Highly passivated TOPCon bottom cells for perovskite/silicon tandem solar cells.

Tunnel oxide passivated contact (TOPCon) silicon solar cells are rising as a competitive photovoltaic technology, seamlessly blending high efficiency with cost-effectiveness and mass production capabilities. However, the numerous defects from the fragile silicon oxide/c-Si interface and the low field-effect passivation due to the inadequate boron in-diffusion in p-type polycrystalline silicon (poly-Si) passivated contact reduce their open-circuit voltages (VOCs), impeding their widespread application in the promising perovskite/silicon tandem solar cells (TSCs) that hold a potential to break 30% module efficiency. To address this, we have developed a highly passivated p-type TOPCon structure by optimizing the oxidation conditions, boron in-diffusion, and aluminium oxide hydrogenation, thus pronouncedly improving the implied VOC (iVOC) of symmetric samples with p-type TOPCon structures on both sides to 715 mV and the VOC of completed double-sided TOPCon bottom cells to 710 mV. Consequently, integrating with perovskite top cells, our proof of concept of 1 cm2 n-i-p perovskite/silicon TSCs exhibit VOCs exceeding 1.9 V and a high efficiency of 28.20% (certified 27.3%), which paves a way for TOPCon cells in the commercialization of future tandems.

High-Efficiency Inverted Perovskite Solar Cells via In Situ Passivation Directed Crystallization.

Lead halide perovskite solar cells (PSCs) have emerged as one of the influential photovoltaic technologies with promising cost-effectiveness. Though with mild processabilities to massive production, inverted PSCs have long suffered from inferior photovoltaic performances due to intractable defective states at boundaries and interfaces. Herein, an in situ passivation (ISP) method is presented to effectively adjust crystal growth kinetics and obtain the well-orientated perovskite films with the passivated boundaries and interfaces, successfully enabled the new access of high-performance inverted PSCs. The study unravels that the strong yet anisotropic ISP additive adsorption between different facets and the accompanied additive engineering yield the high-quality (111)-orientated perovskite crystallites with superior photovoltaic properties. The ISP-derived inverted perovskite solar cells (PSCs) have achieved remarkable power conversion efficiencies (PCEs) of 26.7% (certified as 26.09% at a 5.97 mm2 active area) and 24.5% (certified as 23.53% at a 1.28 cm2 active area), along with decent operational stabilities.

Nanosecond laser annealing processed surface-structured hyperdoped silicon for efficient near-infrared detection.

Surface-structured engineering of hyperdoped silicon can effectively facilitate the absorption of sub-bandgap photons in pristine single-crystal silicon (sc-Si). Here, we conducted different annealing approaches of ordinary thermal annealing (OTA) and nanosecond laser annealing (NLA) on modification of titanium-hyperdoped silicon (Si:Ti) surface structure, to achieve efficient near-infrared detection. It is presented that both OTA and NLA processes can improve the crystallinity of Si:Ti samples. In detail, atomic-resolved STEM characterization illustrates that NLA treatment will further eliminate the amorphous phase on Si:Ti surface to varying degrees. While one-dimensional periodic stacking fault structure of 9R-Si phase is formed at the surface of sc-Si and embedded in the Si matrix during the OTA process, which reveals the seamless interface of 9R-Si/sc-Si along with [11¯0] direction. Due to the high sub-bandgap light absorption and good crystal structure, the Si:Ti photodetector after NLA treatment with an energy density of 2.6 J cm-2exhibited the highest responsivity, reaching 151 mA W-1at 1550 nm even at a low operating voltage of 1 V. We assume the performance enhancement of NLA processed Si:Ti photodetectors can be attributed to two aspects, the one is NLA can reduce the recombination of photo-generated charge carriers in amorphous surface layer by improving crystallization, and the other is that NLA process can weaken the diffusion of titanium impurities due to the extremely rapid heating and cooling rates. This study presents prospects towards surface-structured silicon in infrared light detection.

Eliminating Resistance-Capacitance Coupling Shielding for Depicting the Defect Landscape in Perovskite Solar Cells by Capacitance Spectroscopy.

Capacitance spectroscopy techniques have been widely utilized to evaluate the defect properties in perovskites, which contribute to the efficiency and operation stability development for perovskite solar cells (PSCs). Yet the interplay between the charge transporting layer (CTL) and the perovskite on the capacitance spectroscopy results is still unclear. Here, they show that a pseudo-trap-state capacitance signal is generated in thermal admittance spectroscopy (TAS) due to the enhanced resistance capacitance (RC) coupling caused by the carrier freeze-out of the CTL in PSCs, which could be discerned from the actual defect-induced trap state capacitance signal by tuning the series resistance of PSCs. By eliminating the RC coupling shielding effect on the defect-induced capacitance spectroscopy, it is obtain the actual defect density which is 4-folds lower than the pseudo-trap density, and the spatial distribution of defects in PSCs which reveals that the commonly adopted interface passivators can passivate the defects about 60 nm away from the decorated surface. It is further revealed that phenethylammonium ions (PEA+) possess a better passivation capability over octylammonium ions (OA+) due to the deeper passivation depth for PEA+ on the surface defects in perovskite films.

Visualizing the Structure-Property Nexus of Wide-Bandgap Perovskite Solar Cells under Thermal Stress.

Wide-bandgap perovskite solar cells (PSCs) toward tandem photovoltaic applications are confronted with the challenge of device thermal stability, which motivates to figure out a thorough cognition of wide-bandgap PSCs under thermal stress, using in situ atomic-resolved transmission electron microscopy (TEM) tools combing with photovoltaic performance characterizations of these devices. The in situ dynamic process of morphology-dependent defects formation at initial thermal stage and their proliferations in perovskites as the temperature increased are captured. Meanwhile, considerable iodine enables to diffuse into the hole-transport-layer along the damaged perovskite surface, which significantly degrade device performance and stability. With more intense thermal treatment, atomistic phase transition reveals the perovskite transform to PbI2 along the topo-coherent interface of PbI2/perovskite. In conjunction with density functional theory calculations, a mutual inducement mechanism of perovskite surface damage and iodide diffusion is proposed to account for the structure-property nexus of wide-bandgap PSCs under thermal stress. The entire interpretation also guided to develop a thermal-stable monolithic perovskite/silicon tandem solar cell.

Strain Regulation and Defect Passivation of FA-Based Perovskite Materials for Highly Efficient Solar Cells.

Formamidine lead triiodide (FAPbI3 ) perovskites have attracted increasing interest for photovoltaics attributed to the optimal bandgap, high thermal stability, and the record power conversion efficiency (PCE). However, the materials still face several key challenges, such as phase transition, lattice defects, and ion migration. Therefore, external ions (e.g., cesium ions (Cs+ )) are usually introduced to promote the crystallization and enhance the phase stability. Nevertheless, the doping of Cs+ into the A-site easily leads to lattice compressive strain and the formation of pinholes. Herein, trioctylphosphine oxide (TOPO) is introduced into the precursor to provide tensile strain outside the perovskite lattice through intermolecular forces. The special strain compensation strategy further improves the crystallization of perovskite and inhibits the ion migration. Moreover, the TOPO molecule significantly passivates grain boundaries and undercoordinated Pb2+ defects via the forming of P═O─Pb bond. As a result, the target solar cell devices with the synergistic effect of Cs+ and TOPO additives have achieved a significantly improved PCE of 22.71% and a high open-circuit voltage of 1.16 V (voltage deficit of 0.36 V), with superior stability under light exposure, heat, or humidity conditions.

Exceptional Hole-Selective Properties of Ta2O5 Films via Sn4+ Doping for High Performance Silicon Heterojunction Solar Cells.

Carrier-selective passivating contacts using transition metal oxides (TMOs) have attracted great attention for crystalline silicon (c-Si) heterojunction solar cells recently. Among them, tantalum oxide (Ta2O5) exhibits outstanding advantages, such as a wide bandgap, good surface passivation, and a small conduction band offset with c-Si, which is typically used as an electron-selective contact layer. Interestingly, it is first demonstrated that solution-processed Ta2O5 films exhibit a high hole selectivity, which blocks electrons and promotes hole transport simultaneously. Through the ozone pre-treatment of Ta2O5/p-Si interface and optimization of the film thickness (≈9 nm), the interfacial recombination is suppressed and the contact resistivity is reduced from 178.0 to 29.3 mΩ cm2. Moreover, the Sn4+ doping increases both the work function and oxygen vacancies of the film, contributing to the improved hole-selective contact performance. As a result, the photoelectric conversion efficiencies of Ta2O5/p-Si heterojunction solar cells are significantly improved from 14.84% to 18.47%, with a high thermal stability up to 300 °C. The work has provided a feasible strategy to explore new features of TMOs for carrier-selective contact applications, that is, bipolar carrier transport properties.

Direct growth of graphene on hyper-doped silicon to enhance carrier transport for infrared photodetection.

The importance of infrared photodetectors cannot be overstated, especially in fields such as security, communication, and military. While silicon-based infrared photodetectors are widely used due to the maturity of the semiconductor industry, their band gap of 1.12 eV limits their infrared light absorption above 1100 nm, making them less effective. To overcome this limitation, we report a novel infrared photodetector prepared by growing graphene on the surface of zinc hyper-doped silicon. This technique utilizes hyper-doping to introduce deep level assisted infrared light absorption benefit from the enhanced carrier collection capacity of graphene. Without introducing new energy consumption, the hyper-doped substrate annealing treatment is completed during the growth of graphene. By the improvement of transport and collection of charge carriers, the graphene growth adjusts the band structure to upgrade electrode contact, resulting in a response of 1.6 mA W-1under laser irradiation with a wavelength of 1550 nm and a power of 2 mW. In comparison, the response of the photodetector without graphene was only 0.51 mA W-1, indicating a three-fold performance improvement. Additionally, the device has lower dark current and lower noise current, resulting in a noise equivalent power of 7.6 × 10-8W Hz-0.5. Thus, the combination of transition metal hyper-doping and graphene growth technology has enormous potential for developing the next generation of infrared photodetectors.

Regionalizing Nitrogen Doping of Polysilicon Films Enabling High-Efficiency Tunnel Oxide Passivating Contact Silicon Solar Cells.

Tunnel oxide passivating contact (TOPCon) solar cells (SCs) as one of the most competitive crystalline silicon (c-Si) technologies for the TW-scaled photovoltaic (PV) market require higher passivation performance to further improve their device efficiencies. Here, the successful construction of a double-layered polycrystalline silicon (poly-Si) TOPCon structure is reported using an in situ nitrogen (N)-doped poly-Si covered by a normal poly-Si, which achieves excellent passivation and contact properties simultaneously. The new design exhibits the highest implied open-circuit voltage of 755 mV and the lowest single-sided recombination current density (J0 ) of ≈0.7 fA cm⁻2 for a TOPCon structure and a low contact resistivity of less than 5 mΩ·cm2 , resulting in a high selectivity factor of ≈16. The mechanisms of passivation improvement are disclosed, which suggest that the introduction of N atoms into poly-Si restrains H overflow by forming stronger Si-N and N-H bonds, reduces interfacial defects, and induces favorable energy bending. Proof-of-concept TOPCon SCs with such a design receive a remarkable certified efficiency of 25.53%.

CuCl2-modified SnO2electron transport layer for high efficiency perovskite solar cells.

SnO2film is one of the most widely used electron transport layers (ETL) in perovskite solar cells (PSCs). However, the inherent surface defect states in SnO2film and mismatch of the energy level alignment with perovskite limit the photovoltaic performance of PSCs. It is of great interesting to modify SnO2ETL with additive, aiming to decrease the surface defect states and obtain well aligned energy level with perovskite. In this paper, anhydrous copper chloride (CuCl2) was employed to modify the SnO2ETL. It is found that the adding of a small amount of CuCl2into the SnO2ETL can improve the proportion of Sn4+in SnO2, passivate oxygen vacancies at the surface of SnO2nanocrystals, improve the hydrophobicity and conductivity of ETL, and obtain a good energy level alignment with perovskite. As a result, both the photoelectric conversion efficiency (PCE) and stability of the PSCs based on SnO2ETLs modified with CuCl2(SnO2-CuCl2) is improved in comparison with that of the PSCs on pristine SnO2ETLs. The optimal PSC based on SnO2-CuCl2ETL exhibits a much higher PCE of 20.31% as compared to the control device (18.15%). The unencapsulated PSCs with CuCl2modification maintain 89.3% of their initial PCE after exposing for 16 d under ambient conditions with a relative humidity of 35%. Cu(NO3)2was also employed to modify the SnO2ETL and achieved a similar effect as that of CuCl2, indicating that the cation Cu2+plays the main role in SnO2ETL modification.

Dynamic photoelectrical regulation of ECM protein and cellular behaviors.

Dynamic regulation of cell-extracellular matrix (ECM)-material interactions is crucial for various biomedical applications. In this study, a light-activated molecular switch for the modulation of cell attachment/detachment behaviors was established on monolayer graphene (Gr)/n-type Silicon substrates (Gr/Si). Initiated by light illumination at the Gr/Si interface, pre-adsorbed proteins (bovine serum albumin, ECM proteins collagen-1, and fibronectin) underwent protonation to achieve negative charge transfer to Gr films (n-doping) through π-π interactions. This n-doping process stimulated the conformational switches of ECM proteins. The structural alterations in these ECM interactors significantly reduced the specificity of the cell surface receptor-ligand interaction (e.g., integrin recognition), leading to dynamic regulation of cell adhesion and eventual cell detachment. RNA-sequencing results revealed that the detached bone marrow mesenchymal stromal cell sheets from the Gr/Si system manifested regulated immunoregulatory properties and enhanced osteogenic differentiation, implying their potential application in bone tissue regeneration. This work not only provides a fast and feasible method for controllable cells/cell sheets harvesting but also gives new insights into the understanding of cell-ECM-material communications.

Tandem Electro-Oxidative C-C and C-N Coupling and Aromatization for the Construction of Pyrazine-Fused Bis-aza[7]helicene.

Repeated tandem electro-oxidative C-C and C-N coupling and aromatization were employed for the efficient construction of aza[7]helicene (BA7) as a key intermediate and the targeted pyrazine-fused bis-aza[7]helicene (PBBA7) derivatives in 90.0-93.2% isolated yields under a controlled potential. The electrosynthetic protocol showed high selectivity and enabled rapid access to functionalized organic conjugated materials from readily available polycyclic aromatic amines. A synthetic mechanistic study along with an investigation of the photoelectrical properties and application of PBBA7-C16 as a potential hole-transporting material for perovskite solar cells were performed.

High detectivity graphene/si heterostructure photodetector with a single hydrogenated graphene atomic interlayer for passivation and carrier tunneling.

Hydrogenated graphene is easy to prepare and chemically stable. Besides, hydrogenation of graphene can open the band gap, which is vital for electronic and optoelectronic applications. Graphene/Si photodetector (PD) has been widely studied in imaging, telecommunications, and other fields. The direct contact between graphene and Si can form a Schottky junction. However, it suffers from poor interface state, where the carrier recombination at the interface causes serious leakage current, which in turn leads to a decrease in the detectivity. Hence, in this study, hydrogenated graphene is used as an interfacial layer, which passivates the interface of graphene/Si (Gr/Si) heterostructure. Besides, the single atomic layer thickness of hydrogenated graphene is also crucial for the tunneling transport of charge carriers and its suitable energy band position reduces the recombination of carrier. The fabricated graphene/hydrogenated-graphene/Si (Gr/H-Gr/Si) heterostructure PD showed an extremely low dark current about 10-7A. As a result, it had low noise current and exhibited a high specific detectivity of âˆ¼2.3 × 1011Jones at 0 V bias with 532 nm laser illumination. Moreover, the responsivity of the fabricated PD was found to be 0.245 A W-1at 532 nm illumination with 10µW power. These promising results show a great potential of hydrogenated graphene to be used as an interface passivation and carrier tunneling layer for the fabrication of high-performance Gr/Si heterostructure PDs.

Phase-Stable Wide-Bandgap Perovskites for Four-Terminal Perovskite/Silicon Tandem Solar Cells with Over 30% Efficiency.

Wide-bandgap perovskite solar cells (PSCs) with an optimal bandgap between 1.7 and 1.8 eV are critical to realize highly efficient and cost-competitive silicon tandem solar cells (TSCs). However, such wide-bandgap PSCs easily suffer from phase segregation, leading to performance degradation under operation. Here, it is evident that ammonium diethyldithiocarbamate (ADDC) can reduce the detrimental I2 back to I- in precursor solution, thereby reducing the density of deep level traps in perovskite films. The resultant perovskite film exhibits great phase stability under continuous illumination and 30-60% relative humidity conditions. Due to the suppression of defect proliferation and ion migration, the PSCs deliver great operation stability which retain over 90% of the initial power conversion efficiency (PCE) after 500 h maximum power point tracking. Finally, a highly efficient semitransparent PSC with a tailored bandgap of 1.77 eV, achieving a PCE approaching 18.6% with a groundbreaking open-circuit voltage (VOC ) of 1.24 V enabled by ADDC additive in perovskite films is demonstrated. Integrated with a bottom silicon solar cell, a four-terminal (4T) TSC with a PCE of 30.24% is achieved, which is one of the highest efficiencies in 4T perovskite/silicon TSCs.

Light-Emitting Artificial Synapses for Neuromorphic Computing.

As the key connecting points in the neuromorphic computing systems, synaptic devices have been investigated substantially in recent years. Developing optoelectronic synaptic devices with optical outputs is becoming attractive due to many benefits of optical signals in systems. Colloidal quantum dots (CQDs) are potential luminescent materials for information displays. Light-emitting diodes based on CQDs have become appealing candidates for optoelectronic synaptic devices. Moreover, light-emitting transistors exhibit great application potential in these synaptic devices. From this perspective, light-emitting artificial synapses were discussed on the basis of these structures in the devices. Their mechanisms, performance, and future development were analysed and prospected in detail.

Low-temperature processed tantalum/niobium co-doped TiO2electron transport layer for high-performance planar perovskite solar cells.

A low-temperature preparation process is significantly important for scalable and flexible devices. However, the serious interface defects between the normally used titanium dioxide (TiO2) electron transport layer (ETL) obtained via a low-temperature method and perovskite suppress the further improvement of perovskite solar cells (PSCs). Here, we develop a facile low-temperature chemical bath method to prepare a TiO2ETL with tantalum (Ta) and niobium (Nb) co-doping. Systematic investigations indicate that Ta/Nb co-doping could increase the conduction band level of TiO2and could decrease the trap-state density, boosting electron injection efficiency and reducing the charge recombination between the perovskite/ETL interface. A superior power conversion efficiency of 19.44% can be achieved by a planar PSC with a Ta/Nb co-doped TiO2ETL, which is much higher than that of pristine TiO2(17.60%). Our achievements in this work provide new insights on low-temperature fabrication of low-cost and highly efficient PSCs.

Stabilizing Fullerene for Burn-in-Free and Stable Perovskite Solar Cells under Ultraviolet Preconditioning and Light Soaking.

It is crucial to make perovskite solar cells sustainable and have a stable operation under natural light soaking before they become commercially acceptable. Herein, a small amount of the small molecule bathophenanthroline (Bphen) is introduced into [6,6]-phenyl-C61 -butyric acid methyl ester and it is found that Bphen can stabilize the C60 -cage well through formation of much more thermodynamically stable charge-transfer complexes. Such a strengthened complex is used as an interlayer at the in-light perovskite/SnO2 side to achieve a champion device with efficiency of 23.09% (certified 22.85%). Most importantly, the stability of the resulting devices can be close to meeting the requirements of the International Electrotechnical Commission 61215 standard under simulated UV preconditioning and light-soaking testing. They can retain over 95% and 92% of their initial efficiencies after 1100 h UV irradiation and 1000 h continuous illumination of maximum power point tracking at 60 °C, respectively.

Ink Engineering of Inkjet Printing Perovskite.

Inkjet printing method is one of the most effective ways for fabricating large-area perovskite solar cells (PSCs). However, because ink crystallizes rapidly during printing, the printed perovskite film is discontinuous with increasing defects. It severely restricts the application of the inkjet printing technology to the fabrication of perovskite photovoltaic devices. Here, we designed a new mixed-cation perovskite ink system that can controllably retard the crystallization rate of perovskite. In this new ink system, the printing solvent is composed of n-methyl pyrrolidone (NMP) and dimethyl formamide (DMF), and PbX2 is replaced by PbX2-DMSO (X = Br, I) complex as a printing precursor to create a high-quality perovskite layer. Accordingly, the printed Cs0.05MA0.14FA0.81PbI2.55Br0.45 perovskite film exhibited high homogeneity with a large grain size (over 500 nm). Besides, the printed perovskite film possessed lower defects with improved carrier lifetime compared to the control sample. Combining these advantages, the printed PSC delivers decent power conversion efficiencies (PCEs) of 19.6% (0.04 cm2) and 17.9% (1.01 cm2). The large-area device can still retain its original efficiency of 89% when stored in air with humidity less than 20% for 1000 h.

Effects of vacancy defects on the mechanical properties in neutron irradiated Czochralski silicon.

We have investigated the mechanical properties of neutron irradiated Czochralski (NICZ) silicon using nanoindentations combined with micro-Raman spectroscopy. It is found that NICZ silicon shows higher hardness (∼13% higher) than non-irradiated silicon, with a slightly lower Young's modulus. When the samples were subjected to isochronal anneals in the temperature range of 250 °C-650 °C, the hardness of NICZ silicon gradually decreases as the temperature increases and it is finally comparable to that of the non-irradiated silicon. The vacancies and vacancy-oxygen defects induced by neutron irradiation in NICZ silicon annihilate or transform into more complex defects during the annealing processes. It suggests that the vacancy defects play a role in the evolution of hardness, which promote phase transition from the Si-I phase to the stiffer Si-II phase in NICZ silicon during indentation. In addition, the irradiation induced vacancy defects could lead to the lower Young's modulus.