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At least 19 records

Polarization phenomena in multiphoton ionization of atoms

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.

Jacobs, V. L.↗

Polarization phenomena in multiphoton ionization of atoms.

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.

Jacobs, V. L.↗

Convergent perturbation analysis of intense coherent multiphoton interactions

Use has been made of flow graphs to deduce Feenberg perturbation expansions for radiative interactions. It is demonstrated that these expansions can in certain cases be summed to provide closed form expressions for the molecular response. In particular, it is shown that the coherent state response can be obtained by the summation of a continued fraction perturbation expansion for the harmonic oscillator. Anharmonicity in the lower levels is treated and its shown to introduce Rabi flopping identifiable with multiphoton transitions among isolated tightly coupled subsystems of levels. Relevance to laser induced multiphoton excitation and energy level shift calculations in the presence of a strong field are also discussed.

Gower, M. C.↗

Experimental Resonance Enhanced Multiphoton Ionization (REMPI) studies of small molecules

Resonance enhanced multiphoton ionization (REMPI) utilizes tunable dye lasers to ionize an atom or molecule by first preparing an excited state by multiphoton absorption and then ionizing that state before it can decay. This process is highly selective with respect to both the initial and resonant intermediate states of the target, and it can be extremely sensitive. In addition, the products of the REMPI process can be detected as needed by analyzing the resulting electrons, ions, fluorescence, or by additional REMPI. This points to a number of exciting opportunities for both basic and applied science. On the applied side, REMPI has great potential as an ultrasensitive, highly selective detector for trace, reactive, or transient species. On the basic side, REMPI affords an unprecedented means of exploring excited state physics and chemistry at the quantum-state-specific level. An overview of current studies of excited molecular states is given to illustrate the principles and prospects of REMPI.

Dehmer, J. L.↗

Resonant enhanced multiphoton ionization studies of atomic oxygen

In resonant enhanced multiphoton ionization (REMPI), an atom absorbs several photons making a transition to a resonant intermediate state and subsequently ionizing out of it. With currently available tunable narrow-band lasers, the extreme sensitivity of REMPI to the specific arrangement of levels can be used to selectively probe minute amounts of a single species (atom) in a host of background material. Determination of the number density of atoms from the observed REMPI signal requires a knowledge of the multiphoton ionization cross sections. The REMPI of atomic oxygen was investigated through various excitation schemes that are feasible with available light sources. Using quantum defect theory (QDT) to estimate the various atomic parameters, the REMPI dynamics in atomic oxygen were studied incorporating the effects of saturation and a.c. Stark shifts. Results are presented for REMPI probabilities for excitation through various 2p(3) (4S sup o) np(3)P and 2p(3) (4S sup o) nf(3)F levels.

Dixit, S. N.↗

Generation of High-Order Squeezing in Multiphoton Micromaser

The generation of steady state higher-order squeezing in the sense of Hong and Mandel and also of Hillery in a multiphoton micromaser is studied. The results show that the cotangent state which is generated by the coherent trapping scheme in a multiphoton micromaser can exhibit not only second-order squeezing but also fourth-order and squared field amplitude squeezings. The influence of the cavity loss on the squeezings is investigated.

Li, Fu-Li↗

Calculation of multiphoton ionization processes

We propose an accurate and efficient procedure in the calculation of multiphoton ionization processes. In addition to the calculational advantage, this procedure also enables us to study the relative contributions of the resonant and nonresonant intermediate states.

Chang, T. N.↗

Inclusion of discrete-to-continuum coupling in multiphoton excitation and dissociation calculations

A nonperturbative approach to multiphoton excitation and dissociation of molecules is presented in which coupling to the continuum is treated explicitly. Transitions among continuum levels are not modeled directly, but something of their effect is represented by assuming that the continuum population density is so low as to be effectively zero at all times. Two trial applications are briefly discussed.

Zimmerman, I. H.↗

Line broadening in multiphoton processes with a resonant intermediate transition

It is found that the line width of the excitation spectrum for multiphoton ionization is broadened much more severely than the cascade fluorescence originating from the resonant intermediate level. These results derive from the mutual effects of the ionizing and resonating transitions, which are not properly accounted for in perturbative treatments. In general, the ionization line shape can be expressed as the sum of two Lorentzian components, each with different degrees of broadening. This line shape reduces to that of the resonating transition in the limit of vanishing intensities. Moreover, the fluorescence line shape may also exhibit a second component whose amplitude may become important under certain conditions.

Wang, C. C.↗

(2 + 1) resonant enhanced multiphoton ionization of H2 via the E,F 1Sigma(+)g state

In this paper, the results of ab initio calculations of photoelectron angular distributions and vibrational branching ratios for the (2 + 1) resonant enhanced multiphoton ionization (REMPI) of H2 via the E,F 1Sigma(+)g state are reported, and these are compared with the experimental data of Anderson et al. (1984). These results show that the observed non-Franck-Condon behavior is predominantly due to the R dependence of the transition matrix elements, and to a lesser degree to the energy dependence. This work presents the first molecular REMPI study employing a correlated wave function to describe the Rydberg-valence mixing in the resonant intermediate state.

Rudolph, H.↗

Ionic rotational branching ratios in resonant enhanced multiphoton ionization of NO via the A2Sigma(+)(3s sigma) and D2Sigma(+)(3p sigma) states

Results are presented for the rotationally resolved photoelectron spectra resulting from a (2 + 1) one-color resonant enhanced multiphoton ionization (REMPI) of NO via the rotationally clean S21(11.5) and mixed S11(15.5) + R21(15.5) branches of the 0-0 transition in the D-X band. The calculations were done in the fixed-nuclei frozen core approximation. The resulting photoionization spectra, convoluted with a Lorentzian detection function, agree qualitatively with experimental results of Viswanathan et al. (1986) and support their conclusion that the nonspherical nature of the molecular potential creates a substantial l-mixing in the continuum, which in turn leads to the intense Delta N = 0 peak. The rather strong photoelectron energy dependence of the rotational branching ratios of the D 2Sigma(+) S21(11.5) line was investigated and compared to the weak energy dependence of the A 2Sigma(+) R22(21.5) line.

Rudolph, H.↗

(1 + 1) resonant enhanced multiphoton ionization via the A2Sigma(+) state of NO - Ionic rotational branching ratios and their intensity dependence

Rotational branching ratios resulting from the (1 + 1) resonant enhanced multiphoton ionization spectroscopy of NO via the 0-0 transition of the A-X band for the four possible branches that can be assigned as R(21.5) are explored using calculation performed in the frozen-core approximation at the Hartree-Fock level. The four different branches, of which three are distinctly different in the perturbative limit, have rather different branching ratios. The mixed R12 + Q22(21.5) branch, which is not intense and has the lowest transition energy, appears to give the best agreement with experimental branching ratio for parallel detection. The agreement is less satisfactory for perpendicular detection. Neither the effect of finite-acceptance angle of the photoelectron detector nor high intensities can explain the discrepancy.

Rudolph, H.↗

New electronic states of NH and ND observed by resonance enhanced multiphoton ionization spectroscopy

Resonance Enhanced MultiPhoton Ionization (REMPI) spectra of NH and ND, which reveal four new electronic states are presented. Transitions from NH a 1 delta to 3s and 3p Rydberg states in both NH and ND have been observed and rotationally analyzed. The transitions were observed in the wavelength range of 258 to 288 nm. The state assignments are: e 1 pi (3s sigma) at 82857/cm, f 1 pi (3p sigma) at 86378/cm, g 1 delta (3p pi) at 88141/cm and h 1 sigma (3p pi) at 89151/cm.

Johnson, Russell D., III↗

Quantitative determination of H2, HD, and D2 internal-state distributions by (2+1) resonance-enhanced multiphoton ionization

Results are presented of an experimental study of (2+1) resonance-enhanced multiphoton ionization (REMPI) detection of H2, HD, and D2 via the E,F two-photon transition, in which the relationship between ion signals and quantum-state populations was determined by calibration against a thermal effusive source. Vibrational and rotational correction factors were obtained for 102 rovibrational levels for v-double-prime = 0, 1, and 2 and for J-double-prime ranging from 0 to 17. These correction factors make it possible to convert ion signals into relative quantum-state populations without relying on a theoretical description of the (2+1) REMPI process.

Rinnen, Klaus-Dieter↗

Modeling of the initiation and evolution of a laser-ionized column in the lower atmosphere - 314.5 nm wavelength resonant multiphoton ionization of naturally occurring argon

A 3+1 resonant multiphoton ionization process in naturally occurring argon is studied at 314.5 nm as a candidate for providing a long ionized channel through the atmosphere. Results are presented which indicate peak electron densities up to 10 exp 8/cu cm can be created using laser intensities on the order of 10 exp 8 W/sq cm.

Fetzer, G. J.↗