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We have implemented a cluster-continuum method using density functional theory to model water clusters and various charged species derived from water. The two aims of this study are to determine the minimal basis required for proper modeling of water autoionization and to determine the minimum number of explicit water molecules required to properly model the energetics of solvation. The thermodynamics of water autoionization converge following a modified power law to deliver chemically accurate values of the Gibbs energy change for autoionization with tractably small clusters. Convergence is slower and not exponential as assumed in previous work. We identify the n = 21 set of clusters as the first effectively bulk water like clusters that can capture the energetic influence of both the first and second solvation shells. In this cluster, a water molecule is encapsulated in the center of a closed shell of other water molecules that hydrogen bond to form five-membered rings. The total energy change for clusters with n ≥ 21 calculated using both the RPBE-D3 and ωB97X-D exchange–correlation functionals with the 6-311+G** basis set is shown to deliver good approximations to the free energy change at 298 K. This is true even though neither functional models the individual enthalpy or entropy contributions particularly well. [ABSTRACT FROM AUTHOR]

We present an experimental study of multiple-electron capture-induced fragmentation dynamics of Ar 2 m + (4 ≤ m ≤ 7) dimer ions in 4 keV/u Ar8+–Ar2 collisions. The fragment recoil ion pairs and the charge-changing projectiles are coincidentally measured using a double coincidence technique. The branching ratios between the different charge-sharing fragmentation channels show an inherent enhancement of the asymmetric channels. The kinetic energy release (KER) distributions for the associated electron capture process show a shift in the mean KER values toward the higher side with increasing capture stabilization. The interplay between the different projectile autoionization processes sheds light on the energy depositions to the system during collisions. The Coulomb potential energy curves give a physical insight into the role of the projectile final states in the dimer fragmentation dynamics. The dimer-axis orientation-dependent cross sections for the asymmetric fragmentation channels reveal a forward–backward asymmetry that arises from the geometry of the collision system. Our findings thus give insight into the impact parameter-controlled fragmentation dynamics of multiply charged Ar 2 m + dimer ions in highly charged ion–dimer slow collisions. [ABSTRACT FROM AUTHOR]

New data are presented on the resonant Auger decay of iodobenzene (C6H5I) in the region of the I 4d−1 ionization threshold. The excited molecules decay by participator and spectator processes to populate single-hole valence states and two-hole, one-particle excited states of the cation, providing new information on the structure of C6H5I+. Excitation of dissociative C6H5I (I 4d5/2,3/2−1)σ* resonances can, in principle, result in ultrafast dissociation to C6H5 + I** and the subsequent autoionization of I**, but no evidence for this process is observed. The results are compared with our recent study of the resonant Auger decay of methyl iodide (CH3I). [ABSTRACT FROM AUTHOR]

Resonant Auger processes provide a unique perspective on electronic interactions and excited vibrational and electronic states of molecular ions. Here, new data are presented on the resonant Auger decay of excited CH3I in the region just below the I 4d−1 ionization threshold. The resonances include the Rydberg series converging to the five spin–orbit and ligand-field split CH3I (I 4d−1) thresholds, as well as resonances corresponding to excitation from the I 4d5/2,3/2 orbitals into the σ* lowest unoccupied molecular orbital. This study focuses on participator decay that populates the lowest lying states of CH3I+, in particular, the X ̃ 2E3/2 and 2E1/2 states, and on spectator decay that populates the lowest-lying (CH3I2+)σ* states of CH3I+. The CH3I (I 4d−1)σ* resonances are broad, and dissociation to CH3 + I competes with the autoionization of the core-excited states. Auger decay as the molecule dissociates produces a photoelectron spectrum with a long progression (up to v3+ ∼ 25) in the C–I stretching mode of the X ̃ 2E3/2 and 2E1/2 states, providing insights into the shape of the dissociative core-excited surface. The observed spectator decay processes indicate that CH3I+ is formed on the repulsive wall of the lower-lying (CH3I2+)σ* potentials, and the photon-energy dependence of the processes provides insights into the relative slopes of the (4d−1)σ* and (CH3I2+)σ* potential surfaces. Data are also presented for the spectator decay of higher lying CH3I (I 4d−1)nl Rydberg resonances. Photoelectron angular distributions for the resonant Auger processes provide additional information that helps distinguish these processes from the direct ionization signal. [ABSTRACT FROM AUTHOR]

MXene quantum dots (MQDs), in contrast to their precursor metallic MXenes, display photoluminescence (PL), and with the advantages of non‐toxicity, ease of synthesis, and low cost, they are promising quantum materials for optoelectronic and photonic devices. However, as‐synthesized MQDs suffer from low quantum yield (QY) and a large Stokes shift, limiting efficient UV emission, and are subject to Auger recombination, that is, a severe decline of QY and PL lifetime with increasing exciton density. Here, fluorine‐free Ti2N MQDs are synthesized using a single‐step solvothermal process, which emits UV light of a peak wavelength of 370 nm with a greatly improved QY of 17.4%, and superior resistance to Auger recombination. Band structure calculations and X‐ray photoelectron spectroscopy measurements indicate that Ti2N MQDs synthesized by using the solvothermal process are free of fluorine which is normally prevalent on the surfaces of MQDs prepared by an ordinary hydrothermal process. The results shed light on the mechanism of improving QY and mitigating Auger recombination of MQDs helping their practical applications, especially for photonic devices in the UV range. [ABSTRACT FROM AUTHOR]

We report the experimental measurements of the decay rate of polar cesium nD5/2 − 6S1/2 Rydberg-ground molecules with a large principal quantum number range of 35 ≤ n ≤ 40. Rydberg molecules are prepared employing the method of two-photon photoassociation and the molecular (atomic) ions, due to autoionization (blackbody photoionization), are detected with a microchannel plate detector. The decay rate Γ of the vibrational ground state of the deep and shadow bound molecules for triplet (TΣ) and mixed singlet-triplet (S,TΣ) are measured by fitting the molecular population with the exponential function. Comparing with the parent atom, the decay rate of the polar Rydberg-ground molecule shows an obvious increase with a magnitude of a few μs. The possible dissociation mechanism of polar Rydberg-ground molecules including a collisional decay, blackbody induced decay, and coupling of adjacent Rydberg states and tunneling decay are discussed in detail. The theoretical model is induced to simulate the measurements, showing agreement. [ABSTRACT FROM AUTHOR]

The Zeeman-split spin states of a single quantum dot can be used together with its optical trion transitions to form a spin–photon interface between a stationary (the spin) and a flying (the photon) quantum bit. In addition to long coherence times of the spin state itself, the limiting decoherence mechanisms of the trion states are of central importance. Here, we investigate in time-resolved resonance fluorescence the electron spin and trion dynamics in a single self-assembled quantum dot in an applied magnetic field of up to B = 10 T. The quantum dot is only weakly coupled to an electron reservoir with tunneling rates of about 1 ms − 1 . Using this sample structure, we can measure, in addition to the spin-flip rate of the electron and the spin-flip Raman rate of the trion transition, the Auger recombination process that scatters an Auger electron into the conduction band. The Auger effect destroys the radiative trion transition and leaves the quantum dot empty until an electron tunnels from the reservoir into the dot. The combination of an Auger recombination event with subsequent electron tunneling from the reservoir can flip the electron spin and thus constitutes another mechanism that limits the spin lifetime. [ABSTRACT FROM AUTHOR]

We present a program package for the simulation of ultrafast vibration-induced autoionization dynamics in molecular anions in the manifold of the adiabatic anionic states and the discretized ionization continuum. This program, called HORTENSIA (Hopping Real-time Trajectories for Electron-ejection by Nonadiabatic Self-Ionization in Anions), is based on the nonadiabatic surface-hopping methodology, wherein nuclei are propagated as an ensemble along classical trajectories in the quantum-mechanical potential created by the electronic density of the molecular system. The electronic Schrödinger equation is numerically integrated along the trajectory, providing the time evolution of electronic state coefficients, from which switching probabilities into discrete electronic states are determined. In the case of a discretized continuum state, this hopping event is interpreted as the ejection on an electron. The derived diabatic and nonadiabatic couplings in the time-dependent electronic Schrödinger equation are calculated from anionic and neutral wavefunctions obtained from quantum-chemical calculations with commercially available program packages interfaced with our program. Based on this methodology, we demonstrate the simulation of autoionization electron kinetic energy spectra that are both time- and angle-resolved. In addition, the program yields data that can be interpreted easily with respect to geometric characteristics, such as bonding distances and angles, which facilitate the detection of molecular configurations important for the autoionization process. Furthermore, several useful extensions are included, namely, tools for the generation of initial conditions and input files as well as for the evaluation of output files, all of this both through console commands and a graphical user interface. [ABSTRACT FROM AUTHOR]

The fragmentation of fulminic acid, HCNO, after excitation and ionization of core electrons was investigated using Auger-electron–photoion coincidence spectroscopy. A considerable degree of site-selectivity is observed. Ionization of the carbon and oxygen 1s electron leads to around 70% CH+ + NO+, while ionization at the central N-atom produces only 37% CH+ + NO+, but preferentially forms O+ + HCN+ and O+ + CN+. The mass-selected Auger-electron spectra show that these fragments are associated with higher binding energy final states. Furthermore, ionization of the C 1s electron leads to a higher propensity for C–H bond fission compared to O 1s ionization. Following resonant Auger–Meitner decay after 1s → 3π excitation, 12 different ionic products are formed. At the C 1s edge, the parent ion HCNO+ is significantly more stable compared to the other two edges, which we also attribute to the higher contribution of final states with low binding energies in the C 1s resonant Auger electron spectra. [ABSTRACT FROM AUTHOR]

Intermolecular Coulombic decay or electron transfer-mediated decay are the autoionization processes through which a molecule can relax. This relaxation is only possible if the inner valence's ionization potential (IP) exceeds the system's double ionization potential (DIP). To study the effects of charge and solvation shell, we have calculated the IP, DIP values, and lifetime of Na-2s and Mg-2s temporary bound states in various optimized structures of Na+-(H2O)n and Mg2+-(H2O)n (n = 1–5) micro-solvated clusters, where n water molecules are distributed in a way that some are directly bound to the metal ion and the rest to the water molecules. The first and second solvation shells are the names for the former and the latter water-binding positions, respectively. For a given n, the lifetime of decaying states is longer when water molecules are in the second solvation shell. We found that the Mg-2p state can decay for all n values in Mg2+-(H2O)n clusters, whereas the Na-2p state's decay is possible for n ≥ 2 in Na+-(H2O)n clusters. Our findings highlight the influence of metal ions' charge, different solvation shell structures, and the number of water molecules on the decay rate. These systems are relevant to the human body, which makes this study significant. [ABSTRACT FROM AUTHOR]

Polycyclic aromatic hydrocarbons have widely been conjectured to be ubiquitous in space, as supported by the recent discovery of two isomers of cyanonaphthalene, indene, and 2-cyanoindene in the Taurus molecular cloud-1 using radioastronomy. Here, the photoionization dynamics of 1-cyanonaphthalene (1-CNN) are investigated using synchrotron radiation over the hν = 9.0–19.5 eV range, revealing that prompt autoionization from the plasmon resonance dominates the photophysics for hν = 11.5–16.0 eV. Minimal photo-induced dissociation, whether originating from an excited state impulsive bond rupture or through internal conversion followed by a statistical bond cleavage process, occurs over the microsecond timescale (as limited by the experimental setup). The direct photoionization cross section and photoelectron angular distributions are simulated using an ezDyson model combining Dyson orbitals with Coulomb wave photoejection. When considering these data in conjunction with recent radiative cooling measurements on 1-CNN+, which showed that cations formed with up to 5 eV of internal energy efficiently stabilize through recurrent fluorescence, we conclude that the organic backbone of 1-CNN is resilient to photodestruction by VUV and soft XUV radiation. These dynamics may prove to be a common feature for the survival of small polycyclic aromatic hydrocarbons in space, provided that the cations have a suitable electronic structure to support recurrent fluorescence. [ABSTRACT FROM AUTHOR]

Nonlayered palladium sulfide (PdS) is of interest due to its rich physical properties and promising applications in optoelectronic devices. However, the growth of thin nonlayered PdS remains challenging because of its intrinsic 3D lattice structure. Here, the first demonstration of the direct synthesis of thin rectangular PdS ribbons/flakes on SiO2/Si substrates by a facile chemical vapor deposition (CVD) approach is presented. The atomic structure and high crystalline quality of CVD‐derived PdS crystals are shown by scanning transmission electron microscopy. The nonlinear saturable absorption and absorption enhancement are revealed by using ultrafast optical pump‐probe spectroscopy, and the photocarrier dynamics present the hot phonon bottleneck and Auger recombination effects. Additionally, the Raman vibration modes display the polarization‐dependent properties verified by angle‐resolved polarized Raman spectroscopy. Importantly, the photodetector based on PdS ribbon demonstrates a decent photoresponsivity of ≈7.7 × 103 A W−1. These results provide an effective way to form thin nonlayered PdS with potential applications in the field of photodetection. [ABSTRACT FROM AUTHOR]

Charge transfer between molecules lies at the heart of many chemical processes. Here, we focus on the ultrafast electron dynamics associated with the formation of charge-transfer-to-solvent (CTTS) states following X-ray absorption in aqueous solutions of Na+, Mg2+, and Al3+ ions. To explore the formation of such states in the aqueous phase, liquid-jet photoemission spectroscopy is employed. Using the core-hole-clock method, based on Auger–Meitner (AM) decay upon 1s excitation or ionization of the respective ions, upper limits are estimated for the metal-atom electron delocalization times to the neighboring water molecules. These delocalization processes represent the first steps in the formation of hydrated electrons, which are determined to take place on a timescale ranging from several hundred attoseconds (as) below the 1s ionization threshold to only 20 as far above the 1s ionization threshold. The decrease in the delocalization times as a function of the photon energy is continuous. This indicates that the excited electrons remain in the vicinity of the studied ions even above the ionization threshold, i.e., metal-ion electronic resonances associated with the CTTS state manifolds are formed. The three studied isoelectronic ions exhibit quantitative differences in their electron energetics and delocalization times, which are linked to the character of the respective excited states. The authors investigate the X-ray-induced electron dynamics, on the sub-femtosecond timescale, of hydrated Na+, Mg2+, and Al3+ ions providing insights into the ultrafast charge-transfer processes in aqueous environments. [ABSTRACT FROM AUTHOR]

Extending the emission wavelength of III‐V nanowire (NW) lasers grown on silicon into the mid‐infrared (MIR) spectral range has strong potential for applications. Examples include optical sensing and metrology, as well as integrated silicon photonics for information technologies. NW‐lasers with continuous wave (CW) operation, have remained, however, scarce in the MIR due to significant material physics challenges, and intrinsic effects such as Auger recombination that limit the radiative efficiency. Here, the CW operation of single InAs NW‐lasers site‐selectively grown on Si with emission in the range of 2.4–2.7 µm is reported. The cavity design is optimized via simulations of the threshold material gain and the parameters for selective area growth to minimize the modal gain for the TE01 optical mode. For NW diameters exceeding 700 nm, lasing under CW optical pumping with low thresholds of 1.4–27 kW cm−2 are obtained from 10 to 90 K for NW lengths ranging from 9–30 µm. The observed lasing behavior is quantified by the observation of clear positive net modal gain (630 cm−1) obtained using Hakki‐Paoli analysis. These findings mark an important advancement in the development of nanolasers for integrated MIR photonics. [ABSTRACT FROM AUTHOR]

In this study, we use the UK Molecular r-matrix (ukrmol) codes in the close-coupling approximation to examine the photoionization of hydrogen halides (hydrogen fluoride, hydrogen chloride, and hydrogen bromide). This article reports the total and partial photoionization cross-sections for the |$\mathrm{X}^2 \Pi$|⁠ , |$\mathrm{A}^2 \Sigma ^{+}$|⁠ , and |$\mathrm{B}^2 \Sigma ^{+}$| ionic states of these halides. The calculated cross-sections are compared with the available literature, which does not accurately represent the effective cross-sections near the threshold region, which is dominated by the Rydberg series autoionization resonances converging to the |$\mathrm{A}^2 \Sigma ^{+}$| ionic state. There seems to have been minimal effort to investigate the Rydberg-bound states of these halides. Meanwhile, the r-matrix approaches have traditionally excelled at characterizing such studies. This indicates the effectiveness of this method for molecular photoionization as well as for understanding the resonant contribution to the photoionization cross-sections. The detailed cross-sections calculated comprise the complex autoionizing resonance structures capable of significantly contributing to the computations of total photoionization rates, which are necessary to maintain a steady state of ionization in astrophysical plasmas. Comparisons with the experimental measurements and the theoretical data generally show reasonable agreement across the reported energy range. [ABSTRACT FROM AUTHOR]

We have evaluated total and partial photoionization cross sections, β asymmetry parameters, and molecular frame photoelectron angular distributions (MFPADs) of the water molecule by using the XCHEM methodology. This method accounts for electron correlation in the electronic continuum, which is crucial to describe Feshbach resonances and their autoionization decay. We have identified a large number of Feshbach resonances, some of them previously unknown, in the region between 12.2 and 18.7 eV, for which we provide energy positions and widths. Many of these resonances lead to pronounced peaks in the photoionization spectra, some of them remarkably wide (up to 0.2 eV, for resonances converging to the third ionization threshold), which should be observable in high-energy resolution experiments. We show that, in the vicinity of these peaks, both asymmetry parameters and MFPADs vary very rapidly with photoelectron energy, which, as in atoms and simpler molecules, reflects the interference between direct ionization and autoionization, which is mostly driven by electron correlation. [ABSTRACT FROM AUTHOR]

Characterization of the inner-shell decay processes in molecules containing heavy elements is key to understanding x-ray damage of molecules and materials and for medical applications with Auger-electron-emitting radionuclides. The 1s hole states of heavy atoms can be produced by absorption of tunable x rays and the resulting vacancy decays characterized by recording emitted photons, electrons, and ions. The 1s hole states in heavy elements have large x-ray fluorescence yields that transfer the hole to intermediate electron shells that then decay by sequential Auger-electron transitions that increase the ion's charge state until the final state is reached. In molecules, the charge is spread across the atomic sites, resulting in dissociation to energetic atomic ions. We have used x-ray/ion coincidence spectroscopy to measure charge states and energies of Iq+ and Brq′+ atomic ions following 1s ionization at the I and Br K-edges of IBr. We present the charge states and kinetic energies of the two correlated fragment ions associated with core-excited states produced during the various steps of the cascades. To understand the dynamics leading to the ion data, we develop a computational model that combines Monte-Carlo/Molecular-Dynamics (MC/MD) simulations with a classical over-the-barrier model to track inner-shell cascades and redistribution of electrons in valence orbitals and nuclear motion of fragments. [ABSTRACT FROM AUTHOR]

Protic ionic liquids (PILs), made from anhydrous mixtures of Bronsted acids HA and bases B (HA + B → BH+ + A−), occasionally suffer from limited ionicity. In cases of "poor" PILs (<10% ionicity, e.g., using carboxylic acids), past simulations have hinted that ion-pair association, more than incomplete proton transfer, is at fault. To improve upon the Fuoss equation for predicting the degree of ion pairing, new electrostatic equations (including induced dipoles) are presented, for ion-pair and other associations that occur in anhydrous amine/carboxylic acid mixtures. The equations present the association Gibbs energies ΔGA (and thus the association constants KA) as functions of three fundamental properties: the acid/base mixing ratio (n = xA/xB), the HA-to-B proton-transfer strength (ΔpKa,ε=78), and the dielectric constant (relative permittivity) of the mixture (ε). Parameter values were obtained from fits to constant-dielectric quantum chemistry data (obtained and presented here). These ΔGA functions were then used to predict ΔGioniz values for the net ion-generating (autoionization) equilibrium in carboxylic acid/amine mixtures: 2 B (H A) n ⇄ B (H A) n − d H B + + A (H A) n + d − 1 − , where n = xA/xB and d = degree of disproportionation. The agreement with experiment was excellent, demonstrating that these equations could have useful predictive power. [ABSTRACT FROM AUTHOR]

We present a novel method for the simulation of the vibration-induced autoionization dynamics in molecular anions in the framework of the quantum–classical surface hopping approach. Classical trajectories starting from quantum initial conditions are propagated on a quantum-mechanical potential energy surface while allowing for autoionization through transitions into discretized continuum states. These transitions are induced by the couplings between the electronic states of the bound anionic system and the electron-detached system composed of the neutral molecule and the free electron. A discretization scheme for the detached system is introduced, and a set of formulas is derived that enable the approximate calculation of couplings between the bound and free-electron states. We demonstrate our method on the example of the anion of vinylidene, a high-energy isomer of acetylene, for which detailed experimental data are available. Our results provide information on the time scale of the autoionization process and give insight into the energetic and angular distribution of the ejected electrons, as well as the associated changes in the molecular geometry. We identify the formation of structures with reduced C–C bond lengths and T-like conformations through bending of the CH2 group with respect to the C–C axis and point out the role of autoionization as a driving process for the isomerization to acetylene. [ABSTRACT FROM AUTHOR]

In this work, we study the magnetic phases of a spatially modulated chain of spin-1 Rydberg excitons. Using the Density Matrix Renormalization Group (DMRG) technique, we study various magnetic and topologically nontrivial phases using both single-particle properties, such as local magnetization and quantum entropy, and many-body ones, such as pair-wise Néel and long-range string correlations. In particular, we investigate the emergence and robustness of the Haldane phase, a topological phase of anti-ferromagnetic spin-1 chains. Furthermore, we devise a hybrid quantum algorithm employing restricted Boltzmann machine to simulate the ground state of such a system that shows very good agreement with the results of exact diagonalization and DMRG. [ABSTRACT FROM AUTHOR]

We report the syntheses of tin(II) salts of the types [L1SnX]SnX3 [L1=2,6‐{(i‐PrO)2(O)P}2C5H3N: 1, X=Cl; 2, X=Br], [L2SnCl]SnCl3 [L2=2‐{(i‐PrO)Ph(O)P}‐6‐{(i‐PrO)2(O)P}C5H3N: 3], [L3SnX]SnX3 [L3=2,6‐{MeO(O)C}2C5H3N: 4, X=Cl; 5, X=Br], [L4SnX]SnX3 [L4=2,6‐{Et2N(O)C}2C5H3N: 6, X=Cl; 7, X=Br]. These compounds were obtained by addition of SnX2 to the corresponding ligand inducing autoionization of the respective tin(II) halide. The thermal stability of 1, 3, and 4 was elucidated, giving, under ester cleavage and cyclisation, the tin(II) derivatives 8–12. The reaction of [L1SnCl]SnCl3 (1) with W(CO)4(thf)2 afforded the tungsten tetracarbonyl complex [{L1SnCl}{SnCl3}W(CO)4] (13), representing the first example in which a tin(II) stannate anion and a tin(II) stannylium cation simultaneously coordinate to a transition metal centre. The compounds were characterized by single crystal X‐ray diffraction analyses and in part by elemental analyses, IR and NMR spectroscopy, electrospray ionization mass spectrometry. DFT calculations accompany the experimental work. [ABSTRACT FROM AUTHOR]

The development of renewable sources for energy production has assumed a vital role in recent years, particularly with regard to the preservation of energy supplies and the environment. In this regard, municipal green waste (MGW) can be a potential renewable energy source if it is integrated with emerging technology, like pyrolysis. Therefore, this study aimed at investigating the effect of residence time and particle size on the yield and composition of oil derived from MGW using fast pyrolysis in an auger reactor. The residence time and particle size were varied from 1 min to 4 min and 1 mm to 10 mm, respectively, while keeping the temperature constant at 500 °C. At a residence time of 3 min, a 2 mm particle size provided the highest bio-oil yield (39.86%). At this experimental setting, biochar yield of 27.16% and syngas yield of 32.98% were obtained. The characterization of produced bio-oil revealed that a total of nine functional groups were present in the bio-oil. The phenols were highest in amount, followed by aromatics and ketones. The increase in residence time decreased the amount of acidic compounds present in the bio-oil. The water content was decreased by ~11% and the calorific value was increased by ~6% with the increase in particle size from 1 mm to 10 mm. Other properties, such as viscosity, density, cetane number, and flash point, did not change significantly with the change in experimental conditions. With a calorific value of 25+ MJ/kg, although the bio-oil produced from MGW can be used for heating (such as in boilers and furnaces), the use of MGW bio-oil in engines requires appropriate upgrading through procedures like hydrodeoxygenation, catalytic cracking, esterification, etc. [ABSTRACT FROM AUTHOR]

HAXPES measurements were carried out using a Scienta Omicron HAXPES instrument to provide reference spectra for depleted uranium dioxide. High purity uranium dioxide, as confirmed by trace elemental analysis and x-ray diffraction, was synthesized via the integrated dry route from uranium hexafluoride. The material was fixed on double sided carbon tape for the analysis with charge control measures in place. The expanded energy range, using a Ga Kα x-ray source, presents core level photoelectrons not observed in traditional XPS. In addition, a region associated with the x-ray induced Auger transitions MNN is evident at binding energies only achievable with HAXPES. The reference spectra presented here act as the first in a line of proposed investigations into the comparison of XPS and HAXPES from surface to bulk as well as a fundamental understanding of the electronic structure of uranium materials. [ABSTRACT FROM AUTHOR]

X-ray photodesorption yields of N 2 15 and CO 13 are derived as a function of the incident photon energy near the N (∼400 eV) and O K-edge (∼500 eV) for pure N 2 15 ice and mixed CO 13 : N 2 15 ices. The photodesorption spectra from the mixed ices reveal an indirect desorption mechanism for which the desorption of N 2 15 and CO 13 is triggered by the photoabsorption of CO 13 and N 2 15 , respectively. This mechanism is confirmed by the x-ray photodesorption of CO 13 from a layered CO 13 / N 2 15 ice irradiated at 401 eV on the N 1s → π* transition of N 2 15 . This latter experiment enables us to quantify the relevant depth involved in the indirect desorption process, which is found to be 30–40 monolayers in that case. This value is further related to the energy transport of Auger electrons emitted from the photoabsorbing N 2 15 molecules that scatter toward the ice surface, inducing the desorption of CO 13 . The photodesorption yields corrected from the energy that can participate in the desorption process (expressed in molecules desorbed by eV deposited) do not depend on the photon energy; hence, they depend neither on the photoabsorbing molecule nor on its state after Auger decay. This demonstrates that x-ray induced electron stimulated desorption, mediated by Auger scattering, is the dominant process explaining the desorption of N 2 15 and CO 13 from the ices studied in this work. [ABSTRACT FROM AUTHOR]

We propose an electrically pumped laser diode based on multiple HgTe quantum wells with band structure engineered for Auger recombination suppression. A model for accounting for hot phonons is developed for calculating the nonequilibrium temperature of electrons and holes. Using a comprehensive model accounting for carrier drift and diffusion, Auger recombination, and hot-phonon effects, we predict of lasing at λ ∼ 3 μ m at room temperature in the 2.1 nm HgTe/Cd 0.85 Hg 0.15 Te quantum well heterostructure. The output power in the pulse can reach up to 600 mW for 100 nanosecond-duration pulses. [ABSTRACT FROM AUTHOR]

The first measurement of the photoelectron spectrum of the silylidyne free radical, SiH, is reported between 7 and 10.5 eV. Two main photoionizing transitions involving the neutral ground state, X+1Σ+ ← X2Π and a+3Π ← X2Π, are assigned by using ab initio calculations. The corresponding adiabatic ionization energies are derived, IEad(X+1Σ+) = 7.934(5) eV and IEad(a+3Π) = 10.205(5) eV, in good agreement with our calculated values and the previous determination by Berkowitz et al. [J. Chem. Phys. 86, 1235 (1987)] from a photoionization mass spectrometric study. The photoion yield of SiH recorded in this work exhibits a dense autoionization landscape similar to that observed in the case of the CH free radical [Gans et al., J. Chem. Phys. 144, 204307 (2016)]. [ABSTRACT FROM AUTHOR]

A method to calculate the autoionization width from a discretized pseudo-spectrum is proposed. This method relies on an analytic continuation of Green's function within the Fano–Feshbach formalism. The pseudo-spectrum is obtained at the multireference configuration interaction level in a square-integrable basis set, commonly found in quantum chemistry software. Few states around the desired resonance are needed to perform the analytic continuation. This method was applied to atomic (He and Ne) and molecular (HF and benzene) systems, and the results for the autoionization width show good agreement with the available theoretical and experimental values. [ABSTRACT FROM AUTHOR]

Absorption of slow moving electrons by neutral ground state nucleobases has been known to produce resonance metastable states. There are indications that such metastable states may play a key role in DNA/RNA damage. Therefore, herein, we present an ab initio non-Hermitian investigation of the resonance positions and decay rates for the low lying shape-type states of the uracil anion. In addition, we calculate the complex transition dipoles between these resonance states. We employ the resonance via Padé (RVP) method to calculate these complex properties from real stabilization curves by analytical dilation into the complex plane. This method has already been successfully applied to many small molecular systems, and herein, we present the first application of RVP to a medium-sized system. The presented resonance energies are optimized with respect to the size of the basis set and compared with previous theoretical studies and experimental findings. Complex transition dipoles between the shape-type resonances are computed using the optimal basis set. The ability to calculate ab initio energies and lifetimes of biologically relevant systems paves the way for studying reactions of such systems in which autoionization takes place, while the ability to also calculate their complex transition dipoles opens the door for studying photo-induced dynamics of such biological molecules. [ABSTRACT FROM AUTHOR]

Multi-exciton generation by multi-photon absorption under low-energy photons can be thought a reasonable method to reduce the risk of optical damage, especially in photoelectric quantum dot (QD) devices. The lifetime of the multi-exciton state plays a key role in the utilization of photon-induced carriers, which depends on the dynamics of the exciton generation process in materials. In this paper, the exciton generation dynamics of the photon absorption under low-frequency light in CdSe QDs are successfully detected and studied by the temporal resolution transient absorption (TA) spectroscopy method. Since the cooling time of hot excitons extends while the rate of auger recombination is accelerated when incident energy is increased, the filling time of defect states is irregular, and exciton generation experiences a transition from single-photon absorption to multi-photon absorption. This result shows how to change the excitation. Optical parameters can prolong the lifetime of excitons, thus fully extracting excitons and improving the photoelectric conversion efficiency of QD optoelectronic devices, which provides theoretical and experimental support for the development of QD optoelectronic devices. [ABSTRACT FROM AUTHOR]

Most ionospheric models cannot sufficiently reproduce the observed electron density profiles in the E-region ionosphere, since they usually underestimate electron densities and do not match the profile shape. Mitigation of these issues is often addressed by increasing the solar soft X-ray flux which is ineffective for resolving data-model discrepancies. We show that low-resolution cross sections and solar spectral irradiances fail to preserve structure within the data, which considerably impacts radiative processes in the E-region, and are largely responsible for the discrepancies between observations and simulations. To resolve data-model inconsistencies, we utilize new high-resolution (0.001 nm) atomic oxygen (O) and molecular nitrogen (N2) cross sections and solar spectral irradiances, which contain autoionization and narrow rotational lines that allow solar photons to reach lower altitudes and increase the photoelectron flux. This work improves upon Meier et al. (2007, https://doi.org/10.1029/2006gl028484) by additionally incorporating high-resolution N2 photoionization and photoabsorption cross sections in model calculations. Model results with the new inputs show increased O+ production rates of over 500%, larger than those of Meier et al. (2007, https://doi.org/10.1029/2006gl028484) and total ion production rates of over 125%, while N2+ production rates decrease by ~15% in the E-region in comparison to the results obtained using the cross section compilation from Conway (1988, https://apps.dtic.mil/sti/pdfs/ADA193866.pdf). Low-resolution molecular oxygen (O2) cross sections from the Conway compilation are utilized for all input cases and indicate that O2+ is a dominant contributor to the total ion production rate in the E-region. Specifically, the photoionization contributed from longer wavelengths is a main contributor at ~120 km. [ABSTRACT FROM AUTHOR]

We have experimentally determined the electron collisional excitation cross-sections for several 3d→4f and 3d→5f excitations in Ni- to Ge-like Au at energies of ∼ 0.4, 1, 2, and 3 keV above threshold energy, ET, for the 3d→4f excitations (ET ∼ 2.5 keV) and ∼ 0.2, 1, and 2 keV above threshold energy for the 3d→5f excitations (ET ∼ 3.3 keV). The cross-section measurements are possible by using the GSFC micro-calorimeter to record emission spectra from beam plasmas created in the Livermore EBIT-I electron beam ion trap. The cross-sections are experimentally determined from the ratio of the measured intensities of the collisionally excited lines to the intensities of the radiative recombination lines in monoenergetic electron distribution EBIT-I plasmas. The effects of polarization and Auger processes in the beam plasmas are accounted for in the cross-section determination. Experimentally determined cross-sections are compared with those from HULLAC, DWS, and FAC calculations. The measurements exhibit significant differences with the calculations of these excitation cross-sections. [ABSTRACT FROM AUTHOR]

Based on the detailed term accounting approach, the relationship between extreme ultraviolet conversion efficiency and plasma conditions, which range from 5 to 200 eV for plasma temperature and from 4.63 × 1017 to 4.63 × 1022 cm−3 for plasma density, is studied for lithium plasmas through spectral simulations involving very extended atomic configurations, including a benchmark set of autoionizing states. The theoretical limit of the EUV conversion efficiency and its dependence on sustained plasma time are given for different plasma densities. The present study provides the necessary understanding of EUV formation from the perspective of atomic physics and also provides useful knowledge for improving EUV conversion efficiency with different technologies. [ABSTRACT FROM AUTHOR]

In high orbital angular momentum (ℓ ≥ 3) Rydberg states, the centrifugal barrier hinders the close approach of the Rydberg electron to the ion-core. As a result, these core-nonpenetrating Rydberg states can be well described by a simplified model in which the Rydberg electron is only weakly perturbed by the long-range electric properties (i.e., multipole moments and polarizabilities) of the ion-core. We have used a long-range model to describe the vibrational autoionization dynamics of high-ℓ Rydberg states of nitric oxide (NO). In particular, our model explains the extensive angular momentum exchange between the ion-core and the Rydberg electron that had been previously observed in vibrational autoionization of f (ℓ = 3) Rydberg states. These results shed light on a long-standing mechanistic question around these previous observations and support a direct, vibrational mechanism of autoionization over an indirect, predissociation-mediated mechanism. In addition, our model correctly predicts newly measured total decay rates of g (ℓ = 4) Rydberg states because for ℓ ≥ 4, the non-radiative decay is dominated by autoionization rather than predissociation. We examine the predicted NO+ ion rotational state distributions generated by vibrational autoionization of g states and discuss applications of our model to achieve quantum state selection in the production of molecular ions. [ABSTRACT FROM AUTHOR]

Electron transfer (ET) process is considered a substantial factor in influencing the photoelectric conversion efficiency of optoelectronic devices. While pressure has demonstrated effective tune ET, a comprehensive investigation into the mechanisms for both restraining and promoting ET remains elusive. Herein, we have performed measurements using in situ high-pressure steady-state photoluminescence (PL), Raman scattering spectra, and femtosecond transient absorption (fs-TA) spectroscopy on InP/ZnS quantum dot–anthraquinone (InP/ZnS QD-AQ) complexes. The experimental results have demonstrated that the pressure-suppressed ET process in the InP/ZnS QD-AQ complexes arises from both the aggregation-induced emission (AIE) effect of AQ in toluene and the quantum confinement effect of the InP/ZnS QDs. The reduction in the distance between InP/ZnS QD and AQ under pressure emerges as a key factor that promotes the ET process in the InP/ZnS QD-AQ complexes. Furthermore, we observed that the pressure not only enhances the ET process but also suppresses the auger recombination process in liquid phase I of toluene, consequently leading to an enhancement in the photoelectric conversion efficiency. This study contributes to understanding the mechanism of the ultrafast dynamic processes in the pressure-induced QD-receptor complexes, and it has great potential for preparing efficient and stable optoelectronic devices. [ABSTRACT FROM AUTHOR]

The lowest single and doubly excited autoionizing states of neon have been studied using a non-monochromatic electron beam and a high-resolution electrostatic analyzer at incident electron energies from 43.37 to 202 (±0.4) eV at three ejection angles, 40°, 90° and 130°. The 2s2p63s(3,1S) and 2s2p63p(3,1P) as well as the 2p43s3p doubly excited states have been observed and their energy determined. The influence of the PCI effect in the energy region of the 2s2p63s(3,1S) states has been investigated. New features in the ejected electron spectra in the low kinetic energy region 3–20 eV at 202 eV incident energy have been observed and assigned. [ABSTRACT FROM AUTHOR]

We present a theoretical analysis of mid-infrared radiative recombination in InAs/GaSb superlattices (SLs). We employ a semi-analytical plane wave expansion method in conjunction with an 8-band k ⋅ p Hamiltonian to compute the SL electronic structure, paying careful attention to the identification and mitigation of spurious solutions. The calculated SL eigenstates are used directly to compute spontaneous emission spectra and the radiative recombination coefficient B . We elucidate the origin of the relatively large B coefficients in InAs/GaSb SLs which, despite the presence of spatially indirect (type-II-like) carrier confinement, are close to that of bulk InAs and compare favourably to those calculated for mid-infrared type-I pseudomorphic and metamorphic quantum well structures having comparable emission wavelengths. Our analysis explicitly quantifies the roles played by carrier localisation (specifically, partial delocalisation of bound electron states) and miniband formation (specifically, miniband occupation and optical selection rules) in determining the magnitude of B and its temperature dependence. We perform a high-throughput optimisation of the room temperature B coefficient in InAs/GaSb SLs across the 3.5–7 μ m wavelength range, quantifying the dependence of B on the relative thickness of the electron-confining InAs and hole-confining GaSb layers. This analysis provides guidance for the growth of optimised SLs for mid-infrared light emitters. Our results, combined with the expected low non-radiative Auger recombination rates in structures having spatially indirect electron and hole confinement, corroborate recently observed high output power in prototype InAs/GaSb SL inter-band cascade light-emitting diodes. [ABSTRACT FROM AUTHOR]

In quantum dots (QDs), the Auger recombination is a non-radiative scattering process in which the optical transition energy of a charged exciton (trion) is transferred to an additional electron leaving the dot. Electron tunneling from a reservoir is the competing process that replenishes the QD with an electron again. Here, we study the dependence of the tunneling and Auger recombination rate on the applied electric field using high-resolution time-resolved resonance fluorescence (RF) measurements. With the given p–i–n diode structure and a tunnel barrier between the electron reservoir and the QD of 45 nm, we measured a tunneling rate into the QD in the order of ms−1. This rate shows a strong decrease by almost an order of magnitude for decreasing electric field, while the Auger emission rate decreases by a factor of five in the same voltage range. Furthermore, we study in detail the influence of the Auger recombination and the tunneling rate from the charge reservoir into the QD on the intensity and linewidth of the trion transition. In addition to the well-known quenching of the trion transition, we observe in our time-resolved RF measurements a strong influence of the tunneling rate on the observed linewidth. The steady-state RF measurement yields a broadened trion transition of about 1.5 GHz for an Auger emission rate of the same order as the electron tunneling rate. In a non-equilibrium measurement, the Auger recombination can be suppressed, and a more than four times smaller linewidth of 340 MHz (1.4 μeV) is measured. [ABSTRACT FROM AUTHOR]

Non‐Hermitian theory in photonics revolutionized the understanding of optical resonators, thanks to the concept of quasi‐normal modes (QNM) and to a deep revision of the Purcell factor expression. Counterintuitive effects followed, such as complex modal volumes and non‐Lorentzian local density of states (LDOS) of QNMs. One of the fascinating aspects of non‐Hermitian theory is the analogy with quantum mechanics for autoionizing electronic levels where the absorption cross'section is characterized by Fano lineshapes, caused by interference between the probability of absorption in the continuum and in the bound states. In photonics Fano lineshapes can arise from QNM normalization through the complex modal volume. The link between Fano lineshapes in photonic LDOS of QNMs and in the case of autoionizing states needs to be clarified. Here, by developing an analytical model based on the role of losses in the QNM normalization, they clarify the meaning of the phase of QNM normalized fields (qFano parameter),linking QNMs normalization to the concept of interference among the resonant and the leaky modes. This inspired the design of photonic crystal (PhC) cavity that exhibits LDOS with Fano character inside the itself, providing a proof of principle on how to mold the radiative lifetime by Purcell effect. [ABSTRACT FROM AUTHOR]

The paper reports the calculation of the probabilities of Auger transitions taking place in the process of filling a vacancy on the 2pπ-orbital in an Ne+–Ne quasimolecule, a short-lived system which arises when the ion and atom approach each other and decays when they fly apart. Calculations for various ionization degrees of the quasimolecule particles were performed for the first time. It was found out that the system ionization degree increases very significantly (from 2 to 6) with increasing collision energy and decreasing distance of the particles closest approach. Using of the quantum mechanical approach and taking into account the collision dynamics made it possible to quantitatively describe for the first time the experimental Auger electron spectra of a complex many-electron quasimolecule. The contribution of the transition from the initial 3dπ–3dπ state to the 2pπ-orbital was shown to be predominant among the whole variety of possible Auger decay channels. [ABSTRACT FROM AUTHOR]

Understanding high‐order biexciton dynamics is important for the use of semiconductor quantum dots (QDs) in optoelectronic devices. The core–shell structure can be used to modulate biexciton dynamics by varying the shell thickness and core–shell energy band alignment. In this study, the biexciton dynamics in an unconventional case in which each QD is encapsulated by a submonolayer shell are demonstrated. The result of a transient absorption spectroscopic study shows that InP/ZnS core/shell QDs with submonolayer shell coverage exhibit a prolonged Auger lifetime. However, the QD size dependence of the Auger recombination time features two constant distinct stages instead of the typical monotonic volume scaling law in conventional QDs. It is attributed to the tradeoff between the enlarged QD size and quantum‐well confinement for the Auger processes. However, the abrupt change between the two stages is due to the change in the shell coverage. This study provides a reference for the application of core–shell QDs in optoelectronic devices in which full coverage of the shell is not achieved. [ABSTRACT FROM AUTHOR]

X-ray photon absorption leads to the creation of highly excited species, which often decay through the Auger process. The theoretical treatment of Auger decay is challenging because of the resonance nature of the initial core-excited or core-ionized states and the continuous nature of the ejected electron. In Paper I [W. Skomorowski and A. I. Krylov, J. Chem. Phys. 154, 084124 (2021)], we have introduced a theoretical framework for computing Auger rates based on the Feshbach–Fano approach and the equation-of-motion coupled-cluster ansätze augmented with core–valence separation. The outgoing Auger electron is described with a continuum orbital. We considered two approximate descriptions—a plane wave and a Coulomb wave with an effective charge. Here, we use the developed methodology to calculate Auger transition rates in core-ionized and core-excited benchmark systems (Ne, H2O, CH4, and CO2). Comparison with the available experimental spectra shows that the proposed computational scheme provides reliable ab initio predictions of the Auger spectra. The reliability, cost efficiency, and robust computational setup of this methodology offer advantages in applications to a large variety of systems. [ABSTRACT FROM AUTHOR]

X-ray absorption creates electron vacancies in the core shell. These highly excited states often relax by Auger decay—an autoionization process in which one valence electron fills the core hole and another valence electron is ejected into the ionization continuum. Despite the important role of Auger processes in many experimental settings, their first-principles modeling is challenging, even for small systems. The difficulty stems from the need to describe many-electron continuum (unbound) states, which cannot be tackled with standard quantum-chemistry methods. We present a novel approach to calculate Auger decay rates by combining Feshbach–Fano resonance theory with the equation-of-motion coupled-cluster single double (EOM-CCSD) framework. We use the core–valence separation scheme to define projectors into the bound (square-integrable) and unbound (continuum) subspaces of the full function space. The continuum many-body decay states are represented by products of an appropriate EOM-CCSD state and a free-electron state, described by a continuum orbital. The Auger rates are expressed in terms of reduced quantities, two-body Dyson amplitudes (objects analogous to the two-particle transition density matrix), contracted with two-electron bound-continuum integrals. Here, we consider two approximate treatments of the free electron: a plane wave and a Coulomb wave with an effective charge, which allow us to evaluate all requisite integrals analytically; however, the theory can be extended to incorporate a more sophisticated description of the continuum orbital. [ABSTRACT FROM AUTHOR]

In this study, we investigate the nuclear quantum effects (NQEs) on the acidity constant (pKA) of liquid water isotopologs under the ambient condition by path integral molecular dynamics (PIMD) simulations. We compared simulations using a fully explicit solvent model with a classical polarizable force field, density functional tight binding, and ab initio density functional theory, which correspond to empirical, semiempirical, and ab initio PIMD simulations, respectively. The centroid variable with respect to the proton coordination number of a water molecule was restrained to compute the gradient of the free energy, which measures the reversible work of the proton abstraction for the quantum mechanical system. The free energy curve obtained by thermodynamic integration was used to compute the pKA value based on probabilistic determination. This technique not only reproduces the pKA value of liquid D2O experimentally measured (14.86) but also allows for a theoretical prediction of the pKA values of liquid T2O and aqueous HDO and HTO, which are unknown due to their scarcity. It is also shown that the NQEs on the free energy curve can result in a downshift of 4.5 ± 0.9 pKA units in the case of liquid water, which indicates that the NQEs plays an indispensable role in the absolute determination of pKA. The results of this study can help inform further extensions into the calculation of the acidity constants of isotope substituted species with high accuracy. [ABSTRACT FROM AUTHOR]

Multi-electron coincidence measurements have been performed at the photon energies for the core-to-valence (1s → π*) and core-to-Rydberg (1s → 3sσ and 3pπ) resonant excitations in N2 in order to investigate the dynamics of multiple Auger-electron emissions from these core-excited states in detail. Peaks due to slow electrons from superexcited atomic fragments are observed in the decay processes by emission of two or three Auger electrons, indicating stepwise (cascade) multiple Auger decays that involve faster dissociations than electronic relaxations. Energy partitions between the emitted electrons enable us to reveal the detailed decay mechanisms for these processes. Branching ratios among the decays by emission of one, two, or three Auger electrons and those between the simultaneous (direct) and stepwise (cascade) processes have been determined for each of the core-excited states. Branching ratios of decay channels resulting in molecular or fragment ions have also been substantiated. [ABSTRACT FROM AUTHOR]

The generally accepted pathway to Local Thermodynamic Equilibrium (LTE) in atomic physics, where collision rates need to be much larger than radiative decay rates, is extended to complex autoionizing states. It is demonstrated that the inclusion of the non-radiative decay (autoionization rate) on the same footing, like radiative decay, i.e., the LTE criterion n e , c r i t × C ≫ A + Γ ( n e , c r i t is the critical electron density above which LTE holds, C is the collisional rate coefficient, and A is the radiative decay rate) is inappropriate for estimating the related critical density. An analysis invoking simultaneously different atomic ionization stages identifies the LTE criteria as a theoretical limiting case, which provides orders of magnitude too high critical densities for almost all practical applications. We introduced a new criterion, where the critical densities are estimated from the non-autoionizing capture states rather than from the autoionizing states. The new criterion is more appropriate for complex autoionizing manifolds and provides order of magnitude reduced critical densities. Detailed numerical calculations are carried out for Na-like states of aluminum, where autoionization to the Ne-like ground and excited state occurrences are in excellent agreement with the new criterion. In addition, a complex multi-electron atomic-level structure and electron–electron correlation are identified as simplifying features rather than aggravating ones for the concept of thermalization. [ABSTRACT FROM AUTHOR]

We study photoluminescence temperature quenching in HgTe/CdHgTe quantum wells (QWs) emitting at 3–4 μm wavelengths and recover temperature-dependent interband recombination rates. Recombination coefficients are determined for the process that we identify as a non-threshold ehh Auger process involving valence band continuum states in barriers. With the effective Auger coefficient CA reaching ∼10−13 cm4/s under resonant conditions, such a process is shown to determine stimulated emission thresholds in a wide temperature interval, while the contribution of conventional, activated Auger processes is presumably rather limited. Thus, threshold energy considerations should be used with caution for the optimization of HgCdTe QW lasers operating around 3 μm, and relatively low-barrier QWs may provide better performance than the high-barrier ones despite lower energy thresholds for thermally activated eeh-Auger recombination. It holds as long as the conduction band offset is detuned from the bandgap energy to avoid additional non-threshold eeh-processes and sufficient hole localization at elevated temperatures is maintained. [ABSTRACT FROM AUTHOR]

The evolution of the luminescence blinking of single CsPbBr3 perovskite nanocrystals with a characteristic size of ~25 nm during photodegradation has been experimentally investigated. It has been demonstrated that the blue shift of the luminescence peak and a decrease in the average luminescence intensity are accompanied by the increasing role of nonradiative Auger processes underlying the charging mechanism of blinking. A method based on the analysis of photon antibunching g2(0) and exciton and biexciton recombination rates is used to determine the blinking mechanism. The data obtained have made it possible to reveal a transition from the trapping to charging blinking mechanism with a change in the sizes of a CsPbBr3 single nanocrystal. [ABSTRACT FROM AUTHOR]

Background: In radionuclide therapy, to enhance therapeutic efficacy, an intriguing alternative is to ensure the simultaneous implementation of low- and high-LET radiation emitted from a one radionuclide. In the present study, we introduce the concept of utilizing 109Pd (T1/2 = 13.7 h) in the form of a 109Pd/109mAg in vivo generator. In this system, 109Pd emits beta particles of medium energy, while 109mAg releases a cascade of conversion and Auger electrons. 109Pd was utilized in the form of 15 nm gold nanoparticles, which were coated with a monolayer of 109Pd. In this system, the 109Pd atoms are on the surface of the nanoparticle, while the 109mAg atoms generated in the decay reaction possess the capability for unhindered emission of Auger electrons. Results: 109Pd, obtained through neutron irradiation of natural palladium, was deposited onto 15-nm gold nanoparticles, exceeding a efficiency rate of 95%. In contrast to previously published data on in vivo generators based on chelators, where the daughter radionuclide diffuses away from the molecules, daughter radionuclide 109mAg remains on the surface of gold nanoparticles after the decay of 109Pd. To obtain a radiobioconjugate with an affinity for HER2 receptors, polyethylene glycol chains and the monoclonal antibody trastuzumab were attached to the Au@Pd nanoparticles. The synthesized bioconjugate contained an average of 9.5 trastuzumab molecules per one nanoparticle. In vitro cell studies indicated specific binding of the Au@109Pd-PEG-trastuzumab radiobioconjugate to the HER2 receptor on SKOV-3 cells, resulting in 90% internalization. Confocal images illustrated the accumulation of Au@109Pd-PEG-trastuzumab in the perinuclear area surrounding the cell nucleus. Despite the lack of nuclear localization, which is necessary to achieve an effective cytotoxic effect of Auger electrons, a substantial cytotoxic effect, significantly greater than that of pure β− and pure Auger electron emitters was observed. We hypothesize that in the studied system, the cytotoxic effect of the Auger electrons could have also occurred through the damage to the cell's nuclear membrane by Auger electrons emitted from nanoparticles accumulated in the perinuclear area. Conclusion: The obtained results show that trastuzumab-functionalized 109Pd-labeled nanoparticles can be suitable for the application in combined β−—Auger electron targeted radionuclide therapy. Due to both components decay (β− and conversion/Auger electrons), the 109Pd/109mAg in vivo generator presents unique potential in this field. Despite the lack of nuclear localization, which is highly required for efficient Auger electron therapy, an adequate cytotoxic effect was attained. [ABSTRACT FROM AUTHOR]

We measured spectra of low energy electrons emitted in the interaction of singly charged Ne+ ions with the Mg surface at incident ion energies ranging from 50 eV to 4 keV. The study examines issues related to the excitation of both the surface and the bulk plasmons of the target. We will also focus on the dynamics of the production of the singlet Ne2p4(1D)3s2 and triplet Ne2p4(3P)3s2 autoionizing states of projectiles scattered in a vacuum. The threshold behavior of the autoionization lines show that double excitation occurs simultaneously in a single scattering. The predominant excitation of the triplet state indicates the importance of charge rearrangement and the electron correlation effects during the collisional excitation. [ABSTRACT FROM AUTHOR]