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The combined effect of ultraviolet (UV) light soaking and self-assembled monolayer deposition on the work function (WF) of thin ZnO layers and on the efficiency of hole injection into the prototypical conjugated polymer poly(3-hexylthiophen-2,5-diyl) (P3HT) is systematically investigated. It is shown that the WF and injection efficiency depend strongly on the history of UV light exposure. Proper treatment of the ZnO layer enables ohmic hole injection into P3HT, demonstrating ZnO as a potential anode material for organic optoelectronic devices. The results also suggest that valid conclusions on the energy-level alignment at the ZnO/organic interfaces may only be drawn if the illumination history is precisely known and controlled. This is inherently problematic when comparing electronic data from ultraviolet photoelectron spectroscopy (UPS) measurements carried out under different or ill-defined illumination conditions.
We show that, although the equilibrium band dispersion of the Shockley-type surface state of two-dimensional Au(111) quantum films grown on W(110) does not deviate from the expected free-electron-like behavior, its nonequilibrium energy-momentum dispersion probed by time- and angle-resolved photoemission exhibits a remarkable kink above the Fermi level due to a significant enhancement of the effective mass. The kink is pronounced for certain thicknesses of the Au quantum well and vanishes in the very thin limit. We identify the kink as induced by the coupling between the Au(111) surface state and emergent quantum-well states which probe directly the buried gold-tungsten interface. The signatures of the coupling are further revealed by our time-resolved measurements which show that surface state and quantum-well states thermalize together behaving as dynamically locked electron populations. In particular, relaxation of hot carriers following laser excitation is similar for both surface state and quantum-well states and much slower than expected for a bulk metallic system. The influence of quantum confinement on the interplay between elementary scattering processes of the electrons at the surface and ultrafast carrier transport in the direction perpendicular to the surface is shown to be the reason for the slow electron dynamics.
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.
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.
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.
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.
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.
Subdwarf B stars are core-helium-burning stars located on the extreme horizontal branch (EHB). Extensive mass loss on the red giant branch is necessary to form them. It has been proposed that substellar companions could lead to the required mass loss when they are engulfed in the envelope of the red giant star. J08205+0008 was the first example of a hot subdwarf star with a close, substellar companion candidate to be found. Here, we perform an in-depth re-analysis of this important system with much higher quality data allowing additional analysis methods. From the higher resolution spectra obtained with ESO-VLT/XSHOOTER, we derive the chemical abundances of the hot subdwarf as well as its rotational velocity. Using the Gaia parallax and a fit to the spectral energy distribution in the secondary eclipse, tight constraints to the radius of the hot subdwarf are derived. From a long-term photometric campaign, we detected a significant period decrease of -3.2(8) x 10(-12) dd(-1). This can be explained by the non-synchronized hot subdwarf star being spun up by tidal interactions forcing it to become synchronized. From the rate of period decrease we could derive the synchronization time-scale to be 4 Myr, much smaller than the lifetime on EHB. By combining all different methods, we could constrain the hot subdwarf to a mass of 0.39-0.50 M-circle dot and a radius of R-sdB = 0.194 +/- 0.008 R-circle dot, and the companion to 0.061-0.071 M-circle dot with a radius of R-comp = 0.092 +/- 0.005 R-circle dot, below the hydrogen-burning limit. We therefore confirm that the companion is most likely a massive brown dwarf.