{'}-dicarbocyanine-iodide-glycerin), measurements of ultrashort-pulse transmission as a function of incident energy and optical polarization suggest a value ${T}_{2}=0.4\ifmmode\pm\else\textpm\fi{}0.2$ psec for that system. These results are based on a new set of rate equations for absorption by inhomogeneously broadened organic-dye solutions. The equations display the effects of spectral cross relaxation and are not limited to light intensities less than those at which coherent interaction effects become important. For the case of ultrashort incident pulses, the equations are extended to account for excited-state absorption, the dependence of absorption on optical polarization, and the existence of a multiplicity of interacting excited states.

Physical Review A•Nov 1, 1974•25 citations
Using picopulses generated by a mode-locked ruby laser, we have measured the 3-8-Å bandwidth of a hole burned in the 0-0 transition of cryptocyanine in methanol and demonstrated the inhomogeneous chatacter of this transition. The population-rate equations are written for an inhomogeneous transition with two and four energy levels interacting with continuous or pulsed excitation. Using the numerical solutions of this model together with the experimental result we determine a transverse relaxation timeT_{2} = 0.6-1ps for cryptocyanine in methanol.
The results of frequency locking experiments with coupled ruby lasers are presented. The single axial mode characteristics of an individual saturable dye-switched laser can be understood without requiring spectroscopic hole burning in the dye. For coupled lasers in which frequency locking is observed, the existence of a spectroscopic hole seems necessary to explain the experimental results. The widths of the holes are inferred to be about 0.10 cm-1 using pyridine and 0.04 cm-1 using cyclohexanol as solvents. A relatively slow time dependent perturbation of the dye by thermal density fluctuations in the solvent yields a fluctuation in the transition energy of about 0.12 cm-1, which is in qualitative agreement with the inferred widths.
With a ring dye laser persistent spectral hole-burning was measured by fluorescence excitation spectroscopy in the zero-phonon lines of the 2llg ↔ 2llu transition in KI:S2 − and of the 3H4 → 3P0 transition of a defect center with three D− ions in SrF2:Pr3+:D−and also in the zero-phonon line at 462.5 nm of a color center in neutron-irradiated and annealed α-Al2O3. In all three lines holes with a width in the order of 1 GHz could be obtained at 1.5 K with single frequency laser. With broad-band laser in KI:S2 − and SrF2:Pr3+:D− spectral redistribution within the full range of inhomogeneous broadening could be observed which are explained by a photophysical model based on barrier crossing in asymmetric double-well-potentials. In the case of sapphire a photobleaching process is dominant which is effective also for nonselective excitation, and the holes are thermoresistant up to 300 K.
The authors consider photochem. hole burning of an inhomogeneous and isotropic ensemble of chromophores through excitation with a narrow-bandwidth source of polarized light. The authors derive expressions for the depth and anisotropy of resonant and vibronic satellite spectral holes with increasing fluence. A fit of these satn. curves to exptl. data yields the Debye-Waller factor of the system. A simple rate equation model predicts that the anisotropy of a spectral hole depends only on the angle between the transition dipoles of the burnt and the probed transitions. In expts. with pulsed lasers strong deviations from this ideal behavior are obsd. An extended theory including satn. gives a satisfactory description of this phenomenon and provides a new method for the detn. of photochem. quantum yields.
Abstract The shape of the spectral hole in an inhomogeneous distribution function of centres over the transition frequency is calculated for the case of a quasimonochromatic burning light pulse which characteristic duration time is comparable to the relaxation times of the excited electronic level. Two‐step spectral hole‐burning in the cases of three‐ and four‐level systems as well as one‐step processes are considered. The temporal responses of the spectral holes as spectral filters on δ‐pulse of light are found.
The nonlinear absorption of intense laser light is used to obtain information about the times required for spectral cross relaxation (T3{T}_{3}T3​) and collisional dephasing (T2{T}_{2}T2​) in organic-dye solutions. The steady-state transmission experiment of Huff and DeShazer indicates that T2{T}_{2}T2​ is in the range 0.1-1 psec for cryptocyanine-methanol, while T3{T}_{3}T3​ is in the range 1-10 psec. For DDI-glycerin (1, 1\ensuremath{'}-diethyl-2, 2\ensuremath{'}-dicarbocyanine-iodide-glycerin), measurements of ultrashort-pulse transmission as a function of incident energy and optical polarization suggest a value ${T}_{2}=0.4\ifmmode\pm\else\textpm\fi{}0.2$ psec for that system. These results are based on a new set of rate equations for absorption by inhomogeneously broadened organic-dye solutions. The equations display the effects of spectral cross relaxation and are not limited to light intensities less than those at which coherent interaction effects become important. For the case of ultrashort incident pulses, the equations are extended to account for excited-state absorption, the dependence of absorption on optical polarization, and the existence of a multiplicity of interacting excited states.