We report a new spectroscopic measurement based on fifth order nonlinear response from a molecule in a room temperature liquid. In conjunction with conventional three pulse stimulated photon echo, detailed information on solvent–solute dynamics for a wide range of time scales has been obtained. Both the ultrafast inertial components and much slower dynamics of the solvent are found to make important contributions to the solvent relaxation. The potential of the fifth order measurements is discussed via numerical calculations using model solvent spectral densities.

1.
A. J.
Leggett
,
S.
Chakravarty
,
A. T.
Dorsey
,
M. P. A.
Fisher
,
A.
Garg
, and
W.
Zwerger
,
Rev. Mod. Phys.
59
,
1
(
1987
).
2.
M.
Cho
and
G. R.
Fleming
,
J. Phys. Chem.
98
,
3478
(
1994
).
3.
T. Joo, M. Cho, J. Yu, Y. Jia, and G. R. Fleming, in Ultrafast Phenomena IX, edited by G. A. Mourou, A. H. Zewail, P. F. Barbara, and W. H. Knox (in press, 1994).
4.
A. M.
Weiner
,
S.
De Silvestri
, and
E. P.
Ippen
,
J. Opt. Soc. Am. B
2
,
654
(
1985
).
5.
P. C.
Becker
,
H. L.
Fragnito
,
J. Y.
Bigot
,
C. H.
Brito Cruz
,
R. L.
Fork
, and
C. V.
Shank
,
Phys. Rev. Lett.
63
,
505
(
1989
).
6.
J.-Y.
Bigot
,
M. T.
Portella
,
R. W.
Schoenlein
,
C. J.
Bardeen
,
A.
Migus
, and
C. V.
Shank
,
Phys. Rev. Lett.
66
,
1138
(
1991
).
7.
E. T. J.
Nibbering
,
D. A.
Wiersma
, and
K.
Duppen
,
Phys. Rev. Lett.
66
,
2464
(
1991
).
8.
W. P.
de Boeij
,
M. S.
Pshenichnikov
,
K.
Duppen
, and
D. A.
Wiersma
,
Chem. Phys. Lett.
224
,
243
(
1994
).
9.
T.
Joo
and
A. C.
Albrecht
,
Chem. Phys.
176
,
233
(
1993
).
10.
(a)
C. J.
Bardeen
and
C. V.
Shank
,
Chem. Phys. Lett.
203
,
535
(
1993
);
(b)
C. J.
Bardeen
and
C. V.
Shank
,
Chem. Phys. Lett.
226
,
310
(
1994
).,
Chem. Phys. Lett.
11.
P. Vöhringer, D. C. Arnett, R. A. Westervelt, M. J. Fedstein, and N. F. Scherer, J. Chem. Phys. (in press).
12.
M. T.
Asaki
,
C.-P.
Huang
,
D.
Garvey
,
J.
Zhou
,
H. C.
Kapteyn
, and
M. M.
Murnane
,
Opt. Lett.
18
,
977
(
1993
).
13.
E.
Hanamura
,
J. Phys. Soc. Jpn.
52
,
2258
(
1983
).
14.
B. D.
Fainberg
,
Opt. Spectrosc.
55
,
669
(
1983
).
15.
Y. J.
Yan
and
S.
Mukamel
,
J. Chem. Phys.
94
,
179
(
1991
).
16.
W.
Bosma
,
Y. J.
Yan
,
S.
Mukamel
,
Phys. Rev. A
42
,
6920
(
1990
).
17.
(a)
S. J.
Rosenthal
,
X. L.
Xie
,
M.
Du
, and
G. R.
Fleming
,
J. Chem. Phys.
95
,
4715
(
1991
);
(b)
S. J.
Rosenthal
,
R.
Jimenez
,
G. R.
Fleming
,
P. V.
Kumar
, and
M.
Maroncelli
,
J. Mol. Liq.
60
,
25
(
1994
).
18.
R.
Jimenez
,
G. R.
Fleming
,
P. V.
Kumar
, and
M.
Maroncelli
,
Nature (London)
369
,
471
(
1994
).
19.
P. F.
Barbara
and
W.
Jarzeba
,
Adv. Photochem.
15
,
1
(
1990
).
20.
M.
Maroncelli
and
G. R.
Fleming
,
J. Chem. Phys.
89
,
5044
(
1988
).
21.
M.
Maroncelli
,
J. Chem. Phys.
94
,
2084
(
1991
).
22.
E. A.
Carter
and
J. T.
Hynes
,
J. Chem. Phys.
94
,
5961
(
1991
).
23.
M.
Cho
,
G. R.
Fleming
,
S.
Saito
,
I.
Ohmine
, and
R. M.
Stratt
,
J. Chem. Phys.
100
,
6672
(
1994
).
24.
S.
Roy
and
B.
Bagchi
,
J. Chem. Phys.
99
,
9938
(
1993
).
25.
F. O.
Raineri
,
H.
Resat
,
B.-C.
Perng
,
F.
Hirata
, and
H. L.
Friedman
,
J. Chem. Phys.
100
,
1477
(
1994
).
26.
N. E.
Shemetulskis
and
R. F.
Loring
,
J. Chem. Phys.
97
,
1217
(
1992
).
27.
J. N.
Gehlen
,
M.
Marchi
, and
D.
Chandler
,
Science
263
,
499
(
1994
).
28.
N. Scherer (private communication);
D. A. Wiersma, presented at the International Workshop on Laser Physics, Transient Coherent Phenomena, Oct. 10–14, 1994, New York.
29.
T. Joo, J. Yu, Y. Jia, and G. R. Fleming (manuscript in preparation).
30.
S. J.
Rosenthal
,
B. J.
Schartz
, and
P. J.
Rossky
,
Chem. Phys. Lett.
229
,
443
(
1994
).
31.
R. F.
Loring
and
S.
Mukamel
,
Chem. Phys. Lett.
114
,
426
(
1985
).
32.
R. M.
Stratt
and
M.
Cho
,
J. Chem. Phys.
100
,
6700
(
1994
).
33.
Y. J. Chang and E. W. Castner, J. Chem. Phys. (submitted).
34.
M.
Cho
,
S. J.
Rosenthal
,
N. F.
Scherer
, and
L. D.
Ziegler
,
J. Chem. Phys.
96
,
5033
(
1992
).
35.
M.
Cho
and
G. R.
Fleming
,
J. Phys. Chem.
98
,
2848
(
1993
).
36.
M. Maroncelli, P. V. Kumar, A. Papazyan, M. L. Horng, S. J. Rosenthal, and G. R. Fleming, Proceedings of the International Workshop, Ultrafast Reaction Dynamics and Solvent Effects (Abbaye de Royaumont, France, 1993).
37.
R. O.
Raineri
and
H. L.
Friedman
,
J. Chem. Phys.
101
,
6111
(
1994
).
38.
P.
Cong
,
Y.-J.
Yan
,
H. P.
Deuel
, and
J. D.
Simon
,
J. Chem. Phys.
100
,
7855
(
1994
).
This content is only available via PDF.
You do not currently have access to this content.