We identified the antimony species present in a wide variety of plastic samples by X ray absorption spectroscopy(XAS)at the Sb L_(3)-edge.The samples contained different concentrations of antimony(Sb),ranging from PET...We identified the antimony species present in a wide variety of plastic samples by X ray absorption spectroscopy(XAS)at the Sb L_(3)-edge.The samples contained different concentrations of antimony(Sb),ranging from PET bottles in which Sb compounds are used as catalysts,with concentrations around 300 mg/kg,to electrical equipment in which the element is used as a flame retardant,with concentrations of several tens of thousands of mg/kg.Although the shape of the spectra at the L_(3)-edge is quite similar for all Sb reference materials,we were able to identify antimony glycolate or acetate in PET bottles,bound organic Sb in c-PET trays and senarmontite in electrical materials as themain Sb components.In samples with high Ca content(e.g.,electrical objects,some c-PET food trays and textiles)the Ca Ka emission line interferes with the Sb La line by introducing a high background which reduces the signal-to-noise ratio in the Sb XAS spectrum,resulting in noisy and distorted spectra.The element-resolved map on a PET bottle sample revealed both Sb and Ca hot spots of around 10-20 microns in size,with no correlation.展开更多
Despite the rapid efficiency increase,tin halide perovskite solar cells are significantly behind their lead-based counterpart,with the highest reported efficiency of 15.38%.The main reason for this large difference is...Despite the rapid efficiency increase,tin halide perovskite solar cells are significantly behind their lead-based counterpart,with the highest reported efficiency of 15.38%.The main reason for this large difference is attributed to the instability of Sn^(2+),which easily oxidizes to Sn^(4+),creating Sn vacancies and increasing the open-circuit voltage loss.In this work,we implemented tin thiocyanate(Sn(SCN)_(2))as an additive for passivating the bulk defects of a germanium-doped tin halide perovskite film.Adding Sn^(2+)and SCN-ions reduces the Sn and iodine vacancies,limiting non-radiative recombination and favoring longer charge-carrier dynamics.Moreover,the addition of Sn(SCN)_(2) induces a higher film crystallinity and preferential orientation of the(l00)planes parallel to the substrate.The passivated devices showed improved photovoltaic parameters with the best open-circuit voltage of 0.716 V and the best efficiency of 12.22%,compared to 0.647 V and 10.2%for the reference device.In addition,the passivated solar cell retains 88.7%of its initial efficiency after 80 min of illumination under 100 mW cm^(-2) and is substantially better than the control device,which reaches 82.6%of its initial power conversion efficiency only after 30 min.This work demonstrates the passivation potential of tin-based additives,which combined with different counterions give a relatively large space of choices for passivation of Sn-based perovskites.展开更多
We used fast chlorophyll fluorescence transients(OJIP) to study provenance-related differences in photosynthetic performance and the magnitude of day-to-day chlorophyll fluorescence(ChlF) variation in northern(67°...We used fast chlorophyll fluorescence transients(OJIP) to study provenance-related differences in photosynthetic performance and the magnitude of day-to-day chlorophyll fluorescence(ChlF) variation in northern(67°N)and southern(62°N) silver birches in a common garden at62°N.ChlF transients were measured five times during two weeks in the middle of summer to avoid seasonal variation.Differences in growth and leaf morphological traits between the provenances were also examined.The northern trees had higher chlorophyll content,larger leaf areas,and higher leaf fresh and dry mass than the southern trees,but the leaf mass per area did not differ between the provenances.The southern trees were taller and showed higher annual shoot growth than the northern trees.For all the ChlF parameters,day-to-day variation was significant and followed the same pattern for both provenances with no significant provenance ×day interaction,suggesting a similar response to environmental variation.The northern provenance had higher values in parameters related to the reduction of end electron acceptors at the Photosystem I(PSI) acceptor side as probed by ChlF.This and higher values for performance indices PI_(abs) and PI_(tot) in northern than in southern trees suggest higher photosynthetic performance of northern trees in line with the latitudinal compensation strategy.Provenance differences in these parameters increased towards the end of the measurement period,suggesting preparation for earlier growth cessation in northern trees triggered by the shortening day length.The study shows that provenance differences in ChlF can be relatively stable regardless of environmental variation but might be influenced by physiological alterations in preparation for future changes in environmental conditions.展开更多
We present a 3+1 formulation of the light modes in nonlinear electrodynamics described by Plebanski-type Lagrangians,which include post-Maxwellian,Born-Infeld,ModMax,and Heisenberg-Euler-Schwinger QED Lagrangians.In n...We present a 3+1 formulation of the light modes in nonlinear electrodynamics described by Plebanski-type Lagrangians,which include post-Maxwellian,Born-Infeld,ModMax,and Heisenberg-Euler-Schwinger QED Lagrangians.In nonlinear electrodynamics,strong electromagnetic fields modify the vacuum such that it acquires optical properties.Such a field-modified vacuum can possess electric permittivity,magnetic permeability,and a magneto-electric response,inducing novel phenomena such as vacuum birefringence.By exploiting the mathematical structures of Plebanski-type Lagrangians,we establish a streamlined procedure and explicit formulas to determine light modes,i.e.,refractive indices and polarization vectors for a given propagation direction.We also work out the light modes of the various Lagrangians for an arbitrarily strong magnetic field.The 3+1 formulation advanced in this paper has direct applications to the current vacuum birefringence research:terrestrial experiments using permanent magnets/ultra-intense lasers for the subcritical regime and astrophysical observation of X-rays from highly magnetized neutron stars for the near-critical and supercritical regimes.展开更多
Liquid-liquid phase separation(LLPS)of proteins and nucleic acids is a common phenomenon in cells that underlies the formation of membraneless organelles.Although the macroscopic behavior of biomolecular coacervates h...Liquid-liquid phase separation(LLPS)of proteins and nucleic acids is a common phenomenon in cells that underlies the formation of membraneless organelles.Although the macroscopic behavior of biomolecular coacervates has been elucidated by microscopy,the detailed dynamic properties of proteins/peptides during the LLPS process remain poorly characterized.Here,site-directed spin labeling-electron paramagnetic resonance(SDSL-EPR)spectroscopy was employed to characterize the dynamic properties of a minimal model LLPS system consisting of positively charged peptides and RNA.The degree of phase separation,indicated by broadening of the EPR spectrum of the spin-labeled peptide due to slow molecular tumbling,was monitored by EPR.In addition,three distinct populations with varying molecular motion during LLPS,featuring different spectral lineshapes,were identified.These populations included a fast motion component(Ⅰ),a slower motion component(Ⅱ)associated with peptides in the dispersed phase and an immobile component(Ⅲ)observed in the dense phase.With gradual titration of the peptides to RNA,the EPR spectrum gradually shifted,refiecting changes in the populations of the components.Together,SDSL-EPR method not only provides new insights into the dynamic behavior of biomolecules during LLPS,but also offers a sensitive method for biomolecular phase separation processes at the molecular level.展开更多
The design of a novel photonic crystal waveguide power splitter is presented.The proposed power splitter has three output ports,the coupling among three parallel photonic crystal waveguides can be considered as a mult...The design of a novel photonic crystal waveguide power splitter is presented.The proposed power splitter has three output ports,the coupling among three parallel photonic crystal waveguides can be considered as a multimode interference(MMI),and the positions of output waveguides are determined by those of twofold images which are formed by the self-imaging effect of multimode interference.The transmission characteristics of the splitter are investigated by using the finite-difference time domain(FDTD) and the plane wave expansion method.The output optical power in each port can be controlled by adjusting the radius of the dielectric rods in the coupling region,and the coupling effect among output ports is decreased by using the T-shaped output port.The results indicate that 1 × 1,1 × 2 and 1 × 3 type power splitters can be realized when the normalized radius of dielectric rods in the coupling region is 0.130,0.180,0.152 or 0.221,respectively.展开更多
We numerically investigate the population dynamics in a single photon resonant three-level cascade and non-cascade energy level molecules at 532-nm wavelength. The time-dependent population in the energy levels in the...We numerically investigate the population dynamics in a single photon resonant three-level cascade and non-cascade energy level molecules at 532-nm wavelength. The time-dependent population in the energy levels in the presence of 100 ps(pico-second) and 100 ns(nano-second) laser pulses is described in the form of rate equations. We provide a brief idea of how the optical energy transfer takes place in the light-matter interaction and we also discuss the absorption as a function of pulse width and repetition rate. We also plot the z-scan transmittance curve as a function of number of excitation pulses participating in the absorption.展开更多
Two-photon photopolymerization （TPP） of femtosecond laser is a promising method to fabricate three-dimensional woodpile photonic crystals （PCs）. We build micro-fabricatlon system based on the principle of TPP. Thr...Two-photon photopolymerization （TPP） of femtosecond laser is a promising method to fabricate three-dimensional woodpile photonic crystals （PCs）. We build micro-fabricatlon system based on the principle of TPP. Three- dimensional woodpile PCs consisting of in-plane rod distances ranging from 1000nm to 2000nm are fabricated by focusing femtosecond laser in photosensitive liquid resin ORMOCER. The properties of the PCs are also discussed, and fundamental photonic band gaps in middle-infrared range are measured, whose in-plane rod distances are 1500nm and 2000 nm. Three-dimenslonal woodpile PC devices with desired defects, such as cross-waveguide and micro-laser structures, are introduced easily by TPP. We fabricate the three-dimensional woodpile PCs in the liquid resin at the fast scanning speed of 120μm/s.展开更多
NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy leve...NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy levels and possible redox reactions at the NiO_(x)/perovskite interface severely limit the performance of NiO_(x) based inverted perovskite solar cells.Herein,we introduce a p-type self-assembled monolayer between NiO_(x)and perovskite layers to modify the interface and block the undesirable redox reaction between perovskite and NiO_(x)The selfassembled monolayer molecules all contain phosphoric acid function groups,which can be anchored onto the NiOr surface and passivate the surface defect.Moreover,the introduction of self-assembled monolayers can regulate the energy level structure of NiO_(x),reduce the interfacial band energy offset,and hence promote the hole transport from perovskite to NiO_(x)layer.Consequently,the device performance is significantly enhanced in terms of both power conversion efficiency and stability.展开更多
The parasitic hydrogen evolution reaction(HER)in the negative half-cell of vanadium redox flow batteries(VRFBs)causes severe efficiency losses.Thus,a deeper understanding of this process and the accompanying bubble fo...The parasitic hydrogen evolution reaction(HER)in the negative half-cell of vanadium redox flow batteries(VRFBs)causes severe efficiency losses.Thus,a deeper understanding of this process and the accompanying bubble formation is crucial.This benchmarking study locally analyzes the bubble distribution in thick,porous electrodes for the first time using deep learning-based image segmentation of synchrotron X-ray micro-tomograms.Each large three-dimensional data set was processed precisely in less than one minute while minimizing human errors and pointing out areas of increased HER activity in VRFBs.The study systematically varies the electrode potential and material,concluding that more negative electrode potentials of-200 m V vs.reversible hydrogen electrode(RHE)and lower cause more substantial bubble formation,resulting in bubble fractions of around 15%–20%in carbon felt electrodes.Contrarily,the bubble fractions stay only around 2%in an electrode combining carbon felt and carbon paper.The detected areas with high HER activity,such as the border subregion with more than 30%bubble fraction in carbon felt electrodes,the cutting edges,and preferential spots in the electrode bulk,are potential-independent and suggest that larger electrodes with a higher bulk-to-border ratio might reduce HER-related performance losses.The described combination of electrochemical measurements,local X-ray microtomography,AI-based segmentation,and 3D morphometric analysis is a powerful and novel approach for local bubble analysis in three-dimensional porous electrodes,providing an essential toolkit for a broad community working on bubble-generating electrochemical systems.展开更多
Herein,we report the facile synthesis of a highly strained hexabenzocoronene-containing carbon nanoring,cyclo[4]-paraphenylene[2]-2,11-hexabenzocoronenylene([4,2]CPHBC),as the segment of a[10,10]single-walled carbon n...Herein,we report the facile synthesis of a highly strained hexabenzocoronene-containing carbon nanoring,cyclo[4]-paraphenylene[2]-2,11-hexabenzocoronenylene([4,2]CPHBC),as the segment of a[10,10]single-walled carbon nanotube([10,10]SWNT).[4,2]CPHBC was synthesized based on the platinummediated assembly of diborylbiphenyl and diborylhexabenzocoronene,forming a tetranuclear platinum complex,followed by reductive elimination.This nanoring molecule was confirmed by NMR and HRMS,and its photophysical properties were studied using steady-state and time-resolved spectroscopies.Moreover,the selective supramolecular host-vip interaction between[4,2]CPHBC and C_(60) was also investigated.展开更多
Bacterial small laccases(SLAC) are promising industrial biocatalysts due to their ability to oxidize a broad range of substrates with exceptional thermostability and tolerance for alkaline p H. Electron transfer betwe...Bacterial small laccases(SLAC) are promising industrial biocatalysts due to their ability to oxidize a broad range of substrates with exceptional thermostability and tolerance for alkaline p H. Electron transfer between substrate, copper centers, and O2is one of the key steps in the catalytic turnover of SLAC. However, limited research has been conducted on the electron transfer pathway of SLAC and SLAC-catalyzed reactions, hindering further engineering of SLAC to produce tunable biocatalysts for novel applications. Herein, the combinational use of electron paramagnetic resonance(EPR) and ultraviolet-visible(UV-vis) spectroscopic methods coupled with redox titration were employed to monitor the electron transfer processes and obtain further insights into the electron transfer pathway in SLAC. The reduction potentials for type 1 copper(T1Cu), type 2 copper(T2Cu) and type 3copper(T3Cu) were determined to be 367 ± 2 mV, 378 ± 5 m V and 403 ± 2 mV,respectively. Moreover, the reduction potential of a selected substrate of SLAC, hydroquinone(HQ), was determined to be 288 mV using cyclic voltammetry(CV). In this way, an electron transfer pathway was identified based on the reduction potentials. Specifically,electrons are transferred from HQ to T1Cu, then to T2Cu and T3Cu, and finally to O2.Furthermore, superhyperfine splitting observed via EPR during redox titration indicated a modification in the covalency of T2Cu upon electron uptake, suggesting a conformational alteration in the protein environment surrounding the copper sites, which could potentially influence the reduction potential of the copper sites during catalytic processes. The results presented here not only provide a comprehensive method for analyzing the electron transfer pathway in metalloenzymes through reduction potential measurements, but also offer valuable insights for further engineering and directed evolution studies of SLAC in the aim for biotechnological and industrial applications.展开更多
The generation of a plasma with an ultrahigh energy density of 1.2 GJ/cm^(3)(which corresponds to about 12 Gbar pressure) is investigated by irradiating thin stainless-steel foils with high-contrast femtosecond laser ...The generation of a plasma with an ultrahigh energy density of 1.2 GJ/cm^(3)(which corresponds to about 12 Gbar pressure) is investigated by irradiating thin stainless-steel foils with high-contrast femtosecond laser pulses with relativistic intensities of up to 10^(22) W/cm^(2).The plasma parameters are determined by X-ray spectroscopy.The results show that most of the laser energy is absorbed by the plasma at solid density,indicating that no pre-plasma is generated in the current experimental setup.展开更多
Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy...Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO_(4))group is introduced to modify the surface of PrBa_(0.5)Ca_(0.5)Co_(2)O_(5)+δ(PBCC).The achieved catalyst(PO_(4)-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO_(4)on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm^(-2).This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.展开更多
We report on an experiment performed at the FLASH2 free-electron laser(FEL)aimed at producing warm dense matter via soft x-ray isochoric heating.In the experiment,we focus on study of the ions emitted during the soft ...We report on an experiment performed at the FLASH2 free-electron laser(FEL)aimed at producing warm dense matter via soft x-ray isochoric heating.In the experiment,we focus on study of the ions emitted during the soft x-ray ablation process using time-of-flight electron multipliers and a shifted Maxwell–Boltzmann velocity distribution model.We find that most emitted ions are thermal,but that some impurities chemisorbed on the target surface,such as protons,are accelerated by the electrostatic field created in the plasma by escaped electrons.The morphology of the complex crater structure indicates the presence of several ion groups with varying temperatures.We find that the ion sound velocity is controlled by the ion temperature and show how the ion yield depends on the FEL radiation attenuation length in different materials.展开更多
Precision drilling with picosecond laser has been advocated to significantly improve the quality of micro-holes with reduced recast layer thickness and almost no heat affected zone.However,a detailed comparison betwee...Precision drilling with picosecond laser has been advocated to significantly improve the quality of micro-holes with reduced recast layer thickness and almost no heat affected zone.However,a detailed comparison between nanosecond and picosecond laser drilling techniques has rarely been reported in previous research.In the present study,a series of micro-holes are manufactured on stainless steel 304 using a nanosecond and a picosecond laser drilling system,respectively.The quality of the micro-holes,e.g.,recast layer,micro-crack,circularity,and conicity,etc,is evaluated by employing an optical microscope,an optical interferometer,and a scanning electron microscope.Additionally,the micro-structure of the samples between the edges of the micro-holes and the parent material is compared following etching treatment.The researching results show that a great amount of spattering material accumulated at the entrance ends of the nanosecond laser drilled micro-holes.The formation of a recast layer with a thickness of;5μm is detected on the side walls,associated with initiation of micro-cracks.Tapering phenomenon is also observed and the circularity of the micro-holes is rather poor.With regard to the micro-holes drilled by picosecond laser,the entrance ends,the exit ends,and the side walls are quite smooth without accumulation of spattering material,formation of recast layer and micro-cracks.The circularity of the micro-holes is fairly good without observation of tapering phenomenon.Furthermore,there is no obvious difference as for the micro-structure between the edges of the micro-holes and the parent material.This study proposes a picosecond laser helical drilling technique which can be used for effective manufacturing of high quality micro-holes.展开更多
Multi-walled carbon nanotubes （MWCNTs） are grown by arc discharge method in a controlled methane environment. The arc discharge is produced between two graphite electrodes at the ambient pressures of 100 tort, 300 t...Multi-walled carbon nanotubes （MWCNTs） are grown by arc discharge method in a controlled methane environment. The arc discharge is produced between two graphite electrodes at the ambient pressures of 100 tort, 300 torr, and 500 torr. Arc plasma parameters such as temperature and density are estimated to investigate the influences of the ambient pressure and the contributions of the ambient pressure to the growth and the structure of the nanotubes. The plasma temperature and density are observed to increase with the increase in the methane ambient pressure. The samples of MWCNT synthesized at different ambient pressures are analyzed using transmission electron microscopy, scanning electron microscopy, Raman spectroscopy, Fourier transform infrared spectroscopy, and X-ray diffraction. An increase in the growth of MWCNT and a decrease in the inner tube diameter are observed with the increase in the methane ambient pressure.展开更多
Twelve samples with periodic array square pillars microstructure were prepared on the silicon wafer by plasma etching techniques, on which space b of the square pillars increased from 5 to 60 μm. In order to study th...Twelve samples with periodic array square pillars microstructure were prepared on the silicon wafer by plasma etching techniques, on which space b of the square pillars increased from 5 to 60 μm. In order to study the effect ofb on the wettability of the rough surface, the effects of apparent contact angle （CA） and sliding angle （a） of the droplet on the rough surface were measured with the contact angle meter. The results show that the experimental values of CA well agree with the classical wetting theory and a decreases with the increase of b. Two drop shapes exist on the samples＇ surface, corresponding to the Cassie state and the Wenzel state respectively. The contact state in which a drop would settle depends typically on the size of b. On the role of gravitation, the irreversible transition of a drop from Cassie state to Wenzel state should occur at a certain space of the square pillars. Since the transition has implications on the application of super-hydrophobic rough surfaces, theoretically, the prediction of wetting state transition on square pillar array micro-structured surfaces provides an intuitionistic guidance for the design of steady superhydrophobic surfaces.展开更多
Organic–inorganic hybrid perovskite materials demonstrate promising applications in high-efficiency perovskite solar cells (PSCs) with a certified power conversion efficiency(PCE) of 25.5%(https://www.nrel.gov/pv/cel...Organic–inorganic hybrid perovskite materials demonstrate promising applications in high-efficiency perovskite solar cells (PSCs) with a certified power conversion efficiency(PCE) of 25.5%(https://www.nrel.gov/pv/cell-efficiency.html).展开更多
This study deals with Nd：YAG laser cutting nonmetallic materials, which is one of the most important and popular industrial applications of laser. The main theme is to evaluate the effects of Nd：YAG laser beam power...This study deals with Nd：YAG laser cutting nonmetallic materials, which is one of the most important and popular industrial applications of laser. The main theme is to evaluate the effects of Nd：YAG laser beam power besides work piece scanning speed. For approximate cutting depth, a theoretical study is conducted in terms of material property and cutting speed. Results show a nonlinear relation between the cutting depth and input energy. There is no significant effect of speed on cutting depth with the speed being larger than 30 mm/s. An extra energy is utilized in the deep cutting. It is inferred that as the laser power increases, cutting depth increases. The experimental outcomes are in good agreement with theoretical results. This analysis will provide a guideline for laser-based industry to select a suitable laser for cutting, scribing, trimming, engraving, and marking nonmetallic materials.展开更多
文摘We identified the antimony species present in a wide variety of plastic samples by X ray absorption spectroscopy(XAS)at the Sb L_(3)-edge.The samples contained different concentrations of antimony(Sb),ranging from PET bottles in which Sb compounds are used as catalysts,with concentrations around 300 mg/kg,to electrical equipment in which the element is used as a flame retardant,with concentrations of several tens of thousands of mg/kg.Although the shape of the spectra at the L_(3)-edge is quite similar for all Sb reference materials,we were able to identify antimony glycolate or acetate in PET bottles,bound organic Sb in c-PET trays and senarmontite in electrical materials as themain Sb components.In samples with high Ca content(e.g.,electrical objects,some c-PET food trays and textiles)the Ca Ka emission line interferes with the Sb La line by introducing a high background which reduces the signal-to-noise ratio in the Sb XAS spectrum,resulting in noisy and distorted spectra.The element-resolved map on a PET bottle sample revealed both Sb and Ca hot spots of around 10-20 microns in size,with no correlation.
基金support from the Focus Group‘Next Generation Organic Photovoltaics’participating with the Dutch Institute for Fundamental Energy Research(DIFFER)(FOM130)Advanced Materials research program of the Zernike National Research Centre under the Bonus Incentive Scheme(BIS)of the Dutch Ministry for Education,Culture and Science.
文摘Despite the rapid efficiency increase,tin halide perovskite solar cells are significantly behind their lead-based counterpart,with the highest reported efficiency of 15.38%.The main reason for this large difference is attributed to the instability of Sn^(2+),which easily oxidizes to Sn^(4+),creating Sn vacancies and increasing the open-circuit voltage loss.In this work,we implemented tin thiocyanate(Sn(SCN)_(2))as an additive for passivating the bulk defects of a germanium-doped tin halide perovskite film.Adding Sn^(2+)and SCN-ions reduces the Sn and iodine vacancies,limiting non-radiative recombination and favoring longer charge-carrier dynamics.Moreover,the addition of Sn(SCN)_(2) induces a higher film crystallinity and preferential orientation of the(l00)planes parallel to the substrate.The passivated devices showed improved photovoltaic parameters with the best open-circuit voltage of 0.716 V and the best efficiency of 12.22%,compared to 0.647 V and 10.2%for the reference device.In addition,the passivated solar cell retains 88.7%of its initial efficiency after 80 min of illumination under 100 mW cm^(-2) and is substantially better than the control device,which reaches 82.6%of its initial power conversion efficiency only after 30 min.This work demonstrates the passivation potential of tin-based additives,which combined with different counterions give a relatively large space of choices for passivation of Sn-based perovskites.
基金supported by the University of Eastern FinlandCzech University of Life Sciences doctoral research funding to O.A+5 种基金North Karelia Regional Fund to O.A (grant number 55232028)University of Eastern Finland(strategic fundingproject 931060)the Academy of Finland(C-NEUT,project number 347862)part of the Academy of Finland Flagship on Photonics Research and Innovation (PREIN) decision (320166)the Finnish National Plant Phenotyping Infrastructure (NaPPI/Biocenter Finland)
文摘We used fast chlorophyll fluorescence transients(OJIP) to study provenance-related differences in photosynthetic performance and the magnitude of day-to-day chlorophyll fluorescence(ChlF) variation in northern(67°N)and southern(62°N) silver birches in a common garden at62°N.ChlF transients were measured five times during two weeks in the middle of summer to avoid seasonal variation.Differences in growth and leaf morphological traits between the provenances were also examined.The northern trees had higher chlorophyll content,larger leaf areas,and higher leaf fresh and dry mass than the southern trees,but the leaf mass per area did not differ between the provenances.The southern trees were taller and showed higher annual shoot growth than the northern trees.For all the ChlF parameters,day-to-day variation was significant and followed the same pattern for both provenances with no significant provenance ×day interaction,suggesting a similar response to environmental variation.The northern provenance had higher values in parameters related to the reduction of end electron acceptors at the Photosystem I(PSI) acceptor side as probed by ChlF.This and higher values for performance indices PI_(abs) and PI_(tot) in northern than in southern trees suggest higher photosynthetic performance of northern trees in line with the latitudinal compensation strategy.Provenance differences in these parameters increased towards the end of the measurement period,suggesting preparation for earlier growth cessation in northern trees triggered by the shortening day length.The study shows that provenance differences in ChlF can be relatively stable regardless of environmental variation but might be influenced by physiological alterations in preparation for future changes in environmental conditions.
基金supported by the Ultrashort Quantum Beam Facility operation program(Grant No.140011)through APRI,GISTalso by the Institute of Basic Science(Grant No.IBSR038-D1).
文摘We present a 3+1 formulation of the light modes in nonlinear electrodynamics described by Plebanski-type Lagrangians,which include post-Maxwellian,Born-Infeld,ModMax,and Heisenberg-Euler-Schwinger QED Lagrangians.In nonlinear electrodynamics,strong electromagnetic fields modify the vacuum such that it acquires optical properties.Such a field-modified vacuum can possess electric permittivity,magnetic permeability,and a magneto-electric response,inducing novel phenomena such as vacuum birefringence.By exploiting the mathematical structures of Plebanski-type Lagrangians,we establish a streamlined procedure and explicit formulas to determine light modes,i.e.,refractive indices and polarization vectors for a given propagation direction.We also work out the light modes of the various Lagrangians for an arbitrarily strong magnetic field.The 3+1 formulation advanced in this paper has direct applications to the current vacuum birefringence research:terrestrial experiments using permanent magnets/ultra-intense lasers for the subcritical regime and astrophysical observation of X-rays from highly magnetized neutron stars for the near-critical and supercritical regimes.
基金supported by the National Natural Science Foundation of China(No.21927814)the National Key Research and Development Program of China(Nos.2019YFA0405600,2019YFA0706900,2021YFA1200104,2022YFC3400500)+2 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(Nos.XDB0540200,XDB37040201)Plans for Major Provincial Science&Technology Projects(No.202303a07020004)the Youth Innovation Promotion Association,CAS(No.2022455)。
文摘Liquid-liquid phase separation(LLPS)of proteins and nucleic acids is a common phenomenon in cells that underlies the formation of membraneless organelles.Although the macroscopic behavior of biomolecular coacervates has been elucidated by microscopy,the detailed dynamic properties of proteins/peptides during the LLPS process remain poorly characterized.Here,site-directed spin labeling-electron paramagnetic resonance(SDSL-EPR)spectroscopy was employed to characterize the dynamic properties of a minimal model LLPS system consisting of positively charged peptides and RNA.The degree of phase separation,indicated by broadening of the EPR spectrum of the spin-labeled peptide due to slow molecular tumbling,was monitored by EPR.In addition,three distinct populations with varying molecular motion during LLPS,featuring different spectral lineshapes,were identified.These populations included a fast motion component(Ⅰ),a slower motion component(Ⅱ)associated with peptides in the dispersed phase and an immobile component(Ⅲ)observed in the dense phase.With gradual titration of the peptides to RNA,the EPR spectrum gradually shifted,refiecting changes in the populations of the components.Together,SDSL-EPR method not only provides new insights into the dynamic behavior of biomolecules during LLPS,but also offers a sensitive method for biomolecular phase separation processes at the molecular level.
基金supported by the National Natural Science Foundation of China (Nos.60977048 and 50975129)Qianjiang Talent Project of Zhejiang Province (No.2007R10015)the Senior Talent Foundation of Jiangsu University (No.07JDG074)
文摘The design of a novel photonic crystal waveguide power splitter is presented.The proposed power splitter has three output ports,the coupling among three parallel photonic crystal waveguides can be considered as a multimode interference(MMI),and the positions of output waveguides are determined by those of twofold images which are formed by the self-imaging effect of multimode interference.The transmission characteristics of the splitter are investigated by using the finite-difference time domain(FDTD) and the plane wave expansion method.The output optical power in each port can be controlled by adjusting the radius of the dielectric rods in the coupling region,and the coupling effect among output ports is decreased by using the T-shaped output port.The results indicate that 1 × 1,1 × 2 and 1 × 3 type power splitters can be realized when the normalized radius of dielectric rods in the coupling region is 0.130,0.180,0.152 or 0.221,respectively.
文摘We numerically investigate the population dynamics in a single photon resonant three-level cascade and non-cascade energy level molecules at 532-nm wavelength. The time-dependent population in the energy levels in the presence of 100 ps(pico-second) and 100 ns(nano-second) laser pulses is described in the form of rate equations. We provide a brief idea of how the optical energy transfer takes place in the light-matter interaction and we also discuss the absorption as a function of pulse width and repetition rate. We also plot the z-scan transmittance curve as a function of number of excitation pulses participating in the absorption.
基金Supported by the National Natural Science Foundation of China under Grant Nos 50435030 and 50375068, and the Programme for New Century Excellent Talents in Universities of the Ministry of Education of China.
文摘Two-photon photopolymerization （TPP） of femtosecond laser is a promising method to fabricate three-dimensional woodpile photonic crystals （PCs）. We build micro-fabricatlon system based on the principle of TPP. Three- dimensional woodpile PCs consisting of in-plane rod distances ranging from 1000nm to 2000nm are fabricated by focusing femtosecond laser in photosensitive liquid resin ORMOCER. The properties of the PCs are also discussed, and fundamental photonic band gaps in middle-infrared range are measured, whose in-plane rod distances are 1500nm and 2000 nm. Three-dimenslonal woodpile PC devices with desired defects, such as cross-waveguide and micro-laser structures, are introduced easily by TPP. We fabricate the three-dimensional woodpile PCs in the liquid resin at the fast scanning speed of 120μm/s.
文摘NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy levels and possible redox reactions at the NiO_(x)/perovskite interface severely limit the performance of NiO_(x) based inverted perovskite solar cells.Herein,we introduce a p-type self-assembled monolayer between NiO_(x)and perovskite layers to modify the interface and block the undesirable redox reaction between perovskite and NiO_(x)The selfassembled monolayer molecules all contain phosphoric acid function groups,which can be anchored onto the NiOr surface and passivate the surface defect.Moreover,the introduction of self-assembled monolayers can regulate the energy level structure of NiO_(x),reduce the interfacial band energy offset,and hence promote the hole transport from perovskite to NiO_(x)layer.Consequently,the device performance is significantly enhanced in terms of both power conversion efficiency and stability.
基金financial support through a KekuléPh.D.fellowship by the Fonds der Chemischen Industrie(FCI)support from the China Scholarship Council(No.202106950013)。
文摘The parasitic hydrogen evolution reaction(HER)in the negative half-cell of vanadium redox flow batteries(VRFBs)causes severe efficiency losses.Thus,a deeper understanding of this process and the accompanying bubble formation is crucial.This benchmarking study locally analyzes the bubble distribution in thick,porous electrodes for the first time using deep learning-based image segmentation of synchrotron X-ray micro-tomograms.Each large three-dimensional data set was processed precisely in less than one minute while minimizing human errors and pointing out areas of increased HER activity in VRFBs.The study systematically varies the electrode potential and material,concluding that more negative electrode potentials of-200 m V vs.reversible hydrogen electrode(RHE)and lower cause more substantial bubble formation,resulting in bubble fractions of around 15%–20%in carbon felt electrodes.Contrarily,the bubble fractions stay only around 2%in an electrode combining carbon felt and carbon paper.The detected areas with high HER activity,such as the border subregion with more than 30%bubble fraction in carbon felt electrodes,the cutting edges,and preferential spots in the electrode bulk,are potential-independent and suggest that larger electrodes with a higher bulk-to-border ratio might reduce HER-related performance losses.The described combination of electrochemical measurements,local X-ray microtomography,AI-based segmentation,and 3D morphometric analysis is a powerful and novel approach for local bubble analysis in three-dimensional porous electrodes,providing an essential toolkit for a broad community working on bubble-generating electrochemical systems.
基金financially supported by the National Natural Science Foundation of China(Nos.22225108,21971229).
文摘Herein,we report the facile synthesis of a highly strained hexabenzocoronene-containing carbon nanoring,cyclo[4]-paraphenylene[2]-2,11-hexabenzocoronenylene([4,2]CPHBC),as the segment of a[10,10]single-walled carbon nanotube([10,10]SWNT).[4,2]CPHBC was synthesized based on the platinummediated assembly of diborylbiphenyl and diborylhexabenzocoronene,forming a tetranuclear platinum complex,followed by reductive elimination.This nanoring molecule was confirmed by NMR and HRMS,and its photophysical properties were studied using steady-state and time-resolved spectroscopies.Moreover,the selective supramolecular host-vip interaction between[4,2]CPHBC and C_(60) was also investigated.
基金supported by the National Natural Science Foundation of China (21825703, 21927814)the National Key R&D Program of China (2019YFA0405600, 2019YFA0706900, 2021YFA1200104, 2022YFC3400500)+3 种基金the Strategic Priority Research Program of Chinese Academy of Sciences (XDB0540200, XDB37040201)Plans for Major Provincial Science&Technology Projects (202303a07020004)Basic Research Program Based on Major Scientific Infrastructures,CAS (JZHKYPT-2021-05)the Youth Innovation Promotion Association,CAS (2022455)
文摘Bacterial small laccases(SLAC) are promising industrial biocatalysts due to their ability to oxidize a broad range of substrates with exceptional thermostability and tolerance for alkaline p H. Electron transfer between substrate, copper centers, and O2is one of the key steps in the catalytic turnover of SLAC. However, limited research has been conducted on the electron transfer pathway of SLAC and SLAC-catalyzed reactions, hindering further engineering of SLAC to produce tunable biocatalysts for novel applications. Herein, the combinational use of electron paramagnetic resonance(EPR) and ultraviolet-visible(UV-vis) spectroscopic methods coupled with redox titration were employed to monitor the electron transfer processes and obtain further insights into the electron transfer pathway in SLAC. The reduction potentials for type 1 copper(T1Cu), type 2 copper(T2Cu) and type 3copper(T3Cu) were determined to be 367 ± 2 mV, 378 ± 5 m V and 403 ± 2 mV,respectively. Moreover, the reduction potential of a selected substrate of SLAC, hydroquinone(HQ), was determined to be 288 mV using cyclic voltammetry(CV). In this way, an electron transfer pathway was identified based on the reduction potentials. Specifically,electrons are transferred from HQ to T1Cu, then to T2Cu and T3Cu, and finally to O2.Furthermore, superhyperfine splitting observed via EPR during redox titration indicated a modification in the covalency of T2Cu upon electron uptake, suggesting a conformational alteration in the protein environment surrounding the copper sites, which could potentially influence the reduction potential of the copper sites during catalytic processes. The results presented here not only provide a comprehensive method for analyzing the electron transfer pathway in metalloenzymes through reduction potential measurements, but also offer valuable insights for further engineering and directed evolution studies of SLAC in the aim for biotechnological and industrial applications.
基金carried out within the framework of Program 10 “Experimental laboratory astrophysics and geophysics,NCPM.”。
文摘The generation of a plasma with an ultrahigh energy density of 1.2 GJ/cm^(3)(which corresponds to about 12 Gbar pressure) is investigated by irradiating thin stainless-steel foils with high-contrast femtosecond laser pulses with relativistic intensities of up to 10^(22) W/cm^(2).The plasma parameters are determined by X-ray spectroscopy.The results show that most of the laser energy is absorbed by the plasma at solid density,indicating that no pre-plasma is generated in the current experimental setup.
基金supported by the National Natural Sci-ence Foundation of China(22272081),Jiangsu Provincial Specially Appointed Professors Foundation.
文摘Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO_(4))group is introduced to modify the surface of PrBa_(0.5)Ca_(0.5)Co_(2)O_(5)+δ(PBCC).The achieved catalyst(PO_(4)-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO_(4)on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm^(-2).This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.
文摘We report on an experiment performed at the FLASH2 free-electron laser(FEL)aimed at producing warm dense matter via soft x-ray isochoric heating.In the experiment,we focus on study of the ions emitted during the soft x-ray ablation process using time-of-flight electron multipliers and a shifted Maxwell–Boltzmann velocity distribution model.We find that most emitted ions are thermal,but that some impurities chemisorbed on the target surface,such as protons,are accelerated by the electrostatic field created in the plasma by escaped electrons.The morphology of the complex crater structure indicates the presence of several ion groups with varying temperatures.We find that the ion sound velocity is controlled by the ion temperature and show how the ion yield depends on the FEL radiation attenuation length in different materials.
基金Supported by National Basic Research Program of China(Grant No.2011CB013004)National Natural Science Foundation of China(Grant No.51005130)Research Fund of State Key Laboratory of Tribology,Tsinghua University(Grant no.SKLT12B06)
文摘Precision drilling with picosecond laser has been advocated to significantly improve the quality of micro-holes with reduced recast layer thickness and almost no heat affected zone.However,a detailed comparison between nanosecond and picosecond laser drilling techniques has rarely been reported in previous research.In the present study,a series of micro-holes are manufactured on stainless steel 304 using a nanosecond and a picosecond laser drilling system,respectively.The quality of the micro-holes,e.g.,recast layer,micro-crack,circularity,and conicity,etc,is evaluated by employing an optical microscope,an optical interferometer,and a scanning electron microscope.Additionally,the micro-structure of the samples between the edges of the micro-holes and the parent material is compared following etching treatment.The researching results show that a great amount of spattering material accumulated at the entrance ends of the nanosecond laser drilled micro-holes.The formation of a recast layer with a thickness of;5μm is detected on the side walls,associated with initiation of micro-cracks.Tapering phenomenon is also observed and the circularity of the micro-holes is rather poor.With regard to the micro-holes drilled by picosecond laser,the entrance ends,the exit ends,and the side walls are quite smooth without accumulation of spattering material,formation of recast layer and micro-cracks.The circularity of the micro-holes is fairly good without observation of tapering phenomenon.Furthermore,there is no obvious difference as for the micro-structure between the edges of the micro-holes and the parent material.This study proposes a picosecond laser helical drilling technique which can be used for effective manufacturing of high quality micro-holes.
文摘Multi-walled carbon nanotubes （MWCNTs） are grown by arc discharge method in a controlled methane environment. The arc discharge is produced between two graphite electrodes at the ambient pressures of 100 tort, 300 torr, and 500 torr. Arc plasma parameters such as temperature and density are estimated to investigate the influences of the ambient pressure and the contributions of the ambient pressure to the growth and the structure of the nanotubes. The plasma temperature and density are observed to increase with the increase in the methane ambient pressure. The samples of MWCNT synthesized at different ambient pressures are analyzed using transmission electron microscopy, scanning electron microscopy, Raman spectroscopy, Fourier transform infrared spectroscopy, and X-ray diffraction. An increase in the growth of MWCNT and a decrease in the inner tube diameter are observed with the increase in the methane ambient pressure.
基金Project(50435030) supported by the National Natural Science foundation of ChinaProject supported by the Program for New Century Excellent Talents in Chinese University Project(GZ080010) supported by the Open Research Fund Program of Jiangsu Province Key Laboratory for Photon Manufacturing Science and Technology
文摘Twelve samples with periodic array square pillars microstructure were prepared on the silicon wafer by plasma etching techniques, on which space b of the square pillars increased from 5 to 60 μm. In order to study the effect ofb on the wettability of the rough surface, the effects of apparent contact angle （CA） and sliding angle （a） of the droplet on the rough surface were measured with the contact angle meter. The results show that the experimental values of CA well agree with the classical wetting theory and a decreases with the increase of b. Two drop shapes exist on the samples＇ surface, corresponding to the Cassie state and the Wenzel state respectively. The contact state in which a drop would settle depends typically on the size of b. On the role of gravitation, the irreversible transition of a drop from Cassie state to Wenzel state should occur at a certain space of the square pillars. Since the transition has implications on the application of super-hydrophobic rough surfaces, theoretically, the prediction of wetting state transition on square pillar array micro-structured surfaces provides an intuitionistic guidance for the design of steady superhydrophobic surfaces.
基金supported by the National Key Research and Development Program of China (2017YFA0402800)National Natural Science Foundation of China (51925206,U1932214)+2 种基金Collaborative Innovation Program of Hefei Science Center (2020HSC-CIP004)the National Key Research and Development Program of China(2017YFA0206600)the National Natural Science Foundation of China (51773045, 21772030, 51922032, 21961160720)for financial support。
文摘Organic–inorganic hybrid perovskite materials demonstrate promising applications in high-efficiency perovskite solar cells (PSCs) with a certified power conversion efficiency(PCE) of 25.5%(https://www.nrel.gov/pv/cell-efficiency.html).
基金supported by the Science Foundation of the Ministry of Science and Technology Malaysiathe Islamic Development Bank Jeddahsupport of the Universiti Teknologi Malaysia for this research work
文摘This study deals with Nd：YAG laser cutting nonmetallic materials, which is one of the most important and popular industrial applications of laser. The main theme is to evaluate the effects of Nd：YAG laser beam power besides work piece scanning speed. For approximate cutting depth, a theoretical study is conducted in terms of material property and cutting speed. Results show a nonlinear relation between the cutting depth and input energy. There is no significant effect of speed on cutting depth with the speed being larger than 30 mm/s. An extra energy is utilized in the deep cutting. It is inferred that as the laser power increases, cutting depth increases. The experimental outcomes are in good agreement with theoretical results. This analysis will provide a guideline for laser-based industry to select a suitable laser for cutting, scribing, trimming, engraving, and marking nonmetallic materials.
