On the spectral difference between electroluminescence and photoluminescence of Si nanocrystals: a mechanism study of electroluminescence

A highly dense and uniform layer of Au nanoparticles (NPs) on poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) film has been produced by the pulsed laser deposition (PLD) technique toward the production of an improved efficiency photovoltaic device. The advantage of PLD over other techniques is the easy and precise control of the Au NPs size and spatial distribution, without needing of further NP surface functionalization. The efficiency enhancement factor related to Au NPs doping has been evaluated in a solar cell based on poly-(3-hexylthiophene):[6,6]-phenyl-C₆₁-butyric acid methyl ester (P3HT:PCBM) diffused bilayer. The short-circuit current density, J _SC, increases by 18 % and the power conversion efficiency by 22 %, respectively, in comparison with an equivalent device without Au NPs. The optical and morphological properties of the Au NPs layer have been selected in order to evaluate the contribution of the surface plasmon resonance as enhancement factor of the solar cell efficiency, in a range size where light scattering is negligible.     

Formation and properties of high density Si nanodots

Laser induced crystallization of ultrathin hydrogenated amorphous Si films or amorphous Si-based multilayered structures were used to get high density Si nanodots. The present technique can get size controllable Si nanodots embedded in various dielectric materials with uniform distribution which was revealed by cross-section transmission electron microscopy. Room temperature photoluminescence and electroluminescence were achieved with the emission wavelength in a visible light region both from a-SiN/Si nanodots/a-SiN sandwiched and Si nanodots/SiO₂ multilayered structures. The luminescence was associated with the radiative recombination of generated electron-hole pairs in Si nanodots or the luminescent surface states. The electroluminescence intensity is increased with increasing the injection current implying the bipolar carrier injection plays an important role in enhancing the luminescence efficiency. The formed Si nanodots by the present approach can be applied for many kinds of devices such as high efficient light emitting diodes and solar cells.     

Emergent Upconversion Sustainable Micro‐Optical Trapping Device

Ultrathin‐thickness single‐junction Si‐based solar cells can be developed to enhance photoelectric conversion efficiency (PECE) approaching to Shockley–Queisser limit. However, loss of short circuit current is a crucial factor that dramatically affects PECE improvement. Even though many studies have focused on rare reflector architecture for facilitating near‐infrared radiation absorption, PECE is still constraint due to its fabrication cost. Herein, an upconversion sustainable micro‐optical trapping device is reported. Using a systematic procedure, a high upconversion performance core–shell‐nanoparticles (CSNPs) structure is synthesized. Accordingly, silica diatom microporous frustule is a good electromagnetic field localization chamber, upon which CSNPs are embedded through a microassemble synthesis. This emerging device can be support on ultrathin‐thickness single‐junction Si‐based solar cells as a rare absorber with its low preparation cost. In the experiment, CSNPs upconversion optical density by surface plasmon resonance of Au nanoparticle's enhancement can be increased five‐time greater than NaYF₄ without SiO₂ coating. A finite difference time domain simulation and real color luminescence images in this study are also demonstrated.     

Excimer laser ablation of gold-loaded inverse polystyrene-block-poly (2-vinylpyridine) micelles

Diblock-copolymers (PS(1700)-b-P2VP(450) or PS(1350)-b-P2VP(400)) forming spherical micelles, can be loaded with a Au-salt and deposited on top of various substrates. Such polymer films have been exposed to a pulsed ArF excimer laser in order to remove the polymer matrix and, in parallel, to chemically reduce the salt into metallic Au nanodots. To analyze this process in detail, it was subdivided into three steps: (a) laser ablation of thick and thin diblock-copolymer films; (b) laser irradiation of Au-salt loaded diblock-copolymer films; and (c) laser irradiation of arrays of metallic Au nanodots. In (a) it was found that a complete removal of the polymer by laser ablation is only possible in air under ambient conditions while identical laser irradiations under vacuum result in a residual layer of approximately 14 nm. Substep (b) revealed a nucleation process of the resulting metallic Au within the micellar core leading to clusters of small Au dots. Furthermore, this substep provided evidence for an asymmetric interplay between the macroscopic temperature of a polymer film during laser treatment and the energy density per laser pulse. In (c) it could be demonstrated that metallic Au nanodots on mica are stable against laser irradiation under conditions leading to a polymer removal. Received: 7 August 2000 / Accepted: 2 November 2000 / Published online: 3 April 2001     

Humidity controlled crystallization of thin CH3NH3PbI3 films for high performance perovskite solar cell

Control of crystallization of a solution‐processed perovskite layer is of prime importance for high performance solar cells. In spite of the negative effect of water on perovskite solar energy conversion in several previous works, we observed that humidity plays a critical role to develop a thin uniform, dense perovskite film with preferred crystals, in particular, in a device with architecture of ITO/PEDOT:PSS/CH₃NH₃PbI₃/ PC₇₁BM/LiF/Al fabricated by two‐step sequential spin‐coating process. Humidity controlled spin‐coating of CH₃NH₃I on the pre‐formed PbI₂ layer was the most influential process and systematic structural investigation as a function of humidity revealed that grains of CH₃NH₃PbI₃ perovskite crystals increase in size with their preferred orientation while film surface becomes roughened as the humidity increases. The performance of a device was closely related to the humidity dependent film morphology and in 40% relative humidity, the device exhibited the maximum power conversion efficiency of approximately 12% more than 10 times greater than that of a device fabricated at 20% humidity. The results suggest that our process with controlled humidity can be another efficient route for high performance and reliable perovskite solar cells. (© 2016 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

Enhanced field emission from PbTiO3 nanodots prepared by phase separation approach

Uniformly distributed PbTiO₃ nanodots were successfully prepared by phase separation approach. A precursor sol film was first spin-coated on Si wafer and then spontaneously separated into two distinct phases owing to the Marangoni instability. PT nanodots with tailorable size and density were obtained after further heat treatment. X-ray diffraction analysis indicated that these nanodots showed a perovskite structure. An excellent room temperature field emission property of PbTiO₃ nanodots was observed: the minimum turn-on voltage was about 5.3 V/μm; while the emission current density reached about 270 μA cm⁻² at an applied field of about 9.25 V/μm.     

Dual plasmonic‐enhanced bulk‐heterojunction solar cell incorporating gold nanoparticles into solution‐processed anode buffer layer and active layer

A dual plasmonic resonance effect on the performance of poly(3‐hexylthiophene) (P3HT):phenyl C61‐butyricacid methyl ester (PC61BM) based polymer solar cells (PSCs) has been demonstrated by selectively incorporating 25 nm colloidal gold nanoparticles (Au NPs) in a solution‐processed molybdenum oxide (MoO₃) anode buffer layer and 5 nm colloidal Au NPs in the active P3HT:PCBM layer. The devices exhibit up to ～20% improvement in power conversion efficiency which is attributed to the dual effect of localized surface plasmon resonance (LSPR) of Au NPs with enhanced light absorption and exciton generation. Our report shows a guideline on the usage of dual LSPR effect for the solution‐processed polymer solar cells to achieve high efficiencies. (© 2015 WILEY‐VCH Verlag GmbH &Co. KGaA, Weinheim)     

MEH-PPV与TiO2共混体系太阳电池性能分析

以MEH-PPV(poly(2-methoxy-5-(2′-ethylhexoxy)-1,4-phenylene vinylene)为电子给体材料(Donor,D), TiO₂纳米线为电子受体材料(Acceptor,A),制成了共混体系太阳电池. 从D/A材料共混体系的紫外可见吸收光谱(UV-vis)、光荧光谱(PL)、器件的电荷传输的光导J-V图等方面,分析了MEH-PPV∶TiO₂体系器件性能变化的原因. 得出了当在纯MEH-PP 关键词： 太阳电池 聚合物 性能     

Characteristic material parameters of CIGS solar cell related with device performance

CIGS solar cells with power conversion efficiency (PCE) in the range of 1.82%–12.30% were obtained by using two-step process, and were further analyzed through various measurement techniques. Material parameters showed diverse values and some trends depending on the device performance. The lower performance device showed small integrated PL intensity, short minority life time, larger defect density and lower activation energy, whereas the higher performance device showed opposite values. We investigated relationship between material parameters and PCE of solar cells, and found that some physical parameters such as integrated PL intensity, minority life time, defect density, and difference between band gap and activation energy (E_g-E_a), which all reflect defect states in bulk and at pn interface, are strongly related with PCE and would be used as a good indicator to evaluate device performance quickly.     

Gradient doping simulation of perovskite solar cells with CH3NH3Sn1−xPbxI3 as the absorber layer

In this study, we built a perovskite solar cells(PSCs) model with a Au/CuSCN/CH₃NH₃Sn_1−xPb_xI₃/TiO₂/FTO glass structure using the SCAPS program and use polynomial fitting to obtain the relationship between the conduction/valence bands of CH₃NH₃Sn_1−xPb_xI₃ and the x value, which is more complex and accurate than that in any previous research. The influences of thickness, electron and hole mobilities, relative permittivity, effective conduction band density, effective valence band density, and the value of x on the solar cell performance are analyzed. Furthermore, we simulate the situation where the doping concentration changes with the absorption layer depth of the device and a special bandgap is formed. The power conversion efficiency of the device improves from 19.96% to 20.52%, with an open-circuit voltage of 0.776 V, a short-circuit current of 33.79 mA/cm², and a filling factor of 77.39% when double gradient doping is performed. The application value of gradient doping in the device absorption layer is obtained.     

Impact of nongeminate recombination on the performance of pristine and annealed P3HT:PCBM solar cells

Transient photovoltage (TPV) and voltage dependent charge extraction (CE) measurements were applied to poly(3‐hexyl‐thiophene) (P3HT):[6,6]‐phenyl‐C61 butyric acid methyl ester (PCBM) bulk heterojunction solar cells to analyze the limitations of solar cell performance in pristine and annealed devices. From the determined charge carrier decay rate under open circuit conditions and the voltage dependent charge carrier densities n (V), the nongeminate loss current j_loss of the device is accessible. We found that j_loss alone is sufficient to describe the j –V characteristics across the whole operational range, for annealed and, not yet shown before, also for the lower performing pristine solar cells. Even in a temperature range from 300 K to 200 K nongeminate recombination is found to be the dominant and, therefore, performance limiting loss process. Consequently, charge photogeneration is voltage independent in the voltage range studied. (© 2012 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

A New Insight of the Photothermal Effect on the Highly Efficient Visible‐Light‐Driven Photocatalytic Performance of Novel‐Designed TiO2 Rambutan‐Like Microspheres Decorated by Au Nanorods

Photocatalyst‐assisted degradation of organic pollutants, which exhibits a novel strategy for solar‐energy utilization, possesses enormous potential in various applications. Extending the light‐absorption range in the spectrum of sunlight and improving light‐conversion efficiency are always primary issues to enhance the catalytic performance of these photocatalysts. Herein, a new structure of gold‐nanorod‐decorated TiO₂ rambutan‐like microspheres is designed, which exhibits superior photocatalytic ability toward Rhodamine B in the range of visible light due to the 3D distribution of the TiO₂ branches on the surface of the microspheres, which prompts the multireflection of photons. The absorption rate of photons is thereby tremendously enhanced. This is beneficial for the generation of hot electrons originating from the localized surface plasmonic resonance of Au nanorods, which can be used to both initiate the reaction and produce the photothermal effect. Hot electrons generated by a single Au nanorod in microspheres to initiate the degradation reaction can be as high as 2.5 times of those in the nanowires' counterpart. Moreover, the heating power of a single Au nanorod in microspheres reaches up to 4.4 times higher than that in nanowires, which further accelerates the degradation rate. The reaction pathway of visible‐light‐assisted RhB degradation catalyzed by Au/TiO₂ microspheres goes through an initial N‐deethylation process instead of the complete cycloreversion catalyzed by pure TiO₂ microspheres under UV irradiation. This strategy of structure design for improved photon absorption, which achieves high degradation rate and photothermal effect, is promising for the development of novel photocatalysts.     

Conductive nanodots on the surface of irradiated CaF2

CaF₂(111) single crystal surfaces have been irradiated with fast heavy ions under oblique angles resulting in chains of nanosized hillocks. In order to characterize these nanodots with respect to their conductivity we have applied non‐contact atomic force microscopy using a magnetic tip. Measurements in ultra high vacuum as well as under ambient conditions reveal a clearly enhanced electromagnetic interaction between the magnetic tip and the nanodots. The dissipated energy per cycle is comparable to the value found for metals, indicating that the interaction of the ion with the target material leads to the creation of metallic Ca nanodots on the surface. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Thin Film Solar Cell Based on ZnSnN2/SnO Heterojunction

In this article, we report the growth of zinc‐tin nitride (ZnSnN₂) thin films as a potential absorber for photovoltaic applications by fabricating a heterojunction of n‐ZnSnN₂/p‐SnO. The performance of the heterojunction has been monitored through selective deposition of top electrode with different materials (Ni/Au or Al). The electron‐transfer process from the ZnSnN₂ layer to the cathode is facilitated by selecting metal electrode with relatively low work function, which also boosts up the electron injection or/and extraction. The diode exhibits a good J–V response in the dark with a rectification ratio of 3 × 10³ at 1.0 V and an ideality factor of 4.2 in particular with Al as the top electrode. Under illumination, the heterostructure solar cell demonstrates a power conversion efficiency of ≈0.37% with an open circuit voltage of 0.25 V and a short circuit current density of 4.16 mA cm^?2. The prime strategies, on how to improve solar cell efficiency concerning band offsets and band alignment engineering are also discussed.     

Controlling the nanodot formation on GaAs surface during focused ion beam processing

GaAs processed using gallium-focused ion beams for the fabrication of photonic devices mostly results in gallium nanodots on the surface. These gallium nanodots may produce unwanted effects and deteriorate the optical and electrical properties of the devices. We have investigated the FIB processing of GaAs with and without exposure to an insulator-enhanced etching precursor gas (XeF₂) to explore the use of XeF₂ during GaAs processing. It is reported that without the gas, FIB processing results in nanodots on the surface that vary in size and density depending on processing parameters such as incident energy, beam current, angle and dwell time. Processing with insulator (XeF₂)-enhanced etching gas irrespective of the process parameters eliminates the nanodots and results in a smooth surface, as characterized by scanning electron microscopy and atomic force microscopy. This method will be useful for surfaces which require dry processing without exposure to any wet chemical etching.     

Growth of high-density Ru- and RuO2-composite nanodots on atomic-layer-deposited Al2O3 film

Growth of Ru- and RuO₂-composite (ROC) nanodots on atomic-layer-deposited Al₂O₃ film has been studied for the first time using ion-beam sputtering followed by post-deposition annealing (PDA). X-ray photoelectron spectroscopy analyses reveal that RuO₂ and Ru co-exist before annealing, and around 10% RuO₂ is reduced to metallic Ru after PDA at 900 °C for 15 s. Scanning electron microscopy measurements show that well-defined spherical ROC nanodots are not formed till the PDA temperature is raised to 900 °C. The mean diameter of the nanodots enlarges with increasing PDA temperature whereas the nanodot density decreases, which is attributed to coalescence process between adjacent nanodots. It is further illustrated that the resulting nanodot size and density are weakly dependent on the annealing time, but are markedly influenced by the decomposition of RuO₂. In this article, the ROC nanodots with a high density of 1.6 × 10¹¹ cm⁻², a mean diameter of 20 nm with a standard deviation of 3.0 nm have been achieved for the PDA at 900 °C for 15 s, which is promising for flash memory application.     

Switching behavior induced by different substituents of group in single molecular device

We investigate the electronic transport properties of photochromic azobenzene-based molecular devices with Au electrodes using non-equilibrium Green’s function and density functional theory. A reversible switching behavior between cis and trans isomerization is found in the device. In addition, the substituent of ?NH₂ on the right end hydrogen atom of azobenzene molecule reduces the switching ratio of current, consequently the disappearance of switching behavior, while the substituent of ?NO₂ improves the switching ratio of current. We discuss the different electronic transport induced by different substituents through the transmission spectra, localized density of states, molecular projected self-consistent Hamiltonian and transmission pathways. The observed polarization effect under bias is explained by the evolution of molecular projected self-consistent Hamiltonian of LUMO level. The results indicate that the electron-withdrawing group ?NO₂ substituting right terminal hydrogen of azobenzene molecule becomes a candidate for improving the performance of molecular device.     

Organic‐inorganic hybrids based on phenanthrene‐functionalized gold nanoparticles for OLEDs

The electroluminescence intensity of the phenanthrene‐functionalized gold nanoparticles, PMPT‐Au nanoparticles/CPB: Ir(PIA)₂ (acac) film, was increased by 4.9 times compared with control device, CPB: Ir(PIA)₂ (acac) due to coupling between the excitons of emissive layer and localized surface plasmonic resonance of PMPT‐Au NPs. The maximum luminous efficiencies of devices II to IV with PMPT‐Au NPs were 39.2 cd A^?1 (11.8 V), 40.1 cd A^?1 (10.5 V), and 43.1 cd A^?1 (9.0 V), respectively. The increment of current efficiency with PMPT‐Au NP coated devices was strongly related to the energy transfer between the radiated light generated from CBP: Ir(PIA)₂ (acac) emissive layer and localized surface plasmonic resonance excited by PMPT‐Au NP layer.     

Fabrication and electrical characterization of a MOS memory device containing self-assembled metallic nanoparticles

Floating gate devices with nanoparticles embedded in dielectrics have recently attracted much attention due to the fact that these devices operate as non-volatile memories with high speed, high density and low power consumption. In this paper, memory devices containing gold (Au) nanoparticles have been fabricated using e-gun evaporation. The Au nanoparticles are deposited on a very thin SiO₂ layer and are then fully covered by a HfO₂ layer. The HfO₂ is a high-k dielectric and gives good scalability to the fabricated devices. We studied the effect of the deposition parameters to the size and the shape of the Au nanoparticles using capacitance–voltage and conductance–voltage measurements, we demonstrated that the fabricated device can indeed operate as a low-voltage memory device.     

Fabrication and characterization of ZnTPP:PCBM bulk heterojunction (BHJ) solar cells

Bulk heterojunction (BHJ) solar cells were fabricated based on blended films of a porphyrin derivative 5,10,15,20-Tetraphenyl-21H,23H-porphine zinc (ZnTPP) and a fullerene derivative [6,6]-phenyl-C₆₁ butyric acid methyl ester (PCBM) as the active layer. The ZnTTP:PCBM BHJ solar cells were fabricated by spin-casting of the blended layer. The weight ratios of ZnTPP and PCBM were varied from 1:1 to 0:10. The electronic and optical properties of each cell were investigated. Optical density (OD) of the blended film for each cell was extracted from its reflection and transmission curves. OD and average absorption coefficients of the active materials were used to determine film thicknesses. Absorption spectra of each component material were compared with the spectra of the blended films. Current density–Voltage (J–V) characteristics were recorded under dark as well as under the illumination of AM 1.5G (1 sun) solar spectrum. The BHJ solar cell with ZnTPP:PCBM ratio of 1:9 showed the best performance . The values of RR, V_OC , J_SC , FF and η for these ratios were 106.3, 0.4 V, 1.316 mA/cm², 0.4 and 0.21%, respectively. The cross-section of this device using SEM was also examined.