Anisotropic spin transport and photoresponse characteristics detected by tip movement in magnetic single-molecule junction

Orientation-dependent transport properties induced by anisotropic molecules are enticing in single-molecule junctions.Here,using the first-principles method,we theoretically investigate spin transport properties and photoresponse characteristics in trimesic acid magnetic single-molecule junctions with different molecular adsorption orientations and electrode contact sites.The transport calculations indicate that a single-molecule switch and a significant enhancement of spin transport and photoresponse can be achieved when the molecular adsorption orientation changes from planar geometry to upright geometry.The maximum spin polarization of current and photocurrent in upright molecular junctions exceeds 90%.Moreover,as the Ni tip electrode moves,the tunneling magnetoresistance of upright molecular junctions can be increased to 70%.The analysis of the spin-dependent PDOS elucidates that the spinterfaces between organic molecule and ferromagnetic electrodes are modulated by molecular adsorption orientation,where the molecule in upright molecular junctions yields higher spin polarization.Our theoretical work paves the way for designing spintronic devices and optoelectronic devices with anisotropic functionality base on anisotropic molecules.

Unusual magnetic relaxation in a single-molecule magnet with toroidal magnetic moments

We report the synthesis and characterization of a single-molecule magnet composed of triangular clusters of dysprosium ions.The structural study shows that the symmetry changes from one polar point group(mm2)at room temperature to another polar point group(m)at low temperature.Magnetic studies and theory calculations illustrate that the vortex distribution of magnetic dipoles in the triangular dysprosium clusters forms a toroidal magnetic moment.Interestingly,the analysis of AC magnetic susceptibility reveals the coexistence of three distinct magnetic relaxation processes,corresponding to the Raman,Orbach,and QTM relaxation pathways,respectively.The sum of three modified Debye functions is successfully used to describe the multiple relaxation behavior.

Electroluminescence explored internal behavior of carriers in InGaAsP single-junction solar cell

The internal behaviors of carriers in InGaAsP single-junction solar cell are investigated by using electroluminescence(EL) measurements. Two emission peaks can be observed in current-dependent electroluminescence spectra at low temperatures, and carrier localization exists for both peaks under low excitation. The trends of power index α extracted from excitation-dependent EL spectra at different temperatures imply that there exists a competition between Shockley–Read–Hall recombination and Auger recombination. Auger recombination becomes dominant at high temperatures, which is probably responsible for the lower current density of InGaAsP solar cell. Besides, the anomalous “S-shape” tendency with the temperature of band-edge peak position can be attributed to potential fluctuation and carrier redistribution, demonstrating delocalization, transfer, and redistribution of carriers in the continuum band-edge. Furthermore, the strong reduction of activation energy at high excitations indicates that electrons and holes escaped independently, and the faster-escaping carriers are holes.

Single-Molecule Confinement Induced Intrinsic Multi-Electron Redox-Activity to Enhance Supercapacitor Performance

Aggregation of polyoxometalates(POM)is largely responsible for the reduced performance of POM-based energy-storage systems.To address this challenge,here,the precise confinement of single Keggin-type POM molecule in a porous carbon(PC)of unimodal super-micropore(micro-PC)is realized.Such precise single-molecule confinement enables sufficient activity center exposure and maximum electron-transfer from micro-PC to POM,which well stabilizes the electron-accepting molecules and thoroughly activates its inherent multi-electron redox-activity.In particular,the redox-activities and electron-accepting properties of the confined POM molecule are revealed to be super-micropore pore size-dependent by experiment and spectroscopy as well as theoretical calculation.Meanwhile,the molecularly dispersed POM molecules confined steadily in the“cage”of micro-PC exhibit unprecedented large-negative-potential stability and multiple-peak redox-activity at an ultra-low loading of~11.4 wt%.As a result,the fabricated solid-state supercapacitor achieves a remarkable areal capacitance,ultrahigh energy and power density of 443 mF cm^(-2),0.12 mWh cm^(-2)and 21.1 mW cm^(-2),respectively.This work establishes a novel strategy for the precise confinement of single POM molecule,providing a versatile approach to inducing the intrinsic activity of POMs for advanced energy-storage systems.

Combination of density-clustering and supervised classification for event identification in single-molecule force spectroscopy data

Single-molecule force spectroscopy(SMFS)measurements of the dynamics of biomolecules typically require identifying massive events and states from large data sets,such as extracting rupture forces from force-extension curves(FECs)in pulling experiments and identifying states from extension-time trajectories(ETTs)in force-clamp experiments.The former is often accomplished manually and hence is time-consuming and laborious while the latter is always impeded by the presence of baseline drift.In this study,we attempt to accurately and automatically identify the events and states from SMFS experiments with a machine learning approach,which combines clustering and classification for event identification of SMFS(ACCESS).As demonstrated by analysis of a series of data sets,ACCESS can extract the rupture forces from FECs containing multiple unfolding steps and classify the rupture forces into the corresponding conformational transitions.Moreover,ACCESS successfully identifies the unfolded and folded states even though the ETTs display severe nonmonotonic baseline drift.Besides,ACCESS is straightforward in use as it requires only three easy-to-interpret parameters.As such,we anticipate that ACCESS will be a useful,easy-to-implement and high-performance tool for event and state identification across a range of single-molecule experiments.

DecodeSTORM:A user-friendly ImageJ plug-in for quantitative data analysis in single-molecule localization microscopy

Quantitative data analysis in single-molecule localization microscopy(SMLM)is crucial for studying cellular functions at the biomolecular level.In the past decade,several quantitative methods were developed for analyzing SMLM data;however,imaging artifacts in SMLM experiments reduce the accuracy of these methods,and these methods were seldom designed as user-friendly tools.Researchers are now trying to overcome these di±culties by developing easyto-use SMLM data analysis software for certain image analysis tasks.But,this kind of software did not pay su±cient attention to the impact of imaging artifacts on the analysis accuracy,and usually contained only one type of analysis task.Therefore,users are still facing di±culties when they want to have the combined use of different types of analysis methods according to the characteristics of their data and their own needs.In this paper,we report an ImageJ plug-in called DecodeSTORM,which not only has a simple GUI for human–computer interaction,but also combines artifact correction with several quantitative analysis methods.DecodeSTORM includes format conversion,channel registration,artifact correction(drift correction and localization¯ltering),quantitative analysis(segmentation and clustering,spatial distribution statistics and colocalization)and visualization.Importantly,these data analysis methods can be combined freely,thus improving the accuracy of quantitative analysis and allowing users to have an optimal combination of methods.We believe DecodeSTORM is a user-friendly and powerful ImageJ plug-in,which provides an easy and accurate data analysis tool for adventurous biologists who are looking for new imaging tools for studying important questions in cell biology.

Magnetic-field-controlled spin valve and spin memory based on single-molecule magnets

A single-molecule magnet is a long-sought-after nanoscale component because it can enable us to miniaturize nonvolatile memory storage devices.The signature of a single-molecule magnet is switching between two bistable magnetic ground states under an external magnetic field.Based on this feature,we theoretically investigate a magnetic-fieldcontrolled reversible resistance change active at low temperatures in a molecular magnetic tunnel junction,which consists of a single-molecule magnet sandwiched between a ferromagnetic electrode and a normal metal electrode.Our numerical results demonstrate that the molecular magnetism orientation can be manipulated by magnetic fields to be parallel/antiparallel to the ferromagnetic electrode magnetization.Moreover,different magnetic configurations can be“read out”based on different resistance states or different spin polarization parameters in the current spectrum,even in the absence of a magnetic field.Such an external magnetic field-controlled resistance state switching effect is similar to that in traditional spin valve devices.The difference between the two systems is that one of the ferromagnetic layers in the original device has been replaced by a magnetic molecule.This proposed scheme provides the possibility of better control of the spin freedom of electrons in molecular electrical devices,with potential applications in future high-density nonvolatile memory devices.

Single-electron transport in H_(2)O@C_(60) single-molecule transistors

Single-molecule transistors(SMTs) based on fullerenes and their derivatives have been recognized as a long-sought platform for studying the single-electron transport properties.H_(2)O@C_(60) is a combination of fullerene and H_(2)O,a typical light molecule.Here we use the 'molecular surgery' technique to synthesize the H_(2)O@C_(60) molecule and then construct the H_(2)O@C_(60) SMTs,together with the C_(60) SMTs.Evidences for single-electron transport have been obtained in our measurements,including explicit Coulomb blockade and Coulomb oscillations.We then calculate the detailed parameters of the H_(2)O@C_(60) and C_(60) SMTs using a capacitance model derived from the Coulomb diamond feature,which gives a capacitance ratio of 1:5.05:8.52 for the H_(2)O@C_(60) SMT and 1:29.5:74.8 for the C_(60) SMT.Moreover,the gate efficiency factor a turns out to be 0.0686 in the H_(2)O@C_(60) SMT,about ten times larger than that in the C_(60) SMT.We propose that the enhanced gate efficiency in H_(2)O@C_(60) SMT may be induced by the closer attachment of molecular orbital electron clouds to the gate substrate due to polarization effects of H_(2)O.

Electron Injection Enhancement by Diamond-Like Carbon Film in Polymer Electroluminescence Devices

A diamond-like carbon （DLC） film is deposited as an electron injection layer between the polymer light-emitting layer（MEH-PPV） and aluminum （Al） cathode electrode in polymer electroluminescence devices （PLEDs） using a radio frequency plasma deposition system. The source material of the DLC is n-butylamine. The devices consist of indium tin oxide （ITO）/MEH-PPV/DLC/Al. Electron injection properties are investigated through I-V characteristics,and the mechanism of electron injection enhancement due to a thin DLC layer has been studied. It is found that： （1） a DLC layer thinner than 1.0nm leads to a higher turn-on voltage and decreased electroluminescent （EL） efficiency; （2） a 5.0nm DLC layer significantly enhances the electron injection and results in the lowest turn-on voltage and the highest EL efficiency; （3） DLC layer that exceeds 5.0nm results in poor device performance;and（4） EL emission can hardly be detected when the layer exceeds 10.0nm. The properties of ITO/MEH-PPV/DLC/Al and ITO/MEH-PPV/LiF/Al are investigated comparatively.

Measurements of Carrier Confinement at β-FeSi_2-Si Heterojunction by Electroluminescence

A Si p-π-n diode with β-FeSi 2 particles embedded in the unintentionally doped Si (p--type) was designed for determining the band offset at β-FeSi 2-Si heterojunction.When the diode is under forward bias,the electrons injected via the Si n-p- junction diffuse to and are confined in the β-FeSi 2 particles due to the band offset.The storage charge at the β-FeSi 2-Si heterojunction inversely hamper the further diffusion of electrons,giving rise to the localization of electrons in the p--Si near the Si junction,which prevents them from nonradiative recombination channels.This results in electroluminescence (EL) intensity from both Si and β-FeSi 2 quenching slowly up to room temperature.The temperature dependent ratio of EL intensity of β-FeSi 2 to Si indicates the loss of electron confinement following thermal excitation model.The conduction band offset between Si and β-FeSi 2 is determined to be about 0 2eV.

Single-molecule optoelectronic devices:physical mechanism and beyond

Single-molecule devices not only promise to provide an alternative strategy to break through the miniaturization and functionalization bottlenecks faced by traditional semiconductor devices,but also provide a reliable platform for exploration of the intrinsic properties of matters at the single-molecule level.Because the regulation of the electrical properties of single-molecule devices will be a key factor in enabling further advances in the development of molecular electronics,it is necessary to clarify the interactions between the charge transport occurring in the device and the external fields,particularly the optical field.This review mainly introduces the optoelectronic effects that are involved in single-molecule devices,including photoisomerization switching,photoconductance,plasmon-induced excitation,photovoltaic effect,and electroluminescence.We also summarize the optoelectronic mechanisms of single-molecule devices,with particular emphasis on the photoisomerization,photoexcitation,and photo-assisted tunneling processes.Finally,we focus the discussion on the opportunities and challenges arising in the single-molecule optoelectronics field and propose further possible breakthroughs.

Red Electroluminescence and Photoluminescence from Novel Binuclear Europium Complex with Squaric Acid Ligand

A novel binuclear europium P-diketone complex with squaric acid ligand was synthesized for the first time. Its structure was elucidated by IR, UV, and Elemental Analysis. Red light emitting diode (LED) was fabricated by using the novel europium complex as an emitting layer, tris(8-quinolinolate) aluminum (III) (Alq(3)) as an electron-transporting layer, N, N'-diphenyl-N, N'-(3-methylphenyl)-1,1'-biphenyl-4,4'-diamine (TPD) as a hole-transporting layer. A cell structure of indium-tin-oxide/TPD/Eu-complex/Alq(3)/Mg: Ag was employed. Red electroluminescence was observed at room temperature with dc bias voltage of 2 V in this cell. 2 Red emission peaks at about 613 nm with maximum luminance of over 106 cd/m(2). Compared with the EL luminance from those europium complexes reported before, one from the Eu-complex is best in the same cells.

Synthesis,characterization,photoluminescence and electroluminescence properties of new 1,3,4-oxadiazole-containing rhenium(I)complex Re(CO)_3(Bphen)(PTOP)

A new 1,3,4-oxadiazole-contanining rhenium（I） complex, with the formula [Re（CO）a（Bphen）（PTOP）], （Bphen = bathophe- nardine, PTOP = 4-（5-p-tolyl-1,3, 4-oxadiazd-2-yl） pyridine）, is synthesized and characterized by elemental analysis, IR, 1H NMR, UV-vis and luminescence spectroscopy. The double-layer electroluminescence devices based on the Re（l） complex have been fabricated by spin-coating technique. The turn-on voltage, maximum efficiency, and brightness for green emission obtained from the devices are 9 V, 2.1 cd/A and 165 cd/m^2, respectively.

Photoluminescence and electroluminescence properties of ZnO films on p-type silicon wafers

A simplified n-ZnO/p-Si heterojunction has been prepared by growing n-type ZnO rods on p-type silicon wafer through the chemical wpour deposition method. The reflectance spectrum of the sample shows an independent absorption peak at 384 nm, which may be originated from the bound states at the junction. In the photoluminescence spectrum a new emission band is shown at 393 nm, besides the bandedge emission at 380nm. The electroluminescence spectrum of the n-ZnO/p-Si heterojunction shows a stable yellow luminescence band centred at 560 nm, which can be attributed to the emission from trapped states. Another kind of discrete ZnO rod has also been prepared on such silicon wafer and is encapsulated with carbonated polystyrene for electroluminescence detection. This composite structure shows a weak ultraviolet electroluminescence band at 395 nm and a yellow electroluminescence band. These data prove that surface modification which blocks the transverse movement of carriers between neighbouring nanorods plays important roles in the ultraviolet emission of ZnO nanorods. These findings are vital for future display device design.

Blue-Green Electroluminescence of Free-Standing Diamond Thin Films

Blue-green electroluminescence has been observed in free-standing diamond films which were deposited by microwave plasma assisted CVD on silicon substrates.The electroluminescence device is driven by a 60 Hz power supply.The threshold voltage was about 112 V peak-to-peak.The electroluminescence spectrum at room temperature,showed a blue-green band with the peak centered at 485nm suggesting band A type emission.Electroluminescence was also observed at 77K.

Rectification and electroluminescence of nanostructured GaN/Si heterojunction based on silicon nanoporous pillar array

A GaN/Si nanoheterojunction is prepared through growing Ga N nanocrystallites（nc-GaN） on a silicon nanoporous pillar array（Si-NPA） by a chemical vapor deposition（CVD） technique at a relatively low temperature. The average size of nc-Ga N is determined to be ~10 nm. The spectral measurements disclose that the photoluminescence（PL） from GaN/SiNPA is composed of an ultraviolet（UV） band and a broad band spanned from UV to red region, with the feature that the latter band is similar to that of electroluminescence（EL）. The electron transition from the energy levels of conduction band and, or, shallow donors to that of deep acceptors of Ga N is indicated to be responsible for both the broad-band PL and the EL luminescence. A study of the I-V characteristic shows that at a low forward bias, the current across the heterojunction is contact-limited while at a high forward bias it is bulk-limited, which follows the thermionic emission model and space-charge-limited current（SCLC） model, respectively. The bandgap offset analysis indicates that the carrier transport is dominated by electron injection from n-GaN into the p-Si-NPA, and the EL starts to appear only when holes begin to be injected from Si-NPA into GaN with biases higher than a threshold voltage.

Mechanism of SrS∶Ce Thin Film Electroluminescence

The influence of the delocalization probability on the mixing interaction between excited levels of Ce3+ and the conduction band of SrS was analysed. The observation of emission wave forms of SrSCe thin film electroluminescence showed that only leading edge emission peak was observed for one sample and the leading and trailing edge emission peaks were observed for another in a half period of sinusoid applied voltage. This difference is related to the influences of sulphur vacancies on the excitation and emission processes. The leading edge emssion is dominated by discrete luminescence caused by direct impact excitation and the trailing edge emission and a part of leading edge emission belong to recombination luminescence caused by impact ionization and delocalization.

White electroluminescence of n-ZnO:Al/p-diamond heterostructure devices

An n-ZnO：A1/p-boron-doped diamond heterostructure electroluminescent device is produced, and a rectifying be- havior can be observed. The electroluminescence spectrum at room temperature exhibits two visible bands centred at 450 nm-485 nm （blue emission） and 570 nm-640 nm （yellow emission）. Light emission with a luminance of 15 cd/m2 is observed from the electroluminescent device at a forward applied voltage of 85 V, which is distinguished from white light by the naked eye.

Monomeric type I and type III transforming growth factor-β receptors and their dimerization revealed by single-molecule imaging

Transforming growth factor-β （TGF-β） binds with two transmembrane serine/threonine kinase receptors, type Ⅱ （TβRII） and type Ⅰ receptors （TβRⅠ）, and one accessory receptor, type Ⅲ receptor （TβRⅢ）, to transduce signals across cell membranes. Previous biochemical studies suggested that TβRI and TβRIII are preexisted homo-dimers. Using single-molecule microscopy to image green fluorescent protein-labeled membrane proteins, for the first time we have demonstrated that TβRI and TβRⅢ could exist as monomers at a low expression level. Upon TGF-β1 stimu- lation, TβRI follows the general ligand-induced receptor dimerization model for activation, but this process is TβRⅡ- dependent. The monomeric status of the non-kinase receptor TβRⅢ is unchanged in the presence of TGF-β1. With the increase of receptor expression, both TβRI and TβRIII can be assembled into dimers on cell surfaces.

Research on Performance of ZnS∶TbF_3 Thin Film Electroluminescence Device

The electroluminescence of ZnS doped with terbium fluoride thin films prepared b y ra dio frequency magnetron sputtering method was reported. The characteristics of t h e ZnS∶TbF 3 thin film electroluminescence devices, such as film characteristi cs of the ZnS∶Tb active layer, substrate temperatures during magnetron sputteri ng and Tb concentration of the active layer, were systematically investigated. The results show that annealing can evidently improve the luminescence performance of the luminescence device.