TY - JOUR
T1 - Photophysics of J-Aggregate-Mediated Energy Transfer on DNA
AU - Banal, James L.
AU - Kondo, Toru
AU - Veneziano, Rémi
AU - Bathe, Mark
AU - Schlau-Cohen, Gabriela S.
N1 - Funding Information:
This work was supported in part by the Center for Excitonics, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences under Award Number DE-SC0001088 (MIT), which provided funding to J.L.B., T.K., M.B., and G.S.S.-C. R.V. and M.B. also acknowledge support from the Army Research Office MURI Award No. W911NF1210420. The Biophysical Instrumentation Facility for the Study of Complex Macromolecular Systems (NSF-0070319) is gratefully acknowledged. We thank T. Sinclair and Dr. J. Caram for assistance with the low-temperature absorbance measurements.
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/12/7
Y1 - 2017/12/7
N2 - Achieving nanoscale spatial and electronic control over the formation of dye aggregates is a major synthetic challenge due to their typically inhomogeneous self-assembly, which limits control over their higher-order organization. To address these challenges, synthetic DNA-templated pseudoisocyanine (PIC) J-aggregates were recently introduced. However, the dependence of the photophysics of the superradiant exciton on the underlying DNA template length and the impact of static disorder on energy transfer through these PIC J-aggregates remain unknown. We examine the delocalization length progression of superradiant PIC excitons by varying the length of poly-A DNA tracts that template PIC J-aggregates. We then investigate the energy-transfer efficiency from PIC J-aggregates with DNA duplex template length, which we found to be limited by static disorder. Utilizing the self-assembled and selective formation of superradiant excitons on DNA provides a platform to determine the function of delocalized excitons in the context of nanoscale energy transport.
AB - Achieving nanoscale spatial and electronic control over the formation of dye aggregates is a major synthetic challenge due to their typically inhomogeneous self-assembly, which limits control over their higher-order organization. To address these challenges, synthetic DNA-templated pseudoisocyanine (PIC) J-aggregates were recently introduced. However, the dependence of the photophysics of the superradiant exciton on the underlying DNA template length and the impact of static disorder on energy transfer through these PIC J-aggregates remain unknown. We examine the delocalization length progression of superradiant PIC excitons by varying the length of poly-A DNA tracts that template PIC J-aggregates. We then investigate the energy-transfer efficiency from PIC J-aggregates with DNA duplex template length, which we found to be limited by static disorder. Utilizing the self-assembled and selective formation of superradiant excitons on DNA provides a platform to determine the function of delocalized excitons in the context of nanoscale energy transport.
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U2 - 10.1021/acs.jpclett.7b01898
DO - 10.1021/acs.jpclett.7b01898
M3 - Article
C2 - 29144136
AN - SCOPUS:85037707876
VL - 8
SP - 5827
EP - 5833
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 23
ER -