Unlocking Anion Reduction of Lithium Perchlorate via Electrochemically Coupled Oxygen Atom Transfer

The growing demand for high energy density electrochemical energy storage necessitates energy vectors that maximize the number of electrons transferred per formula unit of active material. Herein, we ...

pubs.acs.org

Stochastically Generated Digital Twins of 3D Solid‐State Electrolyte Architecture

A stochastic model and validation suite were developed to produce the highest fidelity computer-generated (Digital Twin) microstructures of random porous tape-cast solid-state battery architectures a....

advanced.onlinelibrary.wiley.com

Metal–Amide Chemistry Enables Controlled Heavy-Pnictogen Reduction for Colloidal III–V Nanocrystal Synthesis

Controlling heavy-pnictogen (As, Sb) redox chemistry remains a central challenge in RoHS-compliant III–V colloidal nanocrystal synthesis. The formation of pnictide nanocrystals, where pnictogen must r...

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Ligand-Engineered Methylammonium Lead Bromide Nanoplatelets: Single-Photon Emission and Strong Light-Matter Coupling

Lead halide perovskite nanoplatelets (LHP NPLs) are of immense interest in the materials science and optoelectronics communities owing to their strong quantum confinement leading to narrow emission pe...

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Anisotropic Exciton Transport in a Lamellar CsPbBr3 Nanocrystal Superlattice

Colloidal self-assembly is one strategy for engineering anisotropic properties into otherwise isotropic materials. In this work, we demonstrate anisotropic exciton transport in an A2B-type superlattic...

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Surface-Governed Photoredox Reactivity of CsPbBr3 Quantum Dots

Surface chemistry is central to the design of colloidal quantum dots (QDs) for photoredox catalysis, where charge transfer, access to active sites, and colloidal stability must be balanced. Using CsPb...

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Electrochemical Control over Electron Density of InAs Quantum Dots

Control over the electron density and conductivity is a cornerstone of semiconductor technology. Here, we report electrochemical control over electron density and conductivity in films of InAs colloidal quantum dots (QDs) capped with ethanedithiol ligands. The quantum-confined twofold degenerate 1S1/2(e) electron state can be reversibly and completely filled. Increasing the electron population yields four bleach features in the optical-absorption spectrum associated transitions to the 1S1/2(e) state, and state-resolved electronic conductivity which follows the 1S1/2(e) density of states, reaching a maximum of 0.45 S/m at 0.5 electrons per QD. The absence of 1P(e) bleach features and state-resolved conductivity imply a wide separation between the 1S1/2(e) and 1P(e) states resulting in electronic transport between 1S(e) states exclusively. The reversible electrochemistry of InAs QDs films allows determination of the absolute energy levels. InAs QDs of 4.2 nm in edge length and capped with ethanedithiol ligands are natively n-doped with the Fermi level at −4.6 eV, the 1S1/2(e) state at −4.28 eV and the 1S3/2(h) state at −5.54 eV vs vacuum. This work establishes a way to precisely control the charge carrier density and conductivity and gives insights into the charge transport properties and electronic structure of InAs QD films, opening the possibility of making devices with InAs QDs in which the charge carrier density is precisely controlled electrochemically.

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Noninvasive Quality Assessment of Melt-Grown Cesium Lead Bromide Perovskite by Nuclear Quadrupole Resonance Spectroscopy

Melt-grown, highly crystalline CsPbBr3 has been intensely investigated as a semiconductor for direct hard radiation detection. While the phase purity and crystallinity of the CsPbBr3 ingots are assess...

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Navigating the Catholyte Landscape in All-Solid-State Batteries

All-solid-state batteries are widely regarded as the next frontier in electrochemical energy storage, offering the potential to surpass the energy density and safety limits of conventional lithium-ion batteries. Among the factors governing their performance, paramount are the choice and functionality of the solid-state electrolyte (SSE) as a catholyte within the composite positive electrode. This perspective critically examines the applicability and potential of the three most intensively studied inorganic SSE families, namely oxides, sulfides, and chlorides, as catholytes. We discuss their respective advantages, limitations, and compatibility with common cathode active materials, as well as the remaining knowledge gaps. We then assess whether any of the current SSE classes can be employed as a stand-alone SSE for all-solid-state batteries, or whether composite architectures combining multiple SSEs will ultimately be required.

pubs.acs.org

Mitigating Ion Migration with Alternating Voltage for Stable Perovskite Image Sensors

Perovskite photodetectors have emerged as a potential replacement for silicon photodiodes in modern cameras due to their high sensitivity to visible light and ability to be easily integrated into existing electronics. However, the use of perovskite photodetectors in conventional CMOS image sensors requires the application of reverse bias, which can lead to unstable detector performance due to ion migration effects. In this article, we propose a new approach that involves the application of forward voltage pulses to attenuate ion migration while still enabling the capture of photocurrent under reverse bias. Our results show that using this technique after each cycle of signal integration allows for stable operation of perovskite photodetectors for over 180 h, while applying a constant reverse bias leads to degradation within just 10 min. Additionally, we demonstrate stable imaging using alternating voltage and 8 × 8 crossbar arrays of perovskite photodetectors.

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Perovskite‐based time‐domain signal‐balancing LiDAR sensor with centimeter depth resolution

In this study, we present a monolithic high-speed perovskite-based photodetector capable of directly sensing the time delay between two light pulses with a temporal resolution of at least 170 ps. Thi...

onlinelibrary.wiley.com

Low-Pressure Cycling of Lithium Metal Anodes with Argyrodite Solid-State Electrolytes Enabled by an Sb-Based Interfacial Layer

This study presents a facile and scalable methodology to achieve stable cycling of lithium metal anodes in argyrodite-type Li6PS5Cl (LPSCl)-based soli…

sciencedirect.com

Air‐Stable Aluminum Tris[Bis(mesitoyl)Arsenide] Precursor for Metal Arsenide Quantum Dots

Aluminum tris[bis(mesitoyl)arsenide]: a new enin metal–arsenide QD synthesis.

onlinelibrary.wiley.com

Dual-Layer Li Metal All-Solid-State Battery Based on an Argyrodite-type Li6PS5Cl Catholyte and a Garnet-type Li7La3Zr2O12 Separator

The integration of argyrodite-type Li6PS5Cl (LPSCl) solid-state electrolytes (SSEs) in solid-state batteries faces significant challenges due to their chemical reactivity with lithium metal, which pre...

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Characterizing Emerging Detector Materials for Low‐Dose X‐Ray Imaging

X-ray medical imaging requires detectors that deliver images at as low as reasonably possible dose. This perspective outlines a universal characterization framework of X-ray imaging detectors, suitab...

advanced.onlinelibrary.wiley.com

Prospects of Nanoscience with Nanocrystals: 2025 Edition

Nanocrystals (NCs) of various compositions have made important contributions to science and technology, with their impact recognized by the 2023 Nobel Prize in Chemistry for the discovery and synthesis of semiconductor quantum dots (QDs). Over four decades of research into NCs has led to numerous advancements in diverse fields, such as optoelectronics, catalysis, energy, medicine, and recently, quantum information and computing. The last 10 years since the predecessor perspective “Prospect of Nanoscience with Nanocrystals” was published in ACS Nano have seen NC research continuously evolve, yielding critical advances in fundamental understanding and practical applications. Mechanistic insights into NC formation have translated into precision control over NC size, shape, and composition. Emerging synthesis techniques have broadened the landscape of compounds obtainable in colloidal NC form. Sophistication in surface chemistry, jointly bolstered by theoretical models and experimental findings, has facilitated refined control over NC properties and represents a trusted gateway to enhanced NC stability and processability. The assembly of NCs into superlattices, along with two-dimensional (2D) photolithography and three-dimensional (3D) printing, has expanded their utility in creating materials with tailored properties. Applications of NCs are also flourishing, consolidating progress in fields targeted early on, such as optoelectronics and catalysis, and extending into areas ranging from quantum technology to phase-change memories. In this perspective, we review the extensive progress in research on NCs over the past decade and highlight key areas where future research may bring further breakthroughs.

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Energy-Degenerate Photon-Pair Generation from Individual CsPbBr3 Quantum Dots

Beyond single-photon emission, generating correlated N-photon bundles, e.g., a photon pair, is essential for various quantum technologies including quantum teleportation and metrology. A widely explored approach exploits the radiative biexciton cascade in individual (mainly epitaxially grown) quantum dots (QDs). Here, we investigate such a cascade in colloidal CsPbBr3 QDs, a scalable and solution-processable quantum-light emitter. By matching their size-dependent biexciton binding energies to their size-independent phonon energies, we demonstrate the generation of time-correlated and energy-degenerate photon pairs in large (>15 nm) QDs. Under pulsed excitation at 4 K, we observe pronounced photon bunching, with a g(2)(0) of up to 7 in Hanbury Brown and Twiss measurements. The excitation-density-dependent bunching is quantitatively reproduced by multicolor numerical calculations, suggesting the cascade involving biexciton and phonon-mediated exciton decay as origin of the photon pair. Our findings provide new insights into energy-degenerate photon-pair generation in these highly engineerable quantum-light emitters, marking important steps toward their application in quantum-information technologies.

pubs.acs.org

Critical current density measurements of Li/solid-state electrolyte anodes: Time for a rethink

Critical current density (CCD) measurements are widely used to assess the electrochemical performance of Li metal anodes paired with solid-state electrolytes. Nonetheless, the lack of consensus on the...

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