Atomic-Scale Interfacial Band Mapping across Vertically Phased-Separated Polymer/Fullerene Hybrid Solar Cells

Using cross-sectional scanning tunneling microscope (XSTM) with samples cleaved in situ in an ultrahigh vacuum chamber, this study demonstrates the direct visualization of high-resolution interfacial band mapping images across the film thickness in an optimized bulk heterojunction polymer solar cell consisting of nanoscale phase segregated blends of poly­(3-hexylthiophene) (P3HT) and [6,6]-phenyl C61 butyric acid methyl ester (PCBM). We were able to achieve the direct observation of the interfacial band alignments at the donor (P3HT)-acceptor (PCBM) interfaces and at the interfaces between the photoactive P3HT:PCBM blends and the poly­(3,4-ethylenedioxythiophene) poly­(styrenesulfonate) (PEDOT:PSS) anode modification layer with an atomic-scale spatial resolution. The unique advantage of using XSTM to characterize polymer/fullerene bulk heterojunction solar cells allows us to explore simultaneously the quantitative link between the vertical morphologies and their corresponding local electronic properties. This provides an atomic insight of interfacial band alignments between the two opposite electrodes, which will be crucial for improving the efficiencies of the charge generation, transport, and collection and the corresponding device performance of polymer solar cells

Dopant Diffusion and Activation in Silicon Nanowires Fabricated by ex Situ Doping: A Correlative Study via Atom-Probe Tomography and Scanning Tunneling Spectroscopy

Dopants play a critical role in modulating the electric properties of semiconducting materials, ranging from bulk to nanoscale semiconductors, nanowires, and quantum dots. The application of traditional doping methods developed for bulk materials involves additional considerations for nanoscale semiconductors because of the influence of surfaces and stochastic fluctuations, which may become significant at the nanometer-scale level. Monolayer doping is an ex situ doping method that permits the post growth doping of nanowires. Herein, using atom-probe tomography (APT) with subnanometer spatial resolution and atomic-ppm detection limit, we study the distributions of boron and phosphorus in ex situ doped silicon nanowires with accurate control. A highly phosphorus doped outer region and a uniformly boron doped interior are observed, which are not predicted by criteria based on bulk silicon. These phenomena are explained by fast interfacial diffusion of phosphorus and enhanced bulk diffusion of boron, respectively. The APT results are compared with scanning tunneling spectroscopy data, which yields information concerning the electrically active dopants. Overall, comparing the information obtained by the two methods permits us to evaluate the diffusivities of each different dopant type at the nanowire oxide, interface, and core regions. The combined data sets permit us to evaluate the electrical activation and compensation of the dopants in different regions of the nanowires and understand the details that lead to the sharp p–i–n junctions formed across the nanowire for the ex situ doping process

Atomically Resolved Electronic States and Correlated Magnetic Order at Termination Engineered Complex Oxide Heterointerfaces

We map electronic states, band gaps, and interface-bound charges at termination-engineered BiFeO₃/La_0.7Sr_0.3MnO₃ interfaces using atomically resolved cross-sectional scanning tunneling microscopy. We identify a delicate interplay of different correlated physical effects and relate these to the ferroelectric and magnetic interface properties tuned by engineering the atomic layer stacking sequence at the interfaces. This study highlights the importance of a direct atomically resolved access to electronic interface states for understanding the intriguing interface properties in complex oxides

Spatially Resolved Imaging on Photocarrier Generations and Band Alignments at Perovskite/PbI₂ Heterointerfaces of Perovskite Solar Cells by Light-Modulated Scanning Tunneling Microscopy

The presence of the PbI₂ passivation layers at perovskite crystal grains has been found to considerably affect the charge carrier transport behaviors and device performance of perovskite solar cells. This work demonstrates the application of a novel light-modulated scanning tunneling microscopy (LM-STM) technique to reveal the interfacial electronic structures at the heterointerfaces between CH₃NH₃PbI₃ perovskite crystals and PbI₂ passivation layers of individual perovskite grains under light illumination. Most importantly, this technique enabled the first observation of spatially resolved mapping images of photoinduced interfacial band bending of valence bands and conduction bands and the photogenerated electron and hole carriers at the heterointerfaces of perovskite crystal grains. By systematically exploring the interfacial electronic structures of individual perovskite grains, enhanced charge separation and reduced back recombination were observed when an optimal design of interfacial PbI₂ passivation layers consisting of a thickness less than 20 nm at perovskite crystal grains was applied

Hysteresis-Free Contact Doping for High-Performance Two-Dimensional Electronics

Contact doping is considered crucial for reducing the contact resistance of two-dimensional (2D) transistors. However, a process for achieving robust contact doping for 2D electronics is lacking. Here, we developed a two-step doping method for effectively doping 2D materials through a defect-repairing process. The method achieves strong and hysteresis-free doping and is suitable for use with the most widely used transition-metal dichalcogenides. Through our method, we achieved a record-high sheet conductance (0.16 mS·sq–1 without gating) of monolayer MoS2 and a high mobility and carrier concentration (4.1 × 1013 cm–2). We employed our robust method for the successful contact doping of a monolayer MoS2 Au-contact device, obtaining a contact resistance as low as 1.2 kΩ·μm. Our method represents an effective means of fabricating high-performance 2D transistors

Giant Photoresponse in Quantized SrRuO₃ Monolayer at Oxide Interfaces

The photoelectric effect in semiconductors is the main mechanism for most modern optoelectronic devices, in which the adequate bandgap plays the key role for acquiring high photoresponse. Among numerous material categories applied in this field, the complex oxides exhibit great possibilities because they present a wide distribution of band gaps for absorbing light with any wavelength. Their physical properties and lattice structures are always strongly coupled and sensitive to light illumination. Moreover, the confinement of dimensionality of the complex oxides in the heterostructures can provide more diversities in designing and modulating the band structures. On the basis of this perspective, we have chosen itinerary ferromagnetic SrRuO₃ as the model material, and fabricated it in one-unit-cell thickness in order to open a small band gap for effective utilization of visible light. By inserting this SrRuO₃ monolayer at the interface of the well-developed two-dimensional electron gas system (LaAlO₃/SrTiO₃), the resistance of the monolayer can be further revealed. In addition, a giant enhancement (>300%) of photoresponse under illumination of visible light with power density of 500 mW/cm² is also observed. Such can be ascribed to the further modulation of band structure of the SrRuO₃ monolayer under the illumination, confirmed by cross-section scanning tunneling microscopy (XSTM). Therefore, this study demonstrates a simple route to design and explore the potential low dimensional oxide materials for future optoelectronic devices