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Physical Review A

Double-resonance spectroscopy by a transversely nonuniform pump beam in a three-level molecular system

Gagik P. Djotyan, Jozsef S. Bakos

Published Oct 1, 1993• 3 citations
Publisher

Abstract

We present a theoretical analysis of the influence of the collimation of a strong pump beam on a small-signal-gain line shape in a three-level \ensuremath{\Lambda}-type molecular system in the regime of high pump intensity when saturation and Stark (Autler-Townes) splitting of the levels of the pumping transition take place. The cases of homogeneous and Doppler-broadened pumping transitions have been considered. A significant offset, an asymmetric deformation, and a narrowing of the gain line, i.e., a spectrum focusing, have been obtained and explained as a result of the nonlinear (dispersion) and the active (gain) wave guiding of the small signal in the field of the strong pump beam.

DOI
10.1103/physreva.48.3130

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Small-signal spectrum focusing using a strong nonuniform pumping beam

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Significant offset and narrowing of the small-signal-gain line, i.e., spectrum focusing, in a three-level molecular system at the regime of the saturation and Stark (Autler-Townes) splitting of the pumping transition in the field of a strong collimated pump beam have been obtained and explained.

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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
We present a theoretical analysis of the influence of the collimation of a strong pump beam on a small-signal-gain line shape in a three-level \ensuremath{\Lambda}-type molecular system in the regime of high pump intensity when saturation and Stark (Autler-Townes) splitting of the levels of the pumping transition take place. The cases of homogeneous and Doppler-broadened pumping transitions have been considered. A significant offset, an asymmetric deformation, and a narrowing of the gain line, i.e., a spectrum focusing, have been obtained and explained as a result of the nonlinear (dispersion) and the active (gain) wave guiding of the small signal in the field of the strong pump beam.
This paper presents a theory of lineshapes for molecular Optical-Optical Double Resonance (DR) Spectroscopy with arbitrary strength for both pump and probe fields using the steady-state solutions for the 3-level density matrix. When Doppler broadening can be neglected, the results are analytical, and the probe spectrum is a pair of Lorentzian lines that display Autler-Townes splitting, each with an angular frequency half-width half maximum equal to the relaxation rates, which are assumed to be equal. When Doppler broadening is introduced, one must resort to numerical integration except for the limit of weak pump and probe fields. When the Doppler width is assumed to be much larger than the pump and probe Rabi frequencies and the probe frequency is higher than that of the pump, the calculated DR lineshapes are found to be Lorentzian with a strong pump field limit width that is proportional to the pump Rabi frequency, which is commonly known as power broadening. However, the width does not equal that Rabi frequency and is different for co- and counter-propagating pump and probe fields. Furthermore, that broadening is largely inhomogeneous, despite the Lorentzian shape. The saturation power is found to be about 4 times higher than for the bare probe transition with the same relaxation rate, dramatically lower than that expected if the width is interpreted as homogeneous.
The dynamic Stark effect (Autler-Townes splitting and radiative shift) of a J = 0 ↔ J = 1 optical transition have been investigated. The barium atomic beam is illuminated by a strong pump beam, resonant or slightly non-resonant with the BaI resonance line (λ = 5 535 Å) ; the fluorescence induced by a weak probe beam is detected versus the probe frequency. With linear polarizations for the two beams one deals either with a two-level (parallel polarizations) or with a three-level system (perpendicular polarizations). In the latter case and for small detunings of the pump beam, the Autler-Townes doublet has been observed. For large detunings of the pump beam a single, shifted resonance has been obtained with both polarization settings. In the three-level case the observation of the passage from the Autler-Townes situation to the light-shift situation, is reported. The corresponding calculations are presented; a particular attention is paid to the case of large detunings for the pump beam (light-shift situation). The evolution calculated for the resonance curve (position and relative intensities of the peaks) when the relative polarization directions are changed is consistent with the experimental data.
The effect of an intense pump field and the chemical concentration of the solution on the forward four-wave mixing signal of molecular systems with an inhomogeneous distribution of resonance frequencies, has been studied. A perturbative treatment to all orders in the pump and to first order in the probe and signal beams, including the propagation of the fields as the variable to be studied, was used. The present results are compared to local regimes of propagation and to the case of a homogeneously distributed spectral line. The behaviour of the non-linear signal, characterized by tridimensional intensity surfaces, is explained in terms of saturation and/or absorption processes taking place under the present study conditions.
The influence of the high-pump-field intensity saturation and dynamic Stark effects on the resonant nearly degenerate four-wave-mixing signal (${\mathrm{\ensuremath{\omega}}}_{3}$=2${\mathrm{\ensuremath{\omega}}}_{1}$-${\mathrm{\ensuremath{\omega}}}_{2}$) is studied in a frequency space defined by the pump- and probe-field frequencies, ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, respectively. Variable inhomogeneous widths have been considered ranging from extremely narrow (homogeneous distribution) to extremely wide. Remarkable differences between nearly homogeneously broadened systems and extreme inhomogeneous ones are exhibited. It is shown, for the situation of homogeneous broadening, that the spectra carried on with fixed probe and fixed pump frequency values have substantial differences in shape. These differences disappear in the situation of extreme inhomogeneous broadening. Fixed-pump-frequency resonant and fixed-probe-frequency nonresonant spectra are proposed as very convenient tools to yield useful evidence about the width of the inhomogeneous molecular distribution.
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.