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Tuning the reactivity of semiconductor surfaces by functionalization with amines of different basicity.

Abstract：

:Surface functionalization of semiconductors has been the backbone of the newest developments in microelectronics, energy conversion, sensing device design, and many other fields of science and technology. Over a decade ago, the notion of viewing the surface itself as a chemical reagent in surface reactions was introduced, and adding a variety of new functionalities to the semiconductor surface has become a target of research for many groups. The electronic effects on the substrate have been considered as an important consequence of chemical modification. In this work, we shift the focus to the electronic properties of the functional groups attached to the surface and their role on subsequent reactivity. We investigate surface functionalization of clean Si(100)-2 × 1 and Ge(100)-2 × 1 surfaces with amines as a way to modify their reactivity and to fine tune this reactivity by considering the basicity of the attached functionality. The reactivity of silicon and germanium surfaces modified with ethylamine (CH(3)CH(2)NH(2)) and aniline (C(6)H(5)NH(2)) is predicted using density functional theory calculations of proton attachment to the nitrogen of the adsorbed amine to differ with respect to a nucleophilic attack of the surface species. These predictions are then tested using a model metalorganic reagent, tetrakis(dimethylamido)titanium (((CH(3))(2)N)(4)Ti, TDMAT), which undergoes a transamination reaction with sufficiently nucleophilic amines, and the reactivity tests confirm trends consistent with predicted basicities. The identity of the underlying semiconductor surface has a profound effect on the outcome of this reaction, and results comparing silicon and germanium are discussed.

journal_name

Proc Natl Acad Sci U S A

journal_title

Proceedings of the National Academy of Sciences of the United States of America

authors

Bent SF,Kachian JS,Rodríguez-Reyes JC,Teplyakov AV

doi

10.1073/pnas.1006656107

subject

Has Abstract

pub_date

2011-01-18 00:00:00

pages

956-60

issue

eissn

0027-8424

issn

1091-6490

pii

1006656107

journal_volume

108

pub_type

杂志文章

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Tuning the reactivity of semiconductor surfaces by functionalization with amines of different basicity.