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. 2024 Apr 2;18(13):9557-9565.
doi: 10.1021/acsnano.3c12666. Epub 2024 Mar 4.

Photon-Momentum-Enabled Electronic Raman Scattering in Silicon Glass

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Photon-Momentum-Enabled Electronic Raman Scattering in Silicon Glass

Sergey S Kharintsev et al. ACS Nano. .
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Abstract

The nature of enhanced photoemission in disordered and amorphous solids is an intriguing question. A point in case is light emission in porous and nanostructured silicon, a phenomenon that is still not fully understood. In this work, we study structural photoemission in heterogeneous cross-linked silicon glass, a material that represents an intermediate state between the amorphous and crystalline phases, characterized by a narrow distribution of structure sizes. This model system shows a clear dependence of photoemission on size and disorder across a broad range of energies. While phonon-assisted indirect optical transitions are insufficient to describe observable emissions, our experiments suggest these can be understood through electronic Raman scattering instead. This phenomenon, which is not commonly observed in crystalline semiconductors, is driven by structural disorder. We attribute photoemission in this disordered system to the presence of an excess electron density of states within the forbidden gap (Urbach bridge) where electrons occupy trapped states. Transitions from gap states to the conduction band are facilitated through electron-photon momentum matching, which resembles Compton scattering but is observed for visible light and driven by the enhanced momentum of a photon confined within the nanostructured domains. We interpret the light emission in structured silicon glass as resulting from electronic Raman scattering. These findings emphasize the role of photon momentum in the optical response of solids that display disorder on the nanoscale.

Keywords: Compton scattering; Urbach bridge; electronic Raman scattering; photon momentum; semiconductor glass; structural optical spectroscopy.

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