Single Molecule Spectroscopy as a Probe for Dye-Polymer Interactions

[en] Experimental (Single Molecule Spectroscopy) and theoretical (quantum-chemical calculations and Monte Carlo and molecular dynamics simulations) techniques are combined to investigate the behavior and dynamics of a polymer-dye molecule system. It is shown that the dye molecule of interest (1,1'-dioctadecyl-3,3,3',3'-tetramethylindo-dicarbocyanine) adopts two classes of conformations, namely planar and nonplanar ones, when embedded in a poly(styrene) matrix. From an in-depth analysis of the fluorescence lifetime trajectories, the planar conformers can be further classified according to the way their alkyl side chains interact with the surrounding poly(styrene) chains.

Disciplines :

Physics

Author, co-author :

Vallée, R.A.L.

Marsal, Philippe

Braeken, E.

Habuchi, S.

De Schryver, F.C.

Van Der Auweraer, M.

Beljonne, David ; Université de Mons > Faculté des Sciences > Chimie des matériaux nouveaux

Hofkens, J.

Language :

English

Title :

Single Molecule Spectroscopy as a Probe for Dye-Polymer Interactions

Publication date :

31 August 2005

Journal title :

Journal of the American Chemical Society

ISSN :

0002-7863

Publisher :

American Chemical Society, United States - District of Columbia

Volume :

127

Issue :

Pages :

12011-12020

Peer reviewed :

Peer Reviewed verified by ORBi

Research unit :

S817 - Chimie des matériaux nouveaux

Research institute :

R400 - Institut de Recherche en Science et Ingénierie des Matériaux

Commentary :

Publié en ligne le 6 août 2005

Available on ORBi UMONS :

since 10 June 2010

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Bibliography

Roth, C. B.; Dutcher, J. R. Mobility on Different Length Scales in Thin Polymer Films. In Soft Materials: Stucture and Dynamics; Dutcher, J. R., Marangoni, A. G., Eds.; Marcel Dekker: 2004.
Macklin, J. J.; Trautman, J. K.; Harris, T. D.; Brus, L. E. Science 1996, 272, 255.
Xie, X. S.; Trautman, J. K. Amu. Rev. Phys. Chem. 1998, 49, 441.
Vanden Bout, D. A.; Yip, W.-T.; Hu, D. H.; Swager, T. M.; Barbara, P. F. Science 1997, 277, 1074.
Veerman, J. A.; Garcia Parajo, M. F.; Kuipers, L.; van Hulst, N. F. Phys. Rev. Lett. 1999, 83, 2155.
Boiron, A.-M.; Tamarat, Ph.; Lounis, B.; Orrit, M. Chem. Phys. 1999, 247, 119.
Deschesnes, L. A.; Vanden Bout, D. A. Science 2001, 292, 255.
Bowden, N. B.; Willets, K. A.; Moerner, W. E.; Waymouth, R. M. Macromolecules 2002, 35, 8122.
Vallée, R. A. L.; Tomczak, N.; Kuipers, L.; Vancso, G. J.; van Hulst, N. F. Phys. Rev. Lett. 2003, 91, 038301.
Bartko, A. P.; Dickson, R. M. J. Phys. Chem. B 1999, 103, 3053.
Vallée, R. A. L.; Collet, M.; Hofkens, J.; De Schryver, F. C.; Müllen, K. Macromolecules 2003, 36, 7752.
Vallée, R. A. L.; Collet, M.: Van der Auweraer, M.; Hofkens, J.; Müllen, K.; De Schryver, F. C. J. Am. Chem. Soc. 2004, 126, 2296.
Tomczak, N.; Vallée, R. A. L.; van Dijk, E. M. H. P.; Kuipers, L.; van Hulst, N. F.; Vancso, G. J. J. Am. Chem. Soc. 2004, 126, 4748.
Maus, M.; Collet, M.; Hofkens, J.; Gensch, T.; De Schryver, F. C.; Schaffer, J.; Seidel, C. A. M. Anal. Chem. 2001, 73, 2078.
Stracke, F.; Blum, C.; Becker, S.: Müllen, K.; Meixner, A. J. Chem. Phys. 2004, 300, 153.
Dewar, M. J. S.; Zoebisch, E. G.; Healy, E. F.; Stewart, J. J. P. J. Am. Chem. Soc. 1985, 107, 3902.
AMPAC, Semichem, 7204 Müllen, Shawnee, KS 66216.
Zerner, M. C.; Loew, G. H.; Kichner, R.; Mueller-Westerhoff, U. T. J. Am. Chem. Soc. 2000, 122, 3015.
Reimers, J. J. Chem. Phys. 2001, 115, 9103.
Valĺe R. A. L.; Van der Auweraer, M.; De Schryver, F. C.; Beljonne, D.; Orrit, M. ChemPhysChem 2005, 6, 81.
Sun, H. J. Phys. Chem. B 1998, 102, 7338.
Theodorou, D. N.; Suter, U. W. Macromolecules 1985, 18, 1467.
Mishra, A.; Behera, R. K.; Behera, P. K.; Mishra, B. K.; Behera, G. P. Chem. Rev. 2000, 100, 1973 and references therein.
Vranken, N.; Jordens, S.; De Beider, G.; Lor, M.; Rousseau, E.; Schweitzer, G.: Toppet, S.; Van der Auweraer, M.; De Schryver, F. C. J. Phys. Chem. A 2001, 105, 10196.
To draw the boxes shown in Figure 3c, we have proceeded in the following way. We first centred each of them on the lifetime axis exactly at the positions of the first and second peaks in the lifetime distribution (projections from Figure 3a to 3c). The width of the box in lifetime is determined by continuity of the density of points around the center. We proceeded in the same way on the line width axis. For the right upper box, we had to find a compromise between centering the box at the position of the second peak in the line width distribution (projection from Figure 3b to 3c) and the argument of continuity of the density of points within the box. As the two peaks are not so nicely resolved in this case, compared to the lifetime distribution, we decided to favor the continuity argument, which explains why the center of the right upper box is lower than the projection of the second peak in line width.
Vallée R. A. L.; Tomczak, N.; Kuipers, L.; Vancso, G. J.; van Hulst, N. F. J. Chem. Phys. 2005, 122, 114704.
Böttcher, C. J. F. Theory of electric polarization, 2nd ed.; Elsevier: Amsterdam, 1973; Vol. 1.
The depth of the "dip" between both maxima at 5% holes and 8% holes exceeds the standard deviation on the occurrence. The latter equals (assuming a Poisson distribution) the square root of the occurrence. This amounts to 4.4 and 3.2 for 5% and 89% holes, respectively. On the other hand, the probability for the minimum occurrence at 6% holes to be 0 at an expectation value of 3 events or more is less than 0.05. Hence one can safely assume the distribution to be bimodal.