Entropy-Driven Charge Separation: A Potential Explanation for the Low Energy Loss Found in OPVs with Non-fullerene Acceptors

Chan, Wai-Lun; Rijal, Kushal

doi:10.1021/acs.jpcc.3c06376

Entropy-Driven Charge Separation: A Potential Explanation for the Low Energy Loss Found in OPVs with Non-fullerene Acceptors

Journal Article · Wed Jan 03 00:00:00 EST 2024 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.3c06376· OSTI ID:2337770

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University of Kansas, Lawrence, KS (United States); University of Kansas
University of Kansas, Lawrence, KS (United States)

The recent development of non-fullerene acceptors (NFA) has led to an abrupt increase in the organic photovoltaic (OPV) efficiency from ~12% to ~20%. NFA OPVs can generate photocurrent efficiently without much energy loss, which contrasts with the large energy loss often needed for generating free charges from excitons in fullerene OPVs. Here, we argue that entropy-driven charge separation, which allows excitons to spontaneously gain heat from the environment, is responsible for the exceptionally low energy loss found in NFA OPVs. The entropic driving force is maximized when the delocalized electron and hole wave functions in the CT exciton intersect each other via pointlike junctions. Furthermore, these pointlike junctions are abundant in the polymer/NFA bulk heterojunction which consists of intertwined, stringlike donor and acceptor domains in which electron delocalizes anisotropically. Such microstructure favors entropy-driven charge separation, which can enable charge separation with a minimal energy loss.

View Accepted Manuscript (DOE)

Research Organization:: University of Kansas, Lawrence, KS (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0024525

OSTI ID:: 2337770

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 2 Vol. 128; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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