Kang Chen

Rapid extraction of photogenerated charge carriers is essential to achieve high efficiencies with perovskite solar cells (PSCs). Here, a new mesoscopic architecture as electron-selective contact for PSCs featuring 40 nm sized TiO₂ beads endowed with mesopores of a few nanometer diameters is introduced. The bimodal pore distribution inherent to these films produces a very large contact area of 200 m² g⁻¹ whose access by the perovskite light absorber is facilitated by the interstitial voids between the particles. Modification of the TiO₂ surface by CsBr further strengthens its interaction with the perovskite. As a result, photogenerated electrons are extracted rapidly producing a very high fill factor of close to 80% a V_OC of 1.14 V and a PCE up to 21% with negligible hysteresis.

Cesium modification of bimodal mesoporous TiO₂ surface for perovskite solar cells enhances electron transfer and reduces recombination at the interface between perovskite and elective-selective layers. As a result, photogenerated electrons are extracted rapidly producing a very high fill factor of close to 80% a V_OC of 1.14 V and a power conversion efficiency of 21% with negligible hysteresis.

Achieving efficient bulk-heterojunction (BHJ) solar cells from blends of solution-processable small-molecule (SM) donors and acceptors is proved particularly challenging due to the complexity in obtaining a favorable donor–acceptor morphology. In this report, the BHJ device performance pattern of a set of analogous, well-defined SM donors—DR3TBDTT (DR3), SMPV1, and BTR—used in conjunction with the SM acceptor IDTTBM is examined. Examinations show that the nonfullerene “All-SM” BHJ solar cells made with DR3 and IDTTBM can achieve power conversion efficiencies (PCEs) of up to ≈4.5% (avg. 4.0%) when the solution-processing additive 1,8-diiodooctane (DIO, 0.8% v/v) is used in the blend solutions. The figures of merit of optimized DR3:IDTTBM solar cells contrast with those of “as-cast” BHJ devices from which only modest PCEs <1% can be achieved. Combining electron energy loss spectrum analyses in scanning transmission electron microscopy mode, carrier transport measurements via “metal-insulator-semiconductor carrier extraction” methods, and systematic recombination examinations by light-dependence and transient photocurrent analyses, it is shown that DIO plays a determining role—establishing a favorable lengthscale for the phase-separated SM donor–acceptor network and, in turn, improving the balance in hole/electron mobilities and the carrier collection efficiencies overall.

A set of structurally analogous small-molecule (SM) donors with distinct side-chain manifolds shows significant differences in their performance patterns in bulk-heterojunction (BHJ) devices with the nonfullerene SM acceptor IDTTBM. Reducing the lengthscale of the phase-separated network between donor and acceptor effectively suppresses nongeminate recombination in the BHJ active layers and improves the carrier mobility balance.

In this work, room-temperature-operated ultrasensitive solution-processed perovskite photodetectors (PDs) with near infrared (NIR) photoresponse are reported. In order to enable perovskite PDs possessing extended NIR photoresponse, novel n-type low bandgap conjugated polymer, poly[(N,N′-bis(2-octyldodecyl)-1,4,5,8-naphthalene diimide-2,6-diyl) (2,5-dioctyl-3,6-di(thiophen-2-yl)pyrrolo[3,4-c]pyrrole-1,4-dione-5,5′-diyl)] (NDI-DPP), which has strong absorption in the NIR region, is developed and then employed in perovskite PDs. By the formation of type II band alignment between NDI-DPP with single-wall carbon nanotubes (SWCNTs), the NIR absorption of NDI-DPP is exploited, which contributes to the NIR photoresponse for the perovskite PDs, where perovskite is incorporated with NDI-DPP and SWCNTs as well. In addition, SWCNTs incorporated with perovskite active layer can offer the percolation pathways for high charge-carrier mobility, which tremendously boosts the charge transfer in the photoactive layer, and consequently improves the photocurrent in the visible region. As a result, the perovskite PDs exhibit the responsivities of ≈400 and ≈150 mA W⁻¹ and the detectivities of over 6 × 10¹² Jones (1 Jones = 1 cm Hz^1/2 W⁻¹) and over 2 × 10¹² Jones in the visible and NIR regions, respectively. This work reports the development of perovskite PDs with NIR photoresponse, which is terrifically beneficial for the practical applications of perovskite PDs.

Room temperature operated uncooled broadband ultrasensitive photodetectors with the responsivities of 400 and 150 mA W^-1 and the detectivities of over 6 × 10¹² and 2 × 10¹² Jones in the visible and near infrared regions are realized by utilization of perovskite incorporated with novel n-type low-bandgap conjugated polymer and single-wall carbon nanotubes through type II band alignment.

Organometallic halide perovskite films with good surface morphology and large grain size are desirable for obtaining high-performance photovoltaic devices. However, defects and related trap sites are generated inevitably at grain boundaries and on surfaces of solution-processed polycrystalline perovskite films. Seeking facial and efficient methods to passivate the perovskite film for minimizing defect density is necessary for further improving the photovoltaic performance. Here, a convenient strategy is developed to improve perovskite crystallization by incorporating a 2D polymeric material of graphitic carbon nitride (g-C₃N₄) into the perovskite layer. The addition of g-C₃N₄ results in improved crystalline quality of perovskite film with large grain size by retarding the crystallization rate, and reduced intrinsic defect density by passivating charge recombination centers around the grain boundaries. In addition, g-C₃N₄ doping increases the film conductivity of perovskite layer, which is beneficial for charge transport in perovskite light-absorption layer. Consequently, a champion device with a maximum power conversion efficiency of 19.49% is approached owing to a remarkable improvement in fill factor from 0.65 to 0.74. This finding demonstrates a simple method to passivate the perovskite film by controlling the crystallization and reducing the defect density.

Graphitic carbon nitride (g-C₃N₄) is incorporated into the perovskite precursor solution to modify the perovskite film by controlling the perovskite crystallization, reducing the intrinsic defect density, and improving the film conductivity. As a result, a champion device with a maximum power conversion efficiency of 19.49% is approached.

The synthesis and characterization of oligophenylenevinylene (OPV)–azafullerene (C₅₉N) systems in the form of OPV–C₅₉N donor–acceptor dyad 1 and C₅₉N–OPV–C₅₉N acceptor–donor–acceptor triad 2 is accomplished. Photoinduced electronic interactions between OPV and C₅₉N within 1 and 2 are assessed by UV–vis and photoluminescence. The redox properties of 1 and 2 are investigated, revealing a set of one-electron oxidation and three one-electron reduction processes owed to OPV and C₅₉N, respectively. The electrochemical bandgap for 1 and 2 is calculated as 1.44 and 1.53 eV, respectively, and the free energy for the formation of the charge-separated state for 1 and 2 via the singlet-excited state of OPV is found negative, proving a thermodynamically favorable the process. Photoexcitation assays are performed in toluene and o-dichlorobenzene (oDCB) and the reactions are monitored with time-resolved absorption and emission spectroscopies. Competitive photoinduced energy and electron transfer are identified to occur in both systems, with the former being dominant in 2. Markedly, the charge-separated state in oDCB exhibits a much longer lifetime compared to that in toluene, reaching 20 ms for 1, the highest ever reported value for fullerene-based materials. These unprecedented results are rationalized by considering conformational phenomena affecting the charge-separated state.

Charge separation lasting for 20 ms in ortho-dichlorobenzene is registered for oligophenylenevinylene–azafullerene donor–acceptor dyad. The synthesis, structural characterization, photophysical, and electrochemical properties for the dyad as well as for the azafullerene–oligophenylenevinylene–azafullerene triad are reported.

In article number 1703546, Kilwon Cho and co-workers demonstrate that PCBM molecules chemically passivate the grain boundaries of organometal halide perovskite crystals. The chemical passivation prevents halogens at the crystal boundaries from exiting from the crystal lattice, and thereby retards thermal degradation of the perovskite crystals. The tunability of perovskite grain boundaries by additives is an advance toward the practical use of organometal halide perovskite solar cells.

Non-fullerene acceptors based on perylenediimides (PDIs) have garnered significant interest as an alternative to fullerene acceptors in organic photovoltaics (OPVs), but their charge transport phenomena are not well understood, especially in bulk heterojunctions (BHJs). Here, charge transport and current fluctuations are investigated by performing correlated low-frequency noise and impedance spectroscopy measurements on two BHJ OPV systems, one employing a fullerene acceptor and the other employing a dimeric PDI acceptor. In the dark, these measurements reveal that PDI-based OPVs have a greater degree of recombination in comparison to fullerene-based OPVs. Furthermore, for the first time in organic solar cells, 1/f noise data are fit to the Kleinpenning model to reveal underlying current fluctuations in different transport regimes. Under illumination, 1/f noise increases by approximately four orders of magnitude for the fullerene-based OPVs and three orders of magnitude for the PDI-based OPVs. An inverse correlation is also observed between noise spectral density and power conversion efficiency. Overall, these results show that low-frequency noise spectroscopy is an effective in situ diagnostic tool to assess charge transport in emerging photovoltaic materials, thereby providing quantitative guidance for the design of next-generation solar cell materials and technologies.

Low-frequency electronic noise is measured in polymer solar cells with fullerene and non-fullerene acceptors. Charge carrier lifetimes deduced from impedance spectroscopy enable the noise data to be fit to the Kleinpenning model. The results establish that low-frequency noise elucidates charge recombination processes that limit power conversion efficiency. This correlated analytical tool provides quantitative guidance to the optimization of emerging photovoltaic materials.

CdS thin films are a promising electron transport layer in PbS colloidal quantum dot (CQD) photovoltaic devices. Some traditional deposition techniques, such as chemical bath deposition and RF (radio frequency) magnetron sputtering, have been employed to fabricate CdS films and CdS/PbS CQD heterojunction photovoltaic devices. However, their power conversion efficiencies (PCEs) are moderate compared with ZnO/PbS and TiO₂/PbS heterojunction CQD solar cells. Here, efficiencies have been improved substantially by employing solution-processed CdS thin films from a single-source precursor. The CdS film is deposited by a straightforward spin-coating and annealing process, which is a simple, low-cost, and high-material-usage fabrication process compared to chemical bath deposition and RF magnetron sputtering. The best CdS/PbS CQD heterojunction solar cell is fabricated using an optimized deposition and air-annealing process achieved over 8% PCE, demonstrating the great potential of CdS thin films fabricated by the single-source precursor for PbS CQDs solar cells.

A heterojunction PbS quantum dot solar cell with an efficiency over 8% is achieved by optimizing CdS electron transport layer deposited by a simple single-source precursor spin-coating process. The optimized band alignment of the device improves the short circuit current and fill factor.