A new form of time-resolved multiphoton-excited fluorescence imaging is described and used to study electric-field-induced reorientation dynamics in polymer-dispersed liquid crystal (LC) films. This method provides information on the static and dynamic LC orientation via polarization-dependent three-photon excitation of the nematic ultraviolet chromophores in these materials. Static fluorescence images are obtained with ≈235 nm resolution in all three dimensions. In dynamics studies, the three-photon-excited fluorescence is recorded as a function of time and position over individual LC droplets, as an applied electric field is switched on and off. Time-resolved images with ≈235 nm spatial resolution and 200 μs time resolution are obtained. Movies depicting the local reorientation dynamics are prepared from these data and are presented for common ellipsoidal LC droplets and for novel toroidal droplets. The field-induced reorientation dynamics within the ellipsoidal droplets are shown to be more complex (i.e., spatially variable) than in the toroidal droplets. Dynamical complexity is concluded to arise from LC organizational complexity in the droplets. The bipolar configuration found in ellipsoidal droplets incorporates bend and splay deformations of the nematic phase and two disclination points. In contrast, toroidal droplets incorporate a simpler toroidal configuration in which only bend deformations occur.

1.
P. S.
Drzaic
,
J. Appl. Phys.
60
,
2142
(
1986
).
2.
S.
Zumer
and
J. W.
Doane
,
Phys. Rev. A
34
,
3373
(
1986
).
3.
J. W. Doane, in Liquid Crystals: Applications and Uses, edited by B. Bahadur (World Scientific, Singapore, 1990), Vol. 1, p. 361.
4.
H.-S.
Kitzerow
,
Liq. Cryst.
16
,
1
(
1994
).
5.
G. P. Crawford, J. W. Doane, and S. Zumer, in Handbook of Liquid Crystal Research, edited by P. J. Collings and J. S. Patel (Oxford University Press, New York, 1997), p. 347.
6.
F. P.
Nicoletta
,
G.
De Filpo
,
J.
Lanzo
, and
G.
Chidichimo
,
Appl. Phys. Lett.
74
,
3945
(
1999
).
7.
P. S.
Drzaic
,
Mol. Cryst. Liq. Cryst.
154
,
289
(
1988
).
8.
R.
Ondris-Crawford
,
E. P.
Boyko
,
B. G.
Wagner
,
J. H.
Erdmann
,
S.
Zumer
, and
J. W.
Doane
,
J. Appl. Phys.
69
,
6380
(
1991
).
9.
E.
Berggren
,
C.
Zannoni
,
C.
Chiccoli
,
P.
Pasini
, and
F.
Semeria
,
Chem. Phys. Lett.
197
,
224
(
1992
).
10.
C.
Chiccoli
,
P.
Pasini
,
F.
Semeria
, and
C.
Zannoni
,
Mol. Cryst. Liq. Cryst.
221
,
19
(
1992
).
11.
G. P.
Montgomery
,
J. L.
West
, and
W.
Tamura-Lis
,
J. Appl. Phys.
69
,
1605
(
1991
).
12.
J. B.
Whitehead
,
S.
Zumer
, and
J. W.
Doane
,
J. Appl. Phys.
73
,
1057
(
1993
).
13.
F.
Bloisi
,
C.
Ruocchio
,
P.
Terrecuso
, and
L.
Vicari
,
Opt. Lett.
21
,
95
(
1996
).
14.
G.
Chidichimo
,
Z.
Huang
,
C.
Caruso
,
G.
De Filpo
, and
F. P.
Nicoletta
,
Mol. Cryst. Liq. Cryst. Sci. Technol., Sect. A
299
,
379
(
1997
).
15.
P. G. De Gennes and J. Prost, The Physics of Liquid Crystals, 2nd ed. (Oxford University Press, New York, 1993).
16.
D. A.
Higgins
,
Adv. Mater. (Weinheim, Ger.)
12
,
251
(
2000
).
17.
P. S.
Drzaic
,
Liq. Cryst.
3
,
1543
(
1988
).
18.
J.
Erdmann
,
J. W.
Doane
,
S.
Zumer
, and
G.
Chidichimo
,
Proc. SPIE
1080
,
32
(
1989
).
19.
B.-G.
Wu
,
J. H.
Erdmann
, and
J. W.
Doane
,
Liq. Cryst.
5
,
1453
(
1989
).
20.
C. A.
McFarland
,
J. L.
Koenig
, and
J. L.
West
,
Appl. Spectrosc.
47
,
321
(
1993
).
21.
S. R.
Challa
,
S.-Q.
Wang
, and
J. L.
Koenig
,
Appl. Spectrosc.
49
,
267
(
1995
).
22.
S.
Kohri
,
J.
Kobayashi
,
S.
Tahata
,
S.
Kita
,
I.
Karino
, and
T.
Yokoyama
,
Appl. Spectrosc.
47
,
1367
(
1993
).
23.
R.
Hasegawa
,
M.
Sakamoto
, and
H.
Sasaki
,
Appl. Spectrosc.
47
,
1386
(
1993
).
24.
C.
Chiccoli
,
P.
Pasini
,
G.
Skacej
,
C.
Zannoni
, and
S.
Zumer
,
Phys. Rev. E
62
,
3766
(
2000
).
25.
E.
Mei
and
D. A.
Higgins
,
Appl. Phys. Lett.
73
,
3515
(
1998
).
26.
E.
Mei
and
D. A.
Higgins
,
J. Phys. Chem. A
102
,
7558
(
1998
).
27.
D. A.
Higgins
,
E.
Mei
, and
X.
Liao
,
Proc. SPIE
3607
,
26
(
1999
).
28.
E.
Mei
and
D. A.
Higgins
,
J. Chem. Phys.
112
,
7839
(
2000
).
29.
D. A.
Higgins
,
X.
Liao
,
J.
Hall
, and
E.
Mei
,
J. Phys. Chem. B
105
,
5874
(
2001
).
30.
A.
Golemme
,
S.
Zumer
,
J. W.
Doane
, and
M. E.
Neubert
,
Phys. Rev. A
37
,
559
(
1988
).
31.
K. L.
Buchert
,
J. L.
Koenig
,
S.-Q.
Wang
, and
J. L.
West
,
Appl. Spectrosc.
47
,
942
(
1993
).
32.
M.
Ambrozic
,
P.
Formoso
,
A.
Golemme
, and
S.
Zumer
,
Phys. Rev. E
56
,
1825
(
1997
).
33.
S. C.
Jain
and
D. K.
Rout
,
J. Appl. Phys.
70
,
6988
(
1991
).
34.
S. C.
Jain
,
R. S.
Thakur
, and
S. T.
Lakshmikumar
,
J. Appl. Phys.
73
,
3744
(
1993
).
35.
K.
Amundson
,
Phys. Rev. E
53
,
2412
(
1996
).
36.
K.
Amundson
,
A.
van Blaaderen
, and
P.
Wiltzius
,
Phys. Rev. E
55
,
1646
(
1997
).
37.
W.
Denk
,
J. H.
Strickler
, and
W. W.
Webb
,
Science
248
,
73
(
1990
).
38.
J. B.
Shear
,
Anal. Chem.
71
,
598A
(
1999
).
39.
G. H.
Springer
and
D. A.
Higgins
,
J. Am. Chem. Soc.
122
,
6801
(
2000
).
40.
G. H.
Springer
and
D. A.
Higgins
,
Chem. Mater.
12
,
1372
(
2000
).
41.
B. J.
Luther
,
G. H.
Springer
, and
D. A.
Higgins
,
Chem. Mater.
13
,
2281
(
2001
).
42.
M.
Gu
,
Opt. Lett.
21
,
988
(
1996
).
43.
E.
Mei
and
D. A.
Higgins
,
Langmuir
14
,
1945
(
1998
).
44.
W. M.
McClain
,
J. Chem. Phys.
57
,
2264
(
1974
).
45.
Y. R. Shen, The Principles of Nonlinear Optics (Wiley-Interscience, New York, 1984).
46.
D. Lee and A. C. Albrecht, in Advances in Infrared and Raman Spectroscopy, edited by R. J. H. Clark and R. E. Hester (Wiley, New York, 1985).
47.
D. M.
Friedrich
,
J. Chem. Phys.
75
,
3258
(
1981
).
48.
D. A. Higgins, G. H. Springer, and B. J. Luther (unpublished).
49.
B.
Sick
,
B.
Hecht
, and
L.
Novotny
,
Phys. Rev. Lett.
85
,
4482
(
2000
).
50.
J.
Deitche
,
M.
Kempe
, and
W.
Rudolph
,
J. Microsc.
174
,
69
(
1994
).
51.
P. K.
Chan
and
A. D.
Rey
,
Liq. Cryst.
23
,
677
(
1997
).
52.
H.-S.
Kitzerow
,
H.
Molsen
, and
G.
Heppke
,
Appl. Phys. Lett.
60
,
3093
(
1992
).
53.
H.
Fujikake
,
M.
Kawakita
,
Y.
Iino
,
H.
Sato
, and
H.
Kikuchi
,
Jpn. J. Appl. Phys., Part 1
41
,
4609
(
2002
).
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