Interlayer Charge Transfer Induced Electrical Behavior Transition in 1D AgI@sSWCNT van der Waals Heterostructures.

The emergence of one-dimensional van der Waals heterostructures (1D vdWHs) opens up potential fields with unique properties, but precise synthesis remains a challenge. The utilization of mixed conductive types of carbon nanotubes as templates has imposed restrictions on the investigation of the electrical behavior and interlayer interaction of 1D vdWHs. In this study, we efficiently encapsulated silver iodide in high-purity semiconducting single-walled carbon nanotubes (sSWCNTs), forming 1D AgI@sSWCNT vdWHs. We characterized the semiconductor-metal transition and increased the carrier concentration of individual AgI@sSWCNTs via sensitive dielectric force microscopy and confirmed the results through electrical device tests. The electrical behavior transition was attributed to an interlayer charge transfer, as demonstrated by Kelvin probe force microscopy. Furthermore, we showed that this method of synthesizing 1D heterostructures can be extended to other metal halides. This work opens the door for the further exploration of the electrical properties of 1D vdWHs.

Identification of the conductivity type of single-walled carbon nanotubes via dual-modulation dielectric force microscopy.

The conductivity type is one of the most fundamental transport properties of semiconductors, which is usually identified by fabricating the field-effect transistor, the Hall-effect device, etc. However, it is challenging to obtain an Ohmic contact if the sample is down to nanometer-scale because of the small size and intrinsic heterogeneity. Noncontact dielectric force microscopy (DFM) can identify the conductivity type of the sample by applying a DC gate voltage to the tip, which is effective in tuning the accumulation or depletion of charge carriers. Here, we further developed a dual-modulation DFM, which simplified the conductivity type identification from multiple scan times under different DC gate voltages to a single scan under an AC gate voltage. Taking single-walled carbon nanotubes as testing samples, the semiconducting-type sample exhibits a more significant charge carrier accumulation/depletion under each half-period of the AC gate voltage than the metallic-type sample due to the stronger rectification effect. The charge carrier accumulation or depletion of the p-type sample is opposite to that of the n-type sample at the same half-period of the AC gate voltage because of the reversed charge carrier type.

In Operando Visualization of Interfacial Band Bending in Photomultiplying Organic Photodetectors.

Charge injection is a basic transport process that strongly affects performance of optoelectronic devices such as light-emitting diodes and photodetectors. In these devices, the charge injection barrier is related to the band bending at the active layer/electrode interface and exhibits sophisticated dependence on interface structure and device operating conditions, making it difficult to determine via either theoretical prediction or experimental measurements. Here, in operando cross-sectional scanning Kelvin probe microscopy (SKPM) has been applied in organic photodetectors to visualize the interfacial band bending. The photoinduced interfacial band bending becomes more significant with increasing reverse bias voltage, resulting in reduced charge injection barrier and facilitated charge injection. The photoinduced injection current is orders of magnitude higher than the photocurrent directly generated from light absorption and thus leads to significant photomultiplication. Furthermore, the interfacial structure is tuned to further enhance photoinduced interfacial band bending and the photomultiplication factor.

Quantitative amplitude-modulation scanning Kelvin probe microscopy via the second eigenmode excitation.

Amplitude modulation scanning Kelvin probe microscopy (AM-SKPM) is widely used to measure the contact potential difference (CPD) between probe and samples in ambient or dry inert atmosphere. However, AM-SKPM is generally considered quantitatively inaccurate due to crosstalk between the cantilever and the sample. Here we demonstrate that the accuracy of AM-SKPM-based CPD measurements is drastically improved by exciting the SKPM probe at its second eigenmode. In the second eigenmode of oscillation, there exists a stationary node at the cantilever towards its free end, across which the displacement bears opposite signs; therefore driving the SKPM probe at its second eigenmode helps to partially cancel the virtual work done by the cantilever and reduce the crosstalk effect. The improvement in accuracy is experimentally confirmed with interdigitating electrodes calibration samples as well as practical samples such as the cross-section of wafer-bonded GaAs/GaN heterojunction.

Reconfiguration of interfacial energy band structure for high-performance inverted structure perovskite solar cells.

Charged defects at the surface of the organic-inorganic perovskite active layer are detrimental to solar cells due to exacerbated charge carrier recombination. Here we show that charged surface defects can be benign after passivation and further exploited for reconfiguration of interfacial energy band structure. Based on the electrostatic interaction between oppositely charged ions, Lewis-acid-featured fullerene skeleton after iodide ionization (PCBB-3N-3I) not only efficiently passivates positively charged surface defects but also assembles on top of the perovskite active layer with preferred orientation. Consequently, PCBB-3N-3I with a strong molecular electric dipole forms a dipole interlayer to reconfigure interfacial energy band structure, leading to enhanced built-in potential and charge collection. As a result, inverted structure planar heterojunction perovskite solar cells exhibit the promising power conversion efficiency of 21.1% and robust ambient stability. This work opens up a new window to boost perovskite solar cells via rational exploitation of charged defects beyond passivation.

Efficiency above 12% for 1 cm2 Flexible Organic Solar Cells with Ag/Cu Grid Transparent Conducting Electrode.

With the rapid progress of organic solar cells (OSCs), improvement in the efficiency of large-area flexible OSCs (>1 cm2) is crucial for real applications. However, the development of the large-area flexible OSCs severely lags behind the growth of the small-area OSCs, with the electrical loss due to the large sheet resistance of the electrode being a main reason. Herein, a high conductive and high transparent Ag/Cu composite grid with sheet resistance <1 Ω sq-1 and an average visible light transparency of 84% is produced as the transparent conducting electrode of flexible OSCs. Based on this Ag/Cu composite grid electrode, a high efficiency of 12.26% for 1 cm2 flexible OSCs is achieved. The performances of large-area flexible OSCs also reach 7.79% (4 cm2) and 7.35% (9 cm2), respectively, which are much higher than those of the control devices with conventional flexible indium tin oxide electrodes. Surface planarization using highly conductive PEDOT:PSS and modification of the ZnO buffer layer by zirconium acetylacetonate (ZrAcac) are two necessary steps to achieve high performance. The flexible OSCs employing Ag/Cu grid have excellent mechanical bending resistance, maintaining high performance after bending at a radius of 2 mm.

Functional Scanning Force Microscopy for Energy Nanodevices.

Energy nanodevices, including energy conversion and energy storage devices, have become a major cross-disciplinary field in recent years. These devices feature long-range electron and ion transport coupled with chemical transformation, which call for novel characterization tools to understand device operation mechanisms. In this context, recent developments in functional scanning force microscopy techniques and their application in thin-film photovoltaic devices and lithium batteries are reviewed. The advantages of scanning force microscopy, such as high spatial resolution, multimodal imaging, and the possibility of in situ and in operando imaging, are emphasized. The survey indicates that functional scanning force microscopy is making significant contributions in understanding materials and interfaces in energy nanodevices.