Warm dense matter at the bench-top: Fs-laser-induced confined micro-explosion
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The aim of this project is to develop a comprehensive framework that will lead to a fundamental description of both structural properties and reactions of light nuclei in terms of constituent protons and neutrons interacting through nucleon-nucleon (NN) and three-nucleon (NNN) forces. This project will provide the research community with the theoretical and computational tools that will enable: (1) an accurate prediction for fusion reactions that power stars and Earth-based fusion facilities; (2) an improved description of the spectroscopy of exotic nuclei, including light Borromean systems; and (3) a fundamental understanding of the three-nucleon force in nuclear reactions and nuclei at the drip line. To achieve this goal, we build upon a promising technique emerged recently as a candidate to reach a fundamental description of low-energy binary reactions between light ions, that is the ab initio no-core shell model combined with the resonating-group method (NCSM/RGM). This approach has demonstrated the capability to describe binary reactions below the three-body breakup threshold based, up to now, on similarity-renormalization-group (SRG) 5 evolved NN only potentials. To advance the understanding of nuclear reactions at low energies and light exotic nuclei, this project aims at extending the NCSM/RGM approach to include the full range of NNN interactions as well as the treatment of three-cluster bound and continuum states. Three-nucleon interactions are unavoidable components of a fundamental nuclear Hamiltonian obtained in a low-energy effective theory. In addition, three-nucleon force terms are induced by the SRG procedure and have to be taken into account for such a transformation to be unitary in many-body calculations. At the same time, the introduction of three-body cluster states is key to achieve a microscopic description of Borromean systems as well as three-body breakup reactions. This project will both enhance the fundamentality and enlarge the scope of our microscopic description of nuclear properties. A successful completion of this project will result in improved accuracy of the 3 He( 3 He,2p) 4 He and 3 He(α,γ) 7 Be reaction rates and consequently, in enhancement of the predictive capability of the standard solar model. In addition, we will study also the mirror reactions 3 H( 3 H,2n) 4 He and 3 H(α,γ) 7 Li (a key reaction for the production of 7 Li in the standard big-bang nucleosynthesis), and the spectroscopy of the 6 He, 6 Be, and 11 Li nuclei.
Interfacial charge transfer and core-shell structures play important roles in dye-sensitized photoelectrosynthesis cells (DSPEC) for water splitting into H 2 and O 2 . An important element in the design of the photoanode in these devices is a core/shell structure which controls local electron transfer dynamics. Here, we introduce a new element, an internal layer of Al 2 O 3 lying between the Sb:SnO 2 /TiO 2 layers in a core/shell electrode which can improve photocurrents by up to 300%. In these structures, the results of photocurrent, transient absorption, and linear scan voltammetry measurements point to an important role for the Al 2 O 3 layer in controlling internal electron transfer within the core/shell structure.
Biomass burning emissions often contain brown carbon (BrC), which represents a large family of light-absorbing organics that is chemically complex and therefore difficult to estimate their absorption of incoming solar radiation, resulting in large uncertainties in the estimation of the global direct radiative effect of aerosols. Here we investigate the contribution of BrC to the total light absorption of biomass burning aerosols over the South-East Atlantic Ocean with different optical models utilizing a suite of airborne measurements from the ORACLES 2018 campaign by introducing an effective refractive index of black carbon (BC), m eBC = n eBC +ik eBC , that accounts for all possible absorbing components at 660 nm wavelength to facilitate the attribution of absorption at shorter wavelengths. Most values of the imaginary part of the refractive index, k eBC , were larger than those commonly used for BC from biomass burning emissions, suggesting contributions from absorbers beyond BC at 660 nm. The TEM-EDX single particle analysis further suggests that these long-wavelength absorbers might include iron oxides, as iron is found to be present only when large values of k eBC are derived. Using this effective BC refractive index, we find that the contribution of BrC to the total absorption at 470 nm (R BrC,470 ) ranges from ~5–15 %, with the organic aerosol mass absorption coefficient (MAC OA,470 ) at this wavelength ranging from 0.25 ± 0.34 m 2 g -1 to 0.43 ± 0.12 m 2 g -1 . The core-shell model yielded much higher estimates of MAC OA,470 and R BrC,470 than homogeneous mixing models, underscoring the importance of model treatment. Another key finding was that estimates of the BrC contribution at 470 nm from the commonly used AAE (absorption Ångström exponent) attribution method (< 5 %) are much lower than the BrC contribution estimates (R BrC,470 ) using our new methodology that accounts for contributions from both BrC and non-carbonaceous, long-wavelength absorbers, such as magnetite. Thus, it is recommended that application of any optical properties-based attribution method use absorption coefficients at the longest possible wavelength to minimize the influence of BrC at the long wavelength and to account for potential contributions from other absorbing materials.
It is essential to determine three-dimensional parameters (e.g., radial speed, angular width, and source location) of coronal mass ejections (CMEs) for the space weather forecast. In this study, we investigate which cone type represents a halo CME morphology using 29 CMEs (12 Solar and Heliospheric Observatory (SOHO) /Large Angle and Spectrometric Coronagraph (LASCO) halo CMEs and 17 Solar Terrestrial Relations Observatory ( STEREO )/Sun–Earth Connection Coronal and Heliospheric Investigation COR2 halo CMEs) from 2010 December to 2011 June. These CMEs are identified as halo CMEs by one spacecraft ( SOHO or one of STEREO A and B ) and limb ones by the other spacecraft (One of STEREO A and B or SOHO ). From cone shape parameters of these CMEs, such as their front curvature, we find that the CME observational structures are much closer to a full ice-cream cone type than a shallow ice-cream cone type. Thus, we develop a full ice-cream cone model based on a new methodology that the full ice-cream cone consists of many flat cones with different heights and angular widths to estimate the three-dimensional parameters of the halo CMEs. This model is constructed by carrying out the following steps: (1) construct a cone for a given height and angular width, (2) project the cone onto the sky plane, (3) select points comprising the outer boundary, and (4) minimize the difference between the estimated projection speeds with the observed ones. By applying this model to 12 SOHO /LASCO halo CMEs, we find that 3D parameters from our method are similar to those from other stereoscopic methods (i.e., a triangulation method and a Graduated Cylindrical Shell model).
Ionic liquids are composed of equal quantities of positive and negative ions. In the bulk, electrical neutrality occurs in these liquids due to Coulombic ordering, in which ion shells of alternating charge form around a central ion. Their structure under confinement is far less well understood. This hinders the widespread application of ionic liquids in technological applications. Here we use scattering experiments to resolve the structure of a widely used ionic liquid (EMI–TFSI) when it is confined inside nanoporous carbons. We show that Coulombic ordering reduces when the pores can accommodate only a single layer of ions. Instead, equally charged ion pairs are formed due to the induction of an electric potential of opposite sign in the carbon pore walls. This non-Coulombic ordering is further enhanced in the presence of an applied external electric potential. Furthermore, this finding opens the door for the design of better materials for electrochemical applications.
Using the Van Allen Probe in situ measured magnetic field and electron data, we examine the solar wind dynamic pressure and interplanetary magnetic field (IMF) effects on global magnetic field and outer radiation belt relativistic electrons (≥1.8 MeV). The dynamic pressure enhancements (>2 nPa) cause the dayside magnetic field increase and the nightside magnetic field reduction, whereas the large southward IMFs (B z-IMF < –2nT) mainly lead to the decrease of the nightside magnetic field. In the dayside increased magnetic field region (magnetic local time (MLT) ~ 06:00–18:00, and L > 4), the pitch angles of relativistic electrons are mainly pancake distributions with a flux peak around 90° (corresponding anisotropic index A > 0.1), and the higher-energy electrons have stronger pancake distributions (the larger A), suggesting that the compression-induced betatron accelerations enhance the dayside pancake distributions. However, in the nighttime decreased magnetic field region (MLT ~ 18:00–06:00, and L ≥ 5), the pitch angles of relativistic electrons become butterfly distributions with two flux peaks around 45° and 135° (A < 0). The spatial range of the nighttime butterfly distributions is almost independent of the relativistic electron energy, but it depends on the magnetic field day-night asymmetry and the interplanetary conditions. The dynamic pressure enhancements can make the nighttime butterfly distribution extend inward. The large southward IMFs can also lead to the azimuthal expansion of the nighttime butterfly distributions. As a result, these variations are consistent with the drift shell splitting and/or magnetopause shadowing effect.
Fast reverse shocks (FRSs) cause the magnetosphere to expand, by contrast to the well-known compressions caused by the impact of fast forward shocks (FFS). Usually, FFSs are more geoeffective than FRSs, and consequently the inner magnetosphere dynamic responses to both shock types can be quite different. In this study, we investigate for the first time the radiation belt response to an FRS impact using multi-satellite observations and numerical simulations. Spacecraft on the dayside observed decreases in magnetic field strength and energetic (~40–475 keV) particle fluxes. Timing analysis shows that the magnetic field signature propagated from the dayside to the nightside magnetosphere. Particles with different energies vary simultaneously at each spacecraft, implying a non-dispersive particle response to the shock. Spacecraft located at lower L-shells did not record any significant signatures. The observations indicate a local time dependence of the response associated with the shock inclination, with the clearest signatures being observed in the dusk–midnight sector. Simulations underestimate the amplitude of the magnetic field variations observed on the nightside. The observed decreases in the electron intensities result from a combination of radial gradient and adiabatic effects. The radial gradients in the spectral index appear to be the dominant contributor to the observed variations of electrons seen on the dayside (near noon and dusk) and on the nightside (near midnight). This work shows that even an FRS can affect the radiation belts significantly and provides an opportunity to understand their dynamic response to a sudden expansion of the magnetosphere.
The first-peak s-process elements Rb, Sr, Y and Zr in the post-AGB star Sakurai's object (V4334 Sagittarii) have been proposed to be the result of i-process nucleosynthesis in a post-AGB very-late thermal pulse event. We estimate the nuclear physics uncertainties in the i-process model predictions to determine whether the remaining discrepancies with observations are significant and point to potential issues with the underlying astrophysical model. We find that the dominant source in the nuclear physics uncertainties are predictions of neutron capture rates on unstable neutron rich nuclei, which can have uncertainties of more than a factor 20 in the band of the i-process. We use a Monte Carlo variation of 52 neutron capture rates and a 1D multi-zone post-processing model for the i-process in Sakurai's object to determine the cumulative effect of these uncertainties on the final elemental abundance predictions. We find that the nuclear physics uncertainties are large and comparable to observational errors. Within these uncertainties the model predictions are consistent with observations. A correlation analysis of the results of our MC simulations reveals that the strongest impact on the predicted abundances of Rb, Sr, Y and Zr is made by the uncertainties in the (n, γ) reaction rates of 85 Br, 86 Br, 87 Kr, 88 Kr, 89 Kr, 89 Rb, 89 Sr, and 92 Sr. This conclusion is supported by a series of multi-zone simulations in which we increased and decreased to their maximum and minimum limits one or two reaction rates per run. We also show that simple and fast one-zone simulations should not be used instead of more realistic multi-zone stellar simulations for nuclear sensitivity and uncertainty studies of convective–reactive processes. Lastly, our findings apply more generally to any i-process site with similar neutron exposure, such as rapidly accreting white dwarfs with near-solar metallicities.
The piezo-phototronic effect is about the use of the piezoelectric potential created inside some materials for enhancing the charge carrier generation or separation at the metal-semiconductor contact or p-n junction. We demonstrate the impact of the piezo-phototronic effect on the photon sensitivity for a ZnO-CdS core-shell micro/nanowire based visible and UVsensor. CdS nanowire arrays were grown on the surface of a ZnO micro/nanowire to form a ZnO-CdS core-shell nanostructure by a facile hydrothermal method. With the two ends of a ZnO-CdS wire bonded on a polymer substrate, a flexible photodetector was fabricated, which is sensitive simultaneously to both green light (548 nm) and UV light (372 nm). The photocurrent and sensitivity of the ZnO_CdS wire photodetector is 103 times higher than that of CdS nanoribbon, and the responsivity (11 A W -1 , 548 nm, at 2 V bias) is nearly 100 times higher than that of ZnSe-nanobelt-based blue/UV-light sensor (0.12 AW -1 , 400 nm, at 30 V bias). Moreover, the performance of the ZnO-CdS wire photodetector upon illumination of visible and UV light can be both further enhanced for more than 10 times with the participation of the piezo-phototronic effect when the device is subjected to a -0.31% compressive strain. This investigation extends the application of the piezo-phototronic effect in a wide spectrum photon detector.
A mesoporous atomic layer deposition (ALD) double-shell electrode, Al 2 O 3 (insulating core)//ALD ZnO|ALD TiO 2 , on a fluorine-doped tin oxide (FTO) conducting substrate was explored for a photoanode assembly, FTO//Al 2 O 3 (insulating core)//ALD ZnO|ALD TiO 2 |–chromophore–catalyst, for light-driven water oxidation. Photocurrent densities at photoanodes based on mesoporous ALD double-shell (ALD ZnO|ALD TiO 2 |) and ALD single-shell (ALD ZnO|, ALD TiO 2 |) electrodes were investigated for O 2 evaluation by a generator–collector dual working electrode configuration. The high photocurrent densities obtained based on the mesoporous ALD ZnO|ALD TiO 2 photoanode for O 2 evolution arise from a significant barrier to back electron transfer (BET) by the optimized tunneling barrier in the structure with the built-in electric field at the ALD ZnO|ALD TiO 2 interface. The charge recombination is thus largely decreased. Finally, in the films, BET following injection has been investigated through kinetic nanosecond transient absorption spectra, and the results of energy band analysis are used to derive insight into the internal electronic structure of the electrodes.
Artificial photosynthesis is an attractive approach for renewable fuel generation because it offers the prospect of a technology suitable for deployment on highly abundant, non-arable land. Recent leaps forward in the development of efficient and durable light absorbers and catalysts for oxygen evolution and the growing attention to catalysts for carbon dioxide activation brings into focus the tasks of hierarchically integrating the components into assemblies for closing of the photosynthetic cycle. A particular challenge is the efficient coupling of the multi-electron processes of CO 2 reduction and H 2 O oxidation. Among the most important requirements for a complete integrated system are catalytic rates that match the solar flux, efficient charge transport between the various components, and scalability of the photosynthetic assembly on the unprecedented scale of terawatts in order to have impact on fuel consumption. To address these challenges, we have developed in this paper a heterogeneous inorganic materials approach with molecularly precise control of light absorption and charge transport pathways. Oxo-bridged heterobinuclear units with metal-to-metal charge-transfer transitions absorbing deep in the visible act as single photon, single charge transfer pumps for driving multi-electron catalysts. A photodeposition method has been introduced for the spatially directed assembly of nanoparticle catalysts for selective coupling to the donor or acceptor metal of the light absorber. For CO 2 reduction, a Cu oxide cluster is coupled to the Zr center of a ZrOCo light absorber, while coupling of an Ir nanoparticle catalyst for water oxidation to the Co donor affords closing of the photosynthetic cycle of CO 2 conversion by H 2 O to CO and O 2 . Optical, vibrational, and X-ray spectroscopy provide detailed structural knowledge of the polynuclear assemblies. Time resolved visible and rapid-scan FT-IR studies reveal charge transfer mechanisms and transient surface intermediates under photocatalytic conditions for guiding performance improvements. Separation of the water oxidation and carbon dioxide reduction half reactions by a membrane is essential for efficient photoreduction of CO 2 by H 2 O to liquid fuel products. A concept of a macroscale artificial photosystem consisting of arrays of Co oxide–silica core–shell nanotubes is introduced in which each tube operates as a complete, independent photosynthetic unit with built-in membrane separation. The ultrathin amorphous silica shell with embedded molecular wires functions as a proton conducting, molecule impermeable membrane. Photoelectrochemical and transient optical measurements confirm tight control of charge transport through the membrane by the orbital energetics of the wire molecules. Finally, hierarchical arrangement of the components is accomplished by a combination of photodeposition, controlled anchoring, and atomic layer deposition methods.
The nuclear rates for reactions involving 12 C and 16 O are key to computing the energy release and nucleosynthesis evolution of massive stars during their advanced burning phases. Ultimately, these burning rates shape the stellar structure and evolution and influence the nature of the compact objects produced at the end of the stellar life. We explore the implications of new nuclear reaction rates from both experimental and theoretical studies for 12 C(α, γ) 16 O, 12 C+ 12 C, 12 C+ 16 O, and 16 O+ 16 O reactions for massive stars. Our goal is to investigate how the chemical structure and nucleosynthesis evolve from the He-exhaustion stage to the O-burning phase and how these processes influence the ultimate stellar fate. We computed rotating and non-rotating models for stars of different masses at solar metallicity. We used the stellar evolution code GENEC, which includes a large network of nuclear reactions and isotopes involved in advanced phases, as well as updated rates for 12 C(α,γ) 16 O. For the three fusion reactions involving 12 C and 16 O, we considered new rates following a data-driven fusion suppression scenario (hereafter HIN(RES)) and new theoretical rates obtained with time-dependent Hartree-Fock (TDHF) calculations. The updated 12 C(α, γ) 16 O rates mainly impact the chemical structure evolution changing the 12 C/ 16 O ratio at He-exhaustion and have little effect on the CO core mass. This variation in the 12 C/ 16 O ratio is in some cases critical for predicting the final fate of the model, which is very sensitive to 12 C abundance, and in particular the 20 M ⊙ remnant may change from a black hole to a neutron star. The He-burning (C-burning) lifetime is also decreased (increased) by about −2% (+15%). The combined new rates for 12 C+ 12 C and 16 O+ 16 O fusion reactions according to the HIN(RES) model lead to shorter C- and O-burning lifetimes by ≈ − 10%, and −50%, respectively, and shift the ignition conditions to higher temperatures and densities. In contrast, the theoretical TDHF rates primarily affect C-burning, increasing its duration by about 30% and lowering the ignition temperature. These changes modify the chemical structure of the core, the size and duration of C-burning shells, and hence their compactness. They also impact the central and shell nucleosynthesis (by ±1 dex and by factors of ±2–10, respectively), while 12 C+ 16 O reaction rates variations remain the least important.
Hybrid interfaces combining inorganic and organic materials underpin the operation of many optoelectronic and photocatalytic systems and allow for innovative approaches to photon up- and down-conversion. However, the mechanism of exchange-mediated energy transfer of spin-triplet excitons across these interfaces remains obscure, particularly when both the macroscopic donor and acceptor are composed of many separately interacting nanoscopic moieties. Here, we study the transfer of excitons from colloidal lead sulfide (PbS) nanocrystals to the spin-triplet state of rubrene molecules. By reducing the length of the carboxylic acid ligands on the nanocrystal surface from 18 to 4 carbon atoms, thinning the effective ligand shell from 13 to 6 Å, we are able to increase the characteristic transfer rate by an order of magnitude. However, we observe that the energy transfer rate asymptotes for shorter separation distances (≤10 Å) which we attribute to the reduced Dexter coupling brought on by the increased effective dielectric constant of these solid-state devices when the aliphatic ligands are short. This implies that the shortest ligands, which hinder long-term colloidal stability, offer little advantage for energy transfer. Indeed, we find that hexanoic acid ligands are already sufficient for near-unity transfer efficiency. Using nanocrystals with these optimal-length ligands in an improved solid-state device structure, we obtain an upconversion efficiency of (7 ± 1)% with excitation at λ = 808 nm.
Photoionization fronts play a dominant role in many astrophysical situations but remain difficult to achieve in a laboratory experiment. We present the results from a computational parameter study evaluating the feasibility of the photoionization experiment presented in the design paper by Drake et al. in which a photoionization front is generated in a nitrogen medium. The nitrogen gas density and the Planckian radiation temperature of the X-ray source define each simulation. Simulations modeled experiments in which the X-ray flux is generated by a laser-heated gold foil, suitable for experiments using many kJ of laser energy, and experiments in which the flux is generated by a "z-pinch" device, which implodes a cylindrical shell of conducting wires. The models are run using crash, our block-adaptive-mesh code for multimaterial radiation hydrodynamics. The radiative transfer model uses multigroup, flux-limited diffusion with 30 radiation groups. In addition, electron heat conduction is modeled using a single-group, flux-limited diffusion. In the theory, a photoionization front can exist only when the ratios of the electron recombination rate to the photoionization rate and the electron-impact ionization rate to the recombination rate lie in certain ranges. These ratios are computed for several ionization states of nitrogen. Photoionization fronts are found to exist for laser-driven models with moderate nitrogen densities (~10 21 cm –3 ) and radiation temperatures above 90 eV. For "z-pinch"-driven models, lower nitrogen densities are preferred (<10 21 cm –3 ). Here, we conclude that the proposed experiments are likely to generate photoionization fronts.
We present an overview of the initial results from the Chandra Planetary Nebula Survey (CHANPLANS), the first systematic (volume-limited) Chandra X-Ray Observatory survey of planetary nebulae (PNe) in the solar neighborhood. The first phase of CHANPLANS targeted 21 mostly high-excitation PNe within {approx}1.5 kpc of Earth, yielding four detections of diffuse X-ray emission and nine detections of X-ray-luminous point sources at the central stars (CSPNe) of these objects. Combining these results with those obtained from Chandra archival data for all (14) other PNe within {approx}1.5 kpc that have been observed to date, we find an overall X-ray detection rate of {approx}70% for the 35 sample objects. Roughly 50% of the PNe observed by Chandra harbor X-ray-luminous CSPNe, while soft, diffuse X-ray emission tracing shocks-in most cases, 'hot bubbles'-formed by energetic wind collisions is detected in {approx}30%; five objects display both diffuse and point-like emission components. The presence (or absence) of X-ray sources appears correlated with PN density structure, in that molecule-poor, elliptical nebulae are more likely to display X-ray emission (either point-like or diffuse) than molecule-rich, bipolar, or Ring-like nebulae. All but one of the point-like CSPNe X-ray sources display X-ray spectra that are harder than expected from hot ({approx}100 kK) central stars emitting as simple blackbodies; the lone apparent exception is the central star of the Dumbbell nebula, NGC 6853. These hard X-ray excesses may suggest a high frequency of binary companions to CSPNe. Other potential explanations include self-shocking winds or PN mass fallback. Most PNe detected as diffuse X-ray sources are elliptical nebulae that display a nested shell/halo structure and bright ansae; the diffuse X-ray emission regions are confined within inner, sharp-rimmed shells. All sample PNe that display diffuse X-ray emission have inner shell dynamical ages {approx}< 5 Multiplication-Sign 10{sup 3} yr, placing firm constraints on the timescale for strong shocks due to wind interactions in PNe. The high-energy emission arising in such wind shocks may contribute to the high excitation states of certain archetypical 'hot bubble' nebulae (e.g., NGC 2392, 3242, 6826, and 7009).
The structures in amorphous (a-) Zn, Sn co-doped In 2 O 3 (ZITO) thin films grown by pulsed laser deposition on glass under varying oxygen pressure or with varying Sn:Zn ratios were determined using X-ray absorption spectroscopy and anomalous X-ray scattering. Typical structures around cations in a-ZITO films are described and compared with crystalline (c-) ZITO films. The results show that the Zn cations are fourfold coordinated with Zn–O bond lengths of 1.98 ± 0.02 Å, which is close to that in bulk ZnO. As a consequence, the second coordination shells around Zn contract. At longer distances away from Zn, the structure is commensurate with the averaged structure. The unit volume around In also contracts slightly compared to bulk In 2 O 3 , whereas the Sn–O bond length is similar to the one in bulk SnO 2 . These unique structural characteristics may account for the films' superior thermal stability over amorphous Sn-doped In 2 O 3 , and suggest that Zn and Sn act as network-forming cations. Like in c-ZITO, coordination numbers (N) around Sn, In, and Zn follow the order N Sn > N In > N Zn . Unlike in c-ZITO, where electrical properties change significantly with a slight variation in the Sn:Zn ratio, this variation does not markedly alter the electrical properties, or the local structures, of a-ZITO films. Dramatic changes in the electrical properties occur for films grown under various oxygen pressures, which point to oxygen “defects” as the source of charge carriers.