Poor stability of organic–inorganic halide perovskite materials in humid condition has hindered the success of perovskite solar cells in real applications since controlled atmosphere is required for device fabrication and operation, and there is a lack of effective solutions to this problem until now. Here we report the use of lead (II) thiocyanate (Pb(SCN)2) precursor in preparing perovskite solar cells in ambient air. High-quality CH3NH3PbI3−x(SCN)x perovskite films can be readily prepared even when the relative humidity exceeds 70%. Under optimized processing conditions, we obtain devices with an average power conversion efficiency of 13.49% and the maximum efficiency over 15%. In comparison with typical CH3NH3PbI3-based devices, these solar cells without encapsulation show greatly improved stability in humid air, which is attributed to the incorporation of thiocyanate ions in the crystal lattice. The findings pave a way for realizing efficient and stable perovskite solar cells in ambient atmosphere.

Hydrogen bonding underpins the properties of a vast array of systems spanning a wide variety of scientific fields. From the elegance of base pair interactions in DNA to the symmetry of extended supramolecular assemblies, hydrogen bonds play an essential role in directing intermolecular forces. Yet fundamental aspects of the hydrogen bond continue to be vigorously debated. Here we use dynamic force microscopy (DFM) to quantitatively map the tip-sample force field for naphthalene tetracarboxylic diimide molecules hydrogen-bonded in two-dimensional assemblies. A comparison of experimental images and force spectra with their simulated counterparts shows that intermolecular contrast arises from repulsive tip-sample interactions whose interpretation can be aided via an examination of charge density depletion across the molecular system. Interpreting DFM images of hydrogen-bonded systems therefore necessitates detailed consideration of the coupled tip-molecule system: analyses based on intermolecular charge density in the absence of the tip fail to capture the essential physical chemistry underpinning the imaging mechanism.

Contact electrification between water and a solid surface is crucial for physicochemical processes at water–solid interfaces. However, the nature of the involved processes remains poorly understood, especially in the initial stage of the interface formation. Here we report that H 2 O 2 is spontaneously produced from the hydroxyl groups on the solid surface when contact occurred. The density of hydroxyl groups affects the H 2 O 2 yield. The participation of hydroxyl groups in H 2 O 2 generation is confirmed by mass spectrometric detection of 18 O in the product of the reaction between 4-carboxyphenylboronic acid and 18 O–labeled H 2 O 2 resulting from 18 O 2 plasma treatment of the surface. We propose a model for H 2 O 2 generation based on recombination of the hydroxyl radicals produced from the surface hydroxyl groups in the water–solid contact process. Our observations show that the spontaneous generation of H 2 O 2 is universal on the surfaces of soil and atmospheric fine particles in a humid environment.

HIGHLIGHTS• Nanoscale multi-dimensional heterojunctions in situ grow at the edge of two-dimensional MXene conductive network.• A controlled anneal procedure in 150 °C is for preparing anatase TiO 2 /SnO 2 heterojunctions with oxygen vacancy scramble effect.• The perovskite solar cells achieve high power conversion efficiency and high moisture-resistance stability.ABSTRACT A multi-dimensional conductive heterojunction structure, composited by TiO 2 , SnO 2 , and Ti 3 C 2 T X MXene, is facilely designed and applied as electron transport layer in efficient and stable planar perovskite solar cells.Based on an oxygen vacancy scramble effect, the zero-dimensional anatase TiO 2 quantum dots, surrounding on two-dimensional conductive Ti 3 C 2 T X sheets, are in situ rooted on three-dimensional SnO 2 nanoparticles, constructing nanoscale TiO 2 /SnO 2 heterojunctions. The fabrication is implemented in a controlled lowtemperature anneal method in air and then in N 2 atmospheres. With the optimal MXene content, the optical property, the crystallinity of perovskite layer, and internal interfaces are all facilitated, contributing more amount of carrier with effective and rapid transferring in device. The champion power conversion efficiency of resultant perovskite solar cells achieves 19.14%, yet that of counterpart is just 16.83%. In addition, it can also maintain almost 85% of its initial performance for more than 45 days in 30-40% humidity air; comparatively, the counterpart declines to just below 75% of its initial performance.

We study a low-temperature on-surface reversible chemical reaction of oxygen atoms to molecules in ultrahigh vacuum on the semiconducting rutile TiO2(110)-(1 × 1) surface. The reaction is activated by charge transfer from two sources, natural surface/subsurface polarons and experimental Kelvin probe force spectroscopy as a tool for electronic charge manipulation with single electron precision. We demonstrate a complete control over the oxygen species not attainable previously, allowing us to deliberately discriminate in favor of charge or bond manipulation, using either direct charge injection/removal through the tip-oxygen adatom junction or indirectly via polarons. Comparing our ab initio calculations with experiment, we speculate that we may have also manipulated the spin on the oxygens, allowing us to deal with the singlet/triplet complexities associated with the oxygen molecule formation. We show that the manipulation outcome is fully governed by three experimental parameters, vertical and lateral tip positions and the bias voltage.

Chemical reactions converting sp 2 to sp 3 hybridization have been demonstrated to be a fascinating yet challenging route to functionalize graphene. So far, it has not been possible to precisely control the reaction sites nor their lateral order at the atomic/molecular scale. The application prospects have been limited for reactions requiring long soaking, heating, electric pulses, or probe tip press.Herein, we demonstrate a spatially-selective photocycloaddition reaction of a two-dimensional (2D) molecular network with defect-free basal plane of single-layer graphene. Directly visualized at the sub-molecular level, the cycloaddition is triggered by ultraviolet irradiation in ultrahigh vacuum, requiring no aid of the graphene Moiré pattern. The reaction involves both [2+2] and [2+4] cycloaddition, with the reaction sites aligned into a 2D extended and well-ordered array, inducing a bandgap for the reacted graphene layer. This work provides a solid base for designing and engineering graphene-based optoelectronic and microelectronic devices.

Homogeneous heterostructural wurtzite (WZ)/zincblende (ZB) junctions are successfully fabricated in ZnSe nanobelts. Polarity continuity across the ZB/WZ interface is demonstrated. The saw-tooth-like potential profile induced by spontaneous polarization across the WZ/ZB/WZ interfaces is identified directly at the nanoscale. The polarization-induced charge distribution across the homogeneous heterostructural interfaces is proposed as a viable alternative approach towards charge tailoring in semiconductor nanostructures.

Three-dimensional branched TiO2 architectures (3D BTA) with controllable morphologies were synthesized via a facile template-free one-pot solvothermal route. The volume ratio of deionized water (DI water) and diethylene glycol in solvothermal process is key to the formation of 3D BTA assembled by nanowire-coated TiO2 dendrites, which combines the advantages of 3D hierarchical structure and 1D nanoscale building blocks. Benefiting from such unique structural features, the BTA in full bloom achieved significantly increased specific surface areas and shortened Li(+) ion/electrons diffusion pathway. The lithium-ion batteries based on BTA in full bloom exhibited remarkably enhanced reversible specific capacity and rate performance, attributing to the high contact area with the electrolyte and the short solid state diffusion pathway for Li(+) ion/electrons promoting lithium insertion and extraction.