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Physical Review Letters

Observation of resonant excess-photon detachment via a window resonance in the cesium negative ion

Henrik Stapelfeldt, Harold K. Haugen

Published Nov 2, 1992• 20 citations
Publisher

Abstract

Efficient excess-photon detachment to lowest nonvanishing order is observed with long (\ensuremath{\sim}0.7 ns) optical pulses and intensities of \ensuremath{\le}6\ifmmode\times\else\texttimes\fi{}${10}^{9}$ W/${\mathrm{cm}}^{2}$. A Feshbach (``window'') resonance in ${\mathrm{Cs}}^{\mathrm{\ensuremath{-}}}$ suppresses single-photon detachment, while simultaneously enhancing the probability of absorption of one or more excess photons. The perspectives for future spectroscopic excess-photon detachment and studies of direct two-electron multiphoton detachment are briefly discussed.

DOI
10.1103/physrevlett.69.2638

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Efficient excess-photon detachment to lowest nonvanishing order is observed with long (\ensuremath{\sim}0.7 ns) optical pulses and intensities of \ensuremath{\le}6\ifmmode\times\else\texttimes\fi{}109{10}^{9}109 W/cm2{\mathrm{cm}}^{2}cm2. A Feshbach (``window'') resonance in Cs\ensuremath−{\mathrm{Cs}}^{\mathrm{\ensuremath{-}}}Cs\ensuremath− suppresses single-photon detachment, while simultaneously enhancing the probability of absorption of one or more excess photons. The perspectives for future spectroscopic excess-photon detachment and studies of direct two-electron multiphoton detachment are briefly discussed.
We report the measurement of the two-photon detachment spectrum of the 1De^{1}D^{e}1De resonance of ${\mathrm{H}}^{\ensuremath{-}}$ just below the n=2n\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}2n=2 threshold. The excess photon detachment resonance fits a Fano profile with energy 10.872(2) eV (relative to ${\mathrm{H}}^{\ensuremath{-}}$ ground state), a width of 0.0105(10) eV, and a shape parameter of $\ensuremath{-}8(2)$. To our knowledge, this describes the first time direct multiphoton excitation of a resonance has been observed in any negative atomic ion.
Multiphoton detachment of ${\mathrm{Te}}^{\mathrm{\ensuremath{-}}}$ is studied utilizing two optical fields of wavelengths \ensuremath{\sim}694 and \ensuremath{\sim}1064 nm, respectively. Three-photon detachment is resonantly enhanced when the Raman condition is satisfied for coupling of the ${\mathrm{Te}}^{\mathrm{\ensuremath{-}}}$ 5p5{\mathit{p}}^{5}p5 2^{2}2P3/2{\mathit{P}}_{3/2}P3/2​ and 2^{2}2P1/2{\mathit{P}}_{1/2}P1/2​ fine-structure states. The fine-structure splitting is determined to be 5004.7\ifmmode\pm\else\textpm\fi{}0.2 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$, which represents a 25-fold improvement over earlier measurements. The possibilities for extended spectroscopic measurements, as well as general perspectives for multiphoton experiments at high intensities, are briefly discussed.
We report the observation and study of the excess-photon absorption (EPA) phenomenon in the region of short-lived autodetaching states of negative ions at low intensities . A sensitive resonant-ionization-based technique is utilized here for the first time to investigate nonlinear processes in the continuum, including detailed studies of signal response to laser power. We demonstrate that the sensitivity of the new method is sufficient to obtain actual positions and widths of the states at the limit of low intensities. Higher intensities (i.e. above ) can lead to significant displacement of the EPA signals from the autodetaching state positions and, depending on the shape of the one-photon detachment cross section, to either broadening or narrowing of the signal peaks. The amplitude of the signal at these higher intensities typically displays a sublinear dependence on laser power.
We describe a method for calculating rates for multiphoton detachment or ionization of a two-electron system by a perturbative field. We have applied the method to ${\mathrm{H}}^{\mathrm{\ensuremath{-}}}$, and we present estimates of two- and three-photon detachment rates. In particular, we explore the 1^{1}1Se{\mathit{S}}^{\mathit{e}}Se and 1^{1}1De{\mathit{D}}^{\mathit{e}}De Feshbach resonances below the n=2 and n=3 excitation thresholds of H; these resonances lie in the ``excess-photon detachment'' regime, where one photon is already sufficient to detach the electron.
We have performed an experimental study of the atomic system ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$, for which the ground state 5s2{\mathit{s}}^{2}s2 is coupled to the autoionizing state 5${\mathit{p}}_{1/2}$6s by means of a strong resonant laser field. The investigations are based on irradiation of ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$ with intense (I\ensuremath{\le}1.5\ifmmode\times\else\texttimes\fi{}1010{10}^{10}1010 W/cm2{\mathrm{cm}}^{2}cm2) laser pulses of duration \ensuremath{\sim}1 ns. Single-photon detachment of ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$ is suppressed due to the Fano interference between transitions directly to the continuum and transitions via the autoionizing state. In contrast, two-photon absorption is at the same time resonantly enhanced since no such destructive interference is present in this process. These observations constitute experimental evidence of general features predicted from theoretical considerations of autoionizing states in strong laser fields. Furthermore, we discuss the role of autoionizing states in multiphoton double-ionization processes. Electron spectroscopy has been used to show that double ionization of ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$ primarily is the result of a sequential removal of the two electrons via an excited Rb state. The perspectives for direct two-electron ionization in negative ions are briefly discussed.