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Using two crystals for spontaneous parametric down-conversion in a parallel setup, we observe two-photon interference with high visibility. The high visibility is consistent with complementarity and the absence of which-path information. The observations are explained as the effects of entanglement or equivalently in terms of interfering probability amplitudes and also by the calculation of a second-order field correlation function in the Heisenberg picture. The latter approach brings out explicitly the role of the vacuum fields in the down-conversion at the crystals and in the photon coincidence counting. For comparison, we show that the Hong–Ou–Mandel dip can be explained by the same approach in which the role of the vacuum signal and idler fields, as opposed to entanglement involving vacuum states, is emphasized. We discuss the fundamental limitations of a theory in which these vacuum fields are treated as classical, stochastic fields.
Using two crystals for spontaneous parametric down-conversion in a parallel setup, we observe two-photon interference with high visibility. The high visibility is consistent with complementarity and the absence of which-path information. The observations are explained as the effects of entanglement or equivalently in terms of interfering probability amplitudes and also by the calculation of a second-order field correlation function in the Heisenberg picture. The latter approach brings out explicitly the role of the vacuum fields in the down-conversion at the crystals and in the photon coincidence counting. For comparison, we show that the Hong-Ou-Mandel dip can be explained by the same approach in which the role of the vacuum signal and idler fields, as opposed to entanglement involving vacuum states, is emphasized. We discuss the fundamental limitations of a theory in which these vacuum fields are treated as classical, stochastic fields.
Photothermal conversion (PTC) nanostructures have great potential for applications in many fields, and therefore, they have attracted tremendous attention. However, the construction of a PTC nanoreactor with multi-compartment structure to achieve the combination of unique chemical properties and structural feature is still challenging due to the synthetic difficulties. Herein, we designed and synthesized a catalytically active, PTC gold (Au)@polydopamine (PDA) nanoreactor driven by infrared irradiation using assembled PS-b-P2VP nanosphere as soft template. The particles exhibit multi-compartment structure which is revealed by 3D electron tomography characterization technique. They feature permeable shells with tunable shell thickness. Full kinetics for the reduction reaction of 4-nitrophenol has been investigated using these particles as nanoreactors and compared with other reported systems. Notably, a remarkable acceleration of the catalytic reaction upon near-infrared irradiation is demonstrated, which reveals for the first time the importance of the synergistic effect of photothermal conversion and complex inner structure to the kinetics of the catalytic reduction. The ease of synthesis and fresh insights into catalysis will promote a new platform for novel nanoreactor studies.
The involvement of charge-transfer (CT) states in the photogeneration and recombination of charge carriers has been an important focus of study within the organic photovoltaic community. In this work, we investigate the molecular factors determining the mechanism of photocurrent generation in low-donor-content organic solar cells, where the active layer is composed of vacuum-deposited C-60 and small amounts of organic donor molecules. We find a pronounced decline of all photovoltaic parameters with decreasing CT state energy. Using a combination of steady-state photocurrent measurements and time-delayed collection field experiments, we demonstrate that the power conversion efficiency, and more specifically, the fill factor of these devices, is mainly determined by the bias dependence of photocurrent generation. By combining these findings with the results from ultrafast transient absorption spectroscopy, we show that blends with small CT energies perform poorly because of an increased nonradiative CT state decay rate and that this decay obeys an energy-gap law. Our work challenges the common view that a large energy offset at the heterojunction and/or the presence of fullerene clusters guarantee efficient CT dissociation and rather indicates that charge generation benefits from high CT state energies through a slower decay to the ground state.
Intermolecular charge-transfer states at the interface between electron donating (D) and accepting (A) materials are crucial for the operation of organic solar cells but can also be exploited for organic light-emitting diodes(1,2). Non-radiative charge-transfer state decay is dominant in state-of-the-art D-A-based organic solar cells and is responsible for large voltage losses and relatively low power-conversion efficiencies as well as electroluminescence external quantum yields in the 0.01-0.0001% range(3,4). In contrast, the electroluminescence external quantum yield reaches up to 16% in D-A-based organic light-emitting diodes(5-7). Here, we show that proper control of charge-transfer state properties allows simultaneous occurrence of a high photovoltaic and emission quantum yield within a single, visible-light-emitting D-A system. This leads to ultralow-emission turn-on voltages as well as significantly reduced voltage losses upon solar illumination. These results unify the description of the electro-optical properties of charge-transfer states in organic optoelectronic devices and foster the use of organic D-A blends in energy conversion applications involving visible and ultraviolet photons(8-11).
Plain Language Summary Radiation belts of the Earth, which are the zones of charged energetic particles trapped by the geomagnetic field, comprise enormous and dynamic systems. While the inner radiation belt, composed mainly of high-energy protons, is relatively stable, the outer belt, filled with energetic electrons, is highly variable and depends substantially on solar activity. Hence, extended reliable observations and the improved models of the electron intensities in the outer belt depending on solar wind parameters are necessary for prediction of their dynamics. The Cluster mission has been measuring electron flux intensities in the radiation belts since its launch in 2000, thus providing a huge dataset that can be used for radiation belts analysis. Using 16 years of electron measurements by the Cluster mission corrected for background contamination, we derived a uniform linear-logarithmic dependence of electron fluxes in the outer belt on the solar wind dynamic pressure.
Electrets are dielectrics with quasi-permanent electric charge and/or dipoles, sometimes can be regarded as an electric analogy to a magnet. Since the discovery of the excellent charge retention capacity of poly(tetrafluoro ethylene) and the invention of the electret microphone, electrets have grown out of a scientific curiosity to an important application both in science and technology. The history of electret research goes hand in hand with the quest for new materials with better capacity at charge and/or dipole retention. To be useful, electrets normally have to be charged/poled to render them electro-active. This process involves electric-charge deposition and/or electric dipole orientation within the dielectrics ` surfaces and bulk. Knowledge of the spatial distribution of electric charge and/or dipole polarization after their deposition and subsequent decay is crucial in the task to improve their stability in the dielectrics.
Likewise, for dielectrics used in electrical insulation applications, there are also needs for accumulated space-charge and polarization spatial profiling. Traditionally, space-charge accumulation and large dipole polarization within insulating dielectrics is considered undesirable and harmful to the insulating dielectrics as they might cause dielectric loss and could lead to internal electric field distortion and local field enhancement. High local electric field could trigger several aging processes and reduce the insulating dielectrics' lifetime. However, with the advent of high-voltage DC transmission and high-voltage capacitor for energy storage, these are no longer the case. There are some overlapped between the two fields of electrets and electric insulation. While quasi-permanently trapped electric-charge and/or large remanent dipole polarization are the requisites for electret operation, stably trapped electric charge in electric insulation helps reduce electric charge transport and overall reduced electric conductivity. Controlled charge trapping can help in preventing further charge injection and accumulation as well as serving as field grading purpose in insulating dielectrics whereas large dipole polarization can be utilized in energy storage applications.
In this thesis, the Piezoelectrically-generated Pressure Steps (PPSs) were employed as a nondestructive method to probe the electric-charge and dipole polarization distribution in a range of thin film (several hundred micron) polymer-based materials, namely polypropylene (PP), low-density polyethylene/magnesium oxide (LDPE/MgO) nanocomposites and poly(vinylidene fluoride-co- trifluoro ethylene) (P(VDF-TrFE)) copolymer. PP film surface-treated with phosphoric acid to introduce surfacial isolated nanostructures serves as example of 2-dimensional nano-composites whereas LDPE/MgO serves as the case of 3-dimensional nano-composites with MgO nano-particles dispersed in LDPE polymer matrix. It is evidenced that the nanoparticles on the surface of acid-treated PP and in the bulk of LDPE/MgO nanocomposites improve charge trapping capacity of the respective material and prevent further charge injection and transport and that the enhanced charge trapping capacity makes PP and LDPE/MgO nanocomposites potential materials for both electret and electrical insulation applications. As for PVDF and VDF-based copolymers, the remanent spatial polarization distribution depends critically on poling method as well as specific parameters used in the respective poling method. In this work, homogeneous polarization poling of P(VDF-TrFE) copolymers with different VDF-contents have been attempted with hysteresis cyclical poling. The behaviour of remanent polarization growth and spatial polarization distribution are reported and discussed. The Piezoelectrically-generated Pressure Steps (PPSs) method has proven as a powerful method for the charge storage and transport characterization of a wide range of polymer material from nonpolar, to polar, to polymer nanocomposites category.
Dielectric Relaxation Spectroscopy (DRS) and Thermally Stimulated Depolarization Current (TSDC) measurements were employed to study dielectric-relaxation processes, structural transitions and electric-polarization phenomena in poly(vinylidenefluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CFE)) terpolymer films. Results from DRS confirm the existence of two separate dispersion regions related to a para-to-ferroelectric phase transition and to the glass transition. The dipolar TSDC peak correlates with the loss peak of the ? relaxation that represents the glass transition. The electric polarization calculated from the dipolar TSDC peak (glass transition) shows a non-linear electric-field dependence and saturates at high electric poling fields. As the observed behaviour is essentially the same as that of the electric polarization obtained from direct polarization-versus-electric-field hysteresis measurements, TSDC experiments are also suitable for studying the polarization in relaxor-ferroelectric polymers. A saturation polarization of 44 mC m(?2) was found for an electric field of 190 MV m(?1).
In this paper, we explore the time-energy domain quantum-classical transition comparing a classical pump-probe experiment on a diatomic molecule to its quantum enhanced counterpart, where the pump and probe pulses are substituted by the signal and idler beams of a spontaneous parametric down conversion (SPDC) source. Absorption of biphotons generated with SPDC exploits quantum time-energy entanglement to enhance the overall yield and selectivity of the process, when compared with a classical pump-probe setup, while maintaining femtosecond time resolution. We systematically study the effects of correlation strength on process efficiency and selectivity, comparing the results to classical pump-probe spectra. An excitation scheme to improve the yield based on spectral narrowing of biphotons is shown. The results indicate that the quantum improvements in yield are caused by a more efficient use of the total power available for the process.
The stability of the low thermal conductivity in Fe2TiO5 pseudobrookite ceramics has been studied. An increase in thermal diffusivity is observed after only three cycles of measurement. X-ray refraction shows an increase in the mean value of specific surface after the thermal diffusivity measurements. By using scanning electron microscopy and high-angle annular dark-field scanning transmission electron microscope equipped with energy dispersive Xray spectroscopy, we observe a segregation of Ca- and F-rich nanocrystals at grain boundaries after three cycles of thermal diffusivity measurement. Therefore, impurities seem to be more efficient to scatter phonons as point defects in the pseudobrookite lattice rather than as nanocrystals at pseudobrookite grain boundaries. This emphasizes the importance of precursor purity and the influence of redistribution of impurities on thermoelectric properties: stability of micro-/nano-structures is a key point, and repeated thermoelectric measurements may allow detecting such metastable micro-/nano-structures and producing stable and reliable data.
An understanding of the factors limiting the open-circuit voltage (V-oc) and related photon energy loss mechanisms is critical to increase the power conversion efficiency (PCE) of small-molecule organic solar cells (OSCs), especially those with near-infrared (NIR) absorbers. In this work, two NIR boron dipyrromethene (BODIPY) molecules are characterized for application in planar (PHJ) and bulk (BHJ) heterojunction OSCs. When two H atoms are substituted by F atoms on the peripheral phenyl rings of the molecules, the molecular aggregation type in the thin film changes from the H-type to J-type. For PHJ devices, the nonradiative voltage loss of 0.35 V in the J-aggregated BODIPY is lower than that of 0.49 V in the H-aggregated device. In BHJ devices with a nonradiative voltage loss of 0.35 V, a PCE of 5.5% is achieved with an external quantum efficiency (EQE) maximum of 68% at 700 nm.
Aims. In this study, we analyzed a filament system, which expanded between moving magnetic features (MMFs) of a decaying sunspot and opposite flux outside of the active region from the nearby quiet-Sun network. This configuration deviated from a classical arch filament system (AFS), which typically connects two pores in an emerging flux region. Thus, we called this system an extended AFS. We contrasted classical and extended AFSs with an emphasis on the complex magnetic structure of the latter. Furthermore, we examined the physical properties of the extended AFS and described its dynamics and connectivity. Methods. The extended AFS was observed with two instruments at the Dunn Solar Telescope (DST). The Rapid Oscillations in the Solar Atmosphere (ROSA) imager provided images in three different wavelength regions, which covered the dynamics of the extended AFS at different atmospheric heights. The Interferometric Bidimensional Spectropolarimeter (IBIS) provided spectroscopic Ha data and spectropolarimetric data that was obtained in the near-infrared (NIR) Call lambda 8542 angstrom line. We derived the corresponding line-of-sight (LOS) velocities and used He II lambda 304 angstrom extreme ultraviolet (EUV) images of the Atmospheric Imaging Assembly (AIA) and LOS magnetograms of the Helioseismic and Magnetic Imager (HMI) on board the Solar Dynamics Observatory (SDO) as context data. Results. The NIR Call Stokes-V maps are not suitable to definitively define a clear polarity inversion line and to classify this chromospheric structure. Nevertheless, this unusual AFS connects the MMFs of a decaying sunspot with the network field. At the southern footpoint, we measured that the flux decreases over time. We find strong downflow velocities at the footpoints of the extended AFS, which increase in a time period of 30 min. The velocities are asymmetric at both footpoints with higher velocities at the southern footpoint. An EUV brigthening appears in one of the arch filaments, which migrates from the northern footpoint toward the southern one. This activation likely influences the increasing redshift at the southern footpoint. Conclusions. The extended AFS exhibits a similar morphology as classical AFSs, for example, threaded filaments of comparable length and width. Major differences concern the connection from MMFs around the sunspot with the flux of the neighboring quietSun network, converging footpoint motions, and longer lifetimes of individual arch filaments of about one hour, while the extended AFS is still very dynamic.
Classical Wolf-Rayet (cWR) stars are at a crucial evolutionary stage for constraining the fates of massive stars. The feedback of these hot, hydrogen-depleted stars dominates their surrounding by tremendous injections of ionizing radiation and kinetic energy. The strength of a Wolf-Rayet (WR) wind decides the eventual mass of its remnant, likely a massive black hole. However, despite their major influence and importance for gravitational wave detection statistics, WR winds are particularly poorly understood. In this paper, we introduce the first set of hydrodynamically consistent stellar atmosphere models for cWR stars of both the carbon (C) and the nitrogen (N) sequence, i.e. WC and WN stars, as a function of stellar luminosity-to-mass ratio (or Eddington Gamma) and metallicity. We demonstrate the inapplicability of the CAK wind theory for cWR stars and confirm earlier findings that their winds are launched at the (hot) iron (Fe) opacity peak. For log Z/Z(circle dot) > -2, Fe is also the main accelerator throughout the wind. Contrasting previous claims of a sharp lower mass-loss limit forWR stars, we obtain a smooth transition to optically thin winds. Furthermore, we find a strong dependence of the mass-loss rates on Eddington Gamma, both at solar and subsolar metallicity. Increases inWCcarbon and oxygen abundances turn out to slightly reduce the predicted mass-loss rates. Calculations at subsolar metallicities indicate that below the metallicity of the Small Magellanic Cloud, WR mass-loss rates decrease much faster than previously assumed, potentially allowing for high black hole masses even in the local Universe.
Context. On 27 April 2015, when comet 67P/Churyumov-Gerasimenko was at 1.76 au from the Sun and moving toward perihelion, the OSIRIS and VIRTIS-M instruments on board the Rosetta spacecraft simultaneously observed the evolving dust and gas coma during a complete rotation of the comet. Aims. We aim to characterize the spatial distribution of dust, H2O, and CO2 gas in the inner coma. To do this, we performed a quantitative analysis of the release of dust and gas and compared the observed H2O production rate with the rate we calculated using a thermophysical model. Methods. For this study we selected OSIRIS WAC images at 612 nm (dust) and VIRTIS-M image cubes at 612 nm, 2700 nm (H2O emission band), and 4200 nm (CO2 emission band). We measured the average signal in a circular annulus to study the spatial variation around the comet, and in a sector of the annulus to study temporal variation in the sunward direction with comet rotation, both at a fixed distance of 3.1 km from the comet center. Results. The spatial correlation between dust and water, both coming from the sunlit side of the comet, shows that water is the main driver of dust activity in this time period. The spatial distribution of CO2 is not correlated with water and dust. There is no strong temporal correlation between the dust brightness and water production rate as the comet rotates. The dust brightness shows a peak at 0 degrees subsolar longitude, which is not pronounced in the water production. At the same epoch, there is also a maximum in CO2 production. An excess of measured water production with respect to the value calculated using a simple thermophysical model is observed when the head lobe and regions of the southern hemisphere with strong seasonal variations are illuminated (subsolar longitude 270 degrees-50 degrees). A drastic decrease in dust production when the water production (both measured and from the model) displays a maximum occurs when typical northern consolidated regions are illuminated and the southern hemisphere regions with strong seasonal variations are instead in shadow (subsolar longitude 50 degrees-90 degrees). Possible explanations of these observations are presented and discussed.
The oceans and atmosphere interact via a multiplicity of feedback mechanisms, shaping to a large extent the global climate and its variability. To deepen our knowledge of the global climate system, characterizing and investigating this interdependence is an important task of contemporary research. However, our present understanding of the underlying large-scale processes is greatly limited due to the manifold interactions between essential climatic variables at different temporal scales. To address this problem, we here propose to extend the application of complex network techniques to capture the interdependence between global fields of sea-surface temperature (SST) and precipitation (P) at multiple temporal scales. For this purpose, we combine time-scale decomposition by means of a discrete wavelet transform with the concept of coupled climate network analysis. Our results demonstrate the potential of the proposed approach to unravel the scale-specific interdependences between atmosphere and ocean and, thus, shed light on the emerging multiscale processes inherent to the climate system, which traditionally remain undiscovered when investigating the system only at the native resolution of existing climate data sets. Moreover, we show how the relevant spatial interdependence structures between SST and P evolve across time-scales. Most notably, the strongest mutual correlations between SST and P at annual scale (8-16 months) concentrate mainly over the Pacific Ocean, while the corresponding spatial patterns progressively disappear when moving toward longer time-scales. Published under license by AIP Publishing.
A nova is a cataclysmic event on the surface of a white dwarf in a binary system that increases the overall brightness by several orders of magnitude. Although binary systems with a white dwarf are expected to be overabundant in globular clusters compared with in the Galaxy, only two novae from Galactic globular clusters have been observed. We present the discovery of an emission nebula in the Galactic globular cluster M 22 (NGC 6656) in observations made with the integral-field spectrograph MUSE. We extracted the spectrum of the nebula and used the radial velocity determined from the emission lines to confirm that the nebula is part of NGC 6656. Emission-line ratios were used to determine the electron temperature and density. It is estimated to have a mass of 1-17 x 10(-5) M-circle dot. This mass and the emission-line ratios indicate that the nebula is a nova remnant. Its position coincides with the reported location of a "guest star", an ancient Chinese term for transients, observed in May 48 BCE. With this discovery, this nova may be one of the oldest confirmed extra-solar events recorded in human history.
We report the discovery of a circular shell centred on the Be X-ray binary (BeXB) SXP 1323 in the Small Magellanic Cloud. The shell was detected in an H α image obtained with the Very Large Telescope. Follow-up spectroscopy with the Southern African Large Telescope showed that the shell expands with a velocity of ≈100kms−1 and that its emission is due to shock excitation. We suggest that this shell is a remnant of the supernova explosion that led to the formation of SXP 1323’s neutron star ≈40000 yr ago. SXP 1323 represents the second known case of a BeXB associated with a supernova remnant (the first one is SXP 1062). Interestingly, both of these BeXBs harbour long-period pulsars and are located in a low-metallicity galaxy.
For the layered transition metal dichalcogenide 1T-TaS2, we establish through a unique experimental approach and density functional theory, how ultrafast charge transfer in 1T-TaS2 takes on isotropic three-dimensional character or anisotropic two-dimensional character, depending on the commensurability of the charge density wave phases of 1T-TaS2. The X-ray spectroscopic core-hole-clock method prepares selectively in-and out-of-plane polarized sulfur 3p orbital occupation with respect to the 1T-TaS2 planes and monitors sub-femtosecond wave packet delocalization. Despite being a prototypical two-dimensional material, isotropic three-dimensional charge transfer is found in the commensurate charge density wave phase (CCDW), indicating strong coupling between layers. In contrast, anisotropic two-dimensional charge transfer occurs for the nearly commensurate phase (NCDW). In direct comparison, theory shows that interlayer interaction in the CCDW phase - not layer stacking variations - causes isotropic three-dimensional charge transfer. This is presumably a general mechanism for phase transitions and tailored properties of dichalcogenides with charge density waves.
Electroluminescence (EL) spectra of hybrid charge transfer states at metal oxide/organic type-II heterojunctions exhibit bias-induced spectral shifts. The reasons for this phenomenon have been discussed controversially and arguments for either electric field-induced effects or the filling of trap states at the oxide surface have been put forward. Here, we combine the results of EL and photovoltaic measurements to eliminate the unavoidable effect of the series resistance of inorganic and organic components on the total voltage drop across the hybrid device. For SnOx combined with the conjugated polymer [ladder type poly-(para-phenylene)], we find a one-to-one correspondence between the blue-shift of the EL peak and the increase of the quasi-Fermi level splitting at the hybrid heterojunction, which we unambiguously assign to state filling. Our data are resembled best by a model considering the combination of an exponential density of states with a doped semiconductor. Published under license by AIP Publishing.
The angular size of a star is a critical factor in determining its basic properties1. Direct measurement of stellar angular diameters is difficult: at interstellar distances stars are generally too small to resolve by any individual imaging telescope. This fundamental limitation can be overcome by studying the diffraction pattern in the shadow cast when an asteroid occults a star2, but only when the photometric uncertainty is smaller than the noise added by atmospheric scintillation3. Atmospheric Cherenkov telescopes used for particle astrophysics observations have not generally been exploited for optical astronomy due to the modest optical quality of the mirror surface. However, their large mirror area makes them well suited for such high-time-resolution precision photometry measurements4. Here we report two occultations of stars observed by the Very Energetic Radiation Imaging Telescope Array System (VERITAS)5 Cherenkov telescopes with millisecond sampling, from which we are able to provide a direct measurement of the occulted stars’ angular diameter at the ≤0.1 mas scale. This is a resolution never achieved before with optical measurements and represents an order of magnitude improvement over the equivalent lunar occultation method6. We compare the resulting stellar radius with empirically derived estimates from temperature and brightness measurements, confirming the latter can be biased for stars with ambiguous stellar classifications.