Amorphous/crystalline interfaces that combine structural distortion with local charge redistribution remain poorly understood, mainly owing to limited access to atomically well-defined single-crystalline components and c...Amorphous/crystalline interfaces that combine structural distortion with local charge redistribution remain poorly understood, mainly owing to limited access to atomically well-defined single-crystalline components and correlative probes of interfacial fields. Herein, we construct atomically resolvable single-crystalline/amorphous heterointerfaces by synthesizing a library of transition metal oxytellurides and map the projected electric field and strain by combining scanning transmission electron microscopy (STEM) with four-dimensional STEM (4D-STEM). In RuTeO, 4D-STEM reveals a locally enhanced electrostatic field whose direction reorients at the interface. Charge density maps show electron accumulation in the amorphous region and depletion in the single-crystalline region, suggesting directional electron transfer. Nanometer-scale tensile and compressive strain localized around the heterointerface is identified. Electronic structure calculations indicate enhanced Ru 4 delocalization near the Fermi level, facilitating electron-driven reactions. This work spatially correlates atomic structure with built-in electric fields and lattice strain at disordered-ordered interfaces, providing a general route to elucidating structure-activity relationships.
Stapled peptides exhibit superior proteolytic stability and cell permeability, relative to linear peptides. However, non-specific tissue distribution precipitates dose-limiting toxicities, constraining the therapeutic im...Stapled peptides exhibit superior proteolytic stability and cell permeability, relative to linear peptides. However, non-specific tissue distribution precipitates dose-limiting toxicities, constraining the therapeutic implementation. Here, we designed a self-assembling nanostapled peptide (NSP) comprising hydrophilic mPEG groups surrounding a hydrophobic core made up of a therapeutic stapled peptide. , the nanostructure protected the peptide from non-target tissues, thereby improving bioavailability. Specifically, under the acidic and MMP-9-rich conditions of the tumor microenvironment, the therapeutic peptide could be released through programmed disassembly to penetrate the colorectal cancer cells and activate a downstream apoptotic pathway. Collectively, this study establishes NSP as a promising platform for the precise and effective treatment of colorectal cancers.
Defect functionalization is a promising route to enhance spin-orbit coupling (SOC) in graphene, but achieving controllable fluorination while suppressing irreversible lattice damage remains challenging. Here we demonstra...Defect functionalization is a promising route to enhance spin-orbit coupling (SOC) in graphene, but achieving controllable fluorination while suppressing irreversible lattice damage remains challenging. Here we demonstrate low-damage fluorination of monolayer graphene using a remote CF plasma process that suppresses ion-bombardment-induced lattice damage. Raman spectroscopy with defect-activation analysis and an annealing-reversibility test identifies a processing window where fluorination predominantly yields reversible sp C-F functionalization while minimizing vacancy formation. Nonlocal transport measurements show that the nonlocal resistance increases in fluorinated graphene and decays exponentially with channel length, consistent with spin diffusion and yielding a spin relaxation length of ∼0.4 μm. Within the Elliott-Yafet framework, we estimate an effective SOC energy scale of 4-9 meV. These results provide a Raman-validated, tunable process route for enhancing SOC in graphene while suppressing vacancy damage.
Oh J, Roh J, Gureghian C
… +13 more, Mastrippolito D, Cavallo M, Paye M, Xu XZ, Gage TE, Menguy N, Lafosse X, Silly MG, Pierucci D, Lhuillier E, Climente JI, Diroll BT, Ithurria S
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 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, 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.
Chirality pervades living systems and increasingly guides the design of functional nanomaterials. Yet weak or residual chirality can be difficult to detect, particularly in liquid-phase nanocrystal syntheses requiring no...Chirality pervades living systems and increasingly guides the design of functional nanomaterials. Yet weak or residual chirality can be difficult to detect, particularly in liquid-phase nanocrystal syntheses requiring noninvasive probes. Here we track chirality evolution in colloidal tellurium nanocrystals spanning strong, alloy-tuned, and reduced shape chirality. As morphological chirality decreases, linear circular dichroism drops by roughly an order of magnitude. In contrast, polarization-resolved second-harmonic scattering retains clear handedness-dependent responses. Across six independent observables─the nonlinear g-factor (g) and dual-circular polarization metrics ( and ) measured in forward and right-angled geometries─the signal reverses sign between enantiomorphs and remains well-resolved. The geometry dependence of these responses is consistent with interference between mirror symmetry-even and mirror symmetry-odd nonlinear tensor contributions. These results establish chiroptical second-harmonic scattering as a sensitive probe of weak structural asymmetry in nanocrystals exhibiting coupled shape and crystal chirality.
Nanoscale domain nucleation and domain-wall propagation govern switching in hafnia-based ferroelectrics. However, it is not known how electrode interfaces and thermal processing govern these processes at the grain scale....Nanoscale domain nucleation and domain-wall propagation govern switching in hafnia-based ferroelectrics. However, it is not known how electrode interfaces and thermal processing govern these processes at the grain scale. Here, bias-dependent piezoresponse force microscopy and pulsed switching measurements reveal how bottom electrodes and annealing control polarization reversal in 10-nm-thick HfZrO capacitors. TiN promotes rapid nucleation and cross-grain propagation, NbN leads to gradual intragrain switching, and MoO strongly suppresses ferroelectric switching. The fastest reversal is obtained for TiN/HZO/TiN annealed at 600 °C, consistent with a fine-grained microstructure and grain boundaries that support cooperative propagation. Quantitative analysis of pulse-switching kinetics using a modified Kolmogorov-Avrami-Ishibashi framework yields comparable time constants for nucleation and growth, indicating that both processes proceed concurrently. These results establish a grain-scale mechanistic link between interfaces, microstructure, and switching kinetics in HfZrO capacitors.
Artificial sensory systems with synergistic tactile and nociceptive perception are essential for advanced human-robot interaction and environmental monitoring. However, developing scalable, tunable electronic skin (e-ski...Artificial sensory systems with synergistic tactile and nociceptive perception are essential for advanced human-robot interaction and environmental monitoring. However, developing scalable, tunable electronic skin (e-skin) that combines ultrasensitive tactile and nociceptive sensing remains challenging. Here, inspired by leaf stomata, we present a suspended biomimetic e-skin enabling 3D deformation-mechanical contact interactions for adjustable sensing. By integrating Langmuir-Blodgett assembly with a mechanical strategy, we achieve large-scale, precise alignment of metal nanowires and controlled crack formation, resulting in ultrahigh sensitivity (205.08 kPa) and excellent cyclic stability (120 000 cycles). Leveraging its dual-modal sensing mechanism, the e-skin is incorporated into a robotic tactile system, enabling non-destructive grasping of soft objects and real-time avoidance of sharp objects under closed-loop control. This simple, scalable approach provides a versatile platform for ultrasensitive, adaptive e-skin, advancing robotic tactile and nociceptive perception and promoting intelligent human-robot interaction.
Altermagnetism offers a promising route for next-generation spintronic devices. In two-dimensional (2D) magnets, twist engineering enables its realization by breaking the combined inversion and time-reversal symmetry ()....Altermagnetism offers a promising route for next-generation spintronic devices. In two-dimensional (2D) magnets, twist engineering enables its realization by breaking the combined inversion and time-reversal symmetry (). Here, by first-principles calculations and symmetry analysis, we demonstrate that twisting the recently synthesized metallic van der Waals antiferromagnet Co-doped bilayer FeGaTe (FeCoGaTe) provides a robust platform for altermagnetism, breaking the symmetry between opposite spin sublattices. This results in a nonrelativistic -wave altermagnetic state with spin splitting up to 138 meV. Without spin-orbit coupling (SOC) the electronic states remain spin-degenerate along six high-symmetry directions, whereas including SOC preserves degeneracy along the three directions protected by 2-fold rotation axes. Furthermore, we unveil the microscopic mechanisms governing the magnetic behavior in twisted bilayer FeCoGaTe. Our results establish twist engineering and metallic Fe-based van der Waals antiferromagnets as versatile platforms to realize 2D altermagnetism, with potential for designing high-efficiency ultrathin nanodevices.
Power requirements represent a critical challenge for wearable sensors. Self-powered sensing systems enabled by miniaturized energy-storage devices (MESDs) offer a promising solution. However, the proliferation of MESDs...Power requirements represent a critical challenge for wearable sensors. Self-powered sensing systems enabled by miniaturized energy-storage devices (MESDs) offer a promising solution. However, the proliferation of MESDs inevitably generates electronic waste (e-waste), which causes environmental concerns. Transient electronics that degrade into eco-friendly residuals provide opportunities for the development of green power sources. Herein, flexible e-waste-friendly power sources based on degradable MXene films were developed for the integration of wearable, self-powered biomedical sensors. The proposed transient MXene film-based supercapacitors (TMFSCs) possess good energy storage capability and mechanical flexibility and can be completely degraded into eco-friendly residuals within minutes. Furthermore, a wearable self-powered biomedical smart sensor was designed for real-time monitoring of pulse signals in real-life scenarios, and the obtained pulse rate is conducive to early evaluation of human health. Collectively, TMFSCs are considerably competitive for future eco-friendly flexible MESDs toward next-generation sustainable wearable and portable sensing electronics.
Core-crown CdSe/CdS nanoplatelets combine improved quantum yield with promising optoelectronic performance, yet their emission dynamics remain governed by reversible charge trapping. By correlating single-particle lumine...Core-crown CdSe/CdS nanoplatelets combine improved quantum yield with promising optoelectronic performance, yet their emission dynamics remain governed by reversible charge trapping. By correlating single-particle luminescence decays with intensity fluctuations (blinking/flickering), we uncover a distinct emission regime at intermediate brightness levels where delayed luminescence arises. This behavior reflects a reversible trapping process that reduces light emission and introduces a secondary, slow decay channel. Time-resolved analysis reveals stochastic switching between active and inactive reversible trapping within an individual emitter. Under higher excitation powers, these reversible traps are supplanted by stronger nonradiative quenching pathways.
Interfacial electric fields govern charge separation in van der Waals photodetectors, yet they are typically modulated by electrostatic gates or ferroelectric interlayers, which introduce power consumption and stability...Interfacial electric fields govern charge separation in van der Waals photodetectors, yet they are typically modulated by electrostatic gates or ferroelectric interlayers, which introduce power consumption and stability challenges. Here, we show that the twist angle intrinsically controls interfacial electrostatics in a low-symmetry ReS/ReSe heterostructure. Rotating the anisotropic crystal axes reconstructs the interfacial polarization landscape, leading to a reversal of the built-in electric field in the orthostacking configuration. This enables efficient self-powered photodetection with an on/off ratio of 10 and a high responsivity. Twist-controlled electrostatic reconstruction further modulates carrier separation and anisotropic transport, transforming the polarization-dependent photocurrent from a two-lobed to an approximately four-lobed profile and enabling tunable polarization sensitivity. Moreover, the deterministic twist-angle-dependent photocurrent allows hardware-level encoding. These results establish twist engineering as an effective strategy for tailoring interfacial fields and multifunctional optoelectronic responses in low-symmetry van der Waals heterostructures.
The wafer-scale synthesis of magnetic two-dimensional transition metal dichalcogenides (TMDCs) remains a critical challenge due to their metastability and the rapid oxidation of metallic precursors, which block conventio...The wafer-scale synthesis of magnetic two-dimensional transition metal dichalcogenides (TMDCs) remains a critical challenge due to their metastability and the rapid oxidation of metallic precursors, which block conventional sulfurization routes. Chromium disulfide (CrS), in particular, is highly attractive for spintronic applications because of its robust room-temperature ferromagnetism, yet its wafer-scale growth has remained elusive. Here, we report a universal strategy using ZnS-derived sulfur monomers to overcome the chemical reaction barrier imposed by native oxide layer, enabling the selective formation of crystalline CrS films across 2-in. wafers. The resulting films exhibit excellent uniformity, controllable thickness, and robust ferromagnetism above room temperature. Beyond CrS, this method demonstrates broad application by yielding wafer-scale VS, MnS, FeS, CoS, and the ternary CrCoS with comparable quality. Our results establish a versatile and scalable synthesis platform for 2D magnetic TMDCs, opening a pathway toward their integration in advanced spintronic devices.
We investigate the near-infrared optical response of the semiconducting van der Waals antiferromagnet CrPS and identify previously unreported spin-entangled optical resonances. The strong and anisotropic magnetic-field d...We investigate the near-infrared optical response of the semiconducting van der Waals antiferromagnet CrPS and identify previously unreported spin-entangled optical resonances. The strong and anisotropic magnetic-field dependence of these resonances reflects the underlying magnetic order and confirms the biaxial antiferromagnetic nature of CrPS. From the magnetic field evolution of the optical transition, we extract key magnetic parameters, including the spin-flop ( T) and spin-saturation ( T) fields. These results demonstrate a potential pathway for all-optical probing of spin states in van der Waals antiferromagnets, with relevance for spin-sensitive optoelectronic and magneto-optical devices.
Precisely modulating the coordination structure of neighboring metal atomic sites is urgently required yet remains technically challenging. Herein, we report a carbon-vacancy-induced Fe coordination environment modulatio...Precisely modulating the coordination structure of neighboring metal atomic sites is urgently required yet remains technically challenging. Herein, we report a carbon-vacancy-induced Fe coordination environment modulation in FeZn dual-atom sites (FeZnN-V) to boost bifunctional oxygen electrocatalysis. Finite element simulation and electronic structure characterization reveal that carbon vacancies promote electron transfer from Fe-N to neighboring Zn-N sites, establishing favorable electronic interactions. In situ Raman spectroscopy further identifies the key O-O intermediate (corresponding to OOH*) and the FeOOH active phase during oxygen evolution reaction (OER), both showing significantly lowered onset potentials. Compared with conventional FeZn dual-atom catalysts, FeZnN-V achieves a 174 mV decrease in OER overpotential at 10 mA cm and exhibits improved oxygen reduction reaction performance in alkaline media. The corresponding quasi-solid-state Zn-air battery delivers a long cycling life of 82.3 h at 50 mA cm. This work offers a versatile carbon-vacancy strategy to tune the local coordination of dual-atomic sites for advanced electrocatalysis.
Tuning thermal conductivity (κ) of metal-organic frameworks (MOFs) is pivotal for advancing their emerging thermoelectric applications and addressing the heat dissipation bottleneck in gas adsorption processes, yet heat...Tuning thermal conductivity (κ) of metal-organic frameworks (MOFs) is pivotal for advancing their emerging thermoelectric applications and addressing the heat dissipation bottleneck in gas adsorption processes, yet heat conduction mechanisms in MOFs, particularly from the perspective of intrinsic lattice vibrations, remain elusive, limiting rational thermal engineering. Here, we focus on organic ligand rotational dynamics and elucidate their critical but long-overlooked modulations on thermal transport. Through elaborate atomistic simulations on prototypical MIL-47, we report that low-frequency, anharmonic linker librations dramatically intensify phonon scattering, inducing an over 2-fold reduction in κ. Such a suppression effect is further confirmed to be universal across diverse flexible frameworks featuring rotatable ligands, including the known zeolitic imidazolate and covalent organic families. Accordingly, we evaluate multiple practical strategies to regulate κ by tailoring linker rotational dynamics. These insights open vast avenues for the flexible design of MOFs' thermal performance to meet their energy-related applications.
Films with large anisotropy ratios () between the in-plane and cross-plane thermal conductivity (κ) can be used for directional heat spreading in electronics thermal management. Here, we show that commercially available...Films with large anisotropy ratios () between the in-plane and cross-plane thermal conductivity (κ) can be used for directional heat spreading in electronics thermal management. Here, we show that commercially available solution-spun carbon nanotube (CNT) films with 20 μm thickness and centimeter-scale lateral dimensions exhibit orthotropic thermal conductivity with the highest reported to date, reaching = 1400 ± 160 at room temperature (). We find using laser flash thermal diffusivity (α) measurements over a range from 198 to 573 K. Dedoping of acid residuals via annealing increases the in-plane-aligned α of dedoped samples by a factor of 2 compared to the doped samples. These dedoped CNT films also display a strong α ∝ scaling, indicating that phonon-phonon scattering impacts heat transport along the direction of alignment. Our work motivates further exploration of ultrahigh in macroscopic CNT materials and applications of CNT films for directional heat spreading.
This study demonstrates active control of terahertz (THz) transmission by exploiting the humidity-driven swelling of a submicron poly(vinyl alcohol) (PVA) film integrated with metallic nanoresonators. Conventional THz mo...This study demonstrates active control of terahertz (THz) transmission by exploiting the humidity-driven swelling of a submicron poly(vinyl alcohol) (PVA) film integrated with metallic nanoresonators. Conventional THz modulators typically require bulk-like membranes tens of micrometers thick to compensate for weak light-matter interaction, which inevitably results in slow, diffusion-limited response times. In contrast, our approach utilizes field confinement near nanometer gaps to achieve high modulation depth with an ultrathin layer, offering a potential route to high-speed operation. Under 90% relative humidity, the 193 nm PVA film swells to 380 nm, exhibiting a rapid response time of 373 ms─nearly three times faster than 1.25 μm films. The hybrid structure achieves a 13.6% transmission modulation, driven by a localized dielectric transition at electric-field hot-spots. These findings provide a robust strategy for high-performance THz metasurfaces that bypass the traditional trade-off between modulation depth and response speed.
Hotton C, Trazo JG, Modin E
… +11 more, Bardouil A, Kutalia N, Marcone J, Nag R, Goldmann C, Paineau E, Chuvilin A, Impéror-Clerc M, Bizien T, Constantin D, Hamon C
Evaporation-induced self-assembly transforms dilute nanoparticle suspensions into ordered plasmonic superlattices, yet the microscopic mechanisms remain unclear for anisotropic particles in water. Here, we study the dryi...Evaporation-induced self-assembly transforms dilute nanoparticle suspensions into ordered plasmonic superlattices, yet the microscopic mechanisms remain unclear for anisotropic particles in water. Here, we study the drying kinetics of silver nanorod (AgNR) dispersions in cetyltrimethylammonium chloride (CTAC) using time-resolved levitated small-angle X-ray scattering (SAXS), complemented by microbeam SAXS and focused ion beam-scanning electron microscopy on dried samples. The key parameter governing superlattice formation is the initial surfactant concentration, outweighing nanoparticle concentration and shape effects. AgNR ordering is synchronized with surfactant organization: CTAC micelles induce depletion attractions that drive nucleation and growth, followed by structural arrest upon CTAC gelation. These findings are directly relevant for improving the design of plasmonic metamaterial and nanoparticle (NP) self-assemblies in a broad sense. Moreover, the dual role played by CTAC micelles (promotion of NPs ordering followed by structural arrest) likely represents a mechanism applicable to other systems where depletants undergo gelation during drying.
Colloidal quantum dot photodiodes (QDPDs) are becoming an increasingly mature technology for infrared sensing and imaging that can offer high detectivity, short response times, and micrometer-scale pixelation. Even so, Q...Colloidal quantum dot photodiodes (QDPDs) are becoming an increasingly mature technology for infrared sensing and imaging that can offer high detectivity, short response times, and micrometer-scale pixelation. Even so, QDPDs suffer from a limited linear dynamic range (LDR), with photocurrents saturating at modest light intensities. Here, we analyze this remaining QDPD bottleneck in PbS-based QDPDs through operando transient absorption spectroscopy. As compared to isolated QDs, we find that recombination of photogenerated charge carriers accelerates in device-ready QD films and full QDPD stacks. Supported by kinetic Monte Carlo simulations, we assign this loss pathway to trion recombination mediated by hopping and doping-induced background charges, and we show that the photocurrent saturates when the rate of trion recombination and charge separation match. On the basis of this result, we argue that the widely varying literature data on the linear dynamic range of QDPDs mainly reflect different carrier extraction rates and conclude that faster carrier extraction is essential to extend the linear dynamic range.
Nanoscale heat transport plays an important role in energy conversion and thermal management. Therefore, understanding how nanoscale heat transport can be tuned is critical for developing novel technologies, including co...Nanoscale heat transport plays an important role in energy conversion and thermal management. Therefore, understanding how nanoscale heat transport can be tuned is critical for developing novel technologies, including cooling strategies for microelectronics and nanostructured materials and devices for high-efficiency energy conversion. To probe nanoscale thermal transport phenomena, many calorimetric tools and approaches have been developed. Specifically, suspended microcalorimeters featuring picowatt resolution have been extensively employed for measuring thermal transport in low-dimensional materials, radiative heat transfer in nanoscale gaps, and between subwavelength structures. Further, scanning calorimetric probes, combined with atomic force microscopy and scanning tunneling microscopy, have been utilized for probing atomic-scale thermal transport and near-field thermal radiation. Here, we discuss these advances in calorimetric tools and their use for studying nanoscale thermal transport. We conclude by discussing open experimental challenges and highlighting the importance of future developments in subpicowatt resolution calorimetric tools for accessing unexplored nanoscale thermal transport phenomena.