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Journal of the Physical Society of Japan

Obsevation of Coherence in Two-Photon Excited Rb Vapor

Hiroki Nakatsuka, Jumpei Okada, Masahiro Matsuoka

Published Nov 1, 1974• 17 citations
Publisher

Abstract

A coherent superposition state of 5S and 5D levels of Rb vapor, when it was excited by two-photon resonant transition between these levels, was observed by applying an interrogation pulse which was non-resonant to the system. The emphasis is laid on this coherence in the atomic excitation, instead of just the population inversion, in explaining the origin of various strong collimated emissions observed by many authors. Saturation of the off diagonal density matrix element between 5S and 5D levels was observed at higher excitation level due to the population change. An analysis of the saturation is given using a simple model for the coherence of the dye laser beam.

DOI
10.1143/jpsj.37.1406

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Free Precession Beat of Two-Photon Induced Coherence in Atomic Rubidium Vapor

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Coherent excitation of an atomic excited state occurs during the propagation of near-resonant light pulses and is responsible for the induced polarization. Simultaneously, incoherent excitation occurs due to the relaxation processes described by the absorption coefficient. Here, the theory for the coherent and incoherent excitation is initially presented in terms of the traditional vector model. While a complete understanding of the two-level system is provided by the vector model, it is shown to be incomplete when the problem of directly monitoring the coherent and incoherent excitation is considered. This is because this latter problem involves more than two levels. For this more complicated multilevel problem, adiabatic states are introduced to gain further understanding. The adiabatic states are the stationary states of the atom in the presence of the near-resonant laser field; they help to explain the intimate connection between the coherent excitation and the two-photon resonance. Experimental measurements of the coherent and incoherent excitation associated with near-resonant pulse propagation in Rb vapor are presented. The double-resonance technique used a relatively strong pulsed dye laser tuned near the $5{S}_{\frac{1}{2}}\ensuremath{\leftrightarrow}5{P}_{\frac{1}{2}}$ transition (7948 \AA{}A) of Rb to produce the coherent and incoherent excitation, and a weak, tunable cw dye laser tuned in the region of the $5{P}_{\frac{1}{2}}\ensuremath{\leftrightarrow}6{D}_{\frac{3}{2}}$ transition (6206 \AA{}A) to monitor this excitation. In agreement with theory, the experimental results demonstrate that coherent excitation is responsible for two-photon absorption, while the incoherent excitation corresponds to one-photon absorption to the $5{P}_{\frac{1}{2}}$ state.

Physical Review A•Aug 1, 1976•80 citations
A coherent superposition state of 5S and 5D levels of Rb vapor, when it was excited by two-photon resonant transition between these levels, was observed by applying an interrogation pulse which was non-resonant to the system. The emphasis is laid on this coherence in the atomic excitation, instead of just the population inversion, in explaining the origin of various strong collimated emissions observed by many authors. Saturation of the off diagonal density matrix element between 5S and 5D levels was observed at higher excitation level due to the population change. An analysis of the saturation is given using a simple model for the coherence of the dye laser beam.
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.
Utilizing two-photon excitation in hot Rb vapor we demonstrate the generation of collimated optical fields at 420 and 1324 nm. Input laser beams at 780 and 776 nm enter a heated Rb vapor cell collinear and circularly polarized, driving Rb atoms to the 5D(5/2) state. Under phase-matching conditions coherence among the 5S(1/2)→5P(3/2)→5D(5/2)→6P(3/2) transitions produces a blue (420 nm) beam by four-wave mixing. We also observe a forward and backward propagating IR (1324 nm) beam, due to cascading decays through the 6S(1/2)→5(1/2) states. Power saturation of the generated beams is investigated by scaling the input powers to greater than 200 mW, resulting in a coherent blue beam of 9.1 mW power, almost an order of magnitude larger than previously achieved. We measure the dependences of both beams in relation to the Rb density, the frequency detuning between Rb ground-state hyperfine levels, and the input laser intensities.
Enhancement and reduction of the fluorescence intensity in Rb atomic vapor are observed. The reduction is due to a depopulation of the 5P - {3/2 } state upon illumination of a Rb vapor cell with light corresponding to the 5P - {3/2 }→5D - {5/2 } transition. Collisional transfer of the 5D - {5/2 } atoms to the 5D - {3/2 } state, followed by radiative decay to the 5P - {1/2 } state, creates an increase in the population of the 5P - {1/2 } state. The increase in the excited state population results in an increase in the fluorescence intensity of the 5P - {1/2 }→5S - {1/2 } transition. The laser-induced population changes are monitored by the decrease or increase of the corresponding fluorescence signals. Using the steady-state rate equations, the rate constants for the stimulated emission(i.e., 5D - {5/2 }→5P - {3/2 }) is 2.0×10 +8s + {-1 }. The cross section for the fine-structure changing collision(i.e., 5D - {5/2 }→5D - {3/2 }) is 6.4×10 + {-14 }cm +2.
Calcium vapor has been excited by two-photon absorption of a mode-locked dye-laser pulse, and emission from a coherent superposition state of the $4{s}^{2}^{1}S_{0}$ and 4s3d1D24s3d^{1}D_{2}4s3d1D2​ levels has been observed using a delayed off-resonant interrogation pulse in the picosecond regime. The emission signal intensity was measured as a function of the delay time of the interrogation pulse, and showed a peak well delayed from that of the dye-laser pulse. This reflects the fact that the induced coherence is expressed by a time integral of the excitation. The emission signal was then found to decay as a result of the Doppler effect. The above process is analyzed by Bloch and Maxwell equations. This is the first reported observation of the coherence of an atomic system induced by two-photon absorption, a coherence which persists after the passage of the excitation pulse and decays inhomogeneously as a result of thermal motion. In carrying out the experiment, deformation of the input dye-laser pulse during propagation through the two-photon resonant medium was carefully avoided.
Coherent excitation of an atomic excited state occurs during the propagation of near-resonant light pulses and is responsible for the induced polarization. Simultaneously, incoherent excitation occurs due to the relaxation processes described by the absorption coefficient. Here, the theory for the coherent and incoherent excitation is initially presented in terms of the traditional vector model. While a complete understanding of the two-level system is provided by the vector model, it is shown to be incomplete when the problem of directly monitoring the coherent and incoherent excitation is considered. This is because this latter problem involves more than two levels. For this more complicated multilevel problem, adiabatic states are introduced to gain further understanding. The adiabatic states are the stationary states of the atom in the presence of the near-resonant laser field; they help to explain the intimate connection between the coherent excitation and the two-photon resonance. Experimental measurements of the coherent and incoherent excitation associated with near-resonant pulse propagation in Rb vapor are presented. The double-resonance technique used a relatively strong pulsed dye laser tuned near the $5{S}_{\frac{1}{2}}\ensuremath{\leftrightarrow}5{P}_{\frac{1}{2}}$ transition (7948 \AA{}A) of Rb to produce the coherent and incoherent excitation, and a weak, tunable cw dye laser tuned in the region of the $5{P}_{\frac{1}{2}}\ensuremath{\leftrightarrow}6{D}_{\frac{3}{2}}$ transition (6206 \AA{}A) to monitor this excitation. In agreement with theory, the experimental results demonstrate that coherent excitation is responsible for two-photon absorption, while the incoherent excitation corresponds to one-photon absorption to the 5P125{P}_{\frac{1}{2}}5P21​​ state.