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153 records · Page 9

Two-Dimensional Perovskite Single-Nanowire Photodetectors

High-performance microphotodetectors require materials that combine strong light–matter interaction, fast charge transport, and ambient stability. Here, we demonstrate single-nanowire devices based on the 2D perovskite (TPA3) 2 PbBr 4 , synthesized via a controlled slow-cooling self-assembly process that yields defect-minimized, anisotropic nanowires with smooth facets. These microphotodetectors exhibit ultralow dark currents (∼10 –15 A), high responsivity (up to 156 mA W –1 ), and exceptional specific detectivity (∼10 11 Jones) under near-UV (405 nm) illumination, with rise and fall times in the millisecond regime. The superior detectivity is primarily driven by the suppression of thermal noise through the material’s ultralow dark current, while the millisecond temporal response is governed by high-intensity trap-filling dynamics. The devices maintain stable operation over 4000 s of continuous on/off cycling and show remarkable ambient stability over weeks, attributed to dense crystal packing and robust organic cation layers. Furthermore, the influence of nanowire thickness on the charge collection efficiency is systematically elucidated through optical penetration depth analysis, highlighting design principles for optimizing low-dimensional perovskite photodetectors. This study introduces single 2D perovskite nanowires as a versatile platform for miniaturized, high-performance optoelectronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Giant optical nonlinearity of Fermi polarons in atomically thin semiconductors

In this study, realizing strong nonlinear optical responses is a long-standing goal of both fundamental and technological importance. Recently, substantial efforts have been focused on exploring excitons in solids to achieve nonlinearities even down to few-photon levels. However, a crucial tradeoff arises as strong light–matter interactions require large oscillator strength and short radiative lifetime of excitons, which limits their nonlinearity. Here we experimentally demonstrate strong nonlinear optical responses with large oscillator strength by exploiting the coupling between excitons and carriers in an atomically thin semiconductor. By controlling the electric field and electrostatic doping of trilayer WSe 2 , we observe the hybridization between intralayer and interlayer excitons and the formation of Fermi polarons. Substantial optical nonlinearity is observed under continuous-wave and pulsed laser excitation, where the Fermi polaron resonance blueshifts by as much as ~10 meV. Intriguingly, we observe a remarkable asymmetry in the optical nonlinearity between electron and hole doping, which is tunable by the applied electric field. We attribute these features to the optically induced valley polarization due to the interactions between excitons and free charges. Our results establish atomically thin heterostructures as a highly versatile platform for engineering nonlinear optical response with applications to classical and quantum optoelectronics.

2d materials↗

Non-perturbative cathodoluminescence microscopy of beam-sensitive materials

Cathodoluminescence microscopy is now a wellestablished and powerful tool for probing the photonic properties of nanoscale materials, but in many cases, nanophotonic materials are easily damaged by the electronbeam doses necessary to achieve reasonable cathodoluminescence signal-to-noise ratios. Two-dimensional materials have proven particularly susceptible to beam-induced modifications, yielding both obstacles to high spatial-resolution measurement and opportunities for beam-induced patterning of quantum photonic systems. Here pan-sharpening techniques are applied to cathodoluminescence microscopy in order to address these challenges and experimentally demonstrate the promise of pan-sharpening for minimally-perturbative high-spatial-resolution spectrum imaging of beam-sensitive materials.

2D materials↗

Liquid-like spin dynamics in a hybrid Heisenberg-Ising antiferromagnet

Two-dimensional (2D) materials and their heterostructures enable unconventional electronic properties and functionalities not accessible in their bulk counterparts. This approach is now being extended to magnetic materials to engineer their spin structures and magnetic fields produced by them. However, spin dynamics of 2D magnetic heterostructures remain largely unexplored. Here, we demonstrate that heterointerfacing Heisenberg square-lattice antiferromagnet (AF) Sr 2 IrO 4 with its bilayer variant Ising AF Sr 3 Ir 2 O 7 in a superlattice leads to liquid-like spin dynamics in the former, characterized by slow recovery of the AF order after its transient suppression by an optical pump, and complete absence of spin waves except in an immediate vicinity of the ordering wavevector. Instead, the spin excitation spectra are dominated by isotropic continua, which in previous works have been interpreted as fractional spin excitations, or spinons, that extends to unprecedentedly low energies. Thus, our results provide a pathway to frustrated magnetism in square lattices by heterointerfacing two distinct types of AFs.

RIXS↗

Direct Evidence of Photoinduced Charge Transport Mechanism in 2D Conductive Metal Organic Frameworks

Conductive metal organic frameworks (MOFs) represent a promising class of porous crystalline materials that have demon-strated potential in photo-electronics and photocatalytic applications. However, the lack of fundamental understanding on charge transport (CT) mechanism as well as the correlation of CT mechanism with their structure hampered their further development. Herein, we report the direct evidence of CT mechanism in 2D Cu-THQ MOFs and the correlation of temporal and spatial behaviors of charge carriers with their photoconductivity by combining three advanced spectroscopic methods including time resolved optical and X-ray absorption spectroscopy and terahertz spectroscopy. In addition to Cu-THQ, the CT in Cu/Zn-THQ after incorporating Zn2+ guest metal was also examined to uncover the contribution of through space pathway as the presence of the redox inactive 3d10 Zn2+ is expected to perturb the long range in-plane CT. We show that the hot carriers in Cu-THQ generated after photoexcitation are highly mobile and undergo fast localization to a lower energy state (cool carriers) with electrons occupying Cu center and holes in ligands. The cool carriers, which have super long lifetime (> 17 ns) are responsible for the long-term photoconductivity in Cu-THQ and transport through O-Cu-O motif with negligible contribution from interlayer ligand π-π stacking as incorporation of Zn2+ in Cu-THQ significantly reduced photoconductivi-ty. These unprecedent results not only demonstrate the capability to experimentally probe CT mechanism but also provide important insight in the rational design of 2D MOFs for photoelectronic and photocatalytic applications.

14 SOLAR ENERGY↗

Strain-Induced Growth of Twisted Bilayers during the Coalescence of Monolayer MoS 2 Crystals

Tailoring the grain boundaries (GBs) and twist angles between two-dimensional (2D) crystals are two crucial synthetic challenges to deterministically enable envisioned applications such as moiré excitons, emerging magnetism, or single-photon emission. Here, we reveal how twisted 2D bilayers can be synthesized from the collision and coalescence of two growing monolayer MoS 2 crystals during chemical vapor deposition. The twisted bilayer (TB) moiré angles are found to preserve the misorientation angle (θ) of the colliding crystals. The shapes of the TB regions are rationalized by a kink propagation model that predicts the GB formed by the coalescing crystals. Optical spectroscopy measurements reveal a θ-dependent long-range strain in crystals with stitched grain boundaries and a sharp (θ > 20°) threshold for the appearance of TBs, which relieves this strain. Reactive molecular dynamics simulations explain this strain from the continued growth of the crystals during coalescence due to the insertion of atoms at unsaturated defects along the GB, a process that self-terminates when the defects become saturated. The simulations also reproduce atomic-resolution electron microscopy observations of faceting along the GB, which is shown to arise from the growth-induced long-range strain. These facets align with the axes of the colliding crystals to provide favorable nucleation sites for second-layer growth of a TB with twist angles that preserve the misorientation angle θ. This interplay between strain generation and aligned nucleation provides a synthetic pathway for the growth of TBs with deterministic angles.

2D materials↗

Dehydration Pathway Study of Ultrathin Ni (OH) 2 Probed via In Situ X-Ray Photoelectron Spectromicroscopy

In this work, the conversion of ultrathin 2D-Ni (OH) 2 to NiO is studied using in situ X-ray absorption near edge spectroscopy at the Ni L 3 and O K edges and using variable photon energy X-ray photoelectron spectroscopy at the Ni 2p 3/2 and O 1s edges. The Ni L 3 X-ray absorption spectroscopy and corresponding 2p 3/2 X-ray photoelectron spectroscopy show the oxidation state of the Ni atom to be Ni 2+ in the course of the reaction; however, the film surface and oxygen defect structure show the presence of a large metallic Ni component before the complete disappearance of the hydroxide phase indicating oxygen vacancy formation before the completion of water desorption. O 1s spectral changes during heat treatment under ultrahigh vacuum, O 2 dosing, and H 2 O dosing suggest the spectral features are due to water desorption and adsorption. Furthermore, by comparing the relative probe depths of X-ray photoelectron spectroscopy and X-ray absorption spectroscopy, it is determined that the surface, at each step in the dehydration process, consists of a combination of Ni, NiO, and Ni (OH) 2 phases, which each contain a mixture of adsorbed hydroxyl groups. Repeated dosing with H 2 O, studied with O 1s X-ray photoelectron spectroscopy, suggests that the dissociation of water facilitates the formation of oxygen vacancies.

36 MATERIALS SCIENCE↗

Directing the adsorption and assembly of laponite nano-discs at oil–water interfaces

Achieving tunable controls on the adsorption and self-assembly of nanoscale building blocks at immiscible fluid interfaces is essential for synthesizing advanced materials, stabilizing emulsions, and the sustainable storage and recovery of fluids. Although extensive efforts have been directed toward resolving the assembly of spherical nanoparticles at water–hydrocarbon interfaces, 2D nanoparticles have received far less attention. In this study, we developed novel controls to direct the adsorption and assembly of 2D laponite nano-discs (diameter = ∼30 nm and thickness = ∼1 nm) at water–heptane interfaces using traces of sodium dodecyl sulfate (SDS) surfactant, demonstrated by advanced in situ small-angle X-ray scattering, atomic force microscopy, spinning drop tensiometer measurements and molecular dynamics simulations. The results show that SDS surfactant displaces the adsorbed laponite nano-discs from the interface toward the aqueous phase. The extent of this displacement increases with SDS concentration such that high SDS concentrations convert laponite-rich interfaces to SDS-rich interfaces free of laponite nano-discs. This transformation is associated with significant alterations in the rheological and nanomechanical properties of the host interface. In this context, reduction in interfacial tension and interfacial stiffness and an increase in the interfacial deformation is observed on increasing the SDS concentration from 0 to 0.1 wt%. The displacement of laponite nano-discs from the interface is driven by strong electrostatic interactions between the hydrophilic SDS group and interfacial water molecules. These studies unlock new insights into the adsorption and assembly of 2D nanoscale particles at water–hydrocarbons interfaces that are relevant for various applications related to energy and environmental science and engineering.

interfacial tension↗

Au assisted smooth ultrathin epitaxial ZnO film grown by pulsed laser deposition on sapphire(0001)

High quality ZnO has applications in photonics and electronics. Literature has shown that continuous, but rough ZnO film can be grown on sapphire substrate by pulsed laser deposition (PLD). In this work, ZnO and Au were co-deposited by PLD on sapphire(0001) substrates from a single ZnO target overlaid with an Au strip that serves as a catalyst. The reflection high-energy electron diffraction (RHEED) patterns show paired double stripes from sample of ZnO-Au where the difference of in-plane lattice parameters between ZnO and Au is 11.4 %. The two-dimensional (2D) reciprocal space maps constructed from azimuthal RHEED (ARHEED) patterns reveal parallel epitaxial relationship between ZnO and Au in the continuous ZnO-Au film on sapphire substrate. Transmission electron microscopy (TEM) cross section images and energy dispersive spectroscopy maps show a minute amount of Au nanocrystals distributed in the entire ultrathin ZnO film. Atomic force microscopy shows the root-mean-square roughness of the surface of ultrathin ZnO film with Au is in the sub-nm range. The ARHEED and TEM results show that a couple of atomic percentages of Au co-deposited with ZnO catalyzes the growth of smooth ultrathin epitaxial ZnO film.

36 MATERIALS SCIENCE↗