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1.
Nat Commun ; 14(1): 727, 2023 Feb 09.
Article in English | MEDLINE | ID: mdl-36759624

ABSTRACT

In late June 2021 a heatwave of unprecedented magnitude impacted the Pacific Northwest region of Canada and the United States. Many locations broke all-time maximum temperature records by more than 5 °C, and the Canadian national temperature record was broken by 4.6 °C, with a new record temperature of 49.6 °C. Here, we provide a comprehensive summary of this event and its impacts. Upstream diabatic heating played a key role in the magnitude of this anomaly. Weather forecasts provided advanced notice of the event, while sub-seasonal forecasts showed an increased likelihood of a heat extreme with lead times of 10-20 days. The impacts of this event were catastrophic, including hundreds of attributable deaths across the Pacific Northwest, mass-mortalities of marine life, reduced crop and fruit yields, river flooding from rapid snow and glacier melt, and a substantial increase in wildfires-the latter contributing to landslides in the months following. These impacts provide examples we can learn from and a vivid depiction of how climate change can be so devastating.

2.
Materials (Basel) ; 13(23)2020 Nov 27.
Article in English | MEDLINE | ID: mdl-33261118

ABSTRACT

Partial delignification and densification provide a pathway to significant improvement in the mechanical performance of wood. In order to elucidate potential effects of this treatment on the mechanical anisotropy of wood, partially delignified and densified spruce wood veneers were characterized at varying degrees of off-axis alignment. While the tensile strength and the modulus of elasticity (MOE) were clearly improved in parallel to the axis of wood fibers, this improvement quickly leveled off at misalignment angles ≥30°. For transverse tensile strength, the performance of alkaline-treated and densified wood was even inferior to that of untreated wood. Microscopic examination revealed the presence of microscopic cracks in treated wood, which are assumed to be responsible for this observation. It is concluded that impaired transverse tensile properties are a weakness of partially delignified and densified wood and should be considered when a potential usage in load-bearing applications is intended.

3.
Polymers (Basel) ; 12(8)2020 Aug 11.
Article in English | MEDLINE | ID: mdl-32796560

ABSTRACT

Wood and natural fibers exhibit an advantageous combination of good mechanics at comparably low density. Nevertheless, comparing absolute strength and stiffness, wood is clearly inferior to materials such as metals and engineered composites. Since there is a strong correlation between wood density and wood mechanical performance, densification by transversal compression suggests itself as a route towards improved mechanics. Partially delignified densified spruce veneers with excellent tensile properties were produced by means of an alkaline (AL) and an organosolv (OS) approach. Plywood specimens were manufactured using treated veneers glued with a phenol-resorcinol-formaldehyde adhesive and were compared with plywood samples made of native spruce veneers (Ref) and spruce veneer densified after plasticization by water impregnation (H2O). Roughly, the bending strength and the modulus of elasticity of plywood from partially delignified densified wood were improved by a factor of 2.4 and 3.5, respectively. Interlaminar shear strength did not match this improvement after partial delignification. Together with excessive thickness swelling, this might be a drawback of partially delignified densified wood in need for further research.

4.
Inorg Chem ; 58(9): 6222-6230, 2019 May 06.
Article in English | MEDLINE | ID: mdl-30986041

ABSTRACT

Cu9.1Te4Cl3 is a new polymorphic compound in the class of coinage metal polytelluride halides. Copper is highly mobile, which results in multiple order-disorder phase transitions in a limited temperature interval from 240 to 370 K. Mainly as a consequence of thermal transport properties, the compound's thermoelectric figure of merit reaches values up to ZT = 0.15 in the temperature range between room temperature and 523 K. Its structure is closely related to that of Ag10Te4Br3, another coinage metal polytelluride halide, which represents the first p-n-p-switchable semiconductor approachable by a simple temperature change. The title compound outperforms Ag10Te4Br3 in terms of thermoelectric properties by 1 order of magnitude and therefore acts as a link between the class of p-n-p compounds and thermoelectric materials.

5.
Chemistry ; 25(12): 3061-3067, 2019 Feb 26.
Article in English | MEDLINE | ID: mdl-30600843

ABSTRACT

In this work the temperature-dependent photoluminescence of alkyl-capped silicon nanocrystals with mean diameters of between 3 and 9 nm has been investigated. The nanocrystals were characterized extensively by FTIR, TEM, powder XRD, and X-ray photoelectron spectroscopy prior to low-temperature and time-resolved photoluminescence spectroscopy experiments. The photoluminescence (PL) properties were evaluated in the temperature range of 41-300 K. We found that the well-known temperature-dependent blueshift of the PL maximum decreases with increasing nanocrystal diameter and eventually becomes a redshift for nanocrystal diameters larger than 6 nm. This implies that the observed shifts cannot be explained solely by band-gap widening, as is commonly assumed. We propose that the luminescence of drop-cast silicon nanocrystals is affected by particle ensemble effects, which can explain the otherwise surprising temperature dependence of the luminescence peak.

6.
Chemphyschem ; 20(1): 134-141, 2019 01 07.
Article in English | MEDLINE | ID: mdl-30403318

ABSTRACT

In this work, we present an experimental setup for the in situ and ex situ study of the optical activity of samples, which can be prepared under ultra-high vacuum (UHV) conditions by second-harmonic generation circular dichroism (SHG-CD) over a broad spectral range. The use of a racemic mixture as a qualified reference for the anisotropy factor is described and, as an example, the chiroptical properties of 1.5 µm thick (multilayers) as well as sub-monolayer thin films of the R- and S-enantiomer of 1,1'-Bi-2-naphthol (BINOL) evaporated onto BK7 substrates were investigated.

7.
Chemphyschem ; 20(1): 62-69, 2019 01 07.
Article in English | MEDLINE | ID: mdl-30444574

ABSTRACT

We have studied the circular dichroism (CD), in the ultraviolet and visible regions, of the transparent, chiral molecule 1,1'-Bi-2-naphtol (BINOL) in 1.5 µm thick films. The initial transparent film shows an additional negative cotton effect in the CD compared to solution. With time under room temperature the film undergoes a structural phase transition. This goes hand in hand with a cotton effect at the low energy absorption band which inverts with opposite propagation direction of light through the film which is revealed as a polarity reversal of ellipticity (PRE). After completion of the phase transition the film exhibits circular differential scattering throughout the visible range which also shows PRE. The structure change was studied with Raman, microscopy under cross polarization conditions and nonlinear second-harmonic generation circular dichroism (SHG-CD). The superposition of the optical activity of individual molecules and isotropy effects makes an interpretation challenging. Yet overcoming this challenge by finding a suitable model structural information can be derived from CD measurements.

8.
Nanoscale Res Lett ; 13(1): 383, 2018 Nov 28.
Article in English | MEDLINE | ID: mdl-30488251

ABSTRACT

The luminescence dynamics in ensembles of nanocrystals are complicated by a variety of processes, including the size-dependence of the radiative and non-radiative rates in inhomogeneous broadened samples and interparticle interactions. This results in a non-exponential decay, which for the specific case of silicon nanocrystals (SiNCs) has been widely modeled with a Kohlrausch or "stretched exponential" (SE) function. We first derive the population decay function for a luminescence decay following exp[- (t/τ)ß]. We then compare the distributions and mean times calculated by assuming that either the luminescence decay or the population decay follows this function and show that the results are significantly different for ß much below 1. We then apply these two types of SE functions as well as other models to the luminescence decay data from two thermally grown SiNC samples with different mean sizes. The mean lifetimes are strongly dependent on the experimental setup and the chosen fitting model, none of which appears to adequately describe the ensemble decay dynamics. Frequency-resolved spectroscopy (FRS) techniques are then applied to SiNCs in order to extract the lifetime distribution directly. The rate distribution has a half width of ~ 0.5 decades and mainly resembles a somewhat high-frequency-skewed lognormal function. The combination of TRS and FRS methods appear best suited to uncovering the luminescence dynamics of NC materials having a broad emission spectrum.

9.
Rev Sci Instrum ; 89(9): 093303, 2018 Sep.
Article in English | MEDLINE | ID: mdl-30278695

ABSTRACT

We revise the calibration of scintillating screens commonly used to detect relativistic electron beams with low average current, e.g., from laser-plasma accelerators, based on new and expanded measurements that include higher charge density and different types of screens than previous work [Buck et al., Rev. Sci. Instrum. 81, 033301 (2010)]. Electron peak charge densities up to 10 nC/mm2 were provided by focused picosecond-long electron beams delivered by the Electron Linac for beams with high Brilliance and low Emittance (ELBE) at the Helmholtz-Zentrum Dresden-Rossendorf. At low charge densities, a linear scintillation response was found, followed by the onset of saturation in the range of nC/mm2. The absolute calibration factor (photons/sr/pC) in this linear regime was measured to be almost a factor of 2 lower than that reported by Buck et al. retrospectively implying a higher charge in the charge measurements performed with the former calibration. A good agreement was found with the results provided by Glinec et al. [Rev. Sci. Instrum. 77, 103301 (2006)]. Furthermore long-term irradiation tests with an integrated dose of approximately 50 nC/mm2 indicate a significant decrease of the scintillation efficiency over time. Finally, in order to enable the transfer of the absolute calibration between laboratories, a new constant reference light source has been developed.

10.
Phys Chem Chem Phys ; 20(31): 20347-20351, 2018 Aug 08.
Article in English | MEDLINE | ID: mdl-29971311

ABSTRACT

Water-soluble ligand protected optically active silver nanostructures were synthesised in a one-step reduction and capping process mediated by thiol-containing biomolecules. The synthesis was performed successfully with d- and l-cysteine and l-glutathione. The chiroptical properties of the obtained nanostructures were investigated by circular dichroism spectroscopy in the ultraviolet and visible wavelength range. They exhibit a g-value of up to 0.7%, which is about one order of magnitude larger compared to particles prepared by citrate reduction followed by a ligand exchange reaction. The structure and composition of the prepared materials were characterised by transmission electron microscopy, energy-dispersive X-ray and X-ray photoelectron spectroscopy. Although these structures do not have a chiral geometry, they show mirror image g-values when capped with d- and l-cysteine. This indicates that the underlying chirality transfer mechanism is based on an electric field polarisation process.


Subject(s)
Cysteine/chemistry , Glutathione/chemistry , Metal Nanoparticles/chemistry , Silver/chemistry , Circular Dichroism , Cysteine/metabolism , Electricity , Glutathione/metabolism , Ligands , Microscopy, Electron, Transmission , Photoelectron Spectroscopy , Spectrometry, X-Ray Emission , Stereoisomerism , Water/chemistry
11.
Angew Chem Int Ed Engl ; 57(3): 827-831, 2018 01 15.
Article in English | MEDLINE | ID: mdl-29178574

ABSTRACT

Εniminium ions were prepared from the corresponding α,ß-unsaturated carbonyl compounds (enones and enals), and were found to be promoted to their respective triplet states by energy transfer. The photoexcited intermediates underwent intra- or intermolecular [2+2] photocycloaddition in good yields (50-78 %) upon irradiation at λ=433 nm or λ=457 nm. Iridium or ruthenium complexes with a sufficiently high triplet energy were identified as efficient catalysts (2.5 mol % catalyst loading) for the reaction. The intermolecular [2+2] photocycloaddition of an eniminium ion derived from a chiral secondary amine proceeded with high enantioselectivity (88 % ee).

12.
BMJ Open ; 5(12): e009095, 2015 Dec 15.
Article in English | MEDLINE | ID: mdl-26671957

ABSTRACT

INTRODUCTION: Bloodstream infections are a major cause of death worldwide; blood culture (BC) sampling remains the most important tool for their diagnosis. Current data suggest that BC rates in German hospitals are considerably lower than recommended; this points to shortfalls in the application of microbiological analyses. Since early and appropriate BC diagnostics are associated with reduced case fatality rates and a shorter duration of antimicrobial therapy, a multicomponent study for the improvement of BC diagnostics was developed. METHODS AND ANALYSIS: An electronic BC registry established for the German Federal state of Thuringia is the structural basis of this study. The registry includes individual patient data (microbiological results and clinical data) and institutional information for all clinically relevant positive BCs at the participating centres. First, classic result quality indicators for bloodstream infections (eg, sepsis rates) will be studied using Poisson regression models (adjusted for institutional characteristics) in order to derive relative ranks for feedback to clinical institutions. Second, a target value will be established for the process indicator BC rate. On the basis of this target value, recommendations will be made for a given combination of institutional characteristics as a reference for future use in quality control. An interventional study aiming at the improvement of BC rates will be conducted thereafter. On the basis of the results of a survey in the participating institutions, a targeted educational intervention will be developed. The success of the educational intervention will be measured by changes in the process indicator and the result indicators over time using a pre-post design. ETHICS AND DISSEMINATION: Ethics approval was obtained from the Ethics committee of the University Hospital Jena and from the Ethics committee of the State Chamber of Physicians of Thuringia. Findings of AlertsNet will be disseminated through public media releases and publications in peer-reviewed journals. TRIAL REGISTRATION NUMBER: DRKS00004825.


Subject(s)
Bacteremia/diagnosis , Bacteremia/mortality , Blood Specimen Collection , Drug Resistance, Microbial , Research Design , Sepsis/complications , Germany , Humans , Intensive Care Units/organization & administration , Population Surveillance , Prospective Studies , Registries , Regression Analysis
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