Dielectric barrier discharge low-temperature plasma modification of bamboo charcoal for supercapacitor applications.

Biochar is commonly utilized as an electrode material in supercapacitors. However, the conventional carbonization process often results in macromolecular compounds, which obstruct the porous structure of carbon materials, thereby reducing their capacitance. Dielectric barrier discharge low-temperature plasma (DLTP) is a technology that transforms gases into highly excited states, utilizing high-energy particles for enhanced energy applications. This study investigated the effects of DLTP on the electrochemical performance of bamboo charcoal (BC), utilizing bamboo shavings (BS) as the carbon source. The results indicated that the specific capacitance of BC varied under different atmospheric conditions, input voltages, and treatment durations, thereby achieving a maximum increase of 144 F/g. Furthermore, when combined with KOH activation, DLTP modification further enhanced the specific capacitance of BC to 237 F/g. The DLTP treatment enhanced the specific surface area and the types of functional groups in BC, thereby leading to a significant enhancement of its electrochemical properties.

Ultra-Nonlinear Subcycle Photoemission of Few-Electron States from Sharp Gold Nanotapers.

The generation of ultrashort electron wavepackets is crucial for the development of ultrafast electron microscopes. Recent studies on Coulomb-correlated few-electron number states, photoemitted from sharp metallic tapers, have shown emission nonlinearities in the multiphoton photoemission regime which scale with the electron number. Here, we study few-electron photoemission from gold nanotapers triggered by few-cycle near-infrared pulses, demonstrating extreme 20th-order nonlinearities for electron triplets. We report interferometric autocorrelation traces of the electron yield that are quenched to a single emission peak with subfemtosecond duration due to these high nonlinearities. The modulation of the emission yield by the carrier-envelope phase suggests that electron emission predominantly occurs during a single half cycle of the driving laser field. When applying a bias voltage to the tip, recollisions in the electron trajectories are suppressed and coherent subcycle electron beams are generated with promising prospects for ultrafast electron microscopy with subcycle time resolution.

π-electron injection activated dormant ligands in graphitic carbon nitride for efficient and stable uranium extraction.

Graphitic carbon nitride (CN) as an adsorbent exhibit promising potential for the removal of uranium in water. However, the lack of active sites seriously restricts its practical application. In contrast to the traditional method of introducing new ligands, we propose a strategy to activate original ligands on CN by injecting π electrons, which can be realized by grafting 4-phenoxyphenol (PP) on CN (PCN). Compared with CN, the maximum adsorption capacity of PCN for uranium increased from 150.9 mg/g to 380.6 mg/g. Furthermore, PCN maintains good adsorption properties over a wide range of uranium concentrations (1 ∼ 60 mg/L) and pH (4 ∼ 8). After 5 consecutive cycles, PCN exhibited sustained uranium removal performance with a little of losses. The experimental and theoretical results show that the enhancement of adsorption performance is mainly due to the ligands activation of CN by delocalization of π electrons from PP. Furthermore, this activation can be enhanced by irradiation, as the CN can be photoexcited to provide additional photoelectrons for PP. As a result, dormant ligands such as N-CN, C-O-C, C-N-H and N-(C)3 can be activated to participate in coordination with uranium. This work provides theoretical guidance for the design and preparation of high efficiency uranium adsorbent.

Achieving Efficient Oxygen Evolution on High-Entropy Sulfide Utilizing Low Electronegativity of Al.

Efficient and stable catalysts are in high demand for accelerating the oxygen evolution reaction (OER). Herein, a high-entropy sulfide (HES) of (FeCoNiCrCuAl)S@HCS with a 3D structure is successfully prepared by utilizing a simple one-step solvothermal method and employed as catalyst toward OER. The lower electronegativity of Al compared to the other metal elements and its anti-corrosion character enable an outstanding OER performance of (FeCoNiCrCuAl)S@HCS with an overpotential of 253 mV at 10 mA cm-2 and an excellent durability after 20 000 CV cycles, outperforming the commercial RuO2 and most reported metal-sulfide catalysts. Experiments coupled with theoretical calculations reveal that Al atom primarily serves as electron donor and promotes a redistribution of local electrons from Co and Cr toward adjacent Fe, Ni, and Cu sites. As a result, the Cr-Al site possesses a lowest energy barrier during the rate-determining step and works as the dominant active site for OER process. This study provides a novel insight and strategy into structural design and performance enhancement for HES materials.

Lead-212/Bismuth-212 In Vivo Generator Based on Ultrasmall Silver Telluride Nanoparticles.

Radionuclide therapy employing alpha emitters holds great potential for personalized cancer treatment. However, certain challenges remain when designing alpha radiopharmaceuticals, including the lack of stability of used radioconjugates due to nuclear decay events. In this work, ultrasmall silver telluride nanoparticles with a core diameter of 2.1 nm were prepared and radiolabeled with lead-212 using a chelator-free method with a radiolabeling efficiency of 75%. The results from the in vitro radiochemical stability assay indicated a very high retention of bismuth-212 despite the internal conversion effects originating from the decay of 212Pb. To further evaluate the potential of the nanoparticles, they were radiolabeled with indium-111, and their cell uptake and subcellular distribution were determined in 2D U87 cells, showing accumulation in the nucleus. Although not intentional, it was observed that the indium-111-radiolabeled nanoparticles induced efficient tumor cell killing, which was attributed to the Auger electrons emitted by indium-111. Combining the results obtained in this work with other favorable properties such as fast renal clearance and the possibility to attach targeting vectors on the surface of the nanoparticles, all well-known from the literature, these ultra-small silver telluride nanoparticles provide exciting opportunities for the design of theragnostic radiopharmaceuticals.

Hot Electrons in a Steady State: Interband vs Intraband Excitation of Plasmonic Gold.

Understanding the dynamics of "hot", highly energetic electrons resulting from nonradiative plasmon decay is crucial for optimizing applications in photocatalysis and energy conversion. This study presents an analysis of electron kinetics within plasmonic metals, focusing on the steady-state behavior during continuous-wave (CW) illumination. Using an inelastic spectroscopy technique, we quantify the temperature and lifetimes of distinct carrier populations during excitation. A significant finding is the monotonic increase in hot electron lifetime with decreases in electronic temperature. We also observe a 1.22× increase in hot electron temperature during intraband excitation compared to interband excitation and a corresponding 2.34× increase in carrier lifetime. The shorter lifetimes during interband excitation are hypothesized to result from direct recombination of nonthermal holes and hot electrons, highlighting steady-state kinetics. Our results help bridge the knowledge gap between ultrafast and steady-state spectroscopies, offering critical insights for optimizing plasmonic applications.

Near-infrared detection based on the excitation of hot electrons in Au/Si microcone array.

Although the photoresponse cut-off wavelength of Si is about 1100 nm due to the Si bandgap energy, the internal photoemission effect (IPE) of the Au/Si junction in Schottky detector can extend the absorption wavelength, which makes it a promising candidate for the Si-based infrared detector. However, due to low light absorption, low photon-electron interaction, and poor electron injection efficiency, the near-infrared light detection efficiency of the Schottky detector is still insufficient. The synergistic effect of Si nano/microstructures with a strong light trapping effect and nanoscale Au films with surface plasmon enhanced absorption may provide an effective solution for improving the detection efficiency. In this paper, a large-area periodic Si microcone array covered by an Au film has successfully been fabricated by one-time dry etching based on the mature polystyrene microspheres lithography technique and vacuum thermal deposition, and its properties for hot electron-based near infrared photodetection are investigated. Optical measurements show that the 20 nm-thick Au covered Si microcone array exhibits a low reflectance and a strong absorption (about 85%) in wide wavelength range (900-2500 nm), and the detection responsivity can reach a value as high as 17.1 and 7.0 mA W-1at 1200 and 1310 nm under the front illumination, and 35.9 mA W-1at 1310 nm under the back illumination respectively. Three-dimensional finite difference time domain (3D-FDTD) simulation results show that the enhanced local electric field in the Au layer distributes near the air/Au interface under the front illumination and close to the Au/Si interface under the back illumination. The back illumination favors the injection of photo-generated hot electrons in Au layer into Si, which can explain the higher responsivity under the back illumination. Our research is expected to promote the practical application of Schottky photodetectors to Si-compatible near infrared photodetectors.

Clinical Trial Protocol for VIOLET: A Single-Center, Phase I/II Trial Evaluation of Radioligand Treatment in Patients with Metastatic Castration-Resistant Prostate Cancer with [161Tb]Tb-PSMA-I&T.

[177Lu]Lu-PSMA is an effective class of therapy for patients with metastatic castration-resistant prostate cancer (mCRPC); however, progression is inevitable. The limited durability of response may be partially explained by the presence of micrometastatic deposits, which are energy-sheltered and receive low absorbed radiation with 177Lu due to the approximately 0.7-mm mean pathlength. 161Tb has abundant emission of Auger and conversion electrons that deposit a higher concentration of radiation over a shorter path, particularly to single tumor cells and micrometastases. 161Tb has shown in vitro and in vivo efficacy superior to that of 177Lu. We aim to demonstrate that [161Tb]Tb-PSMA-I&T will deliver effective radiation to sites of metastatic prostate cancer with an acceptable safety profile. Methods: This single-center, single-arm, phase I/II trial will recruit 30 patients with mCRPC. Key eligibility criteria include a diagnosis of mCRPC with progression after at least one line of taxane chemotherapy (unless medically unsuitable) and androgen receptor pathway inhibitor; prostate-specific membrane antigen-positive disease on [68Ga]Ga-PSMA-11 or [18F]DCFPyL PET/CT (SUVmax ≥ 20); no sites of discordance on [18F]FDG PET/CT; adequate bone marrow, hepatic, and renal function; an Eastern Cooperative Oncology Group performance status of no more than 2, and no prior treatment with another radioisotope. The dose escalation is a 3 + 3 design to establish the safety of 3 prespecified activities of [161Tb]Tb-PSMA-I&T (4.4, 5.5, and 7.4 GBq). The maximum tolerated dose will be defined as the highest activity level at which a dose-limiting toxicity occurs in fewer than 2 of 6 participants. The dose expansion will include 24 participants at the maximum tolerated dose. Up to 6 cycles of [161Tb]Tb-PSMA-I&T will be administered intravenously every 6 wk, with each subsequent activity reduced by 0.4 GBq. The coprimary objectives are to establish the maximum tolerated dose and safety profile (Common Terminology Criteria for Adverse Events version 5.0) of [161Tb]Tb-PSMA-I&T. Secondary objectives include measuring absorbed radiation dose (Gy), evaluating antitumor activity (prostate-specific antigen 50% response rate, radiographic and prostate-specific antigen progression-free survival, overall survival, objective response rate), and evaluating pain (Brief Pain Inventory-Short Form) and health-related quality of life (Functional Assessment of Cancer Therapy-Prostate and Functional Assessment of Cancer Therapy-Radionuclide Therapy). Conclusion: Enrollment was completed in February 2024. Patients are still receiving [161Tb]Tb-PSMA-I&T.

Shot noise-mitigated secondary electron imaging with ion count-aided microscopy.

Modern science is dependent on imaging on the nanoscale, often achieved through processes that detect secondary electrons created by a highly focused incident charged particle beam. Multiple types of measurement noise limit the ultimate trade-off between the image quality and the incident particle dose, which can preclude useful imaging of dose-sensitive samples. Existing methods to improve image quality do not fundamentally mitigate the noise sources. Furthermore, barriers to assigning a physically meaningful scale make the images qualitative. Here, we introduce ion count-aided microscopy (ICAM), which is a quantitative imaging technique that uses statistically principled estimation of the secondary electron yield. With a readily implemented change in data collection, ICAM substantially reduces source shot noise. In helium ion microscopy, we demonstrate 3[Formula: see text] dose reduction and a good match between these empirical results and theoretical performance predictions. ICAM facilitates imaging of fragile samples and may make imaging with heavier particles more attractive.

Quantum mechanics of particles constrained to spiral curves with application to polyene chains.

CONTEXT: Due to advances in synthesizing lower-dimensional materials, there is the challenge of finding the wave equation that effectively describes quantum particles moving on 1D and 2D domains. Jensen and Koppe and Da Costa independently introduced a confining potential formalism showing that the effective constrained dynamics is subjected to a scalar geometry-induced potential; for the confinement to a curve, the potential depends on the curve's curvature function. METHOD: To characterize the π electrons in polyenes, we follow two approaches. First, we utilize a weakened Coulomb potential associated with a spiral curve. The solution to the Schrödinger equation with Dirichlet boundary conditions yields Bessel functions, and the spectrum is obtained analytically. We employ the particle-in-a-box model in the second approach, incorporating effective mass corrections. The π - π ∗ transitions of polyenes were calculated in good experimental agreement with both approaches, although with different wave functions.

Development of silicon-on-insulator direct electron detector with analog memories in pixels for sub-microsecond imaging.

We have developed a high-speed recordable direct electron detector based on silicon-on-insulator technology. The detector has sixteen analog memories in each pixel to record sixteen images with sub-microsecond temporal resolution. A dedicated data acquisition system has also been developed to display and record the results on a personal computer. The performance of the direct electron detector as an image sensor is evaluated under electron irradiation with an energy of 30 keV in a low-voltage transmission electron microscope equipped with a photocathode electron gun. We demonstrate that the detector can record images at an exposure time of 100 ns and an interval of 900 ns.

Low-energy Auger and conversion electron spectroscopy of 99Mo ß--decay.

The preparation of nanometer-thick molybdenum-99 (99Mo) sources using the droplet deposition method was investigated. The quality of these prepared sources was analyzed using scanning electron microscopy (SEM), electron Rutherford backscattering (ERBS) techniques, and Geant4 simulations. The emitted electrons resulting from the ß--decay of the prepared 99Mo sources, with energies below 2.2 keV, were measured and compared with existing literature data as well as the results obtained from our in-house Monte-Carlo model, BrIccEmis.

Hot Carrier Nanowire Transistors at the Ballistic Limit.

We demonstrate experimentally nonequilibrium transport in unipolar quasi-1D hot electron devices reaching the ballistic limit at room temperature. The devices are realized with heterostructure engineering in nanowires to obtain dopant- and dislocation-free 1D-epitaxy and flexible bandgap engineering. We show experimentally the control of hot electron injection with a graded conduction band profile and the subsequent filtering of hot and relaxed electrons with rectangular energy barriers. The number of electrons passing the barrier depends exponentially on the transport length with a mean-free path of 200-260 nm, and the electrons reach the ballistic transport regime for the shortest devices with 70% of the electrons flying freely through the base electrode and the barrier reflections limiting the transport to the collector.

Interlayer Delocalized Electrons Activate Basal Plane for Ultrahigh-Current-Density Hydrogen Evolution.

The basal plane of transition metal dichalcogenides (TMDCs) is inert for the hydrogen evolution reaction (HER) due to its low-efficiency charge transfer kinetics. We propose a strategy of filling the van der Waals (vdW) layer with delocalized electrons to enable vertical penetration of electrons from the collector to the adsorption intermediate vertically. Guided by density functional theory, we achieve this concept by incorporating Cu atoms into the interlayers of tantalum disulfide (TaS2). The delocalized electrons of d-orbitals of the interlayered Cu can constitute the charge transfer pathways in the vertical direction, thus overcoming the hopping migration through vdW gaps. The vertical conductivity of TaS2 increased by 2 orders of magnitude. The TaS2 basal plane HER activity was extracted with an on-chip microcell. Modified by the delocalized electrons, the current density increased by 20 times, reaching an ultrahigh value of 800 mA cm-2 at -0.4 V without iR compensation.

Optimizing Surface State Electrons of Topological Semi-Metal by Atomic Doping for Enhanced Hydrogen Evolution Reaction.

Topological materials carrying topological surface states (TSSs) have extraordinary carrier mobility and robustness, which provide a new platform for searching for efficient hydrogen evolution reaction (HER) electrocatalysts. However, the majority of these TSSs originate from the sp band of topological quantum catalysts rather than the d band. Here, based on the density functional theory calculation, it is reported a topological semimetal Pd3Sn carrying TSSs mainly derived from d orbital and proposed that optimizing surface state electrons of Pd3Sn by introduction heteroatoms (Ni) can promote hybridization between hydrogen atoms and electrons, thereby reducing the Gibbs free energy (ΔGH) of adsorbed hydrogen and improving its HER performance. Moreover, this is well verified by electrocatalytic experiment results, the Ni-doped Pd3Sn (Ni0.1Pd2.9Sn) show much lower overpotential (-29 mV vs RHE) and Tafel slope (17 mV dec-1) than Pd3Sn (-39 mV vs RHE, 25 mV dec-1) at a current density of 10 mA cm-2. Significantly, the Ni0.1Pd2.9Sn nanoparticles exhibit excellent stability for HER. The electrocatalytic activity of Ni0.1Pd2.9Sn nanoparticles is superior to that of commercial Pt. This work provides an accurate guide for manipulating surface state electrons to improve the HER performance of catalysts.

Theoretically designed M@diaza[2.2.2]cryptand complexes: the role of non-covalent interactions in promoting NLO properties of organic electrides.

Organic excess electron compounds with significant nonlinear optical (NLO) properties are widely employed in optoelectronic applications. Herein, single-alkali metals with diaza[2.2.2] cryptand (M@crypt,M=Li, Na, and K) are investigated for optoelectronic and NLO properties by using the density functional theory. Thermodynamic and kinetic stabilities of present complexes are computed through interaction energy (Eint) and ab-initio molecular dynamic (AIMD) simulations. M@crypt complexes carry excess electrons and mimic molecular electrides. Quantum theory of atoms in molecules (QTAIM) analysis and reduced density gradient (RDG) spectra demonstrate the roles of the weak van der Waals (vdW) interactions between metal and complexant. The remarkable hyperpolarizability (ßo) value up to 1.41 × 106 au may be credited to the presence of loosely bound excess electrons. The hyper Rayleigh scattering hyperpolarizability (ßHRS) is recorded up to 1.31 × 106 au for the K@crypt. Furthermore, frequency-dependent first-order and second-order hyperpolarizability is more prominent at the applied frequency of ω = 0.042823 au. The electron localizing function (ELF) and localized orbital locator (LOL) analysis further disclose the nature of interaction between alkali metal and complexant. The TD-DFT method is adopted to get excited state parameters and absorbance properties. An electron density difference map (EDDM) is exploited to evaluate the orbital contributions in excited states. Hence, the studied electride may become a promising candidate for NLO materials. We anticipate that the present work will provide insight into further development of molecular electride for optoelectronic applications.

Organic electrides M@cryptand [2.2.2] (where M=Li, Na, and K) are examined as excess electrons, where vdW forces play important roles in promoting the NLO properties.

Prehydrated Electrons Activated by Continuous Electron Transfer Stemmed from Peracetic Acid Homolysis Mediated by Diamond Surface Defects for Enhanced PFOA Destruction.

Research on the use of peracetic acid (PAA) activated by nonmetal solid catalysts for the removal of dissolved refractory organic compounds has gained attention recently due to its improved efficiency and suitability for advanced water treatment (AWT). Among these catalysts, nanocarbon (NC) stands out as an exceptional example. In the NC-based peroxide AWT studies, the focus on the mechanism involving multimedia coordination on the NC surface (reactive species (RS) path, electron reduction non-RS pathway, and singlet oxygen non-RS path) has been confined to the one-step electron reaction, leaving the mechanisms of multichannel or continuous electron transfer paths unexplored. Moreover, there are very few studies that have identified the nonfree radical pathway initiated by electron transfer within PAA AWT. In this study, the complete decomposition (kobs = 0.1995) and significant defluorination of perfluorooctanoic acid (PFOA, deF% = 72%) through PAA/NC has been confirmed. Through the use of multiple electrochemical monitors and the exploration of current diffusion effects, the process of electron reception and conduction stimulated by PAA activation was examined, leading to the discovery of the dynamic process from the PAA molecule → NC solid surface → target object. The vital role of prehydrated electrons (epre-) before the entry of resolvable electrons into the aqueous phase was also detailed. To the best of our knowledge, this is the first instance of identifying the nonradical mechanism of continuous electron transfer in PAA-based AWT, which deviates from the previously identified mechanisms of singlet oxygen, single-electron, or double-electron single-path transfer. The pathway, along with the strong reducibility of epre- initiated by this pathway, has been proven to be essential in reducing the need for catalysts and chemicals in AWT.

Boosting the Zn2+ storage capacity of MoO3 nanoribbons by modulating the electrons spin states of Mo via Ni doping.

Aqueous zinc-ion batteries (AZIBs) have received considerable potential for their affordability and high reliability. Among potential cathodes, α-MoO3 stands out due to its layered structure aligned with the (010) plane, offering extensive ionic insertion channels for enhanced charge storage. However, its limited electrochemical activity and poor Zn2+ transport kinetics present significant challenges for its deployment in energy storage devices. To overcome these limitations, we introduce a new strategy by doping α-MoO3 with Ni (Ni-MoO3), tuning the electron spin states of Mo. Thus modification can activate the reactivity of Ni-MoO3 towards Zn2+ storage and weaken the interaction between Ni-MoO3 and intercalated Zn2+, thereby accelerating the Zn2+ transport and storage. Consequently, the electrochemical properties of Ni-MoO3 significantly surpass those of pure MoO3, demonstrating a specific capacity of 258 mAh g-1 at 1 A g-1 and outstanding rate performance (120 mAh g-1 at 10 A g-1). After 1000 cycles at 8 A g-1, it retains 76 % of the initial capacity, with an energy density of 154.4 Wh kg-1 and a power density of 11.2 kW kg-1. This work proves that the modulation of electron spin states in cathode materials via metal ion doping can effectively boost their capacity and cycling durability.

Memristive Control of Plasmon-Mediated Nonlinear Photoluminescence in Au Nanowires.

Nonlinear photoluminescence (N-PL) is a broadband photon emission arising from a nonequilibrium heated electron distribution generated at the surface of metallic nanostructures by ultrafast pulsed laser illumination. N-PL is sensitive to surface morphology, local electromagnetic field strength, and electronic band structure, making it relevant to probe optically excited nanoscale plasmonic systems. It also has been key to accessing the complex multiscale time dynamics ruling electron thermalization. Here, we show that plasmon-mediated N-PL emitted by a gold nanowire can be modified by an electrical architecture featuring a nanogap. Upon voltage activation, we observe that N-PL becomes dependent on the electrical transport dynamics and can thus be locally modulated. This finding brings an electrical leverage to externally control the photoluminescence generated from metal nanostructures and constitutes an asset for the development of emerging nanoscale interface devices managing photons and electrons.

Hydrothermally Stimulated Molecular Interfaces for Augmented Electron Delocalization in Wet-Chemical Phosphorus Recovery from Incineration Ash of Sewage Sludge.

Wet-chemically recovering phosphorus (P) from sewage sludge incineration ash (SSIA) has already become a global initiative to address P deficit, but effectively isolating P from these accompanying metals (AMs) through adsorption in a SSIA-derived extract remains elusive. Here, we devised a hydrothermal stimulus-motivated thermodynamic and kinetic enhancement to gain anionic ethylenediaminetetraacetic acid (EDTA) molecular interfaces for AM enclosure to resolve this conundrum. A new dosage rule based on the EDTA coordination ratio with AMs was established for the first time. Upon hydrothermal extraction at 140 °C for 1 h, the P extraction efficiency reached 96.7% or higher for these obtained SSIA samples, and then exceptional P sequestration from these EDTA-chelated AMs was realized by the peculiar lanthanum (La)-based nanoadsorbent (having 188.86 mg P/g adsorbent at pH ∼ 3.0). Relevant theoretical calculations unraveled that these delocalized electrons of tetravalent EDTA molecules boosted the enclosure of liberated AMs, thereby entailing a substantially increased negative adsorption energy (-408.7 kcal/mol) of P in the form of H2PO4- through intruding lattice-edged carbonates to coordinate La with monodentate mononuclear over LaCO5(1 0 1). This work highlights the prospect of molecular adaptation of these common extractants in wet-chemical P recovery from various P-included wastes, further sustaining global P circularity.