Efficient transfer of translational energy to electron-hole pair excitation involving multiple collisions dominates H atom collisions with metal surfaces. For this reason, H atom interaction with metal surfaces cannot be modeled within the commonly used Born-Oppenheimer approximation (BOA). This fact makes H atom scattering from metal surfaces an ideal model system for dynamics that go beyond the BOA. We chose the H/Au(111) system as a model system to obtain a detailed dataset that can serve as a benchmark for theoretical models developed for describing electronically nonadiabatic processes at metal surfaces. Therefore, we investigate the influence of various experimental parameters on the energy loss in detail including isotopic variant, incidence translational energy, incidence polar and azimuthal angles, and outgoing scattering angles.

1.
D.
Hollenbach
and
E. E.
Salpeter
, “
Surface recombination of hydrogen molecules
,”
Astrophys. J.
163
,
155
(
1971
).
2.
G.
Federici
,
C. H.
Skinner
,
J. N.
Brooks
,
J. P.
Coad
,
C.
Grisolia
,
A. A.
Haasz
,
A.
Hassanein
,
V.
Philipps
,
C. S.
Pitcher
,
J.
Roth
,
W. R.
Wampler
, and
D. G.
Whyte
, “
Plasma-material interactions in current tokamaks and their implications for next step fusion reactors
,”
Nucl. Fusion
41
,
1967
2137
(
2001
).
3.
J. K.
Norskov
and
B. I.
Lundqvist
, “
Correlation between sticking probability and adsorbate-induced electron-structure
,”
Surf. Sci.
89
,
251
261
(
1979
).
4.
H.
Nienhaus
,
H. S.
Bergh
,
B.
Gergen
,
A.
Majumdar
,
W. H.
Weinberg
, and
E. W.
McFarland
, “
Electron-hole pair creation at Ag and Cu surfaces by adsorption of atomic hydrogen and deuterium
,”
Phys. Rev. Lett.
82
,
446
449
(
1999
).
5.
B.
Gergen
,
H.
Nienhaus
,
W. H.
Weinberg
, and
E. W.
McFarland
, “
Chemically induced electronic excitations at metal surfaces
,”
Science
294
,
2521
2523
(
2001
).
6.
B.
Mildner
,
E.
Hasselbrink
, and
D.
Diesing
, “
Electronic excitations induced by surface reactions of H and D on gold
,”
Chem. Phys. Lett.
432
,
133
138
(
2006
).
7.
B.
Schindler
,
D.
Diesing
, and
E.
Hasselbrink
, “
Electronic excitations in the course of the reaction of H with coinage and noble metal surfaces: A comparison
,”
Z. Phys. Chem.
227
,
1381
1395
(
2013
).
8.
J. R.
Trail
,
M. C.
Graham
,
D. M.
Bird
,
M.
Persson
, and
S.
Holloway
, “
Energy loss of atoms at metal surfaces due to electron-hole pair excitations: First-principles theory of ‘chemicurrents
,’”
Phys. Rev. Lett.
88
,
166802
(
2002
).
9.
J. R.
Trail
,
D. M.
Bird
,
M.
Persson
, and
S.
Holloway
, “
Electron-hole pair creation by atoms incident on a metal surface
,”
J. Chem. Phys.
119
,
4539
4549
(
2003
).
10.
M. S.
Mizielinski
,
D. M.
Bird
,
M.
Persson
, and
S.
Holloway
, “
Newns-Anderson model of chemicurrents in H/Cu and H/Ag
,”
Surf. Sci.
602
,
2617
2622
(
2008
).
11.
D. M.
Bird
,
M. S.
Mizielinski
,
M.
Lindenblatt
, and
E.
Pehlke
, “
Electronic excitation in atomic adsorption on metals: A comparison of ab initio and model calculations
,”
Surf. Sci.
602
,
1212
1216
(
2008
).
12.
M. S.
Mizielinski
and
D. M.
Bird
, “
Accuracy of perturbation theory for nonadiabatic effects in adsorbate-surface dynamics
,”
J. Chem. Phys.
132
,
184704
(
2010
).
13.
M.
Pavanello
,
D. J.
Auerbach
,
A. M.
Wodtke
,
M.
Blanco-Rey
,
M.
Alducin
, and
G. J.
Kroes
, “
Adiabatic energy loss in hyperthermal H atom collisions with Cu and Au: A basis for testing the importance of nonadiabatic energy loss
,”
J. Phys. Chem. Lett.
4
,
3735
3740
(
2013
).
14.
S. M.
Janke
,
M.
Pavanello
,
G. J.
Kroes
,
D.
Auerbach
,
A. M.
Wodtke
, and
A.
Kandratsenka
, “
Toward detection of electron-hole pair excitation in H-atom collisions with Au(111): Adiabatic molecular dynamics with a semi-empirical full-dimensional potential energy surface
,”
Z. Phys. Chem.
227
,
1467
1490
(
2013
).
15.
G. J.
Kroes
,
M.
Pavanello
,
M.
Blanco-Rey
,
M.
Alducin
, and
D. J.
Auerbach
, “
Ab initio molecular dynamics calculations on scattering of hyperthermal H atoms from Cu(111) and Au(111)
,”
J. Chem. Phys.
141
,
054705
(
2014
).
16.
M.
Blanco-Rey
,
J. I.
Juaristi
,
R. D.
Muino
,
H. F.
Busnengo
,
G. J.
Kroes
, and
M.
Alducin
, “
Electronic friction dominates hydrogen hot-atom relaxation on Pd(100)
,”
Phys. Rev. Lett.
112
,
103203
(
2014
).
17.
O.
Buenermann
,
H. Y.
Jiang
,
Y.
Dorenkamp
,
A.
Kandratsenka
,
S. M.
Janke
,
D. J.
Auerbach
, and
A. M.
Wodtke
, “
Electron-hole pair excitation determines the mechanism of hydrogen atom adsorption
,”
Science
350
,
1346
1349
(
2015
).
18.
A.
Kandratsenka
,
H. Y.
Jiang
,
Y.
Dorenkamp
,
S. M.
Janke
,
M.
Kammler
,
A. M.
Wodtke
, and
O.
Buenermann
, “
Unified description of H-atom-induced chemicurrents and inelastic scattering
,”
Proc. Natl. Acad. Sci. U. S. A.
115
,
680
684
(
2018
).
19.
Y.
Dorenkamp
,
H. Y.
Jiang
,
H.
Kockert
,
N.
Hertl
,
M.
Kammler
,
S. M.
Janke
,
A.
Kandratsenka
,
A. M.
Wodtke
, and
O.
Buenermann
, “
Hydrogen collisions with transition metal surfaces: Universal electronically nonadiabatic adsorption
,”
J. Chem. Phys.
148
,
034706
(
2018
).
20.
S. M.
Janke
,
D. J.
Auerbach
,
A. M.
Wodtke
, and
A.
Kandratsenka
, “
An accurate full-dimensional potential energy surface for H-Au(111): Importance of nonadiabatic electronic excitation in energy transfer and adsorption
,”
J. Chem. Phys.
143
,
124708
(
2015
).
21.
M.
Kammler
,
S. M.
Janke
,
A.
Kandratsenka
, and
A. M.
Wodtke
, “
Genetic algorithm approach to global optimization of the full-dimensional potential energy surface for hydrogen atom at fcc-metal surfaces
,”
Chem. Phys. Lett.
683
,
286
290
(
2017
).
22.
Y. G.
Li
and
G.
Wahnstrom
, “
Molecular-dynamics simulation of hydrogen diffusion in palladium
,”
Phys. Rev. B
46
,
14528
14542
(
1992
).
23.
O.
Buenermann
,
H. Y.
Jiang
,
Y.
Dorenkamp
,
D. J.
Auerbach
, and
A. M.
Wodtke
, “
An ultrahigh vacuum apparatus for H atom scattering from surfaces
,”
Rev. Sci. Instrum.
89
,
094101
(
2018
).
24.
L.
Schnieder
,
W.
Meier
,
K. H.
Welge
,
M. N. R.
Ashfold
, and
C. M.
Western
, “
Photodissociation dynamics of H2S at 121.6 nm and a determination of the potential-energy function of SH(A2Σ+)
,”
J. Chem. Phys.
92
,
7027
7037
(
1990
).
25.
Y.
Dorenkamp
,
C.
Volkmann
,
V.
Roddatis
,
S.
Schneider
,
A. M.
Wodtke
, and
O.
Buenermann
, “
Inelastic H atom scattering from ultrathin aluminum oxide films grown by atomic layer deposition on Pt(111)
,”
J. Phys. Chem. C
122
,
10096
10102
(
2018
).
26.
F.
Reinert
and
G.
Nicolay
, “
Influence of the herringbone reconstruction on the surface electronic structure of Au(111)
,”
Appl. Phys. A
78
,
817
821
(
2004
).
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