Recent publications
Precision graphene nanoribbons (GNRs) offer distinctive physicochemical properties that are highly dependent on their geometric topologies, thereby holding great potential for applications in carbon‐based optoelectronics and spintronics. While the edge structure and width control has been a popular strategy for engineering the optoelectronic properties of GNRs, non‐hexagonal‐ring‐containing GNRs remain underexplored due to synthetic challenges, despite offering an equally high potential for tailored properties. Herein, we report the synthesis of a wavy GNR (wGNR) by embedding periodic eight‐membered rings into its carbon skeleton, which is achieved by the A2B2‐type Diels–Alder polymerization between dibenzocyclooctadiyne (6) and dicyclopenta[e,l]pyrene‐5,11‐dione derivative (8), followed by a selective Scholl reaction of the obtained ladder‐type polymer (LTP) precursor. The obtained wGNR, with a length of up to 30 nm, has been thoroughly characterized by solid‐state NMR, FT‐IR, Raman, and UV/Vis spectroscopy with the support of DFT calculations. The non‐planar geometry of wGNR efficiently prevents the inter‐ribbon π–π aggregation, leading to photoluminescence in solution. Consequently, the wGNR can function as an emissive layer for organic light‐emitting electrochemical cells (OLECs), offering a proof‐of‐concept exploration in implementing luminescent GNRs into optoelectronic devices. The fast‐responding OLECs employing wGNR will pave the way for advancements in OLEC technology and other optoelectronic devices.
Metal oxide nanostructures with single-atomic heteroatom incorporation are of interest for many applications. However, a universal and scalable synthesis approach with high heteroatom concentrations represents a formidable challenge, primarily due to the pronounced structural disparities between Mhetero–O and Msub–O units. Here, focusing on TiO2 as the exemplified substrate, we present a diethylene glycol-assisted synthetic platform tailored for the controlled preparation of a library of M1-TiO2 nanostructures, encompassing 15 distinct unary M1-TiO2 nanostructures, along with two types of binary and ternary composites. Our approach capitalizes on the unique properties of diethylene glycol, affording precise kinetic control by passivating the hydrolytic activity of heteroatom and simultaneously achieving thermodynamic control by introducing short-range order structures to dissipate the free energy associated with heteroatom incorporation. The M1-TiO2 nanostructures, characterized by distinctive and abundant M–O–Ti units on the surface, exhibit high efficiency in photochromic photothermal catalysis toward recycling waste polyesters. This universal synthetic platform contributes to the preparation of materials with broad applicability and significance across catalysis, energy conversion, and biomedicine.
Unlocking the potential of topological order in many-body spin systems has been a key goal in quantum materials research. Despite extensive efforts, the quest for a versatile platform enabling site-selective spin manipulation, essential for tuning and probing diverse topological phases, has persisted. Here we utilize on-surface synthesis to construct spin-1/2 alternating-exchange Heisenberg chains by covalently linking Clar’s goblets—nanographenes each hosting two antiferromagnetically coupled spins. Using scanning tunnelling microscopy, we exert atomic-scale control over chain lengths, parities and exchange-coupling terminations, and probe their magnetic response via inelastic tunnelling spectroscopy. Our investigation confirms the gapped nature of bulk excitations in the chains, known as triplons. Their dispersion relation is extracted from the spatial variation of tunnelling spectral amplitudes. Depending on the parity and termination of chains, we observe varying numbers of in-gap spin-1/2 edge excitations, reflecting the degeneracy of distinct topological ground states in the thermodynamic limit. By monitoring interactions between these edge spins, we identify the exponential decay of spin correlations. Our findings present a phase-controlled many-body platform, opening avenues toward spin-based quantum devices.
Superconducting diode effects have recently attracted much attention for their potential applications in superconducting logic circuits. Several pathways have been proposed to give rise to non-reciprocal critical currents in various superconductors and Josephson junctions. In this work, we establish the presence of a large Josephson diode effect in a type-II Dirac semimetal 1T-PtTe2 facilitated by its helical spin-momentum locking and distinguish it from extrinsic geometric effects. The magnitude of the Josephson diode effect is shown to be directly correlated to the large second-harmonic component of the supercurrent. We denote such junctions, where the relative phase between the two harmonics can be tuned by a magnetic field, as ‘tunable second order φ0-junctions’. The direct correspondence between the second harmonic supercurrents and the diode effect in 1T-PtTe2 junctions at relatively low magnetic fields makes it an ideal platform to study the Josephson diode effect and Cooper quartet transport in Josephson junctions.
Recently discovered Mn-based kagome materials, such as RMn6Sn6 (R = rare-earth element), exhibit the coexistence of topological electronic states and long-range magnetic order, offering a platform for studying quantum phenomena. However, understanding the electronic and magnetic properties of these materials remains incomplete. Here, we investigate the electronic structure and magnetic properties of GdMn6Sn6 using x-ray magnetic circular dichroism, photoemission spectroscopy, and theoretical calculations. We observe localized electronic states from spin frustration in the Mn-based kagome lattice and induced magnetic moments in the nonmagnetic element Sn experimentally, which originate from the Sn-p and Mn-d orbital hybridization. Our calculations also reveal ferromagnetic coupling within the kagome Mn-Mn layer, driven by double exchange interaction. This work provides insights into the mechanisms of magnetic interaction and magnetic tuning in the exploration of topological quantum materials.
The manipulation and detection of mobile domain walls in nanoscopic magnetic wires underlies the development of multibit memories. The studies of such domain walls have focused on macroscopic wires that allow for optical detection by using magneto-optic effects. In this study, we demonstrated the electrical tracking with a spatial resolution of better than 40 nm of multiple mobile domain walls in nanoscopic racetracks, using a set of anomalous Hall detectors integrated into the racetracks. Electrical time-series signals from the Hall detectors allow for the static and dynamic phase space visualization of the dynamics of a domain wall or multiple domain walls that can be described by a multicore memristor model. The domain wall dynamics and stochasticity can be controlled in racetracks even to deep submicron dimensions.
Developing earth-abundant electrocatalysts with high activity and durability for acidic oxygen evolution reaction is essential for H2 production, yet it remains greatly challenging. Here, guided by theoretical calculations, the challenge of overcoming the balance between catalytic activity and dynamic durability for acidic OER in Co3O4 was effectively addressed via the preferential substitution of Ru for the Co²⁺ (Td) site of Co3O4. In situ characterization and DFT calculations show that the enhanced Co–O covalency after the introduction of Ru SAs facilitates the generation of OH* species and mitigates the unstable structure transformation via direct O–O coupling. The designed Ru SAs-CoOx catalyst (5.16 wt% Ru) exhibits enhanced OER activity (188 mV overpotential at 10 mA cm⁻²) and durability, outperforming most reported Co3O4-based and Ru-based electrocatalysts in acidic media.
State‐of‐the‐art inverted perovskite solar cells (PSCs) have exhibited considerable promise for commercialization due to their prospective stability. However, the intricate crystallization of halide perovskite, especially for multi‐component perovskites, not only distorts the surface lattice from its ideal form but also introduces numerous unsaturated dangling bonds to form surface defects, which can easily lead to reduced stability and poor performance. Herein, a surface lattice engineering is developed by coupling surface unsaturated ions and regulating ion bonding lengths/angles to achieve efficient and stable inverted PSCs. The renovated surface lattice not only eliminates shallow/deep level defects on the surface of perovskite, but also enhances photo/thermal stability of the materials. Moreover, the surface lattice engineering contributes to uniform potential surface, and improves energy‐level alignment at the interfaces of the perovskite and C60 carrier transport layer, enhancing charge carrier extraction and transportation. Finally, the champion PSC delivers an impressive efficiency of 25.82% (certified 25.5%). Moreover, these PSCs exhibit excellent operational stability, retaining 94% initial efficiency after more than ≈1 000h maximum power point test.
The emerging field of orbitronics aims to generate and control orbital angular momentum for information processing. Chiral crystals are promising orbitronic materials because they have been predicted to host monopole-like orbital textures, where the orbital angular momentum aligns isotropically with the electron’s crystal momentum. However, such monopoles have not yet been directly observed in chiral crystals. Here, we use circular dichroism in angle-resolved photoelectron spectroscopy to image orbital angular momentum monopoles in the chiral topological semimetals PtGa and PdGa. The spectra show a robust polar texture that rotates around the monopole as a function of photon energy. This is a direct consequence of the underlying magnetic orbital texture and can be understood from the interference of local atomic contributions. Moreover, we also demonstrate that the polarity of the monopoles can be controlled through the structural handedness of the host crystal by imaging orbital angular moment monopoles and antimonopoles in the two enantiomers of PdGa, respectively. Our results highlight the potential of chiral crystals for orbitronic device applications, and our methodology could enable the discovery of even more complicated nodal orbital angular momentum textures that could be exploited for orbitronics.
Precision graphene nanoribbons (GNRs) offer distinctive physicochemical properties that are highly dependent on their geometric topologies, thereby holding great potential for applications in carbon‐based optoelectronics and spintronics. While the edge structure and width control has been a popular strategy for engineering the optoelectronic properties of GNRs, non‐hexagonal‐ring‐containing GNRs remain underexplored due to synthetic challenges, despite offering an equally high potential for tailored properties. Herein, we report the synthesis of a wavy GNR (wGNR) embedding periodic eight‐membered rings into its carbon skeleton, which is achieved by the A2B2‐type Diels‐Alder polymerization between dibenzocyclooctadiyne (6) and dicyclopenta[e,l]pyrene‐5,11‐dione derivative (8), followed by a selective Scholl reaction of the obtained ladder‐type polymer (LTP) precursor. The obtained wGNR, with a length of up to 30 nm, is thoroughly characterized by solid‐state NMR, FT‐IR, Raman, and UV‐Vis spectroscopy with the support of DFT calculations. The non‐planar geometry of wGNR efficiently prevents the inter‐ribbon π‐π aggregation, leading to photoluminescence in solution. Consequently, the wGNR can function as an emissive layer for organic light‐emitting electrochemical cells (OLECs), offering a proof‐of‐concept exploration in implementing luminescent GNRs into optoelectronic devices. The fast‐responding OLECs employing wGNR will pave the way for advancements in OLEC technology and other optoelectronic devices.
Interfacial solar evaporation, harnessing sunlight to induce water molecule evaporation, holds great promise for sustainable solar energy conversion. However, challenges such as reduced efficiency and instability due to salt accumulation, inadequate water transport, and the high cost of advanced nanostructured solar evaporators collectively hinder the sustainable and large‐scale practical use of this technology. Herein, an eco‐friendly, floatable 3D solar seawater evaporator is developed by innovatively incorporating a lightweight foam ball enclosed in a porous cellulose hydrogel. The 3D evaporator achieves a high water evaporation rate of ≈2.01 kg m⁻² h⁻¹ under 1 Sun, owing to its super high photothermal efficiency of 117.9% and efficient internal water transport channels. Even at a 0° simulated solar angle, the 3D evaporator maintains 85.8% of the evaporation rate at a 90° simulated solar angle. Moreover, the salt self‐cleaning capability is realized by the autonomous rotation caused by salt deposition. Particularly, the 3D evaporator can be fabricated over a large area and maintain seawater evaporation performance and structural integrity for 28 days. This study provides novel economically feasible and sustainable large‐scale solutions for interfacial solar‐powered seawater treatment.
The coupling of circularly polarized light to local band structure extrema ("valleys”) in two dimensional semiconductors promises a new electronics based on the valley degree of freedom. Such pulses, however, couple only to valley charge and not to the valley current, precluding lightwave manipulation of this second vital element of valleytronic devices. Contradicting this established wisdom, we show that the few cycle limit of circularly polarized light is imbued with an emergent vectorial character that allows direct coupling to the valley current. The underlying physical mechanism involves the emergence of a momentum space valley dipole, the orientation and magnitude of which allows complete control over the direction and magnitude of the valley current. We demonstrate this effect via minimal tight-binding models both for the visible spectrum gaps of the transition metal dichalcogenides (generation time ~ 1 fs) as well as the infrared gaps of biased bilayer graphene ( ~ 14 fs); we further verify our findings with state-of-the-art time-dependent density functional theory incorporating transient excitonic effects. Our findings both mark a striking example of emergent physics in the ultrafast limit of light-matter coupling, as well as allowing the creation of valley currents on time scales that challenge quantum decoherence in matter.
Two‐dimensional polymers (2DPs) and their layer‐stacked 2D covalent organic frameworks (2D COFs) membranes hold great potential for harvesting sustainable osmotic energy. The nascent research has yet to simultaneously achieve high ionic flux and selectivity, primarily due to inefficient ion transport dynamics. This is directly related to ultrasmall pore size (<3 nm), much smaller than the duple Debye length in the diluted electrolyte (6–20 nm), as well as low charge density (<4.5 mC m⁻²). Here, we introduce a π‐conjugated viologen‐based 2DP (V2DP) membrane possessing a large pore size of 4.5 nm, strategically enhancing the overlapping of the electric double layer, coupled with an exceptional positive surface charge density (~6 mC m⁻²). These characteristics enable the membrane to facilitate high anion flux while maintaining ideal selectivity. Notably, V2DP membranes realize an impressive current density of 5.5×10³ A m⁻², surpassing benchmarks set by previously reported nanofluidic membranes. In the practical application scenario involving the mixing of artificial seawater and river water, the V2DP membranes exhibit a considerable ion transference number of 0.70 towards Cl⁻, contributing to an outstanding power density of ~55 W m⁻². Theoretical calculations reveal the important role of the large quantity of anion transport sites, which act as binding sites evenly located in the positively charged N‐containing pyridine rings. These binding sites enable kinematic coupling and decoupling between anions and the V2DP skeleton, establishing a continuous Cl⁻ ion transport pathway. This work demonstrates the great promise of large‐area ultrathin 2DP membranes featuring highly organized charged ion transport networks when applied for osmotic energy conversion.
The biocompatibility and resorption characteristics of β-tricalcium phosphate (β-TCP, Ca3(PO4)2) have made it a coveted alternative for bone grafts. However, the underlying mechanisms governing the biological interactions between β-tricalcium phosphate and osteoclasts remain elusive. It has been speculated that the composition at grain boundaries might vary and affect β-TCP resorption properties. Atom probe tomography (APT) offers a quantitative approach to assess the composition of the grain boundaries, and thus advance our comprehension of the biological responses within the microstructure and chemical composition at the nanoscale. The precise quantitative analysis of chemical composition remains a notable challenge in APT, primarily due to the influence of measurement conditions on compositional accuracy. In this study, we investigated the impact of laser pulse energy on the composition of β-TCP using APT, aiming for the most precise Ca:P ratio and consistent results across multiple analyses performed with different sets of analysis conditions and on two different instruments.
The discovery of topological semimetals with multifold band crossings has opened up a new and exciting frontier in the field of topological physics. These materials exhibit large Chern numbers, leading to long double Fermi arcs on their surfaces, which are protected by either crystal symmetries or topological order. The impact of these multifold crossings extends beyond surface science, as they are not constrained by the Poincar classification of quasiparticles and only need to respect the crystal symmetry of one of the 1651 magnetic space groups. Consequently, we observe the emergence of free fermionic excitations in solid-state systems that have no high-energy counterparts, protected by non-symmorphic symmetries. In this work, we review the recent theoretical and experimental progress made in the field of multifold topological semimetals. We begin with the theoretical prediction of the so-called multifold fermions and discuss the subsequent discoveries of chiral and magnetic topological semimetals. Several experiments that have realized chiral semimetals in spectroscopic measurements are described, and we discuss the future prospects of this field. These exciting developments have the potential to deepen our understanding of the fundamental properties of quantum matter and inspire new technological applications in the future.
Passivation materials play a crucial role in a wide range of high-efficiency, high-stability photovoltaic applications based on crystalline silicon and state-of-the-art perovskite materials. Currently, for perovskite photovoltaic, the mainstream passivation strategies routinely rely on crystalline materials. Herein, we have invented a new amorphous (lysine)2PbI2 layer-enhanced halide perovskite. By utilizing a solid phase reaction between PbI2 and lysine molecule, an amorphous (lysine)2PbI2 layer is formed at surface/grain boundaries in the perovskite films. The amorphous (lysine)2PbI2 with fewer dangling bonds can effectively neutralize surface/interface defects, achieving an impressive efficiency of 26.27% (certified 25.94%). Moreover, this amorphous layer not only reduces crystal lattice stress but also functions as a barrier against the decomposition of organic components, leading to suppressed de-structuring of perovskite and highly stable perovskite solar cells.
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