In the application of polymer gels to profile control and water shutoff,the gelation time will directly determine whether the gel can"go further"in the formation,but the most of the methods for delaying gel ...In the application of polymer gels to profile control and water shutoff,the gelation time will directly determine whether the gel can"go further"in the formation,but the most of the methods for delaying gel gelation time are complicated or have low responsiveness.There is an urgent need for an effective method for delaying gel gelation time with intelligent response.Inspired by the slow-release effect of drug capsules,this paper uses the self-assembly effect of gas-phase hydrophobic SiO_(2) in aqueous solution as a capsule to prepare an intelligent responsive self-assembled micro-nanocapsules.The capsule slowly releases the cross-linking agent under the stimulation of external conditions such as temperature and pH value,thus delaying gel gelation time.When the pH value is 2 and the concentration of gas-phase hydrophobic SiO_(2) particles is 10%,the gelation time of the capsule gel system at 30,60,90,and 120℃is12.5,13.2,15.2,and 21.1 times longer than that of the gel system without containing capsule,respectively.Compared with other methods,the yield stress of the gel without containing capsules was 78 Pa,and the yield stress after the addition of capsules was 322 Pa.The intelligent responsive self-assembled micronanocapsules prepared by gas-phase hydrophobic silica nanoparticles can not only delay the gel gelation time,but also increase the gel strength.The slow release of cross-linking agent from capsule provides an effective method for prolongating the gelation time of polymer gels.展开更多
Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited b...Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited by excessive defects and poor carrier transport at the perovskite-electrode interface,particularly at the buried interface between the perovskite and transparent conductive oxide(TCO).Recent efforts in the perovskite community have focused on designing novel self-assembled molecules(SAMs)to improve the quality of the buried interface.However,a notable gap remains in understanding the regulation of atomic-scale interfacial properties of SAMs between the perovskite and TCO interfaces.This understanding is crucial,particularly in terms of identifying chemically active anchoring groups.In this study,we used the star SAM([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)as the base structure to investigate the defect passivation effects of eight common anchoring groups at the perovskite-TCO interface.Our findings indicate that the phosphonic and boric acid groups exhibit notable advantages.These groups fulfill three key criteria:they provide the greatest potential for defect passivation,exhibit stable adsorption with defects,and exert significant regulatory effects on interface dipoles.Ionized anchoring groups exhibit enhanced passivation capabilities for defect energy levels due to their superior Lewis base properties,which effectively neutralize local charges near defects.Among various defect types,iodine vacancies are the easiest to passivate,whereas iodine-substituted lead defects are the most challenging to passivate.Our study provides comprehensive theoretical insights and inspiration for the design of anchoring groups in SAMs,contributing to the ongoing development of more efficient inverted perovskite solar cells.展开更多
The hydroxyl-terminated self-assembled monolayer(OH-SAM),as a surface resistant to protein adsorption,exhibits substantial potential in applications such as ship navigation and medical implants,and the appropriate str...The hydroxyl-terminated self-assembled monolayer(OH-SAM),as a surface resistant to protein adsorption,exhibits substantial potential in applications such as ship navigation and medical implants,and the appropriate strategies for designing anti-fouling surfaces are crucial.Here,we employ molecular dynamics simulations and alchemical free energy calculations to systematically analyze the factors influencing resistance to protein adsorption on the SAMs terminated with single or double OH groups at three packing densities(∑=2.0 nm^(-2),4.5 nm^(-2),and 6.5 nm^(-2)),respectively.For the first time,we observed that the compactness and order of interfacial water enhance its physical barrier effect,subsequently enhancing the resistance of SAM to protein adsorption.Notably,the spatial hindrance effect of SAM leads to the embedding of protein into SAM,resulting in a lack of resistance of SAM towards protein.Furthermore,the number of hydroxyl groups per unit area of double OH-terminated SAM at ∑=6.5 nm^(-2) is approximately 2 to 3 times that of single OH-terminated SAM at ∑=6.5 nm^(-2) and 4.5 nm^(-2),consequently yielding a weaker resistance of double OH-terminated SAM towards protein.Meanwhile,due to the structure of SAM itself,i.e.,the formation of a nearly perfect ice-like hydrogen bond structure,the SAM exhibits the weakest resistance towards protein.This study will complement and improve the mechanism of OH-SAM resistance to protein adsorption,especially the traditional barrier effect of interfacial water.展开更多
Light confinement induced by spontaneous near-surface resonance is inherently determined by the location and geometry of metallic nanostructures(NSs),offering a facile and effective approach to break through the limit...Light confinement induced by spontaneous near-surface resonance is inherently determined by the location and geometry of metallic nanostructures(NSs),offering a facile and effective approach to break through the limitation of the light-mater interaction within the photoactive layers.Here,we demonstrate high-performance Al NS/ZnO quantum dots(Al/ZnO) heterostructure UV photodetectors with controllable morphologies of the self-assembled Al NSs.The Al/ZnO heterostructures exhibit a superior light utilization than the ZnO/Al heterostructures,and a strong morphological dependence of the Al NSs on the optical properties of the heterostructures.The inter-diffusion of Al atoms into ZnO matrixes is of a great benefit for the carrier transportation.Consequently,the optimal photocurrent of the Al/ZnO heterostructure photodetectors is significantly increased by 275 times to ~1.065 mA compared to that of the pristine ZnO device,and an outstanding photoresponsivity of 11.98 A W-1 is correspondingly achieved under 6.9 MW cm-2 UV light illumination at 10 V bias.In addition,a relatively fast response is similarly witnessed with the Al/ZnO devices,paving a path to fabricate the high-performance UV photodetectors for applications.展开更多
Self-assembled molecules(SAMs) have shown great potential in replacing bulk charge selective contact layers in high-performance perovskite solar cells(PSCs) due to their low material consumption and simple processing....Self-assembled molecules(SAMs) have shown great potential in replacing bulk charge selective contact layers in high-performance perovskite solar cells(PSCs) due to their low material consumption and simple processing. Herein, we design and synthesize a series of donor-acceptor(D-A) type SAMs(MPA-BTCA, MPA-BT-BA, and MPA-BT-RA, where MPA is 4-methoxy-N-(4-methoxyphenyl)-N-phenylaniline;BT is benzo[c][1,2,5]-thiadiazole;CA is 2-cyanoacrylic acid, BA is benzoic acid, RA is rhodanine-3-propionic acid) with distinct anchoring groups, which show dramatically different properties. MPA-BTCA with CA anchoring groups exhibited stronger dipole moments and formed a homogeneous monolayer on the indium tin oxide(ITO) surface by adopting an upstanding self-assembling mode. However, the MPA-BT-RA molecules tend to aggregate severely in solid state due to the sp~3 hybridization of the carbon atom on the RA group, which is not favorable for achieving a long-range ordered self-assembled layer.Consequently, benefiting from high dipole moment, as well as dense and uniform self-assembled film,the device based on MPA-BT-CA yielded a remarkable power conversion efficiency(PCE) of 21.81%.Encouragingly, an impressive PCE approaching 20% can still be obtained for the MPA-BT-CA-based PSCs as the device area is increased to 0.80 cm^(2). Our work sheds light on the design principles for developing hole selecting SAMs, which will pave a way for realizing highly efficient, flexible, and large-area PSCs.展开更多
By three-dimensional kinetic Monte Carlo simulations, the effects of the temperature, the flux rate, the total coverage and the interruption time on the distribution and the number of self-assembled InAs/GaAs （001） ...By three-dimensional kinetic Monte Carlo simulations, the effects of the temperature, the flux rate, the total coverage and the interruption time on the distribution and the number of self-assembled InAs/GaAs （001） quantum dot （QD） islands are studied, which shows that a higher temperature, a lower flux rate and a longer growth time correspond to a better island distribution. The relations between the number of islands and the temperature and the flux rate are also successfully simulated. It is observed that for the total coverage lower than 0.5 ML, the number of islands decreases with the temperature increasing and other growth parameters fixed and the number of islands increases with the flux rate increasing when the deposition is lower than 0.6 ML and the other parameters are fixed.展开更多
By using semiclassical theory combined with multiple-scale method, we analytically study the linear absorption and the nonlinear dynamical properties in a lifetime broadened Λ-type three-level self-assembled quantum ...By using semiclassical theory combined with multiple-scale method, we analytically study the linear absorption and the nonlinear dynamical properties in a lifetime broadened Λ-type three-level self-assembled quantum dots. It is found that this system can exhibit the transparency, and the width of the transparency window becomes wider with the increase of control light field. Interestingly, a weak probe light beam can form spatial weak-light dark solitons. When it propagates along the axial direction, the soliton will transform into a steady spatial weak-light ring dark soltion. In addition, the stability of two-dimensional spatial optical solitons is testified numerically.展开更多
This work details a study based on HfS_(2 )transistors utilizing an n-octadecylphosphonic acid-based self-assembled monolayer(SAM)as the gate dielectric.The fabrication of the SAM-based two-dimensional(2D)material tra...This work details a study based on HfS_(2 )transistors utilizing an n-octadecylphosphonic acid-based self-assembled monolayer(SAM)as the gate dielectric.The fabrication of the SAM-based two-dimensional(2D)material transistor is simple and can be used to improve the quality of the interface of air-sensitive 2D materials.In comparison to HfS_(2) transistors utilizing a conventional Al_2O_(3) gate insulator by atomic layer deposition,HfS_(2) transistors utilizing an SAM as the gate dielectric can reduce the operation region from 4 V to 2 V,enhance the field-effect mobility from 0.03 cm^2/Vs to 0.75 cm^2/Vs,improve the sub-threshold swing from 404 m V/dec to 156 m V/dec,and optimize the hysteresis to 0.03 V,thus demonstrating improved quality of the semiconductor/insulator interface.展开更多
We present a self-assembly method to prepare array nano-wires of colloidal CdSe quantum dots on a substrate of porous Al2 O3 film modified by gold nanoparticles. The photoluminescence(PL) spectra of nanowires are in s...We present a self-assembly method to prepare array nano-wires of colloidal CdSe quantum dots on a substrate of porous Al2 O3 film modified by gold nanoparticles. The photoluminescence(PL) spectra of nanowires are in situ measured by using a scanning near-field optical microscopy(SNOM) probe tip with 100-nm aperture on the scanning near-field optical microscope. The results show that the binding sites from the edge of porous Al2 O3 nanopores are combined with the carboxyl of CdSe quantum dots’ surface to form an array of CdSe nanowires in the process of losing background solvent because of the gold nanoparticles filling the nano-holes of porous Al2 O3 film. Compared with the area of nonself-assembled nano-wire, the fluorescence on the Al2 O3/Au/CdSe interface is significantly enhanced in the self-assembly nano-wire regions due to the electron transfer conductor effect of the gold nanoparticles’ surface. In addition, its full width at half maximum(FWHM) is also obviously widened. The method of enhancing fluorescence and energy transfer can widely be applied to photodetector, photocatalysis, optical display, optical sensing, and biomedical imaging, and so on.展开更多
Here we report the thermo-controllable self-assembled structures of single-layer 4, 4＇＇-diamino-p-terphenyl（DAT）molecules on Au（110）, which are investigated by scanning tunneling microscopy（STM） combined with ...Here we report the thermo-controllable self-assembled structures of single-layer 4, 4＇＇-diamino-p-terphenyl（DAT）molecules on Au（110）, which are investigated by scanning tunneling microscopy（STM） combined with density functional theory（DFT） based calculations. With the deposition of monolayer DAT molecules on Au（110） and subsequent annealing at 100℃, all DAT molecules adsorb on a（1×5） reconstructed surface with a ladder-like structure. After annealing the sample at about 200℃, STM images show three distinct domains, including DAT molecules on a（1×3） reconstructed surface, dehydrogenated molecules with two hydrogen atoms detached from one amino group（–2H-DAT） on a（1×5）reconstructed surface and dehydrogenated molecules with four hydrogen atoms detached from two amino groups（–4HDAT） on a（1×3） reconstructed surface through N–Au bonds. Furthermore, after annealing the sample to 350℃, STM image shows only one self-assembled structure with –4H-DAT molecules on a（1×3） reconstructed surface. Relative STM simulations of different self-assembled structures show excellent agreements with the experimental STM images at different annealing temperatures. Further DFT calculations on the dehydrogenation process of DAT molecule prove that the dehydrogenation barrier on a（1×5） reconstructed surface is lower than that on（1×3） one, which demonstrate the experimental results that the formation temperature of a（1×3） reconstructed surface is higher than that of a（1×5） one.展开更多
Forming a monolayer of mixed nickel and gold nanoparticles through self-assembly via simple solution processing constitutes an important step toward inexpensive nanoparticle-based carbon nanofiber growth.In this work,...Forming a monolayer of mixed nickel and gold nanoparticles through self-assembly via simple solution processing constitutes an important step toward inexpensive nanoparticle-based carbon nanofiber growth.In this work,mixed gold and nickel nanoparticles were anchored on the silicon wafer using self-assembled monolayers(SAMs)as a template.SAMs of 3-mercaptopropyl trimethoxysilane(MPTS-SAMs)were formed on silicon wafer,with the exposed thiol functionality providing ligand exchange sites to form the mixed monolayer of nickel and gold nanoparticles via a two-step sequential soaking approach.The densities of the nickel and gold nanoparticles on the surface can be varied by adjusting the soaking sequence.展开更多
The morphology of the copper iodide （CuI） film as an inorganic p-type material has an important influence on enhancing the performance of polymer solar cells （PSCs）. A self-assembled monolayer of 3-aminopropanoic ...The morphology of the copper iodide （CuI） film as an inorganic p-type material has an important influence on enhancing the performance of polymer solar cells （PSCs）. A self-assembled monolayer of 3-aminopropanoic acid （C3-SAM） was used on the surface of indium tin oxide （ITO） before depositing the CuI films. Consequently, a well-distributed and smooth CuI film was formed with pinhole free and complete surface coverage. The root mean square of the corresponding CuI film was reduced from 3.63 nm for ITO/CuI to 0.77 nm. As a result, the average power conversion efficiency （PCE） of PSCs with the device structure of ITO/C3-SAM/CuI/P3HT：PC61BM/ZnO/Al increased significantly from 2.55% （best 2.66%） to 3.04% （best 3.20%） after C3-SAM treatment. This work provides an effective strategy to control the morphology of CuI films through interracial modification and promotes its application in efficient PSCs.展开更多
Measuring the growth parameters of Ge quantum dots （QDs） embedded in SiO2/Si hetero-structure is pre- requisite for developing the optoelectronic devices such as photovoltaics and sensors. Their optical properties c...Measuring the growth parameters of Ge quantum dots （QDs） embedded in SiO2/Si hetero-structure is pre- requisite for developing the optoelectronic devices such as photovoltaics and sensors. Their optical properties can be tuned by tailoring the growth morphology and structures, where the growth parameters＇ optimizations still need to be explored. We determine the effect of annealing temperature on surface morphology, structures and optical properties of Ge//SiO2//Si hetero-structure. Samples are grown via rf magnetron sputtering and subsequent characterizations are made using imaging and spectroscopic techniques.展开更多
Recent progress of the preparation and applications of superparamagnetic iron oxide（SPIO） clusters as magnetic resonance imaging（MRI） probes is reviewed with regard to their applications in labeling and tracking c...Recent progress of the preparation and applications of superparamagnetic iron oxide（SPIO） clusters as magnetic resonance imaging（MRI） probes is reviewed with regard to their applications in labeling and tracking cells in vivo, in diagnosis of cardiovascular diseases and tumors, and in drug delivery systems. Magnetic nanoparticles（NPs）, especially SPIO nanoparticles, have long been used as MRI contrast agents and as an advantageous nanoplatform for drug delivery,taking advantage of their unique magnetic properties and ability to function at the molecular and cellular levels. Due to advances in nanotechnology, various means to control SPIO NPs＇ size, composition, magnetization and relaxivity have been developed, as well as ways to usefully modify their surface. Recently, self-assembly of SPIO NP clusters in particulate carriers — such as polymeric micelles, vesicles, liposomes, and layer-by-layer（Lb L） capsules — have been widely studied for application as ultrasensitive MRI probes, owing to their remarkably high spin–spin（T2） relaxivity and convenience for further functionalization.展开更多
Affibody molecules are small nonimmunoglobulin affinity proteins,which can precisely target to some cancer cells with specific overexpressed molecular signatures.However,the relatively short in vivo half-life of them ...Affibody molecules are small nonimmunoglobulin affinity proteins,which can precisely target to some cancer cells with specific overexpressed molecular signatures.However,the relatively short in vivo half-life of them seriously limited their application in drug targeted delivery for cancer therapy.Here an amphiphilic affibody-drug conjugate is self-assembled into nanomicelles to prolong circulation time for targeted cancer therapy.As an example of the concept,the nanoagent was prepared through molecular self-assembly of the amphiphilic conjugate of Z_(HHR2:342)-Cys with auristatin E derivate,where the affibody used is capable of binding to the human epidermal growth factor receptor 2(HER2).Such a nanodrug not only increased the blood circulation time,but also enhanced the tumor targeting capacity(abundant affibody arms on the nanoagent surface) and the drug accumulation in tumor.As a result,this affibody-based nanoagent showed excellent antitumor activity in vivo to HER2-positive ovary and breast tumor models,which nearly eradicated both small solid tumors(about 100 mm^(3)) and large established tumors(exceed 500 mm^(3)).The relative tumor proliferation inhibition ratio reaches 99.8% for both models.展开更多
Arrays of noble metal nanoparticles show potential applications in （bio-）sensing, optical storage, surface-enhanced spectroscopy, and waveguides. For all such potential devices, controlling the size, morphology, and...Arrays of noble metal nanoparticles show potential applications in （bio-）sensing, optical storage, surface-enhanced spectroscopy, and waveguides. For all such potential devices, controlling the size, morphology, and interparticle spacing of the nanoparticles is very important. Here, we combine seed-mediated growth with nanosphere lithography to study the controllable growth of gold nanoparticles （Au NPs）, in which the self-assembly monolayer of polystyrene （PS） on a silicon surface is used to guide the modification of allaunesilanes and the subsequent adsorption of gold seeds; seed-mediated growth is applied to controlling the morphology and size of Au NPs. The size of adsorption region （determining the number of adsorbed gold seeds） is controlled by etching PS microspheres with oxygen plasma or annealing PS microspheres at the glass transition temperature. The size and morphology of the Au NPs are controlled by changing growth conditions. In such a way, we have achieved the dual control of the obtained Au NPs. Preliminary results show that this strategy holds a great promise. This approach can also be extended to a wide range of materials and substrates.展开更多
In this paper, core–shell quantum dots(QDs) with two polar surface functional groups(ZnSe/ZnS–COOH QDs and ZnSe/ZnS–NH_2 QDs) are synthesized in an aqueous phase. Photoluminescence(PL) and absorption spectra clearl...In this paper, core–shell quantum dots(QDs) with two polar surface functional groups(ZnSe/ZnS–COOH QDs and ZnSe/ZnS–NH_2 QDs) are synthesized in an aqueous phase. Photoluminescence(PL) and absorption spectra clearly indicate luminescence down-shifting(LDS) properties. On the basis of QDs, surface functional group multilayer LDS films(MLDSs) are fabricated through an electrostatic layer-by-layer(LBL) self-assembly method. The PL intensity increases linearly with the number of bilayers, showing a regular and uniform film growth. When the M-LDS is placed on the surface of a Si-based solar cell as an optical conversion layer for the first time, the external quantum efficiency(EQE) and shortcircuit current density(Jsc) notably increases for the LDS process. The EQE response improves in a wavelength region extending from the UV region to the blue region, and its maximum increase reaches more than 15% between 350 nm and 460 nm.展开更多
Generating sufficient strains on metal surfaces are highly challenging owing to that most metals can deform plastically to relax the strains on the surfaces.In this work,we developed a facile but highly efficient stac...Generating sufficient strains on metal surfaces are highly challenging owing to that most metals can deform plastically to relax the strains on the surfaces.In this work,we developed a facile but highly efficient stacked deposition strategy to in situ activation and reconstruction of NiO/NiOOH on Ni matrix,following with the migration of Fe ions to NiOOH.The Fe sites on the Ni/NiO/NiOOH facilitate the formation of the stable*OH oxygenated intermediates,and the Ni matrix in the catalyst provides the catalyst excellent stability.The oxygen evolution reaction(OER)performance of the stacked NiFe-5 with compressive strain displays the strengthened binding to oxygenated intermediates and superior OER activity,the ultralow overpotentials of 162 versus reversible hydrogen electrode at 10 mA cm^(-2).On the other hand,the Ni-5 without the incorporation of Fe has shown an outstanding hydrogen evolution reaction(HER)activity,affording an overpotential of 47 mV at 10 mA cm^(-2).The NiFe-5‖Ni-5 enables the overall water splitting at a voltage of 1.508 V to achieve 20 mA cm^(-2) with remarkable durability.The stacked deposition strategy improves binding strength of Ni-based catalysts to oxygenated intermediates via generating compressive strain,causing high catalytic activities on OER and HER.展开更多
Hydrophobic nanochannel plays a significant role in many physical, biological, and geological phenomena and ex- hibits impressive applications due to both its ubiquitous distribution and great ability to transport hyd...Hydrophobic nanochannel plays a significant role in many physical, biological, and geological phenomena and ex- hibits impressive applications due to both its ubiquitous distribution and great ability to transport hydrophobic molecules, including various oils and gases. Based on theoretical modeling, we herein reveal that the amphipathic Janus nanoparticles have a large probability to self-assemble into uninterrupted hydrophobic nanochannels inside the aqueous nano-space, al- though there are large portions of the Janus nanoparticles to be hydrophilic. The key to this observation is the attractions between the hydrophobic regimes on neighboring amphipathic Janus particles through hydrophobic interaction in aqueous nano-space. More surprisingly, the permeation efficiency of hydrophobic molecules through the uninterrupted hydrophobic channel in Janus particles aggregate is even higher than that in the aggregate of hydrophobic particles. We note that the proposed amphipathic Janus particles can be transported to the appropriate positions by the water since the hydrophilic regimes still remain a strong particle-water interaction. We also note that most natural subsurface rocks are not completely hydrophobic or hydrophilic but have complex surfaces with inhomogeneous wetting property. Our work therefore provides a detailed molecular level understanding of the formation of underground strata as well as the new insight for constructing the artificial hydrophobic channels for various applications, such as the design of proppants to enhance the recovery of the unconventional oil/gas.展开更多
The interactions between lignin oligomers and solvents determine the behaviors of lignin oligomers self-assembling into uniform lignin nanoparticles(LNPs).Herein,several alcohol solvents,which readily interact with th...The interactions between lignin oligomers and solvents determine the behaviors of lignin oligomers self-assembling into uniform lignin nanoparticles(LNPs).Herein,several alcohol solvents,which readily interact with the lignin oligomers,were adopted to study their effects during solvent shifting process for LNPs’production.The lignin oligomers with widely distributed molecular weight and abundant guaiacyl units were extracted from wood waste(mainly consists of pine wood),exerting outstanding self-assembly capability.Uniform and spherical LNPs were generated in H_(2)O-n-propanol cosolvent,whereas irregular LNPs were obtained in H_(2)O-methanol cosolvent.The unsatisfactory self-assembly performance of the lignin oligomers in H_(2)O-methanol cosolvent could be attributed to two aspects.On one hand,for the initial dissolution state,the distinguishing Hansen solubility parameter and polarity between methanol solvent and lignin oligomers resulted in the poor dispersion of the lignin oligomers.On the other hand,strong hydrogen bonds between methanol solvent and lignin oligomers during solvent shifting process,hindered the interactions among the lignin oligomers for self-assembly.展开更多
基金support and funding from the National Natural Science Foundation of China (No.52174047)Sinopec Project (No.P21063-3)。
文摘In the application of polymer gels to profile control and water shutoff,the gelation time will directly determine whether the gel can"go further"in the formation,but the most of the methods for delaying gel gelation time are complicated or have low responsiveness.There is an urgent need for an effective method for delaying gel gelation time with intelligent response.Inspired by the slow-release effect of drug capsules,this paper uses the self-assembly effect of gas-phase hydrophobic SiO_(2) in aqueous solution as a capsule to prepare an intelligent responsive self-assembled micro-nanocapsules.The capsule slowly releases the cross-linking agent under the stimulation of external conditions such as temperature and pH value,thus delaying gel gelation time.When the pH value is 2 and the concentration of gas-phase hydrophobic SiO_(2) particles is 10%,the gelation time of the capsule gel system at 30,60,90,and 120℃is12.5,13.2,15.2,and 21.1 times longer than that of the gel system without containing capsule,respectively.Compared with other methods,the yield stress of the gel without containing capsules was 78 Pa,and the yield stress after the addition of capsules was 322 Pa.The intelligent responsive self-assembled micronanocapsules prepared by gas-phase hydrophobic silica nanoparticles can not only delay the gel gelation time,but also increase the gel strength.The slow release of cross-linking agent from capsule provides an effective method for prolongating the gelation time of polymer gels.
基金supported by the National Natural Science Foundation of China(Grant Nos.62321166653,22090044,and 12350410372).Calculations were performed in part at the high-performance computing center of Jilin University.
文摘Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited by excessive defects and poor carrier transport at the perovskite-electrode interface,particularly at the buried interface between the perovskite and transparent conductive oxide(TCO).Recent efforts in the perovskite community have focused on designing novel self-assembled molecules(SAMs)to improve the quality of the buried interface.However,a notable gap remains in understanding the regulation of atomic-scale interfacial properties of SAMs between the perovskite and TCO interfaces.This understanding is crucial,particularly in terms of identifying chemically active anchoring groups.In this study,we used the star SAM([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)as the base structure to investigate the defect passivation effects of eight common anchoring groups at the perovskite-TCO interface.Our findings indicate that the phosphonic and boric acid groups exhibit notable advantages.These groups fulfill three key criteria:they provide the greatest potential for defect passivation,exhibit stable adsorption with defects,and exert significant regulatory effects on interface dipoles.Ionized anchoring groups exhibit enhanced passivation capabilities for defect energy levels due to their superior Lewis base properties,which effectively neutralize local charges near defects.Among various defect types,iodine vacancies are the easiest to passivate,whereas iodine-substituted lead defects are the most challenging to passivate.Our study provides comprehensive theoretical insights and inspiration for the design of anchoring groups in SAMs,contributing to the ongoing development of more efficient inverted perovskite solar cells.
基金Project supported by the National Natural Science Foundation of China (Grants No. 12075201)the Science and Technology Planning Project of Jiangsu Province, China (Grant No. BK20201428)+1 种基金the Postgraduate Research & Practice Innovation Program of Jiangsu Province, China (Grant No. KYCX21 3193)the Special Program for Applied Research on Supercomputation of the NSFC–Guangdong Joint Fund (the second phase)。
文摘The hydroxyl-terminated self-assembled monolayer(OH-SAM),as a surface resistant to protein adsorption,exhibits substantial potential in applications such as ship navigation and medical implants,and the appropriate strategies for designing anti-fouling surfaces are crucial.Here,we employ molecular dynamics simulations and alchemical free energy calculations to systematically analyze the factors influencing resistance to protein adsorption on the SAMs terminated with single or double OH groups at three packing densities(∑=2.0 nm^(-2),4.5 nm^(-2),and 6.5 nm^(-2)),respectively.For the first time,we observed that the compactness and order of interfacial water enhance its physical barrier effect,subsequently enhancing the resistance of SAM to protein adsorption.Notably,the spatial hindrance effect of SAM leads to the embedding of protein into SAM,resulting in a lack of resistance of SAM towards protein.Furthermore,the number of hydroxyl groups per unit area of double OH-terminated SAM at ∑=6.5 nm^(-2) is approximately 2 to 3 times that of single OH-terminated SAM at ∑=6.5 nm^(-2) and 4.5 nm^(-2),consequently yielding a weaker resistance of double OH-terminated SAM towards protein.Meanwhile,due to the structure of SAM itself,i.e.,the formation of a nearly perfect ice-like hydrogen bond structure,the SAM exhibits the weakest resistance towards protein.This study will complement and improve the mechanism of OH-SAM resistance to protein adsorption,especially the traditional barrier effect of interfacial water.
基金the National Natural Science Foundation of China(Grant Nos.61705070 and 61974052)China Postdoctoral Science Foundation(Grant Nos.2019M662594)National Research Foundation of Korea(NRF)Grant funded by the Korean Government(MSIP)(Nos.NRF2019R1A2C4069438 and NRF2018R1A6A1A03025242)。
文摘Light confinement induced by spontaneous near-surface resonance is inherently determined by the location and geometry of metallic nanostructures(NSs),offering a facile and effective approach to break through the limitation of the light-mater interaction within the photoactive layers.Here,we demonstrate high-performance Al NS/ZnO quantum dots(Al/ZnO) heterostructure UV photodetectors with controllable morphologies of the self-assembled Al NSs.The Al/ZnO heterostructures exhibit a superior light utilization than the ZnO/Al heterostructures,and a strong morphological dependence of the Al NSs on the optical properties of the heterostructures.The inter-diffusion of Al atoms into ZnO matrixes is of a great benefit for the carrier transportation.Consequently,the optimal photocurrent of the Al/ZnO heterostructure photodetectors is significantly increased by 275 times to ~1.065 mA compared to that of the pristine ZnO device,and an outstanding photoresponsivity of 11.98 A W-1 is correspondingly achieved under 6.9 MW cm-2 UV light illumination at 10 V bias.In addition,a relatively fast response is similarly witnessed with the Al/ZnO devices,paving a path to fabricate the high-performance UV photodetectors for applications.
基金financial support from the National Natural Science Foundation of China (NSFC)(21805128)the National Natural Science Foundation of China (21774055)+3 种基金the financial support from the National Natural Science Foundation of China(21975260)the Shenzhen Science and Technology Innovation Commission(JCYJ20180504165709042)financial support of Guangdong Provincial Key Laboratory Program(2021B1212040001) from the Department of Science and Technology of Guangdong Provincethe NSFC-CNR exchange program of NSFC(22011530391)。
文摘Self-assembled molecules(SAMs) have shown great potential in replacing bulk charge selective contact layers in high-performance perovskite solar cells(PSCs) due to their low material consumption and simple processing. Herein, we design and synthesize a series of donor-acceptor(D-A) type SAMs(MPA-BTCA, MPA-BT-BA, and MPA-BT-RA, where MPA is 4-methoxy-N-(4-methoxyphenyl)-N-phenylaniline;BT is benzo[c][1,2,5]-thiadiazole;CA is 2-cyanoacrylic acid, BA is benzoic acid, RA is rhodanine-3-propionic acid) with distinct anchoring groups, which show dramatically different properties. MPA-BTCA with CA anchoring groups exhibited stronger dipole moments and formed a homogeneous monolayer on the indium tin oxide(ITO) surface by adopting an upstanding self-assembling mode. However, the MPA-BT-RA molecules tend to aggregate severely in solid state due to the sp~3 hybridization of the carbon atom on the RA group, which is not favorable for achieving a long-range ordered self-assembled layer.Consequently, benefiting from high dipole moment, as well as dense and uniform self-assembled film,the device based on MPA-BT-CA yielded a remarkable power conversion efficiency(PCE) of 21.81%.Encouragingly, an impressive PCE approaching 20% can still be obtained for the MPA-BT-CA-based PSCs as the device area is increased to 0.80 cm^(2). Our work sheds light on the design principles for developing hole selecting SAMs, which will pave a way for realizing highly efficient, flexible, and large-area PSCs.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.60908028,60971068,and 10979065)the Fundamental Research Funds for the Central Universities,China(Grant No.2011RC0402)the Program for New Century Excellent Talents in University,China(Grant No.NCET-10-0261)
文摘By three-dimensional kinetic Monte Carlo simulations, the effects of the temperature, the flux rate, the total coverage and the interruption time on the distribution and the number of self-assembled InAs/GaAs （001） quantum dot （QD） islands are studied, which shows that a higher temperature, a lower flux rate and a longer growth time correspond to a better island distribution. The relations between the number of islands and the temperature and the flux rate are also successfully simulated. It is observed that for the total coverage lower than 0.5 ML, the number of islands decreases with the temperature increasing and other growth parameters fixed and the number of islands increases with the flux rate increasing when the deposition is lower than 0.6 ML and the other parameters are fixed.
基金Project supported by the Special Funds of the National Natural Science Foundation of China(Grant No.11247313)
文摘By using semiclassical theory combined with multiple-scale method, we analytically study the linear absorption and the nonlinear dynamical properties in a lifetime broadened Λ-type three-level self-assembled quantum dots. It is found that this system can exhibit the transparency, and the width of the transparency window becomes wider with the increase of control light field. Interestingly, a weak probe light beam can form spatial weak-light dark solitons. When it propagates along the axial direction, the soliton will transform into a steady spatial weak-light ring dark soltion. In addition, the stability of two-dimensional spatial optical solitons is testified numerically.
基金Supported by the Japan Society for the Promotion of Science under Grant No JP25107004
文摘This work details a study based on HfS_(2 )transistors utilizing an n-octadecylphosphonic acid-based self-assembled monolayer(SAM)as the gate dielectric.The fabrication of the SAM-based two-dimensional(2D)material transistor is simple and can be used to improve the quality of the interface of air-sensitive 2D materials.In comparison to HfS_(2) transistors utilizing a conventional Al_2O_(3) gate insulator by atomic layer deposition,HfS_(2) transistors utilizing an SAM as the gate dielectric can reduce the operation region from 4 V to 2 V,enhance the field-effect mobility from 0.03 cm^2/Vs to 0.75 cm^2/Vs,improve the sub-threshold swing from 404 m V/dec to 156 m V/dec,and optimize the hysteresis to 0.03 V,thus demonstrating improved quality of the semiconductor/insulator interface.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.61741505 and 61865002)the Guizhou Provincial Science and Technology Support Plan,China(Grant No QKHZ [2017]2887)+3 种基金the Guiding Local Science and Technology Development Plan of the Central Government of China(Grant No.QKZYD [2017]4004)the Guizhou Province Education and Teaching Reform for Graduate Student(Grant No.QJYH-JG [2016]15)the Guizhou University Introduces Talent Projects,China(Grant No.2016002)the Talents of Guizhou Municipal Science and Technology Cooperation Platform,China(Grant No.[2018]5781)
文摘We present a self-assembly method to prepare array nano-wires of colloidal CdSe quantum dots on a substrate of porous Al2 O3 film modified by gold nanoparticles. The photoluminescence(PL) spectra of nanowires are in situ measured by using a scanning near-field optical microscopy(SNOM) probe tip with 100-nm aperture on the scanning near-field optical microscope. The results show that the binding sites from the edge of porous Al2 O3 nanopores are combined with the carboxyl of CdSe quantum dots’ surface to form an array of CdSe nanowires in the process of losing background solvent because of the gold nanoparticles filling the nano-holes of porous Al2 O3 film. Compared with the area of nonself-assembled nano-wire, the fluorescence on the Al2 O3/Au/CdSe interface is significantly enhanced in the self-assembly nano-wire regions due to the electron transfer conductor effect of the gold nanoparticles’ surface. In addition, its full width at half maximum(FWHM) is also obviously widened. The method of enhancing fluorescence and energy transfer can widely be applied to photodetector, photocatalysis, optical display, optical sensing, and biomedical imaging, and so on.
基金supported by the National Natural Science Foundation of China(Grant Nos.61390501,61471337,61622116,and 51325204)the National Key Scientific Instrument and Equipment Development Project of China(Grant No.2013YQ1203451)+1 种基金the CAS Hundred Talents Program,the Transregional Collaborative Research Center TRR 61(Grant No.21661132006)the National Supercomputing Center in Tianjin.A portion of the research was performed in CAS Key Laboratory of Vacuum Physics
文摘Here we report the thermo-controllable self-assembled structures of single-layer 4, 4＇＇-diamino-p-terphenyl（DAT）molecules on Au（110）, which are investigated by scanning tunneling microscopy（STM） combined with density functional theory（DFT） based calculations. With the deposition of monolayer DAT molecules on Au（110） and subsequent annealing at 100℃, all DAT molecules adsorb on a（1×5） reconstructed surface with a ladder-like structure. After annealing the sample at about 200℃, STM images show three distinct domains, including DAT molecules on a（1×3） reconstructed surface, dehydrogenated molecules with two hydrogen atoms detached from one amino group（–2H-DAT） on a（1×5）reconstructed surface and dehydrogenated molecules with four hydrogen atoms detached from two amino groups（–4HDAT） on a（1×3） reconstructed surface through N–Au bonds. Furthermore, after annealing the sample to 350℃, STM image shows only one self-assembled structure with –4H-DAT molecules on a（1×3） reconstructed surface. Relative STM simulations of different self-assembled structures show excellent agreements with the experimental STM images at different annealing temperatures. Further DFT calculations on the dehydrogenation process of DAT molecule prove that the dehydrogenation barrier on a（1×5） reconstructed surface is lower than that on（1×3） one, which demonstrate the experimental results that the formation temperature of a（1×3） reconstructed surface is higher than that of a（1×5） one.
文摘Forming a monolayer of mixed nickel and gold nanoparticles through self-assembly via simple solution processing constitutes an important step toward inexpensive nanoparticle-based carbon nanofiber growth.In this work,mixed gold and nickel nanoparticles were anchored on the silicon wafer using self-assembled monolayers(SAMs)as a template.SAMs of 3-mercaptopropyl trimethoxysilane(MPTS-SAMs)were formed on silicon wafer,with the exposed thiol functionality providing ligand exchange sites to form the mixed monolayer of nickel and gold nanoparticles via a two-step sequential soaking approach.The densities of the nickel and gold nanoparticles on the surface can be varied by adjusting the soaking sequence.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.61377065 and 61574064)the Science and Technology Planning Project of Guangdong Province,China(Grant Nos.2013CB040402009 and 2015B010132009)the Science and Technology Project of Guangzhou City,China(Grant No.2014J4100056)
文摘The morphology of the copper iodide （CuI） film as an inorganic p-type material has an important influence on enhancing the performance of polymer solar cells （PSCs）. A self-assembled monolayer of 3-aminopropanoic acid （C3-SAM） was used on the surface of indium tin oxide （ITO） before depositing the CuI films. Consequently, a well-distributed and smooth CuI film was formed with pinhole free and complete surface coverage. The root mean square of the corresponding CuI film was reduced from 3.63 nm for ITO/CuI to 0.77 nm. As a result, the average power conversion efficiency （PCE） of PSCs with the device structure of ITO/C3-SAM/CuI/P3HT：PC61BM/ZnO/Al increased significantly from 2.55% （best 2.66%） to 3.04% （best 3.20%） after C3-SAM treatment. This work provides an effective strategy to control the morphology of CuI films through interracial modification and promotes its application in efficient PSCs.
基金Supported by the Advanced Membrane Technology Research Center of the Universities Teknologi Malaysia under Grant No R.J130000.7609.4C112the Postdoctoral Grantthe Frontier Materials Research Alliance
文摘Measuring the growth parameters of Ge quantum dots （QDs） embedded in SiO2/Si hetero-structure is pre- requisite for developing the optoelectronic devices such as photovoltaics and sensors. Their optical properties can be tuned by tailoring the growth morphology and structures, where the growth parameters＇ optimizations still need to be explored. We determine the effect of annealing temperature on surface morphology, structures and optical properties of Ge//SiO2//Si hetero-structure. Samples are grown via rf magnetron sputtering and subsequent characterizations are made using imaging and spectroscopic techniques.
基金Project supported by the National Key Basic Research Program of China(Grant No.2013CB933903)the National Natural Science Foundation of China(Grant Nos.20974065+2 种基金51173117and 50830107)the Scientific Research Start-up Fund of Kunming University of Science and Technology(Grant No.KKSY201305089)
文摘Recent progress of the preparation and applications of superparamagnetic iron oxide（SPIO） clusters as magnetic resonance imaging（MRI） probes is reviewed with regard to their applications in labeling and tracking cells in vivo, in diagnosis of cardiovascular diseases and tumors, and in drug delivery systems. Magnetic nanoparticles（NPs）, especially SPIO nanoparticles, have long been used as MRI contrast agents and as an advantageous nanoplatform for drug delivery,taking advantage of their unique magnetic properties and ability to function at the molecular and cellular levels. Due to advances in nanotechnology, various means to control SPIO NPs＇ size, composition, magnetization and relaxivity have been developed, as well as ways to usefully modify their surface. Recently, self-assembly of SPIO NP clusters in particulate carriers — such as polymeric micelles, vesicles, liposomes, and layer-by-layer（Lb L） capsules — have been widely studied for application as ultrasensitive MRI probes, owing to their remarkably high spin–spin（T2） relaxivity and convenience for further functionalization.
基金Research and Development Plan of China(No.2016YFA0201500,2020YFA0907702)National Facility for Translational Medi-cine(Shanghai)(No.TMST-2020-001)for financial support.
文摘Affibody molecules are small nonimmunoglobulin affinity proteins,which can precisely target to some cancer cells with specific overexpressed molecular signatures.However,the relatively short in vivo half-life of them seriously limited their application in drug targeted delivery for cancer therapy.Here an amphiphilic affibody-drug conjugate is self-assembled into nanomicelles to prolong circulation time for targeted cancer therapy.As an example of the concept,the nanoagent was prepared through molecular self-assembly of the amphiphilic conjugate of Z_(HHR2:342)-Cys with auristatin E derivate,where the affibody used is capable of binding to the human epidermal growth factor receptor 2(HER2).Such a nanodrug not only increased the blood circulation time,but also enhanced the tumor targeting capacity(abundant affibody arms on the nanoagent surface) and the drug accumulation in tumor.As a result,this affibody-based nanoagent showed excellent antitumor activity in vivo to HER2-positive ovary and breast tumor models,which nearly eradicated both small solid tumors(about 100 mm^(3)) and large established tumors(exceed 500 mm^(3)).The relative tumor proliferation inhibition ratio reaches 99.8% for both models.
基金Project supported by the National Natural Science Foundation of China （Grant No 10334060） and The State Key Development Program for Basic Research of China （Grant No 2005CB623602）.
文摘Arrays of noble metal nanoparticles show potential applications in （bio-）sensing, optical storage, surface-enhanced spectroscopy, and waveguides. For all such potential devices, controlling the size, morphology, and interparticle spacing of the nanoparticles is very important. Here, we combine seed-mediated growth with nanosphere lithography to study the controllable growth of gold nanoparticles （Au NPs）, in which the self-assembly monolayer of polystyrene （PS） on a silicon surface is used to guide the modification of allaunesilanes and the subsequent adsorption of gold seeds; seed-mediated growth is applied to controlling the morphology and size of Au NPs. The size of adsorption region （determining the number of adsorbed gold seeds） is controlled by etching PS microspheres with oxygen plasma or annealing PS microspheres at the glass transition temperature. The size and morphology of the Au NPs are controlled by changing growth conditions. In such a way, we have achieved the dual control of the obtained Au NPs. Preliminary results show that this strategy holds a great promise. This approach can also be extended to a wide range of materials and substrates.
基金Project supported by the Natural Science Foundation of Shandong Province,China(Grant No.ZR2017PF011)the National Natural Science Foundation of China(Grant No.E020701)the Doctoral Scientific Research Foundation of Binzhou University,China(Grant No.2014Y10)
文摘In this paper, core–shell quantum dots(QDs) with two polar surface functional groups(ZnSe/ZnS–COOH QDs and ZnSe/ZnS–NH_2 QDs) are synthesized in an aqueous phase. Photoluminescence(PL) and absorption spectra clearly indicate luminescence down-shifting(LDS) properties. On the basis of QDs, surface functional group multilayer LDS films(MLDSs) are fabricated through an electrostatic layer-by-layer(LBL) self-assembly method. The PL intensity increases linearly with the number of bilayers, showing a regular and uniform film growth. When the M-LDS is placed on the surface of a Si-based solar cell as an optical conversion layer for the first time, the external quantum efficiency(EQE) and shortcircuit current density(Jsc) notably increases for the LDS process. The EQE response improves in a wavelength region extending from the UV region to the blue region, and its maximum increase reaches more than 15% between 350 nm and 460 nm.
基金supported by the National Natural Science Foundations of China(21965024,22269016,51721002)the Inner Mongolia funding(2020JQ01,21300-5223601)the funding of Inner Mongolia University(10000-21311201/137,213005223601/003,21300-5223707)。
文摘Generating sufficient strains on metal surfaces are highly challenging owing to that most metals can deform plastically to relax the strains on the surfaces.In this work,we developed a facile but highly efficient stacked deposition strategy to in situ activation and reconstruction of NiO/NiOOH on Ni matrix,following with the migration of Fe ions to NiOOH.The Fe sites on the Ni/NiO/NiOOH facilitate the formation of the stable*OH oxygenated intermediates,and the Ni matrix in the catalyst provides the catalyst excellent stability.The oxygen evolution reaction(OER)performance of the stacked NiFe-5 with compressive strain displays the strengthened binding to oxygenated intermediates and superior OER activity,the ultralow overpotentials of 162 versus reversible hydrogen electrode at 10 mA cm^(-2).On the other hand,the Ni-5 without the incorporation of Fe has shown an outstanding hydrogen evolution reaction(HER)activity,affording an overpotential of 47 mV at 10 mA cm^(-2).The NiFe-5‖Ni-5 enables the overall water splitting at a voltage of 1.508 V to achieve 20 mA cm^(-2) with remarkable durability.The stacked deposition strategy improves binding strength of Ni-based catalysts to oxygenated intermediates via generating compressive strain,causing high catalytic activities on OER and HER.
基金Project supported by the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB10040304)the National Natural Science Foundation of China(Grant Nos.51490654,11290164,and U1262109)the Key Research Program of Chinese Academy of Sciences(Grant No.KJZDEW-M03)
文摘Hydrophobic nanochannel plays a significant role in many physical, biological, and geological phenomena and ex- hibits impressive applications due to both its ubiquitous distribution and great ability to transport hydrophobic molecules, including various oils and gases. Based on theoretical modeling, we herein reveal that the amphipathic Janus nanoparticles have a large probability to self-assemble into uninterrupted hydrophobic nanochannels inside the aqueous nano-space, al- though there are large portions of the Janus nanoparticles to be hydrophilic. The key to this observation is the attractions between the hydrophobic regimes on neighboring amphipathic Janus particles through hydrophobic interaction in aqueous nano-space. More surprisingly, the permeation efficiency of hydrophobic molecules through the uninterrupted hydrophobic channel in Janus particles aggregate is even higher than that in the aggregate of hydrophobic particles. We note that the proposed amphipathic Janus particles can be transported to the appropriate positions by the water since the hydrophilic regimes still remain a strong particle-water interaction. We also note that most natural subsurface rocks are not completely hydrophobic or hydrophilic but have complex surfaces with inhomogeneous wetting property. Our work therefore provides a detailed molecular level understanding of the formation of underground strata as well as the new insight for constructing the artificial hydrophobic channels for various applications, such as the design of proppants to enhance the recovery of the unconventional oil/gas.
基金supported by the National Natural Science Foundation of China(22078211)the China Postdoctoral Science Foundation(2022M721115).
文摘The interactions between lignin oligomers and solvents determine the behaviors of lignin oligomers self-assembling into uniform lignin nanoparticles(LNPs).Herein,several alcohol solvents,which readily interact with the lignin oligomers,were adopted to study their effects during solvent shifting process for LNPs’production.The lignin oligomers with widely distributed molecular weight and abundant guaiacyl units were extracted from wood waste(mainly consists of pine wood),exerting outstanding self-assembly capability.Uniform and spherical LNPs were generated in H_(2)O-n-propanol cosolvent,whereas irregular LNPs were obtained in H_(2)O-methanol cosolvent.The unsatisfactory self-assembly performance of the lignin oligomers in H_(2)O-methanol cosolvent could be attributed to two aspects.On one hand,for the initial dissolution state,the distinguishing Hansen solubility parameter and polarity between methanol solvent and lignin oligomers resulted in the poor dispersion of the lignin oligomers.On the other hand,strong hydrogen bonds between methanol solvent and lignin oligomers during solvent shifting process,hindered the interactions among the lignin oligomers for self-assembly.
