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At least 19 records

Depth-Dependent Emission from Silver Dopants in Single CdSe Nanoplatelets

Dopants in semiconductor nanostructures offer tremendous control over electronic, optical, and magnetic properties beyond what is achievable in bulk materials. We demonstrate that the broad dopant emission in semiconductor nanoplatelets effectively maps the electron wave function across the nanoplatelet thickness. Both the emission energy and lifetime of the dopant transition depend strongly on the depth of the dopant within the nanoplatelet. This dependence arises from the electrostatic self-interaction of the charged dopant, which varies with proximity to the dielectric discontinuity at the nanoplatelet surface. Through comprehensive single-particle spectroscopy of silver-doped CdSe nanoplatelets, we verify that acceptors near the center emit at higher energies with shorter lifetimes, while those near the surface emit at lower energies with longer lifetimes. This spatial mapping also reveals unusual two-color emission from individual nanoplatelets, with enhanced Auger recombination yielding exceptional photon antibunching (>90% purity) at room temperature, suggesting potential applications in quantum information technologies.

cadmium selenide

Ultrafast Dynamics of Plasmon-Coupled Excitons in Semiconducting Nanoplatelets

Exciton-plasmon coupling in nanomaterials produces many relevant phenomena for photonics applications including increased light-matter interactions, enhanced radiative rates of quantum emitters, and coherent energy exchange. In the case of exciton coupling to surface plasmon polaritons (SPPs), dispersive interactions controlled by the wavevector of optical excitation create the opportunity for tunable optical emission. Strong temporal impacts on exciton lifetimes can also occur in coupled systems, creating the opportunity for ultrafast control of exciton lifetime via changes in electronic coupling magnitude to a dispersive SPP. The coupling strength can be impacted by the morphology of the nanomaterials. Here, in this study, we utilize colloidal semiconductor nanoplatelets deposited onto thin silver plasmonic films, and compare the results to semiconductor quantum dots deposited on the silver films. We map the dispersion of the coupled systems and measure the ultrafast transient absorption response of the coupled systems. Due to the larger interaction areas of the nanoplatelets that lie flat on the silver films, a greater degree of coupling is found for the nanoplatelets, and much faster temporal responses are found as compared to quantum dots. Fresnel theory calculations that incorporate heavy and light hole features can reproduce the dispersion of the nanoplatelet-silver film, and a simple three-state model is developed to provide insights into the nature of the coupling at different photon energies along the dispersion curve.

colloidal semiconductor nanoplatelets

Bottom‐Up Synthesis of Metallic CoNi Nanoplatelets with Magnetic Vortex‐Like Spin Configurations

Magnetic nanoplatelets hold significant potential for various technical applications due to their ability to switch between a fully magnetized state with high magnetization and a vortex‐like configuration that eliminates stray fields in the absence of an external field. This study presents the synthesis of uniform CoNi nanoplatelets through the topotactic reduction of metal hydroxides using hydrogen plasma. The reduction process is analyzed via magnetometry, leveraging the transition from paramagnetic hydroxide to ferromagnetic metal. Lorentz transmission electron microscopy and scanning transmission X‐ray microscopy confirm the presence of magnetic vortex‐like structures in isolated Co 0.85 Ni 0.15 nanoplatelets at ambient temperature. Additionally, micromagnetic simulations are conducted to further explore the magnetic properties of the nanoplatelets, revealing the formation of magnetic vortex remanent states at diameters between 200 nm and 1 μm and a thickness of around 12 nm. Notably, structural defects and thickness variations do not directly destabilize the magnetic vortex configurations.

Kräenbring, Mena‐Alexander [Faculty of Physics and

Strong Effect of Nonpolar Solvent Molecular Structure on CdSe Nanoplatelet Stacking

We report a drastic difference in stacking behavior of oleic acid-stabilized 4-monolayer (4 ML) CdSe nanoplatelets (NPLs) in toluene and methylcyclohexane (MCH), two nonpolar solvents that differ in the conformational flexibility of their molecules. Using liquid cell transmission electron microscopy (TEM) and small angle scattering (SAXS) techniques, we show that NPLs form microns-long ribbons consisting of 4 ML CdSe NPLs in toluene, the solvent widely used to form stable colloidal solutions of a broad range of quasi-spherical nanoparticles. In contrast, 4 ML CdSe NPLs are well dispersed in MCH. The difference in stacking behavior of NPLs in toluene and MCH suggests that the conformational flexibility of the solvent molecules, such as the ability to adopt multiple chair conformations, modulates nanoplatelet interactions. Molecular dynamics (MD) simulations reveal that solvent molecules subtly alter the structure of the organic ligand shell. These solvent-dependent changes propagate to the inorganic core, modulating the degree of CdSe nanoplatelet (NPL) twisting and, consequently, the properties of the nanoparticles. We show that toluene better solvates oleate ligands while MCH induces a bimodal oleate span distribution, which can lead to increased solubility of CdSe NPLs. In addition, the solvent can also influence the inorganic core, which, in turn, can modify the nanoparticle properties. We demonstrate that destabilization of toluene solution containing ribbons of 4 ML CdSe NPLs without CdS shells results in the formation of NPL assemblies with amplified spontaneous emission (ASE) with a low threshold of 14 µJ cm−2 that is comparable with that of CdSe/CdS core/shell NPLs. Our results emphasize that the solvent plays a major role in mediating interactions between NPLs and hence their processability for fabrication of functional structures.

CdSe

Manipulating Excitonic Quantum Droplets in Two-Dimensional CdSe Nanoplatelets via Thickness and Core/Shell Morphology

Recently, photoexcitation of high-density 4 or 5 monolayer (ML) thick CdSe nanoplatelet films at temperatures below ~200K was observed to produce pump-intensitydependent, superlinear, progressively red-shifted light output due to amplified spontaneous emission (ASE) from polyexcitonic species, distinct from biexcitonic ASE. These polyexcitonic species comprise Coulombically bound multiexciton states, termed “quantum droplets”, that form when multiexciton binding energy exceeds thermal energy fluctuations. In this work, we investigate thinner samples as well as core/shell nanoplatelet films and find that the 3 ML sample supports quantum droplet ASE up to higher temperatures than the 4 or 5 ML whereas core/shell structures suppress this form of ASE even at very low sample temperatures despite observable biexcitonic ASE, suggesting that the reduced or repulsive Coulomb binding energy of multiple excitons suppresses quantum droplets. These findings help to add understanding of routes to harness quantum droplet optical nonlinearities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Uptake and Binding of At‐211 Into K‐ and Cs‐Derivatives of Alpha‐Zirconium Phosphate Nanoplatelets for Use as a Targeted Alpha Therapy Delivery Platform

The ion exchange behavior of K- and Cs-derivatives of α-zirconium phosphate, A-ZrP, with the targeted alpha therapy (TAT) radionuclide 211 At, as At + and AtO + , has been investigated. The K-ZrP shows strong affinity for both At+ and AtO + , ≥99% uptake. The affinity to Cs-ZrP was less pronounced, 87%–94% uptake, favoring At + . The binding strength was tested against several leaching solutions, including carbonate, phosphate buffered saline (PBS), 4-(2-hydroxyethyl)-1-piperazineethanesulfonic acid (HEPES) buffers, and ethylenediaminetetraacetic acid (EDTA) solutions at various concentrations (0.1–10 mM). K-ZrP retained 211 At in all buffer and EDTA solutions up to 1 mM (<0.5% leaching). The Cs-ZrP showed no leaching of At + , while AtO + leached (1%–3%) in the carbonate and HEPES buffers, along with all of the EDTA solutions, with complete retention only in the PBS buffer. In all cases, when the EDTA concentration reached 10 mM, 211 At leaching was observed. Once incorporated into the ZrP nanoplatelets, significant shielding of the α-particles was observed, not only attenuating the intensity of the emission but also reducing the energy of the α-particles themselves exiting the nanoplatelets. These properties provide the basis for K-ZrP, and to a lesser extent, Cs-ZrP to be further considered as potentially promising candidates for a delivery mechanism of 211 At for application in TAT.

astatine-211

Single-Particle Insights Into the Electronic Structure and Enhanced Stability of CsPbBr 3 /FAPbBr 3 Core/Crown Nanoplatelets at the Nanometer Scale

Colloidal perovskite nanoplatelets (NPLs), despite their exceptional optoelectronic properties, face significant challenges due to their intrinsic instability and trap-assisted non-radiative recombination. Although many studies employing surface engineering, such as selecting ligands or coating to passivate defects, have demonstrated improved optoelectronic properties, these enhancements are typically inferred from bulk-ensemble measurements; the effects at the single-particle level remain elusive. Here, we conduct single-particle-level studies using scanning tunneling spectroscopy (STS) on a unique core–crown system, CsPbBr 3 @FAPbBr 3 NPLs, where the lateral surfaces of the CsPbBr 3 core are coated with an FAPbBr 3 crown. Experimental density-of-states (DOS) analysis reveals a 47% reduction in deep-trap states in core-crown NPLs compared to core-only NPLs, consistent with nearly two-fold enhancements in photoluminescence quantum yields. Progressive I–V sweep measurements demonstrate superior electrical stability in core-crown NPLs, preserving band structure with minimal degradation, while core-only NPLs exhibit rapid bandgap shrinkage and trap formation. Density functional theory (DFT) calculations indicate that FA incorporation distorts Pb octahedral lattice, widening the bandgap. This study elucidates how surface engineering modulates charge localization, passivates defects, and enhances stability at the single-particle level. Moreover, by uncovering bias-induced trap states in single unpassivated NPLs, this study establishes a precise, robust approach for characterizing emerging perovskite nanocrystals.

77 NANOSCIENCE AND NANOTECHNOLOGY

Stabilizing Ultrathin CsPbBr 3 Nanoplatelet Films for Deterministic Strong Light-Matter Coupling

While the excitons in perovskite nanomaterials possess interesting properties central to their use in optoelectronic technologies, their instability limits real world applicability. In this study, we describe a method to stabilize the structures of cesium lead bromide (CsPbBr 3 ) nanoplatelets (NPLs) in spin-casted films. We apply this method to design, fabricate, and characterize exciton cavity polaritons formed from these nanomaterials. These studies show that we can form exciton cavity polaritons from CsPbBr 3 in precisely designed Fabry−Perot microresonators and suggest that the structures of these materials can be stabilized toward their use in other solution-processed optoelectronic devices.

cavities

In-Situ Ligand-Induced Chirality Transfer in Emissive CdSe Nanoplatelets

Terminating semiconductor nanocrystals with chiral organic ligands can induce chiroptical properties that combine the chiral character of the ligands with the strong and tunable optical properties of the nanocrystal. However, the synthesis of such chiral-modified nanocrystals is currently limited by solvent incompatibility between polar chiral ligands and nonpolar traditional ligands, as well as by ligand dissolution behavior that ultimately compromises nanocrystal quality and the degree to which chiroptical properties can be manipulated. In this work, we demonstrate a single-step synthesis of chiral cadmium selenide (CdSe) nanoplatelets (NPLs) that eliminates the need for postsynthetic ligand exchange in aqueous solvents, resulting in highly emissive chiral CdSe NPLs. By directly incorporating chiral aminodecanoic acid ligands during synthesis, we achieve in situ ligand binding and chirality transfer to CdSe NPLs. This approach produces CdSe NPLs with high photoluminescence quantum efficiencies of 50% and circular dichroism dissymmetry factors (gCD) on the order of 10 –4 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Robust photocatalytic hydrogen generation from CdSe nanoplatelets

Mercaptopropionic acid (MPA) capped-CdSe NPLs in-conjunction with a nickel-dihydrolipoic acid (Ni-DHLA) co-catalyst, yielded a robust output of photocatalytically generated hydrogen (H 2 ) at low concentrations of nanoplatelets. Furthermore, etching led to increased catalytic efficiency, suggesting that exposed catalytically active sites are primarily responsible for photocatalytic activity.

Phinney, Elizabeth O. [University of Rochester, NY

Determination of Oscillator Strength of CdSe Nanoplatelets from Strong Light-Matter Coupling

We report exciton-polaritons formed from core-only, core-crown, and core-shell NPLs, which, alongside finite-difference time-domain (FDTD) simulations of Fabry-Pérot cavity mode volume, allow for the verification of core-only and determination of core-crown and core-shell oscillator strengths. Additionally, we show that polaritons can be used not only as a means of altering the properties of coupled emitters, but as an analytical tool to better understand the properties of coupled emitters.

Hancock, Benjamin

Strategy for Ultranarrow Light Down-Conversion for Displays Based on Bicolor-Emitting 2D Colloidal Heterostructures

The demand for ultranarrow spectral emission below 10 nm is critical for next-generation displays. Although current colloidal nanocrystals are successful in light down-conversion applications, they fall short in matching the stringent color purity requirements set by standards like Rec. 2020. Achieving such narrow linewidths through material engineering alone remains elusive, necessitating innovative light management strategies that avoid optical losses and maintain device efficiency. Here, in this work, we present a novel 2D colloidal heterostructure design, combining a CdSe core nanoplatelet, a CdS crown, and a CdZnS shell, to achieve bright bicolor emission in the solid state (green/red) emission with tunable intensity ratios controlled by excitation power (either optical or electrical). Integration of these nanoplatelets into a dielectric cavity further narrows the emission linewidth to sub-2 nm while enhancing the photoluminescence intensity by up to 200 times, meeting the Rec. 2020 color purity targets. This approach paves the way for a strategy avoiding complex laser-based solutions.

2D nanocrystals

Lightweight, Flexible Electromagnetic Shielding Composite Films Reinforced with Recycled Carbon Fibers and Carbon Nanofillers

Lightweight, flexible polymer composites are widely adopted in modern electronic devices and systems for high-efficiency electromagnetic interference (EMI) shielding. Reinforcing polymer composites with conductive fillers offers a promising alternative to conventional metal-based shielding material thanks to their low density, tunable properties, and flexibility. Herein, lightweight, flexible ultra-high molecular weight polyethylene composite films reinforced with recycled carbon fibers (rCFs) and carbon-based nanofillers, including graphene nanoplatelets (GNPs) and carbon nanotubes, are reported for EMI shielding applications. The incorporation of these nanofillers significantly reduces the required content of rCFs and improves processability while maintaining comparable shielding effectiveness. The addition of these nanofillers with rCFs enhances the EMI shielding effectiveness by up to 15 dB. Incorporating 1 wt% GNPs can replace 5 wt% rCFs and achieve comparable EMI shielding performance, while 5 wt% of either nanofillers can substitute for 10 wt% rCFs. Numerical modeling of electromagnetic wave transmission reveals that increasing nanofiller concentrations enhances both reflection and absorption losses, with absorption consistently dominating across all levels. Furthermore, this study not only provides insight into the synergistic contributions of rCFs and carbon nanofillers to shielding effectiveness but also paves the way for the design of sustainable, lightweight EMI shielding composite films for applications in electric vehicles, medical equipment, and portable electronics.

carbon nanofiller

Ion dynamics in hexagonal boron nitride ionogel electrolytes

Ionogel electrolytes incorporating exfoliated hexagonal boron nitride (hBN) nanoplatelets are promising materials for next-generation energy storage systems. However, detailed understanding of their ion transport properties at the molecular level remains limited. This study employs diffusion and relaxation nuclear magnetic resonance (NMR) techniques, including fast-field cycling (FFC) NMR, to investigate the dynamics of ionic species in hBN-ionogels. By spanning a broad frequency range from 30 kHz using FFC NMR to high-field NMR (500–800 MHz), we reveal distinct relaxation mechanisms governing ion dynamics in ionogels with and without lithium salts. Our results highlight the role of hBN in modulating molecular rotation and translational motion, significantly affecting 1 H and 19 F relaxation profiles. The presence of Li + alters the dynamic behavior in ionogels, enhancing anion mobility at the interface. Notably, 7 Li relaxation reveals strong interactions with the hBN surface that cannot be detected by diffusion NMR. Furthermore, these findings underscore the importance of spanning a broad frequency range in NMR studies of ionogels and provide critical insights into optimizing their design as novel electrolytes.

Electrolytes

Scalable Upcycling of Spent Lithium-Ion Battery Anodic Graphite to Electronic-Grade Graphene

Recycling processes for lithium-ion batteries (LIBs) are imperative to support the sustainable growth of global energy storage systems. This study introduces a scalable method for the upcycling of spent graphite anodes from LIBs to produce electronic-grade graphene nanoplatelets. In addition to comprehensive materials characterization, the electronic quality of the upcycled graphene is demonstrated by formulating it into a screen printing ink that achieves high-resolution patterning and thin-film electrical conductivity exceeding 104 S m−1. This screen printing ink is also used to print planar micro-supercapacitors with exceptional areal capacitance (1.78 mF cm−2), areal energy density (0.247 µWh cm−2), and cycling stability (> 10 000 cycles). Life cycle assessment (LCA) and techno-economic analysis (TEA) highlight the environmental benefits and cost reductions attainable through upcycling of graphite from LIBs. By capturing economic value from spent LIBs, this work fosters a sustainable battery supply chain and provides an abundant and geographically distributed raw material for electronic-grade graphene.

energy storage

Hierarchical low Pt-loading “core-shell” electrocatalysts for the oxygen reduction reaction in fuel cells

The sluggish kinetics of the oxygen reduction reaction (ORR) hinder cost-effective polymer electrolyte fuel cells (PEFCs), which rely on scarce, expensive platinum-based electrocatalysts (ECs). Here, we present a novel synthesis method for ORR ECs achieving exceptional platinum utilization. The design features a hierarchical “multi-carbon” support comprising carbon nanoparticles interacting with graphene nanoplatelets as the “core”, encapsulated by a porous carbon nitride (CN) “shell”. This configuration promotes strong core/shell interactions and a bimodal active site distribution, consisting of chemically dispersed Pt and Ni single-atom complexes and PtNix alloy nanoclusters embedded in the CN shell. These advantages enable high activity and durability, achieving an ORR activity of 1.6 A mgPt−1 at 0.9 V vs. RHE-an order of magnitude higher than Pt/C (0.17 A mgPt−1). A proof-of-concept PEFC demonstrates a specific power of 12.0 kW gPt−1 at 0.60 V. This approach offers a significant step toward more efficient and sustainable PEFC technologies.

Pagot, Gioele [University of Padova, Italy]

Graphene Activated Magnesium Diboride for Moderate Pressure and Temperature Hydrogenation to Magnesium Borohydride

The hydrogenation conditions of magnesium diboride (MgB2) to magnesium borohydride (Mg(BH4)2) can be significantly enhanced through the discovery of improved modifiers. This study demonstrates that the modification of MgB2 by mechanical milling with graphene nanoplatelets significantly reduces the hydrogenation conditions of MgB2 from 900 bar and 400 degrees C for pure MgB2 to 400 bar and 300 degrees C while achieving 77% conversion to Mg(BH4)2. The introduction of the graphene additives coupled with milling leads to a reduction of the temperature and pressure required for bulk hydrogenation by 100 degrees C and 500 bar, respectively, from that of pure MgB2. The identification of graphene additives that drastically improve the hydrogenation conditions of MgB2 represents an important step toward improving hydrogen uptake kinetics to Mg(BH4)2.

complex hydrides