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- ItemClimatic windows for human migration out of Africa in the past 300,000 years([London] : Nature Publishing Group UK, 2021) Beyer, Robert M.; Krapp, Mario; Eriksson, Anders; Manica, AndreaWhilst an African origin of modern humans is well established, the timings and routes of their expansions into Eurasia are the subject of heated debate, due to the scarcity of fossils and the lack of suitably old ancient DNA. Here, we use high-resolution palaeoclimate reconstructions to estimate how difficult it would have been for humans in terms of rainfall availability to leave the African continent in the past 300k years. We then combine these results with an anthropologically and ecologically motivated estimate of the minimum level of rainfall required by hunter-gatherers to survive, allowing us to reconstruct when, and along which geographic paths, expansions out of Africa would have been climatically feasible. The estimated timings and routes of potential contact with Eurasia are compatible with archaeological and genetic evidence of human expansions out of Africa, highlighting the key role of palaeoclimate variability for modern human dispersals.
- ItemXUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment([London] : Nature Publishing Group UK, 2015) Marciniak, A.; Despré, V.; Barillot, T.; Rouzée, A.; Galbraith, M.C.E.; Klei, J.; Yang, C.-H.; Smeenk, C.T.L.; Loriot, V.; Nagaprasad Reddy, S.; Tielens, A.G.G.M.; Mahapatra, S.; Kuleff, A.I.; Vrakking, M.J.J.; Lépine, F.Highly excited molecular species are at play in the chemistry of interstellar media and are involved in the creation of radiation damage in a biological tissue. Recently developed ultrashort extreme ultraviolet light sources offer the high excitation energies and ultrafast time-resolution required for probing the dynamics of highly excited molecular states on femtosecond (fs) (1 fs=10−15s) and even attosecond (as) (1 as=10−18 s) timescales. Here we show that polycyclic aromatic hydrocarbons (PAHs) undergo ultrafast relaxation on a few tens of femtoseconds timescales, involving an interplay between the electronic and vibrational degrees of freedom. Our work reveals a general property of excited radical PAHs that can help to elucidate the assignment of diffuse interstellar absorption bands in astrochemistry, and provides a benchmark for the manner in which coupled electronic and nuclear dynamics determines reaction pathways in large molecules following extreme ultraviolet excitation.
- ItemCubosomes from hierarchical self-assembly of poly(ionic liquid) block copolymers([London] : Nature Publishing Group UK, 2017) He, Hongkun; Rahimi, Khosrow; Zhong, Mingjiang; Mourran, Ahmed; Luebke, David R.; Nulwala, Hunaid B.; Möller, Martin; Matyjaszewski, KrzysztofCubosomes are micro- and nanoparticles with a bicontinuous cubic two-phase structure, reported for the self-assembly of low molecular weight surfactants, for example, lipids, but rarely formed by polymers. These objects are characterized by a maximum continuous interface and high interface to volume ratio, which makes them promising candidates for efficient adsorbents and host-guest applications. Here we demonstrate self-assembly to nanoscale cuboidal particles with a bicontinuous cubic structure by amphiphilic poly(ionic liquid) diblock copolymers, poly(acrylic acid)-block-poly(4-vinylbenzyl)-3-butyl imidazolium bis(trifluoromethylsulfonyl)imide, in a mixture of tetrahydrofuran and water under optimized conditions. Structure determining parameters include polymer composition and concentration, temperature, and the variation of the solvent mixture. The formation of the cubosomes can be explained by the hierarchical interactions of the constituent components. The lattice structure of the block copolymers can be transferred to the shape of the particle as it is common for atomic and molecular faceted crystals.
- ItemWeibull-distributed dyke thickness reflects probabilistic character of host-rock strength([London] : Nature Publishing Group UK, 2014) Krumbholz, Michael; Hieronymus, Christoph F.; Burchardt, Steffi; Troll, Valentin R.; Tanner, David C.; Friese, NadineMagmatic sheet intrusions (dykes) constitute the main form of magma transport in the Earth’s crust. The size distribution of dykes is a crucial parameter that controls volcanic surface deformation and eruption rates and is required to realistically model volcano deformation for eruption forecasting. Here we present statistical analyses of 3,676 dyke thickness measurements from different tectonic settings and show that dyke thickness consistently follows the Weibull distribution. Known from materials science, power law-distributed flaws in brittle materials lead to Weibull-distributed failure stress. We therefore propose a dynamic model in which dyke thickness is determined by variable magma pressure that exploits differently sized host-rock weaknesses. The observed dyke thickness distributions are thus site-specific because rock strength, rather than magma viscosity and composition, exerts the dominant control on dyke emplacement. Fundamentally, the strength of geomaterials is scale-dependent and should be approximated by a probability distribution.
- ItemClimate signals in river flood damages emerge under sound regional disaggregation([London] : Nature Publishing Group UK, 2021) Sauer, Inga J.; Reese, Ronja; Otto, Christian; Geiger, Tobias; Willner, Sven N.; Guillod, Benoit P.; Bresch, David N.; Frieler, KatjaClimate change affects precipitation patterns. Here, we investigate whether its signals are already detectable in reported river flood damages. We develop an empirical model to reconstruct observed damages and quantify the contributions of climate and socio-economic drivers to observed trends. We show that, on the level of nine world regions, trends in damages are dominated by increasing exposure and modulated by changes in vulnerability, while climate-induced trends are comparably small and mostly statistically insignificant, with the exception of South & Sub-Saharan Africa and Eastern Asia. However, when disaggregating the world regions into subregions based on river-basins with homogenous historical discharge trends, climate contributions to damages become statistically significant globally, in Asia and Latin America. In most regions, we find monotonous climate-induced damage trends but more years of observations would be needed to distinguish between the impacts of anthropogenic climate forcing and multidecadal oscillations.
- Item3,3-Difluoroallyl ammonium salts: highly versatile, stable and selective gem-difluoroallylation reagents([London] : Nature Publishing Group UK, 2021) Ye, Fei; Ge, Yao; Spannenberg, Anke; Neumann, Helfried; Xu, Li-Wen; Beller, MatthiasThe selective synthesis of fluorinated organic molecules continues to be of major importance for the development of bioactive compounds (agrochemicals and pharmaceuticals) as well as unique materials. Among the established synthetic toolbox for incorporation of fluorine-containing units, efficient and general reagents for introducing -CF2- groups have been largely neglected. Here, we present the synthesis of 3,3-difluoropropen-1-yl ammonium salts (DFPAs) as stable, and scalable gem-difluoromethylation reagents, which allow for the direct reaction with a wide range of fascinating nucleophiles. DFPAs smoothly react with N-, O-, S-, Se-, and C-nucleophiles under mild conditions without necessity of metal catalysts with exclusive regioselectivity. In this way, the presented reagents also permit the straightforward preparation of many analogues of existing pharmaceuticals.
- ItemUltra-strong bio-glue from genetically engineered polypeptides([London] : Nature Publishing Group UK, 2021) Ma, Chao; Sun, Jing; Li, Bo; Feng, Yang; Sun, Yao; Xiang, Li; Wu, Baiheng; Xiao, Lingling; Liu, Baimei; Petrovskii, Vladislav S.; Zhang, Jinrui; Wang, Zili; Li, Hongyan; Zhang, Lei; Li, Jingjing; Wang, Fan; Gӧstl, Robert; Potemkin, Igor I.; Chen, Dong; Zeng, Hongbo; Zhang, Hongjie; Liu, Kai; Herrmann, AndreasThe development of biomedical glues is an important, yet challenging task as seemingly mutually exclusive properties need to be combined in one material, i.e. strong adhesion and adaption to remodeling processes in healing tissue. Here, we report a biocompatible and biodegradable protein-based adhesive with high adhesion strengths. The maximum strength reaches 16.5 ± 2.2 MPa on hard substrates, which is comparable to that of commercial cyanoacrylate superglue and higher than other protein-based adhesives by at least one order of magnitude. Moreover, the strong adhesion on soft tissues qualifies the adhesive as biomedical glue outperforming some commercial products. Robust mechanical properties are realized without covalent bond formation during the adhesion process. A complex consisting of cationic supercharged polypeptides and anionic aromatic surfactants with lysine to surfactant molar ratio of 1:0.9 is driven by multiple supramolecular interactions enabling such strong adhesion. We demonstrate the glue’s robust performance in vitro and in vivo for cosmetic and hemostasis applications and accelerated wound healing by comparison to surgical wound closures.
- ItemSpatially explicit analysis identifies significant potential for bioenergy with carbon capture and storage in China([London] : Nature Publishing Group UK, 2021) Xing, Xiaofan; Wang, Rong; Bauer, Nico; Ciais, Philippe; Cao, Junji; Chen, Jianmin; Tang, Xu; Wang, Lin; Yang, Xin; Boucher, Olivier; Goll, Daniel; Peñuelas, Josep; Janssens, Ivan A.; Balkanski, Yves; Clark, James; Ma, Jianmin; Pan, Bo; Zhang, Shicheng; Ye, Xingnan; Wang, Yutao; Li, Qing; Luo, Gang; Shen, Guofeng; Li, Wei; Yang, Yechen; Xu, SiqingAs China ramped-up coal power capacities rapidly while CO2 emissions need to decline, these capacities would turn into stranded assets. To deal with this risk, a promising option is to retrofit these capacities to co-fire with biomass and eventually upgrade to CCS operation (BECCS), but the feasibility is debated with respect to negative impacts on broader sustainability issues. Here we present a data-rich spatially explicit approach to estimate the marginal cost curve for decarbonizing the power sector in China with BECCS. We identify a potential of 222 GW of power capacities in 2836 counties generated by co-firing 0.9 Gt of biomass from the same county, with half being agricultural residues. Our spatially explicit method helps to reduce uncertainty in the economic costs and emissions of BECCS, identify the best opportunities for bioenergy and show the limitations by logistical challenges to achieve carbon neutrality in the power sector with large-scale BECCS in China.
- ItemDirect supercritical angle localization microscopy for nanometer 3D superresolution([London] : Nature Publishing Group UK, 2021) Dasgupta, Anindita; Deschamps, Joran; Matti, Ulf; Hübner, Uwe; Becker, Jan; Strauss, Sebastian; Jungmann, Ralf; Heintzmann, Rainer; Ries, Jonas3D single molecule localization microscopy (SMLM) is an emerging superresolution method for structural cell biology, as it allows probing precise positions of proteins in cellular structures. In supercritical angle localization microscopy (SALM), z-positions of single fluorophores are extracted from the intensity of supercritical angle fluorescence, which strongly depends on their distance to the coverslip. Here, we realize the full potential of SALM and improve its z-resolution by more than four-fold compared to the state-of-the-art by directly splitting supercritical and undercritical emission, using an ultra-high NA objective, and applying fitting routines to extract precise intensities of single emitters. We demonstrate nanometer isotropic localization precision on DNA origami structures, and on clathrin coated vesicles and microtubules in cells, illustrating the potential of SALM for cell biology.
- ItemA low pre-infall mass for the Carina dwarf galaxy from disequilibrium modeling([London] : Nature Publishing Group UK, 2015) Ural, Uğur; Wilkinson, Mark I.; Read, Justin I.; Walker, Matthew G.Dark matter-only simulations of galaxy formation predict many more subhalos around a Milky Way-like galaxy than the number of observed satellites. Proposed solutions require the satellites to inhabit dark matter halos with masses 109–1010Msun at the time they fell into the Milky Way. Here we use a modelling approach, independent of cosmological simulations, to obtain a pre-infall mass of Msun for one of the Milky Way’s satellites: Carina. This determination of a low halo mass for Carina can be accommodated within the standard model only if galaxy formation becomes stochastic in halos below ∼1010Msun. Otherwise Carina, the eighth most luminous Milky Way dwarf, would be expected to inhabit a significantly more massive halo. The implication of this is that a population of ‘dark dwarfs’ should orbit the Milky Way: halos devoid of stars and yet more massive than many of their visible counterparts.