Hanying Li

High-Mobility Field-Effect Transistors from Large-Area Solution-Grown Aligned C60 Single Crystals

Field-effect transistors based on single crystals of organic semiconductors have the highest reported charge carrier mobility among organic materials, demonstrating great potential of organic semiconductors for electronic applications. However, single-crystal devices are difficult to fabricate. One of the biggest challenges is to prepare dense arrays of single crystals over large-area substrates with controlled alignment. Here, we describe a solution processing method to grow large arrays of aligned C(60) single crystals. Our well-aligned C(60) single-crystal needles and ribbons show electron mobility as high as 11 cm(2)V(-1)s(-1) (average mobility: 5.2 ± 2.1 cm(2)V(-1)s(-1) from needles; 3.0 ± 0.87 cm(2)V(-1)s(-1) from ribbons). This observed mobility is ~8-fold higher than the maximum reported mobility for solution-grown n-channel organic materials (1.5 cm(2)V(-1)s(-1)) and is ~2-fold higher than the highest mobility of any n-channel organic material (~6 cm(2)V(-1)s(-1)). Furthermore, our deposition method is scalable to a 100 mm wafer substrate, with around 50% of the wafer surface covered by aligned crystals. Hence, our method facilitates the fabrication of large amounts of high-quality semiconductor crystals for fundamental studies, and with substantial improvement on the surface coverage of crystals, this method might be suitable for large-area applications based on single crystals of organic semiconductors.

Enhanced Photovoltaic Performance of CH3NH3PbI3 Perovskite Solar Cells through Interfacial Engineering Using Self-Assembling Monolayer

Morphology control is critical to achieve high efficiency CH3NH3PbI3 perovskite solar cells (PSC). The surface properties of the substrates on which crystalline perovskite thin films form are expected to affect greatly the crystallization and, thus, the resulting morphology. However, this topic is seldom examined in PSC. Here we developed a facile but efficient method of modifying the ZnO-coated substrates with 3-aminopropanioc acid (C3-SAM) to direct the crystalline evolution and achieve the optimal morphology of CH3NH3PbI3 perovskite film. With incorporation of the C3-SAM, highly crystalline CH3NH3PbI3 films were formed with reduced pin-holes and trap states density. In addition, the work function of the cathode was better aligned with the conduction band minimum of perovskite for efficient charge extraction and electronic coupling. As a result, the PSC performance remarkably increased from 9.81(±0.99)% (best 11.96%) to 14.25(±0.61)% (best 15.67%). We stress the importance of morphology control through substrate surface modification to obtain the optimal morphology and device performance of PSC, which should generate an impact on developing highly efficient PSC and future commercialization.

Visualizing the 3D internal structure of calcite single crystals grown in agarose hydrogels.

Crystal Growing Kit For single crystals to remain intact, there is a limit to the size and number of defects that can be included before the underlying lattice is destroyed. Biological crystals, however, are known to include large macromolecules. H. Li et al. (p. 1244; see the Perspective by Hollingsworth) used electron tomography to study the crystallization of calcium carbonate inside an agarose gel, observing that the crystals physically entrapped the agarose macromolecules. To accommodate the curvature induced by the polymer chains, both high- and low-energy facets formed at the fiber-crystal interfaces. Thus, physical interactions alone may be sufficient for the incorporation of macromolecules in biological crystals and it may be possible to grow unusually shaped single crystals. Electron tomography shows that physical interactions may be sufficient to incorporate macromolecules into a calcite crystal. Single crystals are usually faceted solids with homogeneous chemical compositions. Biogenic and synthetic calcite single crystals, however, have been found to incorporate macromolecules, spurring investigations of how large molecules are distributed within the crystals without substantially disrupting the crystalline lattice. Here, electron tomography reveals how random, three-dimensional networks of agarose nanofibers are incorporated into single crystals of synthetic calcite by allowing both high- and low-energy fiber/crystal interface facets to satisfy network curvatures. These results suggest that physical entrapment of polymer aggregates is a viable mechanism by which macromolecules can become incorporated inside inorganic single crystals. As such, this work has implications for understanding the structure and formation of biominerals as well as toward the development of new high–surface area, single-crystal composite materials.

High-performance transistors and complementary inverters based on solution-grown aligned organic single-crystals.

Constructing a complementary inverter is technically more complex because both pand n-channel transistors are required to be patterned onto a common substrate. Here, we report a simple solution processing method to fabricate complementary inverters based on n-channel C 60 single crystals and p-channel 6,13-bis(triisopropyl-silylethynyl) pentacene (TIPS-pentacene) single crystals. We achieved a signal gain as high as 155. Hence, this work provides a platform to study high-performance complementary circuits based on organic single-crystals. Organic FETs have been widely used for electronic applications such as displays [ 5 , 6 ] and sensors. [ 7–9 ] Organic single-crystals show the best FET performance with the highest charge mobility among organic materials. The p-channel organic single-crystal FETs have exhibited hole mobility as high as 40 cm 2 V − 1 s − 1 , [ 10–14 ]

A facile room-temperature chemical reduction method to TiO2@CdS core/sheath heterostructure nanowires

We have prepared functional TiO2@CdS core/sheath heterostructure nanowires using a simple chemical reduction method at room temperature. The core/sheath nanowires were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD) and UV-visible spectroscopic techniques. It was found that the thickness of the CdS sheath could be controlled by the concentration of the precursors. The continuous and polycrystalline CdS outer layer could be formed on the TiO2 nanowires when the concentration of the S precursor was higher than 0.2 mmol. A possible multi-site growth mechanism of the formation of the composite nanowires was proposed.

Design of a versatile interconnecting layer for highly efficient series-connected polymer tandem solar cells

A versatile interconnecting layer (ICL) based on reflective ultra-thin Ag (8–14 nm) was developed to enable the fabrication of a series-connected micro-cavity tandem polymer solar cell. This novel ICL can manipulate the optical field distribution between the constituent sub-cells to address the challenge of current matching. As a result, a very high power conversion efficiency (∼11%) and high summed external quantum efficiency of >90% were demonstrated.

C–H activation: making diketopyrrolopyrrole derivatives easily accessible

Diketopyrrolopyrrole (DPP) derivatives are an important class of high-performance pigment used in inks, paints, plastics, and organic electronics. Until now, DPP derivatives containing sophisticated aryl units at the DPP core have usually been obtained via Suzuki, Stille, or Negishi cross-coupling reactions, which require organometallic precursors. In this work, a series of DPP-based π-conjugated molecules bearing diverse aryl substituents on the thiophene- or benzene-DPPs were facilely synthesized in moderate to excellent yields through the Pd-catalyzed direct arylation of C–H bonds. The synthetic procedures feature advantages over traditional C–C cross-coupling reactions such as: (1) avoidance of the use of organometallic reagents in the starting materials leading to simpler byproducts and higher atom economy, (2) fewer synthetic steps, (3) higher yields, (4) better compatibility with chemically sensitive functional groups, and (5) simpler catalytic systems free of phosphine ligands. These advantages make the present protocol an ideal and versatile strategy for the synthesis of DPP derivatives, especially for structurally complicated DPPs that may possess chemically sensitive functionalities. The optical and electrochemical properties of the synthesized DPPs (17 compounds) were systematically investigated using UV-vis spectroscopy, steady-state fluorescence spectroscopy, and cyclic voltammetry (CV).

Star-Shaped D–A Small Molecules Based on Diketopyrrolopyrrole and Triphenylamine for Efficient Solution-Processed Organic Solar Cells

Three star-shaped D-A small molecules, (P-DPP)(3)TPA, (4-FP-DPP)(3)TPA, and (4-BuP-DPP)(3)TPA were designed and synthesized with triphenylamine (TPA) as the core, diketopyrrolopyrrole (DPP) as the arm, and unsubstituted or substituted benzene rings (phenyl, P; 4-fluoro-phenyl, 4-FP; 4-n-butyl-phenyl, 4-BuP) as the end-group. All the three small molecules show relatively narrow optical band gaps (1.68-1.72 eV) and low-lying highest occupied molecular orbital (HOMO) energy levels (-5.09∼-5.13 eV), implying that they are potentially good electron donors for organic solar cells (OSCs). Then, photovoltaic properties of the small molecules blended with [6,6]-phenyl-C(61)-butyric acid methyl ester (PC(61)BM) as electron acceptor were investigated. Among three small molecules, the OSC based on (P-DPP)(3)TPA:PCBM blend exhibits a best power conversion efficiency (PCE) of 2.98% with an open-circuit voltage (V(oc)) of 0.72 V, a short-circuit current density (J(sc)) of 7.94 mA/cm(2), and a fill factor (FF) of 52.2%, which may be ascribed to the highest hole mobility of (P-DPP)(3)TPA.

Low temperature solution processed planar heterojunction perovskite solar cells with a CdSe nanocrystal as an electron transport/extraction layer

A cadmium selenide (CdSe) nanocrystal was used as an electron transport/extraction layer for perovskite solar cells due to its high electron mobility and solution-processability at low temperatures. Power conversion efficiency (PCE) up to 11.7% was achieved under standard AM1.5G conditions in air.

Solution-grown organic single-crystalline p-n junctions with ambipolar charge transport.

Organic single-crystalline p-n junctions are grown from mixed solutions. First, C60 crystals (n-type) form and, subsequently, C8-BTBT crystals (p-type) nucleate heterogeneously on the C60 crystals. Both crystals continue to grow simultaneously into single-crystalline p-n junctions that exhibit ambipolar charge transport characteristics. This work provides a platform to study organic single-crystalline p-n junctions.