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Fluids under extreme confinement exhibit distinctly new properties compared to their bulk analogs. Understanding the structure and intermolecular bonding of confined water lays the foundation for creating and improving applications at the water-energy nexus. However, probing confined water experimentally at the length scale of intermolecular and surface forces has remained a challenge. Here, we report a combined experiment/theory framework to reveal changes in H-bonding environment and the underlying molecular structure of confined water inside individual carbon nanotubes. H-bonding is directly probed through the O-H stretch frequency with vibrational electron energy-loss spectroscopy and compared to spectra from molecular-dynamics simulations based on density-functional-theory. Experimental spectra show that water in larger carbon nanotubes exhibit the bonded O-H vibrations of bulk water, but at smaller diameters, the frequency blueshifts to near the 'free' O-H stretch found in water vapor and hydrophobic surfaces. The matching simulations reveal that, in addition to steric confinement, the tube's vibrations play a key role in breaking up the H-bond network, resulting in an orientationally-dispersed, non-H-bonded phase. Furthermore, the temperature-dependence of the vibrations is investigated, providing insights into phase transitions and the confined-water density. This research demonstrates the potential of the experiment/theory framework to explore unprecedented aspects of structure and bonding in confined fluids.

Four-dimensional scanning transmission electron microscopy (4D-STEM) has recently gained widespread attention for its ability to image atomic electric fields with sub-{\AA}ngstrom spatial resolution. These electric field maps represent the integrated effect of the nucleus, core electrons and valence electrons, and separating their contributions is non-trivial. In this paper, we utilized simultaneously acquired 4D-STEM center of mass (CoM) images and annular dark field (ADF) images to determine the electron charge density in monolayer MoS2. We find that both the core electrons and the valence electrons contribute to the derived electron charge density. However, due to blurring by the probe shape, the valence electron contribution forms a nearly featureless background while most of the spatial modulation comes from the core electrons. Our findings highlight the importance of probe shape in interpreting charge densities derived from 4D STEM.

Orchestration of diverse synaptic plasticity mechanisms across different timescales produces complex cognitive processes. To achieve comparable cognitive complexity in memristive neuromorphic systems, devices that are capable to emulate short- and long-term plasticity (STP and LTP, respectively) concomitantly are essential. However, this fundamental bionic trait has not been reported in any existing memristors where STP and LTP can only be induced selectively because of the inability to be decoupled using different loci and mechanisms. In this work, we report the first demonstration of truly concomitant STP and LTP in a three-terminal memristor that uses independent physical phenomena to represent each form of plasticity. The emerging layered material Bi2O2Se is used in memristor for the first time, opening up the prospects for ultra-thin, high-speed and low-power neuromorphic devices. The concerted action of STP and LTP in our memristor allows full-range modulation of the transient synaptic efficacy, from depression to facilitation, by stimulus frequency or intensity, providing a versatile device platform for neuromorphic function implementation. A recurrent neural circuitry model is developed to simulate the intricate "sleep-wake cycle autoregulation" process, in which the concomitance of STP and LTP is posited as a key factor in enabling this neural homeostasis. This work sheds new light on the highly sophisticated computational capabilities of memristors and their prospects for realization of advanced neuromorphic functions.

Bi2O2Se is an emerging semiconducting, air-stable layered material (Nat. Nanotechnol. 2017, 12, 530; Nano Lett. 2017, 17, 3021), potentially exceeding MoS2 and phosphorene in electron mobility and rivalling typical Van der Waals stacked layered materials in the next-generation high-speed and low-power electronics. Holding the promise of functional versatility, it is arousing rapidly growing interest from various disciplines, including optoelectronics, thermoelectronics and piezoelectronics. In this work, we comprehensively study the electrical properties of the native point defects in Bi2O2Se, as an essential step toward understanding the fundamentals of this material. The defect landscapes dependent on both Fermi energy and the chemical potentials of atomic constituents are investigated. Along with the bulk defect analysis, a complementary inspection of the surface properties, within the simple context of charge neutrality level model, elucidates the observed n-type characteristics of Bi2O2Se based FETs. This work provides important guide to engineer the defects of Bi2O2Se for desired properties, which is key to the successful application of this emerging layered material.