We explore the formation by Free-Electron-Laser radiation of Ar hollow states with two or three inner-shell holes. We find that even charged Ar ion states can be more populated than odd charged Ar ion states. This depends on the pulse intensity and the number of energetically accessible inner- shell holes. Fully accounting for fine structure, we demonstrate that one electron spectra bare the imprints of Ar hollow states with two inner-shell holes. Moreover, we show how the Auger spectra of these hollow states can be extracted from two-electron coincidence spectra.
X-ray spectra of K-shell hollow krypton atoms produced in single collisions with 52 - 197 MeV/u Xe54+ ions are measured in a heavy-ion storage ring equipped with an internal gas-jet target. Energy shifts of the Kα_1,2^s, Kα_1,2^(h,s), and K\b{eta}_1,3^s transitions are obtained. Thus, the average number of the spectator L-vacancies presented during the x-ray emission is deduced. From the relative intensities of the Kα_1,2^s and Kα_1,2^(h,s) transitions, the ratio of K-shell hollow krypton to singly K-shell ionized atoms is determined to be 14 - 24%. In the considered collisions, the K-vacancie…
We have studied the role of virtual excitations of inner shells upon outer shell photoionization. The calculations were performed in the frames of the Random Phase Approximation and its generalized version GRPAE that take into account variation of the atomic field due to electron elimination and the inner vacancies decay. We employ both analytic approximation and numeric computations. The results are presented for 3p electrons in Ar and 4d-electrons in Pd near inner shells thresholds. The effect proved to be noticeable.
The Auger effect from inner shells, which arises from resonance excitation of the valence electron of an atom by a weak electromagnetic wave, is discussed.
The mechanism leading to an Auger transition is based on the residual Coulomb interaction between the valence electron and the core electrons. On the assumption that the wave field is switched on adiabatically, the probability of the Auger effect of the inner electrons of the atom is determined.
Large-scale relativistic configuration-interaction method combined with many-body perturbation theory is consistently applied to calculations of the energy levels of the ground and inner-L-shell excited states of berylliumlike ions in the range $10 \leq Z \leq 92$. The quantum electrodynamics, nuclear recoil, and frequency-dependent Breit corrections are taken into account. The obtained results are supplemented with the systematical estimation of the uncertainties.
The first theoretical investigation on the inner-shell single-photodetachment from the Si- negative ion is presented. The partial and total cross sections, the photoelectron phaseshifts, and the parameters of angular anisotropy are calculated in the framework of Many-Body Theory for L-shell photodetachment from Si- ion in the experimentally accessible range of photon energies (7.5-14 Ry). Comparison is made between the calculations of the response of the ionic many-electron system Si- to an electromagnetic field at the different levels of approximation: the "frozen-field" Random Phase Approxim…
We apply time-dependent R-matrix theory to study inner-shell ionization of C atoms in ultra-short high-frequency light fields with a photon energy between 170 and 245 eV. At an intensity of 10$^{17}$ W/cm$^2$, ionization is dominated by single-photon emission of a $2\ell$ electron, with two-photon emission of a 1s electron accounting for about 2-3\% of all emission processes, and two-photon emission of $2\ell$ contributing about 0.5-1\%. Three-photon emission of a 1s electron is estimated to contribute about 0.01-0.03\%. Around a photon energy of 225 eV, two-photon emission of a 1s electron, l…
Extreme ultraviolet (XUV) attosecond pulses, generated by a process known as laser-induced electron recollision, are a key ingredient for attosecond metrology, providing a tool to precisely initiate and probe sub-femtosecond dynamics in the microcosms of atoms, molecules and solids[1]. However, with the current technology, extending attosecond metrology to scrutinize the dynamics of the inner-shell electrons is a challenge, that is because of the lower efficiency in generating the required soft x-ray \hbarω>300 eV attosecond bursts and the lower absorption cross-sections in this spectral range…
New energy conversion system based on charge-exchange and inner-shell electron transitions
State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Laboratory of Advanced Materials, Institute of Fiber Materials and Devices, Fudan University（复旦大学高分子工程国家重点实验室大分子科学系先进材料实验室纤维材料与器件研究所）；Key Laboratory of Nuclear Physics and Ion-Beam Application, Institute of Modern Physics, Fudan University（复旦大学核物理与离子束应用重点实验室现代物理研究所）
Exchange correlation plays an important role in double-ionization of complex atoms by ultrashort laser pulse. In this work, we investigate two-photon double inner-shell electron ionization of neon induced by an attosecond extreme ultraviolent pulse in the framework of the quantum master equation. Our simulations reveal a distinct non-sequential effect via broadened double peaks, as a result of energy sharing between the two ionized electrons. When dissipation is included to show the interplay of coherence and decoherence, the two-photon double-ionization scaling law breaks down. We further stu…
With direct polarizability measurements we demonstrated extremely low sensitivity of the inner-shell clock transition at $1.14\,μ$m in Tm atoms to external dc electric fields and black-body radiation (BBR). We measured differential polarizabilities of clock levels in Tm at wavelengths of 810--860\,nm and at 1064\,nm and inferred the static scalar differential polarizability of the inner-shell clock transition of $-0.047(18)$ atomic units corresponding to only $2\times10^{-18}$ fractional frequency shift from BBR at the room temperature. This is a few orders of magnitude smaller compared to the…
Development of a cylindrical mirror analyzer electron spectrometer and associated data acquisition system to study inner shell electron emission following ion-atom collision
Inner-shell vacancy production for the O$^{8+}$-Li collision system at 1.5 MeV/amu is studied theoretically. The theory combines single-electron amplitudes for each electron in the system to extract multielectron information about the collision process. Doubly-differential cross sections obtained in this way are then compared with the recent experimental data by LaForge et al. [J. Phys. B 46, 031001 (2013)] yielding good resemblance, especially for low outgoing electron energy. A careful analysis of the processes that contribute to inner-shell vacancy production shows that the improvement of t…
We report on the design and performance of a double-sided coincidence velocity map imaging spectrometer optimized for electron-ion and ion-ion coincidence experiments studying inner-shell photoionization of gas-phase molecules with soft X-ray synchrotron radiation. The apparatus employs two microchannel plate detectors equipped with delay-line anodes for coincident, time- and position-resolved detection of photo- and Auger electrons with kinetic energies up to 300\,eV on one side of the spectrometer and photoions up to 25\,eV per unit charge on the opposite side. We demonstrate its capabilitie…
X-ray free-electron lasers have had an enormous impact on x-ray science by achieving femtosecond pulses with unprecedented intensities. However, present-day facilities operating by the self-amplified spontaneous emission (SASE) principle have a number of shortcomings, namely, their radiation has a chaotic pulse profile and short coherence times. We put forward a scheme for a neon-based atomic inner-shell x-ray laser (XRL) which produces temporally and spatially coherent subfemtosecond pulses that are controlled by and synchronized to an optical laser with femtosecond precision. We envision tha…
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…
Echoing classical physics, quantum electrodynamics predicts the release of a spectral continuum of electromagnetic radiation upon the sudden acceleration of charged particles in quantum matter. Despite apparent theoretical success in describing sister nuclear processes, known as internal bremsstrahlung, following nuclear beta decay and K capture, the situation of the photoejection of an electron from an inner shell of an atom, intraatomic bremsstrahlung (IAB), is far from settled. In this paper we present fresh measurements which rely on contemporary signal processing as well as the high flux …
The predominant reason for the damaging power of high-energy radiation is multiple ionization of a molecule, either direct or via the decay of highly excited intermediates, as e.g., in the case of X-ray irradiation. Consequently, the molecule is irreparably damaged by the subsequent fragmentation in a Coulomb explosion. In an aqueous environment, however, it has been observed that irradiated molecules may be saved from fragmentation presumably by charge and energy dissipation mechanisms. Here, we show that the protective effect of the environment sets in even earlier than hitherto expected, na…
The fragmentation dynamics of 2,6- and 3,5-difluoroiodobenzene after iodine 4$d$ inner-shell photoionization with soft X-rays are studied using coincident electron and ion momentum imaging. By analyzing the momentum correlation between iodine and fluorine cations in three-fold ion coincidence events, we can distinguish the two isomers experimentally. Classical Coulomb explosion simulations are in overall agreement with the experimentally determined fragment ion kinetic energies and momentum correlations and point toward different fragmentation mechanisms and time scales. While most three-body …
We report on the observation and coherent excitation of atoms on the narrow inner-shell orbital transition, connecting the erbium ground state $[\mathrm{Xe}] 4f^{12} (^3\text{H}_6)6s^{2}$ to the excited state $[\mathrm{Xe}] 4f^{11}(^4\text{I}_{15/2})^05d (^5\text{D}_{3/2}) 6s^{2} (15/2,3/2)^0_7$. This transition corresponds to a wavelength of 1299 nm and is optically closed. We perform high-resolution spectroscopy to extract the $g_J$-factor of the $1299$-nm state and to determine the frequency shift for four bosonic isotopes. We further demonstrate coherent control of the atomic state and ext…
Understanding inner-shell excitations in molecules through spectroscopy of the 4f hole states of YbF
Center for Cold Matter, Blackett Laboratory, Imperial College London（帝国理工学院冷物质中心布莱克特实验室）；Fritz-Haber-Institut der Max-Planck-Gesellschaft（马克斯·普朗克学会弗里茨·哈伯研究所）
