Angstrom-Resolved Interfacial Structure in Buried Organic-Inorganic Junctions

Schwartz, Craig P.; Raj, Sumana L.; Jamnuch, Sasawat; Hull, Chris J.; Miotti, Paolo; Lam, Royce K.; Nordlund, Dennis; Uzundal, Can B.; Das Pemmaraju, Chaitanya; Mincigrucci, Riccardo; Foglia, Laura; Simoncig, Alberto; Coreno, Marcello (ORCID:000000034376808X); Masciovecchio, Claudio; Giannessi, Luca; Poletto, Luca (ORCID:0000000209140531); Principi, Emiliano; Zuerch, Michael; Pascal, Tod A. (ORCID:0000000320961143); Drisdell, Walter S. (ORCID:0000000286934562); Saykally, Richard J. (ORCID:0000000189423656)

doi:10.1103/physrevlett.127.096801

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Angstrom-Resolved Interfacial Structure in Buried Organic-Inorganic Junctions

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Abstract

Charge transport processes at interfaces which are governed by complex interfacial electronic structure play a crucial role in catalytic reactions, energy storage, photovoltaics, and many biological processes. Here, the first soft X-ray second harmonic generation (SXR-SHG) interfacial spectrum of a buried interface (boron/Parylene-N) is reported. SXR-SHG shows distinct spectral features that are not observed in X-ray absorption spectra, demonstrating its extraordinary interfacial sensitivity. Comparison to electronic structure calculations indicates a boron-organic separation distance of 1.9 {\AA}, wherein changes as small as 0.1 {\AA} result in easily detectable SXR-SHG spectral shifts (ca. 100s of meV). As SXR-SHG is inherently ultrafast and sensitive to individual atomic layers, it creates the possibility to study a variety of interfacial processes, e.g. catalysis, with ultrafast time resolution and bond specificity.

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74 ATOMIC AND MOLECULAR PHYSICS Electronic structure Interfaces Nonlinear optics Surface reconstruction X-ray techniques

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Schwartz, Craig P., Raj, Sumana L., Jamnuch, Sasawat, Hull, Chris J., Miotti, Paolo, Lam, Royce K., Nordlund, Dennis, Uzundal, Can B., Das Pemmaraju, Chaitanya, Mincigrucci, Riccardo, Foglia, Laura, Simoncig, Alberto, Coreno, Marcello (ORCID:000000034376808X), Masciovecchio, Claudio, Giannessi, Luca, Poletto, Luca (ORCID:0000000209140531), Principi, Emiliano, Zuerch, Michael, Pascal, Tod A. (ORCID:0000000320961143), Drisdell, Walter S. (ORCID:0000000286934562), Saykally, Richard J. (ORCID:0000000189423656). 2021-08-24. Angstrom-Resolved Interfacial Structure in Buried Organic-Inorganic Junctions. https://doi.org/10.1103/physrevlett.127.096801

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