Effect of Hydrophilicity-Imparting Substituents on Exciton Delocalization in Squaraine Dye Aggregates Covalently Templated to DNA Holliday Junctions

Pascual, Gissela; Roy, Simon K.; Barcenas, German; Wilson, Christopher K.; Cervantes-Salguero, Keitel; Obukhova, Olena M.; Krivoshey, Alexander I.; Terpetschnig, Ewald; Tatarets, Anatoliy L.; Li, Lan; Yurke, Bernard; Knowlton, William; Mass, Olga A.; Pensack, Ryan D.; Lee, Jeunghoon

doi:10.1039/d3nr04499h

Effect of Hydrophilicity-Imparting Substituents on Exciton Delocalization in Squaraine Dye Aggregates Covalently Templated to DNA Holliday Junctions

Journal Article · Tue Dec 12 23:00:00 EST 2023 · Nanoscale

DOI:https://doi.org/10.1039/d3nr04499h· OSTI ID:2234233

Pascual, Gissela ^[1]; ^[2]; ^[2]; Wilson, Christopher K. ^[2]; Cervantes-Salguero, Keitel ^[2]; Obukhova, Olena M. ^[3]; Krivoshey, Alexander I. ^[3]; ^[4]; Tatarets, Anatoliy L. ^[3]; ^[5]; ^[2]; ^[2]; ^[2]; ^[2]; ^[2]

Boise State University, ID (United States); Boise State University
Boise State University, ID (United States)
State Scientific Institution “Institute for Single Crystals” of the National Academy of Sciences of Ukraine, Kharkiv (Ukraine)
SETA BioMedicals, LLC, Urbana, IL (United States)
Boise State University, ID (United States); Center for Advanced Energy Studies, Idaho Falls, ID (United States)

Molecular aggregates exhibit emergent properties, including the collective sharing of electronic excitation energy known as exciton delocalization, that can be leveraged in applications such as quantum computing, optical information processing, and light harvesting. In a previous study, we found unexpectedly large excitonic interactions (quantified by the excitonic hopping parameter J_m,n) in DNA-templated aggregates of squaraine (SQ) dyes with hydrophilic-imparting sulfo and butylsulfo substituents. Here, we characterize DNA Holliday junction (DNA-HJ) templated aggregates of an expanded set of SQs and evaluate their optical properties in the context of structural heterogeneity. Specifically, we characterized the orientation of and J_m,n between dyes in dimer aggregates of non-chlorinated and chlorinated SQs. Here, three new chlorinated SQs that feature a varying number of butylsulfo substituents were synthesized and attached to a DNA-HJ via a covalent linker to form adjacent and transverse dimers. Various characteristics of the dye, including its hydrophilicity (in terms of log P_o/w) and surface area, and of the substituents, including their local bulkiness and electron withdrawing capacity, were quantified computationally.

View Accepted Manuscript (DOE)

Research Organization:: Boise State University, ID (United States)

Sponsoring Organization:: USDOE Established Program to Stimulate Competitive Research (EPSCoR) program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: SC0020089

OSTI ID:: 2234233

Alternate ID(s):: OSTI ID: 2246680

Journal Information:: Nanoscale, Journal Name: Nanoscale Journal Issue: 3 Vol. 16; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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