Triplet Exciton Generation in Bulk-Heterojunction Solar Cells based on Endohedral Fullerenes

TL;DR

This study investigates how the incorporation of endohedral fullerenes affects exciton dynamics and charge transport in bulk-heterojunction solar cells, revealing triplet exciton formation and its impact on photocurrent efficiency.

Contribution

It uncovers the role of triplet excitons and charge transfer processes in limiting current in fullerene-based solar cells with endohedral fullerenes.

Findings

Triplet excitons are formed on the polymer chain in Lu3N@C80-PCBEH blends.

Weaker photoluminescence quenching indicates reduced exciton dissociation.

Electron back transfer to triplet states reduces photocurrent.

Abstract

Organic bulk-heterojunctions (BHJ) and solar cells containing the trimetallic nitride endohedral fullerene 1-[3-(2-ethyl)hexoxy carbonyl]propyl-1-phenyl-Lu3N@C80 (Lu3N@C80-PCBEH) show an open circuit voltage (VOC) 0.3 V higher than similar devices with [6,6]-phenyl-C[61]-butyric acid methyl ester (PC61BM). To fully exploit the potential of this acceptor molecule with respect to the power conversion efficiency (PCE) of solar cells, the short circuit current (JSC) should be improved to become competitive with the state of the art solar cells. Here, we address factors influencing the JSC in blends containing the high voltage absorber Lu3N@C80-PCBEH in view of both photogeneration but also transport and extraction of charge carriers. We apply optical, charge carrier extraction, morphology, and spin-sensitive techniques. In blends containing Lu3N@C80-PCBEH, we found 2 times weaker photoluminescence quenching, remainders of interchain excitons, and, most remarkably, triplet excitons formed on the polymer chain, which were absent in the reference P3HT:PC61BM blends. We show that electron back transfer to the triplet state along with the lower exciton dissociation yield due to intramolecular charge transfer in Lu3N@C80-PCBEH are responsible for the reduced photocurrent.