%0 Journal Article %1 Clifford2007 %A Clifford, John N. %A Bell, Toby D. M. %A Tinnefeld, Philip %A Heilemann, Mike %A Melnikov, Sergey M. %A ichi Hotta, Jun %A Sliwa, Michel %A Dedecker, Peter %A Sauer, Markus %A Hofkens, Johan %A Yeow, Edwin K. L. %C 1155 16TH ST, NW, WASHINGTON, DC 20036 USA %D 2007 %I AMER CHEMICAL SOC %J JOURNAL OF PHYSICAL CHEMISTRY B %K mike sauer %N 25 %P 6987-6991 %R 10.1021/jp072864d %T Fluorescence of single molecules in polymer films: Sensitivity of blinking to local environment %U http://dx.doi.org/10.1021/jp072864d %V 111 %X The single-molecule fluorescence blinking behavior of the organic dye Atto647N in various polymer matrixes such as Zeonex, PVK, and PVA as well as aqueous media was investigated. Fluorescence blinking with off-times in the millisecond to second time range is assigned to dye radical ions formed by photoinduced electron transfer reactions from or to the environment. In Zeonex and PVK, the measured off-time distributions show power law dependence, whereas, in PVA, no such dependence is observed. Rather, in this polymer, off-time distributions can be best fitted to monoexponential or stretched exponential functions. Furthermore, treatment of PVA samples to mild heating and low pressure greatly reduces the frequency of blinking events. We tentatively ascribe this to the removal of water pockets within the polymer film itself. Measurements of the dye immobilized in water in the presence of methylviologen, a strongly oxidizing agent, reveal simple exponential on- and off-time distributions. Thus, our data suggest that the blinking behavior of single organic molecules is sensitive to their immediate environment and, moreover, that fluorescence blinking on- and off-time distributions do not inherently and uniquely obey a power law.

@article{Clifford2007, abstract = {The single-molecule fluorescence blinking behavior of the organic dye Atto647N in various polymer matrixes such as Zeonex, PVK, and PVA as well as aqueous media was investigated. Fluorescence blinking with off-times in the millisecond to second time range is assigned to dye radical ions formed by photoinduced electron transfer reactions from or to the environment. In Zeonex and PVK, the measured off-time distributions show power law dependence, whereas, in PVA, no such dependence is observed. Rather, in this polymer, off-time distributions can be best fitted to monoexponential or stretched exponential functions. Furthermore, treatment of PVA samples to mild heating and low pressure greatly reduces the frequency of blinking events. We tentatively ascribe this to the removal of water pockets within the polymer film itself. Measurements of the dye immobilized in water in the presence of methylviologen, a strongly oxidizing agent, reveal simple exponential on- and off-time distributions. Thus, our data suggest that the blinking behavior of single organic molecules is sensitive to their immediate environment and, moreover, that fluorescence blinking on- and off-time distributions do not inherently and uniquely obey a power law.}, added-at = {2011-03-01T10:57:13.000+0100}, address = {1155 16TH ST, NW, WASHINGTON, DC 20036 USA}, affiliation = {Hofkens, J (Reprint Author), Katholieke Univ Leuven, Dept Chem, Celestijnenlaan 200F, B-3001 Heverlee, Belgium. Katholieke Univ Leuven, Dept Chem, B-3001 Heverlee, Belgium. Univ Melbourne, Sch Chem, Parkville, Vic 3010, Australia. Univ Bielefeld, D-33501 Bielefeld, Germany. Univ Oxford, Dept Phys, Clarendon Lab, Oxford OX1 3PU, England. Nanyang Technol Univ, Div Chem \& Biol Chem, Singapore 637616, Singapore.}, author = {Clifford, John N. and Bell, Toby D. M. and Tinnefeld, Philip and Heilemann, Mike and Melnikov, Sergey M. and ichi Hotta, Jun and Sliwa, Michel and Dedecker, Peter and Sauer, Markus and Hofkens, Johan and Yeow, Edwin K. L.}, author-email = {johan.hofkens@chem.kuleuven.be edwinyeow@ntu.edu.sg}, biburl = {https://www.bibsonomy.org/bibtex/2daa31a3c2ad9be3d1e5b7c1a03f8276c/reichert}, cited-references = {AMBROSE WP, 1994, PHYS REV LETT, V72, P160. BELL TDM, 2005, CHEMPHYSCHEM, V6, P942, DOI 10.1002/cphc.200400567. HAASE M, 2004, J PHYS CHEM B, V108, P10445, DOI 10.1021/jp0313674. HEILEMANN M, 2005, J AM CHEM SOC, V127, P3801, DOI 10.1021/ja044686x. HOOGENBOOM JP, 2005, PHYS REV LETT, V95, ARTN 097401. HOOGENBOOM JP, 2006, J CHEM PHYS, V125, ARTN 204713. HOOGENBOOM JP, 2007, CHEMPHYSCHEM, V8, P823, DOI 10.1002/cphc.200600783. HUNG LS, 2002, MAT SCI ENG R, V39, P143. KOHN F, 2002, J PHYS CHEM A, V106, P4808. KOROBOV VE, 1978, J PHOTOCHEM, V9, P411. KULZER F, 2004, ANNU REV PHYS CHEM, V55, P585, DOI 10.1146/annurev.physchem.54.011002.103816. KUNO M, 2003, PHYS REV B, V67, ARTN 125304. LU HP, 1997, NATURE, V385, P143. MARCUS RA, 1956, J CHEM PHYS, V24, P966. MICHALET X, 2006, CHEM REV, V106, P1785, DOI 10.1021/cr0404343. MOERNER WE, 1999, SCIENCE, V283, P1670. ROEFFAERS MBJ, 2006, NATURE, V439, P572, DOI 10.1038/nature04502. SCHUSTER J, 2005, APPL PHYS LETT, V87, ARTN 051915. SCHUSTER J, 2005, OPT SPECTROSC+, V98, P712. SHIMIZU KT, 2001, PHYS REV B, V63, ARTN 205316. TACHIYA M, 1975, CHEM PHYS LETT, V34, P77. TANG J, 2005, PHYS REV LETT, V95, ARTN 107401. TINNEFELD P, 2005, ANGEW CHEM INT EDIT, V44, P2642, DOI 10.1002/anie.200300647. VERBERK R, 2002, PHYS REV B, V66, ARTN 233202. WESTON KD, 1998, J CHEM PHYS, V109, P7474. WESTON KD, 1998, J PHYS CHEM A, V102, P3635. YEOW EKL, 2006, J PHYS CHEM A, V110, P1726, DOI 10.1021/jp055496r. YIP WT, 1998, J PHYS CHEM A, V102, P7564. ZONDERVAN R, 2003, J PHYS CHEM A, V107, P6770, DOI 10.1021/jp034723r.}, doc-delivery-number = {181KN}, doi = {10.1021/jp072864d}, groups = {public}, interhash = {4580a8b213331017eaedfda08e65d7df}, intrahash = {daa31a3c2ad9be3d1e5b7c1a03f8276c}, issn = {1520-6106}, journal = {JOURNAL OF PHYSICAL CHEMISTRY B}, journal-iso = {J. Phys. Chem. B}, keywords = {mike sauer}, keywords-plus = {ROOM-TEMPERATURE; DYE MOLECULES; ELECTRON-TRANSFER; GLASS-SURFACE; INTERMITTENCY; KINETICS; PHOTOCHEMISTRY; SPECTROSCOPY; FLUCTUATIONS; DYNAMICS}, language = {English}, month = {JUN 28}, number = 25, number-of-cited-references = {29}, pages = {6987-6991}, publisher = {AMER CHEMICAL SOC}, subject-category = {Chemistry, Physical}, times-cited = {41}, timestamp = {2011-03-10T13:35:03.000+0100}, title = {Fluorescence of single molecules in polymer films: Sensitivity of blinking to local environment}, type = {Article}, unique-id = {ISI:000247435700005}, url = {http://dx.doi.org/10.1021/jp072864d}, username = {reichert}, volume = 111, year = 2007 }