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In this study X-ray Photoelectron Spectroscopy and Ultraviolet Photoelectron Spectroscopy were combined to investigate the effect of oxygen incorporation on the valence band behaviour of ZrO x . The Auger transitions involving valence bands are found to mimic the self-folded density of state measured using Ultraviolet Photoelectron Spectroscopy. The valence band once constructed in a sub-oxide form, stays at a fixed energy position despite the change in the stoichiometry. This behaviour is found to be useful in setting a reference for X-ray Photoelectron Spectroscopy charge correction. The results of the charged corrected spectra were compared to other methods and found to be in great agreement. Finally, a correlation between the core-level binding energy and the structural property of ZrO x is given.

PurposeThe prostate-specific membrane antigen (PSMA) has emerged as an interesting target for radionuclide therapy of metastasized castration-resistant prostate cancer (mCRPC). The aim of this study was to investigate 161Tb (T1/2 = 6.89 days; Eβ͞av = 154 keV) in combination with PSMA-617 as a potentially more effective therapeutic alternative to 177Lu-PSMA-617, due to the abundant co-emission of conversion and Auger electrons, resulting in an improved absorbed dose profile.Methods161Tb was used for the radiolabeling of PSMA-617 at high specific activities up to 100 MBq/nmol. 161Tb-PSMA-617 was tested in vitro and in tumor-bearing mice to confirm equal properties, as previously determined for 177Lu-PSMA-617. The effects of 161Tb-PSMA-617 and 177Lu-PSMA-617 on cell viability (MTT assay) and survival (clonogenic assay) were compared in vitro using PSMA-positive PC-3 PIP tumor cells. 161Tb-PSMA-617 was further investigated in therapy studies using PC-3 PIP tumor-bearing mice.Results161Tb-PSMA-617 and 177Lu-PSMA-617 displayed equal in-vitro properties and tissue distribution profiles in tumor-bearing mice. The viability and survival of PC-3 PIP tumor cells were more reduced when exposed to 161Tb-PSMA-617 as compared to the effect obtained with the same activities of 177Lu-PSMA-617 over the whole investigated concentration range. Treatment of mice with 161Tb-PSMA-617 (5.0 MBq/mouse and 10 MBq/mouse, respectively) resulted in an activity-dependent increase of the median survival (36 vs 65 days) compared to untreated control animals (19 days). Therapy studies to compare the effects of 161Tb-PSMA-617 and 177Lu-PSMA-617 indicated the anticipated superiority of 161Tb over 177Lu.Conclusion161Tb-PSMA-617 showed superior in-vitro and in-vivo results as compared to 177Lu-PSMA-617, confirming theoretical dose calculations that indicate an additive therapeutic effect of conversion and Auger electrons in the case of 161Tb. These data warrant more preclinical research for in-depth investigations of the proposed concept, and present a basis for future clinical translation of 161Tb-PSMA-617 for the treatment of mCRPC.

Determining the electron neutrino mass by electron capture in 163Ho relies on an accurate understanding of the differential electron capture nuclear decay rate as a function of the distribution of the total decay energy between the neutrino and electronic excitations. The resulting spectrum is dominated by resonances due to local atomic multiplet states with core holes. Coulomb scattering between electrons couples the discrete atomic states, via Auger-Meitner decay, to final states with free electrons. The atomic multiplets are above the auto-ionisation energy, such that the delta functions representing these discrete levels turn into a superposition of Lorentzian, Mahan- and Fano-like line-shapes. We present an ab initio method to calculate nuclear decay modifications due to such processes. It includes states with multiple correlated holes in local atomic orbitals interacting with unbound Auger-Meitner electrons. A strong energy-dependent, asymmetric broadening of the resonances in good agreement with recent experiments is found. We present a detailed analysis of the mechanisms determining the final spectral line-shape and discuss both the Fano interference between different resonances, as well as the energy dependence of the Auger-Meitner Coulomb matrix elements. The latter mechanism is shown to be the dominant channel responsible for the asymmetric line-shape of the resonances in the electron capture spectrum of 163Ho.

We present a measurement of the cosmic-ray spectrum above 100 PeV using the part of the surface detector of the Pierre Auger Observatory that has a spacing of 750 m. An inflection of the spectrum is observed, confirming the presence of the so-called second-knee feature. The spectrum is then combined with that of the 1500 m array to produce a single measurement of the flux, linking this spectral feature with the three additional breaks at the highest energies. The combined spectrum, with an energy scale set calorimetrically via fluorescence telescopes and using a single detector type, results in the most statistically and systematically precise measurement of spectral breaks yet obtained. These measurements are critical for furthering our understanding of the highest energy cosmic rays.

Purpose The β ¯ -emitting terbium-161 also emits conversion and Auger electrons, which are believed to be effective in killing single cancer cells. Terbium-161 was applied with somatostatin receptor (SSTR) agonists that localize in the cytoplasm (DOTATOC) and cellular nucleus (DOTATOC-NLS) or with a SSTR antagonist that localizes at the cell membrane (DOTA-LM3). The aim was to identify the most favorable peptide/terbium-161 combination for the treatment of neuroendocrine neoplasms (NENs). Methods The capability of the 161 Tb- and 177 Lu-labeled somatostatin (SST) analogues to reduce viability and survival of SSTR-positive AR42J tumor cells was investigated in vitro. The radiopeptides’ tissue distribution profiles were assessed in tumor-bearing mice. The efficacy of terbium-161 compared to lutetium-177 was investigated in therapy studies in mice using DOTATOC or DOTA-LM3, respectively. Results In vitro, [ 161 Tb]Tb-DOTA-LM3 was 102-fold more potent than [ 177 Lu]Lu-DOTA-LM3; however, 161 Tb-labeled DOTATOC and DOTATOC-NLS were only 4- to fivefold more effective inhibiting tumor cell viability than their 177 Lu-labeled counterparts. This result was confirmed in vivo and demonstrated that [ 161 Tb]Tb-DOTA-LM3 was significantly more effective in delaying tumor growth than [ 177 Lu]Lu-DOTA-LM3, thereby, prolonging survival of the mice. A therapeutic advantage of terbium-161 over lutetium-177 was also manifest when applied with DOTATOC. Since the nuclear localizing sequence (NLS) compromised the in vivo tissue distribution of DOTATOC-NLS, it was not used for therapy. Conclusion The use of membrane-localizing DOTA-LM3 was beneficial and profited from the short-ranged electrons emitted by terbium-161. Based on these preclinical data, [ 161 Tb]Tb-DOTA-LM3 may outperform the clinically employed [ 177 Lu]Lu-DOTATOC for the treatment of patients with NENs.

Rapid Auger recombination represents an important challenge faced by quasi-2D perovskites, which induces resulting perovskite light-emitting diodes’ (PeLEDs) efficiency roll-off. In principle, Auger recombination rate is proportional to materials’ exciton binding energy ( E b ). Thus, Auger recombination can be suppressed by reducing the corresponding materials’ E b . Here, a polar molecule, p -fluorophenethylammonium, is employed to generate quasi-2D perovskites with reduced E b . Recombination kinetics reveal the Auger recombination rate does decrease to one-order-of magnitude lower compared to its PEA + analogues. After effective passivation, nonradiative recombination is greatly suppressed, which enables resulting films to exhibit outstanding photoluminescence quantum yields in a broad range of excitation density. We herein demonstrate the very efficient PeLEDs with a peak external quantum efficiency of 20.36%. More importantly, devices exhibit a record luminance of 82,480 cd m −2 due to the suppressed efficiency roll-off, which represent one of the brightest visible PeLEDs yet. Designing efficient perovskite light-emitting diodes remains a challenge due to the strong Auger recombination and resulting Joule heating. Here, the authors propose polarizable p -fluorophenethylammonium to generate quasi-2D perovskites with reduced binding energy developing perovskite light-emitting diodes with a peak EQE of 20.36% and a maximum luminance of 82,480 cdm -2 .

Synopsis We report here a detailed experimental study on multiple Auger decay after core excitation into the π* valence and Rydberg orbitals in N2 by an electron-electron coincidence technique.

Metal-halide perovskite light-emitting diodes (PeLEDs) have attracted great interest because of their tunable emission wavelength, narrow emission bandwidth and high external quantum efficiency. However, PeLEDs face two critical issues that limit their potential applications: short device lifetime due to ion migration and low brightness due to severe Auger recombination. Here we demonstrate that both issues can be mitigated by in situ solution-grown perovskite single crystals (SCs). By minimizing the trap density using mixed cations and adding excess ammonium halides and polyvidone to the precursor, the external photoluminescence quantum yield (PLQY) of the SCs is enhanced to 28.3%, corresponding to an internal PLQY of 89.4%. Benefitting from the suppressed Auger recombination in SCs, SC-PeLEDs with a thickness of 1.5 µm exhibit a high luminance of 86,000 cd m−2 and a peak external quantum efficiency of 11.2%. Thanks to suppressed ion migration, the extrapolated T50 lifetime for SC-PeLEDs reaches a value of 12,500 h at an initial luminance of 100 cd m−2. Our results show that SC growth represents a viable route to increase the lifetime of PeLEDs for practical applications.Single-crystal perovskite LEDs exhibit reduced ion migration and Auger recombination and increased device lifetime. Perovskite single-crystals-based LEDs exhibit a maximum brightness of 86,000 cd m−2, a peak EQE of 11.2% and T50 lifetime of 12,500 h at an initial luminance of 100 cd m−2.

Quantum dot (QD) light-emitting diodes (LEDs) are ideal for large-panel displays because of their excellent efficiency, colour purity, reliability and cost-effective fabrication 1 – 4 . Intensive efforts have produced red-, green- and blue-emitting QD-LEDs with efficiencies of 20.5 per cent 4 , 21.0 per cent 5 and 19.8 per cent 6 , respectively, but it is still desirable to improve the operating stability of the devices and to replace their toxic cadmium composition with a more environmentally benign alternative. The performance of indium phosphide (InP)-based materials and devices has remained far behind those of their Cd-containing counterparts. Here we present a synthetic method of preparing a uniform InP core and a highly symmetrical core/shell QD with a quantum yield of approximately 100 per cent. In particular, we add hydrofluoric acid to etch out the oxidative InP core surface during the growth of the initial ZnSe shell and then we enable high-temperature ZnSe growth at 340 degrees Celsius. The engineered shell thickness suppresses energy transfer and Auger recombination in order to maintain high luminescence efficiency, and the initial surface ligand is replaced with a shorter one for better charge injection. The optimized InP/ZnSe/ZnS QD-LEDs showed a theoretical maximum external quantum efficiency of 21.4 per cent, a maximum brightness of 100,000 candelas per square metre and an extremely long lifetime of a million hours at 100 candelas per square metre, representing a performance comparable to that of state-of-the-art Cd-containing QD-LEDs. These as-prepared InP-based QD-LEDs could soon be usable in commercial displays. A method of engineering efficient and stable InP/ZnSe/ZnS quantum dot light-emitting diodes (QD-LEDs) has improved their performance to the level of state-of-the-art cadmium-containing QD-LEDs, removing the problem of the toxicity of cadmium in large-panel displays.

Colloidal quantum dots (QDs) are attractive materials for realizing solution-processable laser diodes that could benefit from size-controlled emission wavelengths, low optical-gain thresholds and ease of integration with photonic and electronic circuits 1 – 7 . However, the implementation of such devices has been hampered by fast Auger recombination of gain-active multicarrier states 1 , 8 , poor stability of QD films at high current densities 9 , 10 and the difficulty to obtain net optical gain in a complex device stack wherein a thin electroluminescent QD layer is combined with optically lossy charge-conducting layers 11 – 13 . Here we resolve these challenges and achieve amplified spontaneous emission (ASE) from electrically pumped colloidal QDs. The developed devices use compact, continuously graded QDs with suppressed Auger recombination incorporated into a pulsed, high-current-density charge-injection structure supplemented by a low-loss photonic waveguide. These colloidal QD ASE diodes exhibit strong, broadband optical gain and demonstrate bright edge emission with instantaneous power of up to 170 μW. Colloidal quantum dot devices demonstrating electrically pumped amplified spontaneous emission are described, showing strong, broadband optical gain and bright edge emission, opening the path to solution-processable laser diodes.