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Title: Scaling Relations and Optimization of Excitonic Energy Transfer Rates between One-Dimensional Molecular Aggregates

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Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC); Center for Excitonics (CE)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
DOE Contract Number:
Resource Type:
Journal Article
Resource Relation:
Journal Name: J. Phys. Chem. B,; Journal Volume: accepted; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University
Country of Publication:
United States
solar (photovoltaic), solid state lighting, photosynthesis (natural and artificial), charge transport, optics, synthesis (novel materials), synthesis (self-assembly), synthesis (scalable processing)

Citation Formats

Chuang, Chern, Knoester, J., and Cao, Jianshu. Scaling Relations and Optimization of Excitonic Energy Transfer Rates between One-Dimensional Molecular Aggregates. United States: N. p., 2014. Web. doi:10.1021/jp4124502.
Chuang, Chern, Knoester, J., & Cao, Jianshu. Scaling Relations and Optimization of Excitonic Energy Transfer Rates between One-Dimensional Molecular Aggregates. United States. doi:10.1021/jp4124502.
Chuang, Chern, Knoester, J., and Cao, Jianshu. Thu . "Scaling Relations and Optimization of Excitonic Energy Transfer Rates between One-Dimensional Molecular Aggregates". United States. doi:10.1021/jp4124502.
title = {Scaling Relations and Optimization of Excitonic Energy Transfer Rates between One-Dimensional Molecular Aggregates},
author = {Chuang, Chern and Knoester, J. and Cao, Jianshu},
abstractNote = {},
doi = {10.1021/jp4124502},
journal = {J. Phys. Chem. B,},
number = ,
volume = accepted,
place = {United States},
year = {Thu Jul 17 00:00:00 EDT 2014},
month = {Thu Jul 17 00:00:00 EDT 2014}
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  • Recent studies have indicated that environmental noise may increase energy-transfer efficiency in quantum systems. For homogeneous networks of chromophores previous studies have primarily considered excitonic transport in one-dimensional (linear) networks. In our study, we expand previous research to a two-dimensional fully coupled topology of chromophore molecules. We demonstrate that not only does an optimal dephasing rate exist in both one- and two-dimensional networks but also that it increases in magnitude with increasing coupling strength between chromophores. Optimal transport occurs when the noise quenches the entanglement between local modes that prevent the exciton from moving efficiently to the target site. Wemore » find that these results are insensitive to minor site defects such as those found in realistic systems. We contrast these findings to systems with a high degree of inhomogeneity, in which the optimal dephasing rate is largely set by the system topology and does not vary significantly with respect to coupling strength. Our findings have potential applications to systems such as quantum dot arrays and carbon nanotube structures.« less
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  • The charge-transfer reaction of decamethylferrocene, Fe(C/sub 5/Me/sub 5/)/sub 2/, Fc*, and 7,7,8,8-tetracyano-p-quinodimethane, TCNQ, has been characterized. Three major reaction products of varying stoichiometry, conductivity, and magnetism are formed: a 1-D metamagnetic 1:1 salt, (Fc*)/sup +/(TCNQ)/sup -/; a paramagnetic (Fc*)/sup 2/ /sup +/(TCNQ)/sup 22 -/; 1:1; dimeric salt, (Fc*)/sup 2/ /sup +/(TCNQ)/sup 22 -/; and a conducting 1:2 salt of (Fc*) /sup +/(TCNQ)/sup 2 -/ composition. The crystal and molecular structures of the 1:1 paramagnetic dimeric and metamagnetic one-dimensional salts were solved. The ions in the dimeric phase crystallize in the centrosymmetric monoclinic space group P2/sub 1//c with a = 9.708more » (1) A, b = 12.211 (2) A, c = 23.585 (4) A, ..beta.. = 95.01 (1)/sup 0/, Z = 4, and R = 0.058 for 3665 independent reflections. The magnetic susceptibility of powder samples of (Fc*)/sup 2/ /sup +/(TCNQ/sub 2/)/sub 2//sup 2 -/ obeys the Curie expression above 1.5 K suggesting very little magnetic coupling between the intradimer S = 1/2 Fe(III)'s which are separated by approx.14 A. The (TCNQ)/sub 2//sup 2 -/ dimer is strongly antiferromagnetically coupled. Ions in the linear chain metamagnetic phase crystallize in the centrosymmetric triclinic space group P1 vector. The unit cell at -106 /sup 0/C is a = 8.635 (4) A, b = 9.384 (6) A, c = 10.635 (9) A; ..cap alpha.. = 116.76 (5)/sup 0/, ..beta.. = 112.58 (5)/sup 0/; ..gamma.. = 72.49 (4)/sup 0/, V = 701.8 A/sup 3/, Z = 1, and R/sub w/ = 0.060 for 1156 reflections. The one-dimensional phase exhibits metamagnetic properties with a Neel temperature of 2.55 K. The intrachain Fe/sup III/-Fe/sup III/separation is 10.540 A. The calculated structure and scaled vibrational frequencies are in excellent agreement with the observed values.« less