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Title: Imaging covalent bond formation by H atom scattering from graphene

Abstract

Viewing the atomic-scale motion and energy dissipation pathways involved in forming a covalent bond is a longstanding challenge for chemistry. We performed scattering experiments of H atoms from graphene and observed a bimodal translational energy loss distribution. Using accurate first-principles dynamics simulations, we show that the quasi-elastic channel involves scattering through the physisorption well where collision sites are near the centers of the six-membered C-rings. The second channel results from transient C–H bond formation, where H atoms lose 1 to 2 electron volts of energy within a 10-femtosecond interaction time. This remarkably rapid form of intramolecular vibrational relaxation results from the C atom’s rehybridization during bond formation and is responsible for an unexpectedly high sticking probability of H on graphene.

Authors:
ORCiD logo; ; ; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1547466
Grant/Contract Number:  
SC0004993; DEFOA-0001912
Resource Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Name: Science Journal Volume: 364 Journal Issue: 6438; Journal ID: ISSN 0036-8075
Publisher:
American Association for the Advancement of Science (AAAS)
Country of Publication:
United States
Language:
English

Citation Formats

Jiang, Hongyan, Kammler, Marvin, Ding, Feizhi, Dorenkamp, Yvonne, Manby, Frederick R., Wodtke, Alec. M., Miller, III, Thomas F., Kandratsenka, Alexander, and Bünermann, Oliver. Imaging covalent bond formation by H atom scattering from graphene. United States: N. p., 2019. Web. doi:10.1126/science.aaw6378.
Jiang, Hongyan, Kammler, Marvin, Ding, Feizhi, Dorenkamp, Yvonne, Manby, Frederick R., Wodtke, Alec. M., Miller, III, Thomas F., Kandratsenka, Alexander, & Bünermann, Oliver. Imaging covalent bond formation by H atom scattering from graphene. United States. doi:10.1126/science.aaw6378.
Jiang, Hongyan, Kammler, Marvin, Ding, Feizhi, Dorenkamp, Yvonne, Manby, Frederick R., Wodtke, Alec. M., Miller, III, Thomas F., Kandratsenka, Alexander, and Bünermann, Oliver. Thu . "Imaging covalent bond formation by H atom scattering from graphene". United States. doi:10.1126/science.aaw6378.
@article{osti_1547466,
title = {Imaging covalent bond formation by H atom scattering from graphene},
author = {Jiang, Hongyan and Kammler, Marvin and Ding, Feizhi and Dorenkamp, Yvonne and Manby, Frederick R. and Wodtke, Alec. M. and Miller, III, Thomas F. and Kandratsenka, Alexander and Bünermann, Oliver},
abstractNote = {Viewing the atomic-scale motion and energy dissipation pathways involved in forming a covalent bond is a longstanding challenge for chemistry. We performed scattering experiments of H atoms from graphene and observed a bimodal translational energy loss distribution. Using accurate first-principles dynamics simulations, we show that the quasi-elastic channel involves scattering through the physisorption well where collision sites are near the centers of the six-membered C-rings. The second channel results from transient C–H bond formation, where H atoms lose 1 to 2 electron volts of energy within a 10-femtosecond interaction time. This remarkably rapid form of intramolecular vibrational relaxation results from the C atom’s rehybridization during bond formation and is responsible for an unexpectedly high sticking probability of H on graphene.},
doi = {10.1126/science.aaw6378},
journal = {Science},
number = 6438,
volume = 364,
place = {United States},
year = {2019},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1126/science.aaw6378

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Cited by: 1 work
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