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arXiv:1902.10761 · Physical Review A

Interference effect and Autler-Townes splitting in coherent blue light generated by four-wave mixing

Marco Polo Moreno de Souza, A. A. C. de Almeida, S. S. Vianna

Published Apr 8, 2019• 14 citations
arXivHTMLPDF

Abstract

An unexpected interference effect between four-wave mixing excitation routes in rubidium vapor is observed using a combination of a cw diode laser and a 1-GHz femtosecond pulse train. The generated coherent blue light is analyzed by scanning the diode frequency and the repetition rate of the frequency comb. In both cases, the cw laser induces an Autler-Townes splitting, and a large separation is observed in the doublet structure due to the configuration of copropagating fields. Remarkably, by scanning the repetition rate, a narrow peak appears as a signature of the interfering pathways. A nonperturbative treatment of the Bloch equations achieves good agreement with the experimental data and demonstrates that the interfering effect appears only when both lasers are resonant with one- and two-photon transitions for the same atomic velocity group.

DOI
10.1103/physreva.99.043410

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Effect of the odd-photon destructive interference on laser-induced transparency and multiphoton excitation and ionization in rubidium

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We report experimental results on two-color multiphoton ionization and four-wave-mixing production under conditions where one form of laser-induced transparency (LIT) occurs. Under the conditions of LIT, multiphoton-ionization line shapes obtained by tuning one laser through a two-photon resonance exhibit a pronounced Autler-Townes splitting at low concentrations, when a second laser couples the two-photon state to a third level. In this concentration region we observed a four-wave-mixing field that increased quadratically with concentration. As the concentration is increased the Autler-Townes splitting starts to decrease, and disappears completely as a critical concentration is reached. Simultaneously, the four-wave-mixing field intensity starts to level off and finally becomes concentration independent. These observations are explained in terms of odd-photon destructive interference between different excitation pathways. In rubidium, we demonstrate that above concentrations of n\ensuremath{\simeq}5\ifmmode\times\else\texttimes\fi{}${10}^{14}$ ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$ the four-wave-mixing field is concentration independent and the multiphoton-ionization line shape shows no Autler-Townes splitting, and the width of the line shape is determined by the laser bandwidth. The results presented here demonstrate that destructive interference significantly limits the high-efficiency and high-intensity nonlinear optical generation promised in early studies on LIT, at least for the multimode laser system used in the present experiment. \textcopyright{} 1996 The American Physical Society.

Physical Review A•Nov 1, 1996•8 citations
An unexpected interference effect between four-wave mixing excitation routes in rubidium vapor is observed using a combination of a cw diode laser and a 1-GHz femtosecond pulse train. The generated coherent blue light is analyzed by scanning the diode frequency and the repetition rate of the frequency comb. In both cases, the cw laser induces an Autler-Townes splitting, and a large separation is observed in the doublet structure due to the configuration of copropagating fields. Remarkably, by scanning the repetition rate, a narrow peak appears as a signature of the interfering pathways. A nonperturbative treatment of the Bloch equations achieves good agreement with the experimental data and demonstrates that the interfering effect appears only when both lasers are resonant with one- and two-photon transitions for the same atomic velocity group.
In this work, we present a set of experiments involving four-wave mixing processes in rubidium atoms. We employ several experimental configurations exploring two- and three-level systems in cascade or Λ configurations, all of which are in a copropagating geometry, to investigate different physical phenomena present in each scenario. In the first experiment, we combine a cw diode laser and a 1 GHz femtosecond pulse train to generate coherent blue light through the four-wave mixing process in hot rubidium vapor. The generated coherent signal is analyzed by scanning either the diode frequency or the repetition rate of the frequency comb. In both cases, the cw laser induces an Autler- Townes splitting with a wide separation in the doublet structure due to the configuration of copropagating fields. To model these results, we employ the density matrix formalism to write the Bloch equations and solve them numerically. The solutions allow us to explore other cases beyond those involving our experimental setup, comparing the response of the upper-level population and the generated signal coherence for homogeneously and non-homogeneously broadened systems. Moreover, in this same experiment, we also observed an unexpected interference effect between excitation routes of the four-wave mixing process when the repetition rate of the pulse train is scanned. The theoretical model demonstrates that the interfering effect appears only when the repetition rate is carefully chosen to produce a pair of modes of the frequency comb resonant with both one- and two-photon transitions for the same atomic velocity group. In the second experiment, still with a hot rubidium vapor, we explore two symmetrical degenerate four- wave mixing signals induced by two almost copropagating laser beams, with~ka and~kb wave-vectors, and detected simultaneously in the 2~ka −~kb and 2~kb −~ka directions. Each spectrum has a single peak with a short frequency separation between them, which our model indicates is due to the nonlinear behavior of the refractive indexes, a consequence of the high intensity of both input fields. Finally, we use the same experimental setup for the two symmetrical signals to study the field intensity fluctuations of the degenerate four-wave mixing signals and the transmission signals. In this case, the sample is an ensemble of cold rubidium atoms in a magneto-optical trap. There is an intensity- intensity cross-correlation between the signals due to the resonant phase-noise to amplitude-noise conversion. In this type of cold system, we can neglect the Doppler- broadening, allowing a straightforward study of the dependency of the correlations on the laser detuning. In these measurements, we observe a type of oscillation in the correlation curves that the theoretical model indicates to be connected with Rabi oscillations, revealed by the fluctuations long after the transient period.
Abstract We report on the direct observation of the frequency comb printed in the blue fluorescence excitation spectrum of rubidium vapor induced by the combined action of an ultrashort pulse train and a cw diode laser. Each laser drives one step of the 5S—5P—5D two-photon transition in a copropagating configuration and the excitation spectrum is obtained while the cw-laser frequency is scanned over the rubidium D 2 lines. Measurements of the fluorescence as a function of the diode intensity and atomic density allow us to investigate how the effect of power broadening and absorption of the diode laser blur the excitation process. The experimental results and the printing process of the comb on the Doppler profile are described well by numerical integration of the Bloch equations for a cascade three-level system.
Abstract The coherent blue light generated in rubidium vapor due to the combined action of an ultrashort pulse train and a continuous wave diode laser is investigated. Each step of the two-photon transition 5S–5P 3 / 2 –5D is excited by one of the lasers, and the induced coherence between the 5S and 6P 3 / 2 states is responsible for generating the blue beam. Measurements of the excitation spectrum reveal the frequency comb structure and allow us to identify the resonant modes responsible for inducing the nonlinear process. Further, each resonant mode excites a different group of atoms, making the process selective in atomic velocity. The signal dependency on the atomic density is characterized by a sharp growth and a rapid saturation. We also show that for high intensity of the diode laser, the Stark shift at resonance causes the signal suppression observed at low atomic density.
We describe several novel experimental effects resulting from optical coherences in multilevel atoms driven with coherent laser fields. Four configurations were explored using Rb vapor cells: lambda dark-line resonances, single beam double-lambda oscillations, and cascade two-photon transitions in co- and counter-propagating geometries. Experiments were performed with high spectral-resolution using low-power diode lasers sources and optically thick cells. Two of the most striking effects we observed are: (1) a self-oscillation that occurs at 3.0 GHz on the 85Rb hyperfine frequency when a single laser field pumps the atoms, and (2) a coherent blue-beam emission that we observe in the co-propagating cascade two-photon case. These phenomena lead to complex lineshapes, and the effects sometimes dominate the well-known 3-level coherence effects. Additional higher-order mixing or cascaded interferences are apparent in all four experimental configurations. Many of these can be viewed as multi-wave mixing enhanced by optical coherences around closed-loop paths of atomic energy levels. The effects are particularly strong when four-photon closed-loop paths with resonant energy levels are possible, as in, the double-lambda system or as a four-wave mixing “box.”
We report experimental results on two-color multiphoton ionization and four-wave-mixing production under conditions where one form of laser-induced transparency (LIT) occurs. Under the conditions of LIT, multiphoton-ionization line shapes obtained by tuning one laser through a two-photon resonance exhibit a pronounced Autler-Townes splitting at low concentrations, when a second laser couples the two-photon state to a third level. In this concentration region we observed a four-wave-mixing field that increased quadratically with concentration. As the concentration is increased the Autler-Townes splitting starts to decrease, and disappears completely as a critical concentration is reached. Simultaneously, the four-wave-mixing field intensity starts to level off and finally becomes concentration independent. These observations are explained in terms of odd-photon destructive interference between different excitation pathways. In rubidium, we demonstrate that above concentrations of n\ensuremath{\simeq}5\ifmmode\times\else\texttimes\fi{}1014{10}^{14}1014 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$ the four-wave-mixing field is concentration independent and the multiphoton-ionization line shape shows no Autler-Townes splitting, and the width of the line shape is determined by the laser bandwidth. The results presented here demonstrate that destructive interference significantly limits the high-efficiency and high-intensity nonlinear optical generation promised in early studies on LIT, at least for the multimode laser system used in the present experiment. \textcopyright{} 1996 The American Physical Society.