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

The Journal of Chemical Physics

Incoherent four-wave-mixing on nile blue and cresyl violet in glass and polymer at 5 K: Single-site line shape analysis

Yiping Zhang, Sven R. Hartmann, Fred Moshary

Published Mar 22, 1996• 8 citations
Publisher

Abstract

Time-delayed-four-wave-mixing (TDFWM) experiments performed on nile blue and cresyl violet at 5 K using incoherent laser radiation yield a response which depends dramatically on excitation conditions. Fast (femtosecond) and slow (picosecond) processes, variable peak shifts, and type I and II quantum beats are all observed according to the laser frequency ωL and bandwidth ΔωL. We model the TDFWM response on the basis of a site-independent molecular response and an associated inhomogeneous distribution function. These functions are constructed by combining information from TDFWM and fluorescence-line-narrowing (FLN) experiments.

DOI
10.1063/1.471189

Related papers

STUDY OF TIME-DELAY FOUR-WAVE MIXING WITH INCOHERENT LIGHT IN ABSORPTION BANDS II: EXPERIMENT

Ruihua Zhang, Xin Mi, Haitian Zhou +2 more

A series of experiments of time-delay four-wave mixing with incoherent light (TDFWM-IL) in absorption bands of ruby and dye molecules at 300 K-20 K are reported, which demonstrate that two-level theory fails in the interpretation of the results, and that our multilevel theory of TDFWM-IL should be applied. The following experimental results are emphasized: the normalized delay-time dependences of the signal intensity IS (τ) are not dependent on the sample temperature from 80 K to 300 K for the pump-beam wavelengths not closed to the zero-phonon line or the absorption edge as the power spectrum S0(ω) of the incoherent light source kept invariable; at low temperature of 20 K, IS(τ) is modulated periodically with a period equal to the interval of two adjacent vibrational transitions in the absorption band 4T2 of ruby, as predicted by the multilevel theory. The experiments performed at the zero-phonon line of ruby and at the absorption edge of Cresyl Violet in PMMA demonstrate that the effective two-level model is suitable to approximately analyze not only the experimental results of TDFWM-IL in the unresolved continuous absorption bands with homogeneous broadening, but also the effects of inhomogeneous broadening on the behavior of TDFWM-IL in these bands. Additionally, some data of the subpicosecond dephasing processes of these materials are also obtained for the first time.

Journal of Nonlinear Optical Physics & Materials•Oct 1, 1992•1 citation

Spontaneous and Induced Coherent Radiation Generation in Atomic Vapors

Sven R. Hartmann

The time delayed four wave mixing technique using very wide band 300 angstroms laser noise has been applied to study nile blue and relaxation times in the low femtosecond regime have been measured as well as quantum beats which reveal vibronic structure. Relaxation in multi level systems has been analyzed and applied to the results in nile blue. Attosecond beats in K vapor have been observed and analyzed. Interference effects have been observed in Na vapor which allowed the erasing of photon echo information. Linear and nonlinear effects of local field corrections have been analyzed and applied to third harmonic generation and selective reflectivity. The local field corrections are found to effect both the line shape and the response frequency. When the input fields are intense an analysis which goes beyond the slowly varying amplitude approximation reveals that the transverse profile of the input beam is modified.

•Jan 31, 1992•0 citations

Femtosecond coherent relaxation measurements using incoherent light

Fred Moshary, Y. Zhang, Richard M. Friedberg +1 more

We have used the incoherent time delayed four wave mixing technique with 400 Å wide, 5 ns long pulses to measure optical phase relaxation times in the oxazine dye molecule, nile blue, in ethanol glass at 4.5 K and in CdSSe semiconductor microcrystallites doped in glass at 300 K. Homogeneous and inhomogeneous relaxation times in the tens of femtoseconds regime are obtained.

AIP conference proceedings•Jan 1, 1993•0 citations

MULTILEVEL THEORY OF TIME-DELAY FOUR-WAVE MIXING WITH INCOHERENT LIGHT——INHOMO-GENEOUS BROADENING CASE

ZHANG RUI-HUA, Xin Mi, ZHOU HAI-TIAN +3 more

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.

Acta Physica Sinica•Jan 1, 1991•0 citations

INTERFERENCE-BEAT MODULATION IN TIME-DELAY FOUR-WAVE MIXING WITH INCOHERENT LIGHT IN ABSORPTION BAND OF RUBY AT 20K

张瑞华, 周海天, 米辛 +3 more

Ⅰ. INTRODUCTIONTime-delay four-wave mixing with incoherent light(TDFWM-IL)is a new nonlinearoptical time-domain technique developed in recent years for studying ultrafast relaxation processes by employing nanosecond pulses or even CW laser sources. Theoretically, two-

中国科学通报：英文版•Jan 1, 1991•0 citations

Time-delayed four-wave mixing using intense incoherent light

Raymond John Beach, D. DeBeer, Sven R. Hartmann

Time-delayed four-wave mixing (TDFWM) on the 3S-3P transition in Na vapor has been studied using intense 7-nsec pulses from a broadband laser. Large-scale 1.9-psec modulation associated with the fine structure of the 3P state is observed throughout. At low buffer-gas pressures and low Na-vapor temperatures, pulse-induced relaxation effects are observed while at higher Na-vapor temperatures an anomalous response develops. In the normal region the TDFWM signal is interpreted in terms of either accumulated free decays or photon echoes. We estimate the relaxation induced by the excitation pulses.

Physical Review A•Dec 1, 1985•90 citations
Time-delayed-four-wave-mixing (TDFWM) experiments performed on nile blue and cresyl violet at 5 K using incoherent laser radiation yield a response which depends dramatically on excitation conditions. Fast (femtosecond) and slow (picosecond) processes, variable peak shifts, and type I and II quantum beats are all observed according to the laser frequency ωL and bandwidth ΔωL. We model the TDFWM response on the basis of a site-independent molecular response and an associated inhomogeneous distribution function. These functions are constructed by combining information from TDFWM and fluorescence-line-narrowing (FLN) experiments.
A series of experiments of time-delay four-wave mixing with incoherent light (TDFWM-IL) in absorption bands of ruby and dye molecules at 300 K-20 K are reported, which demonstrate that two-level theory fails in the interpretation of the results, and that our multilevel theory of TDFWM-IL should be applied. The following experimental results are emphasized: the normalized delay-time dependences of the signal intensity IS (τ) are not dependent on the sample temperature from 80 K to 300 K for the pump-beam wavelengths not closed to the zero-phonon line or the absorption edge as the power spectrum S0(ω) of the incoherent light source kept invariable; at low temperature of 20 K, IS(τ) is modulated periodically with a period equal to the interval of two adjacent vibrational transitions in the absorption band 4T2 of ruby, as predicted by the multilevel theory. The experiments performed at the zero-phonon line of ruby and at the absorption edge of Cresyl Violet in PMMA demonstrate that the effective two-level model is suitable to approximately analyze not only the experimental results of TDFWM-IL in the unresolved continuous absorption bands with homogeneous broadening, but also the effects of inhomogeneous broadening on the behavior of TDFWM-IL in these bands. Additionally, some data of the subpicosecond dephasing processes of these materials are also obtained for the first time.
The time delayed four wave mixing technique using very wide band 300 angstroms laser noise has been applied to study nile blue and relaxation times in the low femtosecond regime have been measured as well as quantum beats which reveal vibronic structure. Relaxation in multi level systems has been analyzed and applied to the results in nile blue. Attosecond beats in K vapor have been observed and analyzed. Interference effects have been observed in Na vapor which allowed the erasing of photon echo information. Linear and nonlinear effects of local field corrections have been analyzed and applied to third harmonic generation and selective reflectivity. The local field corrections are found to effect both the line shape and the response frequency. When the input fields are intense an analysis which goes beyond the slowly varying amplitude approximation reveals that the transverse profile of the input beam is modified.
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.
Time-delayed four-wave mixing (TDFWM) on the 3S-3P transition in Na vapor has been studied using intense 7-nsec pulses from a broadband laser. Large-scale 1.9-psec modulation associated with the fine structure of the 3P state is observed throughout. At low buffer-gas pressures and low Na-vapor temperatures, pulse-induced relaxation effects are observed while at higher Na-vapor temperatures an anomalous response develops. In the normal region the TDFWM signal is interpreted in terms of either accumulated free decays or photon echoes. We estimate the relaxation induced by the excitation pulses.