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Universality of strain-induced anisotropic friction domains on 2D materials
摘要： Van der Waals two-dimensional (2D) materials have shown various physical characteristics depending on their growth methods and conditions. Among those characteristics, the surface structural properties are crucial for the application of 2D materials, as the surface structures readily affect their atomic arrangements and/or interaction with substrates due to their atomic-scale thicknesses. Here, we report on the anisotropic friction domains of MoS2 grown not only by chemical vapor deposition (CVD) under various sulfur pressure conditions but also by a mechanical exfoliation process. The 180° periodicity of each domain and the 60° shift between adjacent domains indicate the presence of linearly aligned structures along the armchair direction of MoS2, which is determined by the optical second-harmonic generation method. The anisotropic friction domains of CVD-grown MoS2 ?akes may be attributed to linearly aligned ripples caused by an inhomogeneous strain ?eld distribution, which is due, in turn, to randomly formed nucleation sites on the substrate. The universality of the anisotropic frictional behaviors of 2D materials, including graphene, hBN, and WS2 with honeycomb lattice stacking, which differ from ReSe2 with a distorted triclinic 1T’ structure, supports our assumption based on the linearly aligned ripples along the crystallographic axes, which result from an inhomogeneous strain ?eld.
关键词： strain-induced ripples,chemical vapor deposition,mechanical exfoliation,anisotropic friction domains,Van der Waals two-dimensional materials
更新于2025-09-04 15:30:14
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Two-dimensional ultraviolet spectroscopy of proteins
摘要： Two-dimensional ultraviolet (2DUV) spectroscopy is a novel technology for probing molecular structure. We have developed a generalized quantum mechanics/molecular mechanics (QM/MM) approach to simulate the electronic transitions of protein backbones and aromatic amino acids in aqueous solution. These transitions, which occur in the ultraviolet (UV) region, provide a sensitive probe of molecular structure. The features of 2DUV spectra are accurately characterized and enable us to trace small variations in the structure and dynamics as well as evolution propensity with high accuracy. Various structures and dynamic phenomena are investigated to construct a systematic framework for 2DUV simulation mechanisms, so as to explore further applications of this technique. In this feature article, we summarize the theory and applications of 2DUV spectroscopy we have engaged in recently, present the important roles of 2DUV spectroscopy, and outline directions for future development. We hope this article can offer a platform for more scientists in different research fields to gain a clear overview of 2DUVand further attract more people to explore this promising field.
关键词： two-dimensional ultraviolet spectroscopy (2DUV),quantum mechanics/molecular dynamics (QM/MM),molecular structure and dynamics,protein
更新于2025-09-04 15:30:14
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Ultrafast Nonlinear Optical Excitation Behaviors of Mono- and Few-Layer Two Dimensional MoS2
摘要： The layered MoS2 has recently attracted significant attention for its excellent nonlinear optical properties. Here, the ultrafast nonlinear optical (NLO) absorption and excited carrier dynamics of layered MoS2 (monolayer, 3?4 layers, and 6?8 layers) are investigated via Z-scan and transient absorption spectra. Our experimental results reveal that NLO absorption coefficients of these MoS2 increase from ?27 × 103 cm/GW with more layers at 400-nm laser excitation, while the values decrease from 2.0 × 103 cm/GW at 800 nm. In addition, at high pump fluence, when the NLO response occurs, the results show that not only the reformation of the excitonic bands, but also the recovery time of NLO response decreases from 150 ps to 100 ps with an increasing number of layers, while the reductive energy of A excitonic band decreases from 191.7 meV to 51.1 meV. The intriguing NLO response of MoS2 provides excellent potentials for the next-generation optoelectronic and photonic devices.
关键词： ultrafast photonic devices,Ultrafast optics,two-dimensional materials
更新于2025-09-04 15:30:14
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Strong coupling of a two-dimensional electron ensemble to a single-mode cavity resonator
摘要： We investigate the regime of strong coupling of an ensemble of two-dimensional electrons to a single-mode cavity resonator. In particular, we realize such a regime of light-matter interaction by coupling the cyclotron motion of a collection of electrons on the surface of liquid helium to the microwave field in a semiconfocal Fabry-Pérot resonator. For the corotating component of the microwave field, the strong coupling is pronouncedly manifested by the normal-mode splitting in the spectrum of coupled field-particle motion. We present a complete description of this phenomenon based on classical electrodynamics, as well as show that the full quantum treatment of this problem results in mean-value equations of motion that are equivalent to our classical result. For the counterrotating component of the microwave field, we observe a strong resonance when the microwave frequency is close to both the cyclotron and cavity frequencies. We show that this surprising effect, which is not expected to occur under the rotating-wave approximation, results from the mixing between two polarization components of the microwave field in our cavity.
关键词： microwave field,classical electrodynamics,cavity resonator,normal-mode splitting,two-dimensional electrons,rotating-wave approximation,Fabry-Pérot resonator,strong coupling,quantum treatment,cyclotron motion
更新于2025-09-04 15:30:14
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Restriction of Molecular Rotors in Ultrathin Two-Dimensional Covalent Organic Framework Nanosheets for Sensing Signal Amplification
摘要： Covalent organic frameworks (COFs) have emerged as promising crystalline porous materials with well-defined structures, high porosity, tunable topology and functionalities suitable for various applications. However, studies of few-layered ultrathin two-dimensional (2D) COF nanosheets, which may lead to unprecedented properties and applications, are still limited. Herein we report the targeted synthesis of three azine-linked and imine-linked 2D COFs named NUS 30-32 using monomers containing aggregation-induced emission (AIE) rotor-active tetraphenylethylene (TPE) moieties, affording micro- and meso- dual pores in NUS-30 and NUS-32, and triple pores in NUS-31. For the first time, we demonstrate that these isostructural bulk COF powders can be exfoliated into ultrathin 2D nanosheets (2 – 4 nm thickness) by temperature-swing gas exfoliation approach. Compared with TPE monomers and COF model compounds, the AIE characteristic of NUS 30-32 nanosheets is distinctly suppressed due to the covalent restriction of the AIE molecular rotors in the confined 2D frameworks. As a result, the enhancement of conjugated conformations of NUS 30-32 nanosheets with unusual structure relaxation show signal amplification effect in biomolecular recognition of amino acids and small pharmaceutical molecules (L-dopa), exhibiting much higher sensitivity than their stacked bulk powders, TPE monomer, and COF model compound. Moreover, the binding affinity of the COF nanosheets toward amino acids can be controlled by increasing the number of azine moieties in the structure. Density functional theory (DFT) calculations reveal that binding affinity control results from the crucial geometric roles and stronger host-guest binding between azine moieties and amino acids. In addition, we demonstrate that minimal loading of the NUS-30 nanosheets in composite membranes can afford excellent performance for biomolecule detection. Our findings pave a way for the development of functional ultrathin 2D COF nanosheets with precise control over the nature, density, and arrangement of the binding active sites involved in enhanced molecule recognition.
关键词： molecular rotors,Covalent organic frameworks,aggregation-induced emission,biomolecular recognition,signal amplification,two-dimensional nanosheets
更新于2025-09-04 15:30:14
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Chemical Vapor Deposition Growth of Single Crystalline CoTe <sub/>2</sub> Nanosheets with Tunable Thickness and Electronic Properties
摘要： Two-dimensional (2D) metallic transition metal dichalcogenides (MTMDs) have recently drawn increasing interest for fundamental studies and potential applications in catalysis, charge density wave (CDW), interconnections, spin-torque devices, as well superconductors. Despite some initial efforts, the thickness-tunable synthesis of atomically thin MTMDs remains a considerable challenge. Here we report controlled synthesis of 2D cobalt telluride (CoTe2) nanosheets with tunable thickness using an atmospheric pressure chemical vapor deposition (APCVD) approach and investigate their thickness-dependent electronic properties. The resulting nanosheets show a well-faceted hexagonal or triangular geometry with a lateral dimension up to ～200 μm. Systematic studies of growth at varying growth temperatures or flow rates demonstrate that nanosheets thickness is readily tunable from over 30 nm down to 3.1 nm. X-ray diffraction (XRD), transmission electron microscopy (TEM), and high-resolution scanning transmission electron microscope (STEM) studies reveal the obtained CoTe2 nanosheets are high-quality single crystals in the hexagonal 1T phase. Electrical transport studies show the 2D CoTe2 nanosheets display excellent electrical conductivities up to 4.0 × 105 S m?1 and very high breakdown current densities up to 2.1 × 107 A/cm2, both with strong thickness tunability.
关键词： Two-dimensional (2D),cobalt telluride (CoTe2),electronic properties,chemical vapor deposition (CVD),metallic transition metal dichalcogenides (MTMDs)
更新于2025-09-04 15:30:14
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Entanglement of single-photons and chiral phonons in atomically thin WSe2
摘要： Quantum entanglement is a fundamental phenomenon that, on the one hand, reveals deep connections between quantum mechanics, gravity and spacetime1,2, and on the other hand, has practical applications as a key resource in quantum information processing3. Although it is routinely achieved in photon–atom ensembles4, entanglement involving solid-state5–7 or macroscopic objects8 remains challenging albeit promising for both fundamental physics and technological applications. Here, we report entanglement between collective, chiral vibrations in a two-dimensional WSe2 host—chiral phonons (CPs)—and single-photons emitted from quantum dots9–13 (QDs) present in it. CPs that carry angular momentum were recently observed in WSe2 and are a distinguishing feature of the underlying honeycomb lattice14,15. The entanglement results from a ‘which-way’ scattering process, involving an optical excitation in a QD and doubly-degenerate CPs, which takes place via two indistinguishable paths. Our unveiling of entanglement involving a macroscopic, collective excitation together with strong interactions between CPs and QDs in two-dimensional materials opens up ways for phonon-driven entanglement of QDs and engineering chiral or non-reciprocal interactions at the single-photon level.
关键词： chiral phonons,WSe2,two-dimensional materials,quantum dots,Quantum entanglement
更新于2025-09-04 15:30:14
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Piezotronics and piezo-phototronics in two-dimensional materials
摘要： This article discusses recent studies of piezotronics and piezo-phototronics of two-dimensional (2D) materials. Two-dimensional semiconductor materials have demonstrated excellent electronic and optoelectronic properties, and these ultrathin materials are candidates for next-generation devices. Among 2D semiconductors, transition-metal dichalcogenides in particular have large in-place piezoelectricity due to the noncentrosymmetry along the armchair direction. A strong coupling of piezoelectric and semiconducting properties has been reported for Schottky contacts and p–n junctions, even in single-layer materials. Since the carrier concentration of ultrathin 2D materials can be easily modulated by external piezocharges, layered composites of ferroelectric/2D materials also show promising piezotronic and piezo-phototronic properties.
关键词： piezo-phototronics,piezoelectricity,transition-metal dichalcogenides,piezotronics,two-dimensional materials
更新于2025-09-04 15:30:14
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A First-Principles Study on the Adsorption of Small Molecules on Arsenene: Comparison of Oxidation Kinetics in Arsenene, Antimonene, Phosphorene and InSe
摘要： Arsenene, a new group V two-dimensional (2D) semiconducting material beyond phosphorene and antimonene, has recently gained an increasing attention owning to its various interesting properties which can be altered or intentionally functionalized by chemical reactions with various molecules. This work provides a systematic study on the interactions of arsenene with the small molecules, including H2, NH3, O2, H2O, NO, and NO2. It is predicted that O2, H2O, NO, and NO2 are strong acceptors, while NH3 serves as a donor. Importantly, it is shown a negligible charge transfer between H2 and arsenene which is ten times lower than that between H2 and phosphorene and about thousand times lower than that between H2 and InSe and antimonene. The calculated energy barrier for O2 splitting on arsenene is found to be as low as 0.67 eV. Thus, pristine arsenene may easily oxidize in ambient conditions as other group V 2D materials. On the other hand, the acceptor role of H2O on arsenene, similarly to the cases of antimonene and InSe, may help to prevent the proton transfer between H2O and O– species by forming acids, which suppresses further structural degradation of arsenene. The structural decomposition of the 2D layers upon interaction with the environment may be avoided due to the acceptor role of H2O molecules as the study predicts from the comparison of common group V 2D materials. However, the protection for arsenene is still required due to its strong interaction with other small environmental molecules. The present work renders the possible ways to protect arsenene from structure degradation and to modulate its electronic properties, which is useful for the material synthesis, storage and applications.
关键词： group V two-dimensional materials,electronic structure,first-principles calculations,O2 molecule splitting,arsenene
更新于2025-09-04 15:30:14
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[Topics in Current Chemistry Collections] Multidimensional Time-Resolved Spectroscopy || Electronic Couplings in (Bio-) Chemical Processes
摘要： During the last two decades, 2D optical techniques have been extended to the visible range, targeting electronic transitions. Since the report of the very first 2D electronic measurement (Hybl et al. in J Chem Phys 115:6606–6622, [2001]), two-dimensional electronic spectroscopy (2DES) has allowed fundamentally new insights into the structure and dynamics of condensed-phase systems (Ginsberg et al. in Acc Chem Res 42:1352–1363, 2009; Jonas in Annu Rev Phys Chem 54:425–463, 2003), producing experiments that measure correlations among electronic states of an absorbing species within complex systems. 2DES is used to investigate photophysical phenomena involving electronic or vibrational couplings in multi-chromophoric systems [energy transfer in photosynthesis is one great example of how 2DES can disentangle various energy transfer pathways (Brixner et al. in Nature 625–628, 2005; Engel et al. in Nature 446:782–786, 2007; Collini et al. in Nature 463:644–647, 2010)], but also ultrafast photochemical processes in which the tracked molecules change permanently or are heterogeneous (Ruetzel et al. in Proc Natl Acad Sci 111:4764–4769, 2014; Consani et al. in Science 339:1586–1589, 2013). We divide this chapter according to some of the major areas that have been established thanks to 2DES in the following fields: heterogeneity of systems, excitation energy transfer mechanisms, photo-induced coherent oscillations associated with electronic and vibrational couplings, and complex chemical reactions (Fig. 1).
关键词： Energy transfer,Vibronic coupling,Two-dimensional electronic spectroscopy,Photoreactivity,Heterogeneity
更新于2025-09-04 15:30:14