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A surface photovoltage (SPV) is observed whenever a doped semiconductor with non-negligible band bending is illuminated by light and charge carriers are excited across the band gap. The sign of the SPV depends on the nature of the doping, the amplitude of the SPV increases with the fluence of the light illumination up to a saturation value, which is determined by the doping concentration. We have investigated Si(100) samples with well-characterized doping levels over a wide range of illumination fluences. Surprisingly, the sign of the SPV upon illumination with 532 nm photons reverses for some p-doping concentrations at high fluences. This is a new effect associated with a crossover between electronic excitations in the bulk and at the surface of the semiconductor.

A prerequisite for advancing hybrid solar light harvesting systems is a comprehensive understanding of the spatiotemporal dynamics of photoinduced interfacial charge separation. Here, we demonstrate access to this transient charge redistribution for a model hybrid system of nanoporous zinc oxide (ZnO) and ruthenium bipyridyl chromophores. The site-selective probing of the molecular electron donor and semiconductor acceptor by time-resolved X-ray photoemission provides direct insight into the depth distribution of the photoinjected electrons and their interaction with the local band structure on a nanometer length scale. Our results show that these electrons remain localized within less than 6 nm from the interface, due to enhanced downward band bending by the photoinjected charge carriers. This spatial confinement suggests that light-induced charge generation and transport in nanoscale ZnO photocatalytic devices proceeds predominantly within the defect-rich surface region, which may lead to enhanced surface recombination and explain their lower performance compared to titanium dioxide (TiO2)-based systems.

Zinc oxide (ZnO) nanomaterials are promising components for chemical and biological sensors and photocatalytic conversion and operate as electron collectors in photovoltaic technologies. Many of these applications involve nanostructures in contact with liquids or exposed to ambient atmosphere. Under these conditions, single-crystal ZnO surfaces are known to form narrow electron accumulation layers with few nanometer spatial penetration into the bulk. A key question is to what extent such pronounced surface potential gradients can develop in the nanophases of ZnO, where they would dominate the catalytic activity by modulating charge-carrier mobility and lifetimes. Here, we follow the temperature-dependent surface electronic structure of nanoporous ZnO with photoemission spectroscopy to reveal a sizable, spatially averaged downward band bending for the hydroxylated state and a conservative upper bound of

We present a novel technique to monitor dynamics in interfacial systems through temporal correlations in x-ray photoelectron spectroscopy (XPS) signals. To date, the vast majority of time-resolved x-ray spectroscopy techniques rely on pump-probe schemes, in which the sample is excited out of equilibrium by a pump pulse, and the subsequent dynamics are monitored by probe pulses arriving at a series of well-defined delays relative to the excitation. By definition, this approach is restricted to processes that can either directly or indirectly be initiated by light. It cannot access spontaneous dynamics or the microscopic fluctuations of ensembles in chemical or thermal equilibrium. Enabling this capability requires measurements to be performed in real (laboratory) time with high temporal resolution and, ultimately, without the need for a well-defined trigger event. The time-correlation XPS technique presented here is a first step toward this goal. The correlation-based technique is implemented by extending an existing optical-laser pump/multiple x-ray probe setup by the capability to record the kinetic energy and absolute time of arrival of every detected photoelectron. The method is benchmarked by monitoring energy-dependent, periodic signal modulations in a prototypical time-resolved XPS experiment on photoinduced surface-photovoltage dynamics in silicon, using both conventional pump-probe data acquisition, and the new technique based on laboratory time. The two measurements lead to the same result. The findings provide a critical milestone toward the overarching goal of studying equilibrium dynamics at surfaces and interfaces through time correlation-based XPS measurements.

The ultrafast dynamics of photon-to-charge conversion in an organic light-harvesting system is studied by femtosecond time-resolved X-ray photoemission spectroscopy (TR-XPS) at the free-electron laser FLASH. This novel experimental technique provides site-specific information about charge separation and enables the monitoring of free charge carrier generation dynamics on their natural timescale, here applied to the model donor-acceptor system CuPc:C60. A previously unobserved channel for exciton dissociation into mobile charge carriers is identified, providing the first direct, real-time characterization of the timescale and efficiency of charge generation from low-energy charge-transfer states in an organic heterojunction. The findings give strong support to the emerging realization that charge separation even from energetically disfavored excitonic states is contributing significantly, indicating new options for light harvesting in organic heterojunctions.

Possibilities of applying automated content analysis in journalism studies include, for example, machine learning to identify topics in journalistic coverage or measuring news diffusion via automated approaches. But how have computational methods been applied thus far? And what are consequences of the “computational turn” in communication science, especially concerning interdisciplinarity? Based on a systematic literature review, this article summarizes the use of automated content analysis in journalism studies. Results illustrate an increasing use of the method by communication scientists, as yet another indicator of methodological interdisciplinarity in communication science. However, there is little evidence of an increase in theoretical interdisciplinarity: Studies relying on computational methods do not increasingly refer to theories from other disciplines. With respect to practical interdisciplinarity, for instance collaborations, our discipline is by no means becoming more interdisciplinary. Instead, we find a shift in favor of technical disciplines. At least up to now, the “computational turn” in communication science should thus not be equated with an “interdisciplinary turn.”

Progress in the development of plasmon-enabled light-harvesting technologies requires a better understanding of their fundamental operating principles and current limitations. Here, we employ picosecond time-resolved X-ray photoemission spectroscopy to investigate photoinduced electron transfer in a plasmonic model system composed of 20 nm sized gold nanoparticles (NPs) attached to a nanoporous film of TiO2. The measurement provides direct, quantitative access to transient local charge distributions from the perspectives of the electron donor (AuNP) and the electron acceptor (TiO2). On average, approximately two electrons are injected per NP, corresponding to an electron injection yield per absorbed photon of 0.1%. Back electron transfer from the perspective of the electron donor is dominated by a fast recombination channel proceeding on a time scale of 60 ± 10 ps and a minor contribution that is completed after ∼1 ns. The findings provide a detailed picture of photoinduced charge carrier generation in this NP-semiconductor junction, with important implications for understanding achievable overall photon-to-charge conversion efficiencies.

The angular momentum of rotating superfluid droplets originates from quantized vortices and capillary waves, the interplay between which remains to be uncovered. Here, the rotation of isolated submicrometer superfluid ^{4}He droplets is studied by ultrafast x-ray diffraction using a free electron laser. The diffraction patterns provide simultaneous access to the morphology of the droplets and the vortex arrays they host. In capsule-shaped droplets, vortices form a distorted triangular lattice, whereas they arrange along elliptical contours in ellipsoidal droplets. The combined action of vortices and capillary waves results in droplet shapes close to those of classical droplets rotating with the same angular velocity. The findings are corroborated by density functional theory calculations describing the velocity fields and shape deformations of a rotating superfluid cylinder.

The angular momentum of rotating superfluid droplets originates from quantized vortices and capillary waves, the interplay between which remains to be uncovered. Here, the rotation of isolated submicrometer superfluid ^{4}He droplets is studied by ultrafast x-ray diffraction using a free electron laser. The diffraction patterns provide simultaneous access to the morphology of the droplets and the vortex arrays they host. In capsule-shaped droplets, vortices form a distorted triangular lattice, whereas they arrange along elliptical contours in ellipsoidal droplets. The combined action of vortices and capillary waves results in droplet shapes close to those of classical droplets rotating with the same angular velocity. The findings are corroborated by density functional theory calculations describing the velocity fields and shape deformations of a rotating superfluid cylinder.

Electronic and lattice contributions to picosecond time-resolved X-ray absorption spectra (trXAS) of CuO at the oxygen K-edge are analyzed by comparing trXAS spectra, recorded using excitation wavelengths of 355 nm and 532 nm, to steady-state, temperature-dependent XAS measurements. The trXAS spectra at pump-probe time-delays ≥150 ps are dominated by lattice heating effects. Insight into the temporal evolution of lattice temperature profiles on timescales up to 100s of nanoseconds after laser excitation are reported, on an absolute temperature scale, with a temporal sensitivity and a spatial selectivity on the order of 10s of picoseconds and 10s of nanometers, respectively, effectively establishing an "ultrafast thermometer". In particular, for the 532 nm experiment at ∼5 mJ cm-2 fluence, both the initial sample temperature and its dynamic evolution are well captured by a one-dimensional thermal energy deposition and diffusion model. The thermal conductivity k = (1.3 ± 0.4) W m-1 K-1 derived from this model is in good agreement with the literature value for CuO powder, kpowder = 1.013 W m-1 K-1. For 355 nm excitation, a quantitative analysis of the experiments is hampered by the large temperature gradients within the probed sample volume owing to the small UV penetration depth. The impact of the findings on mitigating or utilizing photoinduced lattice temperature changes in future X-ray free electron laser (XFEL) experiments is discussed.

The success of many emerging molecular electronics concepts hinges on an atomistic understanding of the underlying electronic dynamics. We employ picosecond time-resolved x-ray photoemission spectroscopy (tr-XPS) to elucidate the roles of singlet and triplet excitons for photoinduced charge generation at a copper-phthalocyanine-C60 heterojunction. Contrary to common belief, fast intersystem crossing to triplet excitons after photoexcitation is not a loss channel but contributes to a significantly larger extent to the time-integrated interfacial charge generation than the initially excited singlet excitons. The tr-XPS data provide direct access to the diffusivity of the triplet excitons DCuPc=(1.8±1.2)×10-5cm2/s (where CuPc is copper-phthalocyanine) and their diffusion length Ldiff=(8±3)nm.

Objective: The COVID-19 pandemic has exacerbated existing health disparities. To provide a historical perspective on health disparities for pandemic acute respiratory viruses, we conducted a scoping review of the public health literature of health disparities in influenza outcomes during the 1918, 1957, 1968, and 2009 influenza pandemics. Methods: We searched for articles examining socioeconomic or racial/ethnic disparities in any population, examining any influenza-related outcome (e.g., incidence, hospitalizations, mortality), during the 1918, 1957, 1968, and 2009 influenza pandemics. We conducted a structured search of English-written articles in PubMed supplemented by a snowball of articles meeting inclusion criteria. Results: A total of 29 articles met inclusion criteria, all but one focusing exclusively on the 1918 or 2009 pandemics. Individuals of low socioeconomic status, or living in low socioeconomic status areas, experienced higher incidence, hospitalizations, and mortality in the 1918 and 2009 pandemics. There were conflicting results regarding racial/ethnic disparities during the 1918 pandemic, with differences in magnitude and direction by outcome, potentially due to issues in data quality by race/ethnicity. Racial/ethnic minorities had generally higher incidence, mortality, and hospitalization rates in the 1957 and 2009 pandemics. Conclusion: Individuals of low socioeconomic status and racial/ethnic minorities have historically experienced worse influenza outcomes during pandemics. These historical patterns can inform current research to understand disparities in the ongoing COVID-19 pandemic and future pandemics.

Themen journalistischer Berichterstattung durch maschinelles Lernen identifizieren oder Nachrichtendiffusion automatisiert messen: Die Anwendungsmöglichkeiten der automatisierten Inhaltsanalyse in der Journalismusforschung scheinen vielfältig. Aber wie wird die computerbasierte Methode bisher eingesetzt - und welche Konsequenzen hat der „Computational Turn“ der Kommunikationswissenschaft, besonders im Hinblick auf Interdisziplinarität? Dieser Beitrag fasst auf Basis eines systematischen Literaturüberblicks zusammen, wie die automatisierte Inhaltsanalyse im Forschungsfeld der Journalismusforschung genutzt wird. Dabei zeigt sich, dass die zunehmende Nutzung der Methode ein Indikator für methodische Interdisziplinarität in der ohnehin interdisziplinären Kommunikationswissenschaft ist. Gleichzeitig finden sich kaum Hinweise auf eine Zunahme theoretischer Interdisziplinarität, z. B. Rückgriffe auf fachfremde Theorien. Auch im Hinblick auf praktische Interdisziplinarität, z. B. Kooperationen mit anderen Disziplinen, wird unser Fach keineswegs interdisziplinärer. Vielmehr findet eine Verschiebung zugunsten technischer Disziplinen statt. Der „Computational Turn“ der Kommunikationswissenschaft ist daher zumindest bisher nur teils als „interdisziplinärer Turn“ zu verstehen.

Many ecological studies examine health outcomes and disparities using administrative boundaries such as census tracts, counties, or states. These boundaries help us to understand the patterning of health by place, along with impacts of policies implemented at these levels. However, additional geopolitical units (units with both geographic and political meaning), such as congressional districts (CDs), present further opportunities to connect research with public policy. Here we provide a step-by-step guide on how to conduct disparities-focused analysis at the CD level. As an applied case study, we use geocoded vital statistics data from 2010-2015 to examine levels of and disparities in infant mortality and deaths of despair in the 19 US CDs of Pennsylvania for the 111th-112th (2009-2012) Congresses and 18 CDs for the 113th-114th (2013-2016) Congresses. We also provide recommendations for extending CD-level analysis to other outcomes, states, and geopolitical boundaries, such as state legislative districts. Increased surveillance of health outcomes at the CD level can help prompt policy action and advocacy and, hopefully, reduce rates of and disparities in adverse health outcomes. [ABSTRACT FROM AUTHOR]