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Physical Review A

Photoionization of xenon below the atomic ionization potential

P. Laporte, V. Saile, R. Reininger, Uri Asaf, I. T. Steinberger

Published Dec 1, 1983• 19 citations
Publisher

Abstract

Experiments using monochromated synchrotron radiation revealed that for densities of the order of ${10}^{19}$ atoms/${\mathrm{cm}}^{3}$ and more, xenon exhibits a continuous photoresponse excitation spectrum below the atomic ionization potential (12.12 eV). The lower limit of the continuum is at about 11.10 eV, the energy difference between the ground state of the molecular ion $\mathrm{Xe}_{2}^{}{}_{}{}^{+}$ and that of the free atom. This is attributed to excimer formation at the wings of the atomic absorption lines followed by ionization and creation of xenon dimer ions. Dips appearing in the continuum very near to positions of atomic lines are discussed invoking the quasistatic theory.

DOI
10.1103/physreva.28.3613

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Experiments using monochromated synchrotron radiation revealed that for densities of the order of 1019{10}^{19}1019 atoms/cm3{\mathrm{cm}}^{3}cm3 and more, xenon exhibits a continuous photoresponse excitation spectrum below the atomic ionization potential (12.12 eV). The lower limit of the continuum is at about 11.10 eV, the energy difference between the ground state of the molecular ion Xe2+\mathrm{Xe}_{2}^{}{}_{}{}^{+}Xe2​​+ and that of the free atom. This is attributed to excimer formation at the wings of the atomic absorption lines followed by ionization and creation of xenon dimer ions. Dips appearing in the continuum very near to positions of atomic lines are discussed invoking the quasistatic theory.
Coherent control provides a quantum interference based method for controlling atomic and molecular dynamics. We report two experimental observations of different ways to achieve such a control in atomic photoionization continuum. One is the photoionization of sodium atoms, initially prepared in the 3P1/2 excited state, by a non resonant three-photon interaction with 1064-nm laser light and by a one-photon interaction with the third-harmonic field, at 355 nm. Interference between the two transition paths allows the control of the total ionization rate by varying the relative phase of the laser fields. The second experiment is the observation of the modification of the ionization continua of xenon through laser induced continuum structure (LICS). The multiphoton radiative decay of the xenon ground state into the two electronic continua, that correspond to the two fine structure levels of the ground state of the xenon ion, is varied by electromagnetically embedding a bound state of the atom into the two continua. Both experiments are performed on an atomic beam apparatus which uses a time-of-flight spectrometer for energy analyzing the emitted photoelectrons.
Two-photon absorption cross sections of ground-state xenon atoms to the 2p5{p}_{5}p5​(J=0), 2p6{p}_{6}p6​(J=2), and 2p9{p}_{9}p9​(J=2) states in the 5${p}^{5}6pconfigurationandphotoionizationcrosssectionsat193and248nmfromthe26p configuration and photoionization cross sections at 193 and 248 nm from the 26pconfigurationandphotoionizationcrosssectionsat193and248nmfromthe2{p}_{5}$ and 2p6{p}_{6}p6​ states have been determined and are compared with previous experimental and theoretical values where such exist. Fluorescence depletion spectroscopy as a method for determining excited-state photoionization cross sections is described and discussed and shown to have many attractive features. Based on our cross-section measurements, we calculate that (2+1)-photon photoionization in Xe with a laser intensity of 30 MW/cm2{\mathrm{cm}}^{2}cm2 during 25 ns at 249.6 nm, using the 2p5{p}_{5}p5​(J=0) state as an intermediate state, can produce a fractional ionization of 10%.
We report the observation of pronounced, spectrally narrow laser-induced continuum structures (LICS) in the two ionization continua of xenon. A nanosecond laser pulse with nearly transform-limited bandwidth induces a LICS by coupling the initially unpopulated 5p59p[1/2]0{5p}^{5}9p[1/2{]}_{0}5p59p[1/2]0​ state to the continuum. The LICS is probed by one-photon ionization of the 5p56p[1/2]0{5p}^{5}6p[1/2{]}_{0}5p56p[1/2]0​ state. This state is populated in an independent excitation step by an additional laser pulse acting prior to the probe and dressing pulses. The two ionization channels that leave the xenon ion in either the 2P1/2{}^{2}{P}_{1/2}2P1/2​ or the 2P3/2{}^{2}{P}_{3/2}2P3/2​ fine-structure state are detected separately by monitoring the kinetic energy of the photoelectrons in a time-of-flight electron spectrometer. A suppression of the photoelectron signal of up to 80% as compared to the far off resonance value is achieved. The line shapes reveal a Fano parameter close to zero. The LICS is identical for the coupling into the two continua. Therefore the branching ratio into the two ionization channels does not vary with the dressing-laser detuning for the coupling scheme implemented here.
Self-broadening of the 146.96 nm xenon line and 123.58 nm krypton line is studied in the density range 1-100 amagat (2.7 x 1019 — 2.7 × 1021 at. cm-3). The absorption profile is deduced from reflection experiments by a modified Kramers-Krönig analysis. A detailed discussion of the criteria for validity of available theories is given, allowing the determination of the extent to which the cases studied are related to many-body interactions and/or pure resonance forces. The quasistatic theory, in the nearest neighbour approximation, is shown to be valid for interpreting the far wings. Thus it is possible at increasing density, to underline the specific effect of the various kinds of forces : resonance, Van der Waals and repulsive, and to specify the 1u excited state potential which is found weakly attractive for Xe2 and Kr2.
The experiment demonstrates at low pressure the resonant excitation of the 3 P 1 atomic state of xenon by three-photon absorption; as the pressure increases the xenon molecules in the ground state intervene in the absorption process. The emission spectra present the VUV continua characteristic of the excimer. In the same experimental conditions but with observation along the excitation axis, the frequency tripling phenomenon is seen close to the resonance line at 147 nm and the authors have measured new values of the phase matching parameter C Xe between 145 and 147 nm.