skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: A Mixed‐Pure Planar Heterojunction Structure of Active Layers for Efficient Sequential Blade‐Coating Organic Solar Cells
Abstract Precise modulating the vertical structure of active layers to boost charge transfer is an effective way to achieve high power conversion efficiencies (PCEs) in organic solar cells (OSCs). Herein, efficient OSCs with a well‐controlled vertical structure are realized by a rapid film‐forming method combining low boiling point solvent and the sequential blade‐coating (SBC) technology. The results of grazing incident wide‐angle X‐ray scattering measurement show that the vertical component distribution is varied by changing the processing solvent. Novel characterization technique such as tilt resonant soft X‐ray scattering is used to test the vertical structure of the films, demonstrating the dichloromethane (DCM)‐processed film is truly planar heterojunction. The devices with chloroform (CF) processed upper layer show an increased mixed phase region compared to these devices with toluene (TL) or ‐DCM‐, which is beneficial for improving charge generation and achieving a superior PCE of 17.36%. Despite significant morphological varies, the DCM‐processed devices perform slightly lower PCE of 16.66%, which is the highest value in truly planar heterojunction devices, demonstrating higher morphological tolerance. This work proposes a solvent‐regulating method to optimize the vertical structure of active layers through SBC technology, and provides a practical guidance for the optimization of the active‐layer microstructure.  more » « less
Award ID(s):
2247711
PAR ID:
10638354
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
Wiley
Date Published:
Journal Name:
Small
Volume:
21
Issue:
2
ISSN:
1613-6810
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Organic solar cells (OSCs) using non-fullerene acceptors (NFAs) afford exceptional photovoltaic performance metrics, however, their stability remains a significant challenge. Existing OSC stability studies focus on understanding degradation rate-performance relationships, improving interfacial layers, and suppressing degradative chemical reaction pathways. Nevertheless, there is a knowledge gap concerning how such degradation affects crystal structure, electronic states, and recombination dynamics that ultimately impact NFA performance. Here we seek a quantitative relationship between OSC metrics and blend morphology, trap density of states, charge carrier mobility, and recombination processes during the UV-light-induced degradation of PBDB-TF:Y6 inverted solar cells as the PCE (power conversion efficiency) falls from 17.3 to 5.0%. Temperature-dependent electrical and impedance measurements reveal deep traps at 0.48 eV below the conduction band that are unaffected by Y6 degradation, and shallow traps at 0.15 eV below the conduction band that undergo a three-fold density of states increase at the PCE degradation onset. Computational analysis correlates vinyl oxidation with a new trap state at 0.25 eV below the conduction band, likely involving charge transfer from the UV-absorbing ZnO electron transport layer. In-situ integrated photocurrent analysis and transient absorption spectroscopy reveal that these traps lower electron mobility and increase recombination rates during degradation. Grazing-incidence wide-angle x-ray scattering and computational analysis reveal that the degraded Y6 crystallite morphology is largely preserved but that <1% of degraded Y6 molecules cause OSC PCE performance degradation by ≈50%. Together the detailed electrical, impedance, morphological, ultrafast spectroscopic, matrix-assisted laser desorption/ionization time-of-flight (MALDI-ToF) spectroscopy, and computational data reveal that the trap state energies and densities accompanying Y6 vinyl oxidation are primarily responsible for the PCE degradation in these operating NFA-OSCs. 
    more » « less
  2. Group V doping in CdSeTe device can improve power conversion efficiency (PCE) and device stability. Arsenic (As) incorporation into CdSeTe has been demonstrated via both in situ and ex situ techniques; however, optimizing the back contact for group V‐doped CdSeTe devices remains a critical challenge. Here, solution‐processed arsenic chalcogenides (i.e., As2Te3and As2Se3) as dual‐role materials, serving as both dopants and back‐contact materials for high‐efficiency CdSeTe devices, are investigated. During the formation of the back contact, a portion of the arsenic chalcogenides diffuses into the CdSeTe absorber, facilitating p‐type doping. The remaining materials forms a stable back‐contact layer that facilitate carrier collection and reducing recombination losses at the CdSeTe back surface. Particularly, CdSeTe device employing Te rich As2Te3layer as the dopant and back‐contact materials achieves a PCE of 18.34%, demonstrating the dual functionality of solution‐processed arsenic chalcogenides in simultaneously doping the absorber and optimizing charge extraction. This solution based cost‐effective As doping approach offers a promising pathway for advancing CdSeTe photovoltaic technology. 
    more » « less
  3. The field-effect electron mobility of aqueous solution-processed indium gallium oxide (IGO) thin-film transistors (TFTs) is significantly enhanced by polyvinyl alcohol (PVA) addition to the precursor solution, a >70-fold increase to 7.9 cm 2 /Vs. To understand the origin of this remarkable phenomenon, microstructure, electronic structure, and charge transport of IGO:PVA film are investigated by a battery of experimental and theoretical techniques, including In K-edge and Ga K-edge extended X-ray absorption fine structure (EXAFS); resonant soft X-ray scattering (R-SoXS); ultraviolet photoelectron spectroscopy (UPS); Fourier transform-infrared (FT-IR) spectroscopy; time-of-flight secondary-ion mass spectrometry (ToF-SIMS); composition-/processing-dependent TFT properties; high-resolution solid-state 1 H, 71 Ga, and 115 In NMR spectroscopy; and discrete Fourier transform (DFT) analysis with ab initio molecular dynamics (MD) liquid-quench simulations. The 71 Ga{ 1 H} rotational-echo double-resonance (REDOR) NMR and other data indicate that PVA achieves optimal H doping with a Ga···H distance of ∼3.4 Å and conversion from six- to four-coordinate Ga, which together suppress deep trap defect localization. This reduces metal-oxide polyhedral distortion, thereby increasing the electron mobility. Hydroxyl polymer doping thus offers a pathway for efficient H doping in green solvent-processed metal oxide films and the promise of high-performance, ultra-stable metal oxide semiconductor electronics with simple binary compositions. 
    more » « less
  4. X-ray reflectivity was used to study the several-nanometer-thick “crowded” layers that form at the interfaces between a planar electrode and concentrated solutions of ionic liquids. The ionic liquid [P14,6,6,6]+[NTf2]− was dissolved in either strongly polar propylene carbonate or weakly polar dimethyl carbonate. In the range of 19–100 vol % ionic liquid, between working electrode potentials +2 and +2.75 V, uniform 2–7 nm thick interfacial layers were observed. These layers are not pure anions but contain three to five times as many anions as cations and about the same percentage of solvent as the bulk solution. On the other side of the layer, the density is that of the bulk solution. These features are inconsistent with a picture of the crowded layer as a region of pure, close-packed counterions. Not only the layer thickness but also the charge density decrease with increasing dilution at any given applied voltage. This appears to indicate, counterintuitively, that a thinner layer with lower net charge density will screen an electric field as effectively as a thicker layer with higher charge density. 
    more » « less
  5. Predicting the mechanical properties of organic semiconductors is important when using these materials in flexible electronics applications. For instance, knowledge of the mechanical and thermal stability of thin film organic solar cells (OSCs) is critical for the roll-to-roll production of photovoltaic devices and their use under various operating conditions. Here, we examine the thermal and elasto-mechanical properties of the conjugated donor polymer poly-(3-hexylthiophene) (P3HT) and the interpenetrating mixtures of P3HT and phenyl- C 61 -butyric acid methyl (PCBM) ester bulk heterojunction (BHJ) active layers under the application of unidirectional tensile deformation using coarse-grained molecular dynamics (CGMD) simulations. The predictions are validated against previous experimental reports as well as with earlier modeling results derived using different intermolecular force fields. Our results reveal that PCBM molecules behave as anti-plasticizers when mixed with P3HT and tend to increase the tensile modulus and glass transition temperature, while decreasing the crack-onset strain relative to pure P3HT. The variations in the mechanical properties with the composition of the BHJ active layer suggest that, in the presence of small oligomers as additives in the BHJ, the P3HT:PCBM mixture resists the anti-plasticizing effect of PCBM molecules due to the low tensile modulus of the short polymer chains. 
    more » « less