Spontaneous S-Si bonding of alkanethiols to Si(111)-H: towards Si-molecule-Si circuits.

Chemical Science
Chandramalika R PeirisNadim Darwish

Abstract

We report the synthesis of covalently linked self-assembled monolayers (SAMs) on silicon surfaces, using mild conditions, in a way that is compatible with silicon-electronics fabrication technologies. In molecular electronics, SAMs of functional molecules tethered to gold via sulfur linkages dominate, but these devices are not robust in design and not amenable to scalable manufacture. Whereas covalent bonding to silicon has long been recognized as an attractive alternative, only formation processes involving high temperature and/or pressure, strong chemicals, or irradiation are known. To make molecular devices on silicon under mild conditions with properties reminiscent of Au-S ones, we exploit the susceptibility of thiols to oxidation by dissolved O2, initiating free-radical polymerization mechanisms without causing oxidative damage to the surface. Without thiols present, dissolved O2 would normally oxidize the silicon and hence reaction conditions such as these have been strenuously avoided in the past. The surface coverage on Si(111)-H is measured to be very high, 75% of a full monolayer, with density-functional theory calculations used to profile spontaneous reaction mechanisms. The impact of the Si-S chemistry in single-mo...Continue Reading

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Citations

Jul 10, 2021·The Journal of Chemical Physics·Yaling KeMichael Thoss
Oct 3, 2020·The Journal of Chemical Physics·Riley J PrestonDaniel S Kosov
Aug 4, 2021·ACS Applied Materials & Interfaces·Soraya RahpeimaNadim Darwish
Dec 4, 2020·Langmuir : the ACS Journal of Surfaces and Colloids·Essam M DiefNadim Darwish

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Methods Mentioned

BETA
X-ray
atomic force microscopy
AFM
scanning tunneling microscopy

Software Mentioned

LabVIEW
CasaXPS©
MOTOFIT
DUSHIN
VASP

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