Experimental evidence of interatomic coulombic decay from the auger final states in argon dimers

Interatomic Coulombic decay (ICD) from an Auger-final dicationic state is observed in the Ar dimer. A 2p inner-shell vacancy created by photoionization is replaced with 3s and 3p vacancies via intra-atomic Auger decay. The Auger-final dicationic state is subject to ICD in which one of the 3p electrons in the same Ar atom fills the 3s vacancy while one of the 3p electrons from the neighboring Ar atom is emitted as an ICD electron. This ICD process is unambiguously identified by electron-ion-ion coincidence spectroscopy in which the kinetic energy of the ICD electron and the kinetic energy release between Ar+ and Ar2+ are measured in coincidence.     

Acoustic phonon impact on the inter-Coulombic decay process in charged quantum dot pairs

ABSTRACT

Recently, highly accurate multi-configuration time-dependent Hartree electron dynamics calculations demonstrated the efficient long-range energy transfer inter-Coulombic decay (ICD) process to happen in charged semiconductor quantum dot (QD) pairs. ICD is initiated by intraband photoexcitation of one of the QDs and leads to electron emission from the other within a duration of about 150 ps. On the same time scale electronically excited states are reported to relax due to the coupling of electrons to acoustic phonons. Likewise, phonons promote ionisation. Here, the QDs' acoustic breathing mode is implemented in a frozen-phonon approach. A detailed comparison of the phonon effects on electron relaxation and emission as well as on the full ICD process is presented, which supports the previous empirical finding of ICD being the dominant decay channel in paired QDs. In addition the relative importance of phonon–phonon, phonon–electron and electron–electron interaction is analysed.     

Electron-transfer-mediated decay and interatomic Coulombic decay from the triply ionized states in argon dimers

We report the first observation of electron-transfer-mediated decay (ETMD) and interatomic Coulombic decay (ICD) from the triply charged states with an inner-valence vacancy, using the Ar dimer as an example. These ETMD and ICD processes, which lead to fragmentation of Ar(3+)-Ar into Ar(2+)-Ar(2+) and Ar(3+)-Ar+, respectively, are unambiguously identified by electron-ion-ion coincidence spectroscopy in which the kinetic energy of the ETMD or ICD electron and the kinetic energy release between the two fragment ions are measured in coincidence.     

Partial widths and branching ratios for the emitted electron resulting from interatomic Coulombic decay in quantum wells heterostructure

Interatomic coulomb decay (ICD) is a decay process relying on the Coulombic interaction between neighbouring atoms, molecules or nanostructures. Due to this process, an electron is emitted into the continuum. We study the ICD process in a system of the double quantum well heterostructure and investigate how we can manipulate the structure's parameters such that a better detection of the ICD's emitted electron is achieved. For this purpose, we calculated the partial widths (PWs) and branching ratios (BRs) of the ICD's emitted electron to the left and right asymptotes of the heterostructure; these will give an estimation of the detection current. We manipulated the structure's parameters and took into account the repulsion from the electron in the ground state located in the left well. By introducing two small barriers in the vicinity of the right QW, we observed a BR three times larger than in the structure without the barriers. We also investigate the effect of repulsion due to the second electron. This work gives a better understanding of the dynamics of the scattered ICD's electron, and realisation of better design rules for future experimental observation of ICD in nanostructures.     

Radiative relaxation in 2p-excited argon clusters

The emission of ultraviolet fluorescence radiation from variable size argon clusters is investigated with high spectral resolution in the Ar 2p-excitation regime. The fluorescence excitation spectra reveal strong fluorescence intensity in the Ar 2p-continuum, but no evidence for the occurrence of discrete low-lying core-exciton states in the near-edge regime. This finding is different from the absorption and photoionization cross section of argon clusters and the solid. The dispersed fluorescence shows a broad molecular band centered near 280 nm. The present work indicates that double and triple ionization via the LMM-Auger decay are required to initiate the fluorescence processes in the Ar 2p-continuum. The present results are consistent with the formation of singly charged, excited moieties within the clusters, which are assigned as sources of the radiative emission in the 280 nm regime. A fast energy transfer process (interatomic Coulombic decay (ICD)), which has been proposed by recent theoretical work, is assigned to be primarily the origin of these singly charged, excited cations besides intra-cluster electron impact ionization by the Auger electrons. Our findings give first possible experimental evidence for ICD in the core level regime.     

Properties of resonant interatomic Coulombic decay in Ne dimers

Properties of the interatomic Coulombic decay (ICD) process in Ne dimers have been obtained by tracking the formation of energetic Ne+ ions. The double photoionization cross section, deduced from the Ne+/Ne+ coincidence signal, is dominated by the ICD process and presents a threshold 280 meV below the atomic Ne+2s(-1) threshold. Rydberg excitation of a 2s electron in the dimer creates molecular Rydberg states whose Sigma and Pi symmetries have been resolved. These excited states decay by a resonant ICD process releasing an energetic Ne+ ion and a neutral excited Ne* fragment. Subsequent autoionization of the Ne* fragment explains a double photoionization threshold below the dimer 2s ionization threshold.     

Intermolecular coulomb decay at weakly coupled heterogeneous interfaces

Surface ejection of H(+)(H(2)O)(n=1-8) from low energy electron irradiated water clusters adsorbed on graphite and graphite with overlayers of Ar, Kr or Xe results from intermolecular Coulomb decay (ICD) at the mixed interface. Inner valence holes in water (2a(1)(-1)), Ar (3s(-1)), Kr (4s(-1)), and Xe (5s(-1)) correlate with the cluster appearance thresholds and initiate ICD. Proton transfer occurs during or immediately after ICD and the resultant Coulomb explosion leads to H(+)(H(2)O)(n=1-8) desorption with kinetic energies that vary with initiating state, final state, and interatomic or molecular distances.     

Tracing ultrafast interatomic electronic decay processes in real time and space

Advances in laser pump-probe techniques open the door for observations in real time of ultrafast electronic processes. Particularly attractive is the visualization of interatomic processes where one can follow the energy transfer from one atom to another. The interatomic Coulombic decay (ICD) provides such a process which is abundant in nature. A wave packet propagation method now enables us to trace fully ab initio the electron dynamics of the process in real time and space, taking into account all electrons of the system and their correlations. The evolution of the electronic cloud during the ICD process in NeAr following Ne2s ionization is computed and analyzed. The process takes place on a femtosecond time scale, and a surprisingly strong response is found already in the attosecond regime.     

反射式GaN光电阴极表面势垒对量子效率衰减的影响

针对反射式GaN光电阴极长波段量子效率衰减较大, 短波段量子效率衰减较小的实验现象, 在考虑谷间散射的情况下, 利用玻尓兹曼分布和基于Airy函数的传递矩阵法, 计算了发射电子能量分布, 分析了表面势垒变化对量子效率衰减的影响, 理论与实验符合较好. 激活层有效偶极子数的减少使表面势垒宽度和高度增加, 引起长波光子激发产生的发射电子能量分布衰减较大, 短波光子激发产生的发射电子能量分布衰减较小, 这是量子效率在长波段衰减较大, 短波段衰减较小的根本原因.     

Exploring interatomic Coulombic decay by free electron lasers

To exploit the high intensity of laser radiation, we propose to select frequencies at which single-photon absorption is of too low energy and two or more photons are needed to produce states of an atom that can undergo interatomic Coulombic decay (ICD) with its neighbors. For Ne(2) it is explicitly demonstrated that the proposed multiphoton absorption scheme is much more efficient than schemes used until now, which rely on single-photon absorption. Extensive calculations on Ne(2) show how the low-energy ICD electrons and Ne(+) pairs are produced for different laser intensities and pulse durations. At higher intensities the production of Ne(+) pairs by successive ionization of the two atoms becomes competitive and the respective emitted electrons interfere with the ICD electrons. It is also shown that a measurement after a time delay can be used to determine the contribution of ICD even at high laser intensity.     

Multiple photoionization of atoms and small molecules by synchrotron radiation

Absorption of one VUV photon by an atom or a molecule can induce the ejection of several electrons through different processes. Such multiple ionization processes, studied by coincidence electron spectroscopy, provide a wealth of information on electron correlations. A magnetic bottle electron time of flight spectrometer implemented on synchrotron radiation centers has allowed the efficient detection in coincidence of two, three and up to five electrons with good energy resolution. The branching ratios of the different processes are easily extracted from the experimental spectra due to the constant transmission of the spectrometer. Multiple Auger decay was observed in rare gases atoms after inner-shell ionization, while core-valence and core-core initial double ionization followed by Auger decay are other pathways to multiple ionization. For molecules, Coulomb explosion with energy released in ionic fragments may occur after multiple ionization, nevertheless, coincidence electron spectroscopy can also provide a clear interpretation for peculiar decay channels in molecules.     

Observation of the neutron radiative decay

The aim of this work is the experimental observation of and research into a rare neutron mode, the radiative beta decay, where a new particle, the radiative gamma quantum, is formed along with the expected decay products: a beta electron, a recoil proton, and an antineutrino. The discovery of this rare neutron decay mode was conducted through identification of triple-coincidence events: simultaneous registration of a beta electron, a proton, and a radiative gamma quantum. The ordinary neutron decay was registered by double coincidences of a beta electron and a recoil proton. The statistics collected allow one to deduce the branching ratio (BR) BR = (3.2 ± 1.6) × 10⁻³ (90% C.L.) in the gamma energy region greater than 35 keV. This value of BR is consistent with standard electroweak theory. The text was submitted by the authors in English. An erratum to this article is available at .     

Importance of electronic relaxation for inter-coulombic decay in aqueous systems

Inspired by recent photoelectron spectroscopy experiments on hydroxide solutions, we have examined the conditions necessary for enhanced (and, in the case of solutions, detectable) inter-Coulombic decay (ICD)--Auger emission from an atomic site other than that originally excited. We present general guidelines, based on energetic and spatial overlap of molecular orbitals, for this enhancement of inter-Coulombic decay-based energy transfer in solutions. These guidelines indicate that this decay process should be exhibited by broad classes of biomolecules and suggest a design criterion for targeted radiooncology protocols. Our findings show that photoelectron spectroscopy cannot resolve the current hydroxide coordination controversy.     

Rare decay modes of fission fragments

The experimental data on rare modes of radioactive decay of fission fragments is reviewed. These decay modes are due to a large excess of neutrons and a high energy of β decay fragments. They appear in delayed emission of various particles after the β decay (several neutrons, α particles, or heavy clusters) and excitation of unusual states (giant multipole resonances and shape isomers). The β decay and internal conversion of γ radiation into bound states of the atomic electron shell and their influence on the probability of secondary particle emission are considered. The possibility is discussed of observing decays that have not yet been experimentally detected, but theoretically predicted, as well as information on the nuclear structure obtained by studying such decay modes.     

Measured lifetime of SF6-

The lifetime of the SF6 anion was measured at the electrostatic ion storage ring ELISA, where decays in the time span from 100 mus to a few seconds were recorded. We find a nonexponential decay with an approximate t(-1.5) power-law dependence. The observed decay rate is accounted for by a model for thermionic emission that takes into account the initial energy spread of the SF6 molecule prior to electron capture as well as some kinetic energy of the captured electron in the applied plasma-ion source. The energy dependent decay rate is described by an Arrhenius decay constant with a pre-exponential factor and the electron affinity.     

Energy splitting of the ground-state doublet in the nucleus 229Th

The energy splitting of the 229Th ground-state doublet is measured to be 7.6+/-0.5 eV, significantly greater than earlier measurements. Gamma rays produced following the alpha decay of 233U (105 muCi) were counted in the NASA/electron beam ion trap x-ray microcalorimeter spectrometer with an experimental energy resolution of 26 eV (FWHM). A difference technique was applied to the gamma-ray decay of the 71.82 keV level that populates both members of the doublet. A positive correction amounting to 0.6 eV was made for the unobserved interband decay of the 29.19 keV state (29.19-->0 keV).     

Experimental separation of virtual photon exchange and electron transfer in interatomic coulombic decay of neon dimers

We investigate the interatomic Coulombic decay (ICD) of neon dimers following photoionization with simultaneous excitation of the ionized atom (shakeup) in a multiparticle coincidence experiment. We find that, depending on the parity of the excited state, which determines whether ICD takes place via virtual dipole photon emission or overlap of the wave functions, the decay happens at different internuclear distances, illustrating that nuclear dynamics heavily influence the electronic decay in the neon dimer.     

Experimental evidence for interatomic coulombic decay in Ne clusters

Electron spectra of photoexcited Ne clusters are shown to display a signal at low kinetic energies that is neither present in the Ne monomer nor at photon energies below the inner-valence 2s threshold. These findings are strong evidence for the existence of interatomic Coulombic decays (ICD), a mechanism that was recently predicted theoretically [Phys. Rev. Lett. 79, 4778 (1997)]]. In ICD, an inner-valence hole state in a weakly bonded system can undergo ultrafast relaxation due to energy transfer to a neighboring atom, followed by electron emission from this neighboring site.     

Interatomic coulombic decay in van der waals clusters and impact of nuclear motion

It is demonstrated that excited van der Waals systems can relax by electron emission via a novel interatomic mechanism. The process is analyzed by means of extensive ab initio calculations of potential energy surfaces and electronic decay rates. The electronic emission, taking place on the same time scale as the motion of the atomic nuclei, is accompanied by interesting dynamical effects amenable to experimental observations. These effects arise as a consequence of the weak chemical bond in van der Waals clusters and the Coulomb repulsion pattern originating from electron emission.     

Self-quenching effects of excitons in CaWO4 under high density XUV free electron laser excitation

Using free electron laser excitation in the XUV range, CaWO₄ samples were exposed to ultrashort intense photon pulses (photon energy, 89.84 eV; average pulse energy, 10 μJ; pulse length, 25 fs), and their luminescence was studied with time-resolved spectroscopy. In the decay curves measured in the temperature range 8–300 K, a nonexponential emission decay with shortening of the lifetimes over the first few microseconds was observed, depending on the excitation density. Using a model for dipole-dipole interaction of excitons under nonuniform excitation densities, the structure of the decay curves can be reproduced in good agreement with the experimental data, and parameters for the initial exciton interaction can be calculated. The text was submitted by the authors in English.