Publications

@article{,

title = {Atomically dispersed asymmetric Cu-B pair on 2D carbon nitride synergistically boosts the conversion of CO into C-2 products},

author = {T W He and K Reuter and A J Du},

url = {\<Go to ISI\>://WOS:000505561500008},

doi = {10.1039/c9ta12090d},

issn = {2050-7488},

year  = {2019},

date = {2019-12-09},

journal = {Journal of Materials Chemistry A},

volume = {8},

number = {2},

pages = {599-606},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Bottom-Up Fabrication of a Metal-Supported Oxo-Metal Porphyrin},

author = {D A Duncan and P S Deimel and A Wiengarten and M Paszkiewicz and P C Aguilar and R G Acres and F Klappenberger and W Auwarter and A P Seitsonen and J V Barth and F Allegretti},

url = {\<Go to ISI\>://WOS:000505632900028},

doi = {10.1021/acs.jpcc.9b08661},

issn = {1932-7447},

year  = {2019},

date = {2019-11-25},

journal = {Journal of Physical Chemistry C},

volume = {123},

number = {51},

pages = {31011-31025},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Excitons and narrow bands determine the optical properties of cesium bismuth halides},

author = {S Rieger and B J Bohn and M Doblinger and A F Richter and Y Tong and K Wang and P Muller-Buschbaum and L Polavarapu and L Leppert and J K Stolarczyk and J Feldmann},

url = {\<Go to ISI\>://WOS:000498055800001},

doi = {10.1103/PhysRevB.100.201404},

issn = {2469-9950},

year  = {2019},

date = {2019-11-20},

journal = {Physical Review B},

volume = {100},

number = {20},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Efficient OER Catalyst with Low Ir Volume Density Obtained by Homogeneous Deposition of Iridium Oxide Nanoparticles on Macroporous Antimony-Doped Tin Oxide Support},

author = {D Bohm and M Beetz and M Schuster and K Peters and A G Hufnagel and M Doblinger and B Boller and T Bein and D Fattakhova-Rohlfing},

url = {\<Go to ISI\>://WOS:000492384200001},

doi = {10.1002/adfm.201906670},

issn = {1616-301X},

year  = {2019},

date = {2019-10-25},

journal = {Advanced Functional Materials},

volume = {30},

number = {1},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Broadband SERS detection with disordered plasmonic hybrid aggregates},

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

url = {\<Go to ISI\>://WOS:000504106900036},

doi = {10.1039/c9nr08118f},

issn = {2040-3364},

year  = {2019},

date = {2019-10-14},

journal = {Nanoscale},

volume = {12},

number = {1},

pages = {93-102},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Optical absorption of composition-tunable InGaAs nanowire arrays},

author = {J Treu and X Xu and K Ott and K Saller and G Abstreiter and J J Finley and G Koblm\"{u}ller},

url = {http://dx.doi.org/10.1088/1361-6528/ab3ef7},

doi = {10.1088/1361-6528/ab3ef7},

issn = {0957-4484 

1361-6528},

year  = {2019},

date = {2019-09-20},

journal = {Nanotechnology},

volume = {30},

number = {49},

pages = {495703},

abstract = {InGaAs nanowire (NW) arrays have emerged as important active materials in future photovoltaic and photodetector applications, due to their excellent electronic properties and tunable band gap. Here, we report a systematic investigation of the optical absorption characteristics of composition-tunable vertical InGaAs NW arrays. Using finite-difference time-domain simulations we first study the effect of variable composition (Ga-molar fraction) and NW array geometry (NW diameter, period, fill factor) on the optical generation rate. NWs with typical diameters in the range of ∼100\textendash250 nm lead to generation rates higher than the equivalent bulk case for moderate fill factors (NW period of ∼0.3\textendash0.8 μm), while slightly smaller fill factors and increased diameters are required to maintain high generation rates at increased Ga-molar fraction. The optical absorption was further measured using spectrally resolved ultraviolet\textendashvisible-near-infrared (UV\textendashvis-NIR) spectroscopy on NW arrays transferred to transparent substrates. Interestingly, large variations in Ga-molar fraction (0 \< x(Ga) \< 0.5) have a negligible influence, while minute changes in NW diameter of less than ±20 nm affect the absorption spectra very strongly, leading to pronounced shifts in the peak absorption energies by more than ∼700 meV. These results clearly highlight the much larger sensitivity of the optical absorption behavior to geometric parameters rather than to variations in the electronic band gap of the underlying NW array.},

keywords = {Foundry Inorganic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{Mallmann2019,

title = {Solid Solutions of Grimm\textendashSommerfeld Analogous Nitride Semiconductors II‐IV‐N2 (II=Mg, Mn, Zn; IV=Si, Ge): Ammonothermal Synthesis and DFT Calculations },

author = {M Mallmann and R Niklaus and T Rackl and M Benz and T G Chau and D Johrendt and J Min\'{a}r and W Schnick},

doi = {https://doi.org/10.1002/chem.201903897},

issn = {1521-3765},

year  = {2019},

date = {2019-09-17},

journal = {Chem. Eur. J.},

volume = {25},

pages = {1-10},

abstract = {Grimm\textendashSommerfeld analogous II‐IV‐N2 nitrides such as ZnSiN2, ZnGeN2, and MgGeN2 are promising semiconductor materials for substitution of commonly used (Al,Ga,In)N. Herein, the ammonothermal synthesis of solid solutions of II‐IV‐N2 compounds (II=Mg, Mn, Zn; IV=Si, Ge) having the general formula (IIa1−xIIbx)‐IV‐N2 with x≈0.5 and ab initio DFT calculations of their electronic and optical properties are presented. The ammonothermal reactions were conducted in custom‐built, high‐temperature, high‐pressure autoclaves by using the corresponding elements as starting materials. NaNH2 and KNH2 act as ammonobasic mineralizers that increase the solubility of the reactants in supercritical ammonia. Temperatures between 870 and 1070 K and pressures up to 200 MPa were chosen as reaction conditions. All solid solutions crystallize in wurtzite‐type superstructures with space group Pna21 (no. 33), confirmed by powder XRD. The chemical compositions were analyzed by energy‐dispersive X‐ray spectroscopy. Diffuse reflectance spectroscopy was used for estimation of optical bandgaps of all compounds, which ranged from 2.6 to 3.5 eV (Ge compounds) and from 3.6 to 4.4 eV (Si compounds), and thus demonstrated bandgap tunability between the respective boundary phases. Experimental findings were corroborated by DFT calculations of the electronic structure of pseudorelaxed mixed‐occupancy structures by using the KKR+CPA approach.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Directing Single-Molecule Emission with DNA Origami-Assembled Optical Antennas},

author = {K H\"{u}bner and M Pilo-Pais and F Selbach and T Liedl and P Tinnefeld and F D Stefani and G P Acuna},

url = {https://doi.org/10.1021/acs.nanolett.9b02886},

doi = {10.1021/acs.nanolett.9b02886},

issn = {1530-6984},

year  = {2019},

date = {2019-09-11},

urldate = {2019-09-11},

journal = {Nano Letters},

volume = {19},

number = {9},

pages = {6629-6634},

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

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A highly crystalline anthracene-based MOF-74 series featuring electrical conductivity and luminescence},

author = {P I Scheurle and A M\"{a}hringer and A C Jakowetz and P Hosseini and A F Richter and G Wittstock and D D Medina and T Bein},

url = {http://dx.doi.org/10.1039/C9NR05431F},

doi = {10.1039/C9NR05431F},

issn = {2040-3364},

year  = {2019},

date = {2019-09-10},

journal = {Nanoscale},

volume = {11},

number = {43},

pages = {20949-20955},

abstract = {Recently, a small group of metal\textendashorganic frameworks (MOFs) has been discovered featuring substantial charge transport properties and electrical conductivity, hence promising to broaden the scope of potential MOF applications in fields such as batteries, fuel cells and supercapacitors. In combination with light emission, electroactive MOFs are intriguing candidates for chemical sensing and optoelectronic applications. Here, we incorporated anthracene-based building blocks into the MOF-74 topology with five different divalent metal ions, that is, Zn2+, Mg2+, Ni2+, Co2+ and Mn2+, resulting in a series of highly crystalline MOFs, coined ANMOF-74(M). This series of MOFs features substantial photoluminescence, with ANMOF-74(Zn) emitting across the whole visible spectrum. The materials moreover combine this photoluminescence with high surface areas and electrical conductivity. Compared to the original MOF-74 materials constructed from 2,5-dihydroxy terephthalic acid and the same metal ions Zn2+, Mg2+, Ni2+, Co2+ and Mn2+, we observed a conductivity enhancement of up to six orders of magnitude. Our results point towards the importance of building block design and the careful choice of the embedded MOF topology for obtaining materials with desired properties such as photoluminescence and electrical conductivity.},

keywords = {Foundry Inorganic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {In Situ Monitoring Mesoscopic Deformation of Nanostructured Porous Titania Films Caused by Water Ingression},

author = {L Song and M Rawolle and N Hohn and J S Gutmann and H Frielinghaus and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.9b10750},

doi = {10.1021/acsami.9b10750},

issn = {1944-8244},

year  = {2019},

date = {2019-09-04},

journal = {ACS Applied Materials \& Interfaces},

volume = {11},

number = {35},

pages = {32552-32558},

abstract = {Nanostructured porous titania films are used in many energy-related applications. In this work, the temporal evolution of the mesoscopic deformation of mesoporous titania films synthesized via block copolymer-assisted sol\textendashgel chemistry is investigated with in situ grazing incidence small-angle neutron scattering (GISANS) during exposure to D2O vapor. Two types of mesoporous titania films are compared, which have a different degree of structural stability, depending on the applied annealing temperature (400 °C vs 600 °C) in a nitrogen atmosphere. Water ingression causes a gradual structure deformation in terms of decreasing center-to-center distances and broadening of the size distribution of the titania nanostructures. Based on the evolution of the mesopore size obtained from in situ GISANS measurements, the results show that structures synthesized at lower temperature undergo a stronger deformation because of the lower elastic modulus originating from larger pores, despite having a higher degree of order.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Present and Future of Surface-Enhanced Raman Scattering},

author = {J Langer and De D J Aberasturi and J Aizpurua and R A Alvarez-Puebla and B Auguie and J J Baumberg and G C Bazan and S E J Bell and A Boisen and A G Brolo and J Choo and D Cialla-May and V Deckert and L Fabris and K Faulds and De F J G Abajo and R Goodacre and D Graham and A J Haes and C L Haynes and C Huck and T Itoh and M Ka and J Kneipp and N A Kotov and H Kuang and Le E C Ru and H K Lee and J F Li and X Y Ling and S A Maier and T Mayerhofer and M Moskovits and K Murakoshi and J M Nam and S Nie and Y Ozaki and I Pastoriza-Santos and J Perez-Juste and J Popp and A Pucci and S Reich and B Ren and G C Schatz and T Shegai and S Schlucker and L L Tay and K G Thomas and Z Q Tian and Van R P Duyne and T Vo-Dinh and Y Wang and K A Willets and C Xu and H Xu and Y Xu and Y S Yamamoto and B Zhao and L M Liz-Marzan},

url = {\<Go to ISI\>://WOS:000510531500006},

doi = {10.1021/acsnano.9b04224},

issn = {1936-0851},

year  = {2019},

date = {2019-09-03},

journal = {Acs Nano},

volume = {14},

number = {1},

pages = {28-117},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Recent Approaches to Design Electrocatalysts Based on Metal\textendashOrganic Frameworks and Their Derivatives},

author = {J Liu and S Hou and W Li and A S Bandarenka and R A Fischer},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/asia.201900748},

doi = {https://doi.org/10.1002/asia.201900748},

issn = {1861-4728},

year  = {2019},

date = {2019-08-20},

journal = {Chemistry \textendash An Asian Journal},

volume = {14},

number = {20},

pages = {3474-3501},

abstract = {Abstract Rational design and synthesis of efficient electrocatalysts are important constituents in addressing the currently growing provision issues. Typical reactions, which are important to catalyze in this respect, include CO2 reduction, the hydrogen and oxygen evolution reactions as well as the oxygen reduction reaction. The most efficient catalysts known up-to-date for these processes usually contain expensive and scarce elements, substantially impeding implementation of such electrocatalysts at a larger scale. Metal-organic frameworks (MOFs) and their derivatives containing affordable components and building blocks, as an emerging class of porous functional materials, have been recently attracting a great attention thanks to their tunable structure and composition together with high surface area, just to name a few. Up to now, several MOFs and MOF-derivatives have been reported as electrode materials for the energy-related electrocatalytic application. In this review article, we summarize and analyze current approaches to design such materials. The design strategies to improve the Faradaic efficiency and selectivity of these catalysts are discussed. Last but not least, we discuss some novel strategies to enhance the conductivity, chemical stability and efficiency of MOF-derived electrocatalysts.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Low-Scaling Self-Consistent Minimization of a Density Matrix Based Random Phase Approximation Method in the Atomic Orbital Space},

author = {D Graf and M Beuerle and C Ochsenfeld},

url = {\<Go to ISI\>://WOS:000480826800016},

doi = {10.1021/acs.jctc.9b00444},

issn = {1549-9618},

year  = {2019},

date = {2019-08-01},

journal = {Journal of Chemical Theory and Computation},

volume = {15},

number = {8},

pages = {4468-4477},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Ultracompact Photodetection in Atomically Thin MoSe2},

author = {M Blauth and G Vest and S L Rosemary and M Prechtl and O Hartwig and M Jurgensen and M Kaniber and A V Stier and J J Finley},

url = {\<Go to ISI\>://WOS:000482545400012},

doi = {10.1021/acsphotonics.9b00785},

issn = {2330-4022},

year  = {2019},

date = {2019-07-30},

journal = {Acs Photonics},

volume = {6},

number = {8},

pages = {1902-1909},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Polymer Nanoreactors Shield Perovskite Nanocrystals from Degradation},

author = {V A Hintermayr and C Lampe and M Low and J Roemer and W Vanderlinden and M Gramlich and A X Bohm and C Sattler and B Nickel and T Lohmuller and A S Urban},

url = {\<Go to ISI\>://WOS:000481563800015},

doi = {10.1021/acs.nanolett.9b00982},

issn = {1530-6984},

year  = {2019},

date = {2019-07-19},

journal = {Nano Letters},

volume = {19},

number = {8},

pages = {4928-4933},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Influence of Local Defects on the Dynamics of O-H Bond Breaking and Formation on a Magnetite Surface},

author = {A Bourgund and B A J Lechner and M Meier and C Franchini and G S Parkinson and U Heiz and F Esch},

url = {\<Go to ISI\>://WOS:000481568900054},

doi = {10.1021/acs.jpcc.9b05547},

issn = {1932-7447},

year  = {2019},

date = {2019-07-17},

urldate = {2019-07-17},

journal = {Journal of Physical Chemistry C},

volume = {123},

number = {32},

pages = {19742-19747},

keywords = {Foundry Inorganic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Using Polar Alcohols for the Direct Synthesis of Cesium Lead Halide Perovskite Nanorods with Anisotropic Emission},

author = {Y X Li and H Huang and Y Xiong and A F Richter and S V Kershaw and J Feldmann and A L Rogach},

url = {\<Go to ISI\>://WOS:000477786400088},

doi = {10.1021/acsnano.9b03508},

issn = {1936-0851},

year  = {2019},

date = {2019-07-11},

journal = {Acs Nano},

volume = {13},

number = {7},

pages = {8237-8245},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Site-selectively generated photon emitters in monolayer MoS2 via local helium ion irradiation},

author = {J Klein and M Lorke and M Florian and F Sigger and L Sigl and S Rey and J Wierzbowski and J Cerne and K M\"{u}ller and E Mitterreiter and P Zimmermann and T Taniguchi and K Watanabe and U Wurstbauer and M Kaniber and M Knap and R Schmidt and J J Finley and A W Holleitner},

url = {https://doi.org/10.1038/s41467-019-10632-z},

doi = {10.1038/s41467-019-10632-z},

issn = {2041-1723},

year  = {2019},

date = {2019-06-21},

journal = {Nature Communications},

volume = {10},

number = {1},

pages = {2755},

abstract = {Quantum light sources in solid-state systems are of major interest as a basic ingredient for integrated quantum photonic technologies. The ability to tailor quantum emitters via site-selective defect engineering is essential for realizing scalable architectures. However, a major difficulty is that defects need to be controllably positioned within the material. Here, we overcome this challenge by controllably irradiating monolayer MoS2 using a sub-nm focused helium ion beam to deterministically create defects. Subsequent encapsulation of the ion exposed MoS2 flake with high-quality hBN reveals spectrally narrow emission lines that produce photons in the visible spectral range. Based on ab-initio calculations we interpret these emission lines as stemming from the recombination of highly localized electron\textendashhole complexes at defect states generated by the local helium ion exposure. Our approach to deterministically write optically active defect states in a single transition metal dichalcogenide layer provides a platform for realizing exotic many-body systems, including coupled single-photon sources and interacting exciton lattices that may allow the exploration of Hubbard physics.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Hydrophobic Metal\textendashOrganic Frameworks},

author = {K Jayaramulu and F Geyer and A Schneemann and \v{S} Kment and M Otyepka and R Zboril and D Vollmer and R A Fischer},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.201900820},

doi = {https://doi.org/10.1002/adma.201900820},

issn = {0935-9648},

year  = {2019},

date = {2019-06-03},

journal = {Advanced Materials},

volume = {31},

number = {32},

pages = {1900820},

abstract = {Abstract Metal\textendashorganic frameworks (MOFs) have diverse potential applications in catalysis, gas storage, separation, and drug delivery because of their nanoscale periodicity, permanent porosity, channel functionalization, and structural diversity. Despite these promising properties, the inherent structural features of even some of the best-performing MOFs make them moisture-sensitive and unstable in aqueous media, limiting their practical usefulness. This problem could be overcome by developing stable hydrophobic MOFs whose chemical composition is tuned to ensure that their metal\textendashligand bonds persist even in the presence of moisture and water. However, the design and fabrication of such hydrophobic MOFs pose a significant challenge. Reported syntheses of hydrophobic MOFs are critically summarized, highlighting issues relating to their design, characterization, and practical use. First, wetting of hydrophobic materials is introduced and the four main strategies for synthesizing hydrophobic MOFs are discussed. Afterward, critical challenges in quantifying the wettability of these hydrophobic porous surfaces and solutions to these challenges are discussed. Finally, the reported uses of hydrophobic MOFs in practical applications such as hydrocarbon storage/separation and their use in separating oil spills from water are summarized. Finally, the state of the art is summarized and promising future developments of hydrophobic MOFs are highlighted.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Cu9.1Te4Cl3: A Thermoelectric Compound with Low Thermal and High Electrical Conductivity},

author = {A Vogel and T Miller and C Hoch and M Jakob and O Oeckler and T Nilges},

url = {https://doi.org/10.1021/acs.inorgchem.9b00453},

doi = {10.1021/acs.inorgchem.9b00453},

issn = {0020-1669},

year  = {2019},

date = {2019-05-06},

journal = {Inorganic Chemistry},

volume = {58},

number = {9},

pages = {6222-6230},

abstract = {Cu9.1Te4Cl3 is a new polymorphic compound in the class of coinage metal polytelluride halides. Copper is highly mobile, which results in multiple order\textendashdisorder phase transitions in a limited temperature interval from 240 to 370 K. Mainly as a consequence of thermal transport properties, the compound’s thermoelectric figure of merit reaches values up to ZT = 0.15 in the temperature range between room temperature and 523 K. Its structure is closely related to that of Ag10Te4Br3, another coinage metal polytelluride halide, which represents the first p\textendashn\textendashp-switchable semiconductor approachable by a simple temperature change. The title compound outperforms Ag10Te4Br3 in terms of thermoelectric properties by 1 order of magnitude and therefore acts as a link between the class of p\textendashn\textendashp compounds and thermoelectric materials.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Oriented Thin Films of Electroactive Triphenylene Catecholate-Based Two-Dimensional Metal\textendashOrganic Frameworks},

author = {A M\"{a}hringer and A C Jakowetz and J M Rotter and B J Bohn and J K Stolarczyk and J Feldmann and T Bein and D D Medina},

url = {https://doi.org/10.1021/acsnano.9b01137},

doi = {10.1021/acsnano.9b01137},

issn = {1936-0851},

year  = {2019},

date = {2019-05-02},

journal = {ACS Nano},

volume = {13},

number = {6},

pages = {6711-6719},

abstract = {Two-dimensional triphenylene-based metal\textendashorganic frameworks (TP-MOFs) attract significant scientific interest due to their long-range order combined with significant electrical conductivity. The deposition of these structures as oriented films is expected to promote their incorporation into diverse optoelectronic devices. However, to date, a controlled deposition strategy applicable for the different members of this MOF family has not been reported yet. Herein, we present the synthesis of highly oriented thin films of TP-MOFs by vapor-assisted conversion (VAC). We targeted the M-CAT-1 series comprising hexahydroxytriphenylene organic ligands and metal-ions such as Ni2+, Co2+, and Cu2+. These planar organic building blocks are connected in-plane to the metal-ions through a square planar node forming extended sheets which undergo self-organization into defined stacks. Highly oriented thin Ni- and Co-CAT-1 films grown on gold substrates feature a high surface coverage with a uniform film topography and thickness ranging from 180 to 200 nm. The inclusion of acid modulators in the synthesis enabled the growth of films with a preferred orientation on quartz and on conductive substrates such as indium-doped tin oxide (ITO). The van der Pauw measurements performed across the M-CAT-1 films revealed high electrical conductivity values of up to 10\textendash3 S cm\textendash1 for both the Ni- and Co-CAT-1 films. Films grown on quartz allowed for a detailed photophysical characterization by means of UV\textendashvis, photoluminescence, and transient absorption spectroscopy. The latter revealed the existence of excited states on a nanosecond time scale, sufficiently long to demonstrate a photoinduced charge generation and extraction in Ni-CAT-1 films. This was achieved by fabricating a basic photovoltaic device with an ITO/Ni-CAT-1/Al architecture, thus establishing this MOF as a photoactive material. Our results point to the intriguing capabilities of these conductive M-CAT-1 materials and an additional scope of applications as photoabsorbers enabled through VAC thin-film synthesis.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Monitoring the morphological evolution in mixed-dimensional lead bromide perovskite films with lamellar-stacked perovskite nanoplatelets},

author = {R Wang and Y Tong and K Wang and S Xia and E Kentzinger and O Soltwedel and P M\"{u}ller-Buschbaum and H Frielinghaus},

url = {http://dx.doi.org/10.1039/C9NH00156E},

doi = {10.1039/C9NH00156E},

issn = {2055-6756},

year  = {2019},

date = {2019-04-23},

journal = {Nanoscale Horizons},

volume = {4},

number = {5},

pages = {1139-1144},

abstract = {Mixed-dimensional lead bromide perovskite films combine the properties of both three-dimensional (3D) and two-dimensional (2D) perovskite crystals, and due to their good humidity tolerance, they emerge as promising candidates for long-term stable optoelectronic applications. In order to further tailor the film morphology aiming for a better device performance, it is important to unravel the structural formation mechanism in these perovskite thin films. In the present study, the formation of 3D lead bromide perovskite crystals and the self-assembly of lamellar-stacked 2D perovskite nanoplatelets are comprehensively studied. Samples are prepared through a two-step vapor assisted route with different vapor exposure times in order to monitor the detailed morphology at the specific reaction stage. With grazing incidence X-ray scattering techniques, the preferential orientation of the 3D crystals is found to decrease upon increasing the reaction time. Also, it is evidenced that well-ordered in-plane lamellar-stacked 2D nanoplatelets form aggregates in the bulk structure only. The obtained hierarchical morphology shows excellent structural stability in a humid atmosphere even at a relative humidity level of 80%. Our findings statistically offer a morphological understanding, which is important for the optimization of the sample preparation route and thus the resulting performance of moisture-tolerant perovskite based optoelectronic devices.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Tuning the optical bandgap in layered hybrid perovskites through variation of alkyl chain length},

author = {J A Sichert and A Hemmerling and C Cardenas-Daw and A S Urban and J Feldmann},

url = {\<Go to ISI\>://WOS:000466615300017},

doi = {10.1063/1.5087296},

issn = {2166-532X},

year  = {2019},

date = {2019-04-16},

journal = {Apl Materials},

volume = {7},

number = {4},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Structure and Charge Carrier Dynamics in Colloidal PbS Quantum Dot Solids},

author = {W Chen and J L Zhong and J Z Li and N Saxena and L P Kreuzer and H C Liu and L Song and B Su and D Yang and K Wang and J Schlipf and V Korstgens and T C He and K Wang and P Muller-Buschbaum},

url = {\<Go to ISI\>://WOS:000466991300006},

doi = {10.1021/acs.jpclett.9b00869},

issn = {1948-7185},

year  = {2019},

date = {2019-04-09},

urldate = {2019-04-09},

journal = {Journal of Physical Chemistry Letters},

volume = {10},

number = {9},

pages = {2058-2065},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Unprecedented High Oxygen Evolution Activity of Electrocatalysts Derived from Surface-Mounted Metal\textendashOrganic Frameworks},

author = {W Li and S Watzele and H A El-Sayed and Y Liang and G Kieslich and A S Bandarenka and K Rodewald and B Rieger and R A Fischer},

url = {https://doi.org/10.1021/jacs.9b00549},

doi = {10.1021/jacs.9b00549},

issn = {0002-7863},

year  = {2019},

date = {2019-03-19},

journal = {Journal of the American Chemical Society},

volume = {141},

number = {14},

pages = {5926-5933},

abstract = {The oxygen evolution reaction (OER) is a key process for renewable energy storage. However, developing non-noble metal OER electrocatalysts with high activity, long durability and scalability remains a major challenge. Herein, high OER activity and stability in alkaline solution were discovered for mixed nickel/cobalt hydroxide electrocatalysts, which were derived in one-step procedure from oriented surface-mounted metal\textendashorganic framework (SURMOF) thin films that had been directly grown layer-by-layer on macro- and microelectrode substrates. The obtained mass activity of ∼2.5 mA·μg\textendash1 at the defined overpotential of 300 mV is 1 order of magnitude higher than that of the benchmarked IrO2 electrocatalyst and at least 3.5 times higher than the mass activity of any state-of-the-art NiFe-, FeCoW-, or NiCo-based electrocatalysts reported in the literature. The excellent morphology of the SURMOF-derived ultrathin electrocatalyst coating led to a high exposure of the most active Ni- and Co-based sites.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Flexible and Ultrasoft Inorganic 1D Semiconductor and Heterostructure Systems Based on SnIP},

author = {C Ott and F Reiter and M Baumgartner and M Pielmeier and A Vogel and P Walke and S Burger and M Ehrenreich and G Kieslich and D Daisenberger and J Armstrong and U K Thakur and P Kumar and S Chen and D Donadio and L S Walter and R T Weitz and K Shankar and T Nilges},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.201900233},

doi = {10.1002/adfm.201900233},

issn = {1616-301X},

year  = {2019},

date = {2019-03-13},

journal = {Advanced Functional Materials},

volume = {29},

number = {18},

pages = {1900233},

abstract = {Abstract Low dimensionality and high flexibility are key demands for flexible electronic semiconductor devices. SnIP, the first atomic-scale double helical semiconductor combines structural anisotropy and robustness with exceptional electronic properties. The benefit of the double helix, combined with a diverse structure on the nanoscale, ranging from strong covalent bonding to weak van der Waals interactions, and the large structure and property anisotropy offer substantial potential for applications in energy conversion and water splitting. It represents the next logical step in downscaling the inorganic semiconductors from classical 3D systems, via 2D semiconductors like MXenes or transition metal dichalcogenides, to the first downsizeable, polymer-like atomic-scale 1D semiconductor SnIP. SnIP shows intriguing mechanical properties featuring a bulk modulus three times lower than any IV, III-V, or II-VI semiconductor. In situ bending tests substantiate that pure SnIP fibers can be bent without an effect on their bonding properties. Organic and inorganic hybrids are prepared illustrating that SnIP is a candidate to fabricate flexible 1D composites for energy conversion and water splitting applications. SnIP@C3N4 hybrid forms an unusual soft material core\textendashshell topology with graphenic carbon nitride wrapping around SnIP. A 1D van der Waals heterostructure is formed capable of performing effective water splitting.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{,

title = {Carbonaceous Oxygen Evolution Reaction Catalysts: From Defect and Doping-Induced Activity over Hybrid Compounds to Ordered Framework Structures},

author = {F Zoller and S H\"{a}ringer and D B\"{o}hm and J Luxa and Z Sofer and D Fattakhova-Rohlfing},

doi = {10.1002/smll.202007484},

issn = {1613-6810},

journal = {Small},

pages = {e2007484},

abstract = {Oxygen evolution reaction (OER) is expected to be of great importance for the future energy conversion and storage in form of hydrogen by water electrolysis. Besides the traditional noble-metal or transition metal oxide-based catalysts, carbonaceous electrocatalysts are of great interest due to their huge structural and compositional variety and unrestricted abundance. This review provides a summary of recent advances in the field of carbon-based OER catalysts ranging from "pure" or unintentionally doped carbon allotropes over heteroatom-doped carbonaceous materials and carbon/transition metal compounds to metal oxide composites where the role of carbon is mainly assigned to be a conductive support. Furthermore, the review discusses the recent developments in the field of ordered carbon framework structures (metal organic framework and covalent organic framework structures) that potentially allow a rational design of heteroatom-doped 3D porous structures with defined composition and spatial arrangement of doping atoms to deepen the understanding on the OER mechanism on carbonaceous structures in the future. Besides introducing the structural and compositional origin of electrochemical activity, the review discusses the mechanism of the catalytic activity of carbonaceous materials, their stability under OER conditions, and potential synergistic effects in combination with metal (or metal oxide) co-catalysts.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Optoelectronics Meets Optoionics: Light Storing Carbon Nitrides and Beyond},

author = {F Podjaski and B V Lotsch},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202003049},

doi = {https://doi.org/10.1002/aenm.202003049},

issn = {1614-6832},

journal = {Advanced Energy Materials},

volume = {11},

number = {4},

pages = {2003049},

abstract = {Abstract Known for decades, Liebig's carbon nitrides have evolved into a burgeoning class of macromolecular semiconductors over the past 10+ years, front and center of many efforts revolving around the discovery of resource-efficient and high-performance photocatalysts for solar fuel generation. The recent discovery of a new class of “ionic” 2D carbon nitrides\textemdashpoly(heptazine imide) (PHI)\textemdashhas given new momentum to this field, driven both by unconventional properties and the prospect of new applications at the intersection between solar energy conversion and electrochemical energy storage. In this essay, key concepts of the emerging field of optoionics are delineated and the “light storing” ability of PHI-type carbon nitrides is rationalized by an intricate interplay between their optoelectronic and optoionic properties. Based on these insights, key characteristics and general principles for the de novo design of optoionic materials across the periodic table are derived, opening up new research avenues such as “dark photocatalysis”, direct solar batteries, light-driven autonomous systems, and photomemristive devices.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Quantitative electric field mapping between electrically biased needles by scanning transmission electron microscopy and electron holography},

author = {J F Dushimineza and J Jo and R E Dunin-Borkowski and K M\"{u}ller-Caspary},

url = {https://www.sciencedirect.com/science/article/pii/S0304399123001250},

doi = {https://doi.org/10.1016/j.ultramic.2023.113808},

issn = {0304-3991},

journal = {Ultramicroscopy},

volume = {253},

pages = {113808},

abstract = {Stray electric fields in free space generated by two biased gold needles have been quantified in comprehensive finite-element (FE) simulations, accompanied by first moment (FM) scanning TEM (STEM) and electron holography (EH) experiments. The projected electrostatic potential and electric field have been derived numerically under geometrical variations of the needle setup. In contrast to the FE simulation, application of an analytical model based on line charges yields a qualitative understanding. By experimentally probing the electric field employing FM STEM and EH under alike conditions, a discrepancy of about 60% became apparent initially. However, the EH setup suggests the reconstructed phase to be significantly affected by the perturbed reference wave effect, opposite to STEM where the field-free reference was recorded subsequently with unbiased needles in which possibly remaining electrostatic influences are regarded as being minor. In that respect, the observed discrepancy between FM imaging and EH is resolved after including the long-range potential landscape from FE simulations into the phase of the reference wave in EH.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Mechanistic Insights into ZIF-8 Encapsulation of Atom-Precise Pt(M) Carbonyl Clusters},

author = {K L Kollmannsberger and Poonam and C Cesari and R Khare and T Kratky and M Boniface and O Tomanec and J Michali\v{c}ka and E Mosconi and A Gagliardi and S G\"{u}nther and W Kaiser and T Lunkenbein and S Zacchini and J Warnan and R A Fischer},

url = {https://doi.org/10.1021/acs.chemmater.3c00807},

doi = {10.1021/acs.chemmater.3c00807},

issn = {0897-4756},

journal = {Chemistry of Materials},

volume = {35},

number = {14},

pages = {5475-5486},

abstract = {Precisely designing metal nanoparticles (NPs) is the cornerstone for maximizing their efficiency in applications like catalysis or sensor technology. Metal\textendashorganic frameworks (MOFs) with their defined and tunable pore systems provide a confined space to host and stabilize small metal NPs. In this work, the MOF encapsulation of various atom-precise clusters following the bottle-around-ship approach is investigated, providing general insights into the scaffolding mechanism. Eleven carbonyl-stabilized Pt(M) (M = Co, Ni, Fe, and Sn) clusters are employed for the encapsulation in the zeolitic imidazolate framework (ZIF)-8. Infrared and UV/Vis spectroscopy, density functional theory, and ab initio molecular dynamics revealed structure\textendashencapsulation relationship guidelines. Thereby, cluster polarization, size, and composition were found to condition the scaffolding behavior. Encaging of [NBnMe3]2[Co8Pt4C2(CO)24] (Co8Pt4) is thus achieved as the first MOF-encapsulated bimetallic carbonyl cluster, Co8Pt4@ZIF-8, and is fully characterized including X-ray absorption near edge and extended X-ray absorption spectroscopy. ZIF-8 confinement not only promotes property changes, like the T-dependent magnetism, but it also further allows heat-induced ligand-stripping without altering the cluster size, enabling the synthesis of naked, heterometallic, close to atom-precise clusters.},

keywords = {Foundry Inorganic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Dynamical scattering in ice-embedded proteins in conventional and scanning transmission electron microscopy},

author = {M L Leidl and C Sachse and K Muller-Caspary},

url = {https://doi.org/10.1107/S2052252523004505},

doi = {doi:10.1107/S2052252523004505},

issn = {2052-2525},

journal = {IUCrJ},

volume = {10},

number = {4},

pages = {475-486},

abstract = {Structure determination of biological macromolecules using cryogenic electron microscopy is based on applying the phase object (PO) assumption and the weak phase object (WPO) approximation to reconstruct the 3D potential density of the molecule. To enhance the understanding of image formation of protein complexes embedded in glass-like ice in a transmission electron microscope, this study addresses multiple scattering in tobacco mosaic virus (TMV) specimens. This includes the propagation inside the molecule while also accounting for the effect of structural noise. The atoms in biological macromolecules are light but are distributed over several nanometres. Commonly, PO and WPO approximations are used in most simulations and reconstruction models. Therefore, dynamical multislice simulations of TMV specimens embedded in glass-like ice were performed based on fully atomistic molecular-dynamics simulations. In the first part, the impact of multiple scattering is studied using different numbers of slices. In the second part, different sample thicknesses of the ice-embedded TMV are considered in terms of additional ice layers. It is found that single-slice models yield full frequency transfer up to a resolution of 2.5 A, followed by attenuation up to 1.4 A. Three slices are sufficient to reach an information transfer up to 1.0 A. In the third part, ptychographic reconstructions based on scanning transmission electron microscopy (STEM) and single-slice models are compared with conventional TEM simulations. The ptychographic reconstructions do not need the deliberate introduction of aberrations, are capable of post-acquisition aberration correction and promise benefits for information transfer, especially at resolutions beyond 1.8 A.},

keywords = {Foundry Inorganic, Foundry Organic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Fine-Tuning Blue-Emitting Halide Perovskite Nanocrystals},

author = {S Martin and N A Henke and C Lampe and M D\"{o}blinger and K Frank and P Ganswindt and B Nickel and A S Urban},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.202301009},

doi = {https://doi.org/10.1002/adom.202301009},

issn = {2195-1071},

journal = {Advanced Optical Materials},

volume = {n/a},

number = {n/a},

pages = {2301009},

abstract = {Abstract Lead halide perovskite nanocrystals (NCs) with narrow, bright emission in the visible range are promising candidates for light-emitting applications. Near-unity quantum yields have been realized for green and red-emitting perovskites, but efficient, stable blue-emitting perovskite materials are scarce. Current methods to synthesize quantum-confined CsPbBr3 NCs with blue emission are limited to specific wavelength ranges and still suffer from inhomogeneously broadened emission profiles. Herein, anisotropic blue-green emitting CsPbBr3 NCs are synthesized in ambient atmosphere using a spontaneous crystallization method. Optical spectroscopy reveals a gradual, asymptotic photoluminescence (PL) redshift of pristine colloidal NCs after synthesis. During this process, the emission quality improves notably as the PL spectra become narrower and more symmetric, accompanied by a PL intensity increase. Electron microscopy indicates that the gradual redshift stems from an isotropic growth of the CsPbBr3 NCs in at least two dimensions, likely due to residual precursor ions in the dispersion. Most importantly, the growth process can be halted at any point by injecting an enhancement solution containing PbBr2 and organic capping ligands. Thus, excellent control over NC size is achieved, allowing for nanometer-precise tunability of the respective emission wavelength in the range between 475 and 500 nm, enhancing the functionality of these already impressive NCs.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Intrinsic strong light-matter coupling with self-hybridized bound states in the continuum in van der Waals metasurfaces},

author = {T Weber and L K\"{u}hner and L Sortino and A Ben Mhenni and N P Wilson and J K\"{u}hne and J J Finley and S A Maier and A Tittl},

url = {https://doi.org/10.1038/s41563-023-01580-7},

doi = {10.1038/s41563-023-01580-7},

issn = {1476-4660},

journal = {Nature Materials},

volume = {22},

number = {8},

pages = {970-976},

abstract = {Photonic bound states in the continuum (BICs) provide a standout platform for strong light-matter coupling with transition metal dichalcogenides (TMDCs) but have so far mostly been implemented as traditional all-dielectric metasurfaces with adjacent TMDC layers, incurring limitations related to strain, mode overlap and material integration. Here, we demonstrate intrinsic strong coupling in BIC-driven metasurfaces composed of nanostructured bulk tungsten disulfide (WS2) and exhibiting resonances with sharp, tailored linewidths and selective enhancement of light-matter interactions. Tuning of the BIC resonances across the exciton resonance in bulk WS2 is achieved by varying the metasurface unit cells, enabling strong coupling with an anticrossing pattern and a Rabi splitting of 116 meV. Crucially, the coupling strength itself can be controlled and is shown to be independent of material-intrinsic losses. Our self-hybridized metasurface platform can readily incorporate other TMDCs or excitonic materials to deliver fundamental insights and practical device concepts for polaritonic applications.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Active Loss Engineering in Vanadium Dioxide Based BIC Metasurfaces},

author = {A Aigner and F Ligmajer and K Rovensk\'{a} and J Holobr\'{a}dek and B Idesov\'{a} and S A Maier and A Tittl and L D S Menezes},

url = {https://arxiv.org/abs/2312.00547},

doi = {https://doi.org/10.48550/arXiv.2312.00547},

journal = {arXiv preprint arXiv:2312.00547},

abstract = {Metasurfaces have unlocked significant advancements across photonics, yet their efficient active control remains challenging. The active materials required often lack continuous tunability, exhibit inadequate refractive index (RI) changes, or suffer from high losses. These aspects pose an inherent limitation for resonance-shifting based switching: when RI changes are small, the resulting shift is also minor. Conversely, high RI changes typically come with high intrinsic losses necessitating broad modes because narrow ones cannot tolerate such losses. Therefore, larger spectral shifts are required to effectively detune the modes. This paper introduces a novel active metasurface approach that converts the constraint of high intrinsic losses into a beneficial feature. This is achieved by controlling the losses in a hybrid vanadium dioxide (VO2) - silicon metasurface, supporting symmetry-protected bound states in the continuum (BICs) within the infrared spectrum. By leveraging the temperature-controlled losses in VO2 and combining them with the inherent far-field-coupling tunability of BICs, we gain unprecedented precision in independently controlling both the radiative and nonradiative losses of the resonant system. Our dual-control mechanism allows us to optimize our metasurfaces and we experimentally demonstrate quality factors above 200, a maximum reflectance amplitude of 90%, a relative switching contrast of 78%, and continuous tuning from under- to over-coupling within the infrared spectral range. This study provides a foundation for experimentally and technologically simple, fine-tunable, active metasurfaces for applications ranging from molecular sensors to filters and optical modulators.},

keywords = {Foundry Inorganic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Engineering Defects and Interfaces of Atomic Layer-Deposited TiOx-Protective Coatings for Efficient III\textendashV Semiconductor Photocathodes},

author = {O Bienek and B Fuchs and M Kuhl and T Rieth and J K\"{u}hne and L I Wagner and L M Todenhagen and L Wolz and A Henning and I D Sharp},

url = {https://doi.org/10.1021/acsphotonics.3c00818},

doi = {10.1021/acsphotonics.3c00818},

journal = {ACS Photonics},

volume = {10},

number = {11},

pages = {3985-3997},

abstract = {III\textendashV compound semiconductors offer optoelectronic properties that are well suited for the conversion of solar energy to chemical fuels. While such materials suffer from poor stability under photoelectrochemical (PEC) conditions, atomic layer deposition (ALD) of titanium oxide (TiOx) has emerged as a powerful approach for creating corrosion protection layers, thereby enabling efficient and robust interfaces. However, the role of defects within TiOx layers and at the semiconductor/TiOx interface on the PEC performance remains poorly understood and controlled. Here, we use p-type InP as a model III\textendashV semiconductor to investigate the impact of defects in ALD TiOx on junction formation, interfacial charge transport, and photocarrier recombination, which underpin characteristics of PEC devices. We show that defect concentrations in TiOx can be tuned over a broad range, resulting in significant modulation of the optical constants, electrical conductivity, and interface chemistry. While plasma-enhanced ALD yields films with low midgap-state concentrations, it introduces series resistance losses due to oxidation of the substrate. In contrast, thermal ALD suppresses interface oxidation but leads to electronically active defect states within the band gap of TiOx. By controlling these defect states, the nature of junction formation can be tuned, and high photovoltage photocathodes can be achieved. In particular, ALD TiOx layers possessing high carrier concentrations form buried InP/TiOx pn heterojunctions, whereas less defective layers preserve semiconductor/electrolyte junction energetics to achieve large photovoltages and applied bias photon-to-current efficiencies. These results highlight the power of ALD for engineering photoelectrode interfaces and provide a new route for tailoring the junction formation between buried and PEC junctions.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Synergistic Defect Passivation by Metformin Halides for Improving Perovskite Solar Cell Performance},

author = {H Dong and G Shen and Y Zou and Y Li and Z Lin and Q Cai and X Xu and Q Song and H Duan and P M\"{u}ller-Buschbaum and C Mu},

url = {https://doi.org/10.1021/acs.jpcc.3c02121},

doi = {10.1021/acs.jpcc.3c02121},

issn = {1932-7447},

journal = {The Journal of Physical Chemistry C},

volume = {127},

number = {25},

pages = {11845-11853},

abstract = {Defect passivation plays a critical role in manufacturing high-performance perovskite solar cells (PSCs). Herein, engineered components of metformin halides are introduced to the bulk and surface of perovskite layers in PSCs to realize synergistic defect passivation. It is found that the bulk addition of metformin hydrochloride influences the orientation distribution of perovskite crystals and contributes to better perovskite films. Further, the modification of metformin iodide could treat residual defects on the surface of perovskite films. As a result, the synergistically passivated PSCs shows an improved power conversion efficiency (PCE), which increased from 19.36% to 22.17%, together with a higher short-circuit current and open-circuit voltage than those of the control device. Moreover, the as-treated PSCs exhibit excellent thermal and humidity stabilities, maintaining 95% of their initial PCE after being stored under air conditions for over 1000 h. This work provides a novel strategy to passivate perovskite defects and improve the PCE and stability of PSCs.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Toward a Comprehensive Understanding of Photocatalysis: What Systematic Studies and Alcohol Surface Chemistry on TiO2(110) Have to Offer for Future Developments},

author = {M Eder and M Tschurl and U Heiz},

url = {https://doi.org/10.1021/acs.jpclett.3c00504},

doi = {10.1021/acs.jpclett.3c00504},

journal = {The Journal of Physical Chemistry Letters},

volume = {14},

number = {26},

pages = {6193-6201},

abstract = {Heterogeneous photocatalytic systems are usually described based on electrochemistry, which the vast majority of interpretations and strategies for optimizing photocatalysts rely on. Charge carrier dynamics are usually in the spotlight, whereas the surface chemistry of the photocatalyst is neglected. This is unjustified, because studies on alcohol photoreforming on metal-decorated rutile single crystals revealed that the electrochemical reaction model is not generally applicable. Hence, many photocatalytic reactions may proceed in a different manner and the thermal chemistry needs to be accounted for. The new mechanism is particularly relevant for reactions in gaseous environments in the absence of solvated ionic species. Here, we compare both mechanisms and highlight their differences and consequences for photocatalysis. Based on alcohol photochemistry, we demonstrate the importance of thermal reactions in photocatalytic mechanisms and the relevance of systematic studies in different environments for a holistic understanding of photocatalysis.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Refining the Substrate Surface Morphology for Achieving Efficient Inverted Perovskite Solar Cells},

author = {R Guo and X Wang and X Jia and X Guo and J Li and Z Li and K Sun and X Jiang and E Alvianto and Z Shi and M Schwartzkopf and P M\"{u}ller-Buschbaum and Y Hou},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202302280},

doi = {https://doi.org/10.1002/aenm.202302280},

issn = {1614-6832},

journal = {Advanced Energy Materials},

volume = {13},

number = {43},

pages = {2302280},

abstract = {Abstract Significant advancements in perovskite solar cells (PSCs) have been driven by the engineering of the interface between perovskite absorbers and charge transport layers. Inverted PSCs offer substantial potential with their high power conversion efficiency (PCE) and enhanced compatibility for tandem solar cell applications. Conventional hole transport materials like poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) and poly(triaryl amine) (PTAA) not only constrain the PSC efficiency but also elevate their fabrication costs. In the case of improving inverted structured PSCs according to the aforementioned concerns, utilizing self-assembled monolayers (SAMs) as hole-transporting layers has played a crucial role. However, the growth of self-assembled monolayers on the substrates still limits the performance and reproducibility of inverted structured PSCs. In this study, the authors delve into the growth model of SAMs on different surface morphologies. Moreover, it is found that the plasma treatment can effectively regulate the surface morphologies of substrates and achieve conformal growth of SAMs. This treatment improves the uniformity and suppresses non-radiative recombination at the interface, which leads to a PCE of 24.5% (stabilized at 23.5%) for inverted structured PSCs.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Electrochemical impedance spectroscopy of PEM fuel cells at low hydrogen partial pressures: efficient cell tests for mass production},

author = {F Haimerl and S Kumar and M Heere and A S Bandarenka},

url = {http://dx.doi.org/10.1039/D3IM00075C},

doi = {10.1039/D3IM00075C},

issn = {2755-2608},

journal = {Industrial Chemistry \& Materials},

abstract = {Quality testing costs hinder the large-scale production of PEM fuel cell systems due to long testing times and high safety measures for hydrogen. While eliminating both issues, electrochemical impedance spectroscopy at low hydrogen concentrations can provide valuable insights into fuel cell processes. However, the influence of high anode stream dilutions on PEM fuel cell performance is not yet completely understood. This study presents a new equivalent circuit model to analyze impedance spectra at low hydrogen partial pressures. The proposed model accurately describes the impedance response and explains the performance decrease at low hydrogen concentrations. First, the reduced availability of hydrogen at the anode leads to rising reaction losses from the hydrogen side. Further, the resulting losses lead to potential changes also influencing the cathode processes. The findings indicate that impedance spectroscopy at low hydrogen partial pressure might provide a reliable fuel cell quality control tool, simplifying production processes, reducing costs, and mitigating risks in fuel cell production. Keywords: PEM fuel cells; Electrochemical impedance spectroscopy; EIS; Large scale PEMFC production; Anodes; Cathodes.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Insights into the effects of oriented crystallization on the performance of quasi-two-dimensional perovskite solar cells},

author = {R Jiang and T Tian and B Ke and Z Kou and P M\"{u}ller-Buschbaum and F Huang and Y-B Cheng and T Bu},

url = {https://www.sciencedirect.com/science/article/pii/S2949822823000448},

doi = {https://doi.org/10.1016/j.nxmate.2023.100044},

issn = {2949-8228},

journal = {Next Materials},

volume = {1},

number = {4},

pages = {100044},

abstract = {Long-term operational stability is one of the key problems for the commercialization of the perovskite photovoltaics. During the past decade, a tremendous amount of work has aimed at addressing the stability issues of perovskite solar cells (PSCs). Among them, the intrinsic instability of the ionic crystal structure of perovskite materials is foremost where proper strategies are highly required to complete the crystallization. Reducing the dimensional structure of the photoactive three-dimensional (3D) perovskites by the introduction of a non-photoactive two-dimensional (2D) perovskite phase is a rising topic recently, which generates a quasi-2D perovskite for improving the corresponding device stability. However, the power conversion efficiency (PCE) of quasi-2D perovskite solar cells decreases unfortunately with the increase of the 2D contents, which obviously depends on the orientation of the crystals. In this review, we first review the effect of the crystal orientation on the performance of quasi-2D PSCs. Then, the growth mechanism of the preferred crystal orientation is discussed in detail. The research progress of the modulation strategies which are key segments for the preferred oriented growth of quasi-2D perovskite crystals is summarized emphatically. Finally, we identify some challenges and opportunities for chasing efficient quasi-2D PSCs in furthering our understanding of the above themes.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Tailoring Low-Dimensional Phases for Improved Performance of 2D\textendash3D Tin Perovskite Solar Cells},

author = {Z Kang and Y Tong and K Wang and Y Chen and P Yan and G Pan and P M\"{u}ller-Buschbaum and L Zhang and Y Yang and J Wu and H Xie and S Liu and H Wang},

url = {https://doi.org/10.1021/acsmaterialslett.3c00929},

doi = {10.1021/acsmaterialslett.3c00929},

journal = {ACS Materials Letters},

pages = {1-9},

abstract = {2D\textendash3D tin perovskites are considered as promising candidates for realizing efficient lead-free perovskite solar cells (PSCs). However, the ultrathin 2D phases could unfavorably affect charge transport and device performance. In the present work, we demonstrate that the introduction of D-homoserine lactone hydrochloride (D-HLH) can tailor the low-dimensional phases and improve the quality of 2D\textendash3D tin perovskite films. The functional group in D-HLH can interact with FA+ and I\textendash as well as Sn2+ in the precursor solution. These interactions not only affect the formation of tin perovskite film and favor the formation of thicker 2D phases but also decrease the defect density and suppress the nonradiative recombination. As a result, the efficiency of tin PSCs is significantly improved from 7.97 to 12.45%, and the stability of the device is also enhanced. This work provides a feasible strategy to regulate the low-dimensional phases in 2D\textendash3D tin PSCs toward realizing high efficiency.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Mass transport and charge transfer through an electrified interface between metallic lithium and solid-state electrolytes},

author = {L Katzenmeier and M G\"{o}\sswein and L Carstensen and J Sterzinger and M Ederer and P M\"{u}ller-Buschbaum and A Gagliardi and A S Bandarenka},

url = {https://doi.org/10.1038/s42004-023-00923-4},

doi = {10.1038/s42004-023-00923-4},

issn = {2399-3669},

journal = {Communications Chemistry},

volume = {6},

number = {1},

pages = {124},

abstract = {All-solid-state Li-ion batteries are one of the most promising energy storage devices for future automotive applications as high energy density metallic Li anodes can be safely used. However, introducing solid-state electrolytes needs a better understanding of the forming electrified electrode/electrolyte interface to facilitate the charge and mass transport through it and design ever-high-performance batteries. This study investigates the interface between metallic lithium and solid-state electrolytes. Using spectroscopic ellipsometry, we detected the formation of the space charge depletion layers even in the presence of metallic Li. That is counterintuitive and has been a subject of intense debate in recent years. Using impedance measurements, we obtain key parameters characterizing these layers and, with the help of kinetic Monte Carlo simulations, construct a comprehensive model of the systems to gain insights into the mass transport and the underlying mechanisms of charge accumulation, which is crucial for developing high-performance solid-state batteries.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Automated, Consistent, and Even-handed Selection of Active Orbital Spaces for Quantum Embedding},

author = {E Kolodzeiski and C J Stein},

url = {https://arxiv.org/abs/2306.09488},

doi = {https://doi.org/10.48550/arXiv.2306.09488},

journal = {arXiv preprint arXiv:2306.09488},

abstract = {A widely used strategy to reduce the computational cost in quantum-chemical calculations is to partition the system into an active subsystem, which is the focus of the computational efforts and an environment that is treated at a lower computational level. The system partitioning is mostly based on localized molecular orbitals. When reaction paths or energy differences are to be calculated, it is crucial to keep the orbital space consistent for all structures. Inconsistencies in the orbital space can lead to unpredictable errors in the potential energy surface. While successful strategies to ensure this consistency have been established for organic and even metal-organic systems, these methods often fail for metal clusters or nanoparticles with a high density of near-degenerate and delocalized molecular orbitals. However, such systems are highly relevant for catalysis. Accurate yet feasible quantum-mechanical ab initio calculations are therefore highly desired. In this work, we present an approach based on the SPADE algorithm that allows us to ensure an automated and consistent partitioning even for systems with delocalized and near-degenerate molecular orbitals and demonstrate the validity of this method for the binding energies of small molecules on transition-metal clusters.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Fast-Charging Capability of Thin-Film Prussian Blue Analogue Electrodes for Aqueous Sodium-Ion Batteries},

author = {X Lamprecht and P Zellner and G Yesilbas and L Hromadko and P Moser and P Marzak and S Hou and R Haid and F Steinberger and T Steeger and J M Macak and A S Bandarenka},

url = {https://doi.org/10.1021/acsami.3c02633},

doi = {10.1021/acsami.3c02633},

issn = {1944-8244},

journal = {ACS Applied Materials \& Interfaces},

volume = {15},

number = {19},

pages = {23951-23962},

abstract = {Prussian blue analogues are considered as promising candidates for aqueous sodium-ion batteries providing a decently high energy density for stationary energy storage. However, suppose the operation of such materials under high-power conditions could be facilitated. In that case, their application might involve fast-response power grid stabilization and enable short-distance urban mobility due to fast re-charging. In this work, sodium nickel hexacyanoferrate thin-film electrodes are synthesized via a facile electrochemical deposition approach to form a model system for a robust investigation. Their fast-charging capability is systematically elaborated with regard to the electroactive material thickness in comparison to a ″traditional″ composite-type electrode. It is found that quasi-equilibrium kinetics allow extremely fast (dis)charging within a few seconds for sub-micron film thicknesses. Specifically, for a thickness below ≈ 500 nm, 90% of the capacity can be retained at a rate of 60C (1 min for full (dis)charge). A transition toward mass transport control is observed when further increasing the rate, with thicker films being dominated by this mode earlier than thinner films. This can be entirely attributed to the limiting effects of solid-state diffusion of Na+ within the electrode material. By presenting a PBA model cell yielding 25 Wh kg\textendash1 at up to 10 kW kg\textendash1, this work highlights a possible pathway toward the guided design of hybrid battery\textendashsupercapacitor systems. Furthermore, open challenges associated with thin-film electrodes are discussed, such as the role of parasitic side reactions, as well as increasing the mass loading.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Coherent Phonons in van der Waals MoSe2/WSe2 Heterobilayers},

author = {C Li and A V Scherbakov and P Soubelet and A K Samusev and C Ruppert and N Balakrishnan and V E Gusev and A V Stier and J J Finley and M Bayer and A V Akimov},

url = {https://doi.org/10.1021/acs.nanolett.3c02316},

doi = {10.1021/acs.nanolett.3c02316},

issn = {1530-6984},

journal = {Nano Letters},

volume = {23},

number = {17},

pages = {8186-8193},

abstract = {The increasing role of two-dimensional (2D) devices requires the development of new techniques for ultrafast control of physical properties in 2D van der Waals (vdW) nanolayers. A special feature of heterobilayers assembled from vdW monolayers is femtosecond separation of photoexcited electrons and holes between the neighboring layers, resulting in the formation of Coulomb force. Using laser pulses, we generate a 0.8 THz coherent breathing mode in MoSe2/WSe2 heterobilayers, which modulates the thickness of the heterobilayer and should modulate the photogenerated electric field in the vdW gap. While the phonon frequency and decay time are independent of the stacking angle between the MoSe2 and WSe2 monolayers, the amplitude decreases at intermediate angles, which is explained by a decrease in the photogenerated electric field between the layers. The modulation of the vdW gap by coherent phonons enables a new technology for the generation of THz radiation in 2D nanodevices with vdW heterobilayers.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Assessment of the Degradation Mechanisms of Cu Electrodes during the CO2 Reduction Reaction},

author = {R V Mom and L-E Sandoval-Diaz and D Gao and C-H Chuang and E A Carbonio and T E Jones and R Arrigo and D Ivanov and M H\"{a}vecker and B Roldan Cuenya and R Schl\"{o}gl and T Lunkenbein and A Knop-Gericke and J-J Velasco-V\'{e}lez},

url = {https://doi.org/10.1021/acsami.2c23007},

doi = {10.1021/acsami.2c23007},

issn = {1944-8244},

journal = {ACS Applied Materials \& Interfaces},

volume = {15},

number = {25},

pages = {30052-30059},

abstract = {Catalyst degradation and product selectivity changes are two of the key challenges in the electrochemical reduction of CO2 on copper electrodes. Yet, these aspects are often overlooked. Here, we combine in situ X-ray spectroscopy, in situ electron microscopy, and ex situ characterization techniques to follow the long-term evolution of the catalyst morphology, electronic structure, surface composition, activity, and product selectivity of Cu nanosized crystals during the CO2 reduction reaction. We found no changes in the electronic structure of the electrode under cathodic potentiostatic control over time, nor was there any build-up of contaminants. In contrast, the electrode morphology is modified by prolonged CO2 electroreduction, which transforms the initially faceted Cu particles into a rough/rounded structure. In conjunction with these morphological changes, the current increases and the selectivity changes from value-added hydrocarbons to less valuable side reaction products, i.e., hydrogen and CO. Hence, our results suggest that the stabilization of a faceted Cu morphology is pivotal for ensuring optimal long-term performance in the selective reduction of CO2 into hydrocarbons and oxygenated products.},

keywords = {Foundry Inorganic, Solid-Solid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Ionic Liquid-Induced Inversion of the Humidity-Dependent Conductivity of Thin PEDOT:PSS Films},

author = {A L Oechsle and T Sch\"{o}ner and L Deville and T Xiao and T Tian and A Vagias and S Bernstorff and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.3c08208},

doi = {10.1021/acsami.3c08208},

issn = {1944-8244},

journal = {ACS Applied Materials \& Interfaces},

volume = {15},

number = {40},

pages = {47682-47691},

abstract = {The humidity influence on the electronic and ionic resistance properties of thin post-treated poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) films is investigated. In particular, the resistance of these PEDOT:PSS films post-treated with three different concentrations (0, 0.05, and 0.35 M) of ethyl-3-methylimidazolium dicyanamide (EMIM DCA) is measured while being exposed to a defined humidity protocol. A resistance increase upon elevated humidity is observed for the 0 M reference sample, while the EMIM DCA post-treated samples demonstrate a reverse behavior. Simultaneously performed in situ grazing-incidence small-angle X-ray scattering (GISAXS) measurements evidence changes in the film morphology upon varying the humidity, namely, an increase in the PEDOT domain distances. This leads to a detriment in the interdomain hole transport, which causes a rise in the resistance, as observed for the 0 M reference sample. Finally, electrochemical impedance spectroscopy (EIS) measurements at different humidities reveal additional contributions of ionic charge carriers in the EMIM DCA post-treated PEDOT:PSS films. Therefrom, a model is proposed, which describes the hole and cation transport in different post-treated PEDOT:PSS films dependent on the ambient humidity.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Layer-By-Layer Printed Metal Hybrid (Cs:FA)PbI3 Perovskite Nanocrystal Solar Cells},

author = {M A Reus and A Krifa and Q A Akkerman and A Biewald and Z Xu and D P Kosbahn and C L Weindl and J Feldmann and A Hartschuh and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.202301008},

doi = {https://doi.org/10.1002/adom.202301008},

issn = {2195-1071},

journal = {Advanced Optical Materials},

volume = {n/a},

number = {n/a},

pages = {2301008},

abstract = {Abstract Mixed halide perovskite nanocrystals in the form of cesium/formamidinium lead triiodide ((Cs:FA)PbI3) offer great potential for efficient and stable solar cells. To date, large-scale production with roll-to-roll compatible deposition methods remains difficult and requires detailed research on each involved processing step. Here, a proof-of-concept study about slot-die coating (printing) the active layer of (Cs:FA)PbI3-based nanocrystal solar cells is presented. Structural and morphological changes during ligand exchange of long-chain oleic acid and oleylamine by Pb(NO3)2, and top-layer FAI passivation are investigated. Ligand exchange improves the processability of the nanocrystal layer and enhances charge transport. It also changes texture from face-on toward edge-on orientation as grazing-incidence X-ray scattering studies indicate. Ligand exchange and FAI passivation redshift photoluminescence and prolong charge carrier lifetime in the printed nanocrystal films. The proof-of-concept feasibility of printing metal halide perovskite nanocrystal films for solar cells is shown by building 20 devices with a median power conversion efficiency of 6.39%.},

keywords = {Foundry Inorganic},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Hot Electron Dynamics in InAs\textendashAlAsSb Core\textendashShell Nanowires},

author = {D Sandner and H Esmaielpour and F D Giudice and S Meder and M Nuber and R Kienberger and G Koblm\"{u}ller and H Iglev},

url = {https://doi.org/10.1021/acsaem.3c01565},

doi = {10.1021/acsaem.3c01565},

journal = {ACS Applied Energy Materials},

volume = {6},

number = {20},

pages = {10467-10474},

abstract = {Semiconductor nanowires (NWs) have shown evidence of robust hot-carrier effects due to their small dimensions, making them attractive for advanced photoenergy conversion concepts. Especially, indium arsenide (InAs) NWs are promising candidates for harvesting hot carriers due to their high absorption coefficient, high carrier mobility, and large effective electron-to-hole mass difference. Here, we investigate the cooling and recombination dynamics of photoexcited hot carriers in pure and passivated InAs NWs by using ultrafast near-infrared pump\textendashprobe spectroscopy. We observe reduced Auger recombination in pure InAs NWs compared to that in passivated ones and associate this with charge-carrier separation by surface band bending. Similarly, faster carrier cooling by electron\textendashhole scattering is observed in passivated InAs\textendashAlAsSb NWs at high carrier densities in excess of 1018 cm\textendash3, where hot electron lifetimes in this regime increase substantially with the pump fluence due to Auger heating. These results emphasize the importance of type-II alignment for charge-carrier separation in hot-carrier devices to suppress carrier-mediated cooling channels. In addition, a separate charge-carrier population lasting up to several nanoseconds is observed for photoexcitation of the NW shell. Despite the high conduction band offset, carrier migration is not observed in the range of 40 ps to 2 ns. This observation may open avenues for core\textendashshell NW multijunction solar cells.},

keywords = {Foundry Inorganic, Molecularly-Functionalized},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Elucidating the Active Sites and Synergies in Water Splitting on Manganese Oxide Nanosheets on Graphite Support},

author = {T O Schmidt and A Wark and R W Haid and R M Kluge and S Suzuki and K Kamiya and A S Bandarenka and J Maruyama and E Sk\'{u}lason},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202302039},

doi = {https://doi.org/10.1002/aenm.202302039},

issn = {1614-6832},

journal = {Advanced Energy Materials},

volume = {13},

number = {43},

pages = {2302039},

abstract = {Abstract Photosystem II is nature's solution for driving the oxygen evolution reaction to oxidize water. A manganese-oxide cluster is this protein's active center for water splitting, while the most efficient man-made catalysts are costly noble metal-based oxides. Facing the climate change, research on affordable and abundant electrocatalysts is crucial. To mimic the biological solution, manganese oxide nanosheets are synthesized and deposited on highly-oriented pyrolytic graphite. This electrocatalyst is then examined with spectroscopic and electrochemical measurements, electrochemical noise scanning tunneling microscopy, and density functional theory calculations. The detailed investigation assigns the origin of its enhanced water-splitting performance to detected activity at the nanosheet edges which the proposed mechanism explains further. Therefore, the results provide a blueprint for how to design efficient electrocatalysts for water oxidation with abundant materials.},

keywords = {Foundry Inorganic, Solid-Liquid},

pubstate = {published},

tppubtype = {article}

}