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A synthesis route to controlled and dynamic single polymer chain folding is reported. Sequence-controlled macromolecules containing precisely located selenol moieties within a polymer chain are synthesized. Oxidation of selenol functionalities lead to diselenide bridges and induces controlled intramolecular crosslinking to generate single chain collapse. The cyclization process is successfully characterized by SEC as well as by H-1 NMR and 2D HSQC NMR spectroscopies. In order to gain insight on the molecular level to reveal the degree of structural control, the folded polymers are transformed into folded molecular brushes that are known to be visualizable as single molecule structures by AFM. The "grafting onto" approach is performed by using triazolinedione-diene reaction to graft the side chain polymers. A series of folded molecular brushes as well as the corresponding linear controls are synthesized. AFM visualization is proving the cyclization of the folded backbone by showing globular objects, where non-folded brushes show typical worm-like structures. (C) 2019 The Authors. Journal of Polymer Science published by Wiley Periodicals, Inc.
Bacterial chemotaxis-a fundamental example of directional navigation in the living world-is key to many biological processes, including the spreading of bacterial infections. Many bacterial species were recently reported to exhibit several distinct swimming modes-the flagella may, for example, push the cell body or wrap around it. How do the different run modes shape the chemotaxis strategy of a multimode swimmer? Here, we investigate chemotactic motion of the soil bacterium Pseudomonas putida as a model organism. By simultaneously tracking the position of the cell body and the configuration of its flagella, we demonstrate that individual run modes show different chemotactic responses in nutrition gradients and, thus, constitute distinct behavioral states. On the basis of an active particle model, we demonstrate that switching between multiple run states that differ in their speed and responsiveness provides the basis for robust and efficient chemotaxis in complex natural habitats.
Photoluminescence spectroscopy is a widely applied characterization technique for semiconductor materials in general and halide perovskite solar cell materials in particular. It can give direct information on the recombination kinetics and processes as well as the internal electrochemical potential of free charge carriers in single semiconductor layers, layer stacks with transport layers, and complete solar cells. The correct evaluation and interpretation of photoluminescence requires the consideration of proper excitation conditions, calibration and application of the appropriate approximations to the rather complex theory, which includes radiative recombination, non-radiative recombination, interface recombination, charge transfer, and photon recycling. In this article, an overview is given of the theory and application to specific halide perovskite compositions, illustrating the variables that should be considered when applying photoluminescence analysis in these materials.
Photoluminescence spectroscopy is a widely applied characterization technique for semiconductor materials in general and halide perovskite solar cell materials in particular. It can give direct information on the recombination kinetics and processes as well as the internal electrochemical potential of free charge carriers in single semiconductor layers, layer stacks with transport layers, and complete solar cells. The correct evaluation and interpretation of photoluminescence requires the consideration of proper excitation conditions, calibration and application of the appropriate approximations to the rather complex theory, which includes radiative recombination, non-radiative recombination, interface recombination, charge transfer, and photon recycling. In this article, an overview is given of the theory and application to specific halide perovskite compositions, illustrating the variables that should be considered when applying photoluminescence analysis in these materials.
Transparent conductive materials based on indium oxide remain yet irreplaceable in various optoelectronic applications. Amorphous oxides appear especially attractive for technology as they are isotropic, demonstrate relatively high electron mobility and can be processed at low temperatures. Among them is indium zinc oxide (IZO) with a large zinc content that is crucial for keeping the amorphous state but redundant for the doping. In this work we investigated water-free and water containing IZO films obtained by radio frequency sputtering. The correlation between temperature driven changes of the chemical state, the optical and electrical properties as well as the progression of crystallization was in focus. Such characterization methods as: scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectroscopy, temperature dependent Hall-effect measurements and others were applied. Temperature dependent electrical properties of amorphous IZO and IZO:H2O films were found to evolve similarly. Based on our experience in In2O3:H2O (In2O3:H or IOH) we proposed an explanation for the changes observed. Water admixture was found to decrease crystallization temperature of IZO significantly from similar to 550 degrees C to similar to 280 degrees C. Herewith, the presence and concentration of water and/or hydroxyls was found to determine Zn distribution in the film. In particular, Zn enrichment was detected at the film's surface respective to the high water and/or hydroxyl amount. Raman spectra revealed a two-dimensional crystallization of w-ZnO which precedes regardless water presence an extensive In2O3 crystallization. An abrupt loss of electron mobility as a result of crystallization was attributed to the formation of ZnO interlayer on grain boundaries.
We investigate the initiation and early evolution of 12 solar eruptions, including six active-region hot channel and six quiescent filament eruptions, which were well observed by the Solar Dynamics Observatory, as well as by the Solar Terrestrial Relations Observatory for the latter. The sample includes one failed eruption and 11 coronal mass ejections, with velocities ranging from 493 to 2140 km s(-1). A detailed analysis of the eruption kinematics yields the following main results. (1) The early evolution of all events consists of a slow-rise phase followed by a main-acceleration phase, the height-time profiles of which differ markedly and can be best fit, respectively, by a linear and an exponential function. This indicates that different physical processes dominate in these phases, which is at variance with models that involve a single process. (2) The kinematic evolution of the eruptions tends to be synchronized with the flare light curve in both phases. The synchronization is often but not always close. A delayed onset of the impulsive flare phase is found in the majority of the filament eruptions (five out of six). This delay and its trend to be larger for slower eruptions favor ideal MHD instability models. (3) The average decay index at the onset heights of the main acceleration is close to the threshold of the torus instability for both groups of events (although, it is based on a tentative coronal field model for the hot channels), suggesting that this instability initiates and possibly drives the main acceleration.
We investigate the initiation and early evolution of 12 solar eruptions, including six active-region hot channel and six quiescent filament eruptions, which were well observed by the Solar Dynamics Observatory, as well as by the Solar Terrestrial Relations Observatory for the latter. The sample includes one failed eruption and 11 coronal mass ejections, with velocities ranging from 493 to 2140 km s(-1). A detailed analysis of the eruption kinematics yields the following main results. (1) The early evolution of all events consists of a slow-rise phase followed by a main-acceleration phase, the height-time profiles of which differ markedly and can be best fit, respectively, by a linear and an exponential function. This indicates that different physical processes dominate in these phases, which is at variance with models that involve a single process. (2) The kinematic evolution of the eruptions tends to be synchronized with the flare light curve in both phases. The synchronization is often but not always close. A delayed onset of the impulsive flare phase is found in the majority of the filament eruptions (five out of six). This delay and its trend to be larger for slower eruptions favor ideal MHD instability models. (3) The average decay index at the onset heights of the main acceleration is close to the threshold of the torus instability for both groups of events (although, it is based on a tentative coronal field model for the hot channels), suggesting that this instability initiates and possibly drives the main acceleration.
Fluorination of organic spacer impacts on the structural and optical response of 2D perovskites
(2020)
Low-dimensional hybrid perovskites have triggered significant research interest due to their intrinsically tunable optoelectronic properties and technologically relevant material stability. In particular, the role of the organic spacer on the inherent structural and optical features in two-dimensional (2D) perovskites is paramount for material optimization. To obtain a deeper understanding of the relationship between spacers and the corresponding 2D perovskite film properties, we explore the influence of the partial substitution of hydrogen atoms by fluorine in an alkylammonium organic cation, resulting in (Lc)(2)PbI4 and (Lf)(2)PbI4 2D perovskites, respectively. Consequently, optical analysis reveals a clear 0.2 eV blue-shift in the excitonic position at room temperature. This result can be mainly attributed to a band gap opening, with negligible effects on the exciton binding energy. According to Density Functional Theory (DFT) calculations, the band gap increases due to a larger distortion of the structure that decreases the atomic overlap of the wavefunctions and correspondingly bandwidth of the valence and conduction bands. In addition, fluorination impacts the structural rigidity of the 2D perovskite, resulting in a stable structure at room temperature and the absence of phase transitions at a low temperature, in contrast to the widely reported polymorphism in some non-fluorinated materials that exhibit such a phase transition. This indicates that a small perturbation in the material structure can strongly influence the overall structural stability and related phase transition of 2D perovskites, making them more robust to any phase change. This work provides key information on how the fluorine content in organic spacer influence the structural distortion of 2D perovskites and their optical properties which possess remarkable importance for future optoelectronic applications, for instance in the field of light-emitting devices or sensors.
Fluorination of organic spacer impacts on the structural and optical response of 2D perovskites
(2020)
Low-dimensional hybrid perovskites have triggered significant research interest due to their intrinsically tunable optoelectronic properties and technologically relevant material stability. In particular, the role of the organic spacer on the inherent structural and optical features in two-dimensional (2D) perovskites is paramount for material optimization. To obtain a deeper understanding of the relationship between spacers and the corresponding 2D perovskite film properties, we explore the influence of the partial substitution of hydrogen atoms by fluorine in an alkylammonium organic cation, resulting in (Lc)(2)PbI4 and (Lf)(2)PbI4 2D perovskites, respectively. Consequently, optical analysis reveals a clear 0.2 eV blue-shift in the excitonic position at room temperature. This result can be mainly attributed to a band gap opening, with negligible effects on the exciton binding energy. According to Density Functional Theory (DFT) calculations, the band gap increases due to a larger distortion of the structure that decreases the atomic overlap of the wavefunctions and correspondingly bandwidth of the valence and conduction bands. In addition, fluorination impacts the structural rigidity of the 2D perovskite, resulting in a stable structure at room temperature and the absence of phase transitions at a low temperature, in contrast to the widely reported polymorphism in some non-fluorinated materials that exhibit such a phase transition. This indicates that a small perturbation in the material structure can strongly influence the overall structural stability and related phase transition of 2D perovskites, making them more robust to any phase change. This work provides key information on how the fluorine content in organic spacer influence the structural distortion of 2D perovskites and their optical properties which possess remarkable importance for future optoelectronic applications, for instance in the field of light-emitting devices or sensors.
Organic photovoltaics based on non-fullerene acceptors (NFAs) show record efficiency of 16 to 17% and increased photovoltage owing to the low driving force for interfacial charge-transfer. However, the low driving force potentially slows down charge generation, leading to a tradeoff between voltage and current. Here, we disentangle the intrinsic charge-transfer rates from morphology-dependent exciton diffusion for a series of polymer:NFA systems. Moreover, we establish the influence of the interfacial energetics on the electron and hole transfer rates separately. We demonstrate that charge-transfer timescales remain at a few hundred femtoseconds even at near-zero driving force, which is consistent with the rates predicted by Marcus theory in the normal region, at moderate electronic coupling and at low re-organization energy. Thus, in the design of highly efficient devices, the energy offset at the donor:acceptor interface can be minimized without jeopardizing the charge-transfer rate and without concerns about a current-voltage tradeoff.
Organic photovoltaics based on non-fullerene acceptors (NFAs) show record efficiency of 16 to 17% and increased photovoltage owing to the low driving force for interfacial charge-transfer. However, the low driving force potentially slows down charge generation, leading to a tradeoff between voltage and current. Here, we disentangle the intrinsic charge-transfer rates from morphology-dependent exciton diffusion for a series of polymer:NFA systems. Moreover, we establish the influence of the interfacial energetics on the electron and hole transfer rates separately. We demonstrate that charge-transfer timescales remain at a few hundred femtoseconds even at near-zero driving force, which is consistent with the rates predicted by Marcus theory in the normal region, at moderate electronic coupling and at low re-organization energy. Thus, in the design of highly efficient devices, the energy offset at the donor:acceptor interface can be minimized without jeopardizing the charge-transfer rate and without concerns about a current-voltage tradeoff.
According to established understanding, deep-water formation in the North Atlantic and Southern Ocean keeps the deep ocean cold, counter-acting the downward mixing of heat from the warmer surface waters in the bulk of the world ocean. Therefore, periods of strong Atlantic meridional overturning circulation (AMOC) are expected to coincide with cooling of the deep ocean and warming of the surface waters. It has recently been proposed that this relation may have reversed due to global warming, and that during the past decades a strong AMOC coincides with warming of the deep ocean and relative cooling of the surface, by transporting increasingly warmer waters downward. Here we present multiple lines of evidence, including a statistical evaluation of the observed global mean temperature, ocean heat content, and different AMOC proxies, that lead to the opposite conclusion: even during the current ongoing global temperature rise a strong AMOC warms the surface. The observed weakening of the AMOC has therefore delayed global surface warming rather than enhancing it.
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The overturning circulation in the Atlantic Ocean has weakened in response to global warming, as predicted by climate models. Since it plays an important role in transporting heat, nutrients and carbon, a slowdown will affect global climate processes and the global mean temperature. Scientists have questioned whether this slowdown has worked to cool or warm global surface temperatures. This study analyses the overturning strength and global mean temperature evolution of the past decades and shows that a slowdown acts to reduce the global mean temperature. This is because a slower overturning means less water sinks into the deep ocean in the subpolar North Atlantic. As the surface waters are cold there, the sinking normally cools the deep ocean and thereby indirectly warms the surface, thus less sinking implies less surface warming and has a cooling effect. For the foreseeable future, this means that the slowing of the overturning will likely continue to slightly reduce the effect of the general warming due to increasing greenhouse gas concentrations.
Non-linear dielectric spectroscopy (NLDS) is employed as an effective tool to study relaxation processes and phase transitions of a poly(vinylidenefluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CFE)) relaxor-ferroelectric (R-F) terpolymer in detail. Measurements of the non-linear dielectric permittivity epsilon 2 ' reveal peaks at 30 and 80 degrees C that cannot be identified in conventional dielectric spectroscopy. By combining the results from NLDS experiments with those from other techniques such as thermally stimulated depolarization and dielectric-hysteresis studies, it is possible to explain the processes behind the additional peaks. The former peak, which is associated with the mid-temperature transition, is found in all other vinylidene fluoride-based polymers and may help to understand the non-zero epsilon 2 ' values that are detected on the paraelectric phase of the terpolymer. The latter peak can also be observed during cooling of P(VDF-TrFE) copolymer samples at 100 degrees C and is due to conduction and space-charge polarization as a result of the accumulation of real charges at the electrode-sample interface.
In classical thermodynamic processes the unavoidable presence of irreversibility, quantified by the entropy production, carries two energetic footprints: the reduction of extractable work from the optimal, reversible case, and the generation of a surplus of heat that is irreversibly dissipated to the environment. Recently it has been shown that in the quantum regime an additional quantum irreversibility occurs that is linked to decoherence into the energy basis. Here we employ quantum trajectories to construct distributions for classical heat and quantum heat exchanges, and show that the heat footprint of quantum irreversibility differs markedly from the classical case. We also quantify how quantum irreversibility reduces the amount of work that can be extracted from a state with coherences. Our results show that decoherence leads to both entropic and energetic footprints which both play an important role in the optimization of controlled quantum operations at low temperature.
In classical thermodynamics irreversibility occurs whenever a non-thermal system is brought into contact with a thermal environment. Using quantum trajectories the authors here establish two energetic footprints of quantum irreversible processes, and find that while quantum irreversibility leads to the occurrence of a quantum heat and a reduction of work production, the two are not linked in the same manner as the classical laws of thermodynamics would dictate.
In classical thermodynamic processes the unavoidable presence of irreversibility, quantified by the entropy production, carries two energetic footprints: the reduction of extractable work from the optimal, reversible case, and the generation of a surplus of heat that is irreversibly dissipated to the environment. Recently it has been shown that in the quantum regime an additional quantum irreversibility occurs that is linked to decoherence into the energy basis. Here we employ quantum trajectories to construct distributions for classical heat and quantum heat exchanges, and show that the heat footprint of quantum irreversibility differs markedly from the classical case. We also quantify how quantum irreversibility reduces the amount of work that can be extracted from a state with coherences. Our results show that decoherence leads to both entropic and energetic footprints which both play an important role in the optimization of controlled quantum operations at low temperature.
In classical thermodynamics irreversibility occurs whenever a non-thermal system is brought into contact with a thermal environment. Using quantum trajectories the authors here establish two energetic footprints of quantum irreversible processes, and find that while quantum irreversibility leads to the occurrence of a quantum heat and a reduction of work production, the two are not linked in the same manner as the classical laws of thermodynamics would dictate.
Estimating global mean sea-level rise and its uncertainties by 2100 and 2300 from an expert survey
(2020)
Sea-level rise projections and knowledge of their uncertainties are vital to make informed mitigation and adaptation decisions. To elicit projections from members of the scientific community regarding future global mean sea-level (GMSL) rise, we repeated a survey originally conducted five years ago. Under Representative Concentration Pathway (RCP) 2.6, 106 experts projected a likely (central 66% probability) GMSL rise of 0.30-0.65 m by 2100, and 0.54-2.15 m by 2300, relative to 1986-2005. Under RCP 8.5, the same experts projected a likely GMSL rise of 0.63-1.32 m by 2100, and 1.67-5.61 m by 2300. Expert projections for 2100 are similar to those from the original survey, although the projection for 2300 has extended tails and is higher than the original survey. Experts give a likelihood of 42% (original survey) and 45% (current survey) that under the high-emissions scenario GMSL rise will exceed the upper bound (0.98 m) of the likely range estimated by the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, which is considered to have an exceedance likelihood of 17%. Responses to open-ended questions suggest that the increases in upper-end estimates and uncertainties arose from recent influential studies about the impact of marine ice cliff instability on the meltwater contribution to GMSL rise from the Antarctic Ice Sheet.
Estimating global mean sea-level rise and its uncertainties by 2100 and 2300 from an expert survey
(2020)
Sea-level rise projections and knowledge of their uncertainties are vital to make informed mitigation and adaptation decisions. To elicit projections from members of the scientific community regarding future global mean sea-level (GMSL) rise, we repeated a survey originally conducted five years ago. Under Representative Concentration Pathway (RCP) 2.6, 106 experts projected a likely (central 66% probability) GMSL rise of 0.30-0.65 m by 2100, and 0.54-2.15 m by 2300, relative to 1986-2005. Under RCP 8.5, the same experts projected a likely GMSL rise of 0.63-1.32 m by 2100, and 1.67-5.61 m by 2300. Expert projections for 2100 are similar to those from the original survey, although the projection for 2300 has extended tails and is higher than the original survey. Experts give a likelihood of 42% (original survey) and 45% (current survey) that under the high-emissions scenario GMSL rise will exceed the upper bound (0.98 m) of the likely range estimated by the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, which is considered to have an exceedance likelihood of 17%. Responses to open-ended questions suggest that the increases in upper-end estimates and uncertainties arose from recent influential studies about the impact of marine ice cliff instability on the meltwater contribution to GMSL rise from the Antarctic Ice Sheet.
We investigate a diffusion process with a time-dependent diffusion coefficient, both exponentially increasing and decreasing in time, D(t)=D-0(e +/- 2 alpha t). For this (hypothetical) nonstationary diffusion process we compute-both analytically and from extensive stochastic simulations-the behavior of the ensemble- and time-averaged mean-squared displacements (MSDs) of the particles, both in the over- and underdamped limits. Simple asymptotic relations derived for the short- and long-time behaviors are shown to be in excellent agreement with the results of simulations. The diffusive characteristics in the presence of ageing are also considered, with dramatic differences of the over- versus underdamped regime. Our results for D(t)=D-0(e +/- 2 alpha t) extend and generalize the class of diffusive systems obeying scaled Brownian motion featuring a power-law-like variation of the diffusivity with time, D(t) similar to t(alpha-1). We also examine the logarithmically increasing diffusivity, D(t)=D(0)log[t/tau(0)], as another fundamental functional dependence (in addition to the power-law and exponential) and as an example of diffusivity slowly varying in time. One of the main conclusions is that the behavior of the massive particles is predominantly ergodic, while weak ergodicity breaking is repeatedly found for the time-dependent diffusion of the massless particles at short times. The latter manifests itself in the nonequivalence of the (both nonaged and aged) MSD and the mean time-averaged MSD. The current findings are potentially applicable to a class of physical systems out of thermal equilibrium where a rapid increase or decrease of the particles' diffusivity is inherently realized. One biological system potentially featuring all three types of time-dependent diffusion (power-law-like, exponential, and logarithmic) is water diffusion in the brain tissues, as we thoroughly discuss in the end.
Concentrating Solar Power (CSP) offers flexible and decarbonized power generation and is one of the few dispatchable renewable technologies able to generate renewable electricity on demand. Today (2018) CSP contributes only 5TWh to the European power generation, but it has the potential to become one of the key pillars for European decarbonization pathways. In this paper we investigate how factors and pivotal policy decisions leading to different futures and associated CSP deployment in Europe in the years up to 2050. In a second step we characterize the scenarios with their associated system cost and the costs of support policies. We show that the role of CSP in Europe critically depends on political developments and the success or failure of policies outside renewable power. In particular, the uptake of CSP depends on the overall decarbonization ambition, the degree of cross border trade of renewable electricity and is enabled by the presence of strong grid interconnection between Southern and Norther European Member States as well as by future electricity demand growth. The presence of other baseload technologies, prominently nuclear power in France, reduce the role and need for CSP. Assuming favorable technological development, we find a strong role for CSP in Europe in all modeled scenarios: contributing between 100TWh to 300TWh of electricity to a future European power system. This would require increasing the current European CSP fleet by a factor of 20 to 60 in the next 30 years. To achieve this financial support between € 0.4-2 billion per year into CSP would be needed, representing only a small share of overall support needs for power-system transformation. Cooperation of Member States could further help to reduce this cost.
To study binary neutron star systems and to interpret observational data such as gravitational-wave and kilonova signals, one needs an accurate description of the processes that take place during the final stages of the coalescence, for example, through numerical-relativity simulations. In this work, we present an updated version of the numerical-relativity code BAM in order to incorporate nuclear-theory-based equations of state and a simple description of neutrino interactions through a neutrino leakage scheme. Different test simulations, for stars undergoing a neutrino-induced gravitational collapse and for binary neutron stars systems, validate our new implementation. For the binary neutron stars systems, we show that we can evolve stably and accurately distinct microphysical models employing the different equations of state: SFHo, DD2, and the hyperonic BHB Lambda phi. Overall, our test simulations have good agreement with those reported in the literature.