TY  - JOUR
A1  - Comparot-Moss, Sylviane
A1  - Koetting, Oliver
A1  - Stettler, Michaela
A1  - Edner, Christoph
A1  - Graf, Alexander
A1  - Weise, Sean E.
A1  - Streb, Sebastian
A1  - Lue, Wei-Ling
A1  - MacLean, Daniel
A1  - Mahlow, Sebastian
A1  - Ritte, Gerhard
A1  - Steup, Martin
A1  - Chen, Jychian
A1  - Zeeman, Samuel C.
A1  - Smith, Alison M.
T1  - A putative phosphatase, LSF1, is required for normal starch turnover in Arabidopsis leaves
N2  - A putative phosphatase, LSF1 (for LIKE SEX4; previously PTPKIS2), is closely related in sequence and structure to STARCH-EXCESS4 (SEX4), an enzyme necessary for the removal of phosphate groups from starch polymers during starch degradation in Arabidopsis (Arabidopsis thaliana) leaves at night. We show that LSF1 is also required for starch degradation: lsf1 mutants, like sex4 mutants, have substantially more starch in their leaves than wild-type plants throughout the diurnal cycle. LSF1 is chloroplastic and is located on the surface of starch granules. lsf1 and sex4 mutants show similar, extensive changes relative to wild-type plants in the expression of sugar-sensitive genes. However, although LSF1 and SEX4 are probably both involved in the early stages of starch degradation, we show that LSF1 neither catalyzes the same reaction as SEX4 nor mediates a sequential step in the pathway. Evidence includes the contents and metabolism of phosphorylated glucans in the single mutants. The sex4 mutant accumulates soluble phospho- oligosaccharides undetectable in wild-type plants and is deficient in a starch granule-dephosphorylating activity present in wild-type plants. The lsf1 mutant displays neither of these phenotypes. The phenotype of the lsf1/sex4 double mutant also differs from that of both single mutants in several respects. We discuss the possible role of the LSF1 protein in starch degradation.
Y1  - 2010
UR  - http://www.plantphysiol.org/
U6  - https://doi.org/10.1104/pp.109.148981
SN  - 0032-0889
ER  - 
TY  - JOUR
A1  - Colombo, Stefanie M.
A1  - Wacker, Alexander
A1  - Parrish, Christopher C.
A1  - Kainz, Martin J.
A1  - Arts, Michael T.
T1  - A fundamental dichotomy in long-chain polyunsaturated fatty acid abundance between and within marine and terrestrial ecosystems
JF  - Environmental reviews = Dossiers environnement
N2  - Polyunsaturated fatty acids (PUFA), especially long-chain (i.e., >= 20 carbons) polyunsaturated fatty acids (LC-PUFA), are fundamental to the health and survival of marine and terrestrial organisms. Therefore, it is imperative that we gain a better understanding of their origin, abundance, and transfer between and within these ecosystems. We evaluated the natural variation in PUFA distribution and abundance that exists between and within these ecosystems by amassing and analyzing, using multivariate and analysis of variance (ANOVA) methods, >3000 fatty acid (FA) profiles from marine and terrestrial organisms. There was a clear dichotomy in LC-PUFA abundance between organisms in marine and terrestrial ecosystems, mainly driven by the C-18 PUFA in terrestrial organisms and omega-3 (n-3) LC-PUFA in marine organisms. The PUFA content of an organism depended on both its biome (marine vs terrestrial) and taxonomic group. Within the marine biome, the PUFA content varied among taxonomic groups. PUFA content of marine organisms was dependent on both geographic zone (i.e., latitude, and thus broadly related to temperature) and trophic level (a function of diet). The contents of n-3 LC-PUFA were higher in polar and temperate marine organisms than those from the tropics. Therefore, we conclude that, on a per capita basis, high latitude marine organisms provide a disproportionately large global share of these essential nutrients to consumers, including terrestrial predators. Our analysis also hints at how climate change, and other anthropogenic stressors, might act to negatively impact the global distribution and abundance of n-3 LC-PUFA within marine ecosystems and on the terrestrial consumers that depend on these subsidies.
KW  - climate change
KW  - food webs
KW  - omega-3
KW  - polyunsaturated fatty acids
KW  - trophic ecology
Y1  - 2017
U6  - https://doi.org/10.1139/er-2016-0062
SN  - 1208-6053
SN  - 1181-8700
VL  - 25
SP  - 163
EP  - 174
PB  - NRC Research Press
CY  - Ottawa
ER  - 
TY  - JOUR
A1  - Hixson, Stefanie M.
A1  - Sharma, Bhanu
A1  - Kainz, Martin J.
A1  - Wacker, Alexander
A1  - Arts, Michael T.
T1  - Production, distribution, and abundance of long-chain omega-3 polyunsaturated fatty acids: a fundamental dichotomy between freshwater and terrestrial ecosystems
JF  - Environmental reviews = Dossiers environnement
N2  - Long-chain polyunsaturated fatty acids (LC-PUFA) are critical for the health of aquatic and terrestrial organisms; therefore, understanding the production, distribution, and abundance of these compounds is imperative. Although the dynamics of LC-PUFA production and distribution in aquatic environments has been well documented, a systematic and comprehensive comparison to LC-PUFA in terrestrial environments has not been rigorously investigated. Here we use a data synthesis approach to compare and contrast fatty acid profiles of 369 aquatic and terrestrial organisms. Habitat and trophic level were interacting factors that determined the proportion of individual omega-3 (n-3) or omega-6 (n-6) PUFA in aquatic and terrestrial organisms. Higher total n-3 content compared with n-6 PUFA and a strong prevalence of the n-3 PUFA eicosapentaenoic acid (EPA) and docosahexaenoic acid (DHA) characterized aquatic versus terrestrial organisms. Conversely, terrestrial organisms had higher linoleic acid (LNA) and alpha-linolenic acid (ALA) contents than aquatic organisms; however, the ratio of ALA: LNA was higher in aquatic organisms. The EPA + DHA content was higher in aquatic animals than terrestrial organisms, and increased from algae to invertebrates to vertebrates in the aquatic environment. An analysis of covariance (ANCOVA) revealed that fatty acid composition was highly dependent on the interaction between habitat and trophic level. We conclude that freshwater ecosystems provide an essential service through the production of n-3 LC-PUFA that are required to maintain the health of terrestrial organisms including humans.
KW  - aquatic ecosystems
KW  - conservation
KW  - eicosapentaenoic acid
KW  - docosahexaenoic acid
KW  - food webs
Y1  - 2015
U6  - https://doi.org/10.1139/er-2015-0029
SN  - 1208-6053
SN  - 1181-8700
VL  - 23
IS  - 4
SP  - 414
EP  - 424
PB  - NRC Research Press
CY  - Ottawa
ER  - 
TY  - JOUR
A1  - Heinze, Johannes
A1  - Simons, Nadja K.
A1  - Seibold, Sebastian
A1  - Wacker, Alexander
A1  - Weithoff, Guntram
A1  - Gossner, Martin M.
A1  - Prati, Daniel
A1  - Bezemer, T. Martijn
A1  - Joshi, Jasmin Radha
T1  - The relative importance of plant-soil feedbacks for plant-species performance increases with decreasing intensity of herbivory
JF  - Oecologia
N2  - Under natural conditions, aboveground herbivory and plant-soil feedbacks (PSFs) are omnipresent interactions strongly affecting individual plant performance. While recent research revealed that aboveground insect herbivory generally impacts the outcome of PSFs, no study tested to what extent the intensity of herbivory affects the outcome. This, however, is essential to estimate the contribution of PSFs to plant performance under natural conditions in the field. Here, we tested PSF effects both with and without exposure to aboveground herbivory for four common grass species in nine grasslands that formed a gradient of aboveground invertebrate herbivory. Without aboveground herbivores, PSFs for each of the four grass species were similar in each of the nine grasslands-both in direction and in magnitude. In the presence of herbivores, however, the PSFs differed from those measured under herbivory exclusion, and depended on the intensity of herbivory. At low levels of herbivory, PSFs were similar in the presence and absence of herbivores, but differed at high herbivory levels. While PSFs without herbivores remained similar along the gradient of herbivory intensity, increasing herbivory intensity mostly resulted in neutral PSFs in the presence of herbivores. This suggests that the relative importance of PSFs for plant-species performance in grassland communities decreases with increasing intensity of herbivory. Hence, PSFs might be more important for plant performance in ecosystems with low herbivore pressure than in ecosystems with large impacts of insect herbivores.
KW  - Plant-soil feedback
KW  - Herbivorous insects
KW  - Field conditions
KW  - Selective herbivory
KW  - Nutritional quality
Y1  - 2019
U6  - https://doi.org/10.1007/s00442-019-04442-9
SN  - 0029-8549
SN  - 1432-1939
VL  - 190
IS  - 3
SP  - 651
EP  - 664
PB  - Springer
CY  - New York
ER  - 
TY  - JOUR
A1  - Pröve, Ralf
A1  - Kroll, Stefan
A1  - Asche, Matthias
A1  - Heinecke, Anne
A1  - Huhtamies, Mikko
A1  - Marschke, Benjamin
A1  - Gräf, Holger Th.
A1  - Reimer, Torsten F.
A1  - Schmitt, Bernhard
A1  - Muth, Jörg
A1  - Reiff, Michael
A1  - Gebuhr, Ralf
A1  - Martin, Alexander M.
A1  - Krebs, Daniel
T1  - Militär und Gesellschaft in der Frühen Neuzeit
N2  - Aus dem Inhalt dieser Ausgabe: BEITRAG: Ralf Pröve: Vom Schmuddelkind zur anerkannten Subdisziplin?1Die „neue Militärgeschichte“ der Frühen Neuzeitund der AMG PROJEKTE: Stefan Kroll: Kursächsische Soldaten im 18. Jahrhundert (1728-1789) Matthias Asche: Neusiedler im verheerten Land –Kriegsfolgenbewältigung, Landeswiederaufbau undMigration in der Mark Brandenburg und in Badennach den Kriegen des 17. Jahrhunderts Anne Heinecke: Wahrnehmung und Darstellungvon Plünderung im 17. Jahrhundertim Spiegel von Selbstzeugnissen Militärangehöriger Mikko Huhtamies: Ersatzsoldaten in Europa in der Frühen Neuzeit Benjamin MarschkeThe Development of the Army Chaplaincy inEarly Eighteenth-Century Prussia Holger Th. Gräf: Valentin Wagner – Zeichnungen aus der Zeit desDreißigjährigen Krieges Torsten F. Reimer: magi-e – integriertes Publizierenin der Geschichtswissenschaft Bernhard Schmitt: Militär und Integration im 19. Jahrhundert –Zur Bedeutung und Funktion der Armeebei der Eingliederung neuer Bevölkerungsgruppenin Preußen und der Habsburgermonarchie 1815-1867 Jörg Muth: Flucht aus dem militärischen AlltagUrsachen und individuelle Ausprägung der Desertionin der Armee Friedrichs des Großen Michael Reiff: Strandgut des Krieges: Die soziale Lage Kriegsversehrterin den deutschen Armeen des Absolutismusund der napoleonischen Zeit ( 1648 – 1815 ) Ralf Gebuhr: Nickel von Minckwitzund der frühneuzeitliche Schlossbauin der Niederlausitz Alexander M. Martin: Die Napoleonische Okkupation Moskaus 1812 Daniel Krebs: Deutsche Kriegsgefangeneim Amerikanischen Unabhängigkeitskrieg BERICHTE: REZENSIONEN:
T3  - Militär und Gesellschaft in der frühen Neuzeit - 5, Heft 1 
KW  - Militär / Geschichte
Y1  - 2001
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus-28135
SN  - 1617-9722
SN  - 1861-910X
VL  - 5
IS  - 1
ER  - 
TY  - JOUR
A1  - Gardiner, Lauren M.
A1  - Kocyan, Alexander
A1  - Motes, Martin
A1  - Roberts, David L.
A1  - Emerson, Brent C.
T1  - Molecular phylogenetics of Vanda and related genera (Orchidaceae)
JF  - Botanical journal of the Linnean Society
N2  - The genus Vanda and its affiliated taxa are a diverse group of horticulturally important species of orchids occurring mainly in South-East Asia, for which generic limits are poorly defined. Here, we present a molecular study using sequence data from three plastid DNA regions. It is shown that Vanda s.l. forms a clade containing approximately 73 species, including the previously accepted genera Ascocentrum, Euanthe, Christensonia, Neofinetia and Trudelia, and the species Aerides flabellata. Resolution of the phylogenetic relationships of species in Vanda s.l. is relatively poor, but existing morphological classifications for Vanda are incongruent with the results produced. Some novel species relationships are revealed, and a new morphological sectional classification is proposed based on support for these groupings and corresponding morphological characters shared by taxa and their geographical distributions. The putative occurrence of multiple pollination syndromes in this group of taxa, combined with complex biogeographical history of the South-East Asian region, is discussed in the context of these results.(c) 2013 The Linnean Society of London, Botanical Journal of the Linnean Society, 2013, 173, 549-572.
KW  - Aeridinae
KW  - Ascocentrum
KW  - classification
KW  - Euanthe
KW  - matK
KW  - morphology
KW  - Neofinetia
KW  - psbA-trnH
KW  - trnL
KW  - trnL-F
Y1  - 2013
U6  - https://doi.org/10.1111/boj.12102
SN  - 0024-4074
SN  - 1095-8339
VL  - 173
IS  - 4
SP  - 549
EP  - 572
PB  - Wiley-Blackwell
CY  - Hoboken
ER  - 
TY  - JOUR
A1  - Wernet, Philippe
A1  - Kunnus, Kristjan
A1  - Josefsson, Ida
A1  - Rajkovic, Ivan
A1  - Quevedo, Wilson
A1  - Beye, Martin
A1  - Schreck, Simon
A1  - Gruebel, S.
A1  - Scholz, Mirko
A1  - Nordlund, Dennis
A1  - Zhang, Wenkai
A1  - Hartsock, Robert W.
A1  - Schlotter, William F.
A1  - Turner, Joshua J.
A1  - Kennedy, Brian
A1  - Hennies, Franz
A1  - de Groot, Frank M. F.
A1  - Gaffney, Kelly J.
A1  - Techert, Simone
A1  - Odelius, Michael
A1  - Föhlisch, Alexander
T1  - Orbital-specific mapping of the ligand exchange dynamics of Fe(CO)(5) in solution
JF  - Nature : the international weekly journal of science
N2  - Transition-metal complexes have long attracted interest for fundamental chemical reactivity studies and possible use in solar energy conversion(1,2). Electronic excitation, ligand loss from the metal centre, or a combination of both, creates changes in charge and spin density at the metal site(3-11) that need to be controlled to optimize complexes for photocatalytic hydrogen production(8) and selective carbon-hydrogen bond activation(9-11). An understanding at the molecular level of how transition-metal complexes catalyse reactions, and in particular of the role of the short-lived and reactive intermediate states involved, will be critical for such optimization. However, suitable methods for detailed characterization of electronic excited states have been lacking. Here we show, with the use of X-ray laser-based femtosecond-resolution spectroscopy and advanced quantum chemical theory to probe the reaction dynamics of the benchmark transition-metal complex Fe(CO)(5) in solution, that the photo-induced removal of CO generates the 16-electron Fe(CO)(4) species, a homogeneous catalyst(12,13) with an electron deficiency at the Fe centre(14,15), in a hitherto unreported excited singlet state that either converts to the triplet ground state or combines with a CO or solvent molecule to regenerate a penta-coordinated Fe species on a sub-picosecond timescale. This finding, which resolves the debate about the relative importance of different spin channels in the photochemistry of Fe(CO)(5) (refs 4, 16-20), was made possible by the ability of femtosecond X-ray spectroscopy to probe frontier-orbital interactions with atom specificity. We expect the method to be broadly applicable in the chemical sciences, and to complement approaches that probe structural dynamics in ultrafast processes.
Y1  - 2015
U6  - https://doi.org/10.1038/nature14296
SN  - 0028-0836
SN  - 1476-4687
VL  - 520
IS  - 7545
SP  - 78
EP  - 81
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Kissling, W. D.
A1  - Dormann, Carsten F.
A1  - Groeneveld, Juergen
A1  - Hickler, Thomas
A1  - Kühn, Ingolf
A1  - McInerny, Greg J.
A1  - Montoya, Jose M.
A1  - Römermann, Christine
A1  - Schiffers, Katja
A1  - Schurr, Frank Martin
A1  - Singer, Alexander
A1  - Svenning, Jens-Christian
A1  - Zimmermann, Niklaus E.
A1  - O'Hara, Robert B.
T1  - Towards novel approaches to modelling biotic interactions in multispecies assemblages at large spatial extents
JF  - Journal of biogeography
N2  - Aim Biotic interactions within guilds or across trophic levels have widely been ignored in species distribution models (SDMs). This synthesis outlines the development of species interaction distribution models (SIDMs), which aim to incorporate multispecies interactions at large spatial extents using interaction matrices. Location Local to global. Methods We review recent approaches for extending classical SDMs to incorporate biotic interactions, and identify some methodological and conceptual limitations. To illustrate possible directions for conceptual advancement we explore three principal ways of modelling multispecies interactions using interaction matrices: simple qualitative linkages between species, quantitative interaction coefficients reflecting interaction strengths, and interactions mediated by interaction currencies. We explain methodological advancements for static interaction data and multispecies time series, and outline methods to reduce complexity when modelling multispecies interactions. Results Classical SDMs ignore biotic interactions and recent SDM extensions only include the unidirectional influence of one or a few species. However, novel methods using error matrices in multivariate regression models allow interactions between multiple species to be modelled explicitly with spatial co-occurrence data. If time series are available, multivariate versions of population dynamic models can be applied that account for the effects and relative importance of species interactions and environmental drivers. These methods need to be extended by incorporating the non-stationarity in interaction coefficients across space and time, and are challenged by the limited empirical knowledge on spatio-temporal variation in the existence and strength of species interactions. Model complexity may be reduced by: (1) using prior ecological knowledge to set a subset of interaction coefficients to zero, (2) modelling guilds and functional groups rather than individual species, and (3) modelling interaction currencies and species effect and response traits. Main conclusions There is great potential for developing novel approaches that incorporate multispecies interactions into the projection of species distributions and community structure at large spatial extents. Progress can be made by: (1) developing statistical models with interaction matrices for multispecies co-occurrence datasets across large-scale environmental gradients, (2) testing the potential and limitations of methods for complexity reduction, and (3) sampling and monitoring comprehensive spatio-temporal data on biotic interactions in multispecies communities.
KW  - Community ecology
KW  - ecological networks
KW  - global change
KW  - guild assembly
KW  - multidimensional complexity
KW  - niche theory
KW  - prediction
KW  - species distribution model
KW  - species interactions
KW  - trait-based community modules
Y1  - 2012
U6  - https://doi.org/10.1111/j.1365-2699.2011.02663.x
SN  - 0305-0270
VL  - 39
IS  - 12
SP  - 2163
EP  - 2178
PB  - Wiley-Blackwell
CY  - Hoboken
ER  - 
TY  - JOUR
A1  - Salzmann, Ingo
A1  - Heimel, Georg
A1  - Duhm, Steffen
A1  - Oehzelt, Martin
A1  - Pingel, Patrick
A1  - George, Benjamin M.
A1  - Schnegg, Alexander
A1  - Lips, Klaus
A1  - Blum, Ralf-Peter
A1  - Vollmer, Antje
A1  - Koch, Norbert
T1  - Intermolecular hybridization governs molecular electrical doping
JF  - Physical review letters
N2  - Current models for molecular electrical doping of organic semiconductors are found to be at odds with other well-established concepts in that field, like polaron formation. Addressing these inconsistencies for prototypical systems, we present experimental and theoretical evidence for intermolecular hybridization of organic semiconductor and dopant frontier molecular orbitals. Common doping-related observations are attributed to this phenomenon, and controlling the degree of hybridization emerges as a strategy for overcoming the present limitations in the yield of doping-induced charge carriers.
Y1  - 2012
U6  - https://doi.org/10.1103/PhysRevLett.108.035502
SN  - 0031-9007
VL  - 108
IS  - 3
PB  - American Physical Society
CY  - College Park
ER  - 
TY  - JOUR
A1  - Altenbach, Alexander V.
A1  - Pflaum, U.
A1  - Scheibel, Thomas R.
A1  - Thies, A.
A1  - Timm, M.
A1  - Trauth, Martin H.
T1  - Scaling percentages of benthic forminifera with flux rates of organic carbon
Y1  - 1999
ER  - 
TY  - JOUR
A1  - Wernet, Philippe
A1  - Leitner, T.
A1  - Josefsson, Ida
A1  - Mazza, T.
A1  - Miedema, P. S.
A1  - Schroder, H.
A1  - Beye, Martin
A1  - Kunnus, K.
A1  - Schreck, S.
A1  - Radcliffe, P.
A1  - Dusterer, S.
A1  - Meyer, M.
A1  - Odelius, Michael
A1  - Fohlisch, Alexander
T1  - Communication: Direct evidence for sequential dissociation of gas-phase Fe(CO)(5) via a singlet pathway upon excitation at 266 nm
JF  - The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr
N2  - We prove the hitherto hypothesized sequential dissociation of Fe(CO)(5) in the gas phase upon photoexcitation at 266 nm via a singlet pathway with time-resolved valence and core-level photoelectron spectroscopy with an x-ray free-electron laser. Valence photoelectron spectra are used to identify free CO molecules and to determine the time constants of stepwise dissociation to Fe(CO)(4) within the temporal resolution of the experiment and further to Fe(CO)(3) within 3 ps. Fe 3p core-level photoelectron spectra directly reflect the singlet spin state of the Fe center in Fe(CO)(5), Fe(CO)(4), and Fe(CO)(3) showing that the dissociation exclusively occurs along a singlet pathway without triplet-state contribution. Our results are important for assessing intra- and intermolecular relaxation processes in the photodissociation dynamics of the prototypical Fe(CO)(5) complex in the gas phase and in solution, and they establish time-resolved core-level photoelectron spectroscopy as a powerful tool for determining the multiplicity of transition metals in photochemical reactions of coordination complexes. Published by AIP Publishing.
Y1  - 2017
U6  - https://doi.org/10.1063/1.4984774
SN  - 0021-9606
SN  - 1089-7690
VL  - 146
PB  - American Institute of Physics
CY  - Melville
ER  - 
TY  - JOUR
A1  - Sellberg, Jonas A.
A1  - McQueen, Trevor A.
A1  - Laksmono, Hartawan
A1  - Schreck, Simon
A1  - Beye, Martin
A1  - DePonte, Daniel P.
A1  - Kennedy, Brian
A1  - Nordlund, Dennis
A1  - Sierra, Raymond G.
A1  - Schlesinger, Daniel
A1  - Tokushima, Takashi
A1  - Zhovtobriukh, Iurii
A1  - Eckert, Sebastian
A1  - Segtnan, Vegard H.
A1  - Ogasawara, Hirohito
A1  - Kubicek, Katharina
A1  - Techert, Simone
A1  - Bergmann, Uwe
A1  - Dakovski, Georgi L.
A1  - Schlotter, William F.
A1  - Harada, Yoshihisa
A1  - Bogan, Michael J.
A1  - Wernet, Philippe
A1  - Föhlisch, Alexander
A1  - Pettersson, Lars G. M.
A1  - Nilsson, Anders
T1  - X-ray emission spectroscopy of bulk liquid water in "no-man's land"
JF  - The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr
N2  - The structure of bulk liquid water was recently probed by x-ray scattering below the temperature limit of homogeneous nucleation (T-H) of similar to 232 K [J. A. Sellberg et al., Nature 510, 381-384 (2014)]. Here, we utilize a similar approach to study the structure of bulk liquid water below T-H using oxygen K-edge x-ray emission spectroscopy (XES). Based on previous XES experiments [T. Tokushima et al., Chem. Phys. Lett. 460, 387-400 (2008)] at higher temperatures, we expected the ratio of the 1b(1)' and 1b(1)" peaks associated with the lone-pair orbital in water to change strongly upon deep supercooling as the coordination of the hydrogen (H-) bonds becomes tetrahedral. In contrast, we observed only minor changes in the lone-pair spectral region, challenging an interpretation in terms of two interconverting species. A number of alternative hypotheses to explain the results are put forward and discussed. Although the spectra can be explained by various contributions from these hypotheses, we here emphasize the interpretation that the line shape of each component changes dramatically when approaching lower temperatures, where, in particular, the peak assigned to the proposed disordered component would become more symmetrical as vibrational interference becomes more important. (C) 2015 AIP Publishing LLC.
Y1  - 2015
U6  - https://doi.org/10.1063/1.4905603
SN  - 0021-9606
SN  - 1089-7690
VL  - 142
IS  - 4
PB  - American Institute of Physics
CY  - Melville
ER  - 
TY  - JOUR
A1  - Jay, Raphael M.
A1  - Norell, Jesper
A1  - Eckert, Sebastian
A1  - Hantschmann, Markus
A1  - Beye, Martin
A1  - Kennedy, Brian
A1  - Quevedo, Wilson
A1  - Schlotter, William F.
A1  - Dakovski, Georgi L.
A1  - Minitti, Michael P.
A1  - Hoffmann, Matthias C.
A1  - Mitra, Ankush
A1  - Moeller, Stefan P.
A1  - Nordlund, Dennis
A1  - Zhang, Wenkai
A1  - Liang, Huiyang W.
A1  - Kunnus, Kristian
A1  - Kubicek, Katharina
A1  - Techert, Simone A.
A1  - Lundberg, Marcus
A1  - Wernet, Philippe
A1  - Gaffney, Kelly
A1  - Odelius, Michael
A1  - Föhlisch, Alexander
T1  - Disentangling Transient Charge Density and Metal-Ligand Covalency in Photoexcited Ferricyanide with Femtosecond Resonant Inelastic Soft X-ray Scattering
JF  - The journal of physical chemistry letters
N2  - Soft X-ray spectroscopies are ideal probes of the local valence electronic structure of photocatalytically active metal sites. Here, we apply the selectivity of time resolved resonant inelastic X-ray scattering at the iron L-edge to the transient charge distribution of an optically excited charge-transfer state in aqueous ferricyanide. Through comparison to steady-state spectra and quantum chemical calculations, the coupled effects of valence-shell closing and ligand-hole creation are experimentally and theoretically disentangled and described in terms of orbital occupancy, metal-ligand covalency, and ligand field splitting, thereby extending established steady-state concepts to the excited-state domain. pi-Back-donation is found to be mainly determined by the metal site occupation, whereas the ligand hole instead influences sigma-donation. Our results demonstrate how ultrafast resonant inelastic X-ray scattering can help characterize local charge distributions around catalytic metal centers in short-lived charge-transfer excited states, as a step toward future rationalization and tailoring of photocatalytic capabilities of transition-metal complexes.
Y1  - 2018
U6  - https://doi.org/10.1021/acs.jpclett.8b01429
SN  - 1948-7185
VL  - 9
IS  - 12
SP  - 3538
EP  - 3543
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Schreck, Simon
A1  - Beye, Martin
A1  - Sellberg, Jonas A.
A1  - McQueen, Trevor
A1  - Laksmono, Hartawan
A1  - Kennedy, Brian
A1  - Eckert, Sebastian
A1  - Schlesinger, Daniel
A1  - Nordlund, Dennis
A1  - Ogasawara, Hirohito
A1  - Sierra, Raymond G.
A1  - Segtnan, Vegard H.
A1  - Kubicek, Katharina
A1  - Schlotter, William F.
A1  - Dakovski, Georgi L.
A1  - Moeller, Stefan P.
A1  - Bergmann, Uwe
A1  - Techert, Simone
A1  - Pettersson, Lars G. M.
A1  - Wernet, Philippe
A1  - Bogan, Michael J.
A1  - Harada, Yoshihisa
A1  - Nilsson, Anders
A1  - Föhlisch, Alexander
T1  - Reabsorption of soft x-ray emission at high x-ray free-electron laserfluences
JF  - Physical review letters
N2  - We report on oxygen K-edge soft x-ray emission spectroscopy from a liquid water jet at the Linac Coherent Light Source. We observe significant changes in the spectral content when tuning over a wide range of incident x-ray fluences. In addition the total emission yield decreases at high fluences. These modifications result from reabsorption of x-ray emission by valence-excited molecules generated by the Auger cascade. Our observations have major implications for future x-ray emission studies at intense x-ray sources. We highlight the importance of the x-ray pulse length with respect to the core-hole lifetime.
Y1  - 2014
U6  - https://doi.org/10.1103/PhysRevLett.113.153002
SN  - 0031-9007
SN  - 1079-7114
VL  - 113
IS  - 15
PB  - American Physical Society
CY  - College Park
ER  - 
TY  - JOUR
A1  - Reifarth, Martin
A1  - Bekir, Marek
A1  - Bapolisi, Alain M.
A1  - Titov, Evgenii
A1  - Nusshardt, Fabian
A1  - Nowaczyk, Julius
A1  - Grigoriev, Dmitry
A1  - Sharma, Anjali
A1  - Saalfrank, Peter
A1  - Santer, Svetlana
A1  - Hartlieb, Matthias
A1  - Böker, Alexander
T1  - A dual pH- and light-responsive spiropyrane-based surfactant
BT  - investigations on Its switching behavior and remote control over emulsion stability
JF  - Angewandte Chemie : a journal of the Gesellschaft Deutscher Chemiker ; International edition
N2  - A cationic surfactant containing a spiropyrane unit is prepared exhibiting a dual-responsive adjustability of its surface-active characteristics. The switching mechanism of the system relies on the reversible conversion of the non-ionic spiropyrane (SP) to a zwitterionic merocyanine (MC) and can be controlled by adjusting the pH value and via light, resulting in a pH-dependent photoactivity: While the compound possesses a pronounced difference in surface activity between both forms under acidic conditions, this behavior is suppressed at a neutral pH level. The underlying switching processes are investigated in detail, and a thermodynamic explanation based on a combination of theoretical and experimental results is provided. This complex stimuli-responsive behavior enables remote-control of colloidal systems. To demonstrate its applicability, the surfactant is utilized for the pH-dependent manipulation of oil-in-water emulsions.
KW  - Dual-Responsiveness
KW  - Manipulation of Emulsion Stability
KW  - Spiropyrane
KW  - Surfactant
KW  - Switchable Surfactants
KW  - pH-Dependent Photoresponsivity
Y1  - 2022
U6  - https://doi.org/10.1002/anie.202114687
SN  - 1433-7851
SN  - 1521-3773
VL  - 61
IS  - 21
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Katayama, T.
A1  - Anniyev, Toyli
A1  - Beye, Martin
A1  - Coffee, Ryan
A1  - Dell'Angela, M.
A1  - Föhlisch, Alexander
A1  - Gladh, J.
A1  - Kaya, S.
A1  - Krupin, O.
A1  - Nilsson, A.
A1  - Nordlund, D.
A1  - Schlotter, W. F.
A1  - Sellberg, J. A.
A1  - Sorgenfrei, Nomi
A1  - Turner, J. J.
A1  - Wurth, W.
A1  - Öström, H.
A1  - Ogasawara, H.
T1  - Ultrafast soft X-ray emission spectroscopy of surface adsorbates using an X-ray free electron laser
JF  - Journal of electron spectroscopy and related phenomena : the international journal on theoretical and experimental aspects of electron spectroscopy
N2  - We report on an experimental system designed to probe chemical reactions on solid surfaces on a sub-picosecond timescale using soft X-ray emission spectroscopy at the Linac Coherent Light Source (LCLS) free electron laser (FEL) at the SLAC National Accelerator Laboratory. We analyzed the O 1s X-ray emission spectra recorded from atomic oxygen adsorbed on a Ru(0001) surface at a synchrotron beamline (SSRL, BL13-2) and an FEL beamline (LCLS, SXR). We have demonstrated conditions that provide negligible amount of FEL induced damage of the sample. In addition we show that the setup is capable of tracking the temporal evolution of electronic structure during a surface reaction of submonolayer quantities of CO molecules desorbing from the surface.
KW  - X-ray emission spectroscopy
KW  - Surface science
KW  - Free electron laser
KW  - Ultrafast
Y1  - 2013
U6  - https://doi.org/10.1016/j.elspec.2013.03.006
SN  - 0368-2048
VL  - 187
IS  - 1
SP  - 9
EP  - 14
PB  - Elsevier
CY  - Amsterdam
ER  - 
TY  - JOUR
A1  - Brinkmann, Kai Oliver
A1  - Becker, Tim
A1  - Zimmermann, Florian
A1  - Kreusel, Cedric
A1  - Gahlmann, Tobias
A1  - Theisen, Manuel
A1  - Haeger, Tobias
A1  - Olthof, Selina
A1  - Tückmantel, Christian
A1  - Günster, M.
A1  - Maschwitz, Timo
A1  - Göbelsmann, Fabian
A1  - Koch, Christine
A1  - Hertel, Dirk
A1  - Caprioglio, Pietro
A1  - Peña-Camargo, Francisco
A1  - Perdigón-Toro, Lorena
A1  - Al-Ashouri, Amran
A1  - Merten, Lena
A1  - Hinderhofer, Alexander
A1  - Gomell, Leonie
A1  - Zhang, Siyuan
A1  - Schreiber, Frank
A1  - Albrecht, Steve
A1  - Meerholz, Klaus
A1  - Neher, Dieter
A1  - Stolterfoht, Martin
A1  - Riedl, Thomas
T1  - Perovskite-organic tandem solar cells with indium oxide interconnect
JF  - Nature
N2  - Multijunction solar cells can overcome the fundamental efficiency limits of single-junction devices. The bandgap tunability of metal halide perovskite solar cells renders them attractive for multijunction architectures(1). Combinations with silicon and copper indium gallium selenide (CIGS), as well as all-perovskite tandem cells, have been reported(2-5). Meanwhile, narrow-gap non-fullerene acceptors have unlocked skyrocketing efficiencies for organic solar cells(6,7). Organic and perovskite semiconductors are an attractive combination, sharing similar processing technologies. Currently, perovskite-organic tandems show subpar efficiencies and are limited by the low open-circuit voltage (V-oc) of wide-gap perovskite cells(8) and losses introduced by the interconnect between the subcells(9,10). Here we demonstrate perovskite-organic tandem cells with an efficiency of 24.0 per cent (certified 23.1 per cent) and a high V-oc of 2.15 volts. Optimized charge extraction layers afford perovskite subcells with an outstanding combination of high V-oc and fill factor. The organic subcells provide a high external quantum efficiency in the near-infrared and, in contrast to paradigmatic concerns about limited photostability of non-fullerene cells(11), show an outstanding operational stability if excitons are predominantly generated on the non-fullerene acceptor, which is the case in our tandems. The subcells are connected by an ultrathin (approximately 1.5 nanometres) metal-like indium oxide layer with unprecedented low optical/electrical losses. This work sets a milestone for perovskite-organic tandems, which outperform the best p-i-n perovskite single junctions(12) and are on a par with perovskite-CIGS and all-perovskite multijunctions(13).
Y1  - 2022
U6  - https://doi.org/10.1038/s41586-022-04455-0
SN  - 0028-0836
SN  - 1476-4687
VL  - 604
IS  - 7905
SP  - 280
EP  - 286
PB  - Nature Research
CY  - Berlin
ER  -