TY - GEN A1 - Phuong, Le Quang A1 - Hosseini, Seyed Mehrdad A1 - Sandberg, Oskar J. A1 - Zou, Yingping A1 - Woo, Han Young A1 - Neher, Dieter A1 - Shoaee, Safa T1 - Quantifying quasi-fermi level splitting and open-circuit voltage losses in highly efficient nonfullerene organic solar cells T2 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - The power conversion efficiency (PCE) of state-of-the-art organic solar cells is still limited by significant open-circuit voltage (V-OC) losses, partly due to the excitonic nature of organic materials and partly due to ill-designed architectures. Thus, quantifying different contributions of the V-OC losses is of importance to enable further improvements in the performance of organic solar cells. Herein, the spectroscopic and semiconductor device physics approaches are combined to identify and quantify losses from surface recombination and bulk recombination. Several state-of-the-art systems that demonstrate different V-OC losses in their performance are presented. By evaluating the quasi-Fermi level splitting (QFLS) and the V-OC as a function of the excitation fluence in nonfullerene-based PM6:Y6, PM6:Y11, and fullerene-based PPDT2FBT:PCBM devices with different architectures, the voltage losses due to different recombination processes occurring in the active layers, the transport layers, and at the interfaces are assessed. It is found that surface recombination at interfaces in the studied solar cells is negligible, and thus, suppressing the non-radiative recombination in the active layers is the key factor to enhance the PCE of these devices. This study provides a universal tool to explain and further improve the performance of recently demonstrated high-open-circuit-voltage organic solar cells. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1384 KW - nonfullerene acceptors KW - organic solar cells KW - quasi-Fermi level KW - splitting KW - quasi-steady-state photoinduced absorptions KW - surface KW - recombinations KW - voltage losses Y1 - 2020 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-570018 SN - 1866-8372 IS - 1 ER - TY - GEN A1 - Poch, Olivier A1 - Istiqomah, Istiqomah A1 - Quirico, Eric A1 - Beck, Pierre A1 - Schmitt, Bernard A1 - Theulé, Patrice A1 - Faure, Alexandre A1 - Hily-Blant, Pierre A1 - Bonal, Lydie A1 - Kappel, David T1 - Ammonium salts are a reservoir of nitrogen on a cometary nucleus and possibly on some asteroids T2 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - The measured nitrogen-to-carbon ratio in comets is lower than for the Sun, a discrepancy which could be alleviated if there is an unknown reservoir of nitrogen in comets. The nucleus of comet 67P/Churyumov-Gerasimenko exhibits an unidentified broad spectral reflectance feature around 3.2 micrometers, which is ubiquitous across its surface. On the basis of laboratory experiments, we attribute this absorption band to ammonium salts mixed with dust on the surface. The depth of the band indicates that semivolatile ammonium salts are a substantial reservoir of nitrogen in the comet, potentially dominating over refractory organic matter and more volatile species. Similar absorption features appear in the spectra of some asteroids, implying a compositional link between asteroids, comets, and the parent interstellar cloud. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1389 KW - resolution infrared-spectroscopy KW - ice absorption features KW - young stellar objects KW - exposed water ice KW - MU-M KW - bidirectional reflectance KW - murchison meteorite KW - interstellar ice KW - spectra KW - surface Y1 - 2020 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-513751 SN - 1866-8372 N1 - This secondary publication was withdrawn for copyright reasons. IS - 6483 ER - TY - JOUR A1 - Poch, Olivier A1 - Istiqomah, Istiqomah A1 - Quirico, Eric A1 - Beck, Pierre A1 - Schmitt, Bernard A1 - Theulé, Patrice A1 - Faure, Alexandre A1 - Hily-Blant, Pierre A1 - Bonal, Lydie A1 - Kappel, David T1 - Ammonium salts are a reservoir of nitrogen on a cometary nucleus and possibly on some asteroids JF - Science N2 - The measured nitrogen-to-carbon ratio in comets is lower than for the Sun, a discrepancy which could be alleviated if there is an unknown reservoir of nitrogen in comets. The nucleus of comet 67P/Churyumov-Gerasimenko exhibits an unidentified broad spectral reflectance feature around 3.2 micrometers, which is ubiquitous across its surface. On the basis of laboratory experiments, we attribute this absorption band to ammonium salts mixed with dust on the surface. The depth of the band indicates that semivolatile ammonium salts are a substantial reservoir of nitrogen in the comet, potentially dominating over refractory organic matter and more volatile species. Similar absorption features appear in the spectra of some asteroids, implying a compositional link between asteroids, comets, and the parent interstellar cloud. KW - resolution infrared-spectroscopy KW - ice absorption features KW - young stellar objects KW - exposed water ice KW - MU-M KW - bidirectional reflectance KW - murchison meteorite KW - interstellar ice KW - spectra KW - surface Y1 - 2020 U6 - https://doi.org/10.1126/science.aaw7462 SN - 1095-9203 SN - 0036-8075 VL - 367 IS - 6483 SP - 1 EP - 8 PB - AAAS, American Association for the Advancement of Science CY - Washington, DC ER - TY - JOUR A1 - Perovic, Milena A1 - Qin, Qing A1 - Oschatz, Martin T1 - From molecular precursors to nanoparticles BT - tailoring the adsorption properties of porous carbon materials by controlled chemical functionalization JF - Advanced functional materials N2 - Nanoporous carbon materials (NCMs) provide the "function" of high specific surface area and thus have large interface area for interactions with surrounding species, which is of particular importance in applications related to adsorption processes. The strength and mechanism of adsorption depend on the pore architecture of the NCMs. In addition, chemical functionalization can be used to induce changes of electron density and/or electron density distribution in the pore walls, thus further modifying the interactions between carbons and guest species. Typical approaches for functionalization of nanoporous materials with regular atomic construction like porous silica, metal-organic frameworks, or zeolites, cannot be applied to NCMs due to their less defined local atomic construction and abundant defects. Therefore, synthetic strategies that offer a higher degree of control over the process of functionalization are needed. Synthetic approaches for covalent functionalization of NCMs, that is, for the incorporation of heteroatoms into the carbon backbone, are critically reviewed with a special focus on strategies following the concept "from molecules to materials." Approaches for coordinative functionalization with metallic species, and the functionalization by nanocomposite formation between pristine carbon materials and heteroatom-containing carbons, are introduced as well. Particular focus is given to the influences of these functionalizations in adsorption-related applications. KW - composites KW - heteroatoms KW - metal species KW - porous carbon materials KW - surface KW - functionalization Y1 - 2020 U6 - https://doi.org/10.1002/adfm.201908371 SN - 1616-301X SN - 1616-3028 VL - 30 IS - 41 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Phuong, Le Quang A1 - Hosseini, Seyed Mehrdad A1 - Sandberg, Oskar J. A1 - Zou, Yingping A1 - Woo, Han Young A1 - Neher, Dieter A1 - Shoaee, Safa T1 - Quantifying quasi-fermi level splitting and open-circuit voltage losses in highly efficient nonfullerene organic solar cells JF - Solar RRL N2 - The power conversion efficiency (PCE) of state-of-the-art organic solar cells is still limited by significant open-circuit voltage (V-OC) losses, partly due to the excitonic nature of organic materials and partly due to ill-designed architectures. Thus, quantifying different contributions of the V-OC losses is of importance to enable further improvements in the performance of organic solar cells. Herein, the spectroscopic and semiconductor device physics approaches are combined to identify and quantify losses from surface recombination and bulk recombination. Several state-of-the-art systems that demonstrate different V-OC losses in their performance are presented. By evaluating the quasi-Fermi level splitting (QFLS) and the V-OC as a function of the excitation fluence in nonfullerene-based PM6:Y6, PM6:Y11, and fullerene-based PPDT2FBT:PCBM devices with different architectures, the voltage losses due to different recombination processes occurring in the active layers, the transport layers, and at the interfaces are assessed. It is found that surface recombination at interfaces in the studied solar cells is negligible, and thus, suppressing the non-radiative recombination in the active layers is the key factor to enhance the PCE of these devices. This study provides a universal tool to explain and further improve the performance of recently demonstrated high-open-circuit-voltage organic solar cells. KW - nonfullerene acceptors KW - organic solar cells KW - quasi-Fermi level KW - splitting KW - quasi-steady-state photoinduced absorptions KW - surface KW - recombinations KW - voltage losses Y1 - 2020 U6 - https://doi.org/10.1002/solr.202000649 SN - 2367-198X VL - 5 IS - 1 PB - Wiley-VCH CY - Weinheim ER - TY - GEN A1 - Güntner, Andreas A1 - Reich, Marvin A1 - Mikolaj, Michal A1 - Creutzfeldt, Benjamin A1 - Schroeder, Stephan A1 - Wziontek, Hartmut T1 - Landscape-scale water balance monitoring with an iGrav superconducting gravimeter in a field enclosure T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - In spite of the fundamental role of the landscape water balance for the Earth's water and energy cycles, monitoring the water balance and its components beyond the point scale is notoriously difficult due to the multitude of flow and storage processes and their spatial heterogeneity. Here, we present the first field deployment of an iGrav superconducting gravimeter (SG) in a minimized enclosure for long-term integrative monitoring of water storage changes. Results of the field SG on a grassland site under wet-temperate climate conditions were compared to data provided by a nearby SG located in the controlled environment of an observatory building. The field system proves to provide gravity time series that are similarly precise as those of the observatory SG. At the same time, the field SG is more sensitive to hydrological variations than the observatory SG. We demonstrate that the gravity variations observed by the field setup are almost independent of the depth below the terrain surface where water storage changes occur (contrary to SGs in buildings), and thus the field SG system directly observes the total water storage change, i.e., the water balance, in its surroundings in an integrative way. We provide a framework to single out the water balance components actual evapotranspiration and lateral subsurface discharge from the gravity time series on annual to daily timescales. With about 99 and 85% of the gravity signal due to local water storage changes originating within a radius of 4000 and 200m around the instrument, respectively, this setup paves the road towards gravimetry as a continuous hydrological field-monitoring technique at the landscape scale. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 663 KW - gravity measurements KW - local hydrology KW - storage changes KW - noise-levels KW - time KW - system KW - attraction KW - athmosphere KW - surface Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-419105 SN - 1866-8372 IS - 663 ER - TY - GEN A1 - Puppe, Daniel A1 - Höhn, Axel A1 - Kaczorek, Danuta A1 - Wanner, Manfred A1 - Wehrhan, Marc A1 - Sommer, Michael T1 - How big is the influence of biogenic silicon pools on short-term changes in water-soluble silicon in soils? BT - Implications from a study of a 10-year-old soil–plant system T2 - Postprints der Universität Potsdam : Mathematisch Naturwissenschaftliche Reihe N2 - The significance of biogenic silicon (BSi) pools as a key factor for the control of Si fluxes from terrestrial to aquatic ecosystems has been recognized for decades. However, while most research has been focused on phytogenic Si pools, knowledge of other BSi pools is still limited. We hypothesized that different BSi pools influence short-term changes in the water-soluble Si fraction in soils to different extents. To test our hypothesis we took plant (Calamagrostis epigejos, Phragmites australis) and soil samples in an artificial catchment in a post-mining landscape in the state of Brandenburg, Germany. We quantified phytogenic (phytoliths), protistic (diatom frustules and testate amoeba shells) and zoogenic (sponge spicules) Si pools as well as Tironextractable and water-soluble Si fractions in soils at the beginning (t(0)) and after 10 years (t(10)) of ecosystem development. As expected the results of Tiron extraction showed that there are no consistent changes in the amorphous Si pool at Chicken Creek (Huhnerwasser) as early as after 10 years. In contrast to t(0) we found increased water-soluble Si and BSi pools at t(10); thus we concluded that BSi pools are the main driver of short-term changes in water-soluble Si. However, because total BSi represents only small proportions of water-soluble Si at t(0) (< 2 %) and t(10) (2.8-4.3 %) we further concluded that smaller (< 5 mu m) and/or fragile phytogenic Si structures have the biggest impact on short-term changes in water-soluble Si. In this context, extracted phytoliths (> 5 mu m) only amounted to about 16% of total Si con-tents of plant materials of C. epigejos and P. australis at t(10); thus about 84% of small-scale and/or fragile phytogenic Si is not quantified by the used phytolith extraction method. Analyses of small-scale and fragile phytogenic Si structures are urgently needed in future work as they seem to represent the biggest and most reactive Si pool in soils. Thus they are the most important drivers of Si cycling in terrestrial biogeosystems. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 633 KW - brook experimental forest KW - protozoic Si pool KW - testate amebas KW - biochemical cycle KW - temperate forest KW - amorphous silica KW - dissolution KW - carbon KW - phytoliths KW - surface Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-417141 IS - 633 SP - 5239 EP - 5252 ER - TY - GEN A1 - Rubey, Michael A1 - Brune, Sascha A1 - Heine, Christian A1 - Davies, D. Rhodri A1 - Williams, Simon E. A1 - Müller, R. Dietmar T1 - Global patterns in Earth’s dynamic topography since the Jurassic BT - the role of subducted slabs T2 - Postprints der Universität Potsdam : Mathematisch Naturwissenschaftliche Reihe N2 - We evaluate the spatial and temporal evolution of Earth's long-wavelength surface dynamic topography since the Jurassic using a series of high-resolution global mantle convection models. These models are Earth-like in terms of convective vigour, thermal structure, surface heat-flux and the geographic distribution of heterogeneity. The models generate a degree-2-dominated spectrum of dynamic topography with negative amplitudes above subducted slabs (i.e. circum-Pacific regions and southern Eurasia) and positive amplitudes elsewhere (i.e. Africa, north-western Eurasia and the central Pacific). Model predictions are compared with published observations and subsidence patterns from well data, both globally and for the Australian and southern African regions. We find that our models reproduce the long-wavelength component of these observations, although observed smaller-scale variations are not reproduced. We subsequently define "geodynamic rules" for how different surface tectonic settings are affected by mantle processes: (i) locations in the vicinity of a subduction zone show large negative dynamic topography amplitudes; (ii) regions far away from convergent margins feature long-term positive dynamic topography; and (iii) rapid variations in dynamic support occur along the margins of overriding plates (e.g. the western US) and at points located on a plate that rapidly approaches a subduction zone (e.g. India and the Arabia Peninsula). Our models provide a predictive quantitative framework linking mantle convection with plate tectonics and sedimentary basin evolution, thus improving our understanding of how subduction and mantle convection affect the spatio-temporal evolution of basin architecture. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 623 KW - spherical mantle convection KW - southern African plateau KW - vertical motion KW - sea-level KW - seismic tomography KW - models KW - surface KW - gravity KW - lithosphere KW - Australia Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-418241 SN - 1866-8372 IS - 623 SP - 899 EP - 919 ER - TY - GEN A1 - Frieler, Katja A1 - Mengel, Matthias A1 - Levermann, Anders T1 - Delaying future sea-level rise by storing water in Antarctica T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - Even if greenhouse gas emissions were stopped today, sea level would continue to rise for centuries, with the long-term sea-level commitment of a 2 degrees C warmer world significantly exceeding 2 m. In view of the potential implications for coastal populations and ecosystems worldwide, we investigate, from an ice-dynamic perspective, the possibility of delaying sea-level rise by pumping ocean water onto the surface of the Antarctic ice sheet. We find that due to wave propagation ice is discharged much faster back into the ocean than would be expected from a pure advection with surface velocities. The delay time depends strongly on the distance from the coastline at which the additional mass is placed and less strongly on the rate of sea-level rise that is mitigated. A millennium-scale storage of at least 80% of the additional ice requires placing it at a distance of at least 700 km from the coastline. The pumping energy required to elevate the potential energy of ocean water to mitigate the currently observed 3 mmyr(-1) will exceed 7% of the current global primary energy supply. At the same time, the approach offers a comprehensive protection for entire coastlines particularly including regions that cannot be protected by dikes. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 533 KW - carbon-dioxide emissions KW - ice-sheet KW - climate-change KW - model KW - collapse KW - commitment KW - Greenland KW - discharge KW - project KW - surface Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-410234 SN - 1866-8372 IS - 533 ER - TY - THES A1 - Feldmann, David T1 - Light-driven diffusioosmosis T1 - Licht-getriebene Diffusioosmose BT - the manipulation of colloids using azobenzene containing surfactant BT - Manipulation von Kolloiden mittels azobenzolhaltigen Tensiden N2 - The emergence of microfluidics created the need for precise and remote control of micron-sized objects. I demonstrate how light-sensitive motion can be induced at the micrometer scale by a simple addition of a photosensitive surfactant, which makes it possible to trigger hydrophobicity with light. With point-like laser irradiation, radial inward and outward hydrodynamic surface flows are remotely switched on and off. In this way, ensembles of microparticles can be moved toward or away from the irradiation center. Particle motion is analyzed according to varying parameters, such as surfactant and salt concentration, illumination condition, surface hydrophobicity, and surface structure. The physical origin of this process is the so-called light-driven diffusioosmosis (LDDO), a phenomenon that was discovered in the framework of this thesis and is described experimentally and theoretically in this work. To give a brief explanation, a focused light irradiation induces a local photoisomerization that creates a concentration gradient at the solid-liquid interface. To compensate for the change in osmotic pressure near the surface, a hydrodynamic flow along the surface is generated. Surface-surfactant interaction largely governs LDDO. It is shown that surfactant adsorption depends on the isomerization state of the surfactant. Photoisomerization, therefore, triggers a surfactant attachment or detachment from the surface. This change is considered to be one of the reasons for the formation of LDDO flow. These flows are introduced not only by a focused laser source but also by global irradiation. Porous particles show reversible repulsive and attractive interactions when dispersed in the solution of photosensitive surfactant. Repulsion and attraction is controlled by the irradiation wavelength. Illumination with red light leads to formation of aggregates, while illumination with blue light leads to the formation of a well-separated grid with equal interparticle distances, between 2µm and 80µm, depending on the particle surface density. These long-range interactions are considered to be a result of an increase or decrease of surfactant concentration around each particle, depending on the irradiation wavelength. Surfactant molecules adsorb inside the pores of the particles. A light-induced photoisomerization changes adsorption to the pores and drives surfactant molecules to the outside. The concentration gradients generate symmetric flows around each single particle resulting in local LDDO. With a break of the symmetry (i.e., by closing one side of the particle with a metal cap), one can achieve active self-propelled particle motion. N2 - Mit Aufkommen der Mikrofluidik entstand eine größere Nachfrage nach präziser und berührungsfreier Manipulation von mikrometergroßen Objekten. In dieser Arbeit wird gezeigt, wie Bewegung im Mikrometerbereich durch ein lichtschaltbares Tensid erzeugt werden kann, deren Hydrophobizität sich durch Beleuchtung ändert. Eine fokussierte punktförmige Laserbestrahlung erzeugt einen radial nach außen oder innen gerichteten Fluss an der Substratoberfläche je nach Laserwellenlänge. Mikropartikel die sich auf der Oberfläche befinden, bewegen sich dadurch passiv mit dem Fluss entweder zum Bestrahlungspunkt hin oder vom Bestrahlungspunkt weg. Die Partikelbewegung wird in Abhängigkeit von den folgenden Parametern untersucht: Tensid- und Salzkonzentration, Bestrahlungsbedingungen, Hydrophobizität der Oberfläche und Oberflächenstruktur. Der Grund für die Bewegung kann in einem Prozess gefunden werden, der sogenannten lichtgetriebenen Diffusioosmose (LDDO), die im Rahmen dieser Dissertation entdeckt und theoretisch sowie experimentell beschrieben wurde. Der Prozess kann wie folgt betrachtet werden: Die fokussierte Bestrahlung induziert eine lokale Photo-Isomerisation der Tensidmoleküle, die eine Monomer-Konzentrationsänderung zur Folge hat. Lokal entsteht ein hierdurch ein höherer osmotischer Druck an der Oberfläche. Um den Druckunterschied an der Oberfläche auszugleichen, wird ein hydrodynamischer Fluss nahe der Oberfläche erzeugt. Hierbei bestimmt vor allem die Wechselwirkung zwischen Tensid und Oberfläche den induzierten Fluss. Es wird gezeigt, dass die Oberflächenadsorption des Tensids vom Isomerisationszustand abhängt. Somit kann eine Bestrahlung ein Ablösen von oder Anhaften an der Oberfläche erzeugen. Diese Änderung der Oberflächenkonzentration kann als einer der Gründe für die Flussentstehung angesehen werden. Diese hydrodynamischen Oberflächenflüssen können nicht nur durch einen fokussierten Laser erzeugt werden, sondern auch durch eine gesamte Bestrahlung der Oberfläche. Hierbei zeigen poröse Partikel eine reversible Anziehung und Abstoßung, wenn sie sich in einer Tensidlösung und an einer Substratoberfläche befinden. Die Wechselwirkung kann hierbei durch die Bestrahlungswellenlänge kontrolliert werden. In Dunkelheit oder in rotem Licht ziehen sich die Partikel gegenseitig an, währenddessen sie sich unter blauer Bestrahlung abstoßen und ein Partikelnetz erzeugen mit äquidistanten Abständen zwischen den Partikeln. Die Partikelabstände hängen von der Partikeldichte an der Oberfläche ab und variieren zwischen 2µm und 80µm. Der Grund für die reversible Anziehung und Abstoßung wird ähnlich zu LDDO in einer lichtinduzierten Konzentrationsänderung gesehen. Tensidmoleküle adsorbieren innerhalb der Poren der Partikel. Durch eine lichtinduzierte Isomerisation werden die Moleküle ausgestoßen. Hierbei entsteht die Konzentrationsänderung um jedes poröse Partikel herum, währenddessen sie in LDDO um den Laserpunkt entsteht. Somit werden diffusioosmotische Flüsse symmetrisch um jedes Partikel erzeugt, wohingegen sie in LDDO nur um den Laserpunkt erzeugt werden.Demzufolge stoßen sich die Partikel durch eine hydrodynamische Wechselwirkung ab. Es wird gezeigt, dass aufgrund eines Symmetriebruchs durch ein Abdecken einer Partikelhälfte eine aktive selbstgetriebene Partikelbewegung erzeugt werden kann. KW - azobenzene surfactant KW - Diffusioosmosis KW - Janus particle KW - surface KW - solid-liquid interface KW - surface flow KW - micro swimmer KW - self-propelled particle KW - light-driven KW - particles KW - azobenzolhaltige Tenside KW - Diffusioosmose KW - Janus Partikel KW - Oberfläche KW - fest-flüssig Grenzfläche KW - Oberflächenfluss KW - Mikroschwimmer KW - selbst-getriebene Partikel KW - licht-getrieben KW - Partikel Y1 - 2018 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-417184 ER -