The vibrationally excited reaction O(1D) + CHD3(ν1 = 1) has been investigated by crossed-molecular-beam experiments with a time-sliced velocity map imaging technique. Detailed and quantitative information is extracted on the C–H stretching excitation effects on the reactivity and dynamics of the title reaction, with the help of preparation of C–H stretching excited CHD3 molecules by direct infrared excitation. Experimental results show that the vibrational stretching excitation of the C–H bond almost does not affect the relative contributions between different dynamical pathways for all product channels. For the OH + CD3 product channel, the vibrational energy of the C–H stretching excited CHD3 reagent is channeled exclusively into the vibrational energy of the OH products. The vibrational excitation of the CHD3 reactant changes the reactivities for the ground-state and umbrella-mode-excited CD3 channels very modestly, while it significantly suppresses the corresponding CHD2 channels. For the CHD2(ν1 = 1) channel, the stretching excited C–H bond of the CHD3 molecule acts almost as a pure spectator.
REFERENCES
1.
R. N.
Zare
, Science
279
, 1875
–1879
(1998
).2.
J. C.
Polanyi
, Acc. Chem. Res.
5
, 161
–168
(1972
).3.
T. J.
Odiorne
, P. R.
Brooks
, and J. V. V.
Kasper
, J. Chem. Phys.
55
, 1980
–1982
(1971
).4.
J. G.
Pruett
and R. N.
Zare
, J. Chem. Phys.
64
, 1774
–1783
(1976
).5.
C. B.
Moore
and I. W. M.
Smith
, Faraday Discuss. Chem. Soc.
67
, 146
–161
(1979
).6.
G. C.
Schatz
, M. C.
Colton
, and J. L.
Grant
, J. Phys. Chem.
88
, 2971
–2977
(1984
).7.
T.
Ebata
and R. N.
Zare
, Chem. Phys. Lett.
130
, 467
–472
(1986
).8.
A.
Sinha
, M. C.
Hsiao
, and F. F.
Crim
, J. Chem. Phys.
92
, 6333
–6335
(1990
).9.
M. J.
Bronikowski
, W. R.
Simpson
, B.
Girard
, and R. N.
Zare
, J. Chem. Phys.
95
, 8647
–8648
(1991
).10.
J. M.
Bowman
and D.
Wang
, J. Chem. Phys.
96
, 7852
–7854
(1992
).11.
A.
Sinha
, J. D.
Thoemke
, and F. F.
Crim
, J. Chem. Phys.
96
, 372
–376
(1992
).12.
Y. h.
Chiu
, H.
Fu
, J. t.
Huang
, and S. L.
Anderson
, J. Chem. Phys.
101
, 5410
–5412
(1994
).13.
R. D.
Guettler
, G. C.
Jones
, L. A.
Posey
, and R. N.
Zare
, Science
266
, 259
–261
(1994
).14.
K.
Ravichandran
, R.
Williams
, and T. R.
Fletcher
, Chem. Phys. Lett.
217
, 375
–380
(1994
).15.
H.
Tachikawa
and S.
Tomoda
, Chem. Phys.
182
, 185
–194
(1994
).16.
W. T.
Duncan
and T. N.
Truong
, J. Chem. Phys.
103
, 9642
–9652
(1995
).17.
W. R.
Simpson
, T. P.
Rakitzis
, S. A.
Kandel
, A. J.
Orr‐Ewing
, and R. N.
Zare
, J. Chem. Phys.
103
, 7313
–7335
(1995
).18.
S. J.
Klippenstein
, J. Chem. Phys.
104
, 5437
–5445
(1996
).19.
C.
Kreher
, R.
Theinl
, and K. H.
Gericke
, J. Chem. Phys.
104
, 4481
–4489
(1996
).20.
J. M.
Pfeiffer
, R. B.
Metz
, J. D.
Thoemke
, E.
Woods
, and F. F.
Crim
, J. Chem. Phys.
104
, 4490
–4501
(1996
).21.
D. H.
Zhang
and J. C.
Light
, J. Chem. Soc., Faraday Trans.
93
, 691
–697
(1997
).22.
H.
Fu
, J.
Qian
, R. J.
Green
, and S. L.
Anderson
, J. Chem. Phys.
108
, 2395
–2407
(1998
).23.
F. F.
Crim
, Acc. Chem. Res.
32
, 877
–884
(1999
).24.
J.
Palma
, J.
Echave
, and D. C.
Clary
, Chem. Phys. Lett.
363
, 529
–533
(2002
).25.
Z.
Xie
and J. M.
Bowman
, Chem. Phys. Lett.
429
, 355
–359
(2006
).26.
S.
Yan
, Y.-T.
Wu
, B.
Zhang
, X.-F.
Yue
, and K.
Liu
, Science
316
, 1723
–1726
(2007
).27.
D. L.
Proctor
and H. F.
Davis
, Proc. Natl. Acad. Sci. U. S. A.
105
, 12673
–12677
(2008
).28.
G.
Czakó
and J. M.
Bowman
, J. Am. Chem. Soc.
131
, 17534
–17535
(2009
).29.
W.
Zhang
, H.
Kawamata
, and K.
Liu
, Science
325
, 303
–306
(2009
).30.
F.
Wang
and K.
Liu
, Chem. Sci.
1
, 126
–133
(2010
).31.
Z.
Zhang
, Y.
Zhou
, D. H.
Zhang
, G.
Czakó
, and J. M.
Bowman
, J. Phys. Chem. Lett.
3
, 3416
–3419
(2012
).32.
M.
Stei
, E.
Carrascosa
, A.
Dörfler
, J.
Meyer
, B.
Olasz
, G.
Czakó
, A.
Li
, H.
Guo
, and R.
Wester
, Sci. Adv.
4
, eaas9544
(2018
).33.
Y.
Wang
, H.
Song
, I.
Szabó
, G.
Czakó
, H.
Guo
, and M.
Yang
, J. Phys. Chem. Lett.
7
, 3322
–3327
(2016
).34.
I.
Szabó
and G.
Czakó
, J. Chem. Phys.
145
, 134303
(2016
).35.
B.
Olasz
and G.
Czakó
, J. Phys. Chem. A
122
, 8143
–8151
(2018
).36.
D.
Papp
and G.
Czakó
, J. Chem. Phys.
155
, 154302
(2021
).37.
V.
Tajti
and G.
Czakó
, Phys. Chem. Chem. Phys.
24
, 8166
–8181
(2022
).38.
C.
Yin
and G.
Czakó
, Phys. Chem. Chem. Phys.
25
, 3083
–3091
(2023
).39.
C.
Yin
and G.
Czakó
, Phys. Chem. Chem. Phys.
25
, 9944
–9951
(2023
).40.
J.
Hernando
, J.
Millán
, R.
Sayós
, and M.
González
, J. Chem. Phys.
119
, 9504
–9512
(2003
).41.
K.
Shao
, B.
Fu
, and D. H.
Zhang
, Phys. Chem. Chem. Phys.
17
, 24098
–24107
(2015
).42.
J. J.
Lin
, J.
Shu
, Y. T.
Lee
, and X.
Yang
, J. Chem. Phys.
113
, 5287
–5301
(2000
).43.
C. C.
Miller
, R. D.
van Zee
, and J. C.
Stephenson
, J. Chem. Phys.
114
, 1214
–1232
(2001
).44.
H.-G.
Yu
and J. T.
Muckerman
, J. Phys. Chem. A
108
, 8615
–8623
(2004
).45.
H.
Kohguchi
, Y.
Ogi
, and T.
Suzuki
, Phys. Chem. Chem. Phys.
10
, 7222
–7225
(2008
).46.
Q.
Shuai
, H.
Pan
, J.
Yang
, D.
Zhang
, B.
Jiang
, D.
Dai
, and X.
Yang
, J. Phys. Chem. Lett.
3
, 1310
–1314
(2012
).47.
Q.
Shuai
, H.
Pan
, J.
Yang
, D.
Zhang
, B.
Jiang
, D.
Dai
, and X.
Yang
, J. Chem. Phys.
137
, 224301
(2012
).48.
H.
Kohguchi
, Y.
Ogi
, and T.
Suzuki
, Phys. Chem. Chem. Phys.
13
, 8371
–8378
(2011
).49.
Y.
Ogi
, H.
Kohguchi
, and T.
Suzuki
, Phys. Chem. Chem. Phys.
15
, 12946
–12957
(2013
).50.
J.
Yang
, K.
Shao
, D.
Zhang
, Q.
Shuai
, B.
Fu
, D. H.
Zhang
, and X.
Yang
, J. Phys. Chem. Lett.
5
, 3106
–3111
(2014
).51.
R.
Atkinson
, D. L.
Baulch
, R. A.
Cox
, R. F.
Hampson
, Jr., J. A.
Kerr
, M. J.
Rossi
, and J.
Troe
, J. Phys. Chem. Ref. Data
28
, 191
–393
(1999
).52.
Q.
Meng
, K. M.
Hickson
, K.
Shao
, J.-C.
Loison
, and D. H.
Zhang
, Phys. Chem. Chem. Phys.
18
, 29286
–29292
(2016
).53.
B. M.
Hays
, N.
Wehres
, B. A.
DePrince
, A. A. M.
Roy
, J. C.
Laas
, and S. L.
Widicus Weaver
, Chem. Phys. Lett.
630
, 18
–26
(2015
).54.
H.
Pan
, J.
Yang
, D.
Zhang
, Q.
Shuai
, D.
Dai
, G.
Wu
, B.
Jiang
, and X.
Yang
, J. Chem. Phys.
140
, 154305
(2014
).55.
X.
Liu
, J. J.
Lin
, S.
Harich
, G. C.
Schatz
, and X.
Yang
, Science
289
, 1536
–1538
(2000
).56.
H.
Guo
, Int. Rev. Phys. Chem.
31
, 1
–68
(2012
).57.
H.
Kawamata
, S.
Tauro
, and K.
Liu
, Phys. Chem. Chem. Phys.
10
, 4378
–4382
(2008
).58.
G.
Wu
, W.
Zhang
, H.
Pan
, Q.
Shuai
, B.
Jiang
, D.
Dai
, and X.
Yang
, Rev. Sci. Instrum.
79
, 094104
(2008
).59.
J. W.
Hudgens
, T. G.
DiGiuseppe
, and M. C.
Lin
, J. Chem. Phys.
79
, 571
–582
(1983
).60.
D. H.
Parker
, Z. W.
Wang
, M. H. M.
Janssen
, and D. W.
Chandler
, J. Chem. Phys.
90
, 60
–67
(1989
).61.
D. G.
Rea
and H. W.
Thompson
, Trans. Faraday Soc.
52
, 1304
–1309
(1956
).62.
J.
Riedel
, S.
Yan
, H.
Kawamata
, and K.
Liu
, Rev. Sci. Instrum.
79
, 033105
(2008
).63.
A. J. C.
Varandas
, P. J. S. B.
Caridade
, J. Z. H.
Zhang
, Q.
Cui
, and K. L.
Han
, J. Chem. Phys.
125
, 064312
(2006
).64.
J.
Yang
, D.
Zhang
, Z.
Chen
, F.
Blauert
, B.
Jiang
, D.
Dai
, G.
Wu
, D.
Zhang
, and X.
Yang
, J. Chem. Phys.
143
, 044316
(2015
).65.
J.
Yang
, D.
Zhang
, B.
Jiang
, D.
Dai
, G.
Wu
, D.
Zhang
, and X.
Yang
, J. Phys. Chem. Lett.
5
, 1790
–1794
(2014
).66.
J. J.
Lin
, J.
Zhou
, W.
Shiu
, and K.
Liu
, Rev. Sci. Instrum.
74
, 2495
–2500
(2003
).67.
J.
Zhou
, J. J.
Lin
, W.
Shiu
, S.-C.
Pu
, and K.
Liu
, J. Chem. Phys.
119
, 2538
–2544
(2003
).68.
H.
Guo
and B.
Jiang
, Acc. Chem. Res.
47
, 3679
–3685
(2014
).69.
B.
Jiang
and H.
Guo
, J. Chin. Chem. Soc.
61
, 847
–859
(2014
).70.
D.
Zhang
, J.
Yang
, Z.
Chen
, R.
Chen
, B.
Jiang
, D.
Dai
, G.
Wu
, D.
Zhang
, and X.
Yang
, Phys. Chem. Chem. Phys.
19
, 13070
–13074
(2017
).© 2023 Author(s). Published under an exclusive license by AIP Publishing.
2023
Author(s)
You do not currently have access to this content.
