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The saga of the primary photoexcitations in $\pi$-conjugated polymers hasbeen a source of extraordinary scientific curiosity that has lasted for morethan three decades. From soliton excitations in trans-polyacetylene, to singletand triplet excitons and polarons in other polymers, to charge transferexcitons in blends of polymers and fullerenes, the field has been rich with avariety of different photoexcitation species. Here we show the photogenerationof a novel primary intrachain photoexcitation species, namely the compositemulti-exciton (CME) in $\pi$-conjugated donor-acceptor (DA)-copolymers used inorganic photovoltaic (OPV) solar cells. We utilized the magnetic field responseof the transient photoinduced absorption from sub-picosecond to millisecond toshow in pristine DA-copolymer early photogeneration of the CME species that iscomposed of four coupled spin 1/2 particles, having unique optical and magneticsignatures. This species decomposes into two independent triplets in themicrosecond time domain. Importantly in copolymer/fullerene blends the CMEionization generates photocarriers by a unique process that may enhance thephotocurrent in OPV solar cells.

Novel primary photoexcitations in $\pi$-conjugated donor-acceptor copolymers probed by transient magneto-photoinduced-absorption