Benzene and Pyridine on Silicon (001): A Trial Ground for Long Range Corrections in Density Functional Theory

被引：2

作者：

Warschkow, O. ^{[1
]}

Bennett, J. M. ^{[1
]}

Miwa, J. A. ^{[2
]}

Lopinski, G. P. ^{[3
]}

Rosei, F. ^{[4
]}

McKenzie, D. R. ^{[1
]}

Marks, N. A. ^{[5
,6
]}

机构：

[1] Univ Sydney, Sch Phys, Ctr Quantum Computat & Commun Technol, Sydney, NSW 2006, Australia

[2] Aarhus Univ, Interdisciplinary Nanosci Ctr iNano, Dept Phys & Astron, DK-8000 Aarhus C, Denmark

[3] Natl Res Council Canada, Measurement Sci & Stand, Ottawa, ON K1A 0R6, Canada

[4] Inst Natl Rech Sci Energie Mat & Telecommun, Varennes, PQ J3X 1S2, Canada

[5] Curtin Univ, Nanochem Res Inst, GPO Box U1987, Perth, WA 6845, Australia

[6] Curtin Univ, Discipline Phys & Astron, GPO Box U1987, Perth, WA 6845, Australia

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2017年 / 121卷 / 19期

基金：

澳大利亚研究理事会; 加拿大自然科学与工程研究理事会;

关键词：

GENERALIZED-GRADIENT-APPROXIMATION; SCANNING-TUNNELING-MICROSCOPY; ELECTRONIC-STRUCTURE; SURFACE-CHEMISTRY; SI(100) SURFACE; BINDING STATES; ADSORPTION; EXCHANGE; SI(001); ACCURACY;

D O I：

10.1021/acs.jpcc.7b03618

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The adsorption chemistry of benzene and pyridine on the silicon (001) surface is characterized by two prominent adsorbate configurations: a precursor structure bonded to a single Si Si dimer and a "tight-bridge" configuration that connects two adjacent dimers. We examine here the performance of 20 density functionals in predicting the relative stability of these two configurations. Discrepancies between the predicted and experimentally observed preferred structures highlight the importance of long-range exact-exchange terms in these adsorbate systems. These terms, however, tend to be detrimental to the prediction of adsorption and activation energies. We discuss this conundrum in terms of systematic exchange-correlation errors that scale with the number of molecule-surface bonds.

引用

页码：10484 / 10500

页数：17

共 80 条

[1] Toward control of surface reactions with a scanning tunneling microscope. Structure and dynamics of benzene desorption from a silicon surface [J].

Alavi, S ;

Rousseau, R ;

Seideman, T .

JOURNAL OF CHEMICAL PHYSICS, 2000, 113 (10) :4412-4423

[2]

[Anonymous], J CHEM PHYS

[3] DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].

BECKE, AD .

JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652

[4] Reaction pathways for pyridine adsorption on silicon (001) [J].

Bennett, J. M. ;

Marks, N. A. ;

Miwa, J. A. ;

Lopinski, G. P. ;

Rosei, F. ;

McKenzie, D. R. ;

Warschkow, O. .

JOURNAL OF PHYSICS-CONDENSED MATTER, 2015, 27 (05)

[5] Metastable adsorption of benzene on the Si(001) surface [J].

Borovsky, B ;

Krueger, M ;

Ganz, E .

PHYSICAL REVIEW B, 1998, 57 (08) :R4269-R4272

[6] Perspective on density functional theory [J].

Burke, Kieron .

JOURNAL OF CHEMICAL PHYSICS, 2012, 136 (15)

[7] Long-range corrected hybrid density functionals with damped atom-atom dispersion corrections [J].

Chai, Jeng-Da ;

Head-Gordon, Martin .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2008, 10 (44) :6615-6620

[8] Systematic optimization of long-range corrected hybrid density functionals [J].

Chai, Jeng-Da ;

Head-Gordon, Martin .

JOURNAL OF CHEMICAL PHYSICS, 2008, 128 (08)

[9] Insights into current limitations of density functional theory [J].

Cohen, Aron J. ;

Mori-Sanchez, Paula ;

Yang, Weitao .

SCIENCE, 2008, 321 (5890) :792-794

[10] Adsorption geometry of pyridine on the single domain Si(100)-2 x 1 surface: Fully polarization resolved NEXAFS [J].

Coustel, R. ;

Witkowski, N. .

JOURNAL OF PHYSICAL CHEMISTRY C, 2008, 112 (36) :14102-14107

← 1 2 3 4 5 6 7 8 →