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A robust understanding of the sub-seasonal cold season (November–March) precipitation variability over the High Mountains of Asia (HMA) is lacking. Here, we identify dynamic and thermodynamic pathways through which natural modes of climate variability establish their teleconnections over the HMA. First, we identify evaporative sources that contribute to the cold season precipitation over the HMA and surrounding areas. The predominant moisture contribution comes from the mid-latitude regions, including the Mediterranean/Caspian Seas and Mediterranean land. Second, we establish that several tropical and extratropical forcings display a sub-seasonally fluctuating influence on precipitation distribution over the region during the cold season. Many of them varyingly interact, so their impacts cannot be explained independently or at seasonal timescales. Lastly, a single set of evaporative sources is not identifiable as the key determinant in propagating a remote teleconnection because the sources of moisture anomalies depend on the pattern of sub-seasonally varying dynamical forcing in the atmosphere.
The monsoons in Pakistan have been exceptionally harsh in recent decades, resulting in extraordinary drought conditions and record flooding events. The changing characteristics of extreme events are widely attributed to climate change. However, given this region’s long history of floods and droughts, the role of natural climate variability cannot be rejected without a careful diagnosis. Here, we examine how oceanic and atmospheric variability has contributed to unusual precipitation distributions in West South Asia. Variations in sea surface temperatures in the tropical Pacific and northern Arabian Sea, and internal atmospheric variability related to the circumglobal teleconnection pattern and the subtropical westerly jet stream, explain more than 70% of monthly summer precipitation variability in the 21st century. Several of these forcings have co-occurred with record strength during episodes of extreme monsoons, which have exacerbated the overall effect. Climate change may have contributed to increased variability and the in-phase co-occurrences of the identified mechanisms, but further research is required to confirm any such connection.
In Central Southwest Asia (CSWA; 22°N to 40°N and 30°E to 70°E), winter (November to February) precipitation contributes up to 70% of the annual mean, but substantial interannual variations exist. Dynamical models exhibit subpar predictability in this region, but the limits of their skills are not well established. Here, we identify the tropical and extratropical forcings that explain ~75% of area-averaged seasonal variability in CSWA winter precipitation. Tropical forcing comes from the indirect El Niño-Southern Oscillation (ENSO) pathway, the leading mode of tropical Indian Ocean precipitation variability. This mode is coupled with ENSO-related Pacific Ocean sea surface temperature variability. A direct ENSO influence on CSWA does not extend beyond its Indian Ocean connection. Extratropical forcing comes from a large-scale mode of internal atmospheric variability. The spatial structure, variability of tropical forcing, and teleconnection with CSWA winter precipitation are skillfully depicted in two seasonal forecasting systems: the fifth-generation seasonal forecasting system (SEAS5) and Seamless System for Prediction and Earth System Research (SPEAR). Extratropical forcing’s spatial structure is also produced skillfully in the two modelling systems; however, the representation of its interannual variability and teleconnection requires improvement. While SEAS5 displays skill in representing extratropical forcing influence on CSWA winter precipitation and marginal skill in reproducing interannual variability, SPEAR has negligible ability in both areas. Consequently, these models have limited predictive skills over CSWA in winter. While improvements in representing extratropical forcing may be inherently limited as it arises from internal atmospheric variability, further research is needed to establish its predictability limits fully.
Abundant sodium (Na) batteries are a sustainable alternative to resource-constrained lithium-ion batteries, offering huge cost advantages. However, developing high-voltage anode-free sodium metal batteries (SMBs) to narrow the energy density gap with lithium-ion batteries is hindered by a critical challenge: existing electrolytes cannot simultaneously achieve ultra-high Na coulombic efficiency and anodic stability. Here, in this study, we present a rationally designed non-fluorinated electrolyte (1.0 M NaPF 6 in 1,2-diethoxyethane/1,2-di-tert-butoxyethane) to address this key limitation, achieving Na coulombic efficiency of >99.95% and anodic stability of >4.8 V. For coin cells (2.0 mAh cm −2 , N/P = 1.7), our electrolyte design enables 4.0 V Na | |Na 3 V 2 (PO 4 ) 3 (NVP) at 5 C and 4.3 V Na | |NaNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) at 0.3 C for 5,000 and 500 cycles with a capacity retention >80%. Remarkably, the 50 mAh anode-free pouch cells 4.0 V Al | |NVP and 4.3 V Al | |NMC622 also achieve 500 and 300 cycles (retention >75%) with a specific energy of >360 Wh kg (electrode) −1 . This work focuses on electrolyte optimization and conceptual advances, whereas critical aspects such as safety, large-scale manufacturability and practical feasibility of SMBs require further investigation. The electrolyte design using non-fluorinated solvents enhances the anodic stability without sacrificing Na efficiency, laying groundwork for advancing low-cost, high-energy SMBs and supporting the transition to sustainable battery technologies.
Different intensities of high temperatures affect the growth of photosynthetic cells in nature. To elucidate the underlying mechanisms, we cultivated the unicellular green alga Chlamydomonas reinhardtii under highly controlled photobioreactor conditions and revealed systems-wide shared and unique responses to 24-hour moderate (35°C) and acute (40°C) high temperatures and subsequent recovery at 25°C. We identified previously overlooked unique elements in response to moderate high temperature. Heat at 35°C transiently arrested the cell cycle followed by partial synchronization, up-regulated transcripts/proteins involved in gluconeogenesis/glyoxylate-cycle for carbon uptake and promoted growth. But 40°C disrupted cell division and growth. Both high temperatures induced photoprotection, while 40°C distorted thylakoid/pyrenoid ultrastructure, affected the carbon concentrating mechanism, and decreased photosynthetic efficiency. We demonstrated increased transcript/protein correlation during both heat treatments and hypothesize reduced post-transcriptional regulation during heat may help efficiently coordinate thermotolerance mechanisms. During recovery after both heat treatments, especially 40°C, transcripts/proteins related to DNA synthesis increased while those involved in photosynthetic light reactions decreased. We propose down-regulating photosynthetic light reactions during DNA replication benefits cell cycle resumption by reducing ROS production. Our results provide potential targets to increase thermotolerance in algae and crops.
Naturally occurring tropical Pacific variations at timescales of 7–70 years — tropical Pacific decadal variability (TPDV) — describe basin-scale sea surface temperature (SST), sea-level pressure and heat content anomalies. Several mechanisms are proposed to explain TPDV, which can originate through oceanic processes, atmospheric processes or as an El Niño/Southern Oscillation (ENSO) residual. In this Review, we synthesize knowledge of these mechanisms, their characteristics and contribution to TPDV. Oceanic processes include off-equatorial Rossby waves, which mediate oceanic adjustment and contribute to variations in equatorial thermocline depth and SST; variations in the strength of the shallow upper-ocean overturning circulation, which exhibit a large anti-correlation with equatorial Pacific SST at interannual and decadal timescales; and the propagation of salinity-compensated temperature (spiciness) anomalies from the subtropics to the equatorial thermocline. Atmospheric processes include midlatitude internal variability leading to tropical and subtropical wind anomalies, which result in equatorial SST anomalies and feedbacks that enhance persistence; and atmospheric teleconnections from Atlantic and Indian Ocean SST variability, which induce winds conducive to decadal anomalies of the opposite sign in the Pacific. Although uncertain, the tropical adjustment through Rossby wave activity is likely a dominant mechanism. Finally, a deeper understanding of the origin and spectral characteristics of TPDV-related winds is a key priority.
Nanotendril “fuzz” will grow under He bombardment under tokamak-relevant conditions on tungsten plasma-facing materials in a magnetic fusion energy device. We have grown tungsten nanotendrils at low (50 eV) and high (12 keV) He bombardment energy, in the range 900–1000 °C, and characterized them using electron microscopy. Low energy tendrils are finer (~22 nm diameter) than high-energy tendrils (~176 nm diameter), and low-energy tendrils have a smoother surface than high-energy tendrils. Cavities were omnipresent and typically ~5–10 nm in size. Oxygen was present at tendril surfaces, but tendrils were all BCC tungsten metal. Electron diffraction measured tendril growth axes and grain boundary angle/axis pairs; no preferential growth axes or angle/axis pairs were observed, and low-energy fuzz grain boundaries tended to be high angle; high energy tendril grain boundaries were not observed. We speculate that the strong tendency to high-angle grain boundaries in the low-energy tendrils implies that as the tendrils twist or bend, strain must accumulate until nucleation of a grain boundary is favorable compared to further lattice rotation. Finally, the high-energy tendrils consisted of very large (>100 nm) grains compared to the tendril size, so the nature of the high energy irradiation must enable faster growth with less lattice rotation.
The field-effect hole mobility of rubicene having high ionization energy (~5.5 eV) is 0.20 cm 2 V -1 s -1 and is improved to 0.32 cm 2 V -1 s -1 with PFBT SAM treatment which reduces the hole injection barrier and induces an edge-on configuration.
Novel electronically efficient s -indacene 1,3,5,7-tetraone derivatives were synthesized, which exhibit unique thermally induced polymorphic transformation.
We recently outlined an efficient multi-tiered parallel ab initio excitonic framework that utilizes time dependent density functional theory (TDDFT) to calculate ground and excited state energies and gradients of large supramolecular complexes in atomistic detail – enabling us to undertake non-adiabatic simulations which explicitly account for the coupled anharmonic vibrational motion of all the constituent atoms in a supramolecular system. Here we apply that framework to the 27 coupled bacterio-chlorophyll-a chromophores which make up the LH2 complex, using it to compute an on-the-fly nonadiabatic surface-hopping (SH) trajectory of electronically excited LH2. Part one of this article is focussed on calibrating our ab initio exciton Hamiltonian using two key parameters: a shift δ, which corrects for the error in TDDFT vertical excitation energies; and an effective dielectric constant ε, which describes the average screening of the transition-dipole coupling between chromophores. Using snapshots obtained from equilibrium molecular dynamics simulations (MD) of LH2, we tune the values of both δ and ε through fitting to the thermally broadened experimental absorption spectrum, giving a linear absorption spectrum that agrees reasonably well with experiment. In part two of this article, we construct a time-resolved picture of the coupled vibrational and excitation energy transfer (EET) dynamics in the sub-picosecond regime following photo-excitation. Assuming Franck–Condon excitation of a narrow eigenstate band centred at 800 nm, we use surface hopping to follow a single nonadiabatic dynamics trajectory within the full eigenstate manifold. Consistent with experimental data, this trajectory gives timescales for B800→B850 population transfer (τ B800→B850 ) between 650–1050 fs, and B800 population decay (τ 800→ ) between 10–50 fs. The dynamical picture that emerges is one of rapidly fluctuating LH2 eigenstates that are delocalized over multiple chromophores and undergo frequent crossing on a femtosecond timescale as a result of the atomic vibrations of the constituent chromophores. The eigenstate fluctuations arise from disorder that is driven by vibrational dynamics with multiple characteristic timescales. The scalability of our ab initio excitonic computational framework across massively parallel architectures opens up the possibility of addressing a wide range of questions, including how specific dynamical motions impact both the pathways and efficiency of electronic energy-transfer within large supramolecular systems.
We report the regioselective ortho -functionalization of PDI with aryl Grignard reagents. OPVs with these non-fullerene acceptors showed PCEs up to 5%, the highest reported for an acceptor with a single PDI core.
Time-resolved microwave conductivity reveals good carrier mobility and long carrier lifetimes in the layered organic metal halide compound (CH 3 NH 3 ) 2 Pb(SCN) 2 I 2 .
Here, perovskite-derived hybrid platinum iodides with the general formula A 2 Pt IV I 6 (A = formamidinium FA and guanidinium GUA) accommodate excess I 2 to yield hydrogen-bond-stabilized compounds where the I 2 forms catenates with I - anions on the PtI 6 octahedra.
Uncertainty analysis combines cost, performance and market factors to guide research and investment decisions for selected c-Si PV technologies.
Carbon nanotubes (CNTs) are stiff, all-carbon macromolecules with diameters as small as one nanometer and few microns long. Solutions of CNTs in chlorosulfonic acid (CSA) follow the phase behavior of rigid rod polymers interacting via a repulsive potential and display a liquid crystalline phase at sufficiently high concentration. Here, we show that small-angle X-ray scattering and polarized light microscopy data can be combined to characterize quantitatively the morphology of liquid crystalline phases formed in CNT solutions at concentrations from 3 to 6.5% by volume. We find that upon increasing their concentration, CNTs self-assemble into a liquid crystalline phase with a pleated texture and with a large inter-particle spacing that could be indicative of a transition to higher-order liquid crystalline phases. We explain how thermal undulations of CNTs can enhance their electrostatic repulsion and increase their effective diameter by an order of magnitude. By calculating the critical concentration, where the mean amplitude of undulation of an unconstrained rod becomes comparable to the rod spacing, we find that thermal undulations start to affect steric forces at concentrations as low as the isotropic cloud point in CNT solutions.
Vat photopolymerization (VP) has emerged as a promising additive manufacturing technique to allow rapid light-based fabrication of 3D objects from a liquid resin. Research in the field of vat photopolymerization spans across multiple disciplines from engineering and materials science to applied chemistry and physics. This perspective brings together early-career researchers from various disciplines in academia and national laboratories around the world to summarize the most recent advancements with special emphasis on the research highlighted as part of the Gordon Research Conference (GRC) 2024 meeting on Additive Manufacturing of Soft Materials. We provide an outlook on next-generation polymer processing methods from synthesis of novel materials to multimodality manufacturing and performance engineering. Further, this article combines the ideas of many of these junior researchers to present a vision for the future of the field by highlighting the challenges and opportunities that lie ahead.
Owing to the recent power outages caused by extreme events, installing battery energy storage and backup generators is important to improve resiliency for a grid-tied microgrid. In the design stage, the event occurrence time and duration, which are highly uncertain and cannot be effectively predicted, may affect the needed battery and backup generator capacity but are usually assumed to be pre-determined in utility planning tools. This study investigates the optimal battery and backup generator sizing problem considering the stochastic event occurrence time and duration for the grid-tied microgrid under islanded operation. The reliability requirement is quantified by the mean value of the critical customer interruption time in each stochastic islanding time window (ITW), whose length is the duration and the centre is the occurrence time. The stochastic ITW constraint is then transformed to a probability-weighted expression to derive an equivalent Mixed Integer Linear Programming model. Numerical simulations on a realistic grid-tied PV-based microgrid demonstrate that the total cost is reduced by 11.5% considering the stochastic ITW, compared with the deterministic ITW under the same reliability requirement.