Giant pyroelectricity in nanomembranes.

Pyroelectricity describes the generation of electricity by temporal temperature change in polar materials1-3. When free-standing pyroelectric materials approach the 2D crystalline limit, how pyroelectricity behaves remained largely unknown. Here, using three model pyroelectric materials whose bonding characters along the out-of-plane direction vary from van der Waals (In2Se3), quasi-van der Waals (CsBiNb2O7) to ionic/covalent (ZnO), we experimentally show the dimensionality effect on pyroelectricity and the relation between lattice dynamics and pyroelectricity. We find that, for all three materials, when the thickness of free-standing sheets becomes small, their pyroelectric coefficients increase rapidly. We show that the material with chemical bonds along the out-of-plane direction exhibits the greatest dimensionality effect. Experimental observations evidence the possible influence of changed phonon dynamics in crystals with reduced thickness on their pyroelectricity. Our findings should stimulate fundamental study on pyroelectricity in ultra-thin materials and inspire technological development for potential pyroelectric applications in thermal imaging and energy harvesting.

Soliton and dispersive wave generation with third-order dispersion and temporal boundary.

We investigate the pulse evolution and energy conservation condition at the temporal boundary under third-order dispersion. When the fundamental soliton crosses the temporal boundary and forms two reflected pulses and one transmitted pulse, the power of the transmitted pulse first increases and then decreases as the incident spectrum shifts toward the blue side. If the transmitted spectrum lies in the anomalous group-velocity dispersion region, second-order soliton is formed and dispersive wave is radiated. We present a modified phase-matching condition to predict the resonance frequencies. The predicted results are in good agreement with the results obtained by numerically solving the nonlinear Schrödinger equation.

Electrical Control and Transport of Tightly Bound Interlayer Excitons in a MoSe_{2}/hBN/MoSe_{2} Heterostructure.

Controlling interlayer excitons in Van der Waals heterostructures holds promise for exploring Bose-Einstein condensates and developing novel optoelectronic applications, such as excitonic integrated circuits. Despite intensive studies, several key fundamental properties of interlayer excitons, such as their binding energies and interactions with charges, remain not well understood. Here we report the formation of momentum-direct interlayer excitons in a high-quality MoSe_{2}/hBN/MoSe_{2} heterostructure under an electric field, characterized by bright photoluminescence (PL) emission with high quantum yield and a narrow linewidth of less than 4 meV. These interlayer excitons show electrically tunable emission energy spanning ∼180 meV through the Stark effect, and exhibit a sizable binding energy of ∼81 meV in the intrinsic regime, along with trion binding energies of a few millielectronvolts. Remarkably, we demonstrate the long-range transport of interlayer excitons with a characteristic diffusion length exceeding 10 µm, which can be attributed, in part, to their dipolar repulsive interactions. Spatially and polarization-resolved spectroscopic studies reveal rich exciton physics in the system, such as valley polarization, local trapping, and the possible existence of dark interlayer excitons. The formation and transport of tightly bound interlayer excitons with narrow linewidth, coupled with the ability to electrically manipulate their properties, open exciting new avenues for exploring quantum many-body physics, including excitonic condensate and superfluidity, and for developing novel optoelectronic devices, such as exciton and photon routers.

Spatiotemporal patterns, sustainability, and primary drivers of NDVI-derived vegetation dynamics (2003-2022) in Nepal.

Understanding the vegetation dynamics and their drivers in Nepal has significant scientific reference value for implementing sustainable ecological policies. This study provides a comprehensive analysis of the spatio-temporal variations in vegetation cover in Nepal from 2003 to 2022 using MODIS NDVI data and explores the effects of climatic factors and anthropogenic activities on vegetation. Mann-Kendall test was used to assess the significant trend in NDVI and was integrated with the Hurst exponent to predict future trends. The driving factors of NDVI dynamics were analyzed using Pearson's correlation, partial derivative, and residual analysis methods. The results indicate that over the last 20 years, Nepal has experienced an increasing trend in NDVI at 0.0013 year-1, with 80% of the surface area (vegetation cover) showing an increasing vegetation trend (~ 28% with a significant increase in vegetation). Temperature influenced vegetation dynamics in the higher elevation areas, while precipitation and human interventions influenced the lower elevation areas. The Hurst exponent analysis predicts an improvement in the vegetation cover (greening) for a larger area compared to vegetation degradation (browning). A significantly increased area of NDVI residuals indicates a positive anthropogenic influence on vegetation cover. Anthropogenic activities have a higher relative contribution to NDVI variation followed by temperature and then precipitation. The results of residual trend and Hurst analysis in different regions of Nepal help identify degraded areas, both in the present and future. This information can assist relevant authorities in implementing appropriate policies for a sustainable ecological environment.

Halogen-Free Donor Polymers Based on Dicyanobenzotriazole with Low Energy Loss and High Efficiency in Organic Solar Cells.

Halogenation of organic semiconductors is an efficient strategy for improving the performance of organic solar cells (OSCs), while the introduction of halogens usually involves complex synthetic process and serious environment pollution problems. Herein, three halogen-free ternary copolymer donors (PCNx, x = 3, 4, 5) based on electron-withdrawing dicyanobenzotriazole are reported. When blended with the Y6, PCN3 with strong interchain interactions results in appropriate crystallinity and thermodynamic miscibility of the blend film. Grazing-incidence wide-angle X-ray scattering measurements indicate that PCN3 has more ordered arrangement and stronger π-π stacking than previous PCN2. Fourier-transform photocurrent spectroscopy and external quantum efficiency of electroluminescence measurements show that PCN3-based OSCs have lower energy loss than PCN2, which leads to their higher open-circuit voltage (0.873 V). The device based on PCN3 reaches power conversion efficiency (PCE) of 15.33% in binary OSCs, one of the highest values for OSCs with halogen-free donor polymers. The PCE of 17.80% and 18.10% are obtained in PM6:PCN3:Y6 and PM6:PCN3:BTP-eC9 ternary devices, much higher than those of PM6:Y6 (16.31%) and PM6:BTP-eC9 (17.33%) devices. Additionally, this ternary OSCs exhibit superior stability compared to binary host system. This work gives a promising path for halogen-free donor polymers to achieve low energy loss and high PCE.

Nonlinear evolution of modulational instability under the interaction of Kerr nonlinearity with pure higher, even-order dispersion.

We investigate the nonlinear evolutions of modulation instability (MI) under the interaction of Kerr nonlinearity with pure higher, even-order dispersion (HEOD) by using the truncating method of three-wave mixing. For any HEOD, we find the phase-plane topological structure of the MI changes in three frequency regions whose ranges depend on the order of HEOD. And we present the novel types of nonlinear evolutions of the MI, which do not exist in the case of quadratic dispersion. Taking the pure-sextic dispersion as an example, the theoretical predictions of the MI evolutions are confirmed by numerically solving the modified nonlinear Schrödinger equation. Our results not only further deepen the understanding of MI, but also provide a universal guideline for experimental investigation of nonlinear waves, such as breather solitons or rogue waves excitation, in nonlinear Kerr media with pure HEOD.

Manipulating dispersive wave emission via temporal sinusoidal phase modulation.

We report the dispersive wave (DW) emission from the Gaussian pulse with temporal sinusoidal phase (TSP) modulation. The TSP-induced chirp can enhance or cancel the chirp generated by self-phase modulation by properly selecting the modulation parameters of TSP, which can influence the nonlinear propagation of the TSP-modulated pulse. It is shown that the TSP can effectively control the resonant frequency and energy conversion efficiency of the DW emission. We give a modified phase-matching condition to predict the resonant frequencies, which agree with the simulation results obtained by numerically solving the nonlinear Schrödinger equation. The enhanced conversion efficiency of the DWs can be increased up to 28% with only TSP modulation. Our results can extend the application of temporal phase modulation technology for wavelength conversion, and broadband supercontinuum generation.

Soliton-sinc optical pulse propagation in the presence of high-order effects.

We investigate the propagation dynamics of the soliton-sinc, a kind of novel hybrid pulse, in the presence of higher-order effects with emphasis on the third-order dispersion (TOD) and Raman effects. At variance with the fundamental sech soliton, the traits of the band-limited soliton-sinc pulse can effectively manipulate the radiation process of dispersive waves (DWs) induced by the TOD. The energy enhancement and the radiated frequency tunability strongly depend on the band-limited parameter. A modified phase-matching condition is proposed for predicting the resonant frequency of the DWs emitted by soliton-sinc pulses, which is verified by the numerically calculated results. In addition, Raman-induced frequency shift (RIFS) of the soliton sinc pulse increases exponentially with a decrease of the band-limited parameter. Finally, we further discuss the simultaneous contribution of the Raman and TOD effects to the generation of the DWs emitted from the soliton-sinc pulses. The Raman effect can then either reduce or amplify the radiated DWs depending on the sign of the TOD. These results show that soliton-sinc optical pulses should be relevant for practical applications such as broadband supercontinuum spectra generation as well as nonlinear frequency conversion.

Dispersive wave manipulation by the spectral Heaviside step phase modulation.

We investigate the dispersive waves (DWs) emitted from shaped pulses with spectral Heaviside step phases (HSPs). The spectrally HSP-modulated pulse exhibits a unique double-peak structure, where the intensity and separation of the twin peaks are determined by the modulation depth and frequency detuning. By tailoring the parameters of the HSP suitably, we can control the DW emission with regard to resonant frequency and conversion efficiency. As the intensity ratio or relative separation of neighboring peaks is elaborately chosen, the DW emission can be effectively boosted, or a solitonic cage can be constructed for realizing temporal reflections and refractions associated with spectral broadening and multi-peak spectra of the output DWs. These findings offer a straightforward and efficient approach for controlling the DW emission, which is highly relevant to the advancement of supercontinuum generation and wavelength conversion technology.

Spatio-temporal fusion of meteorological factors for multi-site PM2.5 prediction: A deep learning and time-variant graph approach.

In the field of environmental science, traditional methods for predicting PM2.5 concentrations primarily focus on singular temporal or spatial dimensions. This approach presents certain limitations when it comes to deeply mining the joint influence of multiple monitoring sites and their inherent connections with meteorological factors. To address this issue, we introduce an innovative deep-learning-based multi-graph model using Beijing as the study case. This model consists of two key modules: firstly, the 'Meteorological Factor Spatio-Temporal Feature Extraction Module'. This module deeply integrates spatio-temporal features of hourly meteorological data by employing Graph Convolutional Networks (GCN) and Long Short-Term Memory (LSTM) for spatial and temporal encoding respectively. Subsequently, through an attention mechanism, it retrieves a feature tensor associated with air pollutants. Secondly, these features are amalgamated with PM2.5 concentration values, allowing the 'PM2.5 Concentration Prediction Module' to predict with enhanced accuracy the joint influence across multiple monitoring sites. Our model exhibits significant advantages over traditional methods in processing the joint impact of multiple sites and their associated meteorological factors. By providing new perspectives and tools for the in-depth understanding of urban air pollutant distribution and optimization of air quality management, this model propels us towards a more comprehensive approach in tackling air pollution issues.

Liquid-Phase van der Waals Epitaxy of a Few-Layer and Unit-Cell Thick Ruddlesden-Popper Halide Perovskite.

2D Ruddlesden-Popper (RP) halide perovskites with natural multiple quantum well structures are an ideal platform to integrate into vertical heterostructures, which may introduce plentiful intriguing optoelectronic properties that are not accessible in a single bulk crystal. Here, we report liquid-phase van der Waals epitaxy of a 2D RP hybrid perovskite (4,4-DFPD)2PbI4 (4,4-DFPD is 4,4-difluoropiperidinium) on muscovite mica and fabricate a series of perovskite-perovskite vertical heterostructures by integrating it with a second 2D RP perovskite R-NPB [NPB = 1-(1-naphthyl)ethylammonium lead bromide] sheets. The grown (4,4-DFPD)2PbI4 nanobelt array can be multiple layers to unit-cell thin and are crystallographically aligned on the mica substrate. An interlayer photo emission in this R-NPB/(4,4-DFPD)2PbI4 heterostructure with a lifetime of about 25 ns at 120 K has been revealed. Our demonstration of epitaxial (4,4-DFPD)2PbI4 array grown on mica via liquid-phase van der Waals epitaxy provides a paradigm to prepare orderly distributed 2D RP hybrid perovskites for further integration into multiple heterostructures. The discovery of a new interlayer emission in the R-NPB/(4,4-DFPD)2PbI4 heterostructure enriches the basic understanding of interlayer charge transition in halide perovskite systems.

Defect-Assisted Anchoring of Pt Single Atoms on MoS2 Nanosheets Produces High-Performance Catalyst for Industrial Hydrogen Evolution Reaction.

Pt-based catalysts are currently the most efficient electrocatalysts for the hydrogen evolution reaction (HER), but the scarcity and high cost of Pt limit industrial applications. Downsizing Pt nanoparticles (NPs) to single atoms (SAs) can expose more active sites and increase atomic utilization, thus decreasing the cost. Here, a solar-irradiation strategy is used to prepare hybrid SA-Pt/MoS2 nanosheets (NSs) that demonstrate excellent HER activity (the overpotential at a current density of 10 mA cm-2 (η10 ) of 44 mV, and Tafel slope of 34.83 mV dec-1 in acidic media; η10 of 123 mV, and Tafel slope of 76.71 mV dec-1 in alkaline media). Defects and deformations introduced by thermal pretreatment of the hydrothermal MoS2 NSs promote anchoring and stability of Pt SAs. The fabrication of Pt SAs and NPs is easily controlled using different Pt-precursor concentrations. Moreover, SA-Pt/MoS2 produced under natural sunlight exhibits high HER performance (η10 of 55 mV, and Tafel slope of 43.54 mV dec-1 ), which indicates its viability for mass production. Theoretical simulations show that Pt improves the absorption of H atoms and the charge-transfer kinetics of MoS2 , which significantly enhance HER activity. A simple, inexpensive strategy for preparing SA-Pt/MoS2 hybrid catalysts for industrial HER is provided.

Controllable focusing behavior of chirped Pearcey-Gaussian pulses under time-dependent potentials.

We investigate the propagation dynamics of the Pearcey-Gaussian (PG) pulses in the presence of time-dependent potentials in a linear medium both theoretically and numerically. We demonstrate that the combination of the linear potential and the initial chirp of PG pulses can flexibly control the propagation trajectory and inherent focusing properties of the PG pulses. When the parabolic potential is taken into account, the chirped PG pulses are periodically focused and reversed. By adjusting the parabolic potential and the pulse chirp, the characteristics of the focal points, such as position, intensity, and spacing between focal points, can be manipulated effectively. The interaction of two temporally separated PG pulses still shows a periodic evolution with controllable focusing characteristics. These results can broaden the application range of PG pulses and provide some inspiration for the control of PG pulses under nonlinear conditions.

Effect of chirp on pulse reflection and refraction at a moving temporal boundary.

The reflection and refraction of chirped Gaussian pulse at a moving step refractive-index boundary are investigated. When a chirped Gaussian pulse crosses a temporal boundary, the shape of the reflected spectra is distorted by adjusting chirp parameters. However, the transmitted spectra retain the Gaussian shape. The shape of the final output spectra is the same if the absolute values of the chirp are the same. By changing the chirp values, we can control the energy of the reflected and transmitted pulses, and the splitting distance of the pulse at the temporal boundary. By adjusting the time-dependent refractive index, chirped Gaussian pulses can experience total internal reflection at the temporal boundary. When pulse splitting occurs in an anomalous dispersion region, the velocity of the transmitted pulse decreases.

Spatiotemporal doubly periodic waves in a phase-mismatched second-harmonic generation.

In this Letter, we present an analytical and numerical investigation to characterize the formation of quadratic doubly periodic waves originating from coherent modulation instability in a dispersive quadratic medium in the regime of cascading second-harmonic generation. To the best of our knowledge, such an endeavor has not been undertaken before, despite the growing relevance of doubly periodic solutions as the precursor of highly localized wave structures. Unlike the case with cubic nonlinearity, the periodicity of quadratic nonlinear waves can also be controlled by the wave-vector mismatch in addition to the initial input condition. Our results may impact widely on the formation, excitation, and control of extreme rogue waves and the description of modulation instability in a quadratic optical medium.

Raman-induced frequency shift of pure quartic solitons in optical fiber with quartic dispersion.

We investigate the impact of Raman scattering on pure quartic solitons (PQSs) in an optical fiber with quartic dispersion. An analytical expression of the Raman-induced frequency shift (RIFS) of a PQS is obtained by using the variational approach with the Gaussian function ansatz. We find the RIFS of a PQS is inversely proportional to the sixth power of pulse width, when the fiber is short enough. The RIFS of a PQS is more sensitive to the pulse width, compared with that of a conventional soliton which is inversely proportional to the fourth power of pulse width. The theoretical predictions show good agreement with numerical results. In addition, we also discuss the RIFS of the other three typical pulses with the same peak power and pulse width as the PQS. These results provide a thorough understanding of the role of higher-order nonlinear effects on the propagation dynamics of PQSs.

Automated detection of mild cognitive impairment and dementia from voice recordings: A natural language processing approach.

INTRODUCTION: Automated computational assessment of neuropsychological tests would enable widespread, cost-effective screening for dementia. METHODS: A novel natural language processing approach is developed and validated to identify different stages of dementia based on automated transcription of digital voice recordings of subjects' neuropsychological tests conducted by the Framingham Heart Study (n = 1084). Transcribed sentences from the test were encoded into quantitative data and several models were trained and tested using these data and the participants' demographic characteristics. RESULTS: Average area under the curve (AUC) on the held-out test data reached 92.6%, 88.0%, and 74.4% for differentiating Normal cognition from Dementia, Normal or Mild Cognitive Impairment (MCI) from Dementia, and Normal from MCI, respectively. DISCUSSION: The proposed approach offers a fully automated identification of MCI and dementia based on a recorded neuropsychological test, providing an opportunity to develop a remote screening tool that could be adapted easily to any language.

Activating Inert Surface Pt Single Atoms via Subsurface Doping for Oxygen Reduction Reaction.

The performance of single-atom catalysts strongly depends on their particular coordination environments in the near-surface region. Herein, we discover that engineering extra Pt single atoms in the subsurface (Ptsubsurf) can significantly enhance the catalytic efficiency of surface Pt single atoms toward the oxygen reduction reaction (ORR). We experimentally and theoretically investigated the effects of the Ptsubsurf single atoms implanted in different positions of the subsurface of Co particles. The local environments and catalytic properties of surface Pt1 are highly tunable via Ptsubsurf doping. Specifically, the obtained Pt1@Co/NC catalyst displays a remarkable performance for ORR, achieving mass activity of 4.2 mA µgPt-1 (28 times higher than that of commercial Pt/C) at 0.9 V versus reversible hydrogen electrode (RHE) in 0.1 M HClO4 solution with high stability over 30000 cycles.

Online water quality monitoring based on UV-Vis spectrometry and artificial neural networks in a river confluence near Sherfield-on-Loddon.

Water quality monitoring is very important in agricultural catchments. UV-Vis spectrometry is widely used in place of traditional analytical methods because it is cost effective and fast and there is no chemical waste. In recent years, artificial neural networks have been extensively studied and used in various areas. In this study, we plan to simplify water quality monitoring with UV-Vis spectrometry and artificial neural networks. Samples were collected and immediately taken back to a laboratory for analysis. The absorption spectra of the water sample were acquired within a wavelength range from 200 to 800 nm. Convolutional neural network (CNN) and partial least squares (PLS) methods are used to calculate water parameters and obtain accurate results. The experimental results of this study show that both PLS and CNN methods may obtain an accurate result: linear correlation coefficient (R2) between predicted value and true values of TOC concentrations is 0.927 with PLS model and 0.953 with CNN model, R2 between predicted value and true values of TSS concentrations is 0.827 with PLS model and 0.915 with CNN model. CNN method may obtain a better linear correlation coefficient (R2) even with small number of samples and can be used for online water quality monitoring combined with UV-Vis spectrometry in agricultural catchment.

Oligomer-Assisted Photoactive Layers Enable >18 % Efficiency of Organic Solar Cells.

Although ternary organic solar cells (OSCs) have unique advantages in improving device performance, the morphology assembly in the ternary-phase would be more uncertain or complex than that in the binary-phase. Here, we propose a new concept of oligomer-assisted photoactive layers for high-performance OSCs. The formed alloy-like phase of the oligomer : host polymer blend enabled the oligomer-assisted OSCs to fuse the advantages of both binary and ternary devices, exhibiting substantially enhanced performance and stability compared to the control devices. With the addition of oligomers, outstanding efficiencies of 17.33 % for a PM6 : Y6 device, 18.32 % for a PM6 : BTP-eC9 device, and 17.13 % for a PM6/Y6 pseudo-bilayer device were achieved, all of which are one of the highest values in their corresponding fields. The improved performance originated from the downshift energy levels, enhanced light absorption, optimized blend morphology, favorable charge dynamics, and reduced non-radiative energy loss.