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BaZrO₃(BZO) one-dimensional artificial pinning centers (1D-APCs) aligned along thec-axis of the YBa₂Cu₃O₇(YBCO) have been adopted to enhance the magnetic vortex pinning in BZO/YBCO nanocomposite films. However, the pinning force densityF_pof the BZO 1D-APCs remains moderate at temperatures near 77 K. A hypothesis of the major limiting factor is the defective BZO 1D-APCs/YBCO interface as a direct consequence of the large interfacial strain originated from the BZO/YBCO lattice mismatch of ∼7.7%. Herein, we explore enlarging thec-axis of the YBCO dynamically to reduce the lattice mismatch and hence to prevent formation of the defective BZO 1D-APCs/YBCO interface. Specifically, thec-axis enlargement was achieved by partial replacement of Cu with Ca on the YBCO lattice using strain-directed Ca diffusion into YBCO from two Ca_0.3Y_0.7Ba₂Cu₃O_7−x(CaY-123) spacers of only 10 nm in thickness inserted into the 2 vol% BZO 1D-APC/YBCO nanocomposite thin films of ∼150 nm in total thickness. The achieved elongatedc-axis is attributed to the formation of stacking faults induced by Ca-replacement of Cu on YBCO lattice. The reduced BZO/YBCO lattice mismatch allows formation of a coherent BZO 1D-APC/YBCO interface with negligible defects. This leads to an enhancedF_pvalue up to 98 GN m⁻³at 65 K, which is 70% higher than that of the reference 2 vol% BZO 1D-APC/YBCO sample. Furthermore, the benefit of the enhanced pinning of the BZO 1D-APCs with a coherent interface with YBCO can be extended to a large angular range of the magnetic field orientation. This study reveals the significant effect of the BZO/YBCO interface on the pinning efficiency of BZO 1D-APCs and provides a promising approach to achieve a coherent interface in BZO/YBCO nanocomposite films.

Localized surface plasmon resonance (LSPR) is shown to be effective in trapping light for enhanced light absorption and hence performance in photonic and optoelectronic devices. Implementation of LSPR in all‐inorganic perovskite nanocrystals (PNCs) is particularly important considering their unique advantages in optoelectronics. Motivated by this, the first success in colloidal synthesis of AuCu/CsPbCl₃core/shell PNCs and observation of enhanced light absorption by the perovskite CsPbCl₃shell of thickness in the range of 2–4 nm, enabled by the LSPR AuCu core of an average diameter of 7.1 nm, is reported. This enhanced light absorption leads to a remarkably enhanced photoresponse in PNCs/graphene nanohybrid photodetectors using the AuCu/CsPbCl₃core/shell PNCs, by more than 30 times as compared to the counterparts with CsPbCl₃PNCs only (8–12 nm in dimension). This result illustrates the feasibility in implementation of LSPR light trapping directly in core/shell PNCs for high‐performance optoelectronics.

Cation–π interactions between molecules and graphene are known to have a profound effect on the properties of the molecule/graphene nanohybrids and motivate this study to quantify the attachment of the rhodamine 6G (R6G) dye molecules on graphene and the photocarrier transfer channel formed across the R6G/graphene interface. By increasing the R6G areal density of the R6G on graphene field‐effect transistor (GFET) from 0 up to ≈3.6 × 10¹³cm⁻², a linear shift of the Dirac point of the graphene from originally 1.2 V (p‐doped) to −1 V (n‐doped) is revealed with increasing number of R6G molecules. This indicates that the attachment of the R6G molecules on graphene is determined by the cation–π interaction between the NH+ in R6G and π electrons in graphene. Furthermore, a linear dependence of the photoresponse on the R6G molecule concentration to 550 nm illumination is observed on the R6G/graphene nanohybrid, suggesting that the cation–π interaction controls the R6G attachment configuration to graphene to allow formation of identical photocarrier transfer channels. On R6G/graphene nanohybrid with 7.2 × 10⁷R6G molecules, high responsivity up to 5.15 × 10²A W⁻¹is obtained, suggesting molecule/graphene nanohybrids are promising for high‐performance optoelectronics.

Van der Waals (vdW) heterostructures of 2D atomically thin layered materials (2DLMs) provide a unique platform for constructing optoelectronic devices by staking 2D atomic sheets with unprecedented functionality and performance. A particular advantage of these vdW heterostructures is the energy band engineering of 2DLMs to achieve interlayer excitons through type‐II band alignment, enabling spectral range exceeding the cutoff wavelengths of the individual atomic sheets in the 2DLM. Herein, the high performance of GaTe/InSe vdW heterostructures device is reported. Unexpectedly, this GaTe/InSe vdWs p–n junction exhibits extraordinary detectivity in a new shortwave infrared (SWIR) spectrum, which is forbidden by the respective bandgap limits for the constituent GaTe (bandgap of ≈1.70 eV in both the bulk and monolayer) and InSe (bandgap of ≈1.20–1.80 eV depending on thickness reduction from bulk to monolayer). Specifically, the uncooled SWIR detectivity is up to ≈10¹⁴Jones at 1064 nm and ≈10¹²Jones at 1550 nm, respectively. This result indicates that the 2DLM vdW heterostructures with type‐II band alignment produce an interlayer exciton transition, and this advantage can offer a viable strategy for devising high‐performance optoelectronics in SWIR or even longer wavelengths beyond the individual limitations of the bandgaps and heteroepitaxy of the constituent atomic layers.

Two‐dimensional transition metal dichalcogenides (TMDs)/graphene van der Waals (vdW) heterostructures integrate the superior light–solid interaction in TMDs and charge mobility in graphene, and therefore are promising for surface‐enhanced Raman spectroscopy (SERS). Herein, a novel TMD (MoS₂and WS₂) nanodome/graphene vdW heterostructure SERS substrate, on which an extraordinary SERS sensitivity is achieved, is reported. Using fluorescent Rhodamine 6G (R6G) as probe molecules, the SERS sensitivity is in the range of 10⁻¹¹to 10⁻¹²mon the TMD nanodomes/graphene vdW heterostructure substrates using 532 nm Raman excitation, which is comparable to the best sensitivity reported so far using plasmonic metal nanostructures/graphene SERS substrates, and is more than three orders of magnitude higher than that on single‐layer TMD and graphene substrates. Density functional theory simulation reveals enhanced electric dipole moments and dipole–dipole interaction at the TMD/graphene vdW interface, yielding an effective means to facilitate an external electrostatic perturbation on the graphene surface and charge transfer. This not only promotes chemical enhancement on SERS, but also enables electromagnetic enhancement of SERS through the excitation of localized surface plasmonic resonance on the TMD nanodomes. This TMD nanodome/graphene vdW heterostructure is therefore promising for commercial applications in high‐performance optoelectronics and sensing.

Graphene, a single layer conductor, can be combined with other functional materials for building efficient optoelectronic devices. However, transferring large‐area graphene onto another material often involves dipping the material into water and other solvents. This process is incompatible with water‐sensitive materials such as organometal halide perovskites. Here, a dry method is used and succeeded, for the first time, in stacking centimeter‐sized graphene directly onto methylammonium lead iodide thin films without exposing the perovskite film to any liquid. Photoemission spectroscopy and nanosecond time‐resolved photoelectrical measurement show that the graphene/perovskite interface does not contain significant amount of contaminants and sustain efficient interfacial electron transfer. The use of this method in fabricating graphene‐on‐perovskite photodetectors is further demonstrated. Besides a better photoresponsivity compared to detectors fabricated by the conventional perovskite‐on‐graphene structure, this dry transfer method provides a scalable pathway to incorporate graphene in multilayer devices based on water‐sensitive materials.

Lateral p–n junctions take the unique advantages of 2D materials, such as graphene, to enable single‐atomic layer microelectronics. A major challenge in fabrication of the lateral p–n junctions is in the control of electronic properties on a 2D atomic sheet with nanometer precision. Herein, a facile approach that employs decoration of molecular anions of bis‐(trifluoromethylsulfonyl)‐imide (TFSI) to generate p‐doping on the otherwise n‐doped graphene by positively polarized surface electric dipoles (pointing toward the surface) formed on the surface oxygen‐deficient layer “intrinsic” to an oxide ferroelectric back gate is reported. The characteristic double conductance minimaV_Dirac−andV_Dirac+illustrated in the obtained lateral graphene p–n junctions can be tuned in the range of −1 to 0 V and 0 to +1 V, respectively, by controlling the TFSI anions and surface dipoles quantitatively. The unique advantage of this approach is in adoption of polarity‐controlled molecular ion attachment on graphene, which could be further developed for various lateral electronics on 2D materials.

2D atomic sheets of transition metal dichalcogenides (TMDs) have a tremendous potential for next‐generation optoelectronics since they can be stacked layer‐by‐layer to form van der Waals (vdW) heterostructures. This allows not only bypassing difficulties in heteroepitaxy of lattice‐mismatched semiconductors of desired functionalities but also providing a scheme to design new optoelectronics that can surpass the fundamental limitations on their conventional semiconductor counterparts. Herein, a novel 2D h‐BN/p‐MoTe₂/graphene/n‐SnS₂/h‐BN p–g–n junction, fabricated by a layer‐by‐layer dry transfer, demonstrates high‐sensitivity, broadband photodetection at room temperature. The combination of the MoTe₂and SnS₂of complementary bandgaps, and the graphene interlayer provides a unique vdW heterostructure with a vertical built‐in electric field for high‐efficiency broadband light absorption, exciton dissociation, and carrier transfer. The graphene interlayer plays a critical role in enhancing sensitivity and broadening the spectral range. An optimized device containing 5−7‐layer graphene has been achieved and shows an extraordinary responsivity exceeding 2600 A W⁻¹with fast photoresponse and specific detectivity up to ≈10¹³Jones in the ultraviolet–visible–near‐infrared spectrum. This result suggests that the vdW p–g–n junctions containing multiple photoactive TMDs can provide a viable approach toward future ultrahigh‐sensitivity and broadband photonic detectors.