Anisotropic Disorder and Thermal Stability of Silicane

Thumbnail Image
Ryan, Bradley J.
Roling, Luke T.
Major Professor
Committee Member
Journal Title
Journal ISSN
Volume Title
American Chemical Society
Research Projects
Organizational Units
Journal Issue
Is Version Of
Chemical and Biological Engineering
Atomically thin silicon nanosheets (SiNSs), such as silicane, have potential for next-generation computing paradigms, such as integrated photonics, owing to their efficient photoluminescence emission and complementary-metal-oxide-semiconductor (CMOS) compatibility. To be considered as a viable material for next-generation photonics, the SiNSs must retain their structural and optical properties at operating temperatures. However, the intersheet disorder of SiNSs and their nanoscale structure makes structural characterization difficult. Here, we use synchrotron X-ray diffraction and atomic pair distribution function (PDF) analysis to characterize the anisotropic disorder within SiNSs, demonstrating they exhibit disorder within the intersheet spacing, but have little translational or rotational disorder among adjacent SiNSs. Furthermore, we identify changes in their structural, chemical, and optical properties after being heated in an inert atmosphere up to 475 °C. We characterized changes of the annealed SiNSs using synchrotron-based total X-ray scattering, infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, electron paramagnetic resonance, absorbance, photoluminescence, and excited-state lifetime. We find that the silicon framework is robust, with an onset of amorphization at ∼300 °C, which is well above the required operating temperatures of photonic devices. Above ∼300 °C, we demonstrate that the SiNSs begin to coalesce while keeping their translational alignment to yield amorphous silicon nanosheets. In addition, our DFT results provide information on the structure, energetics, band structures, and vibrational properties of 11 distinct oxygen-containing SiNSs. Overall, these results provide critical information for the implementation of atomically thin silicon nanosheets in next-generation CMOS-compatible integrated photonic devices.
This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in ACS Nano, copyright © 2021 American Chemical Society after peer review. To access the final edited and published work see DOI: 10.1021/acsnano.1c04230. Posted with permission.
silicon nanosheets, pair distribution function, photonics, optoelectronic, density functional theory