A highly NIR-absorptive organic dye forms monomers when kinetically trapped in a polymer matrix, but upon thermal annealing, aggregation causes changes in excited-state processes, which are assayed via in situ transient absorption.
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Walbrun, Zachary S. ; Leibfried, Laura C. ; Hoban, Áine R. ; Rasmussen, Brandon C. ; Wiegand, Tyler J. ; Collison, Christopher J. ; Wong, Cathy Y. ( , MRS Advances)This study aimed to investigate the effects of thermal annealing on a film of squaraine (SQ) molecules in a polymethyl methacrylate (PMMA) matrix. Molecular aggregation is inferred from in situ absorption measurements, and excited state dynamics are measured using a spatially encoded transient absorption (TA) spectroscopy. TA spectra were well-replicated using a kinetic model that evolves as a function of annealing time and extent of aggregation. While linear absorbance spectra indicate that the SQ molecules are primarily uncoupled or weakly-coupled when initially deposited in a PMMA matrix, the kinetic model shows that some pi-stacked aggregates are already present. Excitons are funnelled by energy transfer to these aggregates in just a few picoseconds. The amount of pi-stacked aggregates increases during thermal annealing, further increasing the population of excitons that end up in these aggregates.more » « less