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Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
(2022)
Mayer, Dennis ; Lever, Fabiano ; Picconi, David ; Metje, Jan ; Ališauskas, Skirmantas ; Calegari, Francesca ; Düsterer, Stefan ; Ehlert, Christopher ; Feifel, Raimund ; Niebuhr, Mario ; Manschwetus, Bastian ; Kuhlmann, Marion ; Mazza, Tommaso ; Robinson, Matthew Scott ; Squibb, Richard J. ; Trabattoni, Andrea ; Wallner, Måns ; Saalfrank, Peter ; Wolf, Thomas J. A. ; Gühr, Markus
Imaging the charge flow in photoexcited molecules would provide key information on photophysical and photochemical processes. Here the authors demonstrate tracking in real time after photoexcitation the change in charge density at a specific site of 2-thiouracil using time-resolved X-ray photoelectron spectroscopy. The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using time-resolved x-ray photoelectron spectroscopy (TR-XPS). We extend the concept of static chemical shift from conventional XPS by the excited-state chemical shift (ESCS), which is connected to the charge in the framework of a potential model. This allows us to invert TR-XPS spectra to the dynamic charge at a specific atom. We demonstrate the power of TR-XPS by using sulphur 2p-core-electron-emission probing to study the UV-excited dynamics of 2-thiouracil. The method allows us to discover that a major part of the population relaxes to the molecular ground state within 220-250 fs. In addition, a 250-fs oscillation, visible in the kinetic energy of the TR-XPS, reveals a coherent exchange of population among electronic states.
Busse, David ; Simon, Philipp ; Petroff, David ; El-Najjar, Nahed ; Schmitt, Lisa ; Bindellini, Davide ; Dietrich, Arne ; Zeitlinger, Markus ; Huisinga, Wilhelm ; Michelet, Robin ; Wrigge, Hermann ; Kloft, Charlotte
The objectives of this study were the identification in (morbidly) obese and nonobese patients of (i) the most appropriate body size descriptor for fosfomycin dose adjustments and (ii) adequacy of the currently employed dosing regimens. Plasma and target site (interstitial fluid of subcutaneous adipose tissue) concentrations after fosfomycin administration (8 g) to 30 surgery patients (15 obese/15 nonobese) were obtained from a prospective clinical trial. After characterization of plasma and microdialysis-derived target site pharmacokinetics via population analysis, short-term infusions of fosfomycin 3 to 4 times daily were simulated. The adequacy of therapy was assessed by probability of pharmacokinetic/pharmacodynamic target attainment (PTA) analysis based on the unbound drug-related targets of an %fT(>= MIC) (the fraction of time that unbound fosfomycin concentrations exceed the MIC during 24 h) of 70 and an fAUC(0-24h)/MIC (the area under the concentration-time curve from 0 to 24 h for the unbound fraction of fosfomycin relative to the MIC) of 40.8 to 83.3. Lean body weight, fat mass, and creatinine clearance calculated via adjusted body weight (ABW) (CLCRCG_ABW) of all patients (body mass index [BMI] = 20.1 to 52.0 kg/m(2)) explained a considerable proportion of between-patient pharmacokinetic variability (up to 31.0% relative reduction). The steady-state unbound target site/plasma concentration ratio was 26.3% lower in (morbidly) obese than nonobese patients. For infections with fosfomycin-susceptible pathogens (MIC <= 16 mg/L), intermittent "high-dosage" intravenous (i.v.) fosfomycin (8 g, three times daily) was sufficient to treat patients with a CLCRCG_ABW of,130 mL/min, irrespective of the pharmacokinetic/pharmacodynamic indices considered. For infections by Pseudomonas aeruginosa with a MIC of 32 mg/L, when the index fAUC0-24h/MIC is applied, fosfomycin might represent a promising treatment option in obese and nonobese patients, especially in combination therapy to complement beta-lactams, in which carbapenem-resistant P. aeruginosa is critical. In conclusion, fosfomycin showed excellent target site penetration in obese and nonobese patients. Dosing should be guided by renal function rather than obesity status.
Tian, Fang ; Qin, Wen ; Zhang, Ran ; Herzschuh, Ulrike ; Ni, Jian ; Zhang, Chengjun ; Mischke, Steffen ; Cao, Xianyong
The terrestrial ecosystem in the Yellow River Source Area (YRSA) is sensitive to climate change and human impacts, although past vegetation change and the degree of human disturbance are still largely unknown. A 170-cm-long sediment core covering the last 7,400 years was collected from Lake Xingxinghai (XXH) in the YRSA. Pollen, together with a series of other environmental proxies (including grain size, total organic carbon (TOC) and carbonate content), were analysed to explore past vegetation and environmental changes for the YRSA. Dominant and common pollen components-Cyperaceae, Poaceae, Artemisia, Chenopodiaceae and Asteraceae-are stable throughout the last 7,400 years. Slight vegetation change is inferred from an increasing trend of Cyperaceae and decreasing trend of Poaceae, suggesting that alpine steppe was replaced by alpine meadow at ca. 3.5 ka cal bp. The vegetation transformation indicates a generally wetter climate during the middle and late Holocene, which is supported by increased amounts of TOC and Pediastrum (representing high water-level) and is consistent with previous past climate records from the north-eastern Tibetan Plateau. Our results find no evidence of human impact on the regional vegetation surrounding XXH, hence we conclude the vegetation change likely reflects the regional climate signal.
Vatova, Mariyana ; Rubin, Conrad ; Grossart, Hans-Peter ; Goncalves, Susana C. ; Schmidt, Susanne I. ; Jarić, Ivan
Glückler, Ramesh ; Geng, Rongwei ; Grimm, Lennart ; Baisheva, Izabella ; Herzschuh, Ulrike ; Stoof-Leichsenring, Kathleen R. ; Kruse, Stefan ; Andreev, Andrej Aleksandrovic ; Pestryakova, Luidmila ; Dietze, Elisabeth
Wildfires play an essential role in the ecology of boreal forests.
In eastern Siberia, fire activity has been increasing in recent years, challenging the livelihoods of local communities. Intensifying fire regimes also increase disturbance pressure on the boreal forests, which currently protect the permafrost beneath from accelerated degradation.
However, long-term relationships between changes in fire regime and forest structure remain largely unknown.
We assess past fire-vegetation feedbacks using sedimentary proxy records from Lake Satagay, Central Yakutia, Siberia, covering the past c. 10,800 years.
Results from macroscopic and microscopic charcoal analyses indicate high amounts of burnt biomass during the Early Holocene, and that the present-day, low-severity surface fire regime has been in place since c. 4,500 years before present.
A pollen-based quantitative reconstruction of vegetation cover and a terrestrial plant record based on sedimentary ancient DNA metabarcoding suggest a pronounced shift in forest structure toward the Late Holocene.
Whereas the Early Holocene was characterized by postglacial open larch-birch woodlands, forest structure changed toward the modern, mixed larch-dominated closed-canopy forest during the Mid-Holocene.
We propose a potential relationship between open woodlands and high amounts of burnt biomass, as well as a mediating effect of dense larch forest on the climate-driven intensification of fire regimes.
Considering the anticipated increase in forest disturbances (droughts, insect invasions, and wildfires), higher tree mortality may force the modern state of the forest to shift toward an open woodland state comparable to the Early Holocene.
Such a shift in forest structure may result in a positive feedback on currently intensifying wildfires.
These new long-term data improve our understanding of millennial-scale fire regime changes and their relationships to changes of vegetation in Central Yakutia, where the local population is already being confronted with intensifying wildfire seasons.
Wright, Michelle F. ; Wachs, Sebastian ; Huang, Zheng ; Kamble, Shanmukh V. ; Soudi, Shruti ; Bayraktar, Fatih ; Li, Zheng ; Lei, Li ; Shu, Chang
Drawing on the social-ecological perspective, this longitudinal study investigated the potential moderating effect of gender in the relationships among Machiavellianism, popularity goals, and cyberbullying involvement (i.e. victimization, perpetration) among adolescents from China, Cyprus, India, and the United States.
There were 2,452 adolescents (M-age = 14.85; SD = .53; 13-16 years old; 49.1% girls) from China, Cyprus, India, and the United States included in this study.
They completed surveys on Machiavellianism, popularity goals, and cyberbullying victimization and perpetration during the fall of 2014 (Time 1). One year later, during the fall of 2015, adolescents completed surveys on cyberbullying victimization and perpetration.
Findings revealed that Machiavellianism and popularity goals were both associated positively with Time 2 cyberbullying victimization and perpetration for all adolescents. The associations between Machiavellianism and Time 2 cyberbullying perpetration and between popularity goals and Time 2 cyberbullying perpetration were stronger for Chinese and Indian boys than girls.
Opposite patterns were found for popularity goals and Time 2 cyberbullying perpetration for adolescents from the United States.
Gender did not moderate any of the associations for Cypriot adolescents or for Time 2 cyberbullying victimization.
The social-ecological perspective provides a useful understanding of how various contexts influence bullying.
Liu, Ji-Cai ; Ignatova, Nina ; Kimberg, Victor ; Krasnov, Pavel ; Föhlisch, Alexander ; Simon, Marc ; Gel'mukhanov, Faris
Modern stationary X-ray spectroscopy is unable to resolve rotational structure.
In the present paper, we propose to use time-resolved two color X-ray pump-probe spectroscopy with picosecond resolution for real-time monitoring of the rotational dynamics induced by the recoil effect.
The proposed technique consists of two steps.
The first short pump X-ray pulse ionizes the valence electron, which transfers angular momentum to the molecule.
The second time-delayed short probe X-ray pulse resonantly excites a 1s electron to the created valence hole.
Due to the recoil-induced angular momentum the molecule rotates and changes the orientation of transition dipole moment of core-excitation with respect to the transition dipole moment of the valence ionization, which results in a temporal modulation of the probe X-ray absorption as a function of the delay time between the pulses.
We developed an accurate theory of the X-ray pump-probe spectroscopy of the recoil-induced rotation and study how the energy of the photoelectron and thermal dephasing affect the structure of the time-dependent X-ray absorption using the CO molecule as a case-study.
We also discuss the feasibility of experimental observation of our theoretical findings, opening new perspectives in studies of molecular rotational dynamics.
Abiuso, Paolo ; Holubec, Viktor ; Anders, Janet ; Ye, Zhuolin ; Cerisola, Federico ; Perarnau-Llobet, Marti
We characterize finite-time thermodynamic processes of multidimensional quadratic overdamped systems.
Analytic expressions are provided for heat, work, and dissipation for any evolution of the system covariance matrix.
The Bures-Wasserstein metric between covariance matrices naturally emerges as the local quantifier of dissipation.
General principles of how to apply these geometric tools to identify optimal protocols are discussed.
Focusing on the relevant slow-driving limit, we show how these results can be used to analyze cases in which the experimental control over the system is partial.
Welke, Robert-William ; Sperber, Hannah Sabeth ; Bergmann, Ronny ; Koikkarah, Amit ; Menke, Laura ; Sieben, Christian ; Krüger, Detlev H. ; Chiantia, Salvatore ; Herrmann, Andreas ; Schwarzer, Roland
Hantaviruses are enveloped viruses that possess a tri-segmented, negative-sense RNA genome.
The viral S-segment encodes the multifunctional nucleocapsid protein (N), which is involved in genome packaging, intracellular protein transport, immunoregulation, and several other crucial processes during hantavirus infection.
In this study, we generated fluorescently tagged N protein constructs derived from Puumalavirus (PUUV), the dominant hantavirus species in Central, Northern, and Eastern Europe.
We comprehensively characterized this protein in the rodent cell line CHO-K1, monitoring the dynamics of N protein complex formation and investigating co-localization with host proteins as well as the viral glycoproteins Gc and Gn.
We observed formation of large, fibrillar PUUV N protein aggregates, rapidly coalescing from early punctate and spike-like assemblies.
Moreover, we found significant spatial correlation of N with vimentin, actin, and P-bodies but not with microtubules. N constructs also co-localized with Gn and Gc albeit not as strongly as the glycoproteins associated with each other.
Finally, we assessed oligomerization of N constructs, observing efficient and concentration-dependent multimerization, with complexes comprising more than 10 individual proteins.
In Krisenzeiten ist der Ruf nach Führung besonders populär. Dabei ist gerade Führung selbst eines der unsichersten Mittel, die der Organisation zur Verfügung stehen. Hingegen wird das Potenzial von Strukturen zu wenig gesehen. Wenn in unsicheren Situationen der Wunsch nach Orientierung und Klarheit groß ist, können häufig strukturelle Entscheidungen die notwendigen Sicherheiten vermitteln.