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Register a new userAutoionizing Polaritons in Attosecond Atomic Ionization
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Light-induced states are commonly observed in the photoionization spectra of laser-dressed atoms. The properties of autoionizing polaritons, entangled states of light and Auger resonances, however, are largely unexplored. We employ attosecond transient-absorption spectroscopy to study the evolution of autoionizing states in argon, dressed by a tunable femtosecond laser pulse. The avoided crossings between the $3s^{-1}4p$ and several light-induced states indicates the formation of polariton multiplets. We measure a controllable stabilization of the polaritons against ionization, in excellent agreement with emph{ab initio} theory. Using an extension of the Jaynes-Cummings model to autoionizing states, we show that this stabilization is due to the destructive interference between the Auger decay and the radiative ionization of the polaritonic components. These results give new insights into the optical control of electronic structure in the continuum, and unlock the door to applications of autoionizing polaritons in poly-electronic systems.
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We develop the two-electron attosecond streak camera under realistic conditions using a quasi-classical model. We assume extreme ultra-violet (XUV) attosecond pulses with a full width at half maximum (FWHM) of 24 attoseconds, centered at 120 eV and a streaking infrared laser field of 1600 nm, and intensity of $1.8 times 10^{12}$ W/cm$^2$. The proposed method is shown to be capable to time resolve intra-atomic collisions in double ionization.
We study photoionization of argon atoms excited by attosecond pulses using an interferometric measurement technique. We measure the difference in time delays between electrons emitted from the $3s^2$ and from the $3p^6$ shell, at different excitation energies ranging from 32 to 42 eV. The determination of single photoemission time delays requires to take into account the measurement process, involving the interaction with a probing infrared field. This contribution can be estimated using an universal formula and is found to account for a substantial fraction of the measured delay.
Tunnelling, one of the key features of quantum mechanics, ignited an ongoing debate about the value, meaning and interpretation of tunnelling time. Until recently the debate was purely theoretical, with the process considered to be instantaneous for all practical purposes. This changed with the development of ultrafast lasers and in particular, the attoclock technique that is used to probe the attosecond dynamics of electrons. Although the initial attoclock measurements hinted at instantaneous tunnelling, later experiments contradicted those findings, claiming to have measured finite tunnelling times. In each case these measurements were performed with multi-electron atoms. Atomic hydrogen (H), the simplest atomic system with a single electron, can be exactly (subject only to numerical limitations) modelled using numerical solutions of the 3D-TDSE with measured experimental parameters and acts as a convenient benchmark for both accurate experimental measurements and calculations. Here we report the first attoclock experiment performed on H and find that our experimentally determined offset angles are in excellent agreement with accurate 3D-TDSE simulations performed using our experimental pulse parameters. The same simulations with a short-range Yukawa potential result in zero offset angles for all intensities. We conclude that the offset angle measured in the attoclock experiments originates entirely from electron scattering by the long-range Coulomb potential with no contribution from tunnelling time delay. That conclusion is supported by empirical observation that the electron offset angles follow closely the simple formula for the deflection angle of electrons undergoing classical Rutherford scattering by the Coulomb potential. Thus we confirm that, in H, tunnelling is instantaneous (with an upperbound of 1.8 as) within our experimental and numerical uncertainty.
Multi-step laser resonance ionization spectroscopy of lutetium (Lu) has been performed at TRIUMFs off-line laser ion source test stand. The even-parity Rydberg series $6s^2nd$ $^2D_{3/2}$, $6s^2nd$ $^2D_{5/2}$ and $6s^2ns$ $^2S_{1/2}$ were observed converging to the 6s$^2$ ionization potential. The experimental results has been compared to previous work. 51 levels of Rydberg series $6s^2nd$ $^2D_{5/2}$ and 52 levels of Rydberg series $6s^2ns$ $^2S_{1/2}$ were reported new. Additionally six even-parity autoionization (AI) series converging to Lu ionic states $5d6s$ $^3D_1$ and $5d6s$ $^3D_2$ were observed. The level energies of these AI states were measured. The configurations of the AI states were assigned by relativistic multichannel theory (RMCT) within the framework of multichannel quantum defect theory (MQDT).
We present an experimental and theoretical energy- and angle-resolved study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral N$_2$ molecules. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from one-color two-photon ionization in coincidence. Photoionization of N$_2$ populates the X $^2Sigma^+_g$, A $^2Pi_u$, and B $^2Sigma^+_u$ ionic states of N$_2^+$, where the photoelectron angular distributions associated with the X $^2Sigma^+_g$ and A $^2Pi_u$ states both vary with changes in photoelectron kinetic energy of only a few hundred meV. We attribute the rapid evolution in the photoelectron angular distributions to the excitation and decay of dipole-forbidden autoionizing resonances that belong to series of different symmetries, all of which are members of the Hopfield series, and compete with the direct two-photon single ionization.
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