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Creators/Authors contains: "Kong, Jing"

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  1. Abstract

    Van der Waals (vdW) ferroelectrics have attracted significant attention for their potential in next-generation nano-electronics. Two-dimensional (2D) group-IV monochalcogenides have emerged as a promising candidate due to their strong room temperature in-plane polarization down to a monolayer limit. However, their polarization is strongly coupled with the lattice strain and stacking orders, which impact their electronic properties. Here, we utilize four-dimensional scanning transmission electron microscopy (4D-STEM) to simultaneously probe the in-plane strain and out-of-plane stacking in vdW SnSe. Specifically, we observe large lattice strain up to 4% with a gradient across ~50 nm to compensate lattice mismatch at domain walls, mitigating defects initiation. Additionally, we discover the unusual ferroelectric-to-antiferroelectric domain walls stabilized by vdW force and may lead to anisotropic nonlinear optical responses. Our findings provide a comprehensive understanding of in-plane and out-of-plane structures affecting domain properties in vdW SnSe, laying the foundation for domain wall engineering in vdW ferroelectrics.

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    Free, publicly-accessible full text available December 1, 2024
  2. Memristors are promising candidates for constructing neural networks. However, their dissimilar working mechanism to that of the addressing transistors can result in a scaling mismatch, which may hinder efficient integration. Here, we demonstrate two-terminal MoS2 memristors that work with a charge-based mechanism similar to that in transistors, which enables the homogeneous integration with MoS2 transistors to realize one-transistor-one-memristor addressable cells for assembling programmable network. The homogenously integrated cells are implemented in a 2×2 network array to demonstrate the enabled addressability and programmability. The potential for assembling scalable network is evaluated in a simulated neural network using obtained realistic device parameters, which achieves over 91% pattern recognition accuracy. This study also reveals a generic mechanism and strategy that can be applied to other semiconducting devices for the engineering and homogeneous integration of memristive systems. 
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    Free, publicly-accessible full text available July 12, 2024
  3. Quantum multireference effects are associated with degeneracies and near-degeneracies of the ground state and are critical to a variety of systems. Most approximate functionals of density functional theory (DFT) fail to properly describe such effects. A number of diagnostics have been proposed to estimate in advance the reliability of a given single-reference solution in this respect. Some of these diagnostics, however, lack size-consistency while remaining computationally expensive. In this work, we propose the DFT method of atomic populations of effectively localized electrons (APELE) as a novel diagnostic in this vein. It is compared with existing diagnostics of nondynamic correlation on select exemplary systems. The APELE method is on average in good agreement with the popular T1 index, while being size-consistent and less costly. It becomes particularly informative in cases involving bond stretching or bond breaking. The APELE method is applied next to organic diradicals like the bis-acridine dimer and the p-quinodimethane molecule which possess unusually high nonlinear optical response, and to the reaction of ethylene addition to Ni dithiolene. Our results for this reaction are consistent with the T1 diagnostics and in addition, shed some light on the degree of d-electron localization at the Ni center. 
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  4. Abstract

    The development of compact and fieldable mid-infrared (mid-IR) spectroscopy devices represents a critical challenge for distributed sensing with applications from gas leak detection to environmental monitoring. Recent work has focused on mid-IR photonic integrated circuit (PIC) sensing platforms and waveguide-integrated mid-IR light sources and detectors based on semiconductors such as PbTe, black phosphorus and tellurene. However, material bandgaps and reliance on SiO2substrates limit operation to wavelengthsλ ≲ 4 μm. Here we overcome these challenges with a chalcogenide glass-on-CaF2PIC architecture incorporating split-gate photothermoelectric graphene photodetectors. Our design extends operation toλ = 5.2 μm with a Johnson noise-limited noise-equivalent power of 1.1 nW/Hz1/2, no fall-off in photoresponse up tof = 1 MHz, and a predicted 3-dB bandwidth off3dB > 1 GHz. This mid-IR PIC platform readily extends to longer wavelengths and opens the door to applications from distributed gas sensing and portable dual comb spectroscopy to weather-resilient free space optical communications.

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  6. Achieving large-size two-dimensional (2D) crystals is key to fully exploiting their remarkable functionalities and application potentials. Chemical vapor deposition growth of 2D semiconductors such as monolayer MoS 2 has been reported to be activated by halide salts, for which various investigations have been conducted to understand the underlying mechanism from different aspects. Here, we provide experimental evidence showing that the MoS 2 growth dynamics are halogen dependent through the Brønsted-Evans-Polanyi relation, based on which we build a growth model by considering MoS 2 edge passivation by halogens, and theoretically reproduce the trend of our experimental observations. These mechanistic understandings enable us to further optimize the fast growth of MoS 2 and reach record-large domain sizes that should facilitate practical applications. 
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