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

Journal of the Optical Society of America B

Polarization spectra of homogeneously and inhomogeneously broadened two-level systems

A. Marcano O., L. Marquez, L. Aranguren, M. Salazar

Published Nov 1, 1990• 12 citations
Publisher

Abstract

Polarization spectra of homogeneously and inhomogeneously broadened two-level systems are calculated. The observed remarkable differences can be used for the identification of the type of broadening. Experimental evidence of the spectral homogeneity of an ethanol solution of Malachite Green Oxalate is presented.
DOI
10.1364/josab.7.002145

Related papers

Nonlinear spectra of a homogeneously and inhomogeneously broadened two-level system

Amenaida Ferrer Marcano, O. M. C. Salazar, J. L. Paz +2 more

Polarization and Rayleigh type optical mixing spectra of a homogeneously and inhomogeneously broadened two-level system are calculated. We show that the nonlinear signal has contributions from the population pulsation and saturation effect. In the homogeneous system these effects can induce an asymmetric spectrum when the probe frequency is different from the resonant value. In the inhomogeneous system the spectral response is always symmetric independent of the probe frequency value. Line saturation and dynamic stark splitting are substantially reduced in the inhomogeneous case. The mentioned differences can be used to identify the type of broadening of a given spectral line.

Annual Meeting Optical Society of America•Jan 1, 1989•0 citations

Resonant Rayleigh-type optical mixing spectra of homogeneously and inhomogeneously broadened two-level systems

O. Arístides Marcano, Isaac Reif, José Luis Paz +1 more

Resonant Rayleigh-type optical mixing spectra for homogeneously and inhomogeneously broadened two-level systems are calculated. Differences in the forms of the spectra, such as symmetry, saturation and AC Stark splitting are presented. The observed differences can be used to discriminate whether the spectrum is homogeneously or inhomogeneously broadened.

Journal of Physics B Atomic Molecular and Optical Physics•Apr 14, 1990•3 citations

Spectral-diffusion effects in polarization spectroscopy

F. García–Golding

The effect of cross relaxation on the third-order nonlinear susceptibility, χ(3) (−ω2, ω1, −ω1, ω2), describing polarization spectroscopy experiments is calculated with a density matrix formalism. By using a model of inhomogeneously broadened two-level systems with a reservoir state and allowing for cross relaxation within the inhomogeneous line, we find that both the ratio of the maximum signal at ω1 = ω2 to the background and the broad component resembling the absorption band depend on the cross-relaxation rate. Also, one additional component with a characteristic width of the order of the spectral-diffusion rate Γ3 is expected to appear, depending on the value of this parameter. Furthermore, we estimate from published data [ Phys. Rev. A17, 1439 ( 1978)] the product of the transverse-relaxation time times the cross-relaxation time T2T3 to be 0.014 psec2 for cyanine dye and 0.0009 psec2 for malachite green oxalate.

Journal of the Optical Society of America•Jan 1, 1983•10 citations

Intramolecular coupling effects on the four-wave mixing signal

Teresa Cusati, José Luis Paz, M. C. Salazar +1 more

In this work we have studied the effect of the intramolecular coupling on the spectral properties of an ensemble of two-level systems carrying homogeneously distributed resonance frequencies, considering permanent dipole moments non zero for a Malachite Green solution.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Jul 19, 1999•0 citations

Strong-field theory of nonlinear polarization spectroscopy Fundamentals and the two-level system

Wichard J. D. Beenken, Volkhard May

To formulate a description of nonlinear polarization spectroscopy that is valid over a wide range of pump intensities, we present an approach that considers any order of the external fields. The Liouville von Neumann equation governing the dynamics of a multilevel molecular system is made tractable by expansion of the particular density matrix into powers of the carrier waves of the external fields. For a two-level system a solution of the resulting set of equations to first order of the probe field but to all orders of pump field is demonstrated. A remarkable change in the homogeneously broadened line shape is obtained at high pump intensities, caused by the optical Stark effect among others. Improvements over results derived by other authors are discussed.

Journal of the Optical Society of America B•Nov 1, 1997•15 citations

Correlation analysis of spectral fluctuations in inhomogeneously broadened spectra

Valerii S Zapasskii, G. G. Kozlov

It is shown that the lineshapes of inhomogeneously broadened spectra, due to the statistical nature of their formation, exhibit spectral fluctuations. Formulas are obtained that allow one, based on correlation analysis of different realizations of the inhomogeneously broadened line, to reconstruct its homogeneous lineshape and to evaluate the number of centers involved in its formation. The magnitude of these spectral fluctuations is estimated and it is shown that the proposed method can be efficiently used in practice.

Optics Express•Apr 23, 2001•5 citations
Polarization and Rayleigh type optical mixing spectra of a homogeneously and inhomogeneously broadened two-level system are calculated. We show that the nonlinear signal has contributions from the population pulsation and saturation effect. In the homogeneous system these effects can induce an asymmetric spectrum when the probe frequency is different from the resonant value. In the inhomogeneous system the spectral response is always symmetric independent of the probe frequency value. Line saturation and dynamic stark splitting are substantially reduced in the inhomogeneous case. The mentioned differences can be used to identify the type of broadening of a given spectral line.
The effect of cross relaxation on the third-order nonlinear susceptibility, χ(3) (−ω2, ω1, −ω1, ω2), describing polarization spectroscopy experiments is calculated with a density matrix formalism. By using a model of inhomogeneously broadened two-level systems with a reservoir state and allowing for cross relaxation within the inhomogeneous line, we find that both the ratio of the maximum signal at ω1 = ω2 to the background and the broad component resembling the absorption band depend on the cross-relaxation rate. Also, one additional component with a characteristic width of the order of the spectral-diffusion rate Γ3 is expected to appear, depending on the value of this parameter. Furthermore, we estimate from published data [ Phys. Rev. A17, 1439 ( 1978)] the product of the transverse-relaxation time times the cross-relaxation time T2T3 to be 0.014 psec2 for cyanine dye and 0.0009 psec2 for malachite green oxalate.
To formulate a description of nonlinear polarization spectroscopy that is valid over a wide range of pump intensities, we present an approach that considers any order of the external fields. The Liouville von Neumann equation governing the dynamics of a multilevel molecular system is made tractable by expansion of the particular density matrix into powers of the carrier waves of the external fields. For a two-level system a solution of the resulting set of equations to first order of the probe field but to all orders of pump field is demonstrated. A remarkable change in the homogeneously broadened line shape is obtained at high pump intensities, caused by the optical Stark effect among others. Improvements over results derived by other authors are discussed.
It is shown that the lineshapes of inhomogeneously broadened spectra, due to the statistical nature of their formation, exhibit spectral fluctuations. Formulas are obtained that allow one, based on correlation analysis of different realizations of the inhomogeneously broadened line, to reconstruct its homogeneous lineshape and to evaluate the number of centers involved in its formation. The magnitude of these spectral fluctuations is estimated and it is shown that the proposed method can be efficiently used in practice.