Stability-limiting heterointerfaces of perovskite photovoltaics.

Optoelectronic devices consist of heterointerfaces formed between dissimilar semiconducting materials. The relative energy-level alignment between contacting semiconductors determinately affects the heterointerface charge injection and extraction dynamics. For perovskite solar cells (PSCs), the heterointerface between the top perovskite surface and a charge-transporting material is often treated for defect passivation1-4 to improve the PSC stability and performance. However, such surface treatments can also affect the heterointerface energetics1. Here we show that surface treatments may induce a negative work function shift (that is, more n-type), which activates halide migration to aggravate PSC instability. Therefore, despite the beneficial effects of surface passivation, this detrimental side effect limits the maximum stability improvement attainable for PSCs treated in this way. This trade-off between the beneficial and detrimental effects should guide further work on improving PSC stability via surface treatments.

An Asymmetry Field-Effect Phototransistor for Solving Large Exciton Binding Energy of 2D TMDCs.

The probing of fundamental photophysics is a key prerequisite for the construction of diverse optoelectronic devices and circuits. To date, though, photocarrier dynamics in 2D materials remains unclear, plagued primarily by two issues: a large exciton binding energy, and the lack of a suitable system that enables the manipulation of excitons. Here, a WSe2 -based phototransistor with an asymmetric split-gate configuration is demonstrated, which is named the "asymmetry field-effect phototransistor" (AFEPT). This structure allows for the effective modulation of the electric-field profile across the channel, thereby providing a standard device platform for exploring the photocarrier dynamics of the intrinsic WSe2 layer. By controlling the electric field, this work the spatial evolution of the photocurrent is observed, notably with a strong signal over the entire WSe2 channel. Using photocurrent and optical spectroscopy measurements, the physical origin of the novel photocurrent behavior is clarified and a room-temperature exciton binding energy of 210 meV is determined with the device. In the phototransistor geometry, lateral p-n junctions serve as a simultaneous pathway for both photogenerated electrons and holes, reducing their recombination rate and thus enhancing photodetection. The study establishes a new device platform for both fundamental studies and technological applications.

Direct tuning of graphene work function via chemical vapor deposition control.

Besides its unprecedented physical and chemical characteristics, graphene is also well known for its formidable potential of being a next-generation device material. Work function (WF) of graphene is a crucial factor in the fabrication of graphene-based electronic devices because it determines the energy band alignment and whether the contact in the interface is Ohmic or Schottky. Tuning of graphene WF, therefore, is strongly demanded in many types of electronic and optoelectronic devices. Whereas study on work function tuning induced by doping or chemical functionalization has been widely conducted, attempt to tune the WF of graphene by controlling chemical vapor deposition (CVD) condition is not sufficient in spite of its simplicity. Here we report the successful WF tuning method for graphene grown on a Cu foil with a novel CVD growth recipe, in which the CH4/H2 gas ratio is changed. Kelvin probe force microscopy (KPFM) verifies that the WF-tuned regions, where the WF increases by the order of ~250 meV, coexist with the regions of intrinsic WF within a single graphene flake. By combining KPFM with lateral force microscopy (LFM), it is demonstrated that the WF-tuned area can be manipulated by pressing it with an atomic force microscopy (AFM) tip and the tuned WF returns to the intrinsic WF of graphene. A highly plausible mechanism for the WF tuning is suggested, in which the increased graphene-substrate distance by excess H2 gases may cause the WF increase within a single graphene flake. This novel WF tuning method via a simple CVD growth control provides a new direction to manipulate the WF of various 2-dimensional nanosheets as well as graphene.

Probing the Importance of Charge Balance and Noise Current in WSe2/WS2/MoS2 van der Waals Heterojunction Phototransistors by Selective Electrostatic Doping.

Heterojunction structures using 2D materials are promising building blocks for electronic and optoelectronic devices. The limitations of conventional silicon photodetectors and energy devices are able to be overcome by exploiting quantum tunneling and adjusting charge balance in 2D p-n and n-n junctions. Enhanced photoresponsivity in 2D heterojunction devices can be obtained with WSe2 and BP as p-type semiconductors and MoS2 and WS2 as n-type semiconductors. In this study, the relationship between photocurrent and the charge balance of electrons and holes in van der Waals heterojunctions is investigated. To observe this phenomenon, a p-WSe2/n-WS2/n-MoS2 heterojunction device with both p-n and n-n junctions is fabricated. The device can modulate the charge carrier balance between heterojunction layers to generate photocurrent upon illumination by selectively applying electrostatic doping to a specific layer. Using photocurrent mapping, the operating transition zones for the device is demonstrated, allowing to accurately identify the locations where photocurrent generates. Finally, the origins of flicker and shot noise at the different semiconductor interfaces are analyzed to understand their effect on the photoresponsivity and detectivity of unit active area (2.5 µm2, λ = 405 nm) in the p-WSe2/n-WS2/n-MoS2 heterojunction device.

Two-dimensional semiconducting and single-crystalline antimony trioxide directly-grown on monolayer graphene.

The first successful synthesis and characterization of single-crystalline two-dimensional (2D) semiconducting antimony tri oxide (Sb2O3) by direct chemical vapor deposition (CVD) growth on monolayer graphene is presented herein. The Sb2O3 flakes on graphene are regular triangles with smooth edges and a thickness of ∼1.45 nm. The thickness dependence of the Raman spectra and scanning Kelvin probe microscopy (SKPM) were systematically studied.