Prof. Dr. Tom Nilges

- Polyphosphides
- Solid State Batteries and Ion Conductors
- Polymorphism, Phase Transitions, and Element Allotropes
- Recycling processes for Rare Earth Element capturing
- Thermoelectrics and Energy Materials
- Non-harmonic refinement of crystal structures
A Vogel, A Rabenbauer, P Deng, R Steib, T Böger, W G Zeier, R Siegel, J Senker, D Daisenberger, K Nisi, A W Holleitner, J Venturini, T Nilges
A Switchable One-Compound Diode Journal Article
In: Advanced Materials, vol. n/a, no. n/a, pp. 2208698, 2022, ISSN: 0935-9648.
@article{nokey,
title = {A Switchable One-Compound Diode},
author = {A Vogel and A Rabenbauer and P Deng and R Steib and T B\"{o}ger and W G Zeier and R Siegel and J Senker and D Daisenberger and K Nisi and A W Holleitner and J Venturini and T Nilges},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.202208698},
doi = {https://doi.org/10.1002/adma.202208698},
issn = {0935-9648},
year = {2022},
date = {2022-10-25},
journal = {Advanced Materials},
volume = {n/a},
number = {n/a},
pages = {2208698},
abstract = {Abstract A diode or transistor requires the combination of p- and n-type semiconductors or at least the defined formation of such areas within a given compound. This is a prerequisite for any IT application, energy conversion technology, and electronic semiconductor devices. Since 2009, when the first pnp-switchable compound Ag10Te4Br3 was described, it is in principle possible to fabricate a diode from a single material without adjusting the semiconduction type by a defined doping level. After this discovery, a handful of other materials that are capable of reversibly switching between these two semiconducting stages was reported. In all cases, a structural phase transition accompanied by a dynamic change of charge carriers or a charge density wave (CDW) within certain substructures are responsible for this effect. Unfortunately, a certain feature hinders the application of this phenomenon in convenient devices, namely the pnp-switching temperature, which generally occurs well above room temperature, between 364 and 580 K. This effect is far removed from a suitable operation temperature at ambient conditions. Here, we report on Ag18Cu3Te11Cl3, a room temperature pnp-switching material, and the realization of the first single-material position-independent diode. The title compound shows the highest ever reported Seebeck coefficient drop that takes place within a few Kelvin at room temperature. Combined with its reasonably low thermal conductivity, this material offers great application potential within an easily accessible and applicable temperature window. Ag18Cu3Te11Cl3 and pnp-switching materials have the potential for applications and processes where diodes, transistors, or any defined charge separation with junction formation are utilized. This article is protected by copyright. All rights reserved},
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F Reiter, M Pielmeier, A Vogel, C Jandl, M Plodinec, C Rohner, T Lunkenbein, K Nisi, A W Holleitner, T Nilges
SnBrP-A SnIP-type representative in the Sn−Br−P system Journal Article
In: Zeitschrift für anorganische und allgemeine Chemie, vol. n/a, no. n/a, pp. e202100347, 2022, ISSN: 0044-2313.
@article{nokey,
title = {SnBrP-A SnIP-type representative in the Sn−Br−P system},
author = {F Reiter and M Pielmeier and A Vogel and C Jandl and M Plodinec and C Rohner and T Lunkenbein and K Nisi and A W Holleitner and T Nilges},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/zaac.202100347},
doi = {https://doi.org/10.1002/zaac.202100347},
issn = {0044-2313},
year = {2022},
date = {2022-01-07},
urldate = {2022-01-07},
journal = {Zeitschrift f\"{u}r anorganische und allgemeine Chemie},
volume = {n/a},
number = {n/a},
pages = {e202100347},
abstract = {Abstract One-dimensional semiconductors are interesting materials due to their unique structural features and anisotropy, which grant them intriguing optical, dielectric and mechanical properties. In this work, we report on SnBrP, a lighter homologue of the first inorganic double helix compound SnIP. This class of compounds is characterized by intriguing mechanical and electronic properties, featuring a high flexibility without modulation of physical properties. Semiconducting SnBrP can be synthesized from red phosphorus, tin and tin(II)bromide at elevated temperatures and crystallizes as red-orange, cleavable needles. Raman measurements pointed towards a double helical building unit in SnBrP, showing similarities to the SnIP structure. After taking PL measurements, HR-TEM, and quantum chemical calculations into account, we were able to propose a sense full structure model for SnBrP.},
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pubstate = {published},
tppubtype = {article}
}
A Vogel, T Nilges
Ion Dynamics and Polymorphism in Cu20Te11Cl3 Journal Article
In: Inorganic Chemistry, vol. 60, no. 20, pp. 15233-15241, 2021, ISSN: 0020-1669.
@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.},
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D N Purschke, M R P Pielmeier, E Üzer, C Ott, C Jensen, A Degg, A Vogel, N Amer, T Nilges, F A Hegmann
Ultrafast Photoconductivity and Terahertz Vibrational Dynamics in Double-Helix SnIP Nanowires Journal Article
In: Advanced Materials, vol. n/a, no. n/a, pp. 2100978, 2021, ISSN: 0935-9648.
@article{,
title = {Ultrafast Photoconductivity and Terahertz Vibrational Dynamics in Double-Helix SnIP Nanowires},
author = {D N Purschke and M R P Pielmeier and E \"{U}zer and C Ott and C Jensen and A Degg and A Vogel and N Amer and T Nilges and F A Hegmann},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.202100978},
doi = {https://doi.org/10.1002/adma.202100978},
issn = {0935-9648},
year = {2021},
date = {2021-07-19},
journal = {Advanced Materials},
volume = {n/a},
number = {n/a},
pages = {2100978},
abstract = {Abstract Tin iodide phosphide (SnIP), an inorganic double-helix material, is a quasi-1D van der Waals semiconductor that shows promise in photocatalysis and flexible electronics. However, the understanding of the fundamental photophysics and charge transport dynamics of this new material is limited. Here, time-resolved terahertz (THz) spectroscopy is used to probe the transient photoconductivity of SnIP nanowire films and measure the carrier mobility. With insight into the highly anisotropic electronic structure from quantum chemical calculations, an electron mobility as high as 280 cm2 V−1s−1 along the double-helix axis and a hole mobility of 238 cm2 V−1 s−1 perpendicular to the double-helix axis are detected. Additionally, infrared-active (IR-active) THz vibrational modes are measured, which shows excellent agreement with first-principles calculations, and an ultrafast photoexcitation-induced charge redistribution is observed that reduces the amplitude of a twisting mode of the outer SnI helix on picosecond timescales. Finally, it is shown that the carrier lifetime and mobility are limited by a trap density greater than 1018 cm−3. The results provide insight into the optical excitation and relaxation pathways of SnIP and demonstrate a remarkably high carrier mobility for such a soft and flexible material, suggesting that it could be ideally suited for flexible electronics applications.},
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S Zhao, E Wang, E A Üzer, S Guo, R Qi, J Tan, K Watanabe, T Taniguchi, T Nilges, P Gao, Y Zhang, H-M Cheng, B Liu, X Zou, F Wang
Anisotropic moiré optical transitions in twisted monolayer/bilayer phosphorene heterostructures Journal Article
In: Nature Communications, vol. 12, no. 1, pp. 3947, 2021, ISSN: 2041-1723.
@article{nokey,
title = {Anisotropic moir\'{e} optical transitions in twisted monolayer/bilayer phosphorene heterostructures},
author = {S Zhao and E Wang and E A \"{U}zer and S Guo and R Qi and J Tan and K Watanabe and T Taniguchi and T Nilges and P Gao and Y Zhang and H-M Cheng and B Liu and X Zou and F Wang},
url = {https://doi.org/10.1038/s41467-021-24272-9},
doi = {10.1038/s41467-021-24272-9},
issn = {2041-1723},
year = {2021},
date = {2021-06-24},
journal = {Nature Communications},
volume = {12},
number = {1},
pages = {3947},
abstract = {Moir\'{e} superlattices of van der Waals heterostructures provide a powerful way to engineer electronic structures of two-dimensional materials. Many novel quantum phenomena have emerged in graphene and transition metal dichalcogenide moir\'{e} systems. Twisted phosphorene offers another attractive system to explore moir\'{e} physics because phosphorene features an anisotropic rectangular lattice, different from isotropic hexagonal lattices previously reported. Here we report emerging anisotropic moir\'{e} optical transitions in twisted monolayer/bilayer phosphorenes. The optical resonances in phosphorene moir\'{e} superlattice depend sensitively on twist angle and are completely different from those in the constitute monolayer and bilayer phosphorene even for a twist angle as large as 19°. Our calculations reveal that the Γ-point direct bandgap and the rectangular lattice of phosphorene give rise to the remarkably strong moir\'{e} physics in large-twist-angle phosphorene heterostructures. This work highlights fresh opportunities to explore moir\'{e} physics in phosphorene and other van der Waals heterostructures with different lattice configurations.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
M R P Pielmeier, T Nilges
Formation Mechanisms for Phosphorene and SnIP Journal Article
In: Angewandte Chemie International Edition, vol. n/a, no. n/a, 2021, ISSN: 1433-7851.
@article{,
title = {Formation Mechanisms for Phosphorene and SnIP},
author = {M R P Pielmeier and T Nilges},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202016257},
doi = {https://doi.org/10.1002/anie.202016257},
issn = {1433-7851},
year = {2021},
date = {2021-01-29},
journal = {Angewandte Chemie International Edition},
volume = {n/a},
number = {n/a},
abstract = {Abstract Phosphorene\textemdashthe monolayered material of the element allotrope black phosphorus (Pblack)\textemdashand SnIP are 2D and 1D semiconductors with intriguing physical properties. Pblack and SnIP have in common that they can be synthesized via short way transport or mineralization using tin, tin(IV) iodide and amorphous red phosphorus. This top-down approach is the most important access route to phosphorene. The two preparation routes are closely connected and differ mainly in reaction temperature and molar ratios of starting materials. Many speculative intermediates or activator side phases have been postulated especially for top-down Pblack/phosphorene synthesis, such as Hittorf's phosphorus or Sn24P19.3I8 clathrate. The importance of phosphorus-based 2D and 1D materials for energy conversion, storage, and catalysis inspired us to elucidate the formation mechanisms of these two compounds. Herein, we report on the reaction mechanisms of Pblack/phosphorene and SnIP from P4 and SnI2 via direct gas phase formation.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
A Vogel, T Miller, C Hoch, M Jakob, O Oeckler, T Nilges
Cu9.1Te4Cl3: A Thermoelectric Compound with Low Thermal and High Electrical Conductivity Journal Article
In: Inorganic Chemistry, vol. 58, no. 9, pp. 6222-6230, 2019, ISSN: 0020-1669.
@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 = {},
pubstate = {published},
tppubtype = {article}
}
C Ott, F Reiter, M Baumgartner, M Pielmeier, A Vogel, P Walke, S Burger, M Ehrenreich, G Kieslich, D Daisenberger, J Armstrong, U K Thakur, P Kumar, S Chen, D Donadio, L S Walter, R T Weitz, K Shankar, T Nilges
Flexible and Ultrasoft Inorganic 1D Semiconductor and Heterostructure Systems Based on SnIP Journal Article
In: Advanced Functional Materials, vol. 29, no. 18, pp. 1900233, 2019, ISSN: 1616-301X.
@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.},
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}