NDLI: Apparent failure of the Born–Oppenheimer static surface model for vibrational excitation of molecular hydrogen on copper

Content Provider	PubMed Central
Author	Kroes, Geert-jan Díaz, Cristina Pijper, Ernst Olsen, Roar A. Auerbach, Daniel J.
Abstract	The accuracy of dynamical models for reactive scattering of molecular hydrogen, H2, from metal surfaces is relevant to the validation of first principles electronic structure methods for molecules interacting with metal surfaces. The ability to validate such methods is important to progress in modeling heterogeneous catalysis. Here, we study vibrational excitation of H2 on Cu(111) using the Born–Oppenheimer static surface model. The potential energy surface (PES) used was validated previously by calculations that reproduced experimental data on reaction and rotationally inelastic scattering in this system with chemical accuracy to within errors ≤ 1 kcal/mol ≈ 4.2 kJ/mol [Díaz C, et al. (2009) Science 326:832–834]. Using the same PES and model, our dynamics calculations underestimate the contribution of vibrational excitation to previously measured time-of-flight spectra of H2 scattered from Cu(111) by a factor 3. Given the accuracy of the PES for the experiments for which the Born–Oppenheimer static surface model is expected to hold, we argue that modeling the effect of the surface degrees of freedom will be necessary to describe vibrational excitation with similar high accuracy.
Related Links	http://dx.doi.org/10.1073/pnas.1001098107
Ending Page	20886
Page Count	6
Starting Page	20881
File Format	PDF
ISSN	00278424
e-ISSN	10916490
Journal	Proceedings of the National Academy of Sciences of the United States of America
Issue Number	49
Volume Number	107
Language	English
Publisher	National Academy of Sciences
Publisher Date	2010-12-07
Access Restriction	Open
Rights Holder	National Academy of Sciences
Subject Keyword	General Research in Higher Education
Content Type	Text
Resource Type	Article
Subject	Multidisciplinary

Sl.	Authority	Responsibilities	Communication Details
1	Ministry of Education (GoI), Department of Higher Education	Sanctioning Authority	https://www.education.gov.in/ict-initiatives
2	Indian Institute of Technology Kharagpur	Host Institute of the Project: The host institute of the project is responsible for providing infrastructure support and hosting the project	https://www.iitkgp.ac.in
3	National Digital Library of India Office, Indian Institute of Technology Kharagpur	The administrative and infrastructural headquarters of the project	Dr. B. Sutradhar bsutra@ndl.gov.in
4	Project PI / Joint PI	Principal Investigator and Joint Principal Investigators of the project	Dr. B. Sutradhar bsutra@ndl.gov.in Prof. Saswat Chakrabarti will be added soon
5	Website/Portal (Helpdesk)	Queries regarding NDLI and its services	support@ndl.gov.in
6	Contents and Copyright Issues	Queries related to content curation and copyright issues	content@ndl.gov.in
7	National Digital Library of India Club (NDLI Club)	Queries related to NDLI Club formation, support, user awareness program, seminar/symposium, collaboration, social media, promotion, and outreach	clubsupport@ndl.gov.in
8	Digital Preservation Centre (DPC)	Assistance with digitizing and archiving copyright-free printed books	dpc@ndl.gov.in
9	IDR Setup or Support	Queries related to establishment and support of Institutional Digital Repository (IDR) and IDR workshops	idr@ndl.gov.in

HOW GOOD IS THE BORN-OPPENHEIMER APPROXIMATION?

Femtosecond dynamics coupled to chemical barrier crossing in a Born-Oppenheimer enzyme

Study of Vibronic and Born-Oppenheimer Couplings

Is the Breakdown of the Born-Oppenheimer Approximation Responsible for Internal Conversion in Large Molecules? *

Enhancing dissociative chemisorption of H2O on Cu(111) via vibrational excitation

Hydrogen bond dynamics in liquid water: Ab initio molecular dynamics simulation

On the Hydrogen Atom Beyond the Born-Oppenheimer Approximation

Radiationless relaxation in “large” molecules: Experimental evidence for preparation of true molecular eigenstates and Born-Oppenheimer states by a coherent light source

Regulating energy transfer of excited carriers and the case for excitation-induced hydrogen dissociation on hydrogenated graphene

Apparent failure of the Born–Oppenheimer static surface model for vibrational excitation of molecular hydrogen on copper

Similar Documents

HOW GOOD IS THE BORN-OPPENHEIMER APPROXIMATION?

Femtosecond dynamics coupled to chemical barrier crossing in a Born-Oppenheimer enzyme

Study of Vibronic and Born-Oppenheimer Couplings

Is the Breakdown of the Born-Oppenheimer Approximation Responsible for Internal Conversion in Large Molecules? *

Enhancing dissociative chemisorption of H2O on Cu(111) via vibrational excitation

Hydrogen bond dynamics in liquid water: Ab initio molecular dynamics simulation

On the Hydrogen Atom Beyond the Born-Oppenheimer Approximation

Radiationless relaxation in “large” molecules: Experimental evidence for preparation of true molecular eigenstates and Born-Oppenheimer states by a coherent light source

Regulating energy transfer of excited carriers and the case for excitation-induced hydrogen dissociation on hydrogenated graphene

Apparent failure of the Born–Oppenheimer static surface model for vibrational excitation of molecular hydrogen on copper