Crystallography, Morphology, Electronic Structure, and Transport in Non-Fullerene/Non-Indacenodithienothiophene Polymer:Y6 Solar Cells

Zhu, Weigang; Spencer, Austin P.; Mukherjee, Subhrangsu; Alzola, Joaquin M.; Sangwan, Vinod K.; Amsterdam, Samuel H.; Swick, Steven M.; Jones, Leighton O.; Heiber, Michael C.; Herzing, Andrew A.; Li, Guoping; Stern, Charlotte L.; DeLongchamp, Dean M.; Kohlstedt, Kevin L.; Hersam, Mark C.; Schatz, George C.; Wasielewski, Michael R.; Chen, Lin X.; Facchetti, Antonio; Marks, Tobin J.

doi:10.1021/jacs.0c05560

Crystallography, Morphology, Electronic Structure, and Transport in Non-Fullerene/Non-Indacenodithienothiophene Polymer:Y6 Solar Cells

Journal Article · Wed Jul 22 00:00:00 EDT 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c05560· OSTI ID:1798342

^[1]; ^[2]; ^[3]; Alzola, Joaquin M. ^[2]; ^[2]; Amsterdam, Samuel H. ^[2]; Swick, Steven M. ^[2]; ^[2]; Heiber, Michael C. ^[4]; Herzing, Andrew A. ^[3]; ^[2]; Stern, Charlotte L. ^[2]; DeLongchamp, Dean M. ^[4]; ^[2]; ^[2]; ^[2]; ^[2]; ^[5]; ^[6]; ^[2]

Northwestern Univ., Evanston, IL (United States); Northwestern University
Northwestern Univ., Evanston, IL (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Northwestern Univ., Evanston, IL (United States); National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
Northwestern Univ., Evanston, IL (United States); Flexterra Corporation, Skokie, IL (United States)

Emerging non-fullerene acceptors (NFAs) with crystalline domains enable high-performance bulk heterojunc-tion (BHJ) solar cells. Thermal annealing is known to enhance BHJ photoactive layer morphology and performance. However, the microscopic mechanism of annealing-induced performance enhancement is poorly understood in emerging NFAs, espe-cially regarding competing factors. Here, optimized thermal annealing of the model system PBDB-TF:Y6 (Y6 = 2,2'-((2Z,2'Z)-((12,13-bis(2-ethylhexyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2",3’':4’,5']thieno[2',3':4,5]pyrrolo[3,2-g]thieno[2',3':4,5]-thieno[3,2-b]indole-2,10-diyl)bis(methanylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diyli-dene))dimalononitrile) decreases open circuit voltage (VOC) but increases the short circuit current (J_SC) and fill factor (FF) such that the resulting power conversion efficiency (PCE) increases from 14% to 15% in ambient. Here we systematically investi-gate these thermal annealing effects through in-depth characterizations of carrier mobility, film morphology, charge photo-generation and recombination, using SCLC, GIXRD, AFM, XPS, NEXAFS, R-SoXS, TEM, STEM, fs/ns TA spectroscopy, 2DES, and impedance spectroscopy. Surprisingly, thermal annealing does not alter film crystallinity, nor R-SoXS characteristic size scale, relative average phase purity, nor TEM-imaged phase separation, but rather facilitates Y6 migration to the BHJ film top surface, changes the PBDB-TF/Y6 vertical phase separation and intermixing, and reduces bottom surface roughness. While these morphology changes increase bimolecular recombination (BR) and lower the free charge (FC) yield, they also increase the average of electron and hole mobility by at least two-fold. Importantly, the increased μh dominates and underlies the increased FF and PCE. Single-crystal X-ray diffraction reveals that Y6 molecules co-facially pack via their end-groups/cores, with the shortest π-π distance as close as 3.34 Å, clarifying out-of-plane π-face-on molecular orientation in the nano-crystalline BHJ domains. DFT analysis of Y6 crystals reveals hole/electron reorganization energies as low as 160/150 meV, large intermo-lecular electronic coupling integrals of 12.1 - 37.9 meV, rationalizing the 3D electron transport and relatively high μe of 10^-4 cm² V^-1 s^-1. Altogether, this work clarifies the richness of thermal annealing effects in high-efficiency NFA solar cells and tasks for future materials design.

View Accepted Manuscript (DOE)

Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Office of Naval Research (ONR); AFOSR; NSF

Grant/Contract Number:: SC0001059; SC0012704; AC02-06CH11357; AC02-05CH11231

OSTI ID:: 1798342

Alternate ID(s):: OSTI ID: 1690198

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 34 Vol. 142; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Crystallography, Morphology, Electronic Structure, and Transport in Non-Fullerene/Non-Indacenodithienothiophene Polymer:Y6 Solar Cells

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