Abstract

We report the femtosecond dynamics of fluorescence anisotropy excited through the two-photon absorption (TPA), which provides direct signatures of delocalized electronic excitations for symmetrical macromolecular architectures. Two-photon excited fluorescence anisotropy is strongly correlated with the orientation and value of the transition moment from the excited state to the second and higher lying states. For macromolecular systems it leads to a relatively low initial fluorescence anisotropy and specific femtosecond anisotropy dynamics. We have experimentally demonstrated qualitatively different anisotropy dynamics for two- and one-photon absorption excitations for strongly coupled ring architecture prospective for artificial-light-harvesting applications and possessing an enhanced TPA-absorption cross section.

© 2007 Optical Society of America

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2007

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mancal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, Nature 446, 782 (2007).
[CrossRef] [PubMed]

O. Varnavski, X. Yan, O. Mongin, M. Blanchard-Desce, and T. Goodson III, J. Phys. Chem. C. 111, 149 (2007).
[CrossRef]

2006

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Y. L. Slominsky, and A. D. Kachkovski, Chem. Phys. 321, 257 (2006).
[CrossRef]

A. Bhaskar, G. Ramakrishna, K. Hagedorn, O. Varnavski, E. Mena-Osteritz, P. Bäuerle, and T. Goodson III, J. Phys. Chem. B 111, 946 (2006).
[CrossRef]

A. M. Kelley, L. C. T. Shoute, M. Blanchard-Desce, G. P. Bartolomew, and G. C. Bazan, Mol. Phys. 104, 1239 (2006).
[CrossRef]

2005

T. Goodson III, Annu. Rev. Phys. Chem. 56, 581 (2005).
[CrossRef]

T. Goodson III, Acc. Chem. Res. 38, 99 (2005).
[CrossRef]

2004

G. R. Fleming and G. Scholes, Nature 431, 256 (2004).
[CrossRef] [PubMed]

S.-H. Lim, T. G. Bjorklund, F. C. Spano, and C. J. Bardeen, Phys. Rev. Lett. 92, 107402 (2004).
[CrossRef] [PubMed]

2003

X. Zhang and A. Matzger, J. Org. Chem. 68, 9813 (2003).
[CrossRef] [PubMed]

2002

D. Beljonne, W. Wenseleers, E. Zojer, Z. Shuai, H. Vogel, S. J. K. Pond, J. W. Perry, S. R. Marder, and J.-L. Bredas, Adv. Funct. Mater. 12, 631 (2002).
[CrossRef]

P. Cronstrand, Y. Luo, and H. Angren, J. Chem. Phys. 117, 11102 (2002).
[CrossRef]

2001

M. Dahlbom, T. Pullerits, S. Mukamel, and V. Sundström, J. Phys. Chem. B 105, 5515 (2001).
[CrossRef]

2000

S. V. Frolov, Z. Bao, M. Wohlgenannt, and Z. V. Vardeny, Phys. Rev. Lett. 85, 2196 (2000).
[CrossRef] [PubMed]

J. Krömer, I. R. Carreras, G. Fuhrmannn, C. Munsch, M. Wunderlin, T. Debaerdemaeker, E. Mena-Osteriritz, and P. Bäuerle, Angew. Chem., Int. Ed. 39, 3481 (2000).
[CrossRef]

1999

J. R. Lakowicz, Principles of Fluorescence Spectroscopy (Kluwer, 1999).

1997

A. Volkmer, D. A. Hatrick, and D. J. S. Birch, Meas. Sci. Technol. 8, 1337 (1997).
[CrossRef]

1996

1994

C. Wan and C. K. Johnson, Chem. Phys. 179, 513 (1994).
[CrossRef]

1993

K. Wynne and R. M. Hochstrasser, Chem. Phys. 171, 179 (1993).
[CrossRef]

1992

J. R. Lakowicz, I. Gryczynski, Z. Gryczynski, E. Danielsen, and M. J. Wirth, J. Phys. Chem. 96, 3000 (1992).
[CrossRef]

1974

W. M. McClain, Acc. Chem. Res. 7, 129 (1974).
[CrossRef]

1973

W. M. McClain, J. Chem. Phys. 58, 324 (1973).
[CrossRef]

Ahn, T.-K.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mancal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, Nature 446, 782 (2007).
[CrossRef] [PubMed]

Angren, H.

P. Cronstrand, Y. Luo, and H. Angren, J. Chem. Phys. 117, 11102 (2002).
[CrossRef]

Bao, Z.

S. V. Frolov, Z. Bao, M. Wohlgenannt, and Z. V. Vardeny, Phys. Rev. Lett. 85, 2196 (2000).
[CrossRef] [PubMed]

Bardeen, C. J.

S.-H. Lim, T. G. Bjorklund, F. C. Spano, and C. J. Bardeen, Phys. Rev. Lett. 92, 107402 (2004).
[CrossRef] [PubMed]

Bartolomew, G. P.

A. M. Kelley, L. C. T. Shoute, M. Blanchard-Desce, G. P. Bartolomew, and G. C. Bazan, Mol. Phys. 104, 1239 (2006).
[CrossRef]

Bäuerle, P.

A. Bhaskar, G. Ramakrishna, K. Hagedorn, O. Varnavski, E. Mena-Osteritz, P. Bäuerle, and T. Goodson III, J. Phys. Chem. B 111, 946 (2006).
[CrossRef]

J. Krömer, I. R. Carreras, G. Fuhrmannn, C. Munsch, M. Wunderlin, T. Debaerdemaeker, E. Mena-Osteriritz, and P. Bäuerle, Angew. Chem., Int. Ed. 39, 3481 (2000).
[CrossRef]

Bazan, G. C.

A. M. Kelley, L. C. T. Shoute, M. Blanchard-Desce, G. P. Bartolomew, and G. C. Bazan, Mol. Phys. 104, 1239 (2006).
[CrossRef]

Belfield, K. D.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Y. L. Slominsky, and A. D. Kachkovski, Chem. Phys. 321, 257 (2006).
[CrossRef]

Beljonne, D.

D. Beljonne, W. Wenseleers, E. Zojer, Z. Shuai, H. Vogel, S. J. K. Pond, J. W. Perry, S. R. Marder, and J.-L. Bredas, Adv. Funct. Mater. 12, 631 (2002).
[CrossRef]

Bhaskar, A.

A. Bhaskar, G. Ramakrishna, K. Hagedorn, O. Varnavski, E. Mena-Osteritz, P. Bäuerle, and T. Goodson III, J. Phys. Chem. B 111, 946 (2006).
[CrossRef]

Birch, D. J. S.

A. Volkmer, D. A. Hatrick, and D. J. S. Birch, Meas. Sci. Technol. 8, 1337 (1997).
[CrossRef]

Bjorklund, T. G.

S.-H. Lim, T. G. Bjorklund, F. C. Spano, and C. J. Bardeen, Phys. Rev. Lett. 92, 107402 (2004).
[CrossRef] [PubMed]

Blanchard-Desce, M.

O. Varnavski, X. Yan, O. Mongin, M. Blanchard-Desce, and T. Goodson III, J. Phys. Chem. C. 111, 149 (2007).
[CrossRef]

A. M. Kelley, L. C. T. Shoute, M. Blanchard-Desce, G. P. Bartolomew, and G. C. Bazan, Mol. Phys. 104, 1239 (2006).
[CrossRef]

Blankenship, R. E.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mancal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, Nature 446, 782 (2007).
[CrossRef] [PubMed]

Bondar, M. V.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Y. L. Slominsky, and A. D. Kachkovski, Chem. Phys. 321, 257 (2006).
[CrossRef]

Bredas, J.-L.

D. Beljonne, W. Wenseleers, E. Zojer, Z. Shuai, H. Vogel, S. J. K. Pond, J. W. Perry, S. R. Marder, and J.-L. Bredas, Adv. Funct. Mater. 12, 631 (2002).
[CrossRef]

Calhoun, T. R.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mancal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, Nature 446, 782 (2007).
[CrossRef] [PubMed]

Carreras, I. R.

J. Krömer, I. R. Carreras, G. Fuhrmannn, C. Munsch, M. Wunderlin, T. Debaerdemaeker, E. Mena-Osteriritz, and P. Bäuerle, Angew. Chem., Int. Ed. 39, 3481 (2000).
[CrossRef]

Cheng, Y.-C.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mancal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, Nature 446, 782 (2007).
[CrossRef] [PubMed]

Cronstrand, P.

P. Cronstrand, Y. Luo, and H. Angren, J. Chem. Phys. 117, 11102 (2002).
[CrossRef]

Dahlbom, M.

M. Dahlbom, T. Pullerits, S. Mukamel, and V. Sundström, J. Phys. Chem. B 105, 5515 (2001).
[CrossRef]

Danielsen, E.

J. R. Lakowicz, I. Gryczynski, Z. Gryczynski, E. Danielsen, and M. J. Wirth, J. Phys. Chem. 96, 3000 (1992).
[CrossRef]

Debaerdemaeker, T.

J. Krömer, I. R. Carreras, G. Fuhrmannn, C. Munsch, M. Wunderlin, T. Debaerdemaeker, E. Mena-Osteriritz, and P. Bäuerle, Angew. Chem., Int. Ed. 39, 3481 (2000).
[CrossRef]

Engel, G. S.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mancal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, Nature 446, 782 (2007).
[CrossRef] [PubMed]

Fleming, G. R.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mancal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, Nature 446, 782 (2007).
[CrossRef] [PubMed]

G. R. Fleming and G. Scholes, Nature 431, 256 (2004).
[CrossRef] [PubMed]

Frolov, S. V.

S. V. Frolov, Z. Bao, M. Wohlgenannt, and Z. V. Vardeny, Phys. Rev. Lett. 85, 2196 (2000).
[CrossRef] [PubMed]

Fu, J.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Y. L. Slominsky, and A. D. Kachkovski, Chem. Phys. 321, 257 (2006).
[CrossRef]

Fuhrmannn, G.

J. Krömer, I. R. Carreras, G. Fuhrmannn, C. Munsch, M. Wunderlin, T. Debaerdemaeker, E. Mena-Osteriritz, and P. Bäuerle, Angew. Chem., Int. Ed. 39, 3481 (2000).
[CrossRef]

Goodson III, T.

O. Varnavski, X. Yan, O. Mongin, M. Blanchard-Desce, and T. Goodson III, J. Phys. Chem. C. 111, 149 (2007).
[CrossRef]

A. Bhaskar, G. Ramakrishna, K. Hagedorn, O. Varnavski, E. Mena-Osteritz, P. Bäuerle, and T. Goodson III, J. Phys. Chem. B 111, 946 (2006).
[CrossRef]

T. Goodson III, Annu. Rev. Phys. Chem. 56, 581 (2005).
[CrossRef]

T. Goodson III, Acc. Chem. Res. 38, 99 (2005).
[CrossRef]

Gryczynski, I.

J. R. Lakowicz, I. Gryczynski, Z. Gryczynski, E. Danielsen, and M. J. Wirth, J. Phys. Chem. 96, 3000 (1992).
[CrossRef]

Gryczynski, Z.

J. R. Lakowicz, I. Gryczynski, Z. Gryczynski, E. Danielsen, and M. J. Wirth, J. Phys. Chem. 96, 3000 (1992).
[CrossRef]

Hagan, D. J.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Y. L. Slominsky, and A. D. Kachkovski, Chem. Phys. 321, 257 (2006).
[CrossRef]

Hagedorn, K.

A. Bhaskar, G. Ramakrishna, K. Hagedorn, O. Varnavski, E. Mena-Osteritz, P. Bäuerle, and T. Goodson III, J. Phys. Chem. B 111, 946 (2006).
[CrossRef]

Hatrick, D. A.

A. Volkmer, D. A. Hatrick, and D. J. S. Birch, Meas. Sci. Technol. 8, 1337 (1997).
[CrossRef]

Hochstrasser, R. M.

K. Wynne and R. M. Hochstrasser, Chem. Phys. 171, 179 (1993).
[CrossRef]

Johnson, C. K.

C. Wan and C. K. Johnson, Chem. Phys. 179, 513 (1994).
[CrossRef]

Kachkovski, A. D.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Y. L. Slominsky, and A. D. Kachkovski, Chem. Phys. 321, 257 (2006).
[CrossRef]

Kelley, A. M.

A. M. Kelley, L. C. T. Shoute, M. Blanchard-Desce, G. P. Bartolomew, and G. C. Bazan, Mol. Phys. 104, 1239 (2006).
[CrossRef]

Krömer, J.

J. Krömer, I. R. Carreras, G. Fuhrmannn, C. Munsch, M. Wunderlin, T. Debaerdemaeker, E. Mena-Osteriritz, and P. Bäuerle, Angew. Chem., Int. Ed. 39, 3481 (2000).
[CrossRef]

Lakowicz, J. R.

J. R. Lakowicz, Principles of Fluorescence Spectroscopy (Kluwer, 1999).

J. R. Lakowicz, I. Gryczynski, Z. Gryczynski, E. Danielsen, and M. J. Wirth, J. Phys. Chem. 96, 3000 (1992).
[CrossRef]

Lim, S.-H.

S.-H. Lim, T. G. Bjorklund, F. C. Spano, and C. J. Bardeen, Phys. Rev. Lett. 92, 107402 (2004).
[CrossRef] [PubMed]

Luo, Y.

P. Cronstrand, Y. Luo, and H. Angren, J. Chem. Phys. 117, 11102 (2002).
[CrossRef]

Mancal, T.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mancal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, Nature 446, 782 (2007).
[CrossRef] [PubMed]

Marder, S. R.

D. Beljonne, W. Wenseleers, E. Zojer, Z. Shuai, H. Vogel, S. J. K. Pond, J. W. Perry, S. R. Marder, and J.-L. Bredas, Adv. Funct. Mater. 12, 631 (2002).
[CrossRef]

Matzger, A.

X. Zhang and A. Matzger, J. Org. Chem. 68, 9813 (2003).
[CrossRef] [PubMed]

McClain, W. M.

W. M. McClain, Acc. Chem. Res. 7, 129 (1974).
[CrossRef]

W. M. McClain, J. Chem. Phys. 58, 324 (1973).
[CrossRef]

Mena-Osteriritz, E.

J. Krömer, I. R. Carreras, G. Fuhrmannn, C. Munsch, M. Wunderlin, T. Debaerdemaeker, E. Mena-Osteriritz, and P. Bäuerle, Angew. Chem., Int. Ed. 39, 3481 (2000).
[CrossRef]

Mena-Osteritz, E.

A. Bhaskar, G. Ramakrishna, K. Hagedorn, O. Varnavski, E. Mena-Osteritz, P. Bäuerle, and T. Goodson III, J. Phys. Chem. B 111, 946 (2006).
[CrossRef]

Mongin, O.

O. Varnavski, X. Yan, O. Mongin, M. Blanchard-Desce, and T. Goodson III, J. Phys. Chem. C. 111, 149 (2007).
[CrossRef]

Mukamel, S.

M. Dahlbom, T. Pullerits, S. Mukamel, and V. Sundström, J. Phys. Chem. B 105, 5515 (2001).
[CrossRef]

Munsch, C.

J. Krömer, I. R. Carreras, G. Fuhrmannn, C. Munsch, M. Wunderlin, T. Debaerdemaeker, E. Mena-Osteriritz, and P. Bäuerle, Angew. Chem., Int. Ed. 39, 3481 (2000).
[CrossRef]

Padilha, L. A.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Y. L. Slominsky, and A. D. Kachkovski, Chem. Phys. 321, 257 (2006).
[CrossRef]

Perry, J. W.

D. Beljonne, W. Wenseleers, E. Zojer, Z. Shuai, H. Vogel, S. J. K. Pond, J. W. Perry, S. R. Marder, and J.-L. Bredas, Adv. Funct. Mater. 12, 631 (2002).
[CrossRef]

Pond, S. J. K.

D. Beljonne, W. Wenseleers, E. Zojer, Z. Shuai, H. Vogel, S. J. K. Pond, J. W. Perry, S. R. Marder, and J.-L. Bredas, Adv. Funct. Mater. 12, 631 (2002).
[CrossRef]

Przhonska, O. V.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Y. L. Slominsky, and A. D. Kachkovski, Chem. Phys. 321, 257 (2006).
[CrossRef]

Pullerits, T.

M. Dahlbom, T. Pullerits, S. Mukamel, and V. Sundström, J. Phys. Chem. B 105, 5515 (2001).
[CrossRef]

Ramakrishna, G.

A. Bhaskar, G. Ramakrishna, K. Hagedorn, O. Varnavski, E. Mena-Osteritz, P. Bäuerle, and T. Goodson III, J. Phys. Chem. B 111, 946 (2006).
[CrossRef]

Read, E. L.

G. S. Engel, T. R. Calhoun, E. L. Read, T.-K. Ahn, T. Mancal, Y.-C. Cheng, R. E. Blankenship, and G. R. Fleming, Nature 446, 782 (2007).
[CrossRef] [PubMed]

Scholes, G.

G. R. Fleming and G. Scholes, Nature 431, 256 (2004).
[CrossRef] [PubMed]

Shoute, L. C. T.

A. M. Kelley, L. C. T. Shoute, M. Blanchard-Desce, G. P. Bartolomew, and G. C. Bazan, Mol. Phys. 104, 1239 (2006).
[CrossRef]

Shuai, Z.

D. Beljonne, W. Wenseleers, E. Zojer, Z. Shuai, H. Vogel, S. J. K. Pond, J. W. Perry, S. R. Marder, and J.-L. Bredas, Adv. Funct. Mater. 12, 631 (2002).
[CrossRef]

Slominsky, Y. L.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Y. L. Slominsky, and A. D. Kachkovski, Chem. Phys. 321, 257 (2006).
[CrossRef]

Spano, F. C.

S.-H. Lim, T. G. Bjorklund, F. C. Spano, and C. J. Bardeen, Phys. Rev. Lett. 92, 107402 (2004).
[CrossRef] [PubMed]

Sundström, V.

M. Dahlbom, T. Pullerits, S. Mukamel, and V. Sundström, J. Phys. Chem. B 105, 5515 (2001).
[CrossRef]

Van Stryland, E. W.

J. Fu, O. V. Przhonska, L. A. Padilha, D. J. Hagan, E. W. Van Stryland, K. D. Belfield, M. V. Bondar, Y. L. Slominsky, and A. D. Kachkovski, Chem. Phys. 321, 257 (2006).
[CrossRef]

Vardeny, Z. V.

S. V. Frolov, Z. Bao, M. Wohlgenannt, and Z. V. Vardeny, Phys. Rev. Lett. 85, 2196 (2000).
[CrossRef] [PubMed]

Varnavski, O.

O. Varnavski, X. Yan, O. Mongin, M. Blanchard-Desce, and T. Goodson III, J. Phys. Chem. C. 111, 149 (2007).
[CrossRef]

A. Bhaskar, G. Ramakrishna, K. Hagedorn, O. Varnavski, E. Mena-Osteritz, P. Bäuerle, and T. Goodson III, J. Phys. Chem. B 111, 946 (2006).
[CrossRef]

Vogel, H.

D. Beljonne, W. Wenseleers, E. Zojer, Z. Shuai, H. Vogel, S. J. K. Pond, J. W. Perry, S. R. Marder, and J.-L. Bredas, Adv. Funct. Mater. 12, 631 (2002).
[CrossRef]

Volkmer, A.

A. Volkmer, D. A. Hatrick, and D. J. S. Birch, Meas. Sci. Technol. 8, 1337 (1997).
[CrossRef]

Wan, C.

C. Wan and C. K. Johnson, Chem. Phys. 179, 513 (1994).
[CrossRef]

Webb, W. W.

Wenseleers, W.

D. Beljonne, W. Wenseleers, E. Zojer, Z. Shuai, H. Vogel, S. J. K. Pond, J. W. Perry, S. R. Marder, and J.-L. Bredas, Adv. Funct. Mater. 12, 631 (2002).
[CrossRef]

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Figures (3)

Fig. 1
Fig. 1

Structures of oligothiophene systems investigated in this work. a, Macrocyclic thiophene oligimer C [ 3 T ̱ DA ] 5 ; b, α-quaterthiophene.

Fig. 2
Fig. 2

Time-resolved fluorescence anisotropy decay under two-photon excitation for (1) macrocyclic thiophene as compared with that for (2) α-quaterthiophene. The fluorescence detection wavelength is 540 nm . The instrument response function for fluorescence intensity is also shown (dashed–dotted curve). 3, Fluorescence anisotropy dynamics for Rhodamine 6G at 575 nm .

Fig. 3
Fig. 3

Fluorescence anisotropy decay of the macrocyclic thiophene after two- and one-photon excitation. Best fits for the anisotropy after convolution procedure are shown by solid curves. Instrument response function for fluorescence intensity is represented by the dashed-dotted curve. Inset: Best fit fluorescence anisotropy (before convolution procedure) for OPE (dash curve) and TPE (solid curve). Energy level structure for three-state model is also shown.

Equations (2)

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σ 2 i N [ 2 ( p μ i g ) ( μ f i p ) ν i g ν + i Γ i g ] 2 ,
r TPE = 18 cos ( γ β e m ) cos ( β e m ) cos γ 7 cos 2 γ + 1 7 ( 2 cos 2 γ + 1 ) ,

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