Singlet fission and triplet-triplet annihilation (TTA) are spin-dependent phenomena critical to optoelectronics. The dynamics of spin populations during geminate triplet pair separation are crucial for controlling fission and TTA rates. We show that the Dzyaloshinskii-Moriya interaction (DMI) induces level crossings between spin manifolds, affecting spin populations and TTA rates in crystalline fission semiconductors. By investigating spin-dependent fluorescence in a triplet exciton pair with the magnetic field aligned along the fine structure tensor, we isolate the effect of DMI, as the triplet wavefunctions remain unaffected by the field. Our results reveal that DMI introduces additional TTA pathways that are forbidden by spin conservation, explaining the observed evolution of optically detected magnetic resonance signals with varying magnetic field. This study highlights the significant impact of DMI on the optical properties of triplet excitons, advancing our understanding of spin dynamics in these systems.

Extended energy levels and transition data for Au LXVI are computed using the GRASPG program package, which is founded on the multiconfiguration Dirac-Hartree-Fock and relativistic configuration interaction methods. This work provides complete, consistent datasets encompassing energy levels, transition rates, and lifetimes for electric-dipole (E1), electric-quadrupole (E2), magnetic-dipole (M1), and magnetic-quadrupole (M2) transitions across all these levels. The uncertainty estimation methods are employed to assess the accuracy of the transition data, and the computed results are further compared with other theoretical calculations. The present results are reported as benchmarks to support future computational and experimental measurements.

Metal-covalent organic frameworks (MCOFs) present bright prospect in photocatalytic application. However, their performance constrained by the kinetic mismatch between rapid charge recombination and slow proton transfer. This work achieves precise control over the proton-coupled electron transfer (PCET) process by rationally regulating from molecular scale for two MCOFs, TAPB-MCOF and TAPP-MCOF. Owing to the uniform electron cloud of benzene unit in TAPB-MCOF instead of electron distribution breaking of pyridine in TAPP-MCOF, a motivated charge migration of TAPB-MCOF is revealed by lower electrochemical impedance and higher transient photocurrent; still, the broader interlayer space of TAPB-MCOF ensures a smooth proton delivery. The synergistical advantages establish an "electron-dominated, proton-assisted" reaction dynamics, leading to an apparently improved performance in both photocatalytic carbon dioxide reduction reaction (CO2RR) and hydrogen peroxide (H2O2) photosynthesis of TAPB-MCOF. The carbon monoxide (CO) and H2O2 generation rates are 100.9 and 314.69 μmol·g-1·h-1, respectively. This charge-proton cooperative mechanism expands a new landscape for exploring effectively photocatalytic systems.

The multi-configuration Dirac-Hartree-Fock method (MCDHF) and the corresponding large-scale calculation program GRASP2K were used to systematically study the 2p-1s radiative transition processes of the inner-shell excited states of Z = 12-54 C-like ions. The electric dipole E1 radiation transition and the magnetic quadrupole M2 forbidden transition process are included. The X-ray spectra of some C-like ions are given. Electron correlation effect is fully considered. The high-order relativistic effects, such as Breit Interaction (BI) correction, quantum electro dynamics (QED) correction and finite nuclear mass correction etc. are also considered. The calculated results are in good agreement with other theoretical and experimental results.

Energy levels, lifetimes, line strengths, oscillator strengths, and transition probabilities for the 1s2s2nl, 1s2s2pnl, and 1s2p2nl (n <= 3, l = s,p,d) configurations of the Be-like Sc17+ ion were calculated using the multiconfiguration Dirac-Hartree-Fock (MCDHF) method, with the contributions of the Breit interaction and quantum electrodynamics (QED) corrections included. Atomic parameters for 250 K-shell excited fine-structure levels and 2441 corresponding electric dipole (E1) transitions are presented. The computed Ka X-ray wavelengths are in good agreement with previous experimental and theoretical results, with most differences below 0.095%. The uncertainty of the calculated transition data was carefully estimated based on relative deviations from transition probabilities from different gauges. Furthermore, the accuracy of each E1 transition was individually assessed. These high-precision results are crucial for identifying and analysing X-ray spectral lines in astrophysical sources and in high-temperature laboratory plasmas, thereby enabling more accurate plasma diagnostics and modelling.

High-harmonic generation (HHG) from an idealized theoretical model of the molecular nanoring is numerically investigated by using an intense mid-infrared laser pulse. The resultant nonperturbative HHG exhibits some distinctly different radiation characteristics compared to the traditional gas HHG. Specifically, the harmonic cutoff for a molecular nanoring extends slightly beyond the cutoff law of the gas HHG due to its large spatial scale. The observed extension of the harmonic cutoff in the molecular nanoring can be well explained by a generalized semiclassical three-step model. In the simulation, we also find that the ellipticity dependence of the harmonic intensity for the molecular nanoring is distinguishably weaker than that for the atomic target. The harmonic ellipticities from the molecular nanoring can be continuously controlled by the elliptically polarized laser field within a certain ellipticity range, which offers a promising route to produce ellipticity-tunable harmonic emissions. Our results obtained from the numerical idealized model of the molecular nanoring suggest a potential pathway for achieving atomic-like HHG by a laser pulse only with the intensity on the order of 1012 W/cm2, just like the case of the solid HHG. Compared with the gas HHG triggered generally by the laser pulse with the intensity order of 1014 W/cm2, the novel scheme has the advantages of better accessibility and practicability.

We theoretically demonstrate the effects of interferences and asymmetries between K and K' valleys for pristine graphene in high-order harmonic generation (HHG) by a single-color laser pulse. It is shown that the allowed orders of the observed overall HHG spectra are attributed to the consequences of quantum interferences between K and K' valleys. The cancellations of forbidden harmonics are caused by the destructive interferences between two different valleys due to the dynamical symmetries of the laser-solid systems. Apparent valley-contrasting and helicity-resolved harmonic signals can be observed for the 3k-order (k E N) harmonics when the polarization state of the driving laser field slightly deviates from the ideal circular polarization. The valley discriminations for these emerging 3k-order (k E N) harmonics originate from the unequal responses of the HHG from two different valleys within the perturbation regime. In addition, the valley asymmetries of the electronic excitations are also observed by using an elliptically polarized laser pulse. Our work clearly illustrates the essential intervalley interplay in the HHG process for pristine graphene, facilitating the understanding of ultrafast electron dynamics in zero-band-gap materials.

To alleviate urea wastewater pollution and achieve sustainable hydrogen production, development of highly active, low-cost, and stable bifunctional catalysts is urgently required. Using a deposition method, NixMny/NF (x = 1, y = 1) alloy materials were successfully synthesized, which can effectively generate hydrogen across the full pH range. The overpotentials (g100) of Ni1Mn1/NF in alkaline, acidic, and neutral solutions were 197, 261, and 338 mV, respectively. During the urea oxidation reaction (UOR), HRTEM, XPS, and in-situ Raman results confirmed that the NiMn alloy undergoes reconstruction into a highly active composite structure NiMn/NiMnOOH, achieving an g100 of just 1.384 V. Density functional theory (DFT) indicates that Mn incorporation optimizes intermediate adsorption (Urea*)/desorption (CO2*), accelerating the deprotonation rate of the CONHN* intermediate (rate-determining step, RDS), thus enhancing catalytic activity. Notably, in the dual-electrode electrolyzer composed of Ni1Mn1/NF, the cell voltage in the overall human urine electrolysis system (HOUS) is 1.724 V@100 mA cm- 2, which is approximately 333 mV lower than that in the overall water electrolysis system (OWS). Compared to recent studies, Ni1Mn1/NF demonstrates better catalytic activity and stability. This work presents a fresh perspective on catalyst design for mitigating urine pollution and enabling efficient hydrogen production.

The fluorescence of triplet excitons and color-centers is strongly dependent on magnetic field that mixes the zero field spin eigenstates that determine the radiative recombination rates back into the singlet ground state through spin-orbit coupling. For films of molecules, and polycristaline color-centers samples an average over molecular orientations has to be performed to model the magneto-fluorescence lineshapes. This limits our analytical understanding of the lineshapes and complicates the analysis of the fluorescence dependence on magnetic field. Here, we present a framework that allows to average over triplet molecular orientations analytically. Our approach achieves provides very accurate numerical routines computing precisely the averages matrix elements that appear in magneto-fluorescence and semi-analytical approximations that can be used to model experimental traces.

Self-assembled monolayer (SAM)-based inverted perovskite solar cells (PSCs) have exhibited excellent performance in efficiency, while the stability and reproducibility of the PSCs still need to be improved. In this work, we present a multifunctional hole transport approach for inverted PSCs, where NiOX, SAM ((E)-3-(4-(bis(4-methoxyphenyl)amino)phenyl)acrylic acid, abbreviated as MPTCA) and a wetting agent (2-phenylethylamine hydroiodide, known as PEAI) are employed for hole-transport materials (HTMs). This NiOX/MPTCA/PEAI composite layer is uniform and has good wetting properties, which enables the formation of a high-quality perovskite film, effectively minimizing defects that typically occur at the buried interface. An outstanding champion efficiency of 24.74% was obtained for the devices, followed by enhanced reproducibility with an average power conversion efficiency (PCE) of 24.13 ± 0.26%, which is notably higher than that (22.73 ± 0.62%) of the pristine MPTCA-based PSCs. More importantly, the composited HTL-based devices without encapsulation demonstrated remarkable stability, with a decrease of less than 10% in the initial efficiency after 500 h of continuous light soaking.

In highly efficiently inverted perovskite solar cells (PSCs), fullerene derivative [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) is commonly utilized as an electron transport layer (ETL). However, its inadequate passivation, poor surface coverage, and energy level mismatch limit the improvement of power conversion efficiency (PCE) and stability of PSCs. In this work, a multifunctional interface manipulation strategy is developed by introducing dimethyl 2,2 '-bipyridine-4,4 '-dicarboxylate (DMCBPy) into the interface between perovskite and PCBM layers to improve the photovoltaic performance of the PSCs. The 2,2 '-bipyridine in DMCBPy can strongly anchor the uncoordinated Pb2+ ion on the perovskite surface via coordination interactions, while the methyl ester groups in DMCBPy can adjust the surface polarity of perovskite and improve the coverage of PCBM. Moreover, the incorporation of DMCBPy can regulate the interface energy level alignment to reduce nonradiative recombination. The resulting devices have achieved the highest PCE of 25.04 % and retain about 90 % of the initial values after aging at 85 degrees C for 1000 h in N2 atmosphere.

Based on the multiconfiguration Dirac-Hartree-Fock (MCDHF) method, accurate atomic spectra data including the transition rates, line strengths, and oscillator strengths for the inner-shell excited configuration 2s2p2(4P)3p in N II ion are reported by taking into account the core-core, core-valence and valence correlation effects as well as the Breit interaction. Good accordance can be found in the comparison with other calculations and measurements. Meanwhile, by studying the effects of electron correlations on the energy levels and transition rates of 2s2p2(4P)3p configuration, it is found that the valence correlations of active space nl = {n = 2-7, l = s-i} and the core correlations with regard to 1s2 electrons have the strongly adjusted effect and the balancing influence, respectively. Furthermore, the quintet transitions 2s2p2(4P)3s 5P-2s2p2(4P)3p 5L degrees (L = P, D) are found to strictly obey the selection rule dS = 0. The branching fractions under this case tend to 1, which is a peculiarly intrinsic property that is recommended to diagnose the lifetimes or rates of quintet states.

Expanding the moiré material library continues to unlock novel quantum phases and emergent electronic behaviors. In this work, we introduce PbI2 into the moiré family and investigate the magnetotransport properties of moiré superlattice in a hexagonal boron nitride/graphene/PbI2 heterostructures. In high-field quantum Hall regime, we observe a robust dissipationless transport at charge neutrality point, indicative of incompressible states stabilized at the filling factor vh = 0. Additionally, a fractional conductance plateau at 2/3 e2/h emerges, which we attribute to a Chern junction between domains with distinct Chern numbers originating from moiré-modulated and conventional integer quantum Hall states. The moiré Hofstadter spectrum displays an unconventional flavor sequence, likely influenced by proximity-induced spin-orbit coupling from the PbI2 layer. We also see coherent electronic interference along lines with Chern number vm = -2. These findings position PbI2-based heterostructures as a versatile platform for realizing spin-orbit-enhanced moiré phenomena and engineering coherent edge transport in two-dimensional quantum materials.

Identifying multi-exciton states generated from singlet fission is key to understanding the carrier multiplication process, which presents a strategy for improving the efficiency of photovoltaics and bio-imaging. Broadband optically detected magnetic resonance is a sensitive technique to detect multi-exciton states. Here we report a dominant species emerging under intense light excitation corresponding to a weakly exchange coupled triplet pair located on adjacent molecules oriented by nearly 90 degrees, contrasting to the pi-stacked triplet pair under low excitation intensity. The weakly coupled species model precisely reproduces the intricate spin transitions in the Hilbert space of the triplet pair. Combining the magneto photoluminescence and high-magnetic field ODMR, we also identify a strongly exchange-coupled state of three triplet excitons formed by photoexcited V2, which manifests through the magnetic field induced level crossings between its quintet and triplet manifolds. The excellent agreement between the experimental Zeeman fan and the two-triplet spin Hamiltonian highlights the potential of multi-exciton states for quantum information processing.

Abstract Understanding the quantum transport properties of (Two‐dimensional) 2D perovskite heterostructures is key to interpreting their electronic performance and promoting optoelectronic devices. Here, it is shown that clear Shubnikov‐de Hass oscillation appears in the heterostructure of monocrystalline 2D perovskites and graphene, thanks to the clean interface. An efficient charge transfer between perovskite nanosheets and graphene is found, facilitating the separation of electrons and holes at the interface. The relation between the charge transfer efficiency and microscopic interface structures is quantitatively described. The evidence of photo‐assisted transport from the photo‐response of magnetoresistance is revealed, which happens between Landau levels of two graphene layers mediated by hot carriers in the perovskite layer, overcoming the barrier from the organic layers in the Ruddlesden‐Popper perovskite phase. These results provide a picture to understand the transport behavior of 2D perovskite/graphene heterostructure and a reference for the controlled design of interfaces in perovskite optoelectronic devices.

Extended energy levels and transition data for the Yb LVII are calculated with the GRASP2018 package, which is based on the multiconfiguration Dirac-Hartree-Fock and relativistic configuration methods. Complete and consistent data sets of energy levels, transition rates and lifetimes for electric-dipole (E1), electric-quadrupole (E2), magnetic-dipole (M1), and magnetic-quadrupole (M2) transitions among all these levels are given in this calculation. Three methods of uncertainty estimators are used to evaluate the accuracy of transition data. The computed results are also compared with other theoretical computations. The present results are reported as benchmarks for future calculations and measurements.

Nickel-doped iridium echinus-like nanosheets (NiIr-ENS) have a superior acidic oxygen evolution reaction (OER) activity with a TOF of 1.72 s(-1) at an overpotential of 300 mV, 8.6-fold higher than that of IrO2.

Excitation energies belonging to the (1s2)2s22p2, 2s22p3p, 2s2p3, 2s22p3s, and 2s22p3d configurations of carbon-like Na VI and Al VIII have been calculated with the multi-configuration Rayleigh–Ritz variation method and restricted variation method, as well as wavelengths, line strengths, oscillator strengths, transition rates for electric dipole transitions among these terms. High-accuracy calculations have been performed using a moderate scale of Slater basis function and accurate treatments of relativity, electron correlation, and quantum electrodynamic (QED) effects. The line strengths, transition oscillator strengths, and transition probabilities for the electric dipole transitions are determined. Deviations of line strengths between the length and velocity gauges are discussed, as well as with the experimentally compiled values from the National Institute for Standards and Technology (NIST) and other theoretical data wherever available. Furthermore, the accuracy of each electric dipole transition is assessed. The present results are accurate enough for identification of emission lines involving these terms and are also useful for precise spectral modeling and diagnosing in astrophysical and laboratory plasmas.

Poly(3,4-ethylenedioxythiophene) (PEDOT) aggregate-deposited counter electrodes (CEs) were applied to bifacial dye-sensitized solar cells with a cobalt complex electrolyte. The high transparency and excellent electrochemical activity of PEDOT CEs result in an impressive cell bifaciality of 0.92 under standard test conditions (AM 1.5G, 100 mW cm-2), and maximum power production of 11.3% under realistic conditions with an effective albedo of 50%.

All-solid-state batteries are one of the most important game changers in electrochemical energy storage since they are free from the risk of leakage of hazardous flammable liquid solvents. Among the various types of solid-state electrolytes, Li7-xLa3Zr2-xTaxO12 garnets possess many desirable advantages to be considered a suitable candidate for lithium-ion batteries. However, their practical application has been hindered by premature short-circuits due to lithium dendrite growth, nonnegligible electronic conductivity and interfacial air sensitivity issues. Herein, we propose a multifunctional layer strategy to simultaneously address both the interface and electronic conductivity issues. With the help of a facile chemical process based on reactive cobalt boride, electron leakage was effectively blocked and the electrochemical performance/stability could be well maintained over extended cycles. The cobalt boride-coating layer also possessed an impressive Li metal wetting ability while sustaining a low interfacial resistance. A full cell paired with a commercialized cathode showed satisfactory performance with low overpotentials and a high specific capacity over 150 mA h g-1. Moreover, first-principle calculations further revealed the status of the rearrangement of the electron cloud behind the charge-density difference, and the nature of the low diffusion energy barrier of the reactive cobalt boride protective layer. Our strategy highlights the necessity of designing proper multifunctional layers in the garnet-type solid-state lithium-ion battery system.