When a nonadiabatic system that has an ionic state (large dipole moment) and a covalent state (small dipole moment) is located in a strong laser field, the crossing point of the two potential energy curves is forced to oscillate due to the oscillating laser field and to meet wavepackets moving on the potential curves many times. This leads to additional transitions between the two states, and under favorable conditions, the wavepacket may be confined in a spatial region rich in nonadiabatic interaction. In this paper, taking the LiF molecule system in a continuous-wave driving field as a prototypical example, the dynamical origins of the wavepacket confinement are theoretically investigated.

1.
Conical Intersections
, edited by
W.
Domcke
,
D.
Yarkony
, and
H.
Köppel
(
World Scientific
,
New Jersey
,
2004
).
2.
M.
Baer
,
Beyond Born–Oppenheimer: Electronic Nonadiabatic Coupling Terms and Conical Intersections
(
Wiley
,
New Jersey
,
2006
).
3.
H.
Nakamura
,
Nonadiabatic Transition: Concepts, Basic Theories and Applications
, 2nd ed. (
World Scientific
,
Singapore
,
2012
).
4.
S. N.
Shevchenko
,
S.
Ashhab
, and
F.
Nori
,
Phys. Rep.
492
,
1
(
2010
).
5.
Y.
Arasaki
,
K.
Takatsuka
,
K.
Wang
, and
V.
McKoy
,
J. Chem. Phys.
119
,
7913
(
2003
).
6.
Y.
Arasaki
,
K.
Takatsuka
,
K.
Wang
, and
V.
McKoy
,
J. Chem. Phys.
132
,
124307
(
2010
).
7.
K.
Takatsuka
,
T.
Yonehara
,
K.
Hanasaki
, and
Y.
Arasaki
,
Chemical Theory Beyond the Born–Oppenheimer Paradigm
(
World Scientific
,
Singapore
,
2015
).
8.
B. J.
Sussman
,
D.
Townsend
,
M. Y.
Ivanov
, and
A.
Stolow
,
Science
314
,
278
(
2006
).
9.
Y.-C.
Han
,
K.-J.
Yuan
,
W.-H.
Hu
, and
S.-L.
Cong
,
J. Chem. Phys.
130
,
044308
(
2009
).
10.
S.
Scheit
,
Y.
Arasaki
, and
K.
Takatsuka
,
J. Phys. Chem. A
116
,
2644
(
2012
).
11.
C.
Sanz-Sanz
,
G. W.
Richings
, and
G. A.
Worth
,
Faraday Discuss.
153
,
275
(
2011
).
12.
G. W.
Richings
and
G. A.
Worth
,
J. Phys. Chem. A
116
,
11228
(
2012
).
13.
M.
Saab
,
L. J.
Doriol
,
B.
Lasorne
,
S.
Guérin
, and
F.
Gatti
,
Chem. Phys.
442
,
93
(
2014
).
14.
M.
Sala
,
M.
Saab
,
B.
Lasorne
,
F.
Gatti
, and
S.
Guérin
,
J. Chem. Phys.
140
,
194309
(
2014
).
15.
M.
Saab
,
M.
Sala
,
B.
Lasorne
,
F.
Gatti
, and
S.
Guérin
,
J. Chem. Phys.
141
,
134114
(
2014
).
16.
Y.
Arasaki
and
K.
Takatsuka
,
Phys. Chem. Chem. Phys.
12
,
1239
(
2010
).
17.
Y.
Arasaki
,
K.
Wang
,
V.
McKoy
, and
K.
Takatsuka
,
Phys. Chem. Chem. Phys.
13
,
8681
(
2011
).
18.
Y.
Arasaki
,
S.
Scheit
, and
K.
Takatsuka
,
J. Chem. Phys.
138
,
161103
(
2013
).
19.
Y.
Arasaki
,
Y.
Mizuno
,
S.
Scheit
, and
K.
Takatsuka
,
J. Chem. Phys.
141
,
234301
(
2014
).
20.
K.
Hader
and
V.
Engel
,
J. Chem. Phys.
140
,
184316
(
2014
).
21.
M. F.
Kling
,
P.
von den Hoff
,
I.
Znakovskaya
, and
R.
de Vivie-Riedle
,
Phys. Chem. Chem. Phys.
15
,
9448
(
2013
).
22.
E.
Persson
,
M.
Pichler
,
G.
Wachter
,
T.
Hisch
,
W.
Jakubetz
,
J.
Burgdörfer
, and
S.
Gräfe
,
Phys. Rev. A
84
,
043421
(
2011
).
23.
C. R.
Calvert
,
R. B.
King
,
W. A.
Bryan
,
W. R.
Newell
,
J. F.
McCann
,
J. B.
Greenwood
, and
I. D.
Williams
,
J. Phys. B
43
,
011001
(
2010
).
24.
P.
von den Hoff
,
I.
Znakovskaya
,
M. F.
Kling
, and
R.
de Vivie-Riedle
,
Chem. Phys.
366
,
139
(
2009
).
25.
J. F.
Pérez-Torres
,
F.
Morales
,
J. L.
Sanz-Vicario
, and
F.
Martín
,
Phys. Rev. A
80
,
011402(R)
(
2009
).
26.
A. D.
Bandrauk
,
S.
Chelkowski
,
P. B.
Corkum
,
J.
Manz
, and
G. L.
Yudin
,
J. Phys. B
42
,
134001
(
2009
).
27.
S.
Gräfe
,
V.
Engel
, and
M. Y.
Ivanov
,
Phys. Rev. Lett.
101
,
103001
(
2008
).
28.
D.
Geppert
,
P.
von den Hoff
, and
R.
de Vivie-Riedle
,
J. Phys. B
41
,
074006
(
2008
).
29.
X. M.
Tong
and
C. D.
Lin
,
Phys. Rev. Lett.
98
,
123002
(
2007
).
30.
P. W.
Anderson
,
Phys. Rev.
109
,
1492
(
1958
).
31.
E.
Abrahams
,
P. W.
Anderson
,
D. C.
Licciardello
, and
T. V.
Ramakrishnan
,
Phys. Rev. Lett.
42
,
673
(
1979
).
32.
B.
Horstmann
,
S.
Dürr
, and
T.
Roscilde
,
Phys. Rev. Lett.
105
,
160402
(
2010
).
33.
M. F.
Kling
,
Ch.
Siedschlag
,
A. J.
Verhoef
,
J. I.
Khan
,
M.
Schultze
,
Th.
Uphues
,
Y.
Ni
,
M.
Uiberacker
,
M.
Drescher
,
F.
Krausz
, and
M. J. J.
Vrakking
,
Science
312
,
246
(
2006
).
34.
A. D.
Bandrauk
,
E. E.
Aubanel
, and
J.-M.
Gauthier
, in
Molecules in Laser Fields
, edited by
A. D.
Bandrauk
(
Marcel Dekker
,
New York
,
1994
).
35.
C.
Wunderlich
,
E.
Kobler
,
H.
Figger
, and
T. W.
Hänsch
,
Phys. Rev. Lett.
78
,
2333
(
1997
).
36.
B. M.
Garraway
and
K.-A.
Suominen
,
Phys. Rev. Lett.
80
,
932
(
1998
).
37.
I. R.
Solá
,
B. Y.
Chang
,
J.
Santamaría
,
V. S.
Malinovsky
, and
J. L.
Krause
,
Phys. Rev. Lett.
85
,
4241
(
2000
).
38.
J. G.
Underwood
,
M.
Spanner
,
M. Y.
Ivanov
,
J.
Mottershead
,
B. J.
Sussman
, and
A.
Stolow
,
Phys. Rev. Lett.
90
,
223001
(
2003
).
39.
P. H.
Bucksbaum
,
A.
Zavriyev
,
H. G.
Muller
, and
D. W.
Schumacher
,
Phys. Rev. Lett.
64
,
1883
(
1990
).
40.
A.
Natan
,
U.
Lev
,
V. S.
Prabhudesai
,
B. D.
Bruner
,
D.
Strasser
,
D.
Schwalm
,
I.
Ben-Itzhak
,
O.
Heber
,
D.
Zajfman
, and
Y.
Silberberg
,
Phys. Rev. A
86
,
043418
(
2012
).
41.
M.
Šindelka
,
N.
Moiseyev
, and
L. S.
Cederbaum
,
J. Phys. B
44
,
045603
(
2011
).
42.
G. J.
Halász
,
Á.
Vibók
,
M.
Šindelka
,
N.
Moiseyev
, and
L. S.
Cederbaum
,
J. Phys. B
44
,
175102
(
2011
).
43.
G. J.
Halász
,
M.
Šindelka
,
N.
Moiseyev
,
L. S.
Cederbaum
, and
Á.
Vibók
,
J. Phys. Chem. A
116
,
2636
(
2011
).
44.
N.
Moiseyev
and
M.
Šindelka
,
J. Phys. B
44
,
111002
(
2011
).
45.
P. V.
Demekhin
and
L. S.
Cederbaum
,
J. Chem. Phys.
139
,
154314
(
2013
).
46.
S.
Scheit
,
Y.
Arasaki
, and
K.
Takatsuka
,
J. Chem. Phys.
140
,
244115
(
2014
).
47.
K.
Yagi
and
K.
Takatsuka
,
J. Chem. Phys.
123
,
224103
(
2005
).
48.
T.-S.
Ho
and
S.-I.
Chu
,
Chem. Phys. Lett.
141
,
315
(
1987
).
49.
K.
Hanasaki
and
K.
Takatsuka
,
Phys. Rev. A
88
,
053426
(
2014
).
50.
Y.
Mizuno
,
Y.
Arasaki
, and
K.
Takatsuka
,
J. Chem. Phys.
144
,
024106
(
2016
).
51.
T. J.
Giese
and
D. M.
York
,
J. Chem. Phys.
120
,
7939
(
2004
).
52.
H.-J.
Werner
,
P. J.
Knowles
,
G.
Knizia
,
F. R.
Manby
, and
M.
Schütz
,
Wiley Interdiscip. Rev.: Comput. Mol. Sci.
2
,
242
253
(
2012
).
53.
H.-J.
Werner
,
P. J.
Knowles
,
G.
Knizia
,
F. R.
Manby
,
M.
Schütz
,
P.
Celani
,
W.
Györffy
,
D.
Kats
,
T.
Korona
,
R.
Lindh
,
A.
Mitrushenkov
,
G.
Rauhut
,
K. R.
Shamasundar
,
T. B.
Adler
,
R. D.
Amos
,
A.
Bernhardsson
,
A.
Berning
,
D. L.
Cooper
,
M. J. O.
Deegan
,
A. J.
Dobbyn
,
F.
Eckert
,
E.
Goll
,
C.
Hampel
,
A.
Hesselmann
,
G.
Hetzer
,
T.
Hrenar
,
G.
Jansen
,
C.
Köppl
,
Y.
Liu
,
A. W.
Lloyd
,
R. A.
Mata
,
A. J.
May
,
S. J.
McNicholas
,
W.
Meyer
,
M. E.
Mura
,
A.
Nicklass
,
D. P.
O’Neill
,
P.
Palmieri
,
D.
Peng
,
K.
Pflüger
,
R.
Pitzer
,
M.
Reiher
,
T.
Shiozaki
,
H.
Stoll
,
A. J.
Stone
,
R.
Tarroni
,
T.
Thorsteinsson
, and
M.
Wang
, molpro, version 2015.1, a package of ab initio programs, 2015, see http://www.molpro.net.
54.
B. P.
Prascher
,
D. E.
Woon
,
K. A.
Peterson
,
T. H.
Dunning
, Jr.
, and
A. K.
Wilson
,
Theor. Chem. Acc.
128
,
69
(
2011
).
55.
T. H.
Dunning
, Jr.
,
J. Chem. Phys.
90
,
1007
(
1989
).
56.
H.-J.
Werner
and
P. J.
Knowles
,
J. Chem. Phys.
82
,
5053
(
1985
).
57.
P. J.
Knowles
and
H.-J.
Werner
,
Chem. Phys. Lett.
115
,
259
(
1985
).
58.
H.-J.
Werner
and
P. J.
Knowles
,
J. Chem. Phys.
89
,
5803
(
1988
).
59.
P. J.
Knowles
and
H.-J.
Werner
,
Chem. Phys. Lett.
145
,
514
(
1988
).
60.
P. J.
Knowles
and
H.-J.
Werner
,
Theor. Chim. Acta
84
,
95
(
1992
).
61.
See supplementary material at http://dx.doi.org/10.1063/1.4940341 for additional details.
62.
M. D.
Feit
,
J. A.
Fleck
, Jr.
, and
A.
Steiger
,
J. Comput. Phys.
47
,
412
(
1982
).
63.
D.
Neuhasuer
and
M.
Baer
,
J. Chem. Phys.
90
,
4351
(
1989
).
64.
P.
Dietrich
and
P. B.
Corkum
,
J. Chem. Phys.
97
,
3187
(
1992
).
65.
J.
Berkowitz
,
H. A.
Tasman
, and
W. A.
Chupka
,
J. Chem. Phys.
36
,
2170
(
1962
).

Supplementary Material

You do not currently have access to this content.