Above 54.4 eV, two-photon double ionization of helium is dominated by a sequential absorption process, producing characteristic behavior in the single and triple differential cross sections. We show that the signature of this process is visible in the nuclear recoil cross section, integrated over all energy sharings of the ejected electrons, even below the threshold for the sequential process. Since nuclear recoil momentum imaging does not require coincident photoelectron measurement, the predicted images present a viable target for future experiments with new short-pulse VUV and soft X-ray sources.
Future metrology standards will be partly based on physical quantities computed from first principles rather than measured. In particular, a new pressure standard can be established if the dynamic polarizability of helium can be determined from theory with an uncertainty smaller than 0.2 ppm. We present calculations of the frequency-dependent part of this quantity including relativistic effects with full account of leading nuclear recoil terms and using highly optimized explicitly correlated basis sets. A particular emphasis is put on uncertainty estimates. At the He-Ne laser wavelength of 632…
The multiconfigurational time-dependent Hartree-Fock method (MCTDHF) is applied for simulations of the two-photon ionization of Helium. We present results for the single- and double ionization from the groundstate for photon energies in the non-sequential regime, and compare them to direct solutions of the Schrödinger equation using the time-dependent (full) Configuration Interaction method (TDCI). We find that the single-ionization is accurately reproduced by MCTDHF, whereas the double ionization results correctly capture the main trends of TDCI.
Ionization of helium-like ions with simultaneous excitation of the ns-states due to photon scattering is considered. The differential and total cross sections of the process are calculated to leading order of perturbation theory with respect to the interelectron interaction. The formulas obtained are applicable in the nonrelativistic energy range far beyond the ionization threshold.
We investigate the finite nuclear mass corrections in the helium atom in order to resolve a significant disagreement between the $2^3S - 2^3P$ and $2^3S - 2^1S$ transition isotope shifts. These two transitions lead to discrepant results for the nuclear charge radii difference between $^4$He and $^3$He. The accurate treatment of the finite nuclear mass effects is quite complicated and requires the use of the quantum field theoretical approach. We derive $α^6 m^2/M$ correction with the help of nonrelativistic QED and dimensional regularization of the three body Coulombic system, and present accu…
We investigate the laser-assisted single XUV photon double ionization of ground state helium. By solving full six-dimensional time-dependent schr{ö}dinger equation, we study the correlation and angular distribution. The discussion in joint energy and angular distributions reveals the competition in odd and even parity double ionization processes in the presence of weak laser field. The emission angle between two photoelectrons can be adjusted by the laser parameters. We depicts how the laser field enhance and/or enable the back-to-back and side-by-side emission of double ionization.
Attosecond pump-probe ionization process can be used to prepare atomic ions in the coherent superposition of states with opposite parity. The multiphoton shake-up ionization of Helium, in particular, generates ions with same principal quantum number and a net dipole moment that evolves on a time scale of few picoseconds, due to spin-orbit coupling. In this work we use an ab initio time-dependent close-coupling code to study how the coherence between levels of Helium ion can be controlled from the parameters of the ionizing-pulse sequence. The observed periodic revivals, on a picosecond time sc…
The reduced-mass dependence of relativistic and radiative effects in simple muonic bound systems is investigated. The spin-dependent nuclear recoil correction of order (Zalpha)^4 mu^3/m_N^2 is evaluated for muonic hydrogen and deuterium, and muonic helium ions (mu is the reduced mass and m_N is the nuclear mass). Relativistic corrections to vacuum polarization of order alpha (Zalpha)^4 mu are calculated, with a full account of the reduced-mass dependence. The results shift theoretical predictions. The radiative-recoil correction to vacuum polarization of order alpha (Zα)^5 ln^2(Zalpha) mu^2/m_…
With the classical three-dimensional ensemble model, we have investigated the microscopic recollision dynamics in nonsequential double ionization of helium by 800 nm laser pulses at 2.0 PW/cm^2. We demonstrate that the asymmetric energy sharing between the two electrons at recollision plays a decisive role in forming the experimentally observed V-shaped structure in the correlated longitudinal electron momentum spectrum at the high laser intensity [Phys. Rev. Lett. 99, 263003 (2007)]. This asymmetric energy sharing recollision leaves footprints on the transverse electron momentum spectra, whic…
Multiphoton ionization provides a clear window into the nature of electron correlations in the helium atom. In the present study, the final state energy range extends up to the region near the $N=2$ and $N=3$ ionization thresholds, where two-photon ionization proceeds via continuum intermediate states above the lowest threshold. Our calculations are performed using multichannel quantum defect theory (MQDT) and the streamlined R-matrix method. The sum and integration over all intermediate states in the two-photon ionization amplitude is evaluated using the inhomogeneous R-matrix method develope…
We report on the observation of phase space modulations in the correlated electron emission after strong field double ionization of helium using laser pulses with a wavelength of 394~nm and an intensity of $3\cdot10^{14}$W/cm$^2$. Those modulations are identified as direct results of quantum mechanical selection rules predicted by many theoretical calculations. They only occur for an odd number of absorbed photons. By that we attribute this effect to the parity of the continuum wave function.
We demonstrate the control of $^4$He(2$^3$S$_1$)-$^7$Li(2$^2$S$_{1/2}$) chemi-ionization reactions by all-optical electron-spin-state preparation of both atomic species prior to the collision process. Our results demonstrate that chemi-ionization is strongly suppressed (enhanced) for non-spin-conserving (spin-conserving) collisions at thermal energies. These findings are in good agreement with a model based on spin angular momentum coupling of the prepared atomic states to the quasi-molecular states. Small deviations from the model indicate the contribution of the $^4Σ^+$ channel to the reacti…
We present a unified treatment of the prevalence of different double ionization (DI) pathways as a function of the sum of the final electron energies in strongly driven Helium. We do so as a function of laser frequency and intensity. At small total energy a new DI pathway prevails where both electrons are ionized with a delay after re-collision. We find that three-body collisions between the two electrons and the nucleus underly this pathway--we refer to it as triple collision (TC) pathway. At high total energy the pathway that prevails is the one where one electron is ionized with a delay fol…
We show that time ordering underlying time-dependent quantum dynamics is a physical observable accessible by attosecond streaking. We demonstrate the extraction of time ordering for the prototypical case of time-resolved two-photon double ionization (TPDI) of helium by an attosecond XUV pulse. The Eisenbud-Wigner-Smith time delay for the emission of a two-electron wavepacket and the time interval between subsequent emission events can be unambiguously determined by attosecond streaking. The delay between the two emission events sensitively depends on the energy, pulse duration, and angular dis…
We present the momentum distributions of the nucleus and of the electrons from double ionization of the helium atom by Compton scattering of photons with $hν=40$ keV. We find that the doubly charged ion momentum distribution is very close to the Compton profile of the nucleus in the ground state of the helium atom, and the momentum distribution of the singly charged ion to give a precise image of the electron Compton profile. To reproduce these results, non-relativistic calculations require the use of highly correlated initial- and final-state wavefunctions.
Without a formal derivation, we propose a formula for the total and single-differential cross in the problem of one-photon double ionization of an atom. The formula is benchmarked against accurate experimental data for the total cross section of helium. Furthermore, a direct comparison with ab initio calculations for the double ionization of Li+ suggests that the framework is valid for the entire helium isoelectronic sequence. To this end, we introduce a formula for the double ionization of lithium, as well as for the triple ionization of lithium and beryllium.
We study resonant two-photon ionization of helium atoms via the $1s3p$, $1s4p$ and $1s5p^1$P$_1$ states using the 15$^\mathrm{th}$ harmonic of a titanium-sapphire laser for the excitation and a weak fraction of the laser field for the ionization. The phase of the photoelectron wavepackets is measured by an attosecond interferometric technique, using the 17$^\mathrm{th}$ harmonic. We perform experiments with angular resolution using a velocity map imaging spectrometer and with high energy resolution using a magnetic bottle electron spectrometer. Our results are compared to calculations using th…
Phase-shift differences and amplitude ratios of the outgoing $s$ and $d$ continuum wave packets generated by two-photon ionization of helium atoms are determined from the photoelectron angular distributions obtained using velocity map imaging. Helium atoms are ionized with ultrashort extreme-ultraviolet free-electron laser pulses with a photon energy of 20.3, 21.3, 23.0, and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The measured values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to an excited …
Testing Exotic Electron-Electron Interactions with the Helium Ionization-Energy Anomaly
Helmholtz Institute Mainz（亥姆霍兹马因茨研究所）；GSI Helmholtzzentrum für Schwerionenforschung GmbH（GSI重离子研究中心有限公司）；Johannes Gutenberg University（约翰内斯·古腾堡大学）；Faculty of Mathematics, University of Vienna（维也纳大学数学学院）；Gravitational Physics Group, University of Vienna（维也纳大学引力物理组）；Department of Physics, University of California at Berkeley（加州大学伯克利分校物理系）
Compton scattering is one of the fundamental interaction processes of light with matter. Already upon its discovery [1] it was described as a billiard-type collision of a photon kicking a quasi-free electron. With decreasing photon energy, the maximum possible momentum transfer becomes so small that the corresponding energy falls below the binding energy of the electron. Then ionization by Compton scattering becomes an intriguing quantum phenomenon. Here we report a kinematically complete experiment on Compton scattering at helium atoms below that threshold. We determine the momentum correlati…
Comparison of high accuracy calculations with precision measurement of the 413 nm tune-out wavelength of the He($2\,^3S_1$) state provides a unique test of quantum electro-dynamic (QED). We perform large-scale relativistic-configuration-interaction (RCI) calculations of the tune-out wavelength, that include the mass-shift operator, and fully account for leading relativistic nuclear recoil terms in the Dirac-Coulomb-Breit (DCB) Hamiltonian. We obtain the QED correction to the tune-out wavelength using perturbation theory, and the effect of finite nuclear size is also evaluated. The resulting tu…
Recent angle-resolved RABBITT experiments have shown that the photoionization time delay depends on the emission angle of the photoelectron. In this work we demonstrate that for photoemission from helium accompanied by shake-up (correlation satellites), the angular variation of the time delay is dramatically enhanced by the dipolar coupling between the photoelectron and the highly polarizable bound electron in the IR field. We show that the additivity rule for the time delays due to the atomic potential, the continuum-continuum (cc) coupling by the IR field, and due to this two-electron proces…
We theoretically investigate the single and double ionization of the He atom by antiproton impact for projectile energies ranging from $3$~keV up to $1000$~keV. We obtain accurate total cross sections by directly solving the fully correlated two-electron time-dependent Schrödinger equation and by performing classical trajectory Monte-Carlo calculations. The obtained quantum-mechanical results are in excellent agreement with the available experimental data. Along with the total cross sections, we also present the first fully \textit{ab initio} doubly differential data for single ionization at 1…
It is shown that it is feasible to use ultrashort time delay between two XUV femtosecond pulses in order to control two photon resonant ionization. The proposal is demonstrated on the spectrum of Helium, in terms of nonperturbative solutions of the time dependent Schroedinger equation. Comparison with results from second order time dependent perturbation theory provides additional insight.
The momentum distribution of the electron in the reaction p+He $\rightarrow$ H + He$^{2+}$ + $e$ is measured for projectile energies $E_p$=300 and 630 keV/u at very small scattering angles of hydrogen. We mainly present two dimensional distributions parallel $(k_{||})$ and perpendicular $(k_{\perp})$ to the projectile beam. Theoretical calculations were carried out within the Plane Wave First Born Approximation (PWFBA), which includes both electron emission mechanisms, shake-off and sequential capture and ionization. It is shown that electron correlations in the target wave function play the m…
Even though ion/atom-collision is a mature field of atomic physics great discrepancies between experiment and theoretical calculations are still common. Here we present experimental results with highest momentum resolution on single ionization of helium induced by 1\,MeV protons and compare these to different theoretical calculations. The overall agreement is strikingly good and already the first Born approximation yields good agreement between theory and experiment. This has been expected since several decades, but so far has not been accomplished. The influence of projectile coherence effect…
We explore excitation and ionization by neutron impact as a novel tool for the investigation of electron-electron correlations in helium. We present single and double ionization spectra calculated in accurate numerical ab-initio simulations for incoming neutrons with kinetic energies of up to 150 keV. The resulting electron spectra are found to be fundamentally different from photoioniza- tion or charged particle impact due to the intrinsic many-body character of the interaction. In particular, doubly excited resonances that are strongly suppressed in electron or photon impact become prominent…
Triple differential cross sections (TDCSs) for electron vortex projectile ionization of helium into the azimuthal plane are calculated using the distorted wave Born approximation. In this collision geometry, the TDCSs at low and intermediate energies exhibit unique qualitative features that can be used to identify single and double scattering mechanisms. In general, our results predict that the ionization dynamics for vortex projectiles are similar to those of their non-vortex counterparts. However, some key differences are observed. For non-vortex projectiles, a double scattering mechanism is…
The collision-ionization mechanism of nonsequential double ionization (NSDI) process in IR+XUV two-color laser fields [\PRA \textbf{93}, 043417 (2016)] has been investigated by us recently. Here we extend this work to study the collision-excitation-ionization (CEI) mechanism of NSDI processes in the two-color laser fields with different laser conditions. It is found that the CEI mechanism makes a dominant contribution to the NSDI as the XUV photon energy is smaller than the ionization threshold of the He$^+$ ion, and the momentum spectrum shows complex interference patterns and symmetrical str…
By using the B-spline numerical method, we investigate a two-photon double-ionization (TPDI) process of helium in a high-frequency laser field with its frequency ranging from 1.6~a.u. to 3.0~a.u. and the pulse duration ranging from 75 to 160~attoseconds. We found that there exists a characteristic time $t_{c}$ for a TPDI process, such that the pattern of energy distribution of two ionized electrons presents a peak or two, depending respectively on whether the pulse duration is shorter or longer than $t_{c}$. Especially, as the pulse duration is larger than $t_c$, the TPDI spectrum shows a doub…
We calculate various differential and double differential characteristics of ionization by a single photon for H$^-$, He and for the two-electron ions with Z=3,4,5 in the region of the so-called quasi-free mechanism (QFM) domination. We employ highly accurate wave functions at the electron-electron coalescence line where coordinates of both ionized electrons coincide. We trace the Z dependence for the double differential distribution. For all considered targets we discuss the dependence of the photoelectron energy distribution on the photon energy. Our calculation demonstrated the rapid decrea…
We study resonant two-color two-photon ionization of Helium via the 1s3p 1P1 state. The first color is the 15th harmonic of a tunable titanium sapphire laser, while the second color is the fundamental laser radiation. Our method uses phase-locked high-order harmonics to determine the {\it phase} of the two-photon process by interferometry. The measurement of the two-photon ionization phase variation as a function of detuning from the resonance and intensity of the dressing field allows us to determine the intensity dependence of the transition energy.
Detection of nascent O($^3P_j$, $j=2,1,0$) atoms using one-photon resonant excitation to the $3s\,^3S^o_1$ state at $\sim 130$ nm followed by near-threshold ionization, i. e., 1 + 1' resonance enhanced multi-photon ionization (REMPI), has been investigated. The aim was to achieve low ion recoil, improved sensitivity, and reliable angular momentum polarization information, with an as simple as possible laser setup. An efficient 1 + 1' scheme has been found where the VUV light for the first step 1 is generated by difference frequency ($2ω_1 - ω_2$) VUV generation by four wave mixing in Kr gas, a…
The nonrelativistic ionization energy levels of a helium atom are calculated for $S$, $P$, $D$ and $F$ states. The calculations are based on the variational method of "exponential" expansion. The convergence of the calculated energy levels is studied as a function of the number of basis functions $N$. This allows us to claim that the obtained energy values (including the values for the states with a nonzero angular momentum) are accurate up to 28-35 significant digits. Calculations of the nonrelativistic ionization energy of the negative hydrogen ion H$^-$ are also presented.
Quantum electrodynamical (QED) calculations of ionization energies of the $1snd\,D$ states are performed for the helium atom. We reproduce the previously known relativistic and QED effects up to order $mα^5$ and extend the theory by calculating the complete $mα^6$ correction. The total contribution of the $mα^6$ effects is shown to be much smaller than previously estimated, due to a large cancelation between the radiative and non-radiative parts of this correction. As a result of our calculations, we confirm the previously reported deviations between measured transition energies and theoretica…
