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Acta Optica Sinica

Transient coherent effect of two-photo resonant excitation of a high excitation state of Rb atoms

Iu S, Hong Zhang

Published Jan 1, 1983• 0 citations
OpenAlex

Abstract

We have studied the two-photon resonant excitation and enhancement effect of a high excitation state 15d in Rb atom by using a synchronously pumped tunable mode-locked dye laser and obtained the frequency up-conversion at 1.065μm→4210 A. The relationship between self-phase matching and output of UV coherent radiation output is given. This paper emphasizes the study of the transient coherent effect and dephasing process of this state. It has been shown experimentally that the maximun polarized time by two-photon resonant excitation is 120 ps and UV coherent radiation could be induced under the action of probing signal until 350ps. However up to now no report has been declared about the study of trasient coherent dephasing in higher excitation states oi atom systems. All experimental set-ups, results, principle explanation are given.

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Femtosecond-pulse two-photon resonant difference-frequency mixing in gases: A technique for tunable vacuum-ultraviolet femtosecond-pulse generation and a spectroscopic tool for studying atoms in strong laser fields

A. Nazarkin, G. Korn, Olaf Kittelmann +2 more

Two-photon resonant and near-resonant four-wave difference-frequency mixing in gases in the interaction regime when laser pulse durations are comparable to or shorter than the medium polarization relaxation time ${T}_{2}^{\ensuremath{'}}$ is investigated. The results of experimental studies of the process in Ar and Kr using pump pulses from the ArF-excimer laser are presented demonstrating a generation of tunable short pulse radiation in the range 102--124 nm. The results are discussed in terms of a theoretical model based on a self-consistent solution of the Bloch equations for the atomic transitions and the Maxwell equations for the fields. This enables one to interpret specific nonstationary resonant and quasiresonant phenomena involved in the frequency conversion process. It is shown that the femtosecond-pulse four-wave frequency-mixing technique with probe pulses significantly shorter than the pump pulses makes it possible to study the coherent dynamics of an atomic transition exposed to an intense field. Using atomic Kr as the nonlinear medium, coherent Rabi oscillations and the subsequent phase relaxation of excitation were observed under the condition of two-photon interaction of Kr with femtosecond 193-nm laser pulses. The obtained information is important for controlling and optimizing processes of two-photon resonant frequency conversion and for time-resolved studies of Rydberg states in atoms and molecules.

Physical Review A•Jul 1, 1997•19 citations

Coherent excitation, incoherent excitation, and adiabatic states

D. Grischkowsky

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.

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Coherent blue emission generated by Rb two-photon excitation using diode and femtosecond lasers

Jesus P Lopez, Marco Polo Moreno de Souza, Marcio H G de Miranda +1 more

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.

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Spectroscopic studies in the picosecond domain with synchronously mode-locked dye lasers

T. R. Royt, Chi H. Lee

Synchronous mode locking of two dye lasers was employed to obtain pairs of independently tunable picosecond pulses that were precisely synchronized in time. Overlapped pulses in strontium vapor were used to generate tunable picosecond pulses in the vacuum uv. The tunability was employed to study resonant enhancement of a four-wave parametric process by the 4d6p autoionizing resonance. Mutually separated pulses were employed to measure the build-up and decay of coherence for a two-quantum excited state. The decay was found to be faster than theoretical predictions that assume only velocity dephasing.

Applied Physics Letters•Apr 1, 1977•27 citations

Frequency up-conversion of intense, ultrashort laser pulses at maximal atomic coherence

Fabian Cipura, Patric Ackermann, Thomas Halfmann

We present experimental data on adiabatically driven frequency conversion with ultrashort (picosecond) laser pulses towards the vacuum-ultraviolet regime, enhanced by coherent population return and preparation of maximal atomic coherences. We generate the sum frequency of an intense pump pulse and a probe pulse via a two-photon resonance in xenon. When we slightly detune the pump laser from two-photon resonance, the atomic populations are adiabatically driven forth and back from the atomic ground state to an excited state. This coherent population return (CPR) prepares the medium in a transient state of maximal atomic coherence, which enhances frequency mixing with a probe laser. We thoroughly study the variation of CPR-enhanced frequency conversion with experimental parameters and compare CPR with conventional, resonantly enhanced frequency conversion. In particular, we investigate the temporal evolution of the atomic coherence and the effect of inevitable ac Stark shifts. We find that ac Stark shifts induce an asymmetry in the spectral characteristics of CPR, which nevertheless permits enhanced frequency conversion. For the case of resonantly enhanced frequency conversion, we show that the atomic coherences are maintained for several tens of picoseconds after the pump pulse, which permits time-delayed frequency conversion. Moreover, we analyze the pressure dependence of the atomic coherence' lifetime and observe a free induction decay at the two-photon coherence with the generation of a second harmonic field. These findings shall push applications of adiabatic light-matter interactions also to the regime of nonlinear optics, driven by intense laser pulses.

Physical Review A•Sep 30, 2020•2 citations

Tunable UV coherent radiation and infrared stimulated radiation generated by hybrid pumping in the Na2-Na system

Zugeng Wang, Xiaoling Tang, Kai-Chang Zhang +2 more

For the first time by means of two-photon hybrid excitation in the Na2-Na system, which is distinguished from the usual two-photon excitation in atomic vapor, tunable UV coherent radiation (between 337.6 and 339.1 nm and between 358.0 and 359.6 nm) and tunable infrared stimulated radiation (3.38-3.46 µm) were generated. By optically pumping with a pulsed dye laser scanning from 614.5 to 617.4 nm for sodium vapor in a heat-pipe oven, Na2 was excited by the first photon absorption from the X ′ Σ g + to the A ′ Σ u + state. The energy was transferred to Na by Na2*-Na collision to populate the levels 3p1/2,3/2 in Na, which was followed by another photon excitation from the same beam up to near the 5S level, resulting in SERS (3P1/2-4P and 3P3/2-4P) and OPSE(5S → 4P and 4P → 4S) radiation. Assuming the detunings of pumping frequency ω1, from ω(5S,3P3/2) and ω(5s,3p1/2) to be Δ1 and Δ2, respectively, the three UV coherent radiation components were supposed to be generated by the following mixing processes: ωUV = 2ω1 − ω(5S − 4P); ω U V ′ = 2 ω 1 − [ ω ( 5 S → 4 P ) + Δ 1 ] ; ω U V ′ ′ = 2 ω 1 − [ ω ( 5 S → 4 P ) + Δ 2 ] , and also ω U V ′ ′ ′ = 2 ω 1 − ω ( 4 P → 4 S ) . The SERS and the UV signals were tuned as the pumping wavelength was tuned. The measured wavelengths agreed well with the calculated values.

International Laser Science Conference•Jan 1, 1986•0 citations
We have studied the two-photon resonant excitation and enhancement effect of a high excitation state 15d in Rb atom by using a synchronously pumped tunable mode-locked dye laser and obtained the frequency up-conversion at 1.065μm→4210 A. The relationship between self-phase matching and output of UV coherent radiation output is given. This paper emphasizes the study of the transient coherent effect and dephasing process of this state. It has been shown experimentally that the maximun polarized time by two-photon resonant excitation is 120 ps and UV coherent radiation could be induced under the action of probing signal until 350ps. However up to now no report has been declared about the study of trasient coherent dephasing in higher excitation states oi atom systems.
All experimental set-ups, results, principle explanation are given.
Two-photon resonant and near-resonant four-wave difference-frequency mixing in gases in the interaction regime when laser pulse durations are comparable to or shorter than the medium polarization relaxation time ${T}_{2}^{\ensuremath{'}}$ is investigated. The results of experimental studies of the process in Ar and Kr using pump pulses from the ArF-excimer laser are presented demonstrating a generation of tunable short pulse radiation in the range 102--124 nm. The results are discussed in terms of a theoretical model based on a self-consistent solution of the Bloch equations for the atomic transitions and the Maxwell equations for the fields. This enables one to interpret specific nonstationary resonant and quasiresonant phenomena involved in the frequency conversion process. It is shown that the femtosecond-pulse four-wave frequency-mixing technique with probe pulses significantly shorter than the pump pulses makes it possible to study the coherent dynamics of an atomic transition exposed to an intense field. Using atomic Kr as the nonlinear medium, coherent Rabi oscillations and the subsequent phase relaxation of excitation were observed under the condition of two-photon interaction of Kr with femtosecond 193-nm laser pulses. The obtained information is important for controlling and optimizing processes of two-photon resonant frequency conversion and for time-resolved studies of Rydberg states in atoms and molecules.
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.
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.
Synchronous mode locking of two dye lasers was employed to obtain pairs of independently tunable picosecond pulses that were precisely synchronized in time. Overlapped pulses in strontium vapor were used to generate tunable picosecond pulses in the vacuum uv. The tunability was employed to study resonant enhancement of a four-wave parametric process by the 4d6p autoionizing resonance. Mutually separated pulses were employed to measure the build-up and decay of coherence for a two-quantum excited state. The decay was found to be faster than theoretical predictions that assume only velocity dephasing.
We present experimental data on adiabatically driven frequency conversion with ultrashort (picosecond) laser pulses towards the vacuum-ultraviolet regime, enhanced by coherent population return and preparation of maximal atomic coherences. We generate the sum frequency of an intense pump pulse and a probe pulse via a two-photon resonance in xenon. When we slightly detune the pump laser from two-photon resonance, the atomic populations are adiabatically driven forth and back from the atomic ground state to an excited state. This coherent population return (CPR) prepares the medium in a transient state of maximal atomic coherence, which enhances frequency mixing with a probe laser. We thoroughly study the variation of CPR-enhanced frequency conversion with experimental parameters and compare CPR with conventional, resonantly enhanced frequency conversion. In particular, we investigate the temporal evolution of the atomic coherence and the effect of inevitable ac Stark shifts. We find that ac Stark shifts induce an asymmetry in the spectral characteristics of CPR, which nevertheless permits enhanced frequency conversion. For the case of resonantly enhanced frequency conversion, we show that the atomic coherences are maintained for several tens of picoseconds after the pump pulse, which permits time-delayed frequency conversion. Moreover, we analyze the pressure dependence of the atomic coherence' lifetime and observe a free induction decay at the two-photon coherence with the generation of a second harmonic field. These findings shall push applications of adiabatic light-matter interactions also to the regime of nonlinear optics, driven by intense laser pulses.
For the first time by means of two-photon hybrid excitation in the Na2-Na system, which is distinguished from the usual two-photon excitation in atomic vapor, tunable UV coherent radiation (between 337.6 and 339.1 nm and between 358.0 and 359.6 nm) and tunable infrared stimulated radiation (3.38-3.46 µm) were generated. By optically pumping with a pulsed dye laser scanning from 614.5 to 617.4 nm for sodium vapor in a heat-pipe oven, Na2 was excited by the first photon absorption from the X ′ Σ g + to the A ′ Σ u + state. The energy was transferred to Na by Na2*-Na collision to populate the levels 3p1/2,3/2 in Na, which was followed by another photon excitation from the same beam up to near the 5S level, resulting in SERS (3P1/2-4P and 3P3/2-4P) and OPSE(5S → 4P and 4P → 4S) radiation. Assuming the detunings of pumping frequency ω1, from ω(5S,3P3/2) and ω(5s,3p1/2) to be Δ1 and Δ2, respectively, the three UV coherent radiation components were supposed to be generated by the following mixing processes: ωUV = 2ω1 − ω(5S − 4P); ω U V ′ = 2 ω 1 − [ ω ( 5 S → 4 P ) + Δ 1 ] ; ω U V ′ ′ = 2 ω 1 − [ ω ( 5 S → 4 P ) + Δ 2 ] , and also ω U V ′ ′ ′ = 2 ω 1 − ω ( 4 P → 4 S ) . The SERS and the UV signals were tuned as the pumping wavelength was tuned. The measured wavelengths agreed well with the calculated values.