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  1. Abstract

    Continuous device downsizing and circuit complexity have motivated atomic-scale tuning of memristors. Herein, we report atomically tunable Pd/M1/M2/Al ultrathin (<2.5 nm M1/M2 bilayer oxide thickness) memristors using in vacuo atomic layer deposition by controlled insertion of MgO atomic layers into pristine Al2O3atomic layer stacks guided by theory predicted Fermi energy lowering leading to a higher high state resistance (HRS) and a reduction of oxygen vacancy formation energy. Excitingly, memristors with HRS and on/off ratio increasing exponentially with M1/M2 thickness in the range 1.2–2.4 nm have been obtained, illustrating tunneling mechanism and tunable on/off ratio in the range of 10–104. Further dynamic tunability of on/off ratio by electric field is possible by designing of the atomic M2 layer and M1/M2 interface. This result probes ways in the design of memristors with atomically tunable performance parameters.

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  2. Abstract

    Instability of colloidal iodine‐based inorganic perovskite CsPbX3(X = Cl, Br, I) nanocrystals (IPNCs) represents a major obstacle in lead‐halide IPNC research and application. Herein, a ligand‐anchoring process is reported that enables significantly improved colloidal stability of the iodine‐based IPNCs for over 10 months in ambient. Apart from the previous efforts in searching for strong binding ligands to cap the IPNCs to incrementally reduce the exposure of the IPNC surface to the harsh colloidal environment, the ligand‐anchoring method demonstrates that such an exposure can be reduced substantially by suppressing the dynamic ligand exchange around the colloidal IPNCs. In the IPNC synthesis solution with common oleic acid (OA) and oleylamine (OLA) ligands with relative weak binding to IPNCs, a systematic reduction of the ligand concentration using hexane by an order of magnitude has shown to be effective in achieving OA/OLA ligand‐anchored iodine‐based IPNCs with superior stability as confirmed in optical absorption, photoluminescence,1H solution nuclear magnetic resonance spectroscopy, and photoresponse. This result has revealed that the intermittent exposure of the IPNC surface during the dynamic ligand exchange is a primary mechanism underlying the colloidal IPNC instability, which can be resolved in the ligand‐anchoring process by suppressing such dynamic activities.

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  3. Abstract

    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 densityFpof 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 Ca0.3Y0.7Ba2Cu3O7x(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 enhancedFpvalue 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.

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  4. Abstract

    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.

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  5. Abstract

    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.

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  6. Abstract

    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.

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  7. Abstract

    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 minimaVDirac−andVDirac+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.

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  8. Abstract

    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.

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  9. Abstract This work examines the pinning enhancement in BaZrO 3 (BZO) +Y 2 O 3 doubly-doped (DD) YBa 2 Cu 3 O 7 (YBCO) nanocomposite multilayer (DD-ML) films. The film consists of two 10 nm thin Ca 0.3 Y 0.7 Ba 2 Cu 3 O 7-x (CaY-123) spacers stacking alternatively with three BZO + Y 2 O 3 /YBCO layers of 50 nm each in thickness that contain 3 vol% of Y 2 O 3 and BZO doping in the range of 2–6 vol%. Enhanced magnetic vortex pinning and improved pinning isotropy with respect to the orientation of magnetic field (B) have been achieved in the DD-ML samples at lower BZO doping as compared to that in the single-layer counterparts (DD-SL) without the CaY-123 spacers. For example, the pinning force density ( F p ) of ∼58 GNm −3 in 2 vol.% of DD-ML film is ∼110% higher than in 2 vol% of DD-SL at 65 K and B // c -axis, which is attributed to the improved pinning efficiency by c -axis aligned BZO nanorods through diffusion of Calcium (Ca) along the tensile-strained channels at BZO nanorods/YBCO interface for improvement of the interface microstructure and hence pinning efficiency of BZO nanorods. An additional benefit is in the considerably improved J c ( θ ) and reduced J c anisotropy in the former over the entire range of the B orientations. However, at higher BZO doping, the BZO nanorods become segmented and misoriented, which may change the Ca diffusion pathways and reduce the benefit of Ca in improving the pinning efficiency of BZO nanorods. 
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