The application of liquid‐exfoliated 2D transition metal disulfides (TMDs) as the hole transport layers (HTLs) in nonfullerene‐based organic solar cells is reported. It is shown that solution ...processing of few‐layer WS2 or MoS2 suspensions directly onto transparent indium tin oxide (ITO) electrodes changes their work function without the need for any further treatment. HTLs comprising WS2 are found to exhibit higher uniformity on ITO than those of MoS2 and consistently yield solar cells with superior power conversion efficiency (PCE), improved fill factor (FF), enhanced short‐circuit current (JSC), and lower series resistance than devices based on poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) and MoS2. Cells based on the ternary bulk‐heterojunction PBDB‐T‐2F:Y6:PC71BM with WS2 as the HTL exhibit the highest PCE of 17%, with an FF of 78%, open‐circuit voltage of 0.84 V, and a JSC of 26 mA cm−2. Analysis of the cells' optical and carrier recombination characteristics indicates that the enhanced performance is most likely attributed to a combination of favorable photonic structure and reduced bimolecular recombination losses in WS2‐based cells. The achieved PCE is the highest reported to date for organic solar cells comprised of 2D charge transport interlayers and highlights the potential of TMDs as inexpensive HTLs for high‐efficiency organic photovoltaics.
The use of liquid exfoliated 2D WS2 and MoS2 as hole‐transporting layers (HTLs) in ultrahigh efficiency organic solar cells is reported. WS2 yields cells with higher power conversion efficiency (PCE), fill‐factor, and short‐circuit current than MoS2 and poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate). When WS2 is introduced as HTL in PBDB‐T‐2F:Y6:PC71BM organic solar cells, a maximum PCE value of 17% is achieved.
The performance of organic photovoltaic (OPV) material systems are hypothesized to depend strongly on the intermolecular arrangements at the donor:fullerene interfaces. A review of some of the most ...efficient polymers utilized in polymer:fullerene PV devices, combined with an analysis of reported polymer donor materials wherein the same conjugated backbone was used with varying alkyl substituents, supports this hypothesis. Specifically, the literature shows that higher-performing donor–acceptor type polymers generally have acceptor moieties that are sterically accessible for interactions with the fullerene derivative, whereas the corresponding donor moieties tend to have branched alkyl substituents that sterically hinder interactions with the fullerene. To further explore the idea that the most beneficial polymer:fullerene arrangement involves the fullerene docking with the acceptor moiety, a family of benzo1,2-b:4,5-b′dithiophene–thieno3,4-cpyrrole-4,6-dione polymers (PBDTTPD derivatives) was synthesized and tested in a variety of PV device types with vastly different aggregation states of the polymer. In agreement with our hypothesis, the PBDTTPD derivative with a more sterically accessible acceptor moiety and a more sterically hindered donor moiety shows the highest performance in bulk-heterojunction, bilayer, and low-polymer concentration PV devices where fullerene derivatives serve as the electron-accepting materials. Furthermore, external quantum efficiency measurements of the charge-transfer state and solid-state two-dimensional (2D) 13C{1H} heteronuclear correlation (HETCOR) NMR analyses support that a specific polymer:fullerene arrangement is present for the highest performing PBDTTPD derivative, in which the fullerene is in closer proximity to the acceptor moiety of the polymer. This work demonstrates that the polymer:fullerene arrangement and resulting intermolecular interactions may be key factors in determining the performance of OPV material systems.
Self‐assembled monolayers (SAMs) based on Br‐2PACz (2‐(3,6‐dibromo‐9H‐carbazol‐9‐yl)ethylphosphonic acid) 2PACz (2‐(9H‐Carbazol‐9‐yl)ethylphosphonic acid) and MeO‐2PACz ...(2‐(3,6‐dimethoxy‐9H‐carbazol‐9‐yl)ethylphosphonic acid) molecules were investigated as hole‐extracting interlayers in organic photovoltaics (OPVs). The highest occupied molecular orbital (HOMO) energies of these SAMs were measured at −6.01 and −5.30 eV for Br‐2PACz and MeO‐2PACz, respectively, and found to induce significant changes in the work function (WF) of indium‐tin‐oxide (ITO) electrodes upon chemical functionalization. OPV cells based on PM6 (poly(2,6‐(4,8‐bis(5‐(2‐ethylhexyl‐3‐fluoro)thiophen‐2‐yl)‐benzo1,2‐b:4,5‐b’dithiophene))‐alt‐(5,5‐(1’,3’‐di‐2‐thienyl‐5’,7’‐bis(2‐ethylhexyl)benzo1’,2’‐c:4’,5’‐c’dithiophene‐4,8‐dione)) : BTP‐eC9 : PC71BM (6,6‐phenyl‐C71‐butyric acid methyl ester) using ITO/Br‐2PACz anodes exhibited a maximum power conversion efficiency (PCE) of 18.4 %, outperforming devices with ITO/MeO‐2PACz (14.5 %) and ITO/poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT : PSS) (17.5 %). The higher PCE was found to originate from the much higher WF of ITO/Br‐2PACz (−5.81 eV) compared to ITO/MeO‐2PACz (4.58 eV) and ITO/PEDOT : PSS (4.9 eV), resulting in lower interface resistance, improved hole transport/extraction, lower trap‐assisted recombination, and longer carrier lifetimes. Importantly, the ITO/Br‐2PACz electrode was chemically stable, and after removal of the SAM it could be recycled and reused to construct fresh OPVs with equally impressive performance.
Super SAM: Two self‐assembled monolayers (SAMs; Br‐2PACz and MeO‐2PACz) are investigated as hole‐extracting interlayer in organic photovoltaics and compared against the widely used PEDOT : PSS. Cells based on the ternary bulk‐heterojunction blend PM6 : BTP‐eC9 : PC71BM and ITO/Br‐2PACz as the anode exhibit the highest power conversion efficiency of 18.4 %, outperforming devices with ITO/MeO‐2PACz (14.5 %) and even ITO/PEDOT : PSS (17.5 %).
Benzo1,2‐b:4,5‐b'difuran–thieno3,4‐cpyrrole‐4,6‐dione (PBDFTPD) polymers prepared by microwave‐assisted synthesis can achieve power conversion efficiencies (PCEs) >7% in bulk‐heterojunction solar ...cells with phenyl‐C61/71‐butyric acid methyl ester (PCBM). In “as‐cast” PBDFTPD‐based devices solution‐processed without a small‐molecule additive, high PCEs can be obtained in spite of the weak propensity of the polymers to self‐assemble and form π‐aggregates in thin films.
Metalenses are one of the most promising metasurface applications. However, all-dielectric reflective metalenses are rarely studied, especially regarding their off-axis focusing performance. After ...experimentally studying the material optical properties in this work, we propose reflective metalens based on titanium dioxide (TiO
2
) and silicon dioxide (SiO
2
), which operate at a visible wavelength of 0.633 µm. Unlike conventional reflective metalenses based on metallic mirrors, the proposed device was designed based on a modified parabolic phase profile and was integrated onto a dielectric distributed Bragg reflector periodic structure to achieve high reflectivity with five dielectric pairs. The focusing efficiency characteristics of the metalens were experimentally studied for beam angles of incidence between
0
∘
and
30
∘
. The results reveal that the focusing efficiency for the modified metalens design remains higher than 54%, which is higher than 50%, making it promising for photonic miniaturization and integration.
Chemical bath deposition (CBD) of tin oxide (SnO2) thin films as an electron-transport layer (ETL) in a planar-heterojunction n–i–p organohalide lead perovskite and organic bulk-heterojunction (BHJ) ...solar cells is reported. The amorphous SnO2 (a-SnO2) films are grown from a nontoxic aqueous bath of tin chloride at a very low temperature (55 °C) and do not require postannealing treatment to work very effectively as an ETL in a planar-heterojunction n–i–p organohalide lead perovskite or organic BHJ solar cells, in lieu of the commonly used ETL materials titanium oxide (TiO2) and zinc oxide (ZnO), respectively. Ultraviolet photoelectron spectroscopy measurements on the glass/indium–tin oxide (ITO)/SnO2/methylammonium lead iodide (MAPbI3)/2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenylamine)-9,9′-spirobifluorene device stack indicate that extraction of photogenerated electrons is facilitated by a perfect alignment of the conduction bands at the SnO2/MAPbI3 interface, while the deep valence band of SnO2 ensures strong hole-blocking properties. Despite exhibiting very low electron mobility, the excellent interfacial energetics combined with high transparency (E gap,optical > 4 eV) and uniform substrate coverage make the a-SnO2 ETL prepared by CBD an excellent candidate for the potentially low-cost and large-scale fabrication of organohalide lead perovskite and organic photovoltaics.
Among π-conjugated polymer donors for efficient bulk-heterojunction (BHJ) solar cell applications, poly(benzo1,2-b:4,5-b′dithiophene–thieno3,4-cpyrrole-4,6-dione) (PBDTTPD) polymers yield some of the ...highest open-circuit voltages (VOC, ca. 0.9 V) and fill-factors (FF, ca. 70%) in conventional (single-cell) BHJ devices with PCBM acceptors. In PBDTTPD, side chains of varying size and branching affect polymer self-assembly, nanostructural order, and impact material performance. However, the role of the polymer side-chain pattern in the intimate mixing between polymer donors and PCBM acceptors, and on the development of the BHJ morphology is in general less understood. In this contribution, we show that ring substituents such as furan (F), thiophene (T) and selenophene (S)incorporated into the side chains of PBDTTPD polymerscan induce significant and, of importance, very different morphological effects in BHJs with PCBM. A combination of experimental and theoretical (via density functional theory) characterizations sheds light on how varying the heteroatom of the ring substituents impacts (i) the preferred side-chain configurations and (ii) the ionization, electronic, and optical properties of the PBDTTPD polymers. In parallel, we find that the PBDT(X)TPD analogs (with X = F, T, or S) span a broad range of power conversion efficiencies (PCEs, 3–6.5%) in optimized devices with improved thin-film morphologies via the use of 1,8-diiodooctane (DIO), and discuss that persistent morphological impediments at the nanoscale can be at the origin of the spread in PCE across optimized PBDT(X)TPD-based devices. With their high V OC ∼1 V, PBDT(X)TPD polymers are promising candidates for use in the high-band gap cell of tandem solar cells.