The femtosecond second hyperpolarizability due to the nonresonant electronic polarization for two intramolecular charge-transfer molecules, 6-propionyl-2-dimethylamino naphthalene and 2-anilinonaphthalene-6-sulfonic acid which possess the great permanent dipole-moment difference between the excited state and the ground state, is obtained from the measurement of the ultrafast change in refractive index using a time-resolved interferometer. It is found that the second hyperpolarizability increases parabolically from 5×10−34 to 4.3×10−32esu with increasing the dipole-moment difference from 7.7 to 40 D, and this quantitative relationship is well explained by a quantum-mechanical equation describing the electronic second hyperpolarizability of one molecule with the permanent dipole-moment difference.

1.
J. L.
Bredas
,
C.
Adant
,
P.
Tackx
,
A.
Persoons
, and
B. M.
Pierce
,
Chem. Rev.
94
,
243
(
1994
).
2.
L.-T.
Cheng
,
W.
Tam
,
S. H.
Stevenson
,
G. R.
Meredith
,
G.
Rikken
, and
S. R.
Marder
,
J. Phys. Chem.
95
,
10631
(
1991
).
3.
G.
Weber
and
F. J.
Farris
,
Biochemistry
18
,
3075
(
1979
).
4.
C. J.
Seliskar
and
L.
Brand
,
J. Am. Chem. Soc.
93
,
5414
(
1971
).
5.
T.
Suemura
,
M.
Ohtani
,
R.
Morita
, and
M.
Yamashita
,
Jpn. J. Appl. Phys., Part 2
36
,
L1307
(
1997
).
6.
K. L.
Hall
,
A. M.
Darwish
,
E. P.
Ippen
,
U.
Koren
, and
G.
Raybon
,
Appl. Phys. Lett.
62
,
1320
(
1993
).
7.
Y.
Sato
,
R.
Morita
, and
M.
Yamashita
,
Jpn. J. Appl. Phys., Part 1
36
,
2109
(
1997
).
8.
A.
Mito
,
K.
Hagimoto
, and
C.
Takahashi
,
Nonlinear Opt.
13
,
3
(
1995
).
9.
K.
Kamada
,
M.
Ueda
,
T.
Sakaguchi
,
K.
Ohta
, and
T.
Fukumi
,
J. Opt. Soc. Am. B
15
,
838
(
1998
).
10.
R. W. Boyd, Nonlinear Optics (Academic, San Diego, 1992).
11.
G. M.
Carter
,
M. K.
Thakur
,
Y. J.
Chen
, and
J. V.
Hryniewicz
,
Appl. Phys. Lett.
47
,
457
(
1985
).
12.
Y.
Pang
and
P. N.
Prasad
,
J. Chem. Phys.
93
,
2201
(
1990
).
13.
Y.
Yamaoka
,
R.
Morita
, and
M.
Yamashita
,
Nonlinear Opt.
22
,
381
(
1999
).
14.
H.
Murakami
,
R.
Morita
, and
M.
Yamashita
,
Nonlinear Opt.
22
,
385
(
1999
).
15.
W. Liptay, Excited States, edited by E. C. Lim (Academic, New York, 1974), p. 129.
16.
R.
Morita
and
M.
Yamashita
,
Jpn. J. Appl. Phys., Part 2
32
,
L905
(
1993
).
17.
C. C.
Teng
and
A. F.
Garito
,
Phys. Rev. B
28
,
6766
(
1983
).
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