Flaw-size-dependent mechanical interlayer coupling and edge-reconstruction embrittlement in van der Waals materials.

Van der Waals (vdW) materials consisting of two-dimensional (2D) building blocks have strong in-plane covalent bonding and weak interlayer interactions. While monolayer 2D materials exhibit impressive fracture resistance, as demonstrated in hexagonal boron nitride (h-BN), preserving these remarkable properties in vdW materials remains a challenge. Here we reveal an anomalous mechanical interlayer coupling that involves interlayer-friction toughening and edge-reconstruction embrittlement during the fracture of multilayer h-BN.

Simultaneous Enhancement of Efficiency and Operational-Stability of Mesoscopic Perovskite Solar Cells via Interfacial Toughening.

The combined effects of compact TiO (c-TiO ) electron-transport layer (ETL) are investigated without and with mesoscopic TiO (m-TiO ) on top, and without and with an iodine-terminated silane self-assembled monolayer (SAM), on the mechanical behavior, opto-electronic properties, photovoltaic (PV) performance, and operational-stability of solar cells based on metal-halide perovskites (MHPs). The interfacial toughness increases almost threefold in going from c-TiO without SAM to m-TiO with SAM. This is attributed to the synergistic effect of the m-TiO /MHP nanocomposite at the interface and the enhanced adhesion afforded by the iodine-terminated silane SAM.

Tailoring the thermal conductivity of two-dimensional metal halide perovskites.

Proper thermal management of solar cells based on metal halide perovskites (MHPs) is key to increasing their efficiency as well as their durability. Although two-dimensional (2D) MHPs possess enhanced thermal stability as compared to their three-dimensional (3D) counterparts, the lack of comprehensive knowledge of the heat transfer mechanisms dictating their ultralow thermal conductivities is a bottleneck for further improvements in their thermal performance. Here, we experimentally and computationally study the Dion-Jacobson (DJ) and Ruddlesden-Popper (RP) phases of MHPs ( = 1) to demonstrate that the length of the organic spacers has a negligible influence on their thermal transport properties; we experimentally measure thermal conductivities of 0.

Dual-Interface-Reinforced Flexible Perovskite Solar Cells for Enhanced Performance and Mechanical Reliability.

Two key interfaces in flexible perovskite solar cells (f-PSCs) are mechanically reinforced simultaneously: one between the electron-transport layer (ETL) and the 3D metal-halide perovskite (MHP) thin film using self-assembled monolayer (SAM), and the other between the 3D-MHP thin film and the hole-transport layer (HTL) using an in situ grown low-dimensional (LD) MHP capping layer. The interfacial mechanical properties are measured and modeled. This rational interface engineering results in the enhancement of not only the mechanical properties of both interfaces but also their optoelectronic properties holistically.

Time-resolved vibrational-pump visible-probe spectroscopy for thermal conductivity measurement of metal-halide perovskites.

Understanding thermal transport at the microscale to the nanoscale is crucially important for a wide range of technologies ranging from device thermal management and protection systems to thermal-energy regulation and harvesting. In the past decades, non-contact optical methods, such as time-domain and frequency-domain thermoreflectance, have emerged as extremely powerful and versatile thermal metrological techniques for the measurement of material thermal conductivities. Here, we report the measurement of thermal conductivity of thin films of CHNHPbI (MAPbI), a prototypical metal-halide perovskite, by developing a time-resolved optical technique called vibrational-pump visible-probe (VPVP) spectroscopy.

Knowledge extraction and transfer in data-driven fracture mechanics.

Data-driven approaches promise to usher in a new phase of development in fracture mechanics, but very little is currently known about how data-driven knowledge extraction and transfer can be accomplished in this field. As in many other fields, data scarcity presents a major challenge for knowledge extraction, and knowledge transfer among different fracture problems remains largely unexplored. Here, a data-driven framework for knowledge extraction with rigorous metrics for accuracy assessments is proposed and demonstrated through a nontrivial linear elastic fracture mechanics problem encountered in small-scale toughness measurements.

Linking melem with conjugated Schiff-base bonds to boost photocatalytic efficiency of carbon nitride for overall water splitting.

Developing an efficient single component photocatalyst for overall water splitting under visible-light irradiation is extremely challenging. Herein, we report a metal-free graphitic carbon nitride (g-CxN4)-based nanosheet photocatalyst (x = 3.2, 3.

Interfacial toughening with self-assembled monolayers enhances perovskite solar cell reliability.

Iodine-terminated self-assembled monolayer (I-SAM) was used in perovskite solar cells (PSCs) to achieve a 50% increase of adhesion toughness at the interface between the electron transport layer (ETL) and the halide perovskite thin film to enhance mechanical reliability. Treatment with I-SAM also increased the power conversion efficiency from 20.2% to 21.

Interpenetrating interfaces for efficient perovskite solar cells with high operational stability and mechanical robustness.

The perovskite solar cell has emerged rapidly in the field of photovoltaics as it combines the merits of low cost, high efficiency, and excellent mechanical flexibility for versatile applications. However, there are significant concerns regarding its operational stability and mechanical robustness. Most of the previously reported approaches to address these concerns entail separate engineering of perovskite and charge-transporting layers.

p-p orbital interaction via magnesium isovalent doping enhances optoelectronic properties of halide perovskites.

p-p orbital interaction through Mg(ii) isovalent doping in methylammonium lead chloride perovskite significantly enhances the electronic properties while not affecting the optical bandgap. This chemical behaviour shows promising applications to optoelectronic devices.

Arrays of Plasmonic Nanostructures for Absorption Enhancement in Perovskite Thin Films.

We report optical characterization and theoretical simulation of plasmon enhanced methylammonium lead iodide (MAPbI 3 ) thin-film perovskite solar cells. Specifically, various nanohole (NH) and nanodisk (ND) arrays are fabricated on gold/MAPbI 3 interfaces. Significant absorption enhancement is observed experimentally in 75 nm and 110 nm-thick perovskite films.

Anomalous 3D nanoscale photoconduction in hybrid perovskite semiconductors revealed by tomographic atomic force microscopy.

While grain boundaries (GBs) in conventional inorganic semiconductors are frequently considered as detrimental for photogenerated carrier transport, their exact role remains obscure for the emerging hybrid perovskite semiconductors. A primary challenge for GB-property investigations is that experimentally they need to be performed at the top surface, which is not only insensitive to depth-dependent inhomogeneities but also could be susceptible to topographic artifacts. Accordingly, we have developed a unique approach based on tomographic atomic force microscopy, achieving a fully-3D, photogenerated carrier transport map at the nanoscale in hybrid perovskites.

transfer of CHNHPbI single crystals in mesoporous scaffolds for efficient perovskite solar cells.

Printable mesoscopic perovskite solar cells are usually fabricated by drop-casting perovskite precursor solution on a screen-printed mesoporous TiO/ZrO/carbon triple-layer followed by thermal annealing. They have attracted much attention due to their simple fabrication process and remarkable stability. However, challenges lie in how to achieve complete pore fillings of perovskites in the meso-pores and to obtain high-quality perovskite crystals.

Sub-1.4eV bandgap inorganic perovskite solar cells with long-term stability.

State-of-the-art halide perovskite solar cells have bandgaps larger than 1.45 eV, which restricts their potential for realizing the Shockley-Queisser limit. Previous search for low-bandgap (1.

Publisher Correction: Carrier lifetime enhancement in halide perovskite via remote epitaxy.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Carrier lifetime enhancement in halide perovskite via remote epitaxy.

Crystallographic dislocation has been well-known to be one of the major causes responsible for the unfavorable carrier dynamics in conventional semiconductor devices. Halide perovskite has exhibited promising applications in optoelectronic devices. However, how dislocation impacts its carrier dynamics in the 'defects-tolerant' halide perovskite is largely unknown.

Highly stable and efficient all-inorganic lead-free perovskite solar cells with native-oxide passivation.

There has been an urgent need to eliminate toxic lead from the prevailing halide perovskite solar cells (PSCs), but the current lead-free PSCs are still plagued with the critical issues of low efficiency and poor stability. This is primarily due to their inadequate photovoltaic properties and chemical stability. Herein we demonstrate the use of the lead-free, all-inorganic cesium tin-germanium triiodide (CsSnGeI) solid-solution perovskite as the light absorber in PSCs, delivering promising efficiency of up to 7.

Synthetic Approaches for Halide Perovskite Thin Films.

Halide perovskites are an intriguing class of materials that have recently attracted considerable attention for use as the active layer in thin film optoelectronic devices, including thin-film transistors, light-emitting devices, and solar cells. The "soft" nature of these materials, as characterized by their low formation energy and Young's modulus, and high thermal expansion coefficients, not only enables thin films to be fabricated via low-temperature deposition methods but also presents rich opportunities for manipulating film formation. This comprehensive review explores how the unique chemistry of these materials can be exploited to tailor film growth processes and highlights the connections between processing methods and the resulting film characteristics.

Bandgap Optimization of Perovskite Semiconductors for Photovoltaic Applications.

The bandgap is the most important physical property that determines the potential of semiconductors for photovoltaic (PV) applications. This Minireview discusses the parameters affecting the bandgap of perovskite semiconductors that are being widely studied for PV applications, and the recent progress in the optimization of the bandgaps of these materials. Perspectives are also provided for guiding future research in this area.

Homogenous Alloys of Formamidinium Lead Triiodide and Cesium Tin Triiodide for Efficient Ideal-Bandgap Perovskite Solar Cells.

The alloying behavior between FAPbI and CsSnI perovskites is studied carefully for the first time, which has led to the realization of single-phase hybrid perovskites of (FAPbI ) (CsSnI ) (0 View Article and Find Full Text PDF

Methylammonium-Mediated Evolution of Mixed-Organic-Cation Perovskite Thin Films: A Dynamic Composition-Tuning Process.

Methylammonium-mediated phase-evolution behavior of FA MA PbI mixed-organic-cation perovskite (MOCP) is studied. It is found that by simply enriching the MOCP precursor solutions with excess methylammonium cations, the MOCPs form via a dynamic composition-tuning process that is key to obtaining MOCP thin films with superior properties. This simple chemical approach addresses several key challenges, such as control over phase purity, uniformity, grain size, composition, etc.

Thin-Film Transformation of NH PbI to CH NH PbI Perovskite: A Methylamine-Induced Conversion-Healing Process.

Methylamine-induced thin-film transformation at room-temperature is discovered, where a porous, rough, polycrystalline NH PbI non-perovskite thin film converts stepwise into a dense, ultrasmooth, textured CH NH PbI perovskite thin film. Owing to the beneficial phase/structural development of the thin film, its photovoltaic properties undergo dramatic enhancement during this NH PbI -to-CH NH PbI transformation process. The chemical origins of this transformation are studied at various length scales.

Lithium-ion battery electrolyte mobility at nano-confined graphene interfaces.

Interfaces are essential in electrochemical processes, providing a critical nanoscopic design feature for composite electrodes used in Li-ion batteries. Understanding the structure, wetting and mobility at nano-confined interfaces is important for improving the efficiency and lifetime of electrochemical devices. Here we use a Surface Forces Apparatus to quantify the initial wetting of nanometre-confined graphene, gold and mica surfaces by Li-ion battery electrolytes.

Observation of phase-retention behavior of the HC(NH2)2PbI3 black perovskite polymorph upon mesoporous TiO2 scaffolds.

The α→δ phase transition, which occurs favorably in planar films of a black α-HC(NH2)2PbI3 (α-FAPbI3) perovskite in the amibent, is retarded when α-FAPbI3 is deposited upon mesoporous TiO2 scaffolds. It is hypothesized that this is due to the synergistic effect of the partial encapsulation of α-FAPbI3 by the mesoporous TiO2 and the elevated activation energy for the transition reaction associated with the substantial increase of the TiO2/α-FAPbI3 interfacial area in the mesoscopic system.