Microscopic Structures, Dynamics, and Spin Configuration of the Charge Carriers in Organic Photovoltaic Solar Cells Studied by Advanced Time-Resolved Spectroscopic Methods.

Organic photovoltaics (OPVs) are promising solutions for renewable energy and sustainable technologies and have attracted much attention in recent years. Two types of organic semiconductors are used as donor materials to fabricate OPV cells. One type is a photoconductive polymer, and the other type is a small-molecule-based compound. The discovery of a bulk-heterojunction (BHJ) structure using a mixture of p- and n-type organic semiconductors has dramatically increased the power conversion efficiency (PCE) of OPV cells. In this feature article, we review our recent studies on organic BHJ thin films and OPVs by using advanced time-resolved spectroscopic techniques. Two topics regarding the microscopic behaviors of the charge carriers are discussed. The first topic is focused on how to quantify the local mobility of the charge carriers. Here, we discuss charge carrier dynamics in diketopyrrolopyrrole-linked tetrabenzoporphyrin (DPP-BP) BHJ thin films studied by time-resolved terahertz spectroscopy on a subpicosecond to several tens of picoseconds time scale and by transient photocurrent measurements on a microsecond time scale. The second topic concerns the spin configuration and interaction of the electron and hole of the polaron pairs in polymer-based BHJ thin films and OPV cells studied by the time-resolved electron paramagnetic resonance method, time-resolved simultaneous optical and electrical detection, and measurement of the magnetoconductance effect.