The effect of a weak electric field on helium doubly excited states has been analyzed by time resolved fluorescence spectroscopy as a function of the E-field amplitude and relative orientation with respect to synchrotron light polarization. In addition to the possible excitation of parity forbidden states (i.e. 2pnp 1P e ), the effect of the weak Stark mixing induces a strong variation of fluorescence signal and decay lifetime for the states with an unfavored autoionization decay. For 2pnd 1 P o states a strong quenching of the fluorescence decay is observed when the E-field is parallel to the incident light polarization due to their mixing with 2sns 1 S e dark states.
The effect of a weak electric field on helium doubly excited states has been analyzed by time resolved fluorescence spectroscopy as a function of the E-field amplitude and relative orientation with respect to synchrotron light polarization. In addition to the possible excitation of parity forbidden states (i.e. 2pnp 1P e ), the effect of the weak Stark mixing induces a strong variation of fluorescence signal and decay lifetime for the states with an unfavored autoionization decay. For 2pnd 1 P o states a strong quenching of the fluorescence decay is observed when the E-field is parallel to the incident light polarization due to their mixing with 2sns 1 S e dark states.
We have measured the lifetimes of 1Pe(n=9−−12) doubly excited states in static electric fields (1−−6kV∕cm) by observing the decay of the fluorescence signal as a function of time. The effects of the field on these helium states below the second ionization threshold are twofold: their excitation becomes possible due to the Stark mixing with the optically allowed 1Po series, and their lifetime is strongly modified by the opening of the autoionization channel, not accessible in zero field. Although the electric field represents only a tiny perturbation of the atomic potential, a substantial shortening of the lifetimes below 100ps is observed. This is the simplest quantum system where the ratio of autoionization to fluorescence decay probability can be effectively controlled by an electric field of moderate strength.
The fluorescence yield quenching of low-lying doubly excited 2pnd1Po states is observed to depend strongly on a dc electric field strength and its orientation with respect to the polarization of the incoming photon beam. The reduction of the yield accompanied by the lifetime shortening is attributed to the Stark mixing with the neighboring 2sns1Se states, which redirects the 2pnd1Po decay to the prompt autoionization channel. For $n\ensuremath{\ge}4$, the lifetimes decrease from several hundred picoseconds down to several tens of picoseconds when an electric field in the kV/cm range is applied parallel to the photon probe polarization. Practically no lifetime change is observed for polarization perpendicular to the electric field direction. The results of the complex-scaling calculations are in a good agreement with the experimental data.
Vacuum ultraviolet fluorescence decay spectra of Ar atom resonance lines excited by pulsed vacuum ultraviolet light in a synchrotron single bunch operation were obtained under a static electric field. When an atom under the static electric field was excited simultaneously to both the magnetic sublevels M=0 and ∣M∣=1 by polarized light and the observation area was asymmetric, Stark beats were observed in the fluorescent decay spectra. All observed beat frequencies varied proportionally to the square of the external electric field. The results for 8d and 9d doublet lines were compared with those obtained by the usual second order perturbation theory, assuming mixing ratios between three jl coupling scheme d-type states. The beat frequencies were also measured for other resonance lines.
The helium atom, with one nucleus and two electrons, is a prototypical system to study quantum many-body dynamics. Doubly excited states, or quantum states in which both electrons are excited by one photon, showcase electronic-correlation mediated effects. In this paper, the natural lifetimes of the doubly excited 1 P o 2 s n p Rydberg series and the 1 S e 2 p 2 dark state in helium in the 60–65 eV region are measured directly in the time domain with extreme-ultraviolet/near-infrared noncollinear attosecond four-wave-mixing (FWM) spectroscopy. The measured lifetimes agree with lifetimes deduced from spectral linewidths and theoretical predictions, and the roles of specific decay mechanisms are considered. While complex spectral line shapes in the form of Fano resonances are common in absorption spectroscopy of autoionizing states, the background-free and thus homodyned character of noncollinear FWM results exclusively in Lorentzian spectral features in the absence of strong-field effects. The onset of strong-field effects that would affect the extraction of accurate natural lifetimes in helium by FWM is determined to be approximately 0.3 Rabi cycles. This study provides a systematic understanding of the FWM parameters necessary to enable accurate lifetime extractions, which can be utilized in more complex quantum systems in the future. Published by the American Physical Society 2024
Long-lived, excited neutral particles, arising from the interaction of monochromatic synchrotron radiation with ground state He atoms, have been observed at photon energies close to the (N = 1,2,3 and 4) ionization thresholds. The measurements have been made using an unconventional experimental arrangement in which charged particles, responsible for the dominant signal in conventional photon impact studies, are prevented from reaching the detector. For , it appears that the formation, via photoexcitation, of relatively long-lived, doubly excited Rydberg states is a necessary step in the production of the observed signal. Four processes that might account for the production of the excited neutral particles are considered. The simplest, that atoms in the initial doubly excited Rydberg states are themselves directly observable, is considered unlikely. However, the lifetimes of the photoexcited double Rydberg states may be increased through the effects of electric fields present in the apparatus. Transitions from these double Rydberg states, occurring either as a result of collisions or by fluorescence, could result in metastable, singly excited neutral particles. The presence of signal related to the existence of long-lived doubly excited states could be significant in the interpretation of other photon impact measurements.
The asymmetry parameter β for fluorescence photons emitted during the radiative decay of the sp2, n +( 1 P o ), sp2, n −( 1 P o ), 2p n d( 1 P o ) and 2p n d( 3 D o ) series of helium doubly excited states, formed by the absorption of linearly polarized synchrotron radiation, has been measured. The results are compared with recent theoretical calculations (Žitnik et al 2002 Phys. Rev. A 65 032520). At high n the β parameter is shown to increase and oscillate due to the excitation of triplet states, optically accessible from the helium ground state due to spin–orbit effects.