The selectivity of three-step pulse photo-ionization of atoms versus the detuning delta of exciting radiation frequencies from intermediate resonance is investigated in powerful laser fields where the power broadening of the resonant transitions is at least of the order of isotope shifts. The Doppler broadening of the resonant transitions is taken into account and it is assumed that the sum frequency of both exciting laser radiations is tuned to the line centre of the two-photon transition of a selected isotope. It is shown that in this situation the photo-ionization selectivity increases so greatly with the absolute detuning mod delta mod that even in such strong fields the process of photo-ionization can be highly selective. The optimization of selective photo-ionization of atoms is discussed in connection with the decrease in the selective isotope yield with increase of the absolute detuning mod delta mod . Analytical consideration of selective three-step pulse photo-ionization in powerful laser fields, based on the density matrix formalism, is presented together with the results of numerical simulation of the 40 Ca- 48 Ca laser isotope separation process as an example.
The selectivity of three-step pulse photo-ionization of atoms versus the detuning delta of exciting radiation frequencies from intermediate resonance is investigated in powerful laser fields where the power broadening of the resonant transitions is at least of the order of isotope shifts. The Doppler broadening of the resonant transitions is taken into account and it is assumed that the sum frequency of both exciting laser radiations is tuned to the line centre of the two-photon transition of a selected isotope. It is shown that in this situation the photo-ionization selectivity increases so greatly with the absolute detuning mod delta mod that even in such strong fields the process of photo-ionization can be highly selective. The optimization of selective photo-ionization of atoms is discussed in connection with the decrease in the selective isotope yield with increase of the absolute detuning mod delta mod . Analytical consideration of selective three-step pulse photo-ionization in powerful laser fields, based on the density matrix formalism, is presented together with the results of numerical simulation of the 40 Ca- 48 Ca laser isotope separation process as an example.
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 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.
Atomic selective ionization processes provide critical ionization probability and isotopic selectivity in laser isotope separation. Aimed at the general principles of transition cross sections and ionization probabilities under various atomic hyperfine structures and laser parameters, and the optimization of atomic multi-channel photo-excitation and ionization processes of non-zero nuclear spin isotopes, the semi-classical density matrix theory of an imaginary two-step photoionization process is established with the consideration of magnetic sublevels of near-resonantly excited hyperfine levels. For determining the dimensionless transition cross sections of hyperfine transition channels, two methods are proposed in this article, i.e. the saturated excitation line-shape comparison method and weak excitation signal strength method, and a good agreement is achieved between numerical dimensionless transition cross sections and experimental results for several non-zero nuclear spin isotopes. The dependence of saturated ionization probability on laser polarization is studied systematically, and the hyperfine transition of Δ F = +1 is found to be superior to Δ F = −1, 0 in terms of saturated ionization probability. A general formula of oversaturated ionization probability is summarized for different hyperfine transitions. An interesting phenomenon called “magnetic sublevel coherence trapping” is employed to explain the inadequate ionization probability of the Δ F = −1 hyperfine transition even under the oversaturated excitation condition, and its mechanism is discussed through the temporal evolution of the density matrix elements. These numerical studies can provide beneficial references for laser isotope separation of isotopes with non-zero nuclear spin, as well as atomic laser spectroscopy.
The effective isotope-selective excitation and field ionization of the 16F5/2 thallium Rydberg states have been studied experimentally. The 16F5/2 states were excited by the two-step scheme 6P1/2→6D3/2→nF5/2 in a dense collimated atomic beam by means of monochromatic radiation from two frequency tunable lasers (λ1 = 276.9 nm, λ2 = 773–808 nm) with a mean power density of more than 1 W.The largest selectivity of excitation in this scheme takes place in the first step 6P1/2→6D3/2. The experiments showed that the main reason for the limiting selectivity excitation of the Rydberg states is the field broadening of the absorption resonances at the first and second steps of the excitation scheme. The excitation efficiency of this scheme is considerably governed by the parameters of the laser radiation at the second step and an electric field pulse.
A theoretical investigation is made of the photoionisation of a three-level medium intended for laser isotope separation. The results show that the highest ionisation efficiency can be achieved by dividing the process into two stages: coherent population inversion and photoionisation. A study is made of the possibility of inversion of three-level systems for various detunings of the laser frequencies from the radiative transition frequencies. It is shown that there are detunings for which the population of the third level is maximal for any a priori selected parameters of the medium and field. Such detunings lie near a two-photon resonance and depend on the energy density and duration of the laser pulses, and also on the dipole moments of the transitions. The suitability of this method in the case of inhomogeneously broadened optically dense media is considered. It is shown that the method is most efficient in the case of counterpropagating laser pulses. The efficiency of the method is demonstrated for ytterbium.