Syntheses and Molecular Structures of Liquid Pyrophoric Hydridosilanes

Gerwig, Maik; Böhme, Uwe; Friebel, Mike; Gründler, Franziska; Franze, Georg; Rosenkranz, Marco; Schmidt, Horst; Kroke, Edwin

doi:10.1002/open.202000152

Cited by 9 publications

(25 citation statements)

References 104 publications

(185 reference statements)

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“…[2,7] Based on the derived films, solar cells, [9] (photo)resistors, [5,7] and thin-film transistors were produced. [2,11,22] In the particular case of amorphous silicon thin films, hydrogen plays a predominant role for the passivation of defects. As the conversion processing typically drives out nearly all of the hydrogen, measures to restore the passivation of defects have to be undertaken.…”

Section: (3 Of 13)mentioning

confidence: 99%

“…A detailed structural comparison including single‐crystal X‐ray structures of trisilane, isotetrasilane, CHS, and NPS has recently been published. [ 11 ] The moderate deposition temperatures make it possible to prepare Si films also on sensitive substrates like paper and cardboard. [ 12 ] Furthermore, the liquid precursor can be mixed, e.g., with boron or phosphorous compounds to create doped films directly.…”

Section: Introductionmentioning

confidence: 99%

“…[ 11 ] In the latter case or when using formulations incorporating pure CPS or CHS, it is necessary to perform the polymerization of the film during or after deposition [ 7,11 ] to avoid massive material loss during subsequent drying or conversion steps. A crucial process for achieving the desired thin‐film functionality is the transformation of the deposit into amorphous or polycrystalline silicon which is usually done by thermal annealing, [ 5 ] photonic curing, [ 11 ] or combinations thereof (steps III and IV). [ 2,7 ] Based on the derived films, solar cells, [ 9 ] (photo)resistors, [ 5,7 ] and thin‐film transistors were produced.…”

Section: Introductionmentioning

confidence: 99%

“…Layers as thick as 300 nm were realized by doctor blading of pure CPS. [11] In the latter case or when using formulations incorporating pure CPS or CHS, it is necessary to perform the polymerization of Scheme 1. Trends for hydrosilanes with increasing number of Si atoms in a CVD process.…”

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From Cyclopentasilane to Thin‐Film Transistors

Gerwig

Ali

Neubert

et al. 2020

Adv Elect Materials

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Cyclopentasilane (CPS) has been studied as an liquid precursor for the deposition of thin silicon films for printed electronics and related applications. The processing involves a UV‐induced prepolymerization of CPS followed by liquid deposition and low‐temperature thermolysis. An insight into the oligomer and polymer formation including crosslinking in solution using 29Si NMR spectroscopy and electron spin resonance spectroscopy is reported. Formation of SiH (T‐units) and SiH3 (M‐units) is observed as well as short‐lived paramagnetic species. Additionally, the polymerization is followed by Raman spectroscopy. Reactive molecular dynamics simulations are applied to develop a theoretical model for the CPS‐ring‐opening and crosslinking steps. The experimental and computational data correspond well to each other and allow insight into the mechanism of polymer formation. The processing steps include spin‐coating, thermal drying, and conversion to amorphous silicon, H‐passivation, and fabrication of a CPS‐derived thin‐film transistor (TFT), without intermediate silicon crystallization. Further improvement is gained by using tetralene as a solvent, leading to a reduction of the time‐consuming polymerization step by one order of magnitude compared to cyclooctane. The overall quality and characteristics of the CPS‐derived spin‐coated silicon thin films correspond to standard plasma enhanced chemical vapor deposition‐derived devices with respect to performance levels.

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Section: (3 Of 13)mentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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confidence: 99%

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From Cyclopentasilane to Thin‐Film Transistors

Gerwig

Ali

Neubert

et al. 2020

Adv Elect Materials

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“…State of the art of in situ crystallization is summarized recently in a special issue of Zeitschrift fü r Kristallographie (Boese, 2014). We have performed several single-crystal structure determinations of pyrophoric liquids by in situ crystallization on the diffractometer (Schmidt et al, 2013;Gerwig et al 2020). With the experience gained in these processes, we were able to crystallize the title compound on the diffractometer and we report its crystal structure here.…”

Section: Structure Descriptionmentioning

confidence: 99%

(3,5-Dimethyl-1H-pyrazol-1-yl)trimethylsilane

Böhme

Bitto

2020

IUCrData

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The title compound, C8H16N2Si, crystallizes in the the orthorhombic space group P212121 with one molecule in the asymmetric unit. The Si—N bond is 1.782 (2) Å, which is substantially longer than is found in comparable (3,5-dimethylpyrazolyl)silanes. The trimethylsilyl group adopts a staggered conformation with respect to the planar 3,5-dimethylpyrazolyl unit. C—H...N hydrogen bonds between neighboring molecules form a strand of molecules along the b-axis direction.

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Challenges in the Synthesis and Processing of Hydrosilanes as Precursors for Silicon Deposition

Gerwig,

Böhme,

Friebel

2024

Chemistry A European J

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Liquid hydrosilanes are required for the production of silicon films. The silicon layers can be processed for electronic devices like transistors or thin‐film solar cells. Hydrosilanes are highly reactive and pyrophoric. Therefore, the synthesis of these compounds is challenging and dangerous. The available synthesis methods for hydrosilanes are reviewed and compared.Hydrosilanes are highly attractive compounds, which can be processed as liquids with printing technology to amorphous silicon films on nearly any solid substrate. The silicon layers can be processed for electronic devices like transistors or thin‐film solar cells. The endothermic character of hydrosilanes with their positive enthalpies of formation results in favorable properties for processing. The larger the molecules, the lower their decomposition temperature and the higher their photoactivity. Cyclic hydrosilanes such as cyclopentasilane and cyclohexasilane can be easily deposited. The branched neopentasilane is more difficult to deposit but yields better‐quality films after processing.The key challenge is the complex synthesis of the precursors and the hydrosilanes. The available preparative methods are presented in this review and their advantages and disadvantages are evaluated. The following synthesis methods are presented and discussed in this article: Wurtz coupling and other reductive coupling processes, dehydrogenative coupling of silanes, plasma synthesis of chlorinated polysilanes, amine‐ or chloride‐induced disproportionations, and transformation of monosilane to higher silanes.Plasma synthesis is already carried out today as a continuous industrial process. The most effective synthesis methods in the laboratory are currently amine‐ and chloride‐induced disproportionations. There is a great need to further optimize the syntheses of hydrosilanes and to develop new simple synthesis variants.

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Syntheses and Molecular Structures of Liquid Pyrophoric Hydridosilanes

Cited by 9 publications

References 104 publications

From Cyclopentasilane to Thin‐Film Transistors

From Cyclopentasilane to Thin‐Film Transistors

(3,5-Dimethyl-1H-pyrazol-1-yl)trimethylsilane

Challenges in the Synthesis and Processing of Hydrosilanes as Precursors for Silicon Deposition

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