Since magnetic fields can probe fractions of spin singlet
and triplet
at charge-transfer states (CTSs) for organic bulk heterojunction (BHJ)
solar cells, this makes the magneto-photocurrent (MPC) a powerful
and versatile method to unravel the photovoltaic spin-dynamics. The
method is of paramount importance for deeply understanding the spin-dependent
polaron pair (PP) dissociation at excited states. The foundation lies
primarily on the coherent spin mixing. Unfortunately, it remains challenging
and highly demanding to carry on with a comprehensive study for the
objective of precisely and manifestly interpreting the MPC effect.
Herein, a joint experimental and theoretical study is performed for
an in-depth exploration of MPC on prototypical nonfullerene acceptor
ITIC-based organic binary and ternary BHJ solar cells. We are devoted
particularly to MPC with distinct lineshapes, magnitudes, and signs.
With the assistance of analytical models, the singlet PP dissociation
at CTS and triplet exciton–polaron reaction are verified to
be dominant for the photocurrent generations. Our study suggests that
the MPC offers an effective means for revealing the photovoltaic spin-dynamic
process. It helps to quantify dissociation rates for spin polarons
at intermediate CTS of organic BHJ systems.