Among the mainly interesting parameters of an atomic vapor laser isotope separation process is the ionization yield. This parameter can be controlled as long as the laser beam spatial intensity distribution and temporal shape are well defined and not subjected to unexpected disturbing effects such as coherent propagation phenomena, leading to spatial and temporal reshaping with hot spots and pulse lengthening and delays. On the other hand, economical considerations require optically thick atomic columns which can favor such effects. In this work, we study the photoionization yield in atomic thulium vapor when propagation effects occur. We compare our experimental results with those of a coherent propagation code describing a four level system and including inhomogeneous broadening as well as degeneracies. We choose a three step photoionization scheme.
Among the mainly interesting parameters of an atomic vapor laser isotope separation process is the ionization yield. This parameter can be controlled as long as the laser beam spatial intensity distribution and temporal shape are well defined and not subjected to unexpected disturbing effects such as coherent propagation phenomena, leading to spatial and temporal reshaping with hot spots and pulse lengthening and delays. On the other hand, economical considerations require optically thick atomic columns which can favor such effects. In this work, we study the photoionization yield in atomic thulium vapor when propagation effects occur. We compare our experimental results with those of a coherent propagation code describing a four level system and including inhomogeneous broadening as well as degeneracies. We choose a three step photoionization scheme.
The pulse deformation and time delay, which appear when the laser propagates in a thick atom vapor, influence the ionization yield and selectivity of atomic multi-step photoionization process directly. In this paper, we study the propagation of laser pulse and atomic photoionization in a thick atom vapor medium according to the atom vapor laser isotope separation. The process of atomic multi-step photoionization and the propagation of laser in a thick medium are described by density matrix equation and Maxwell equations, respectively. The medium consists of target isotope and non-target isotope, which is non-resonantly excited. Through numerical solution of the coupled equations we illustrate the propagation characteristics of laser and the influences of atom vapor parameters and laser parameters on average ionization yield and average selectivity in a thick medium. The important results of calculation are as follows:when the atom vapor medium is rather thick, the average ionization yield increases while average selectivity decreases with the increase of laser power. When the atom vapor is relatively thin, the average ionization yield and average selectivity increase with the decrease of laser power simultaneously. Besides, there is a positive time delay between two laser pulses in which case the average ionization yield of target isotope reaches its maximum value. Moreover, when the parameters of atom vapor are constant, extending the width of laser pulses as great as possible can not only increase average ionization yield and average selectivity simultaneously, but also loosen the control accuracy of time delay between laser pulses.
The atomic selective multi-step photoionization process is a critical step in laser isotope separation. In this work, we study three-step photoionization processes with non-monochromatic laser fields theoretically based on the semi-classical theory. Firstly, three bandwidth models, including the chaotic field model, de-correlation model, and phase diffusion model, are introduced into the density matrix equations. The numerical results are compared with each other comprehensively. The phase diffusion model is selected for further simulations in terms of the correspondence degree to physical practice. Subsequently, numerical calculations are carried out to identify the influences of systematic parameters, including laser parameters (Rabi frequency, bandwidth, relative time delay, frequency detuning) and atomic Doppler broadening, on photoionization processes. In order to determine the optimal match among different systematic parameters, the ionization yield of resonant isotope, and selectivity factor are adopted as evaluation indexes to guide the design and optimization process. The results in this work can provide a rewarding reference for laser isotope separation.
Numerical computations of ionization efficiency and isotope selectivity of 176 L u have been carried out for the following three-step ladder type photoionization scheme, 5 d 6 s 2 2 D 3 / 2 ( 0.0 c m − 1 ) − − − ⟶ 540.4068 n m 5 d 6 s 6 p 4 F 5 / 2 o ( 18504.58 c m − 1 ) − − − ⟶ 535.0626 n m 5 d 6 s 7 s 4 D 3 / 2 ( 37193.98 c m − 1 ) − − − ⟶ 618.0061 n m 53375 c m − 1 A u t o i o n i z a t i o n S t a t e → L u + , by invoking the density matrix formalism for the laser–atom interactions. Equations of motion have been derived for the odd isotopes by inclusion of hyperfine levels. The line shapes and their effect on the ionization efficiency and isotope selectivity have been discussed in detail. The effects of power of excitation and ionization lasers, spectral bandwidths, pulse delays, Doppler broadening of the atomic ensemble on the ionization efficiency, and degree of enrichment have been presented. Optimum conditions for the power of excitation, detunings, and other system parameters for the selective yet efficient photoionization of 176 L u have been identified.
Photoexcitation and photoionization of atoms, the central part of atom vapor laser isotope separation (AVLIS), relate to the ionization yield and isotope selectivity directly. Doppler broadening of absorption lines is one of the parameters that influence the photoexcitation and photoionization process of atoms. When evaporation temperature is high or beam equipment is absent, Doppler broadening has obvious influence on the ionization yield because most of atoms are non-resonantly excited. In this paper, we study the influences of Doppler broadening of absorption lines on a multi-step photoexcitation and photoionization process of atoms according to the facts of AVLIS. A Doppler-broadened three-level atom system with two resonant lasers is investigated. The interaction between laser field and atoms is described by a density matrix, which is calculated by fourth-order Runge-Kutta numerical method with variable steps. The results show that the ionization yield of atoms decreases with the increase of Doppler broadening of absorption lines under the same laser parameters. At a constant laser power, the ionization yield reaches its maximum value at the best laser bandwidths, which is different from that obtained without Doppler broadening, as reported in published papers. Meanwhile, the best laser bandwidth increases with the increase of Rabi frequency and Doppler broadening when other parameters are constant. Moreover, the best bandwidth of the second laser is smaller than that of the first laser in a multi-step photoionization process of atoms. Therefore, lasers should work at the best bandwidths in AVLIS for highest ionization yield. It is advantageous to make laser bandwidths slightly bigger than the best bandwidths technically for smaller fluctuation of ionization yield, owing to incoercible stochastic volatility in laser bandwidths. The ionization yield increases with the decrease of Doppler broadening, especially at the best laser bandwidths. Therefore, it is necessary to reduce Doppler broadening of atom vapor in laser ionization zone.
The population inversion in a three-level atomic system, interacting with two coherent laser pulses, occurs from the first level to the third level at the optimal detunings of the laser frequencies near the two-photon resonance. An examination is performed to see whether the energy density and time-delay of the photoionizing laser can significantly influence the ion yield for the case where the atom interacts with two coherent pulses and one photoionizing pulse incoherently coupled. The well-known three-colour, three-step, three-photon ionization scheme, which is available for the selective photoionization of 168Yb, is chosen for use in this research with the Bloch equation. It is revealed that the proper time-delay and energy density enable us to achieve higher efficiency for the selective photoionization of 168Yb, regardless of the Doppler-broadening, though the efficiency and selectivity of coherent excitation are prominently enhanced by applying the optimal detunings.
We have studied two-photon resonant three-photon ionization of atomic sodium vapor. A dye laser tuned to either the 4d or 5s two-photon allowed transition was used to excite the atom and a second more intense laser (λ = 7000 Å) was used for ionization. The ion yield was measured as a function of resonant laser intensity and detuning, the nonresonant laser intensity, and the temporal overlap of the exciting and ionizing laser pulses. We have found1 that at high laser intensities the photoionization yield decreases as the nonresonant laser intensity is increased. When tuned to the 5s level a value of ~−0.6 was obtained for the exponential index even with the resonant laser tuned to maximize the ion yield. A theoretical model including the effects of Stark shift of the ground state, power broadening of the intermediate level due to saturation of the two-photon transition and by rapid transitions to the ionization continuum was used to predict the experimental results. Good agreement between theory and experiment required the use of a photoionization cross section for the 5s level which was ~20 times greater than the accepted value. Results for photoionization from the 4d level are also presented.