Enhancing multifunctional photocatalysis with acetate-assisted cesium doping and unlocking the potential of Z-scheme solar water splitting

Graphitic carbon nitride(g-C_(3)N_(4))has been extensively doped with alkali metals to enlarge photocatalytic output,in which cesium(Cs)doping is predicted to be the most efficient.Nevertheless,the sluggish diffusion and doping kinetics of precursors with high melting points,along with imprecise regulation,have raised the debate on whether Cs doping could make sense.For this matter,we attempt to confirm the positive effects of Cs doping on multifunctional photocatalysis by first using cesium acetate with the character of easy manipulation.The optimized Csdoped g-C_(3)N_(4)(CCN)shows a 41.6-fold increase in visible-light-driven hydrogen evolution reaction(HER)compared to pure g-C_(3)N_(4) and impressive degradation capability,especially with 77%refractory tetracycline and almost 100%rhodamine B degradedwithin an hour.The penetration ofCs+is demonstrated to be a mode of interlayer doping,and Cs–N bonds(especially with sp^(2) pyridine N in C═N–C),along with robust chemical interaction and electron exchange,are fabricated.This atomic configuration triggers the broadened spectral response,the improved charge migration,and the activated photocatalytic capacity.Furthermore,we evaluate the CCN/cadmium sulfide hybrid as a Z-scheme configuration,promoting the visible HER yield to 9.02 mmol g^(−1) h^(−1),which is the highest ever reported among all CCN systems.This work adds to the rapidly expanding field of manipulation strategies and supports further development of mediating served for photocatalysis.

Investigation of helicity-dependent photocurrent of surface states in(Bi_(0.7)Sb_(0.3))_(2)Te_(3)nanoplate

Helicity-dependent photocurrent(HDPC)of the surface states in a high-quality topological insulator(Bi_(0.7)Sb_(0.3))_(2)Te_(3)nanoplate grown by chemical vapor deposition(CVD)is investigated.By investigating the angle-dependent HDPC,it is found that the HDPC is mainly contributed by the circular photogalvanic effect(CPGE)current when the incident plane is perpendicular to the connection of the two contacts,whereas the circular photon drag effect(CPDE)dominates the HDPC when the incident plane is parallel to the connection of the two contacts.In addition,the CPGE of the(Bi_(0.7)Sb_(0.3))_(2)Te_(3)nanoplate is regulated by temperature,light power,excitation wavelength,the source–drain and ionic liquid top-gate voltages,and the regulation mechanisms are discussed.It is demonstrated that(Bi_(0.7)Sb_(0.3))_(2)Te_(3)nanoplates may provide a good platform for novel opto-spintronics devices.

Investigation of reflection anisotropy induced by micropipe defects on the surface of a 4H-SiC single crystal using scanning anisotropy microscopy

Optical reflection anisotropy microscopy mappings of micropipe defects on the surface of a 4H-SiC single crystal are studied by the scanning anisotropy microscopy(SAM)system.The reflection anisotropy(RA)image with a'butterfly pattern'is obtained around the micropipes by SAM.The RA image of the edge dislocations is theoretically simulated based on dislocation theory and the photoelastic principle.By comparing with the Raman spectrum,it is verified that the micropipes consist of edge dislocations.The different patterns of the RA images are due to the different orientations of the Burgers vectors.Besides,the strain distribution of the micropipes is also deduced.One can identify the dislocation type,the direction of the Burgers vector and the optical anisotropy from the RA image by using SAM.Therefore,SAM is an ideal tool to measure the optical anisotropy induced by the strain field around a defect.

Effect of drying methods on perovskite films and solar cells

The high efficiency,solution processibility,and flexibility of perovskite solar cells make them promising candidates for the photovoltaic industry[1−8].The deposition method is one of the most critical factors that affect the performance of perovskite films.Various deposition methods have been developed to make perovskite films,including spin-coating,slotdie coating.

Tuning Properties of External Cavity Violet Semiconductor Laser

A tunable grating-coupled external cavity(EC)laser is realized by employing a GaN-based laser diode as the gain device.A tuning range of 4.47 nm from 403.82 to 408.29 nm is achieved.Detailed investigations reveal that the injection current strongly influences the performance of the EC laser.Below the free-running lasing threshold,EC laser works stably.While above the free-running lasing threshold,a Fabry–Pérot(F-P)resonance peak in the emission spectrum and a smooth kink in the output power-injection current characteristic curve are observed,suggesting the competition between the inner F-P cavity resonance and EC resonance.Furthermore,the tuning range is found to be asymmetric and occurs predominantly on the longer wavelength side.This is interpreted in terms of the asymmetric gain distribution of GaN-based quantum well material.

Recent progress and future prospect of novel multi-ion storage devices

Rechargeable batteries,especially lithium-ion batteries(LIBs),have made rapid development since the 21st century,greatly facilitating people's lives[1−6].Based on considerations of cost and existing problems(such as safety issues due to LIBs stacking strategy and unsatisfactory performance for various applications),researchers have explored alternative technologies to LIBs to meet the needs for wide application scenarios[5].Among them,multi-ion storage devices such as dual-ion batteries(DIBs)and metal-ion hybrid capacitors(MIHCs)are considered promising alternative energy storage devices of LIBs due to their unique multi-ion storage mechanism.In a multi-ion storage device,cations and anions carry charges back and forth between the electrolyte and the electrodes at the same time,unlike the rocking chair mechanism of LIBs[7].Generally,the anodes of DIBs and MIHCs work in a similar mechanism to LIBs,storing charge through redox reactions.The main difference among them is the mechanism of the cathodes during charging and discharging[8].In DIBs,the battery-type cathode stores anions through the Faraday reaction.

An in-depth understanding of photophysics in organic photocatalysts

The urgent need to replace conventional fossil fuels with clean energy has stimulated a large number of research efforts on photocatalytic hydrogen evolution[1−4].Alternatively,organic semiconductors with tunable light absorption,well-positioned band edges,and excellent charge separation are highly expected[5−8].Conventionally,a semiconductor material with a wide band gap has a larger exciton binding energy,while a semiconductor material with a narrow band gap has a smaller exciton binding energy[9].Since smaller exciton binding energies are favorable for exciton separation,choosing a semiconductor with a suitable bandgap seems to be the first step toward high solar-to-hydrogen efficiency.The tunable light-harvesting ability determines the advantage and potential of organic semiconductors as photocatalysts.However,the insufficient external quantum efficiency(EQE)and the un-derlying photophysical mechanism remain restricting the orientation toward industrialization[10].

Electronic and thermal properties of Ag-doped single crystal zinc oxide via laser-induced technique

The doping of ZnO has attracted lots of attention because it is an important way to tune the properties of ZnO.Postdoping after growth is one of the efficient strategies.Here,we report a unique approach to successfully dope the single crystalline ZnO with Ag by the laser-induced method,which can effectively further post-treat grown samples.Magnetron sputtering was used to coat the Ag film with a thickness of about 50 nm on the single crystalline ZnO.Neodymium-doped yttrium aluminum garnet(Nd:YAG)laser was chosen to irradiate the Ag-capped ZnO samples,followed by annealing at700℃for two hours to form ZnO:Ag.The three-dimensional(3D)information of the elemental distribution of Ag in ZnO was obtained through time-of-flight secondary ion mass spectrometry(TOF-SIMS).TOF-SIMS and core-level x-ray photoelectron spectroscopy(XPS)demonstrated that the Ag impurities could be effectively doped into single crystalline ZnO samples as deep as several hundred nanometers.Obvious broadening of core level XPS profiles of Ag from the surface to depths of hundred nms was observed,indicating the variance of chemical state changes in laser-induced Ag-doped ZnO.Interesting features of electronic mixing states were detected in the valence band XPS of ZnO:Ag,suggesting the strong coupling or interaction of Ag and ZnO in the sample rather than their simple mixture.The Ag-doped ZnO also showed a narrower bandgap and a decrease in thermal diffusion coefficient compared to the pure ZnO,which would be beneficial to thermoelectric performance.

4‑Terminal Inorganic Perovskite/Organic Tandem Solar Cells Offer 22%Efficiency

After fast developing of single-junction perovskite solar cells and organic solar cells in the past 10 years,it is becoming harder and harder to improve their power conversion efficiencies.Tandem solar cells are receiving more and more attention because they have much higher theoretical efficiency than single-junction solar cells.Good device performance has been achieved for perovskite/silicon and perovskite/perovskite tandem solar cells,including 2-terminal and 4-terminal structures.However,very few studies have been done about 4-terminal inorganic perovskite/organic tandem solar cells.In this work,semi-transparent inorganic perovskite solar cells and organic solar cells are used to fabricate 4-terminal inorganic perovskite/organic tandem solar cells,achieving a power conversion efficiency of 21.25%for the tandem cells with spin-coated perovskite layer.By using drop-coating instead of spin-coating to make the inorganic perovskite films,4-terminal tandem cells with an efficiency of 22.34%are made.The efficiency is higher than the reported 2-terminal and 4-terminal inorganic perovskite/organic tandem solar cells.In addition,equivalent 2-terminal tandem solar cells were fabricated by connecting the sub-cells in series.The stability of organic solar cells under continuous illumination is improved by using semi-transparent perovskite solar cells as filter.

Advances in the Application of Perovskite Materials

Nowadays, the soar of photovoltaic performance of perovskite solar cells has set off a fever in the study of metal halide perovskite materials. The excellent optoelectronic properties and defect tolerance feature allow metal halide perovskite to be employed in a wide variety of applications. This article provides a holistic review over the current progress and future prospects of metal halide perovskite materials in representative promising applications, including traditional optoelectronic devices(solar cells, light-emitting diodes, photodetectors, lasers), and cutting-edge technologies in terms of neuromorphic devices(artificial synapses and memristors) and pressure-induced emission. This review highlights the fundamentals, the current progress and the remaining challenges for each application, aiming to provide a comprehensive overview of the development status and a navigation of future research for metal halide perovskite materials and devices.

Calibration of quantitative rescattering model for simulating vortex high-order harmonic generation driven by Laguerre–Gaussian beam with nonzero orbital angular momentum

We calibrate the macroscopic vortex high-order harmonic generation(HHG)obtained by the quantitative rescattering(QRS)model to compute single-atom induced dipoles against that by solving the time-dependent Schr?dinger equation(TDSE).We show that the QRS perfectly agrees with the TDSE under the favorable phase-matching condition,and the QRS can accurately predict the main features in the spatial profiles of vortex HHG if the phase-matching condition is not good.We uncover that harmonic emissions from short and long trajectories are adjusted by the phase-matching condition through the time-frequency analysis and the QRS can simulate the vortex HHG accurately only when the interference between two trajectories is absent.This work confirms that it is an efficient way to employ the QRS model in the single-atom response for precisely simulating the macroscopic vortex HHG.

Effect of laser focus in two-color synthesized waveform on generation of soft x-ray high harmonics

Synthesis of multi-color laser pulses has been developed as a promising way to improve low conversion efficiency of high-order harmonic generation(HHG). Here we systematically study the effect of laser focus in a two-color waveform on generation of macroscopic HHG in soft x-rays. We find that the dependence of HHG yields on laser focus at low or high gas pressure is sensitive to the characteristics of single-atom harmonic response, in which “short”-or “long”-trajectory emissions can be selectively controlled by changing the waveform of two-color synthesized laser pulse. We uncover the phase-matching mechanism of HHG in the gas medium by examining the propagation of the two-color waveform and the evolution of time-frequency emissions of high-harmonic field. We further reveal that the nonlinear effects, such as geometric phase, atomic dispersion, and plasma defocusing, are responsible for modification of two-color waveform upon propagation. This work can be used to find better macroscopic conditions for generating soft x-ray HHG by employing two-color optimized waveforms.

Enhancing the activity of FeNi bimetallic electrocatalysts on overall water splitting by Nd_(2)O_(3)-induced FeNi lattice contraction

The development of high-efficiency and cost-effective bifunctional electrocatalysts for overall water splitting remains a formidable challenge.Herein,FeNi-Nd_(2)O_(3) nanoparticles anchored on N-doped carbon nanotubes(FeNi-Nd_(2)O_(3)/NCN) are designed for highly effective overall water splitting via a facile two-step hydrothermal approach.The synthetic FeNi-Nd_(2)O_(3) hetero-trimers(Fe 2p-Ni 2p-Nd 3d orbital coupling)on NCN achieve excellent oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) activities with overpotentials of 270 and 120 mV at 10 mA cm^(-2) in 1 M KOH solution.Moreover,a small voltage of 1.52 V at 10 mA cm^(-2) is achieved when FeNi-Nd_(2)O_(3)/NCN is assessed as bifunctional catalyst for overall water splitting,which is superior to the typically integrated Pt/C and RuO_(2) counterparts(1.54 V at 10 mA cm^(-2)).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy show that the remarkably improved activity is originated from Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction.Furthermore,density functional theory(DFT) calculations indicate that the lattice contraction reduces binding energies of intermediates by downshifting the position of FeNi bimetallic d-band center relative to the Fermi level to optimize catalytic performance.Therefore,the Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction may provide a new perspective for designing and synthesizing innovative catalytic systems.

Investigation of Ga_(2)O_(3)/diamond heterostructure solar-blind avalanche photodiode via TCAD simulation

A Ga_(2)O_(3)/diamond separate absorption and multiplication avalanche photodiode(SAM-APD)with mesa structure has been proposed and simulated.The simulation is based on an optimized Ga_(2)O_(3)/diamond heterostructure TCAD physical model,which is revised by repeated comparison with the experimental data from the literature.Since both Ga_(2)O_(3)and diamond are ultra-wide bandgap semiconductor materials,the Ga_(2)O_(3)/diamond SAM-APD shows good solar-blind detection ability,and the corresponding cutoff wavelength is about 263 nm.The doping distribution and the electric field distribution of the SAM-APD are discussed,and the simulation results show that the gain of the designed device can reach 5×10^(4)and the peak responsivity can reach a value as high as 78 A/W.

Influence of Frohlich Interaction on Intersubband Transitions of InGaAs/InAlAs-Based Quantum Cascade Detector Structures Investigated by Infrared Modulated Photoluminescence

We demonstrate the use of an infrared modulated photoluminescence(PL)method based on a step-scan Fourier-transform infrared spectrometer to analyze intersubband transition(ISBT)of InGaAs/InAlAs quantum cascade detector(QCD)structures.By configuring oblique and parallel excitation geometries,high signal-to-noise ratio PL spectra in near-to-far-infrared region are measured.With support from numerical calculations based on the k·p perturbation theory,the spectra is attributed to intraband and interband transitions of InGaAs/InAlAs QCD structures.Temperature evolution results show that the k-dependent transitions caused by longitudinal optical phonon-assisted scattering(Frohlich interaction)plays an important role in the ISBT.These results suggest that this infrared modulated-PL method has great potential in characterizing QCD devices and conducting performance diagnostics.

Structural Characterization of Carbon-implanted GaSb

Ion implantation induced damage in GaSb and its removal by rapid thermal annealing(RTA)have been investigated by Raman spectroscopy.The evolution of the Raman modes as a function of implantation fluence,annealing temperature and time has been analyzed.Results indicate that a lattice quality that is close to as-grown GaSb has been obtained by annealing the implanted samples at 500℃for 45 s.However,consequent surface analyses by scanning electron microscope(SEM)and atomic force microscope(AFM)show that a heavily perturbed layer contains voids due to the outdifiusion of Sb atoms on the surface remains.Mechanism of the damage recovery and the structure of the implanted layer are discussed based on the experimental results.

Flat Top Optical Frequency Combs Based on a Single-Core Quantum Cascade Laser at Wavelength of~8.7μm

We present optical frequency combs with a spectral emission of 48 cm-1and an output power of 420 m W based on a single-core quantum cascade laser at λ ~ 8.7μm. A flat top spectrum sustains up to 130 comb modes delivering ~ 3.2 m W of optical power per mode, making it a valuable tool for dual comb spectroscopy. The homogeneous gain medium, relying on a slightly diagonal bound-to-continuum structure, promises to provide a broad and stable gain for comb operating. Remarkably, the dispersion of this device is measured within 300 fs2/mm to ensure stable comb operation over 90% of the total current range. The comb is observed with a narrow beatnote linewidth around 2 k Hz and has weak dependence on the applied current for stable comb operation.

Helicity-dependent photoconductance of the edge states in the topological insulator Bi_(2)Te_(3)

The helicity-dependent photoconductance of the edge states in three-dimensional topological insulator Bi_(2)Te_(3)films is investigated.It is revealed that the helicity-dependent photoconductivity current on the left edge of the Bi_(2)Te_(3)film shows an opposite sign with that on the right edge.In addition,the helicity-dependent photoconductivity current increases linearly with the applied longitudinal electric field,and it reverses the sign with the reversal of the electric field.As the thickness of the Bi_(2)Te_(3)film increases,the helicity-dependent photoconductivity current also increases.Theoretical analysis suggests that the helicity-dependent photo-conductivity current may come from the intrinsic spin orbit coupling(SOC)or the SOC introduced by the chiral impurities or defects.

Deep-ultraviolet photonics for the disinfection of SARS-CoV-2 and its variants(Delta and Omicron)in the cryogenic environment

Deep-ultraviolet(DUV)disinfection technology provides an expeditious and efficient way to suppress the transmission of coronavirus disease 2019(COVID-19).However,the influences of viral variants(Delta and Omicron)and low temperatures on the DUV virucidal efficacy are still unknown.Here,we developed a reliable and uniform planar light source comprised of 275-nm light-emitting diodes(LEDs)to investigate the effects of these two unknown factors and delineated the principle behind different disinfection performances.We found the lethal effect of DUV at the same radiation dose was reduced by the cryogenic environment,and a negative-U large-relaxation model was used to explain the difference in view of the photoelectronic nature.The chances were higher in the cryogenic environment for the capture of excited electrons within active genetic molecules back to the initial photo-ionised positions.Additionally,the variant of Omicron required a significantly higher DUV dose to achieve the same virucidal efficacy,and this was thanks to the genetic and proteinic characteristics of the Omicron.The findings in this study are important for human society using DUV disinfection in cold conditions(e.g.,the food cold chain logistics and the open air in winter),and the relevant DUV disinfection suggestion against COVID-19 is provided.

The measurement of responsivity of infrared photodetectors using a cavity blackbody

For the measurement of responsivity of an infrared photodetector,the most-used radiation source is a blackbody.In such a measurement system,distance between the blackbody,the photodetector and the aperture diameter are two parameters that contribute most measurement errors.In this work,we describe the configuration of our responsivity measurement system in great detail and present a method to calibrate the distance and aperture diameter.The core of this calibration method is to transfer direct measurements of these two parameters into an extraction procedure by fitting the experiment data to the calculated results.The calibration method is proved experimentally with a commercially extended InGaAs detector at a wide range of blackbody temperature,aperture diameter and distance.Then proof procedures are further extended into a detector fabricated in our laboratory and consistent results were obtained.