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    727 research outputs found

    Facile two-step Synthesis of para-Dithienopyrazines [data]

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    N-Heteropolycyclic compounds are valuable building blocks in organic electronic devices. In this work, a convenient route for the synthesis of para-dithienopyrazines from readily available starting materials is described. A cascade of nucleophilic aromatic substitution and subsequent bidirectional hydrothiolation of alkynes was used as a key step. In total, seven new target compounds were synthesized and investigated regarding their photophysical properties. In solution, these molecules act as blue emitters, which turn to green upon addition of an acid, which demonstrates their potential use as proton sensors. Data includes: CV, IR, MS, NMR, UV VIS and XRAY Data for the compounds in the manuscrip

    Bay-Substituted Octaazaperopyrenedioxides as Solid-State Emitters for Strong Light-Matter Coupling [data]

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    Underlying data for all figures in the paper "Bay-Substituted Octaazaperopyrenedioxides as Solid-State Emitters for Strong Light-Matter Coupling." J. Mater. Chem. C 2024, 12, 2745-2755

    LLMs4Implicit-Knowledge-Generation Public

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    Code for equipping pretrained language models (BART, GPT-2, XLNet) with commonsense knowledge for generating implicit knowledge statements between two sentences, by (i) finetuning the models on corpora enriched with implicit information; and by (ii) constraining models with key concepts and commonsense knowledge paths connecting them

    Two-dimensional coherent electronic spectrometer with switchable multi-color configurations [research data]

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    Broadband implementation of two-dimensional electronic spectroscopy (2DES) is a desirable goal for numerous research groups, yet achieving it presents considerable challenges. An effective strategy to mitigate these challenges is the utilization of two-color approaches, effectively broadening the spectral bandwidth accessible with 2DES. Here, we present a simple approach to include multi-color configurations based on adjustable mirror mounts. This enables seamless toggling between single-color, two-color, and transient 2DES within the same spectroscopic apparatus, which is benchmarked on two common laser dyes, Rhodamine 6G and Nile blue. Upon mixing the dyes, single-color 2DES shows overlapping signals, whereas a high selectivity toward Nile blue responses is maintained in two-color and transient 2DES, owing to the fully resonant excitation that is spectrally shifted relative to the detection window. This method is readily implemented in other setups with similar experimental layouts and can be used as a simple solution to overcome existing bandwidth limitations. With the inclusion of transient 2DES, additional insights into excited-state processes can be gained due to its increased sensitivity toward excited-state coherences

    Highly Efficient Photoninitiators Based on 4H-Pyranylidene Derivatives for Two-Photon Laser Printing [data]

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    A series of four donor–acceptor–donor derivatives bearing 4H-pyranylidene and 4-methylcyclohexan-1-one units as donor and acceptor groups respectively is designed, synthesized, and photophysically characterized. Both experimental and theoretical studies reveal good two-photon absorption (2PA) properties for these systems. Decoration of the exocyclic position of the 4H-pyranylidene moiety with a thiophene ring results in high 2PA cross-section values (σ2PA) ≈700 nm, and remarkably, in the region between 900 and 1000 nm. Furthermore, all chromophores are evaluated as photoinitiators (PIs) for two-photon-laser printing at 780 nm, showing superior performance compared to the commonly used commercially available PI, phenylbis(2,4,6-trimethylbenzoyl)phosphine oxide. Among the studied PIs, the ones equipped with a thiophene unit at the exocyclic position of the 4H-pyranylidene moiety exhibit the highest efficiency, enabling fast printing using low laser powers with even lower concentrations of PI. Overall, this study shows the great potential of this new class of PIs for application in the field of 3D nanoprinting

    Knowledge-Enhanced Neural Networks for Machine Reading Comprehension [Source Code and Additional Material]

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    Machine Reading Comprehension is a language understanding task where a system is expected to read a given passage of text and typically answer questions about it. When humans assess the task of reading comprehension, in addition to the presented text, they usually use the knowledge that they already know, such as commonsense and world knowledge, or language skills that they previously acquired - understanding the events and arguments in a text (who did what to whom), their participants and the relation in discourse. In contrast, neural network approaches for machine reading comprehension focused on training end-to-end systems that rely only on annotated task-specific data. In this thesis, we explore approaches for tackling the reading comprehension problem, motivated by how a human would solve the task, using existing background and commonsense knowledge or knowledge from various linguistic tasks. First, we develop a neural reading comprehension model that integrates external commonsense knowledge encoded as a key-value memory. Instead of relying only on document-to-question interaction or discrete features, our model attends to relevant external knowledge and combines this knowledge with the context representation before inferring the answer. This allows the model to attract and imply knowledge from an external knowledge source that is not explicitly stated in the text but is relevant for inferring the answer. We demonstrated that the proposed approach improves the performance of very strong base models for cloze-style reading comprehension and open-book question answering. By including knowledge explicitly, our model can also provide evidence about the background knowledge used in the reasoning process. Further, we examined the impact of transferring linguistic knowledge from low-level linguistic tasks into a reading comprehension system using neural representations. Our experiments show that the knowledge transferred from the neural representations trained on these linguistic tasks can be adapted and combined together to improve the reading comprehension task early in training and when trained with small portions of the data. Last, we propose to use structured linguistic annotations as a basis for a Discourse-Aware Semantic Self-Attention encoder that we employ for reading comprehension of narrative texts. We extract relations between discourse units, events, and their arguments, as well as co-referring mentions, using available annotation tools. The empirical evaluation shows that the investigated structures improve the overall performance (up to +3.4 Rouge-L), especially intra-sentential and cross-sentential discourse relations, sentence-internal semantic role relations, and long-distance coreference relations. We also show that dedicating self-attention heads to intra-sentential relations and relations connecting neighboring sentences is beneficial for finding answers to questions in longer contexts. These findings encourage the use of discourse-semantic annotations to enhance the generalization capacity of self-attention models for machine reading comprehension

    The Enactment of Public Participation in Rulemaking: A Comparative Analysis [Dataset]

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    These are the data for the replication of the statistical analysis in the article "The Enactment of Public Participation in Rulemaking: A Comparative Analysis". The dataset contains time-series (1995-2015) cross-sectional (39 OECD countries) observations, in csv format which was created for the purpose of explaining the adoption of legislations allowing public participation in and judicial review of rulemaking. The corresponding codebook lists the used variables and sources. The replication codes are for Stata

    Band Formation at Interfaces Between N-Heteropolycycles and Gold Electrodes [research data]

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    Underlying data for figures in the paper "Band Formation at Interfaces Between N-Heteropolycycles and Gold Electrodes

    4D Printing of Adaptable “Living” Materials Based on Alkoxyamine Chemistry [data]

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    4D printing has emerged as a powerful strategy capable of revolutionizing additive manufacturing by enabling objects to dynamically transform over time on demand. Despite significant progress, the full potential remains unrealized, particularly in the utilization of dynamic covalent chemistry. This study introduces a new approach using a multifunctional crosslinker with alkoxyamine functionalities for 4D printing. Digital light processing (DLP) has been employed for high-resolution printing of complex objects. Leveraging alkoxyamine bonds' dynamic and living characteristics, the printed structures can be further modified through nitroxide-mediated polymerization (NMP) using styrene and nitroxide exchange reactions (NER). The resulting "living" printed structures exhibit the unique ability to undergo both "growth" and "degrowth", dynamically adapting their size as well as the reduced Young’s Modulus across a wide range (770 kPa to 1.2 GPa). The chain extension by NMP and softening by NER have been carefully characterized by IR and EPR spectroscopy. The presented approach opens avenues for the development of 4D printed structures with complex adaptive systems, showcasing enormous potential in a wide range of fields

    Nicodemus Frischlin, Korrespondenz

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    Das Ziel des Projektes besteht darin, die gesamte handschriftlich und (in kleinen Teilen) gedruckt überlieferte Korrespondenz des Späthumanisten Nicodemus Frischlin (1547-1590) kritisch zu edieren sowie durch Regesten und Kommentare zu erschließen. Damit wird nicht nur ein zentraler Teil der Produktion eines wichtigen Autors der deutschen Literatur- und Kulturgeschichte zugänglich gemacht; vielmehr werden darüber hinaus zeittypische Konkurrenz- und Ausschließungsmuster im Zusammenprall höfischer, akademischer und genuin ‚humanistischer’ Interessen zur Zeit des Übergangs von ständischer zu frühabsolutistischer Herrschaftsform bzw. im Kontext der beginnenden Legitimationskrise althumanistischer Lebensentwürfe an einem gut dokumentierten, repräsentativen Einzelfall freigelegt. Die Briefe stammen aus dem Zeitraum von 1568 bis 1590. Da Frischlin keinen Briefnachlass hinterlassen hat, ist er mit 351 Schreiben der häufigste Absender, häufigster Adressat ist mit 77 Schreiben Herzog Ludwig von Württemberg, weitere 56 Schreiben gingen an Vertreter des Stuttgarter Hofs. 71 Schreiben gingen an die Gremien und Mitglieder der Universität Tübingen, 65 an auswärtige Gelehrte. 49 Briefe betreffen auswärtige Autoritäten und 24 Briefe Mitglieder von Frischlins Familie

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