Photoionization of an atom in the presence of a neighboring atom of different species is studied. The latter first undergoes resonant photoexcitation, leading to an autoionizing state of the diatomic system. Afterwards, the excitation energy is transferred radiationlessly via a two-center Auger process to the other atom, causing its ionization. Assuming a fixed internuclear distance, it has been predicted theoretically that this indirect ionization pathway can strongly dominate over the direct photoionization. Here, we extend the theory of resonant two-center photoionization by including the nuclear motion in van-der-Waals molecules. An analytical formula is derived reflecting the influence of molecular vibrational dynamics on the relative strength of the two-center channel. For the specific example of Li-He dimers we show that the two-center autoionizing resonances are split by the nuclear motion into multiplets, with the resonance lines reaching a comparable level of enhancement over direct photoionization as is obtained in a model based on spatially fixed nuclei.
An additional channel opens for photoionization of atom $A$ by an electromagnetic field if it traverses a gas of atoms $B$ resonantly coupled to this field. We show that this channel, in which $A$ is ionized via resonant photoexcitation of $B$ with subsequent energy transfer to $A$ through two-center electron correlations and which is very efficient when $A$ and $B$ constitute a bound system, can strongly dominate the ionization of $A$ also in collisions where the average distance between $A$ and $B$ exceeds the typical size of a bound system by orders of magnitude.
Photoionization of an atom via interatomic correlations to N neighboring atoms may be strongly enhanced due to constructive interference of quantum pathways. The ionization proceeds via resonant photoexcitation of a neighbor atom and subsequent interatomic Coulombic decay. The enhancement can scale with N^2, leading to "super-enhanced photoionization".
Modifications of photoionization arising from resonant electron-electron correlations between neighbouring atoms in an atomic sample are studied. The sample contains atomic species A and B, with the ionization potential of A being smaller than the energy of a dipole-allowed transition in B. The atoms are subject to an external radiation field which is near-resonant with the dipole transition in B. Photoionization of an atom A may thus proceed via a two-step mechanism: photoexcitation in the subsystem of species B, followed by interatomic Coulombic decay. As a basic atomic configuration, we inv…
Considering the photoionization of Ar@C60, we predict resonant femtosecond decays of both Ar and C60 vacancies through the continua of atom-fullerene hybrid final states. The resulting resonances emerge from the interference between simultaneous autoionizing and intercoulombic decay (ICD) processes. For Ar 3s-->np excitations, these resonances are far stronger than the Ar-to-C60 resonant ICDs, while for C60 excitations they are strikingly larger than the corresponding Auger features. The results indicate the power of hybridization to enhance decay rates, and modify lifetimes and line profiles.
Characterizing time delays in molecular photoionization as a function of the ejected electron emission direction relative to the orientation of the molecule and the light polarization axis pro-vides unprecedented insights into the attosecond dynamics induced by extreme ultraviolet or X-ray one-photon absorption, including the role of electronic correlation and continuum resonant states. Here, we report completely resolved experimental and computational angular depend-ence of single-photon ionization delays in NO molecules across a shape resonance, relying on synchrotron radiation and time inde…
Two efficient and isotope-selective resonant two-photon ionization techniques for loading barium ions into radio-frequency (RF)-traps are demonstrated. The scheme of using a strong dipole-allowed transition at λ=553 nm as a first step towards ionization is compared to the established technique of using a weak intercombination line (λ=413 nm). An increase of two orders of magnitude in the ionization efficiency is found favoring the transition at 553 nm. This technique can be implemented using commercial all-solid-state laser systems and is expected to be advantageous compared to other narrowban…
Photoionization of an atom $A$, in the presence of a neighboring atom $B$, can proceed via resonant excitation of $B$ with subsequent energy transfer to $A$ through two-center electron-electron correlation. We demonstrate that this two-center mechanism can strongly outperform direct photoionization at nanometer internuclear distances and possesses characteristic features in its time development and the spectrum of emitted electrons.
The theory of resonant Auger decay of atoms in a high intensity coherent X-ray pulse is presented. The theory includes the coupling between the ground state and the resonance due to an intense X-ray pulse, taking into account the decay of the resonance and the direct photoionization of the ground state, both populating the final ionic states coherently. The theory also considers the impact of the direct photoionization of the resonance state itself which typically populates highly-excited ionic states. The combined action of the resonant decay and of the direct ionization of the ground state i…
We study the photoionization and autoionization of Helium atom subject to ultrashort laser pulses by using a Feshbach formalism in the time domain. We solve the time-dependent Schrödinger equation in terms of a configuration interaction (CI) spectral method, in which the total wavefunction is expanded with configurations defined within bound-like ($\mathcal{Q}$) and scattering-like ($\mathcal{P}$) halfspaces. The method allowsone to provide accurate descriptions of both the atomic structure (energy positions and widths) and the photodynamics. We illustrate our approach by i) calculating the ti…
In this work, we apply the Monte Carlo wave packet method to study the ultrafast nuclear dynamics following inner-shell photoionization of N2 exposed to an ultrashort intense X-ray pulse. The photon energy of the X-ray pulse is large enough to remove a 1s electron from the N atom in N2. The intermediate state in N+2 is highly excited so that autoionization takes place from this state to the dissociative or non-dissociative electronic states of ungerade and gerade symmetries in N++2. The possible vibrational resonances allowed by the non-dissociative states prevents a direct extraction of the n…
Resonant two-photon ionization in a system consisting of two spatially well-separated atoms is studied. Due to two-center electron-electron correlations, the ionization may also proceed through photo-excitation of both atoms with subsequent interatomic Coulombic decay. We show that this channel may dominate the photoionization process and qualitatively change its dependence on the field intensity and the spectra of emitted electrons.
Photoionization of an atom $A$ by a strong laser field in the presence of a spatially well-separated neighboring atom $B$ is considered. The laser field frequency is assumed to lie below the ionization potential of atom $A$ and be resonant with a dipole-allowed transition in atom $B$. In this situation, the ionization may occur either directly by multiphoton absorption from the laser field at the first atomic center. Or via an indirect pathway involving two-center electron-electron correlations, where the neighbor atom $B$ is first photoexcited and, afterwards, transfers its energy upon deexci…
The effects of confinement resonances on photoelectron group delay (Wigner time delay) following ionization of an atom encapsulated inside a C$_{60}$ cage have been studied theoretically using both relativistic and non-relativistic random phase approximations. The results indicate clearly the resonant character of the confinement oscillations in time delay of the $4d$ shell of Xe@C$_{60}$ and present a most direct manifestation of Wigner time delay. These oscillations were missed in a previous theoretical investigation of Ar@C$_{60}$ [PRL 111, 203003 (2013)]
It is well known that interatomic or intermolecular interactions driven by two-center electronic dipole-dipole correlations fall off rapidly with the inter-site distance. We show, however, that the effective strength of interatomic reaction channels, which are triggered by a resonant field, can exhibit a nonmonotonous distance dependence, being strongly reduced when the atoms come closer. This surprising result is demonstrated by considering resonant two-center photoionization as an example. Our findings are supported by available experimental data.
We consider the process of double photoionization (DPI) in a rare gas atom as a two-step process, namely (i) photoionization in an inner shell followed by (ii) the emission of an Auger electron from an outer shell. An angular correlation function for the two emitted electrons is defined by analogy with the theory of angular correlation in nuclear physics. An expression is obtained for this angular correlation function by a statistical method which makes use of the density and efficiency operators. The latter takes care of the attenuation of the probability of detection of an electrons due to t…
We investigate nuclear-resonant electron scattering as occurring in the two-step process of nuclear excitation by electron capture (NEEC) followed by internal conversion. The nuclear excitation and decay are treated by a phenomenological collective model in which nuclear states and transition probabilities are described by experimental parameters. We present capture rates and resonant strengths for a number of heavy ion collision systems considering various scenarios for the resonant electron scattering process. The results show that for certain cases resonant electron scattering can have sign…
Double ionization of an atom by single-photon absorption in the presence of a neighbouring atom is studied. The latter is, first, resonantly photoexcited and, afterwards, transfers the excitation energy radiationlessly to the other atom, leading to its double ionization. The process relies on the combined effect of interatomic and intraatomic electron correlations. It can dominate over the direct double photoionization by several orders of magnitude at interatomic distances up to few nanometers. The relative position of the neighbouring atom is shown to exert a characteristic influence on the …
We present a photoionization method to load single 40Ca ions in a linear Paul trap from an atomic beam. Neutral Ca I atoms are resonantly excited from the ground state to the intermediate 4s4p 1P_1-level using coherent 423nm radiation produced by single-pass second harmonic generation in a periodically poled KTiOPO_4 crystal pumped with an 120mW extended cavity diode laser. Ionization is then attained with a high-power light emitting diode imaged to the trap center, using an appropriately designed optical system composed of standard achromatic doublet lenses. The setup simplifies previous impl…
The photoionization of the CO molecule from the C$-1s$ orbital does not obey the Franck-Condon approximation, as a consequence of the nuclear recoil that accompanies the direct emission and intra-molecular scattering of the photoelectron. We use an analytical model to investigate the temporal signature of the entangled nuclear and electronic motion in this process. We show that the photoelectron emission delay can be decomposed into its localization and resonant-confinement components. Finally, photoionization by a broadband soft-x-ray pulse results in a coherent vibrational ionic state with a…
The photon-ion merged-beams technique has been employed at the new Photon-Ion spectrometer at PETRA III (PIPE) for measuring multiple photoionization of Xe$^{q+}$ (q=1-5) ions. Total ionization cross sections have been obtained on an absolute scale for the dominant ionization reactions of the type hν+ Xe$^{q+}$ $\to$ Xe$^{r+}$ + (q-r) e$^-$ with product charge states q+2 $\le$ r $\le$ q+5. Prominent ionization features are observed in the photon-energy range 650-750 eV, which are associated with excitation or ionization of an inner-shell 3d electron. Single-configuration Dirac-Fock calculation…
Electronic bridge excitation of the 76 eV nuclear isomeric state in $^{235}$U is shown to be strongly enhanced in the U$^{7+}$ ion, potentially enabling laser excitation of this nucleus. This is because the electronic spectrum has a very high level density near the nuclear transition energy that ensures the resonance condition is fulfilled. We present a quantum statistical theory based on many-body quantum chaos to demonstrate that typical values for the electronic factor increase the probability of electronic bridge in $^{235}$U$^{7+}$ by many orders of magnitude. We also extract the nuclear …
We present an experimental study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral argon atoms. 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 non-resonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$ and $f$ partial wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the VUV pol…
The newly developed method of time-of-flight (ToF) momentum microscopy was used to analyse the cold electron emission from a Cs 3D magneto-optical trap (MOT). Three-step resonant photoionization was implemented via two intermediate states (6P3/2 pumped with 852 nm laser and 7S1/2 with 1470 nm) and a tuneable femtosecond Ti:sapphire laser for the final ionization step. The magnetic field of the MOT is switched off during the photoionization step. The natural bandwidth of the fs-laser is reduced to 4 meV using optical spectral filters. Precise tuning of the photon energy makes it possible to obs…
Coherent control of interfering one- and two-photon processes has for decades been the subject of research to achieve the redirection of photocurrent. The present study develops two-pathway coherent control of ground state helium atom above-threshold photoionization for energies up to the $N=2$ threshold, based on a multichannel quantum defect and R-matrix calculation. Three parameters are controlled in our treatment: the optical interference phase $ΔΦ$, the reduced electric field strength $χ=\mathcal{E}_ω^2/{\mathcal{E}_{2ω}}$, and the final state energy $ε$. A small energy change near a reso…
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 $^2Σ^+_g$, A $^2Π_u$, and B $^2Σ^+_u$ ionic states of N$_2^+$, where the photoelectron angular distributions associated with the X $^2Σ^+_g$ and A $^2Π_u$ state…
We show that nuclear motion of Rydberg atoms can be induced by resonant dipole-dipole interactions that trigger the energy transfer between two energetically close Rydberg states. How and if the atoms move depends on their initial arrangement as well as on the initial electronic excitation. Using a mixed quantum/classical propagation scheme we obtain the trajectories and kinetic energies of atoms, initially arranged in a regular chain and prepared in excitonic eigenstates. The influence of off-diagonal disorder on the motion of the atoms is examined and it is shown that irregularity in the arr…
We review the ideas and concepts for a clock that is based on a radiative transition in the nucleus rather than in the electron shell. This type of clock offers advantages like an insensitivity against field-induced systematic frequency shifts and the opportunity to obtain high stability from interrogating many nuclei in the solid state. Experimental work concentrates on the low-energy (about 8 eV) isomeric transition in Th-229. We review the status of the experiments that aim at a direct optical observation of this transition and outline the plans for high-resolution laser spectroscopy experi…
Dielectronic recombination (DR) of few-electron ions has evolved into a sensitive spectroscopic tool for highly charged ions. This is due to technological advances in electron-beam preparation and ion-beam cooling techniques at heavy-ion storage rings. Recent experiments prove unambiguously that DR collision spectroscopy has become sensitive to 2nd order QED and to nuclear effects. This review discusses the most recent developments in high-resolution spectroscopy of low-energy DR resonances, experimental studies of KLL DR of very heavy hydrogenlike ions, isotope shift measurements of DR resona…
Nuclear resonant excitation of the 29.19-keV level in $^{229}$Th with high-brilliance synchrotron- radiation and detection of its decay signal, are proposed with the aim of populating the extremely low-energy isomeric state of $^{229}$Th.The proposed experiment, known as nuclear resonant scattering (NRS), has the merit of being free from uncertainties about the isomer level energy. However, it requires higher time resolution and shorter tail in the response function of the detector than that of conventional NRS experiments because of the short lifetime of the 29.19-keV state. We have fabricate…
In the annihilation of a positron with a bound atomic electron, the virtual gamma photon created may excite the atomic nucleus. We put forward this effect as a spectroscopic tool for an energy-selective excitation of nuclear transitions. This scheme can efficiently populate nuclear levels of arbitrary multipolarities in the MeV regime, including monopole transitions and giant resonances. In certain cases, it may have a higher cross sections than the conventionally used Coulomb excitation.
Molecular center-of-mass motion is taken into account in the theory of coherent control of nuclear spin isomers of molecules. It is shown that infrared radiation resonant to the molecular rovibrational transition can substantially enrich nuclear spin isomers and speed up their conversion rate.
We present ionization probability and line shape calculations for the two-step 3-photon ionization process, $1S \stackrel{2\hbar ω}{\longrightarrow}2S \stackrel{\hbar ω}{\longrightarrow}εP $, of the ground state of hydrogenic atoms in a non-monochromatic laser field with a time--dependent amplitude. Within the framework of a three--level model, the {\it AC Stark} shifts and non-zero ionization rates of all states involved were taken into account together with spatial and temporal inhomogeneities of the laser signal. In contrast with the usual perturbative technique, the time evolution of the a…
In a previous report, we have shown that the rhodium lattice consisting of resonant nuclei is an ideal photonic crystal in nature. Plenty of extraordinary observations are attributed to the collective down conversion of the multipolar nuclear transition; in particular the spontaneous open up of photonic band gap. Emissions of directionality depending on the macroscopic geometry manifest that the standing wave is global in the polycrystalline sample. In this work, further observations of the directional emissions are summarized. By applying an external magnetic field at room temperature, not on…
Coherent population trapping (CPT) provides a highly sensitive means for probing the energy level structure of an atomic system. For a nitrogen vacancy center in diamond, the CPT offers an alternative to the standard optically-detected magnetic resonance method for measuring the hyperfine structure of the electronic ground states. We show that the nuclear spin dependent CPT measures directly the hyperfine splitting of these states due to the 14N nuclear spin. The CPT spectral response obtained in the presence of a strong microwave field, resonant or nearly resonant with a ground state spin tra…
We present a multichannel photoelectron interferometry technique based on trichromatic pulse shaping for unambiguous determination of quantum phases in multiphoton ionization (MPI) of potassium atoms. The colors of the laser field are chosen to produce three energetically separated photoelectron interferograms in the continuum. While the red pulse is two-photon resonant with the $3d$-state resulting in a (2+1) resonance-enhanced MPI (REMPI), a (1+2) REMPI occurs via the non-resonant intermediate $4p$-state with an initial green or blue pulse. We show that ionization via a non-resonant intermed…
Interaction with the axion dark matter (DM) field generates an oscillating nuclear electric dipole moment (EDM) with a frequency corresponding to the axion's Compton frequency. Within an atom, an oscillating EDM can drive electric dipole transitions in the electronic shell. In the absence of radiation, and if the axion frequency matches a dipole transition, it can promote the electron into the excited state. The excitation events can be detected, for example, via subsequent uorescence or photoionization. Here we calculate the rates of such transitions. For a single light atom and an axion Comp…
