Chlorine-Substituent Regulation in Dopant-Free Small-Molecule Hole-Transport Materials Improves the Effi ciency and Stability of Inverted Perovskite Solar Cells

Although doped hole-transport materials(HTMs)off er an effi ciency benefi t for perovskite solar cells(PSCs),they inevi-tably diminish the stability.Here,we describe the use of various chlorinated small molecules,specifi cally fl uorenone-triphenylamine(FO-TPA)-x-Cl[x=para,meta,and ortho(p,m,and o)],with diff erent chlorine-substituent positions,as dopant-free HTMs for PSCs.These chlorinated molecules feature a symmetrical donor-acceptor-donor structure and ideal intramolecular charge transfer properties,allowing for self-doping and the establishment of built-in potentials for improving charge extraction.Highly effi cient hole-transfer interfaces are constructed between perovskites and these HTMs by strategi-cally modifying the chlorine substitution.Thus,the chlorinated HTM-derived inverted PSCs exhibited superior effi ciencies and air stabilities.Importantly,the dopant-free HTM FO-TPA-o-Cl not only attains a power conversion effi ciency of 20.82% but also demonstrates exceptional stability,retaining 93.8%of its initial effi ciency even after a 30-day aging test conducted under ambient air conditions in PSCs without encapsulation.These fi ndings underscore the critical role of chlorine-substituent regulation in HTMs in ensuring the formation and maintenance of effi cient and stable PSCs.

Probing the effects of lithium doping on structures, properties, and stabilities of magnesium cluster anions

Bimetallic clusters have aroused tremendous interest because the property changes like structure,size,and composition have occurred.Herein,a structural search of the global minimum for anionic LiMg_(n)^(-)(n=2-11) clusters is performed using an efficient crystal structure analysis by particle swarm optimization(CALYPSO) structural searching program with subsequent density functional theory(DFT) calculations.A great variety of low energetic isomers are converged,and the most stable ones are confirmed by comparing their total energy of each size.It is found that the LiMg_(n)^(-)clusters are structurally consistent with corresponding Mg clusters anions except for LiMg_(5)^(-)and LiMg_(7)^(-).In all the doped clusters,the Li atom prefers to occupy the convex position.Simulated photoelectron spectra(PES),Infrared(IR),and Raman spectra of LiMg_(n)^(-)could be used as an essential evidence for identifying cluster structures experimentally in the future.Stability study reveals that a tower-like structure of LiMg_(9)^(-)has prominent stability and can be identified as a magic number cluster.The reason might be that there are both closed-shell 1S^(2)1P^(6)1D^(10)2S^(2) electronic configurations and stronger Li-Mg bonds caused by sp hybridization in the LiMg_(9)^(-)cluster.

Room Temperature Synthesis of Vertically Aligned Amorphous Ultrathin NiCo-LDH Nanosheets Bifunctional Flexible Supercapacitor Electrodes

Developing a simple scalable method to fabricate electrodes with high capacity and wide voltage range is desired for the real use of electrochemical supercapacitors.Herein,we synthesized amorphous NiCo-LDH nanosheets vertically aligned on activated carbon cloth substrate,which was in situ transformed from Co-metal-organic framework materials nano-columns by a simple ion exchange process at room temperature.Due to the amorphous and vertically aligned ultrathin structure of NiCo-LDH,the NiCo-LDH/activated carbon cloth composites present high areal capacities of 3770 and 1480 mF cm^(-2)as cathode and anode at 2 mA cm^(-2),and 79.5%and 80%capacity have been preserved at 50 mA cm^(-2).In the meantime,they all showed excellent cycling performance with negligible change after>10000 cycles.By fabricating them into an asymmetric supercapacitor,the device achieves high energy densities(5.61 mWh cm^(-2)and 0.352 mW cm^(-3)).This work provides an innovative strategy for simplifying the design of supercapacitors as well as providing a new understanding of improving the rate capabilities/cycling stability of NiCo-LDH materials.

First-principles investigation of the valley and electrical properties of carbon-dopedα-graphyne-like BN sheet

Based on ab initio density functional theory calculations,we demonstrate that two carbon-doped boron nitride analog ofα-graphyne structures,B_(3) C_(2) N_(3)) and BC_(6) N monolayers,are two-dimensional direct wide band gap semiconductors,and there are two inequivalent valleys in the vicinities of the vertices of their hexagonal Brillouin zones.Besides,B_(3)C_(2)N_(3) and BC_(6)N monolayers exhibit relatively high carrier mobilities,and their direct band gap feature is robust against the biaxial strain.More importantly,the energetically most favorable B_(3)C_(2)N_(3) and BC_(6)N bilayers also have direct wide band gaps,and valley polarization could be achieved by optical helicity.Finally,we show that BC_(6) N monolayer might have high efficiency in photo-splitting reactions of water,and a vertical van der Waals heterostructure with a type-Ⅱenergy band alignment could be designed using B_(3)C_(2)N_(3)and BC_(6)N monolayers.All the above-mentioned characteristics make B_(3)C_(2)N_(3) and BC_(6)N monolayers,bilayers,and their heterostructures recommendable candidates for applications in valleytronic devices,metal-free photocatalysts,and photovoltaic cells.

New crystal structure and physical properties of TcB from first-principles calculations

By combining first-principles calculations with the particle swarm optimization algorithm, we predicted a hexagonal Pˉ3m1 structure for Tc B, which is energetically more favorable than the previously reported WC-type and Cmcm structures.The new phase is mechanically and dynamically stable, as confirmed by its phonon and elastic constants calculations.The calculated mechanical properties show that it is an ultra-incompressible and hard material. Meanwhile, the elastic anisotropy is investigated by the shear anisotropic factors and ratio of the directional bulk modulus. Density of states analysis reveals that the strong covalent bonding between Tc and B atoms plays a leading role in forming a hard material. Additionally, the compressibility, bulk modulus, Debye temperature, Gruneisen parameter, specific heat, and thermal expansion coefficient of Tc B are also successfully obtained by using the quasi-harmonic Debye model.

Band Alignment and Band Gap Characterization of La2O3 Films on Si Substrates Grown by Radio Frequency Magnetron Sputtering

La2O3 films are grown on Si （100） substrates by the radio-frequency magnetron sputtering technique. The band alignment of the La203/Si heterojunction is analyzed by the x-ray photoelectron spectroscopy. The valence- band and the conduction-band offsets of La2 Oa films to Si substrates are found to be 2.40±0.1 and 1.66±0.3 eV, respectively. Based on 0 ls energy loss spectrum analysis, it can be noted that the energy gap of La203 films is 5.18±0.2eV, which is confirmed by the ultra-violet visible spectrum. According to the suitable band offset and large band gap, it can be concluded that La2O3 could be a promising candidate to act as high-k gate dielectrics.

Structures and magnetic properties of Fe and Ni monoatomic chains encapsulated by an Au nanotube

Structures and magnetic properties of transition metal （TM） Fe or Ni monoatomic chains （MACs） encapsulated by a Au （5, 5） nanotube （Fe@Au and Ni@Au） are investigated using the density functional theory （DFT）. The calculated results show that both Fe@Au and Ni@Au prefer to adopt ferromagnetic （FM） orders as ground states. In particular, the Fe@Au keeps the magnetic properties of free-standing Fe MAC, indicating that this system may be viewed as a new candidate in electromagnetic devices.

Structural,magnetic,and dielectric properties of Ni-Zn ferrite and Bi_(2)O_(3)nanocomposites prepared by the sol-gel method

Ni-Zn ferrite and Bi_(2)O_(3)composites were developed by the sol-gel method.The structural,magnetic,and dielectric properties were studied for all the prepared samples.X-ray diffraction(XRD)was performed to study the crystal structure.The results of field emission scanning electron microscopy(FE-SEM)showed that the addition of Bi_(2)O_(3)can increase the grain size of the Ni-Zn ferrite.Magnetic properties were analyzed by a hysteresis loop test and it was found that the saturation magnetization and coercivity decreased with the increase of Bi_(2)O_(3)ratio.In addition,the dielectric properties of the Ni-Zn ferrite were also improved with the addition of Bi_(2)O_(3).

Physical generation of random numbers using an asymmetrical Boolean network

Autonomous Boolean networks(ABNs)have been successfully applied to the generation of random number due to their complex nonlinear dynamics and convenient on-chip integration.Most of the ABNs used for random number generators show a symmetric topology,despite their oscillations dependent on the inconsistency of time delays along links.To address this issue,we suggest an asymmetrical autonomous Boolean network(aABN)and show numerically that it provides large amplitude oscillations by using equal time delays along links and the same logical gates.Experimental results show that the chaotic features of aABN are comparable to those of symmetric ABNs despite their being made of fewer nodes.Finally,we put forward a random number generator based on aABN and show that it generates the random numbers passing the NIST test suite at 100 Mbits/s.The unpredictability of the random numbers is analyzed by restarting the random number generator repeatedly.The aABN may replace symmetrical ABNs in many applications using fewer nodes and,in turn,reducing power consumption.

Spectral polarization-encoding of broadband laser pulses by optical rotatory dispersion and its applications in spectral manipulation

We propose a kind of spectral polarization-encoding(SPE)for broadband light pulses,which is realized by inducing optical rotatory dispersion(ORD),and decoded by compensating ORD.Combining with polarization-sensitive devices,SPE can not only work to control polarization-dependent transmission for central wavelength or bandwidth-tunable filtering,but also can be used for broadband regenerative or multi-pass amplification with a polarization-dependent gain medium to improve output bandwidth.SPE is entirely passive thus very simple to be designed and aligned.By using an ORD crystal with a good transmission beyond 3-μm mid-infrared region,e.g.,Ag Ga S_(2),SPE promises to be applied for the wavelength tuning lasers in mid-infrared region,where the tunning devices are rather under developed compared with those in visible and near-infrared region.

Temperature and strain sensitivities of surface and hybrid acoustic wave Brillouin scattering in optical microfibers

Temperature and strain sensitivities of surface acoustic wave(SAW)and hybrid acoustic wave(HAW)Brillouin scat-tering(BS)in 1μm-1.3μm diameter optical microfibers are simulated.In contrast to stimulated Brillouin scattering(SBS)from bulk acoustic wave in standard optical fiber,SAW and HAW BS,due to SAWs and HAWs induced by the coupling of longitudinal and shear waves and propagating along the surface and core of microfiber respectively,facilitate innovative detection in optical microfibers sensing.The highest temperature and strain sensitivities of the hybrid acoustic modes(HAMs)are 1.082 MHz/℃and 0.0289 MHz/με,respectively,which is suitable for microfiber sensing applica-tion of high temperature and strain resolutions.Meanwhile,the temperature and strain sensitivities of the SAMs are less affected by fiber diameter changes,ranging from 0.05 MHz/℃/μm to 0.25 MHz/℃/μm and 1×10^(-4) MHz/με/μm to 5×10^(-4) MHz/με/μm,respectively.It can be found that that SAW BS for temperature and strain sensing would put less stress on manufacturing constraints for optical microfibers.Besides,the simultaneous sensing of temperature and strain can be realized by SAW and HAW BS,with temperature and strain errors as low as 0.30℃-0.34℃and 14.47με-16.25με.

Polar, catalytic, and conductive CoSe2/C frameworks for performance enhanced S cathode in Li–S batteries

Lithium-sulfur battery(Li-S)is considered as one of the new-generation rechargeable batteries with high performance because of its extremely high theoretical capacity,energy density,environmental harmony and low cost.However,low electrical and ionic conductivity of sulfur,safety concerns and parasitic reaction generated by the dissolved polysulfide species in electrolyte hinder the commercialization of Li-S battery.Herein,we report a polyhedral porous structure comprising of carbon coating metal selenide nanoparticles(CoSe2/C),which could not only host sulfur for Li-S battery owing to its porous and conductive structure,but also mitigate the shuttle phenomenon by polysulfides adsorption and catalytic acceleration of redox kinetics.As a result,a performance enhanced CoSe2/C-S electrode for Li-S battery is achieved.

Ultrafast multi-target control of tightly focused light fields

The control of ultrafast optical field is of great interest in developing ultrafast optics as well as the investigation on vari-ous light-matter interactions with ultrashort pulses.However,conventional spatial encoding approaches have only lim-ited steerable targets usually neglecting the temporal effect,thus hindering their broad applications.Here we present a new concept for realizing ultrafast modulation of multi-target focal fields based on the facile combination of time-depend-ent vectorial diffraction theory with fast Fourier transform.This is achieved by focusing femtosecond pulsed light carrying vectorial-vortex by a single objective lens under tight focusing condition.It is uncovered that the ultrafast temporal de-gree of freedom within a configurable temporal duration(~400 fs)plays a pivotal role in determining the rich and exotic features of the focused optical field at one time,namely,bright-dark alternation,periodic rotation,and longitudinal/trans-verse polarization conversion.The underlying control mechanisms have been unveiled.Besides being of academic in-terest in diverse ultrafast spectral regimes,these peculiar behaviors of the space-time evolutionary beams may underpin prolific ultrafast-related applications such as multifunctional integrated optical chip,high-efficiency laser trapping,micro-structure rotation,super-resolution optical microscopy,precise optical measurement,and liveness tracking.

Atom interferometers with weak-measurement path detectors and their quantum mechanical analysis

According to the orthodox interpretation of quantum physics, wave-particle duality(WPD) is the intrinsic property of all massive microscopic particles. All gedanken or realistic experiments based on atom interferometers(AI) have so far upheld the principle of WPD, either by the mechanism of the Heisenberg’s position-momentum uncertainty relation or by quantum entanglement. In this paper, we propose and make a systematic quantum mechanical analysis of several schemes of weak-measurement atom interferometer(WM-AI) and compare them with the historical schemes of strongmeasurement atom interferometer(SM-AI), such as Einstein’s recoiling slit and Feynman’s light microscope. As the critical part of these WM-AI setups, a weak-measurement path detector(WM-PD) deliberately interacting with the atomic internal electronic quantum states is designed and used to probe the which-path information of the atom, while only inducing negligible perturbation of the atomic center-of-mass motion. Another instrument that is used to directly interact with the atomic center-of-mass while being insensitive to the internal electronic quantum states is used to monitor the atomic centerof-mass interference pattern. Two typical schemes of WM-PD are considered. The first is the micromaser-cavity path detector, which allows us to probe the spontaneously emitted microwave photon from the incoming Rydberg atom in its excited electronic state and record unanimously the which-path information of the atom. The second is the optical-lattice Bragg-grating path detector, which can split the incoming atom beam into two different directions as determined by the internal electronic state and thus encode the which-path information of the atom into the internal states of the atom. We have used standard quantum mechanics to analyze the evolution of the atomic center-of-mass and internal electronic state wave function by directly solving Schr¨odinger’s equation for the composite atom-electron-photon system in these WM-AIs. We have also compared our analysis with the theoretical and experimental studies that have been presented in the previous literature. The results show that the two sets of instruments can work separately, collectively, and without mutual exclusion to enable simultaneous observation of both wave and particle nature of the atoms to a much higher level than the historical SM-AIs, while avoiding degradation from Heisenberg’s uncertainty relation and quantum entanglement. We have further investigated the space–time evolution of the internal electronic quantum state, as well as the combined atom–detector system and identified the microscopic origin and role of quantum entanglement, as emphasized in numerous previous studies. Based on these physics insights and theoretical analyses, we have proposed several new WM-AI schemes that can help to elucidate the puzzling physics of the WPD of the atoms. The principle of WM-AI scheme and quantum mechanical analyses made in this work can be directly extended to examine the principle of WPD for other massive particles.

Broadband mid-infrared pulse via intra-pulse difference frequency generation based on supercontinuum from multiple thin plates

We report on the generation of optical pulses with a nearly one octave-spanning spectrum ranging from 1300 nm to2500 nm at 1 kHz repetition rate, which are based on intra-pulse difference frequency generation(DFG) in β-barium borate crystal(β-BBO) and passively carrier-envelope-phase(CEP) stabilized. The DFG is induced by few-cycle pulses initiated from spectral broadening in multiple thin plates driven by a Ti: sapphire chirped-pulse amplifier. Furthermore, a numerical simulation is developed to estimate the conversion efficiency and output spectrum of the DFG. Our results show that the pulses from the DFG have the potential for seeding intense mid-infrared(MIR) laser generation and amplification to study strong-field physics and attosecond science.

Fast-speed self-powered PEDOT:PSS/α-Ga_(2)O_(3)nanorod array/FTO photodetector with solar-blind UV/visible dual-band photodetection

Theα-Ga2 O_(3)nanorod array is grown on FTO by hydrothermal and annealing processes.And a self-powered PEDOT:PSS/α-Ga_(2)O_(3)nanorod array/FTO(PGF)photodetector has been demonstrated by spin coating PEDOT:PSS on theα-Ga_(2)O_(3)nanorod array.Successfully,the PGF photodetector shows solar-blind UV/visible dual-band photodetection.Our device possesses comparable solar-blind UV responsivity(0.18 mA/W at 235 nm)and much faster response speed(0.102 s)than most of the reported self-poweredα-Ga_(2)O_(3)nanorod array solar-blind UV photodetectors.And it presents the featured and distinguished visible band photoresponse with a response speed of 0.136 s at 540 nm.The response time is also much faster than the other non-self-poweredβ-Ga_(2)O_(3)DUV/visible dual-band photodetectors due to the fast-speed separation of photogenerated carries by the built-in electric field in the depletion regions of PEDOT:PSS/α-Ga_(2)O_(3)heterojunction.The results herein may prove a promising way to realize fast-speed self-poweredα-Ga_(2)O_(3)photodetectors with solar-blind UV/visible dual-band photodetection by simple processes for the applications of multiple-target tracking,imaging,machine vision and communication.

TiS_(2)-graphene heterostructures enabling polysulfide anchoring and fast electrocatalyst for lithium-sulfur batteries:A first-principles calculation

Lithium-sulfur batteries have attracted attention because of their high energy density.However,the "shuttle effect" caused by the dissolving of polysulfide in the electrolyte has greatly hindered the widespread commercial use of lithiumsulfur batteries.In this paper,a novel two-dimensional TiS2/graphene heterostructure is theoretically designed as the anchoring material for lithium-sulfur batteries to suppress the shuttle effect.This heterostructure formed by the stacking of graphene and TiS2 monolayer is the van der Waals type,which retains the intrinsic metallic electronic structure of graphene and TiS2 monolayer.Graphene improves the electronic conductivity of the sulfur cathode,and the transferred electrons from graphene enhance the polarity of the TiS2 monolayer.Simulations of the polysulfide adsorption show that the TiS2/graphene hetero structure can maintain good metallic properties and the appropriate adsorption energies of 0.98-3.72 eV,which can effectively anchor polysulfides.Charge transfer analysis suggests that further enhancement of polarity is beneficial to reduce the high proportion of van der Waals(vdW) force in the adsorption energy,thereby further enhancing the anchoring ability.Low Li2 S decomposition barrier and Li-ion migration barrier imply that the heterostructure has the ability to catalyze fast electrochemical kinetic processes.Therefore,TiS2/graphene heterostructure could be an important candidate for ideal anchoring materials of lithium-sulfur batteries.

Dimension effects on the dielectric properties of fine BaTiO_3 ceramics

It is found that the core-shell structured grains are easy to produce for fine grain doped BaTiO3 ceramics in the sintering process. We study the influence of the core-shell structure on the Curie-Weiss temperature and dielectric properties of BaTiO3 ceramics by using effective medium approximation （EMA）. Considering the second approximation, the dielectric properties of fine grain doped BaTiO3 ceramics are consistent with experimental data.

Photo-induced absorption in the pump probe spectroscopy of single-walled carbon nanotubes

Femtosecond pump probe spectroscopy is employed to study the photo-induced absorption feature in the single-walled carbon nanotube transient spectrum. The two advantages of the experiment, a chirality enriched sample and tuning the pump wavelength to the resonance of a specific nanotube species, greatly facilitate the identification of the photo-induced absorption signal of one tube species. It is found that a photo-induced absorption feature is located at one radial breathing mode to the blue side of the E11 state. This finding prompts a new explanation for the origin of the photo-induced absorption： the transition from the ground state to a phonon coupled state near the E ii state. The explanation suggests a superposition mechanism of the photo-bleach and photo-induced absorption signals, which may serve as a key to the interpretation of the complex pump probe transient spectrum of carbon nanotubes. The finding sheds some light on the understanding of the complex non-radiative relaxation process and the electronic structure of single-walled carbon nanotubes.

Topological quantum-phase coherence in full counting statistics of transport electrons with two-body interaction

The full counting statistics of electron transport through two parallel quantum dots with antiparallel magnetic fluxes is investigated as a probe to detect the topological quantum-phase coherence （TQPC）, which results in the characteristic oscillation of the zero-frequency cumulants including the shot noise and skewness. We show explicitly the phase transition of cumulant spectrum-patterns induced by the topology change of electron path-loops while the pattern period, which depends only on the topology （or Chern number）, is robust against the variation of Coulomb interaction and interdot coupling strengths. Most importantly we report for the first time on a new type of TQPC, which is generated by the two- particle interaction and does not exist in the single-particle wave function interference. Moreover, the accurately quantized peaks of Fano-factor spectrum, which characterize the super- and sub-Poissonian shot noises, are of fundamental importance in technical applications similar to the superconducting quantum interference device.