Publications

@article{nokey,

title = {Scalable Fabrication of Metallic Nanogaps at the Sub-10 nm Level},

author = {S Luo and B H Hoff and S A Maier and J C De Mello},

doi = {10.1002/advs.202102756},

issn = {2198-3844},

year  = {2021},

date = {2021-10-31},

journal = {Adv Sci (Weinh)},

pages = {e2102756},

abstract = {Metallic nanogaps with metal-metal separations of less than 10 nm have many applications in nanoscale photonics and electronics. However, their fabrication remains a considerable challenge, especially for applications that require patterning of nanoscale features over macroscopic length-scales. Here, some of the most promising techniques for nanogap fabrication are evaluated, covering established technologies such as photolithography, electron-beam lithography (EBL), and focused ion beam (FIB) milling, plus a number of newer methods that use novel electrochemical and mechanical means to effect the patterning. The physical principles behind each method are reviewed and their strengths and limitations for nanogap patterning in terms of resolution, fidelity, speed, ease of implementation, versatility, and scalability to large substrate sizes are discussed.},

keywords = {Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Abiotic Formation of an Amide Bond via Surface-Supported Direct Carboxyl\textendashAmine Coupling},

author = {B Yang and K Niu and F Haag and N Cao and J Zhang and H Zhang and Q Li and F Allegretti and J Bj\"{o}rk and J V Barth and L Chi},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202113590},

doi = {https://doi.org/10.1002/anie.202113590},

issn = {1433-7851},

year  = {2021},

date = {2021-10-28},

journal = {Angewandte Chemie International Edition},

volume = {61},

number = {5},

pages = {e202113590},

abstract = {Abstract Amide bond formation is one of the most important reactions in biochemistry, notably being of crucial importance for the origin of life. Herein, we combine scanning tunneling microscopy and X-ray photoelectron spectroscopy studies to provide evidence for thermally activated abiotic formation of amide bonds between adsorbed precursors through direct carboxyl\textendashamine coupling under ultrahigh-vacuum conditions by means of on-surface synthesis. Complementary insights from temperature-programmed desorption measurements and density functional theory calculations reveal the competition between cross-coupling amide formation and decarboxylation reactions on the Au(111) surface. Furthermore, we demonstrate the critical influence of the employed metal support: whereas on Au(111) the coupling readily occurs, different reaction scenarios prevail on Ag(111) and Cu(111). The systematic experiments signal that archetypical bio-related molecules can be abiotically synthesized in clean environments without water or oxygen.},

keywords = {Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Bifurcations of Clusters and Collective Oscillations in Networks of Bistable Units},

author = {M Salman and C Bick and K Krischer},

year  = {2021},

date = {2021-10-28},

journal = {arXiv preprint arXiv:2110.15004},

abstract = {We investigate dynamics and bifurcations in a mathematical model that captures electrochemical experiments on arrays of microelectrodes. In isolation, each individual microelectrode is described by a one-dimensional unit with a bistable current-potential response. When an array of such electrodes is coupled by controlling the total electric current, the common electric potential of all electrodes oscillates in some interval of the current. These coupling-induced collective oscillations of bistable one-dimensional units are captured by the model. Moreover, any equilibrium is contained in a cluster subspace, where the electrodes take at most three distinct states. We systematically analyze the dynamics and bifurcations of the model equations: We consider the dynamics on cluster subspaces of successively increasing dimension and analyze the bifurcations occurring therein. Most importantly, the system exhibits an equivariant transcritical bifurcation of limit cycles. From this bifurcation, several limit cycles branch, one of which is stable for arbitrarily many bistable units.},

keywords = {Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Metasurface Photoelectrodes for Enhanced Solar Fuel Generation},

author = {L H\"{u}ttenhofer and M Golibrzuch and O Bienek and F J Wendisch and R Lin and M Becherer and I D Sharp and S A Maier and E Cort\'{e}s},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202102877},

doi = {https://doi.org/10.1002/aenm.202102877},

issn = {1614-6832},

year  = {2021},

date = {2021-10-27},

journal = {Advanced Energy Materials},

volume = {11},

number = {46},

pages = {2102877},

abstract = {Abstract Tailoring optical properties in photocatalysts by nanostructuring them can help increase solar light harvesting efficiencies in a wide range of materials. Whereas plasmon resonances are widely employed in metallic catalysts for this purpose, latest advances of nonradiative, dielectric nanophotonics also enable light confinement and enhanced visible light absorption in semiconductors. Here, a design procedure for large-scale nanofabrication of semiconductor photoelectrodes using imprint lithography is developed. Anapole excitations and metasurface lattice resonances are combined to enhance the absorption of the model material, amorphous gallium phosphide (a-GaP), over the visible spectrum. It is shown that cost-effective, high sample throughput is achieved while retaining the precise signature of the engineered photonic states. Photoelectrochemical measurements under hydrogen evolution reaction conditions and sunlight illumination reveal the contributions of the respective resonances and demonstrate an overall photocurrent enhancement of 5.7, compared to a planar film. These results are supported by optical and numerical analysis of single nanodisks and of the upscaled metasurface.},

keywords = {Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Biopolymer-Templated Deposition of Ordered and Polymorph Titanium Dioxide Thin Films for Improved Surface-Enhanced Raman Scattering Sensitivity},

author = {Q Chen and M Betker and C Harder and C J Brett and M Schwartzkopf and N M Ulrich and M E Toimil-Molares and C Trautmann and L D S\"{o}derberg and C L Weindl and V K\"{o}rstgens and P M\"{u}ller-Buschbaum and M Ma and S V Roth},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202108556},

doi = {https://doi.org/10.1002/adfm.202108556},

issn = {1616-301X},

year  = {2021},

date = {2021-10-27},

journal = {Adv. Funct. Mater.},

volume = {n/a},

number = {n/a},

pages = {2108556},

abstract = {Abstract Titanium dioxide (TiO2) is an excellent candidate material for semiconductor metal oxide-based substrates for surface-enhanced Raman scattering (SERS). Biotemplated fabrication of TiO2 thin films with a 3D network is a promising route for effectively transferring the morphology and ordering of the template into the TiO2 layer. The control over the crystallinity of TiO2 remains a challenge due to the low thermal stability of biopolymers. Here is reported a novel strategy of the cellulose nanofibril (CNF)-directed assembly of TiO2/CNF thin films with tailored morphology and crystallinity as SERS substrates. Polymorphous TiO2/CNF thin films with well-defined morphology are obtained by combining atomic layer deposition and thermal annealing. A high enhancement factor of 1.79 × 106 in terms of semiconductor metal oxide nanomaterial (SMON)-based SERS substrates is obtained from the annealed TiO2/CNF thin films with a TiO2 layer thickness of 10 nm fabricated on indium tin oxide (ITO), when probed by 4-mercaptobenzoic acid molecules. Common SERS probes down to 10 nm can be detected on these TiO2/CNF substrates, indicating superior sensitivity of TiO2/CNF thin films among SMON SERS substrates. This improvement in SERS sensitivity is realized through a cooperative modulation of the template morphology of the CNF network and the crystalline state of TiO2.},

keywords = {Foundry Inorganic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Bimolecular Generation of Excitonic Luminescence from Dark Photoexcitations in Ruddlesden\textendashPopper Hybrid Metal-Halide Perovskites},

author = {M Nuber and D Sandner and T Neumann and R Kienberger and F Deschler and H Iglev},

url = {https://doi.org/10.1021/acs.jpclett.1c03099},

doi = {10.1021/acs.jpclett.1c03099},

year  = {2021},

date = {2021-10-21},

journal = {The Journal of Physical Chemistry Letters},

volume = {12},

number = {42},

pages = {10450-10456},

abstract = {The nature of photoexcitations in Ruddlesden\textendashPopper (RP) hybrid metal halide perovskites is still under debate. While the high exciton binding energy in the hundreds of millielectronvolts indicates excitons as the primary photoexcitations, recent reports found evidence for dark, Coulombically screened populations, which form via strong coupling of excitons and the atomic lattice. Here, we use time-resolved mid-infrared spectroscopy to gain insights into the nature and recombination of such dark excited states in (BA)2(MA)n−1PbnI3n+1 (n = 1,2,3) via their intraband electronic absorption. In stark contrast to results in the bulk perovskites, all samples exhibit a broad, unstructured mid-IR photoinduced absorbance with no infrared activated modes, independent of excitonic confinement. Further, the recombination dynamics are dominated by a bimolecular process. In combination with steady-state photoluminescence experiments, we conclude that screened, dark photoexcitations act as a population reservoir in the RP hybrid perovskites, from which nongeminate formation of bright excitons precedes generation of photoluminescence.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Water jet space charge spectroscopy: Route to direct measurement of electron dynamics for organic systems in their natural environment},

author = {M Mittermair and F Martin and M W\"{o}rle and D Blo\ss and A Duensing and R Kienberger and A Hans and H Iglev and A Knie and W Helml},

year  = {2021},

date = {2021-10-19},

journal = {arXiv preprint arXiv:2110.10044},

abstract = {The toolbox for time-resolved direct measurements of electron dynamics covers a variety of methods. Since the experimental effort is increasing rapidly with achievable time resolution, there is an urge for simple and robust measurement techniques. Within this paper prove of concept experiments and numerical simulations are utilized to investigate the applicability of a new setup for the generation of ultrashort electron pulses in the energy range of 300 eV up to 1.6 keV. The experimental approach combines an in-vacuum liquid microjet and a few-cycle femtosecond laser system, while the threshold for electron impact ionization serves as a gate for the effective electron pulse duration. The experiments prove that electrons in the keV regime are accessible and that the electron spectrum can be easily tuned by laser intensity and focal position alignment with respect to the water jet. Numerical simulations show that a sub-picosecond temporal resolution is achievable.},

keywords = {Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Tip Coupling and Array Effects of Gold Nanoantennas in Near-Field Microscopy},

author = {R B\"{u}chner and T Weber and L K\"{u}hner and S A Maier and A Tittl},

url = {https://doi.org/10.1021/acsphotonics.1c00744},

doi = {10.1021/acsphotonics.1c00744},

year  = {2021},

date = {2021-10-14},

journal = {ACS Photonics},

abstract = {Scattering-type scanning near-field optical microscopy (s-SNOM) is one of the predominant techniques for the nanoscale characterization of optical properties. The optical response of nanoantennas in s-SNOM is highly sensitive to their environment, including influences of the probing tip or neighboring resonators. Dielectric tips are commonly employed to minimize tip-related perturbations, although they provide a comparatively weak scattering signal. Here we show that when using metallic tips, it is possible to select between distinct weak and strong tip\textendashantenna coupling regimes by careful tailoring of the illumination conditions and resonator orientation. This enables the use of highly scattering metallic instead of dielectric tips for mapping plasmonic modes with comparatively higher signal strengths. This is a particular advantage for the retrieval of near-field spectra, which simultaneously require high near-field signals and unperturbed field patterns. We leverage our approach to analyze the collective effects of nanoantenna arrays, phenomena that are well understood in the optical far-field but have not been extensively studied in the near-field. Probing the dependence of the optical response on the array field size, we identify three regimes: the single rod regime, the intermediate regime, and the array-like regime. We show that these array effects give rise to characteristic spectral features originating from a complex interplay of radiative coupling and plasmon hybridization. These results provide evidence that long-range interactions of antennas also influence the local optical response that is probed in s-SNOM and demonstrate how collective resonances emerge from single building blocks, providing guidelines for optimized array designs for near- and far-field applications.},

keywords = {Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {On the origin of chirality in plasmonic meta-molecules},

author = {K Martens and T Funck and E Y Santiago and A O Govorov and S Burger and T Liedl},

url = {https://arxiv.org/abs/2110.06689},

doi = {arXiv:2110.06689v2},

year  = {2021},

date = {2021-10-13},

journal = {arXiv preprint arXiv:2110.06689},

abstract = {Chirality is a fundamental feature in all domains of nature, ranging from particle physics over electromagnetism to chemistry and biology. Chiral objects lack a mirror plane and inversion symmetry and therefore cannot be spatially aligned with their mirrored counterpart, their enantiomer. Both natural molecules and artificial chiral nanostructures can be characterized by their light-matter interaction, which is reflected in circular dichroism (CD). Using DNA origami, we assemble model meta-molecules from multiple plasmonic nanoparticles, representing meta-atoms accurately positioned in space. This allows us to reconstruct piece by piece the impact of varying macromolecular geometries on their surrounding optical near fields. Next to the emergence of CD signatures in the instance that we architect a third dimension, we design and implement sign flipping signals through addition or removal of single particles in the artificial molecules. Our data and theoretical modelling reveal the hitherto unrecognized phenomenon of chiral plasmonic-dielectric coupling, explaining the intricate electromagnetic interactions within hybrid DNA-based plasmonic nanostructures.},

keywords = {Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A Multi-Layer Device for Light-Triggered Hydrogen Production from Alkaline Methanol},

author = {Y Wang and E-P Yao and L Wu and J Feldmann and J K Stolarczyk},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202109979},

doi = {https://doi.org/10.1002/anie.202109979},

issn = {1433-7851},

year  = {2021},

date = {2021-10-13},

journal = {Angewandte Chemie International Edition},

volume = {60},

number = {51},

pages = {26694-26701},

abstract = {Abstract It usually requires high temperature and high pressure to reform methanol with water to hydrogen with high turnover frequency (TOF). Here we show that hydrogen can be produced from alkaline methanol on a light-triggered multi-layer system with a very high hydrogen evolution rate up to ca. 1 μmol s−1 under the illumination of a standard Pt-decorated carbon nitride. The system can achieve a remarkable TOF up to 1.8×106 moles of hydrogen per mole of Pt per hour under mild conditions. The total turnover number (TTN) of 470 000 measured over 38 hours is among the highest reported. The system does not lead to any COx emissions, hence it could feed clean hydrogen to fuel cells. In contrast to a slurry system, the proposed multi-layer system avoids particle aggregation and effectively uses light and Pt active sites. The performance is also attributed to the light-triggered reforming of alkaline methanol. This notable performance is a promising step toward practical light-driven hydrogen generation.},

keywords = {Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A self-healing catalyst for electrocatalytic and photoelectrochemical oxygen evolution in highly alkaline conditions},

author = {C Feng and F Wang and Z Liu and M Nakabayashi and Y Xiao and Q Zeng and J Fu and Q Wu and C Cui and Y Han and N Shibata and K Domen and I D Sharp and Y Li},

url = {https://doi.org/10.1038/s41467-021-26281-0},

doi = {10.1038/s41467-021-26281-0},

issn = {2041-1723},

year  = {2021},

date = {2021-10-13},

journal = {Nature Communications},

volume = {12},

number = {1},

pages = {5980},

abstract = {While self-healing is considered a promising strategy to achieve long-term stability for oxygen evolution reaction (OER) catalysts, this strategy remains a challenge for OER catalysts working in highly alkaline conditions. The self-healing of the OER-active nickel iron layered double hydroxides (NiFe-LDH) has not been successful due to irreversible leaching of Fe catalytic centers. Here, we investigate the introduction of cobalt (Co) into the NiFe-LDH as a promoter for in situ Fe redeposition. An active borate-intercalated NiCoFe-LDH catalyst is synthesized using electrodeposition and shows no degradation after OER tests at 10 mA cm−2 at pH 14 for 1000 h, demonstrating its self-healing ability under harsh OER conditions. Importantly, the presence of both ferrous ions and borate ions in the electrolyte is found to be crucial to the catalyst’s self-healing. Furthermore, the implementation of this catalyst in photoelectrochemical devices is demonstrated with an integrated silicon photoanode. The self-healing mechanism leads to a self-limiting catalyst thickness, which is ideal for integration with photoelectrodes since redeposition is not accompanied by increased parasitic light absorption.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {The Flexible On-Surface Self-Assembly of a Low-Symmetry Mabiq Ligand: An Unconventional Metal-Assisted Phase Transformation on Ag(111)},

author = {F Haag and P S Deimel and P Knecht and L Niederegger and K Seufert and M G. Cuxart and Y Bao and A C Papageorgiou and M Muntwiler and W Auw\"{a}rter and C R Hess and J V Barth and F Allegretti},

url = {https://doi.org/10.1021/acs.jpcc.1c07400},

doi = {10.1021/acs.jpcc.1c07400},

issn = {1932-7447},

year  = {2021},

date = {2021-10-12},

journal = {The Journal of Physical Chemistry C},

volume = {125},

number = {42},

pages = {23178-23191},

abstract = {The self-assembly of metal\textendashorganic complexes and networks of increasing complexity on solid surfaces is important for their application in a variety of fields, such as catalysis, sensing, and molecular magnetism. Here, we have selected a low-symmetry, free-base macrocyclic biquinazoline ligand, H-Mabiq, which upon metalation has the potential to incorporate cations in two different coordination sites, affording multi-valency and multi-electron transfer capacity. We show that H-Mabiq molecules readily self-assemble onto the Ag(111) surface at room temperature, forming a well-ordered monolayer of closely packed molecules. Upon increasing the temperature, a new phase with a different long-range order and molecular packing is obtained. By means of scanning tunneling microscopy and photoelectron spectroscopy, we show that this new phase is characterized by a distinctive silver-bridged dimeric motif, entailing a Ag adatom accommodated at the peripheral coordination site of two opposing H-Mabiq molecules. Thus, the present work reveals the ability of the bio-inspired Mabiq ligands to form surface-confined two-dimensional assemblies incorporating metal adatoms. The results bode promise for the use of metal-containing Mabiq compounds to engineer regular bimetallic arrays with atomic precision.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A Critical Outlook for the Pursuit of Lower Contact Resistance in Organic Transistors},

author = {J W Borchert and R T Weitz and S Ludwigs and H Klauk},

doi = {10.1002/adma.202104075},

issn = {0935-9648},

year  = {2021},

date = {2021-10-07},

journal = {Adv Mater},

pages = {e2104075},

abstract = {To take full advantage of recent and anticipated improvements in the performance of organic semiconductors employed in organic transistors, the high contact resistance arising at the interfaces between the organic semiconductor and the source and drain contacts must be reduced significantly. To date, only a small portion of the accumulated research on organic thin-film transistors (TFTs) has reported channel-width-normalized contact resistances below 100 Ωcm, well above what is regularly demonstrated in transistors based on inorganic semiconductors. A closer look at these cases and the relevant literature strongly suggests that the most significant factor leading to the lowest contact resistances in organic TFTs so far has been the control of the thin-film morphology of the organic semiconductor. By contrast, approaches aimed at increasing the charge-carrier density and/or reducing the intrinsic Schottky barrier height have so far played a relatively minor role in achieving the lowest contact resistances. Herein, the possible explanations for these observations are explored, including the prevalence of Fermi-level pinning and the difficulties in forming optimized interfaces with organic semiconductors. An overview of the research on these topics is provided, and potential device-engineering solutions are discussed based on recent advancements in the theoretical and experimental work on both organic and inorganic semiconductors.},

keywords = {Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Targetable Conformationally Restricted Cyanines Enable Photon-Count-Limited Applications**},

author = {P Eiring and R Mclaughlin and S S Matikonda and Z Han and L Grabenhorst and D A Helmerich and M Meub and G Beliu and M Luciano and V Bandi and N Zijlstra and Z-D Shi and S G Tarasov and R Swenson and P Tinnefeld and V Glembockyte and T Cordes and M Sauer and M J Schnermann},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202109749},

doi = {https://doi.org/10.1002/anie.202109749},

issn = {1433-7851},

year  = {2021},

date = {2021-10-04},

urldate = {2021-10-04},

journal = {Angewandte Chemie International Edition},

volume = {60},

number = {51},

pages = {26685-26693},

abstract = {Abstract Cyanine dyes are exceptionally useful probes for a range of fluorescence-based applications, but their photon output can be limited by trans-to-cis photoisomerization. We recently demonstrated that appending a ring system to the pentamethine cyanine ring system improves the quantum yield and extends the fluorescence lifetime. Here, we report an optimized synthesis of persulfonated variants that enable efficient labeling of nucleic acids and proteins. We demonstrate that a bifunctional sulfonated tertiary amide significantly improves the optical properties of the resulting bioconjugates. These new conformationally restricted cyanines are compared to the parent cyanine derivatives in a range of contexts. These include their use in the plasmonic hotspot of a DNA-nanoantenna, in single-molecule F\"{o}rster-resonance energy transfer (FRET) applications, far-red fluorescence-lifetime imaging microscopy (FLIM), and single-molecule localization microscopy (SMLM). These efforts define contexts in which eliminating cyanine isomerization provides meaningful benefits to imaging performance.},

keywords = {Foundry Inorganic, Foundry Organic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Tunable 2D Group-III Metal Alloys},

author = {S Rajabpour and A Vera and W He and B N Katz and R J Koch and M Lassauni\`{e}re and X Chen and C Li and K Nisi and H El-Sherif and M T Wetherington and C Dong and A Bostwick and C Jozwiak and A C T Van Duin and N Bassim and J Zhu and G-C Wang and U Wurstbauer and E Rotenberg and V Crespi and S Y Quek and J A Robinson},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.202104265},

doi = {https://doi.org/10.1002/adma.202104265},

issn = {0935-9648},

year  = {2021},

date = {2021-10-04},

journal = {Advanced Materials},

volume = {33},

number = {44},

pages = {2104265},

abstract = {Abstract Chemically stable quantum-confined 2D metals are of interest in next-generation nanoscale quantum devices. Bottom-up design and synthesis of such metals could enable the creation of materials with tailored, on-demand, electronic and optical properties for applications that utilize tunable plasmonic coupling, optical nonlinearity, epsilon-near-zero behavior, or wavelength-specific light trapping. In this work, it is demonstrated that the electronic, superconducting, and optical properties of air-stable 2D metals can be controllably tuned by the formation of alloys. Environmentally robust large-area 2D-InxGa1−x alloys are synthesized byConfinement Heteroepitaxy (CHet). Near-complete solid solubility is achieved with no evidence of phase segregation, and the composition is tunable over the full range of x by changing the relative elemental composition of the precursor. The optical and electronic properties directly correlate with alloy composition, wherein the dielectric function, band structure, superconductivity, and charge transfer from the metal to graphene are all controlled by the indium/gallium ratio in the 2D metal layer.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Ion Dynamics and Polymorphism in Cu20Te11Cl3},

author = {A Vogel and T Nilges},

url = {https://doi.org/10.1021/acs.inorgchem.1c01764},

doi = {10.1021/acs.inorgchem.1c01764},

issn = {0020-1669},

year  = {2021},

date = {2021-10-04},

journal = {Inorganic Chemistry},

volume = {60},

number = {20},

pages = {15233-15241},

abstract = {Coinage metal polychalcogenide halides are an intriguing class of materials, and many representatives are solid ion conductors and thermoelectric materials. The materials show high ion mobility, polymorphism, and various attractive interactions in the cation and anion substructures. Especially the latter feature leads to complex electronic structures and the occurrence of charge-density waves (CDWs) and, as a result, the first p\textendashn\textendashp switching materials. During our systematic investigations for new p\textendashn\textendashn switching materials in the Cu\textendashTe\textendashCl phase diagram, we were able to isolate polymorphic Cu20Te11Cl3, which we characterized structurally and with regard to its electronic and thermoelectric properties. Cu20Te11Cl3 is trimorphic, with phase transitions occurring at 288 and 450 K. The crystal structures of two polymorphs, the α phase, stable above 450 K, and the β polymorph (288\textendash450 K), are reported, and the complex structure chemistry featuring twinning upon a phase change is illustrated. We identified a dynamic cation substructure and a static anion substructure for all polymorphs, characterizing Cu20Te11Cl3 as a solid Cu-ion conductor. Temperature-dependent measurements of the Seebeck coefficient and total conductivity were performed and substantiated a linear response of the Seebeck coefficient, a lack of CDWs, and no p\textendashn\textendashp switching. Reasons for a lack of CDWs in Cu20Te11Cl3 are discussed and illustrated in the context of existing p\textendashn\textendashp switching materials.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Dark and Bright Excitons in Halide Perovskite Nanoplatelets},

author = {M Gramlich and M W Swift and C Lampe and M D\"{o}blinger and J L Lyons and A L Efros and P C Sercel and A S Urban},

year  = {2021},

date = {2021-10-01},

journal = {arXiv preprint arXiv},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Degradation mechanisms of perovskite solar cells under vacuum and one atmosphere of nitrogen},

author = {R Guo and D Han and W Chen and L Dai and K Ji and Q Xiong and S Li and L K Reb and M A Scheel and S Pratap and N Li and S Yin and T Xiao and S Liang and A L Oechsle and C L Weindl and M Schwartzkopf and H Ebert and P Gao and K Wang and M Yuan and N C Greenham and S D Stranks and S V Roth and R H Friend and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1038/s41560-021-00912-8},

doi = {10.1038/s41560-021-00912-8},

issn = {2058-7546},

year  = {2021},

date = {2021-10-01},

urldate = {2021-10-01},

journal = {Nature Energy},

volume = {6},

number = {10},

pages = {977-986},

abstract = {Extensive studies have focused on improving the operational stability of perovskite solar cells, but few have surveyed the fundamental degradation mechanisms. One aspect overlooked in earlier works is the effect of the atmosphere on device performance during operation. Here we investigate the degradation mechanisms of perovskite solar cells operated under vacuum and under a nitrogen atmosphere using synchrotron radiation-based operando grazing-incidence X-ray scattering methods. Unlike the observations described in previous reports, we find that light-induced phase segregation, lattice shrinkage and morphology deformation occur under vacuum. Under nitrogen, only lattice shrinkage appears during the operation of solar cells, resulting in better device stability. The different behaviour under nitrogen is attributed to a larger energy barrier for lattice distortion and phase segregation. Finally, we find that the migration of excessive PbI2 to the interface between the perovskite and the hole transport layer degrades the performance of devices under vacuum or under nitrogen.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Two-dimensional MOF-based liquid marbles: surface energy calculations and efficient oil\textendashwater separation using a ZIF-9-III@PVDF membrane},

author = {H Saini and P Kallem and E Otyepkov\'{a} and F Geyer and A Schneemann and V Ranc and F Banat and R Zbo\v{r}il and M Otyepka and R A Fischer and K Jayaramulu},

url = {http://dx.doi.org/10.1039/D1TA05835E},

doi = {10.1039/D1TA05835E},

issn = {2050-7488},

year  = {2021},

date = {2021-09-30},

journal = {Journal of Materials Chemistry A},

volume = {9},

number = {41},

pages = {23651-23659},

abstract = {Superhydrophobic MOF-nanosheets assembled on the outside of an aqueous droplet form ‘liquid marbles’. A facile mechanochemical-based synthesis followed by ultrasonication was used to prepare two-dimensional superhydrophobic\textendasholeophilic MOF nanosheets of a Co2+-based zeolitic imidazolate framework, namely ZIF-9-III ([Co4(bIm)16] with bIm− = benzimidazolate). The resulting ZIF-9-III showed excellent hydrophobicity (advancing water contact angle of 144°) and oleophilicity (oil contact angle of ≈0°). The superhydrophobic behavior originated from its predominant outer (002) surface, which featured nanoscale corrugation caused by the exposed benzimidazole groups. This behavior was corroborated by inverse gas chromatography measurements to determine the surface energies of bulk exfoliated 2D ZIF-9-III nanosheets and 3D ZIF-9-I. Taking advantage of the unique surface properties, including low surface energy and good moisture stability, we prepared ZIF-9-III@PVDF (PVDF = polyvinylidene fluoride) membranes following the non-solvent induced phase inversion (NIPS) process. The resulting membranes were exploited in real-time oil/water separation and featured remarkably high adsorption capacity and anti-staining properties. Therefore, this work opens the door to developing new superhydrophobic MOF-based composite materials with permeant porosity, which may enable applications in self-cleaning membranes for oil\textendashwater separation.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Role of Polycyclic Aromatic Alkylammonium Cations in Tuning the Electronic Properties and Band Alignment of Two-Dimensional Hybrid Perovskite Semiconductors},

author = {D Han and S Chen and M-H Du},

url = {https://doi.org/10.1021/acs.jpclett.1c02603},

doi = {10.1021/acs.jpclett.1c02603},

year  = {2021},

date = {2021-09-30},

journal = {The Journal of Physical Chemistry Letters},

volume = {12},

number = {40},

pages = {9754-9760},

abstract = {Two-dimensional hybrid organic\textendashinorganic perovskites (HOIPs) have recently drawn intense attention as potential photovoltaic materials. However},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {The Effect of Photoinduced Surface Oxygen Vacancies on the Charge Carrier Dynamics in TiO2 Films},

author = {O E Dagdeviren and D Glass and R Sapienza and E Cort\'{e}s and S A Maier and I P Parkin and P Gr\"{u}tter and R Quesada-Cabrera},

url = {https://doi.org/10.1021/acs.nanolett.1c02853},

doi = {10.1021/acs.nanolett.1c02853},

issn = {1530-6984},

year  = {2021},

date = {2021-09-28},

journal = {Nano Letters},

volume = {21},

number = {19},

pages = {8348-8354},

abstract = {Metal-oxide semiconductors (MOS) are widely utilized for catalytic and photocatalytic applications in which the dynamics of charged carriers (e.g., electrons, holes) play important roles. Under operation conditions, photoinduced surface oxygen vacancies (PI-SOV) can greatly impact the dynamics of charge carriers. However, current knowledge regarding the effect of PI-SOV on the dynamics of hole migration in MOS films, such as titanium dioxide, is solely based upon volume-averaged measurements and/or vacuum conditions. This limits the basic understanding of hole-vacancy interactions, as they are not capable of revealing time-resolved variations during operation. Here, we measured the effect of PI-SOV on the dynamics of hole migration using time-resolved atomic force microscopy. Our findings demonstrate that the time constant associated with hole migration is strongly affected by PI-SOV, in a reversible manner. These results will nucleate an insightful understanding of the physics of hole dynamics and thus enable emerging technologies, facilitated by engineering hole-vacancy interactions.},

keywords = {Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating},

author = {S Pratap and F Babbe and N S Barchi and Z Yuan and T Luong and Z Haber and T-B Song and J L Slack and C V Stan and N Tamura and C M Sutter-Fella and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1038/s41467-021-25898-5},

doi = {10.1038/s41467-021-25898-5},

issn = {2041-1723},

year  = {2021},

date = {2021-09-24},

journal = {Nature Communications},

volume = {12},

number = {1},

pages = {5624},

abstract = {Complex phenomena are prevalent during the formation of materials, which affect their processing-structure-function relationships. Thin films of methylammonium lead iodide (CH3NH3PbI3, MAPI) are processed by spin coating, antisolvent drop, and annealing of colloidal precursors. The structure and properties of transient and stable phases formed during the process are reported, and the mechanistic insights of the underlying transitions are revealed by combining in situ data from grazing-incidence wide-angle X-ray scattering and photoluminescence spectroscopy. Here, we report the detailed insights on the embryonic stages of organic-inorganic perovskite formation. The physicochemical evolution during the conversion proceeds in four steps: i) An instant nucleation of polydisperse MAPI nanocrystals on antisolvent drop, ii) the instantaneous partial conversion of metastable nanocrystals into orthorhombic solvent-complex by cluster coalescence, iii) the thermal decomposition (dissolution) of the stable solvent-complex into plumboiodide fragments upon evaporation of solvent from the complex and iv) the formation (recrystallization) of cubic MAPI crystals in thin film.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Real-time observation of nucleation and growth of Au on CdSe quantum dot templates},

author = {N Paul and J Huang and C Liu and T Lin and C Ouyang and Z Liu and C Chen and Z Chen and Z Weng and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum and A Paul},

url = {https://doi.org/10.1038/s41598-021-97485-z},

doi = {10.1038/s41598-021-97485-z},

issn = {2045-2322},

year  = {2021},

date = {2021-09-21},

journal = {Scientific Reports},

volume = {11},

number = {1},

pages = {18777},

abstract = {Semiconductor quantum dot (QD) arrays can be useful for optical devices such as lasers, solar cells and light-emitting diodes. As the size distribution influences the band-gap, it is worthwhile to investigate QDs prepared using different solvents because each of them could influence the overall morphology differently, depending on the ligand network around individual QDs. Here, we follow the nucleation and growth of gold (Au) on CdSe QD arrays to investigate the influence of surface ligands and thereby realized interparticle distance between QDs on Au growth behaviour. We particularly emphasize on the monolayer stage as the Au decoration on individual QDs is expected at this stage. Therefore, we sputter-deposit Au on each QD array to investigate the morphological evolution in real-time using time-resolved grazing-incidence small-angle X-ray scattering (GISAXS). The growth kinetics - independent of the template - signifies that the observed template-mediated nucleation is limited only to the very first few monolayers. Delicate changes in the Au growth morphology are seen in the immediate steps following the initial replicated decoration of the QD arrays. This is followed by a subsequent clustering and finally a complete Au coverage of the QD arrays.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Non-Local Exciton-Photon Interactions in Hybrid High-Q Nanocavities with Embedded hBN-Encapsulated MoS2 Monolayers},

author = {C Qian and V Villafa\~{n}e and P Soubelet and A H\"{o}tger and T Taniguchi and K Watanabe and N P Wilson and A V Stier and A W Holleitner and J J Finley},

url = {https://arxiv.org/abs/2107.04387},

doi = {arXiv:2107.04387v2},

year  = {2021},

date = {2021-09-20},

journal = {arXiv preprint arXiv:2107.04387},

abstract = {Atomically thin semiconductors can be readily integrated into a wide range of nanophotonic architectures for applications in quantum photonics and novel optoelectronic devices. We report the observation of non-local interactions of textitfree trions in pristine hBN/MoS2/hBN heterostructures coupled to single mode (Q \>104) quasi 0D nanocavities. The high excitonic and photonic quality of the interaction system stem from our integrated nanofabrication approach simultaneously with the hBN encapsulation and the maximized local cavity field amplitude within the MoS2 monolayer. We observe a non-monotonic temperature dependence of the cavity-trion interaction strength, consistent with the non-local light-matter interactions in which the free trion diffuse over lengthscales comparable to the cavity mode volume. Our approach can be generalized to other optically active 2D materials, opening the way towards harnessing novel light-matter interaction regimes for applications in quantum photonics.},

keywords = {Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Luminescent perovskite nanocrystal composites via in situ ligand polymerization towards display applications},

author = {J Zhou and F Fang and W Chen and M Mei and P Liu and J Hao and H Tang and S Liang and W Lei and R Pan and J Cheng and P M\"{u}ller-Buschbaum and X W Sun and W Cao and K Zheng and K Wang},

url = {http://dx.doi.org/10.1039/D1TC03775G},

doi = {10.1039/D1TC03775G},

issn = {2050-7526},

year  = {2021},

date = {2021-09-17},

journal = {Journal of Materials Chemistry C},

volume = {9},

number = {41},

pages = {14740-14748},

abstract = {Luminescent inorganic perovskite nanocrystals (PeNCs) are promising in various optical applications, particularly in advanced lighting and displays. The instability of PeNCs and PeNC composites from different aspects hinder their practical applications. Many previous methods indicate that an intact and facile wrapping strategy could effectively address this challenge. In this work, we introduce an in situ ligand polymerization (ILP) method for the fabrication of PeNC composites. By introducing (3-aminopropyl)triethoxysilane (APTES) as the initial ligand of the PeNCs directly and polymethylhydrosiloxane (PMHS) as the monomer to form the polymerized matrix, a polymerized and hydrophobic SiO2 matrix structure is formed, which intrinsically protects the PeNCs against moisture-induced deterioration. The stability test indicates that the ILP composite powders demonstrate an improved stability against various solvent conditions and light exposure compared to the conventional PeNCs\textendashSiO2 composite. More importantly, the ILP composite exhibits an excellent compatibility with the acrylate solvent which is widely used for light-solidification in light converting film fabrication. The ILP composite film demonstrates an ultrastable operational performance in our standard test outperforming the conventional PeNCs\textendashSiO2 composite configuration. Thus, the ILP composite demonstrates great potential for use in advanced lighting and displays.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Acoustic Coupling between Plasmonic Nanoantennas: Detection and Directionality of Surface Acoustic Waves},

author = {M Poblet and R Bert\'{e} and H D Boggiano and Y Li and E Cort\'{e}s and G Grinblat and S A Maier and A V Bragas},

url = {https://doi.org/10.1021/acsphotonics.1c00741},

doi = {10.1021/acsphotonics.1c00741},

year  = {2021},

date = {2021-09-17},

urldate = {2021-09-17},

journal = {ACS Photonics},

abstract = {Hypersound waves can be efficient mediators between optical signals at the nanoscale. Having phase velocities several orders of magnitude lower than the speed of light, they propagate with much shorter wavelengths and can be controlled, directed, and even focused in a very small region of space. This work shows how two optical nanoantennas can be coupled through an acoustic wave that propagates with a certain directionality. An “emitter” antenna is first optically excited to generate acoustic coherent phonons that launch surface acoustic waves through the underlying substrate. These waves travel until they are mechanically detected by a “receiver” nanoantenna whose oscillation produces a detectable optical signal. Generation and detection are studied in detail, and new designs are proposed to improve the directionality of the hypersonic surface acoustic wave.},

keywords = {Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Engineering gallium phosphide nanostructures for efficient nonlinear photonics and enhanced spectroscopies},

author = {G Q Moretti and E Cort\'{e}s and S A Maier and A V Bragas and G Grinblat},

url = {https://doi.org/10.1515/nanoph-2021-0388},

doi = {doi:10.1515/nanoph-2021-0388},

year  = {2021},

date = {2021-09-16},

journal = {Nanophotonics},

number = {000010151520210388},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Photo-memristive sensing with charge storing 2D carbon nitrides},

author = {A Gouder and A Jimenez-Solano and N M Vargas-Barbosa and F Podjaski and B V Lotsch},

url = {https://arxiv.org/abs/2109.06964},

doi = {arXiv:2109.06964v1},

year  = {2021},

date = {2021-09-14},

journal = {arXiv preprint arXiv:2109.06964},

abstract = {We report the charge storing 2D carbon nitride potassium poly(heptazine imide), K-PHI, as a direct memristive (bio)sensing platform. Memristive devices have the potential to innovate current (bio)electronic systems such as photo-electrochemical sensors by incorporating new sensing capabilities including non-invasive, wireless remote and time-delayed (memory) readout. We demonstrate a direct photomemristive sensing platform that capitalizes on K PHI's visible light bandgap, large oxidation potential and intrinsic optoionic light energy storage properties. Our system simultaneously enables analyte concentration information storage as well as potentiometric, impedimetric and coulo-metric readouts on the same material, with no additional reagents required. Utilizing the light-induced charge storage function of K-PHI, we demonstrate analyte sensing via charge accumulation and present various methods to write/erase this information from the material. Additionally, fully wireless colorimetric and fluorometric detection of the charged state of K-PHI is demonstrated and could facilitate its use as particle-based in-situ sensing probe. The various readout options of the K PHI's response enable us to adapt the sensitivities and dynamic ranges without modifying the sensor. We demonstrate these features using glucose as an example analyte over a wide range of concentrations (50 μM to 50 mM). Moreover, due to the strong oxidative power of K-PHI, this sensing platform is able to detect a large variety of organic or biologically relevant analytes. Since PHI is easily synthesized, based on earth abundant precursors, biocompatible, chemically robust and responsive to visible light, we anticipate that the sensing platform presented herein opens up novel memristive and neuromorphic functions.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Multistate Nonvolatile Metamirrors with Tunable Optical Chirality},

author = {Y Huang and T Xiao and Z Xie and J Zheng and Y Su and W Chen and K Liu and M Tang and J Zhu and P M\"{u}ller-Buschbaum and L Li},

url = {https://doi.org/10.1021/acsami.1c14204},

doi = {10.1021/acsami.1c14204},

issn = {1944-8244},

year  = {2021},

date = {2021-09-14},

urldate = {2021-09-14},

journal = {ACS Applied Materials \& Interfaces},

abstract = {Compared with conventional mirrors that behave as isotropic electromagnetic (EM) reflectors, metamirrors composed of periodically aligned artificial meta-atoms exhibit increased degrees of freedom for EM manipulations. However, the functionality of most metamirrors is fixed by design, and how to achieve active EM control is still elusive. Here, we propose a multistate metamirror based on the nonvolatile phase change material Ge2Sb2Te5 (GST) with four distinct functionalities that can be realized in the infrared region by exploiting the temperature-activated phase transition. When varying the crystallinity of GST, the metamirror has the capability to perform as a right-handed circular polarization chiral mirror, a narrowband achiral mirror, a left-handed circular polarization chiral mirror, or a broadband achiral mirror, respectively. The inner physics is further explained by the construction or cancellation of extrinsic two-dimensional chirality. As a proof of concept, experimental verification is carried out and the measured results agree well with their simulated counterparts. Such a multifunctional tunable metamirror could address a wide range of applications from sensing and spectroscopy to analytical chemistry and imaging.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Trions in MoS2 are quantum superpositions of intra-and intervalley spin states},

author = {J Klein and M Florian and A H\"{o}tger and A Steinhoff and A Delhomme and T Taniguchi and K Watanabe and F Jahnke and A W Holleitner and M Potemski},

url = {https://arxiv.org/abs/2109.06281},

doi = {arXiv:2109.06281v1},

year  = {2021},

date = {2021-09-13},

journal = {arXiv preprint arXiv:2109.06281},

abstract = {We report magneto-photoluminescence spectroscopy of gated MoS2 monolayers in high magnetic fields to 28 T. At B = 0T and electron density ns∼1012cm−2, we observe three trion resonances that cannot be explained within a single-particle picture. Employing ab initio calculations that take into account three-particle correlation effects as well as local and non-local electron-hole exchange interaction, we identify those features as quantum superpositions of inter- and intravalley spin states. We experimentally investigate the mixed character of the trion wave function via the filling factor dependent valley Zeeman shift in positive and negative magnetic fields. Our results highlight the importance of exchange interactions for exciton physics in monolayer MoS2 and provide new insights into the microscopic understanding of trion physics in 2D multi-valley semiconductors for low excess carrier densities.},

keywords = {Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Conductivity mechanism in ionic 2D carbon nitrides: from hydrated ion motion to enhanced photocatalysis},

author = {J Kr\"{o}ger and F Podjaski and G Sava\c{s}\c{c}ı and I Moudrakovski and A Jimenez-Solano and M W Terban and S Bette and V Duppel and M Joos and A Senocrate},

year  = {2021},

date = {2021-09-12},

journal = {Cambridge University Press},

keywords = {Foundry Inorganic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Interlayer Interactions as Design Tool for Large-Pore COFs},

author = {S T Emmerling and R Schuldt and S Bette and L Yao and R E Dinnebier and J K\"{a}stner and B V Lotsch},

url = {https://doi.org/10.1021/jacs.1c06518},

doi = {10.1021/jacs.1c06518},

issn = {0002-7863},

year  = {2021},

date = {2021-09-08},

urldate = {2021-09-08},

journal = {Journal of the American Chemical Society},

volume = {143},

number = {38},

pages = {15711-15722},

abstract = {Covalent organic frameworks (COFs) with a pore size beyond 5 nm are still rarely seen in this emerging field. Besides obvious complications such as the elaborated synthesis of large linkers with sufficient solubility, more subtle challenges regarding large-pore COF synthesis, including pore occlusion and collapse, prevail. Here we present two isoreticular series of large-pore imine COFs with pore sizes up to 5.8 nm and correlate the interlayer interactions with the structure and thermal behavior of the COFs. By adjusting interlayer interactions through the incorporation of methoxy groups acting as pore-directing “anchors”, different stacking modes can be accessed, resulting in modified stacking polytypes and, hence, effective pore sizes. A strong correlation between stacking energy toward highly ordered, nearly eclipsed structures, higher structural integrity during thermal stress, and a novel, thermally induced phase transition of stacking modes in COFs was found, which sheds light on viable design strategies for increased structural control and stability in large-pore COFs.},

keywords = {Foundry Organic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Correlation of Thermoelectric Performance, Domain Morphology and Doping Level in PEDOT:PSS Thin Films Post-Treated with Ionic Liquids},

author = {A L Oechsle and J E Heger and N Li and S Yin and S Bernstorff and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/marc.202100397},

doi = {https://doi.org/10.1002/marc.202100397},

issn = {1022-1336},

year  = {2021},

date = {2021-09-07},

journal = {Macromolecular Rapid Communications},

volume = {42},

number = {20},

pages = {2100397},

abstract = {Abstract Ionic liquid (IL) post-treatment of poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) thin films with ethyl-3-methylimidazolium dicyanamide (EMIM DCA), allyl-3-methylimidazolium dicyanamide (AMIM DCA), and 1-ethyl-3-methylimidazolium tetracyanoborate (EMIM TCB) is compared. Doping level modifications of PEDOT are characterized using UV\textendashVis spectroscopy and directly correlate with the observed Seebeck coefficient enhancement. With conductive atomic force microscopy (c-AFM) the authors investigate changes in the topographic-current features of the PEDOT:PSS thin film surface due to IL treatment. Grazing incidence small-angle X-ray scattering (GISAXS) demonstrates the morphological rearrangement towards an optimized PEDOT domain distribution upon IL post-treatment, directly facilitating the interconductivity and causing an increased film conductivity. Based on these improvements in Seebeck coefficient and conductivity, the power factor is increased up to 236 µW m−1K−2. Subsequently, a model is developed indicating that ILs, which contain small, sterically unhindered ions with a strong localized charge, appear beneficial to boost the thermoelectric performance of post-treated PEDOT:PSS films.},

keywords = {Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Self-induced ultrafast electron-hole plasma temperature oscillations in nanowire lasers},

author = {A Thurn and J Bissinger and S Meinecke and P Schmiedeke and S S Oh and W W Chow and K L\"{u}dge and G Koblm\"{u}ller and J J Finley},

url = {https://arxiv.org/abs/2108.11784},

doi = {arXiv:2108.11784v2},

year  = {2021},

date = {2021-09-06},

journal = {arXiv preprint arXiv:2108.11784},

abstract = {Nanowire lasers can be monolithically and site-selectively integrated onto silicon photonic circuits. To assess their full potential for ultrafast opto-electronic devices, a detailed understanding of their lasing dynamics is crucial. However, the roles played by their resonator geometry and the microscopic processes that mediate energy exchange between the photonic, electronic, and phononic systems are largely unexplored. Here, we apply femtosecond pump-probe spectroscopy to show that GaAs-AlGaAs core-shell nanowire lasers exhibit sustained intensity oscillations with frequencies ranging from 160 GHz to 260 GHz. These dynamics are intricately linked to the strong interaction between the lasing mode and the gain material arising from their wavelength-scale dimensions. Combined with dynamic competition between photoinduced carrier heating and cooling via phonon scattering, this enables self-induced electron-hole plasma temperature oscillations, which modulate the laser output. We anticipate that our results will lead to new approaches for ultrafast intensity and phase modulation of chip-integrated nanoscale semiconductor lasers.},

keywords = {Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Single-step-fabricated disordered metasurfaces for enhanced light extraction from LEDs},

author = {P Mao and C Liu and X Li and M Liu and Q Chen and M Han and S A Maier and E H Sargent and S Zhang},

url = {https://doi.org/10.1038/s41377-021-00621-7},

doi = {10.1038/s41377-021-00621-7},

issn = {2047-7538},

year  = {2021},

date = {2021-09-06},

journal = {Light: Science \& Applications},

volume = {10},

number = {1},

pages = {180},

abstract = {While total internal reflection (TIR) lays the foundation for many important applications, foremost fibre optics that revolutionised information technologies, it is undesirable in some other applications such as light-emitting diodes (LEDs), which are a backbone for energy-efficient light sources. In the case of LEDs, TIR prevents photons from escaping the constituent high-index materials. Advances in material science have led to good efficiencies in generating photons from electron\textendashhole pairs, making light extraction the bottleneck of the overall efficiency of LEDs. In recent years, the extraction efficiency has been improved, using nanostructures at the semiconductor/air interface that outcouple trapped photons to the outside continuum. However, the design of geometrical features for light extraction with sizes comparable to or smaller than the optical wavelength always requires sophisticated and time-consuming fabrication, which causes a gap between lab demonstration and industrial-level applications. Inspired by lightning bugs, we propose and realise a disordered metasurface for light extraction throughout the visible spectrum, achieved with single-step fabrication. By applying such a cost-effective light extraction layer, we improve the external quantum efficiency by a factor of 1.65 for commercialised GaN LEDs, demonstrating a substantial potential for global energy-saving and sustainability.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Actinide Coordination Chemistry on Surfaces: Synthesis, Manipulation, and Properties of Thorium Bis(porphyrinato) Complexes},

author = {E Rheinfrank and M P\"{o}rtner and M D C Nu\~{n}ez Beyerle and F Haag and P S Deimel and F Allegretti and K Seufert and J V Barth and M-L Bocquet and P Feulner and W Auw\"{a}rter},

url = {https://doi.org/10.1021/jacs.1c04982},

doi = {10.1021/jacs.1c04982},

issn = {0002-7863},

year  = {2021},

date = {2021-09-03},

journal = {Journal of the American Chemical Society},

volume = {143},

number = {36},

pages = {14581-14591},

abstract = {Actinide-based metal\textendashorganic complexes and coordination architectures encompass intriguing properties and functionalities but are still largely unexplored on surfaces. We introduce the in situ synthesis of actinide tetrapyrrole complexes under ultrahigh-vacuum conditions, on both a metallic support and a 2D material. Specifically, exposure of a tetraphenylporphyrin (TPP) multilayer to an elemental beam of thorium followed by a temperature-programmed reaction and desorption of surplus molecules yields bis(porphyrinato)thorium (Th(TPP)2) assemblies on Ag(111) and hexagonal boron nitride/Cu(111). A multimethod characterization including X-ray photoelectron spectroscopy, scanning tunneling microscopy, temperature-programmed desorption, and complementary density functional theory modeling provides insights into conformational and electronic properties. Supramolecular assemblies of Th(TPP)2 as well as individual double-deckers are addressed with submolecular precision, e.g., demonstrating the reversible rotation of the top porphyrin in Th(TPP)2 by molecular manipulation. Our findings thus demonstrate prospects for actinide-based functional nanoarchitectures.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Surface-Mediated Ring-Opening and Porphyrin Deconstruction via Conformational Distortion},

author = {F Bischoff and A Riss and G S Michelitsch and J Ducke and J V Barth and K Reuter and W Auw\"{a}rter},

url = {https://doi.org/10.1021/jacs.1c05348},

doi = {10.1021/jacs.1c05348},

issn = {0002-7863},

year  = {2021},

date = {2021-09-02},

urldate = {2021-09-02},

journal = {Journal of the American Chemical Society},

volume = {143},

number = {37},

pages = {15131-15138},

abstract = {The breakdown of macrocyclic compounds is of utmost importance in manifold biological and chemical processes, usually proceeding via oxygenation-induced ring-opening reactions. Here, we introduce a surface chemical route to selectively break a prototypical porphyrin species, cleaving off one pyrrole unit and affording a tripyrrin derivative. This pathway, operational in an ultrahigh vacuum environment at moderate temperature is enabled by a distinct molecular conformation achieved via the specific interaction between the porphyrin and its copper support. We provide an atomic-level characterization of the surface-anchored tripyrrin, its reaction intermediates, and byproducts by bond-resolved atomic force microscopy, unequivocally identifying the molecular skeletons. The ring-opening is rationalized by the distortion reducing the macrocycle’s stability. Our findings open a route to steer ring-opening reactions by conformational design and to study intriguing tetrapyrrole catabolite analogues on surfaces.},

keywords = {Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Highly conductive titania supported iridium oxide nanoparticles with low overall iridium density as OER catalyst for large-scale PEM electrolysis},

author = {D B\"{o}hm and M Beetz and C Gebauer and M Bernt and J Schr\"{o}ter and M Kornherr and F Zoller and T Bein and D Fattakhova-Rohlfing},

url = {https://www.sciencedirect.com/science/article/pii/S2352940721001980},

doi = {https://doi.org/10.1016/j.apmt.2021.101134},

issn = {2352-9407},

year  = {2021},

date = {2021-09-01},

journal = {Applied Materials Today},

volume = {24},

pages = {101134},

abstract = {To enable future large-scale generation of hydrogen via proton exchange membrane (PEM) electrolysis, utilization of scarce iridium-based catalysts required for the oxygen evolution reaction (OER) has to be significantly lowered. To address this question, the facile synthesis of a highly active TiO2 supported iridium oxide based OER catalyst with reduced noble metal content and an Ir-density of the catalyst powder as low as 0.05\textendash0.08 gIr cm-3 is described in this work. A high surface area corrosion-resistant titania catalyst support homogeneously coated with a 1-2 nm thin layer of amorphous IrOOHx is oxidized in molten NaNO3 between 350-375°C. This procedure allows for a controllable phase transformation and crystallization to form a layer of interconnected IrO2 nanoparticles of ≈2 nm on the surface of the TiO2 support. The increase in crystallinity is thereby accompanied by a significant increase in conductivity of up to 11 S cm-1 for a 30 wt% Ir loaded catalyst. Oxidized samples further display a significantly increased stability with less detectable Ir dissolution under OER conditions. With a mass-based activity of 59 A g-1 at an overpotential of 300 mV, the electrocatalytic activity is maintained at the level of the highly active amorphous IrOOHx phase used as precursor and outperforms it at higher current densities through the increased conductivity. MEA measurements with catalyst loadings of 0.2-0.3 mg cm-2 further confirm the high catalytic activity and initial stability at industrially relevant current densities. The introduced synthesis approach therefore shows a path for the fabrication of novel highly active and atom-efficient oxide supported catalysts with complex nanostructures and thin homogenous nanoparticle coatings that allows a future large-scale application of PEM electrolysis technology without restrictions by the natural abundance of iridium.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Single Antibody Detection in a DNA Origami Nanoantenna},

author = {M Pfeiffer and K Trofymchuk and S Ranallo and F Ricci and F Steiner and F Cole and V Glembockyte and P Tinnefeld},

url = {https://www.sciencedirect.com/science/article/pii/S2589004221010403},

doi = {https://doi.org/10.1016/j.isci.2021.103072},

issn = {2589-0042},

year  = {2021},

date = {2021-09-01},

urldate = {2021-09-01},

journal = {iScience},

pages = {103072},

abstract = {Summary DNA nanotechnology offers new biosensing approaches by templating different sensor and transducer components. Here, we combine DNA origami nanoantennas with label-free antibody detection by incorporating a nanoswitch in the plasmonic hotspot of the nanoantenna. The nanoswitch contains two antigens that are displaced by antibody binding thereby eliciting a fluorescent signal. Single antibody detection is demonstrated with a DNA origami integrated anti-digoxigenin antibody nanoswitch. In combination with the nanoantenna, the signal generated by the antibody is additionally amplified. This allows the detection of single antibodies on a portable smartphone microscope. Overall, fluorescence enhanced antibody detection in DNA origami nanoantennas shows that fluorescence enhanced biosensing can be expanded beyond the scope of the nucleic acids realm.},

keywords = {Foundry Inorganic, Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Selective functionalization of the 1H-imidazo[1,2-b]pyrazole scaffold. A new potential non-classical isostere of indole and a precursor of push\textendashpull dyes},

author = {K Schw\"{a}rzer and S K Rout and D Bessinger and F Lima and C E Brocklehurst and K Karaghiosoff and T Bein and P Knochel},

url = {http://dx.doi.org/10.1039/D1SC04155J},

doi = {10.1039/D1SC04155J},

issn = {2041-6520},

year  = {2021},

date = {2021-08-30},

urldate = {2021-08-30},

journal = {Chemical Science},

volume = {12},

number = {39},

pages = {12993-13000},

abstract = {We report the selective functionalization of the 1H-imidazo[1,2-b]pyrazole scaffold using a Br/Mg-exchange, as well as regioselective magnesiations and zincations with TMP-bases (TMP = 2,2,6,6-tetramethylpiperidyl), followed by trapping reactions with various electrophiles. In addition, we report a fragmentation of the pyrazole ring, giving access to push\textendashpull dyes with a proaromatic (1,3-dihydro-2H-imidazol-2-ylidene)malononitrile core. These functionalization methods were used in the synthesis of an isostere of the indolyl drug pruvanserin. Comparative assays between the original drug and the isostere showed that a substitution of the indole ring with a 1H-imidazo[1,2-b]pyrazole results in a significantly improved solubility in aqueous media.},

keywords = {Foundry Organic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Chemical Stability and Ionic Conductivity of LGPS-Type Solid Electrolyte Tetra-Li7SiPS8 after Solvent Treatment},

author = {A-K Hatz and R Calaminus and J Feijoo and F Treber and J Blahusch and T Lenz and M Reichel and K Karaghiosoff and N M Vargas-Barbosa and B V Lotsch},

url = {https://doi.org/10.1021/acsaem.1c01917},

doi = {10.1021/acsaem.1c01917},

year  = {2021},

date = {2021-08-30},

journal = {ACS Applied Energy Materials},

volume = {4},

number = {9},

pages = {9932-9943},

abstract = {The large-scale production of solid-state batteries necessitates the development of alternative routes for processing air-sensitive thiophosphate-based solid electrolytes. To set a basis for this, we investigate the chemical stability and ionic conductivity of the LGPS-type lithium-ion conductor tetra-Li7SiPS8 (LiSiPS) processed with various organic solvents. We elucidate the nature of colorful polysulfides that arise during solvent treatment and trace back their origin to the dissolution of the Li3PS4-type amorphous side phase typically present in LiSiPS. We find that water and alcohols decompose LiSiPS by the nucleophilic attack into oxygen-substituted thiophosphates and thioethers and propose a reaction mechanism for the latter. Moreover, we confirm that quaternary thiophosphates can be recrystallized from MeOH solutions upon subsequent high-temperature treatment. Aprotic solvents with donor numbers smaller than 15 kcal mol\textendash1 are suitable for wet-processing quaternary thiophosphates because both the crystal structure of the electrolyte and a high ionic conductivity of \>1 mS cm\textendash1 are retained. Using anisole as a case study, we clarify that a residual water content of up to 800 ppm does not lead to a significant deterioration in the ionic conductivity when compared to dry solvents (≤5 ppm). Additionally, we observe a decrease in ionic conductivity with an increasing amount of the solvent residue, which depends not only on the donor number of the solvent but also on the vapor pressure and interactions between the solvent molecules and thiophosphate groups in the solid electrolyte. Thus, optimization of solvent-processing methods of thiophosphate electrolytes is a multifaceted challenge. This work provides transferable insights regarding the stability of LiSiPS against organic solvents that may enable competitive and large-scale thiophosphate-based solid electrolyte processing.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Defying Thermodynamics: Stabilization of Alane Within Covalent Triazine Frameworks for Reversible Hydrogen Storage},

author = {V Stavila and S Li and C Dun and M T Marple and H E Mason and J L Snider and J E Reynolds Iii and F El Gabaly and J D Sugar and C D Spataru and X Zhou and B Dizdar and E H Majzoub and R Chatterjee and J Yano and H Schlomberg and B V Lotsch and J J Urban and B C Wood and M D Allendorf},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202107507},

doi = {https://doi.org/10.1002/anie.202107507},

issn = {1433-7851},

year  = {2021},

date = {2021-08-29},

journal = {Angewandte Chemie International Edition},

volume = {60},

number = {49},

pages = {25815-25824},

abstract = {Abstract The highly unfavorable thermodynamics of direct aluminum hydrogenation can be overcome by stabilizing alane within a nanoporous bipyridine-functionalized covalent triazine framework (AlH3@CTF-bipyridine). This material and the counterpart AlH3@CTF-biphenyl rapidly desorb H2 between 95 and 154 °C, with desorption complete at 250 °C. Sieverts measurements, 27Al MAS NMR and 27Al1H REDOR experiments, and computational spectroscopy reveal that AlH3@CTF-bipyridine dehydrogenation is reversible at 60 °C under 700 bar hydrogen, \>10 times lower pressure than that required to hydrogenate bulk aluminum. DFT calculations and EPR measurements support an unconventional mechanism whereby strong AlH3 binding to bipyridine results in single-electron transfer to form AlH2(AlH3)n clusters. The resulting size-dependent charge redistribution alters the dehydrogenation/rehydrogenation thermochemistry, suggesting a novel strategy to enable reversibility in high-capacity metal hydrides.},

keywords = {Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Overcoming the Challenges of Freestanding Tin Oxide-Based Composite Anodes to Achieve High Capacity and Increased Cycling Stability},

author = {F Zoller and S H\"{a}ringer and D B\"{o}hm and H Illner and M D\"{o}blinger and Z K Sofer and M Finsterbusch and T Bein and D Fattakhova-Rohlfing},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202106373},

doi = {https://doi.org/10.1002/adfm.202106373},

issn = {1616-301X},

year  = {2021},

date = {2021-08-27},

journal = {Advanced Functional Materials},

volume = {31},

number = {43},

pages = {2106373},

abstract = {Abstract Freestanding electrodes are a promising way to increase the energy density of the batteries by decreasing the overall amount of electrochemically inactive materials. Freestanding antimony doped tin oxide (ATO)-based hybrid materials have not been reported so far, although this material has demonstrated excellent performance in conventionally designed electrodes. Two different strategies, namely electrospinning and freeze-casting, are explored for the fabrication of ATO-based hybrid materials. It is shown that the electrospinning of ATO/carbon based electrodes from polyvinyl pyrrolidone polymer (PVP) solutions was not successful, as the resulting electrode material suffers from rapid degradation. However, freestanding reduced graphene oxide (rGO) containing ATO/C/rGO nanocomposites prepared via a freeze-casting route demonstrates an impressive rate and cycling performance reaching 697 mAh g−1 at a high current density of 4 A g−1, which is 40 times higher as compared to SnO2/rGO and also exceeds the freestanding SnO2-based composites reported so far. Antimony doping of the nanosized tin oxide phase and carbon coating are thereby shown to be essential factors for appealing electrochemical performance. Finally, the freestanding ATO/C/rGO anodes are combined with freestanding LiFe0.2Mn0.8PO4/rGO cathodes to obtain a full freestanding cell operating without metal current collector foils showing nonetheless an excellent cycling stability.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Unveiling the Complex Configurational Landscape of the Intralayer Cavities in a Crystalline Carbon Nitride},

author = {M Pauly and J Kroger and V Duppel and C Murphey and J Cahoon and B V Lotsch and P Maggard},

url = {https://chemrxiv.org/engage/chemrxiv/article-details/6127820165db1ec864a4c3a6},

doi = {10.26434/chemrxiv-2021-90tq7-v2},

year  = {2021},

date = {2021-08-26},

urldate = {2021-08-26},

abstract = {The in-depth understanding of the reported photoelectrochemical properties of the layered carbon nitride, poly(triazine imide)/LiCl (PTI/LiCl), has been limited by the apparent disorder of the Li/H atoms within its framework. To understand and resolve the current structural ambiguities, an optimized one-step flux synthesis (470 oC, 36 h, LiCl/KCl flux) was used to prepare PTI/LiCl and deuterated-PTI/LiCl in high purity. Its structure was characterized by a combination of neutron/X-ray diffraction and transmission electron microscopy. The range of possible Li/H atomic configurations were enumerated for the first time and, combined with total energy calculations, reveals a more complex energetic landscape than previously considered. Experimental data were fitted against all possible structural models, exhibiting the most consistency with a new orthorhombic model (Sp. Grp. Ama2) that also has the lowest total energy. In addition, a new Cu(I)-containing PTI (PTI/CuCl) was prepared with the more strongly scattering Cu(I) cations in place of Li, and which also most closely matched with the partially-disorded structure in Cmc21. Thus, a complex configurational landscape of PTI is revealed to consist of a number of ordered crystalline structures that are new potential synthetic targets, such as with the use of metal-exchange reactions.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {DNA Origami Nanoantennas for Fluorescence Enhancement},

author = {V Glembockyte and L Grabenhorst and K Trofymchuk and P Tinnefeld},

url = {https://doi.org/10.1021/acs.accounts.1c00307},

doi = {10.1021/acs.accounts.1c00307},

issn = {0001-4842},

year  = {2021},

date = {2021-08-26},

urldate = {2021-08-26},

journal = {Accounts of Chemical Research},

volume = {54},

number = {17},

pages = {3338-3348},

abstract = {ConspectusThe possibility to increase fluorescence by plasmonic effects in the near-field of metal nanostructures was recognized more than half a century ago. A major challenge, however, was to use this effect because placing single quantum emitters in the nanoscale plasmonic hotspot remained unsolved for a long time. This not only presents a chemical problem but also requires the nanostructure itself to be coaligned with the polarization of the excitation light. Additional difficulties arise from the complex distance dependence of fluorescence emission: in contrast to other surface-enhanced spectroscopies (such as Raman spectroscopy), the emitter should not be placed as close as possible to the metallic nanostructure but rather needs to be at an optimal distance on the order of a few nanometers to avoid undesired quenching effects.Our group addressed these challenges almost a decade ago by exploiting the unique positioning ability of DNA nanotechnology and reported the first self-assembled DNA origami nanoantennas. This Account summarizes our work spanning from this first proof-of-principle study to recent advances in utilizing DNA origami nanoantennas for single DNA molecule detection on a portable smartphone microscope.We summarize different aspects of DNA origami nanoantennas that are essential for achieving strong fluorescence enhancement and discuss how single-molecule fluorescence studies helped us to gain a better understanding of the interplay between fluorophores and plasmonic hotspots. Practical aspects of preparing the DNA origami nanoantennas and extending their utility are also discussed.Fluorescence enhancement in DNA origami nanoantennas is especially exciting for signal amplification in molecular diagnostic assays or in single-molecule biophysics, which could strongly benefit from higher time resolution. Additionally, biophysics can greatly profit from the ultrasmall effective detection volumes provided by DNA nanoantennas that allow single-molecule detection at drastically elevated concentrations as is required, e.g., in single-molecule DNA sequencing approaches.Finally, we describe our most recent progress in developing DNA NanoAntennas with Cleared HOtSpots (NACHOS) that are fully compatible with biomolecular assays. The developed DNA origami nanoantennas have proven robustness and remain functional after months of storage. As an example, we demonstrated for the first time the single-molecule detection of DNA specific to antibiotic-resistant bacteria on a portable and battery-driven smartphone microscope enabled by DNA origami nanoantennas. These recent developments mark a perfect moment to summarize the principles and the synthesis of DNA origami nanoantennas and give an outlook of new exciting directions toward using different nanomaterials for the construction of nanoantennas as well as for their emerging applications.},

keywords = {Foundry Inorganic, Foundry Organic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Indirect bandgap, optoelectronic properties, and photoelectrochemical characteristics of high-purity Ta3N5 photoelectrodes},

author = {J Eichhorn and S P Lechner and C-M Jiang and G Folchi Heunecke and F Munnik and I D Sharp},

url = {http://dx.doi.org/10.1039/D1TA05282A},

doi = {10.1039/D1TA05282A},

issn = {2050-7488},

year  = {2021},

date = {2021-08-26},

urldate = {2021-08-26},

journal = {Journal of Materials Chemistry A},

volume = {9},

pages = {20653},

abstract = {The (opto)electronic properties of Ta3N5 photoelectrodes are often dominated by defects, such as oxygen impurities, nitrogen vacancies, and low-valent Ta cations, impeding fundamental studies of its electronic structure, chemical stability, and photocarrier transport. Here, we explore the role of ammonia annealing following direct reactive magnetron sputtering of tantalum nitride thin films, achieving near-ideal stoichiometry, with significantly reduced native defect and oxygen impurity concentrations. By analyzing structural, optical, and photoelectrochemical properties as a function of ammonia annealing temperature, we provide new insights into the basic semiconductor properties of Ta3N5, as well as the role of defects on its optoelectronic characteristics. Both the crystallinity and material quality improve up to 940 °C, due to elimination of oxygen impurities. Even higher annealing temperatures cause material decomposition and introduce additional disorder within the Ta3N5 lattice, leading to reduced photoelectrochemical performance. Overall, the high material quality enables us to unambiguously identify the nature of the Ta3N5 bandgap as indirect, thereby resolving a long-standing controversy regarding the most fundamental characteristic of this material as a semiconductor. The compact morphology, low defect content, and high optoelectronic quality of these films provide a basis for further optimization of photoanodes and may open up further application opportunities beyond photoelectrochemical energy conversion.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Time-consistent hopping transport with vibration-mode-resolved electron-phonon couplings},

author = {S Hutsch and M Panhans and F Ortmann},

url = {https://link.aps.org/doi/10.1103/PhysRevB.104.054306},

doi = {10.1103/PhysRevB.104.054306},

year  = {2021},

date = {2021-08-25},

journal = {Physical Review B},

volume = {104},

number = {5},

pages = {054306},

abstract = {Charge transport in organic semiconductors is affected by the complex interaction between charge carriers and molecular vibrations. A common way to treat the molecular vibrations in hopping approaches is by condensing them into a single analytical parameter, the reorganization energy. In contrast, here we present a nonadiabatic hopping transport approach that avoids this approximation by dividing the vibrational spectrum of organic molecules into three distinct analytical classes, namely the quasistatic, low-frequency dynamic, and high-frequency dynamic modes. The quasistatic and dynamic regimes are separated time consistently with respect to the timescale of the hopping events, which results in charge transfer events driven by a set of strongly coupling driving modes. Using these time-consistent hopping rates, we compute the charge carrier mobilities for a set of hopping transport materials and a control set of band-transport materials and compare them to experimental values. The resulting mobilities are consistent for both sets by showing similar values for the hopping transport materials and lower values for the control set of band-transport materials due to the absence of coherent transport contributions. We further study other popular hopping approaches such as the Marcus theory and the Levich-Jortner theory and observe substantial inconsistencies for them.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Fast Water-Assisted Lithium Ion Conduction in Restacked Lithium Tin Sulfide Nanosheets},

author = {A-K Hatz and I Moudrakovski and S Bette and M W Terban and M Etter and M Joos and N M Vargas-Barbosa and R E Dinnebier and B V Lotsch},

url = {https://doi.org/10.1021/acs.chemmater.1c01755},

doi = {10.1021/acs.chemmater.1c01755},

issn = {0897-4756},

year  = {2021},

date = {2021-08-25},

journal = {Chemistry of Materials},

volume = {33},

number = {18},

pages = {7337-7349},

abstract = {While two-dimensional (2D) materials may preserve some intrinsic properties of the corresponding layered bulk material, new characteristics arise from their pronounced anisotropy or confinement effects. Recently, exceptionally high ionic conductivities were discovered in 2D materials such as graphene oxide and vermiculite. Here, we report on the water-assisted fast conduction of lithium ions in restacked lithium tin sulfide nanosheets. Li0.8Sn0.8S2 exfoliates spontaneously in water and can be restacked into homogeneous films in which the lithium content is decreased, and a partial substitution of sulfur with hydroxyl groups takes place. Using a recursive supercell refinement approach in reciprocal space along with real-space pair distribution function analysis, we describe restacked lithium tin sulfide as a partially turbostratically disordered material composed of lithium-containing and lithium-depleted layers. In humid air, the material takes up multiple layers of water that coordinate lithium ions in the space between the layers, increasing the stacking distance and screening the interaction between lithium ions and the anionic layers. This results in a 1000-fold increase in ionic conductivity up to 47 mS cm\textendash1 at high humidities. Orientation-dependent impedance spectroscopy suggests a facile in-plane conduction and a hindered out-of-plane conduction. Pulsed field gradient nuclear magnetic resonance spectroscopy reveals a fast, simultaneous diffusion of a majority and a minority species for both 7Li and 1H, suggesting water-assisted lithium diffusion to be at play. This study enlarges the family of nanosheet-based ionic conductors and helps to rationalize the transport mechanism of lithium ions enabled by hydration in a nanoconfined 2D space.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Recent Advances in Cross-Couplings of Functionalized Organozinc Reagents},

author = {B Wei and P Knochel},

url = {https://www.thieme-connect.com/products/ejournals/abstract/10.1055/a-1589-0150},

doi = {10.1055/a-1589-0150},

issn = {0039-7881 DOI - 10.1055/a-1589-0150},

year  = {2021},

date = {2021-08-16},

journal = {Synthesis},

volume = {54},

number = {02},

pages = {246-254},

abstract = {Cross-couplings involving organozinc reagents usually require a Pd-catalyst (Negishi cross-coupling), however, uncatalyzed cross-couplings of zinc organometallics proceed well in the absence of transition-metal catalysts with reactive electrophiles such as benzal 1,1-diacetates, benzhydryl acetates, and iminium trifluoroacetates. Organozinc compounds also undergo C\textendashN bond formation with O-benzoylhydroxylamines or organic azides in the presence of cobalt- or iron-catalysts. Highly diastereoselective and enantioselective cross-couplings can be readily performed with room-temperature configurationally stable alkylzinc species, producing diastereoselectively and enantiomerically enriched products. Finally, highly regioselective magnesiations of functionalized arenes and heteroarenes undergo Negishi (after transmetalation with ZnCl2) or Cu-catalyzed cross-couplings.},

keywords = {Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Influence of environmental conditions and surface treatments on the photoluminescence properties of GaN nanowires and nanofins},

author = {M Kraut and F Pantle and S W\"{o}rle and E Sirotti and A Zeidler and F Eckmann and M Stutzmann},

issn = {0957-4484},

year  = {2021},

date = {2021-08-16},

journal = {Nanotechnology},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}