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Journal of the Optical Society of America B

Origin and properties of polychromatic directional emission from sodium atoms

A. M. Akulshin, Felipe Pedreros Bustos, Nafia Rahaman, Dmitry Budker

Published Nov 1, 2023• 2 citations
Publisher

Abstract

The parametric and nonparametric nonlinear processes responsible for generation of directional infrared radiation in sodium vapors, excited to the 4D 5/2 energy level by resonant laser radiation, are identified by the transfer of orbital angular momentum from the pump radiation to the generated fields. We show that the optical fields generated by amplified spontaneous emission (ASE) simultaneously participate in several loops of four-wave mixing (FWM) generating new directional emission. The measured spectral linewidth of the FWM emission at 819.7 nm sets an upper limit to the linewidth of two fields resulting from ASE at 2338.6 and 9093.0 nm, assuming their spectra are uncorrelated. Understanding details of the new-field generation is central to applications such as directional laser guide stars, stand-off magnetometry, and entangled field generation.

DOI
10.1364/josab.499977

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The parametric and nonparametric nonlinear processes responsible for generation of directional infrared radiation in sodium vapors, excited to the 4D 5/2 energy level by resonant laser radiation, are identified by the transfer of orbital angular momentum from the pump radiation to the generated fields. We show that the optical fields generated by amplified spontaneous emission (ASE) simultaneously participate in several loops of four-wave mixing (FWM) generating new directional emission. The measured spectral linewidth of the FWM emission at 819.7 nm sets an upper limit to the linewidth of two fields resulting from ASE at 2338.6 and 9093.0 nm, assuming their spectra are uncorrelated. Understanding details of the new-field generation is central to applications such as directional laser guide stars, stand-off magnetometry, and entangled field generation.
The mechanisms responsible for ultraviolet to mid-infrared light generation in sodium vapours two-photon excited with continuous-wave sub-100 mW power resonant laser radiation are elucidated from orbital angular momentum transfer of the applied light to the generated fields. The measured 9.5 MHz-wide spectral linewidth of the light at 819.7 nm generated by four-wave mixing, sets an upper limit to the linewidth of two fields resulting from amplified spontaneous emission at 2338 nm and 9093 nm on population inverted transitions. Understanding details of this new-field generation is central to applications such as stand-off detection and directional laser guide stars.
Directional infrared emission at 1.37 and 5.23 μm is generated in Rb vapors that are stepwise excited by low-power cw resonant light. The radiation at 5.23 μm originating from amplified spontaneous emission on the 5D(5/2)→6P(3/2) transition and wave mixing consists of forward- and backward-directed components with distinctive spectral and spatial properties. Diffraction-limited light at 1.37 μm generated in the copropagating direction only is a product of parametric wave mixing around the 5P(3/2)→5D(5/2)→6P(3/2)→6S(1/2)→5P(3/2) transition loop. This highly nondegenerate mixing process involves one externally applied and two internally generated optical fields. Similarities between wave mixing generated blue and 1.37 μm light are demonstrated.
Frequency up- and down-conversion in warm alkali vapours over a range of applied cw laser intensities has received much attention in recent years due to promising applications in the fields of remote detection, quantum information and computing, specifically in the implementation of correlated photon pairs, photon storage and quantum memory interface to name a few. The generation of directional laser-like blue and infrared light in alkali vapours has been extensively studied. However, important details of the interplay of parametric and nonparametric nonlinear processes, such as the four-wave mixing (FWM) and amplified spontaneous emission (ASE) responsible for the new field generation, are not entirely clear.
Temporal spiking of directional infrared and ultraviolet cooperative emission from sodium vapors excited to the 4D5/24D_{5/2}4D5/2​ level with a continuous-wave resonant laser pump is analyzed. Mirrorless lasing at 2207 and 2338 nm on cascade population-inverted transitions and radiation at 330 nm generated due to four-wave mixing demonstrate a high degree of intensity correlation.
The parametric four-wave mixing (4WM) process responsible for the generation of coherent blue light in alkali vapors is a self-seeded process which starts by population inversion and amplified spontaneous emission (ASE). Lately, attention has been turned toward frequency up- and down-conversion in alkali vapors, using relatively low pump powers with CW diode lasers. In this Letter, we investigate the interplay between ASE and 4WM in rubidium (Rb) vapors by studying the mid-infrared (mid-IR) radiation emitted in the forward direction at 5.23 μm. We show that the ASE can be suppressed by 4WM in the CW regime. Thus, we demonstrate the generation of coherent mid-IR light at 5.23 μm in hot Rb vapors via parametric 4WM.
Competition between amplified spontaneous emission (ASE) and the four-wave-mixing (FWM) process has been observed under conditions of two-photon resonant excitation of the sodium 3d level. The nature of the competition is that the FWM process is able to prevent the occurrence of ASE, even though the gain of the ASE process calculated in the absence of competition effects is much larger than that of FWM. The ASE is suppressed because the fields generated by the FWM process create a new excitation pathway connecting the ground and 3d levels, and under quite general conditions this pathway interferes destructively with that due solely to the applied laser field. These effects are modeled theoretically by solving perturbatively the density-matrix equations of the atomic system, thereby determining the population in the upper level and the nonlinear polarization of the medium. The coupling between the various optical fields due to the nonlinear polarization is described by coupled amplitude equations. The solution to these equations predicts that when the wave-vector mismatch is not too large the fields evolve spatially to reach steady-state values, and that the population excited to the 3d level by the total steady-state optical field is much smaller than that due to the incident laser field alone. We have observed experimentally the suppression of ASE by FWM and have observed that this suppression does not occur when the medium is excited with counterpropagating beams that cannot efficiently excite the FWM process. In addition, we have conducted a series of experiments that shows that the degree of suppression of ASE depends on the intensity and focusing characteristics of the incident laser as expected on the basis of our theoretical model.