The reaction dynamics of methanol and water on Si(001) were investigated by means of molecular beam techniques. The initial sticking probability s0 was determined as a function of the kinetic energy of the incoming molecules, Ekin, and surface temperature, Ts. For both, methanol and water, a nonactivated reactional channel was observed; the dynamics were found to be determined by the reaction into the datively bonded intermediate state. A low conversion barrier was deduced for the conversion from this intermediate into the final state. It is attributed to the reaction mechanism, which proceeds via proton transfer from the OH-group of the datively bonded molecules to a Si surface atom. Despite this low conversion barrier, adsorption into the intermediate and further reaction via proton transfer were found to be largely decoupled.

1.
M. A.
Filler
and
S. F.
Bent
,
Prog. Surf. Sci.
73
,
1
(
2003
).
2.
3.
T. R.
Leftwich
and
A. V.
Teplyakov
,
Surf. Sci. Rep.
63
,
1
(
2008
).
4.
J. H. G.
Owen
,
J. Phys.: Condens. Matter
21
,
443001
(
2009
).
5.
F.
Tao
,
Y.
Zhu
, and
S. L.
Bernasek
, in
Functionalization of Semiconductor Surfaces
, 1st ed., edited by
F.
Tao
and
S. L.
Bernasek
(
John Wiley & Sons
,
Hoboken, New Jersey
,
2012
), pp.
1
10
.
6.
C.
Länger
,
T.
Bohamud
,
J.
Heep
,
T.
Glaser
,
M.
Reutzel
,
U.
Höfer
, and
M.
Dürr
,
J. Phys. Chem. C
122
,
14756
(
2018
).
7.
X. P.
Cao
and
R. J.
Hamers
,
J. Am. Chem. Soc.
123
,
10988
(
2001
).
8.
C.
Mui
,
J. H.
Han
,
G. T.
Wang
,
C. B.
Musgrave
, and
S. F.
Bent
,
J. Am. Chem. Soc.
124
,
4027
(
2002
).
9.
Y. H.
Min
,
H.
Lee
,
D. H.
Kim
, and
S.
Kim
, in
Functionalization of Semiconductor Surfaces
, 1st ed., edited by
F.
Tao
and
S. L.
Bernasek
(
John Wiley & Sons
,
Hoboken, New Jersey
,
2012
), pp.
193
231
.
10.
G.
Mette
,
M.
Reutzel
,
R.
Bartholomäus
,
S.
Laref
,
R.
Tonner
,
M.
Dürr
,
U.
Koert
, and
U.
Höfer
,
ChemPhysChem
15
,
3725
(
2014
).
11.
M.
Reutzel
,
G.
Mette
,
P.
Stromberger
,
U.
Koert
,
M.
Dürr
, and
U.
Höfer
,
J. Phys. Chem. C
119
,
6018
(
2015
).
12.
M.
Reutzel
,
M.
Lipponer
,
M.
Dürr
, and
U.
Höfer
,
J. Phys. Chem. Lett.
6
,
3971
(
2015
).
13.
L.
Pecher
,
S.
Laref
,
M.
Raupach
, and
R.
Tonner
,
Angew. Chem., Int. Ed.
56
,
15150
(
2017
).
14.
J. H.
Cho
and
L.
Kleinman
,
Phys. Rev. B
69
,
075303
(
2004
).
15.
K.
Akagi
and
J.
Yoshinobu
,
Surf. Sci.
652
,
304
(
2016
).
16.
M.
Carbone
,
Surf. Rev. Lett.
24
,
1830001
(
2017
).
17.
P. A.
Taylor
,
R. M.
Wallace
,
C. C.
Cheng
,
W. H.
Weinberg
,
M. J.
Dresser
,
W. J.
Choyke
, and
J. T.
Yates
, Jr.
,
J. Am. Chem. Soc.
114
,
6754
(
1992
).
18.
L.
Clemen
,
R. M.
Wallace
,
P. A.
Taylor
,
M. J.
Dresser
,
W. J.
Choyke
,
W. H.
Weinberg
, and
J. T.
Yates
,
Surf. Sci.
268
,
205
(
1992
).
19.
M. A.
Lipponer
,
N.
Armbrust
,
M.
Dürr
, and
U.
Höfer
,
J. Chem. Phys.
136
,
144703
(
2012
).
20.
M. A.
Lipponer
,
M.
Dürr
, and
U.
Höfer
,
Chem. Phys. Lett.
624
,
69
(
2015
).
21.
M. A.
Lipponer
,
M.
Reutzel
,
M.
Dürr
, and
U.
Höfer
,
Surf. Sci.
653
,
118
(
2016
).
22.
M.
Reutzel
,
N.
Münster
,
M. A.
Lipponer
,
C.
Länger
,
U.
Höfer
,
U.
Koert
, and
M.
Dürr
,
J. Phys. Chem. C
120
,
26284
(
2016
).
23.
C.
Länger
,
J.
Heep
,
P.
Nikodemiak
,
T.
Bohamud
,
P.
Kirsten
,
U.
Höfer
,
U.
Koert
, and
M.
Dürr
,
J. Phys.: Condens. Matter
31
,
034001
(
2019
).
24.
R.
Konecny
and
D. J.
Doren
,
J. Chem. Phys.
106
,
2426
(
1997
).
25.
26.
J.-H.
Cho
,
K. S.
Kim
,
S.-H.
Lee
, and
M.-H.
Kang
,
Phys. Rev. B
61
,
4503
(
2000
).
27.
T.
Kato
,
S. Y.
Kang
,
X.
Xu
, and
T.
Yamabe
,
J. Phys. Chem. B
105
,
10340
(
2001
).
28.
X.
Lu
,
Q.
Zhang
, and
M. C.
Lin
,
Phys. Chem. Chem. Phys.
3
,
2156
(
2001
).
29.
L. H.
Zhang
,
A. J.
Carman
, and
S. M.
Casey
,
J. Phys. Chem. B
107
,
8424
(
2003
).
30.
P. L.
Silvestrelli
,
Surf. Sci.
552
,
17
(
2004
).
31.
M.
Carbone
and
K.
Larsson
,
J. Phys.: Condens. Matter
17
,
1289
(
2005
).
32.
Y. T.
Lee
and
J. S.
Lin
,
RSC Adv.
6
,
1491
(
2016
).
33.
M.
Dürr
,
M. B.
Raschke
, and
U.
Höfer
,
J. Chem. Phys.
111
,
10411
(
1999
).
34.
M.
Dürr
and
U.
Höfer
,
J. Chem. Phys.
121
,
8058
(
2004
).
35.
M.
Dürr
and
U.
Höfer
,
Surf. Sci. Rep.
61
,
465
(
2006
).
36.
D. A.
King
and
M. G.
Wells
,
Surf. Sci.
29
,
454
(
1972
).
37.
T.
Takaoka
and
I.
Kusunoki
,
Surf. Sci.
412-413
,
30
(
1998
).
39.
P.
Kisliuk
,
J. Phys. Chem. Solids
3
,
95
(
1957
).
40.
M. C.
Flowers
,
N. B. H.
Jonathan
,
A.
Morris
, and
S.
Wright
,
Surf. Sci.
351
,
87
(
1996
).
41.
C.
Poncey
,
F.
Rochet
,
G.
Dufour
,
H.
Roulet
,
F.
Sirotti
, and
G.
Panaccione
,
Surf. Sci.
338
,
143
(
1995
).
42.
D.
Pierucci
,
J.-J.
Gallet
,
F.
Bournel
,
F.
Sirotti
,
M. G.
Silly
,
H.
Tissot
,
A.
Naitabdi
, and
F.
Rochet
,
J. Phys. Chem. C
120
,
21631
(
2016
).
43.
G.
Mette
,
A.
Adamkiewicz
,
M.
Reutzel
,
U.
Koert
,
M.
Dürr
, and
U.
Höfer
,
Angew. Chem., Int. Ed.
58
,
3417
(
2019
).
44.
C. T.
Campbell
,
L.
Arnadottir
, and
J. R. V.
Sellers
,
Z. Phys. Chem.
227
,
1435
(
2013
).
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