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Under a radiation power constraint, the maximum signal-to-quantum noise ratio obtainable for any state of a radiation field is found. This maximum value is achieved by the two-photon coherent states introduced previously to describe two-photon lasers.
Transverse spatial diffusion of phase-dispersed pulses, showing effects on dechirped pulse duration, output beam cross section and two-photon fluorescence display
The results of numerical calculations of the transient stimulated Raman scattering reported previously have been verified experimentally under conditions where both linear dispersion and self-focusing effects were negligible. The existence of a delay between maxima of the laser and Stokes pulses is experimentally demonstrated for the first time, while the pulse shortening in time via Raman scattering is established more firmly than in previous work. The incident-laser-pulse duration, generated-Stokes-pulse duration, and delay between intensity maxima for the laser and Stokes pulses were measured with the two-photon absorption-fluorescence technique. The effective phonon-dephasing time is determined via spontaneous Raman scattering. By using these measured quantities, inferences are made as to the magnitude of the transient gain and the shape of the exciting picosecond laser pulse.
Studies of particle excitation processes in the solar corona are reviewed, covering electron affinities, negative ion experiments using two-photon laser and drift tube techniques, geometrical hindrance in molecular ion formation, negative ion-molecule reactions, and negative ions in the ionosphere and astrophysics. Aspects of forbidden atomic transitions are also discussed, including the calculation of transition probabilities, the Fe II problem, and magnetic quadrupole radiation in a relativistic approximation.
The theory of multiphoton ionization for an atomic system of arbitrary complexity is developed using a density matrix formalism. An expression is obtained which determines the differential N-photon ionization cross section as a function of the polarization states of the target atom and the incident radiation. The parameters which characterize the photoelectron angular distribution are related to the general reduced matrix elements for the N-photon transition. Two-photon ionization of unpolarized atoms is treated as an illustration of the use of the theory. The dependence of the multiphoton ionization cross section on the polarization state of the incident radiation, which has been observed in two- and three-photon ionization of Cs, is accounted for by the theory. Finally, the photoelectron spin polarization produced by the multiphoton ionization of unpolarized atoms, like the analogous polarization resulting from single-photon ionization, is found to depend on the circular polarization of the incident radiation.
The theory of multiphoton ionization for an atomic system of arbitrary complexity is developed using a density matrix formalism. An expression is obtained which determines the differential N-photon ionization cross section as a function of the polarization states of the target atom and the incident radiation. The parameters which characterize the photo-electron angular distribution are related to the general reduced matrix elements for the N-photon transition. Two-photon ionization of unpolarized atoms is treated as an illustration of the use of the theory. The dependence of the multiphoton ionization cross section on the polarization state of the incident radiation, which has been observed in two- and three-photon ionization of Cs, is accounted for by the theory. Finally, the photoelectron spin polarization produced by the multiphoton ionization of unpolarized atoms, like the analogous polarization resulting from single-photon ionization, is found to depend on the circular polarization of the incident radiation.
Projects aimed at the generation of tunable visible, infrared, and ultraviolet light, and on the control of this light by means of novel mode-locking and modulation techniques are discussed. During this period the following projects have been active: (1) studies of transient mode-locking of the Nd:YAG laser and the application of short optical pulses; (2) experimental investigations of the Na-Xe excimer laser system; (3) further development of techniques for vacuum ultraviolet holography; and (4) theoretical and initial experimental studies of a new device which should prove very useful for both infrared up-conversion and generation of tunable UV radiation - a two-photon resonantly pumped frequency converter.
Simple ionic systems were studied, such as metastable autoionizing states of the negative He ion, two-photon decay spectrum of metastable He ion, optical excitation with low energy ions, and lifetime measurements of singly ionized Li and metastable He ion. Simple atomic systems were also investigated. Metastable autoionizing atomic energy levels in alkali elements were included, along with lifetime measurements of Cr-53, group 2A isotopes, and alkali metal atoms using level crossing and optical double resonance spectroscopy.
A previous study demonstrated two-photon consecutive absorption as being the most probable mechanism for the photodissociation of NO2 using a pulsed ruby laser at 6943 A. Additional data discussed here confirmed this and also examined an associated phenomenon, that of multiphoton induced fluorescence. The dissociation of NO2 by ON-O bond cleavage requires 3.4 eV, while the laser energy corresponds to 1.785 eV. The pooling of the energy of two photons would give more than enough energy to dissociate the NO2 into NO + O. Several mechanisms including (1) simultaneous absorption of two photons; (2) reaction of two singly excited NO2; (3) reaction of a singly excited NO2 with a ground state NO2; and (4) consecutive absorption of two photons were examined.
Using molecular hydrogen as a model system, we present a calculation which demonstrates the feasibility of efficient third-harmonic and sum-frequency generation of IR laser radiation by diatomic molecular gases. A conversion efficiency of 10% without phase matching is achievable with a modest laser intensity of about 20 MW/sq cm. In addition to a two-photon resonance, the efficient conversion depends on a mechanism which makes use of virtual vibronic transitions exclusively. Possible methods for phase matching are also suggested.
An overview of the Laser Isotope Separation (LIS) methodology is given together with illustrations showing a simplified version of the LIS technique, an example of the two-photon photoionization category, and a diagram depicting how the energy levels of various isotope influence the LIS process. Applications were proposed for the LIS system which, in addition to enriching uranium, could in themselves develop into programs of tremendous scope and breadth. These include the treatment of radioactive wastes from light-water nuclear reactors, enriching the deuterium isotope to make heavy-water, and enriching the light isotopes of such elements as titanium for aerospace weight-reducing programs. Economic comparisons of the LIS methodology with the current method of gaseous diffusion indicate an overwhelming advantage; the laser process promises to be 1000 times more efficient. The technique could also be utilized in chemical reactions with the tuned laser serving as a universal catalyst to determine the speed and direction of a chemical reaction.
The paper extends and improves the radiative cooling coefficient calculations of Cox and Tucker (1969) and Cox and Daltabuit (1971) for a low-density optically thin plasma with no molecules or dust, of cosmic abundances in the range from 10,000 to 100,000,000 K. Earlier rates applied to a plasma containing H, He, C, N, O, Ne, Mg, Si, and S; the present study added Ca, Fe, and Ni. For the elements included, many individual lines are calculated which previously has been averaged together. The cooling processes considered are permitted, forbidden, and semiforbidden line transitions, including contributions from dielectronic recombination and bremsstrahlung, radiative recombination, and two-photon continua. The ionization balance is calculated in collisional equilibrium using an approximate auto-ionization following inner-shell excitation and the low-density limit for the dielectronic recombination rate. Cooling in various observational bands in the soft X-ray region is determined.
Phase holograms have been formed in pure outdiffused LiNbO3 waveguides using the photorefractive effect initiated by two-photon absorption. Efficient holograms were recorded with two guided waves, of less than 100 W peak power, and less than 10 microJ optical energy. This technique automatically compensates for wave front perturbations in the guide and allows the formation of various integrated components such as wavelength multiplexers and optical switches.
A collision between two gas clouds with initial densities of approximately 10 million per cu cm, velocities of about 1000 km/s, and radii of approximately 1 pc is investigated quantitatively by coupling a calculation of the radiation spectrum resulting from the anticipated shock fronts with a computation for the conversion of this high-energy radiation into optical emission in adjacent photoionized regions. The detailed structure of the colliding clouds is discussed, and the effects of an ambient magnetic field are considered. The combined emission-line spectrum is presented along with continuum emission estimates for thermal, synchrotron, and very-high-energy bremsstrahlung mechanisms. It is shown that significant continua can be produced over the range from 300 microns to 3 keV, including a blackbody contribution from a high-density neutral region between the shock fronts, free-free and free-bound radiation from the cooling zones directly behind the shocks, and free-free, free-bound, and two-photon radiation from the photoionized regions immediately ahead of and behind the cooling zones. The theoretical spectrum of the structure resulting from the collision is found to be similar in general and in some details to those observed for typical quasars.
The EUV (100-1000 A) spectrum of an optically thin plasma over the temperature range 100,000-10 million K is calculated, and the effects of free-free, free-bound, and two-photon continuum radiation are considered. The resulting spectra are presented in graphical form, with a separate tabulation of intensities for the emission lines. Results in the 100-200 A region are compared with those of other workers, and the major sources of uncertainty in this type of calculation are discussed. The applicability of the results to EUV observations of the interstellar medium are also mentioned.
Analytical and experimental studies of the rapid transfer of stored populations from metastable states to selected target states of a different species are reported. Both laser-induced or laser-switched collision and laser-induced two-photon spontaneous emission are described. It is shown that the laser-induced collision method is particularly useful in the visible and UV spectral regions. It has applications in photochemistry, gas-phase kinetics, and in high-power, high-energy gas-phase lasers. The anti-Stokes source is useful in the VUV and soft X-ray spectral regions.
Reversible changes in solar cell performance were induced by AM1 illumination and evaluated by measuring short-circuit current, weak light spectral response, and minority carrier diffusion length. In n(+)p cells the change manifests itself as a reduced short-circuit current, a loss of the red response, and a reduction in minority carrier diffusion length. In p(+)n cells there are two-photon induced effects: (1) enhancement of the blue spectral response, presumably occurring in the p(+) layer and (2) degradation in open-circuit voltage at low light levels due to increased leakage occurring only after the junction edge is exposed to bright light. Most of these photon effects are attributed to defects in the silicon.
Na+Xe collisions in the presence of two distinct laser fields (rhodamine 110 and Nd:glass) are investigated with reference to the response to nonresonant radiation of alkali metals collisionally perturbed by a buffer gas. It is found that the excited Na-asterisk (4s)+Xe state is produced with a measurable cross section due to two-photon absorption with field intensities as low as 10 MW/sq cm.