Quantifying Polaron Mole Fractions and Interpreting Spectral Changes in Molecularly Doped Conjugated Polymers

Moulé, Adam J.; Gonel, Goktug; Murrey, Tucker L.; Ghosh, Raja; Saska, Jan; Shevchenko, Nikolay E.; Denti, Ilaria; Fergerson, Alice S.; Talbot, Rachel M.; Yacoub, Nichole L.; Mascal, Mark; Salleo, Alberto; Spano, Frank C.

doi:10.1002/aelm.202100888

Title: Quantifying Polaron Mole Fractions and Interpreting Spectral Changes in Molecularly Doped Conjugated Polymers

Journal Article · 27 December 2021 · Advanced Electronic Materials

DOI: https://doi.org/10.1002/aelm.202100888 · OSTI ID:1976237

Moulé, Adam J. ^[1]; Gonel, Goktug ^[2];

^[2]; Ghosh, Raja ^[3]; Saska, Jan ^[2]; Shevchenko, Nikolay E. ^[2]; Denti, Ilaria ^[4];

^[2]; Talbot, Rachel M. ^[2]; Yacoub, Nichole L. ^[2];

^[2];

^[4];

^[3]

University of California, Davis, CA (United States); OSTI
University of California, Davis, CA (United States)
Temple University, Philadelphia, PA (United States)
Stanford University, CA (United States)

Molecular doping of conjugated polymers causes bleaching of the neutral absorbance and results in new polaron absorbance transitions in the mid and near infrared. In this report the concentration dependent changes in the spectra for a series of molecularly doped diketopyrrolopyrrole (DPP) co-polymers with a series of ultra-high electron affinity cyanotrimethylenecyclopropane-based dopants is analyzed. With these strong dopants the polaron mole fraction (Θ) reaches saturation. Analysis of the full spectrum enables separation of neutral and polaron signals and quantification of the polaron mole fraction using a simple noninteracting site model. The peak ratios for both neutral and polaron peaks change systematically with increasing polaron mole fraction for all measured polymers. Analysis of the spectral changes indicates that the polaron mole fraction can be quantified to within 5%. While the total change in the absorbance spectrum with increasing polaron mole fraction is linear, the lowest energy polaron peak (P1) grows nonlinearly, which indicates increased polarization/delocalization. Molecular doping of polymers that form either H- or J-aggregates shows systematically different spectral changes in the vibronic peak ratios of the neutral spectra and provides insights into the polymer configuration at undoped sites in the film.

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Research Organization:: University of Washington, Seattle, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Wasson Honors Program

Grant/Contract Number:: SC0020046

OSTI ID:: 1976237

Journal Information:: Advanced Electronic Materials, Journal Name: Advanced Electronic Materials Journal Issue: 4 Vol. 8; ISSN 2199-160X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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