Electronic Friction-Based Vibrational Lifetimes of Molecular Adsorbates: Beyond the Independent-Atom Approximation

被引：61

作者：

Rittmeyer, Simon P. ^{[1
,2
]}

Meyer, Joerg ^{[3
]}

Juaristi, J. Inaki ^{[4
,5
,6
]}

Reuter, Karsten ^{[1
,2
]}

机构：

[1] Tech Univ Munich, Chair Theoret Chem, D-85747 Garching, Germany

[2] Tech Univ Munich, Catalysis Res Ctr, D-85747 Garching, Germany

[3] Leiden Univ, Gorlaeus Labs, Leiden Inst Chem, NL-2300 RA Leiden, Netherlands

[4] Univ Basque Country, Fac Quim, Dept Fis Mat, San Sebastian 20080, Spain

[5] CSIC UPV EHU, CFM MPC, Ctr Fis Mat, San Sebastian 20018, Spain

[6] DIPC, San Sebastian 20018, Spain

来源：

PHYSICAL REVIEW LETTERS | 2015年 / 115卷 / 04期

基金：

欧洲研究理事会;

关键词：

STOPPING POWER; DESORPTION; DYNAMICS; GAS; EXCITATION; SCATTERING; RU(0001);

D O I：

10.1103/PhysRevLett.115.046102

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

We assess the accuracy of vibrational damping rates of diatomic adsorbates on metal surfaces as calculated within the local-density friction approximation (LDFA). An atoms-in-molecules (AIM) type charge partitioning scheme accounts for intramolecular contributions and overcomes the systematic underestimation of the nonadiabatic losses obtained within the prevalent independent-atom approximation. The quantitative agreement obtained with theoretical and experimental benchmark data suggests the LDFA-AIM scheme as an efficient and reliable approach to account for electronic dissipation in ab initio molecular dynamics simulations of surface chemical reactions.

引用

页数：5

共 47 条

[1] Exact Factorization of the Time-Dependent Electron-Nuclear Wave Function [J].

Abedi, Ali ;

Maitra, Neepa T. ;

Gross, E. K. U. .

PHYSICAL REVIEW LETTERS, 2010, 105 (12)

[2] Vibrational dynamics of adsorbates - Quo vadis? [J].

Arnolds, Heike .

PROGRESS IN SURFACE SCIENCE, 2011, 86 (1-2) :1-40

[3] SUBPICOSECOND TRANSIENT INFRARED-SPECTROSCOPY OF ADSORBATES - VIBRATIONAL DYNAMICS OF CO/PT(111) [J].

BECKERLE, JD ;

CAVANAGH, RR ;

CASASSA, MP ;

HEILWEIL, EJ ;

STEPHENSON, JC .

JOURNAL OF CHEMICAL PHYSICS, 1991, 95 (07) :5403-5418

[4] Electronic Friction Dominates Hydrogen Hot-Atom Relaxation on Pd(100) [J].

Blanco-Rey, M. ;

Juaristi, J. I. ;

Diez Muino, R. ;

Busnengo, H. F. ;

Kroes, G. J. ;

Alducin, M. .

PHYSICAL REVIEW LETTERS, 2014, 112 (10)

[5] First principles methods using CASTEP [J].

Clark, SJ ;

Segall, MD ;

Pickard, CJ ;

Hasnip, PJ ;

Probert, MJ ;

Refson, K ;

Payne, MC .

ZEITSCHRIFT FUR KRISTALLOGRAPHIE, 2005, 220 (5-6) :567-570

[6] Van der Waals density functional for general geometries -: art. no. 246401 [J].

Dion, M ;

Rydberg, H ;

Schröder, E ;

Langreth, DC ;

Lundqvist, BI .

PHYSICAL REVIEW LETTERS, 2004, 92 (24) :246401-1

[7] DENSITY FUNCTIONAL CALCULATION OF STOPPING POWER OF AN ELECTRON-GAS FOR SLOW IONS [J].

ECHENIQUE, PM ;

NIEMINEN, RM ;

RITCHIE, RH .

SOLID STATE COMMUNICATIONS, 1981, 37 (10) :779-781

[8] NONLINEAR STOPPING POWER OF AN ELECTRON-GAS FOR SLOW IONS [J].

ECHENIQUE, PM ;

NIEMINEN, RM ;

ASHLEY, JC ;

RITCHIE, RH .

PHYSICAL REVIEW A, 1986, 33 (02) :897-904

[9] The CO/Pt(111) puzzle [J].

Feibelman, PJ ;

Hammer, B ;

Norskov, JK ;

Wagner, F ;

Scheffler, M ;

Stumpf, R ;

Watwe, R ;

Dumesic, J .

JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (18) :4018-4025

[10] Vibrational lifetimes of cyanide and carbon monoxide on noble and transition metal surfaces [J].

Forsblom, Mattias ;

Persson, Mats .

JOURNAL OF CHEMICAL PHYSICS, 2007, 127 (15)

← 1 2 3 4 5 →