Impact of Temperature Optimization of ITO Thin Film on Tandem Solar Cell Efficiency.

This study examined the impact of temperature optimization on indium tin oxide (ITO) films in monolithic HJT/perovskite tandem solar cells. ITO films were deposited using magnetron sputtering at temperatures ranging from room temperature (25 °C) to 250 °C. The sputtering target was ITO, with a mass ratio of In2O3 to SnO2 of 90% to 10%. The effects of temperature on the ITO film were analyzed using X-ray diffraction (XRD), spectroscopic ellipsometry, and sheet resistance measurements. Results showed that all ITO films exhibited a polycrystalline morphology, with diffraction peaks corresponding to planes (211), (222), (400), (440), and (622), indicating a cubic bixbyite crystal structure. The light transmittance exceeded 80%, and the sheet resistance was 75.1 Ω/sq for ITO deposited at 200 °C. The optical bandgap of deposited ITO films ranged between 3.90 eV and 3.93 eV. Structural and morphological characterization of the perovskite solar cell was performed using XRD and FE-SEM. Tandem solar cell performance was evaluated by analyzing current density-voltage characteristics under simulated sunlight. By optimizing the ITO deposition temperature, the tandem cell achieved a power conversion efficiency (PCE) of 16.74%, resulting in enhanced tandem cell efficiency.

Performance and optimization study of selected 4-terminal tandem solar cells.

Tandem solar cells owing to their layered structure in which each sub-cell utilizes a certain part of the solar spectrum with reduced thermal losses, are promising applicants to promote the power conversion efficiency beyond the Shockley-Queisser limit of single-junction solar cells. This study delves into the performance and optimization of 4-terminal organic/silicon tandem solar cells through numerical simulations using SCAPS-1D software. The tandem architecture combining organic, perovskite, and silicon materials, shows potential in enhancing light absorption across the solar spectrum with complementary absorption spectra. Through innovative material exploration, optimization techniques are explored to advance the performance boundaries of organic/silicon tandem solar cells. The study employs the Beer-Lambert law to assess the impact of varied physical parameters on tandem solar cell efficiency, aiming to propose optimal configurations. Results indicate a maximum efficiency of 25.86% with P3HT:PC70BM organic active layer (150 nm thickness) and 36.8% with Cs2AgBi0.75Sb0.25Br6 active layer (400 nm thickness) in the studied 4-terminal tandem structures. These findings offer valuable insights into the complex physics of these tandem solar cells, for developing high-performance and commercially practical photovoltaic devices.

Unveiling the Potential of Two-Terminal Perovskite/Organic Tandem Solar Cells: Mechanisms, Status, and Challenges.

Perovskite/organic tandem solar cells (PO-TSCs) demonstrate exceptional suitability for emerging applications such as building-integrated photovoltaics, wearable devices, and greenhouse farming. By leveraging the distinctive attributes of perovskite and organic materials, which encompass expanded solar spectrum utilization, chemically benign solubility, and soft nature, PO-TSCs position themselves as ideal candidates for high-performance semi-transparent photovoltaics (ST-PVs). Despite these advantages, their development significantly lags behind other perovskite-based counterparts, such as perovskite/perovskite, perovskite/silicon, and perovskite/Cu(In, Ga)Se2. To address existing challenges and unlock the full potential of PO-TSCs, an exploration of the fundamental mechanisms governing tandem photovoltaic devices is embarked. Delving into critical aspects such as charge generation/separation, energy level alignment, and material choices becomes pivotal for optimizing PO-TSC performance. The investigation of monolithic two-terminal PO-TSCs offers insights into achievements and barriers, recognizing the competitive landscape with other TSC counterparts. Further scrutiny of perovskite absorbers and organic absorbers in TSCs reveals strategies aimed at enhancing stability and efficiency. The discussion extends to interconnection layers, elucidating their role in optimizing light transmission and balancing carrier recombination. In conclusion, a compelling outlook on the dynamic landscape of PO-TSCs is presented, highlighting the remarkable efficiency progression and signaling their potential to revolutionize solar energy harvesting technologies.

All-Round Passivation Strategy Yield Flexible Perovskite/CuInGaSe2 Tandem Solar Cells with Efficiency Exceeding 26.5.

The perovskite/Cu(InGa)Se2 (CIGS) tandem solar cells (TSCs) presents a compelling technological combination poised for the next generation of flexible and lightweight photovoltaic (PV) tandem devices, featuring a tunable bandgap, high power conversion efficiency (PCE), lightweight flexibility, and enhanced stability and durability. Over the years, the imperative to enhance the performance of wide bandgap (WBG) perovskite solar cells (PSCs) has grown significantly, particularly in the context of a flexible tandem device. In this study, an all-round passivation strategy known as Dual Passivation at Grains and Interfaces (DPGI) is introduced for WBG PSCs in perovskite/CIGS tandem structures. The implementation of DPGI is tailored to improve film crystallinity and passivate defects across the solar cell structure, leading to a substantial performance enhancement for WBG PSCs. Subsequently, both rigid and flexible tandem devices are assembled. Impressively, a fully flexible 4T perovskite/CIGS TSCs is successfully fabricated with a PCE of 26.57%, making it the highest value in this field and highlighting its potential applications in the next generation of flexible lightweight PV tandem devices.

Exploring the impact of defect energy levels in CdTe/Si dual-junction solar cells using wxAMPS.

A numerical analysis of a CdTe/Si dual-junction solar cell in terms of defect density introduced at various defect energy levels in the absorber layer is provided. The impact of defect concentration is analyzed against the thickness of the CdTe layer, and variation of the top and bottom cell bandgaps is studied. The results show that CdTe thin film with defects density between 1014 and 1015 cm-3 is acceptable for the top cell of the designed dual-junction solar cell. The variations of the defect concentrations against the thickness of the CdTe layer indicate that the open circuit voltage, short circuit current density, and efficiency (ƞ) are more affected by the defect density at higher CdTe thickness. In contrast, the Fill factor is mainly affected by the defect density, regardless of the thin film's thickness. An acceptable defect density of up to 1015 cm-3 at a CdTe thickness of 300 nm was obtained from this work. The bandgap variation shows optimal results for a CdTe with bandgaps ranging from 1.45 to 1.7 eV in tandem with a Si bandgap of about 1.1 eV. This study highlights the significance of tailoring defect density at different energy levels to realize viable CdTe/Si dual junction tandem solar cells. It also demonstrates how the impact of defect concentration changes with the thickness of the solar cell absorber layer.

Constructing tin oxides Interfacial Layer with Gradient Compositions for Efficient Perovskite/Silicon Tandem Solar Cells with Efficiency Exceeding 28.

Atomic layer deposition (ALD) growth of conformal thin SnOx films on perovskite absorbers offers a promising method to improve carrier-selective contacts, enable sputter processing, and prevent humidity ingress toward high-performance tandem perovskite solar cells. However, the interaction between perovskite materials and reactive ALD precursor limits the process parameters of ALD-SnOx film and requires an additional fullerene layer. Here, it demonstrates that reducing the water dose to deposit SnOx can reduce the degradation effect upon the perovskite underlayer while increasing the water dose to promote the oxidization can improve the electrical properties. Accordingly, a SnOx buffer layer with a gradient composition structure is designed, in which the compositionally varying are achieved by gradually increasing the oxygen source during the vapor deposition from the bottom to the top layer. In addition, the gradient SnOx structure with favorable energy funnels significantly enhances carrier extraction, further minimizing its dependence on the fullerene layer. Its broad applicability for different perovskite compositions and various textured morphology is demonstrated. Notably, the design boosts the efficiencies of perovskite/silicon tandem cells (1.0 cm2) on industrially textured Czochralski (CZ) silicon to a certified efficiency of 28.0%.

Proposal and Numerical Analysis of Organic/Sb2Se3 All-Thin-Film Tandem Solar Cell.

The low bandgap antimony selenide (Sb2Se3) and wide bandgap organic solar cell (OSC) can be considered suitable bottom and top subcells for use in tandem solar cells. Some properties of these complementary candidates are their non-toxicity and cost-affordability. In this current simulation study, a two-terminal organic/Sb2Se3 thin-film tandem is proposed and designed through TCAD device simulations. To validate the device simulator platform, two solar cells were selected for tandem design, and their experimental data were chosen for calibrating the models and parameters utilized in the simulations. The initial OSC has an active blend layer, whose optical bandgap is 1.72 eV, while the initial Sb2Se3 cell has a bandgap energy of 1.23 eV. The structures of the initial standalone top and bottom cells are ITO/PEDOT:PSS/DR3TSBDT:PC71BM/PFN/Al, and FTO/CdS/Sb2Se3/Spiro-OMeTAD/Au, while the recorded efficiencies of these individual cells are about 9.45% and 7.89%, respectively. The selected OSC employs polymer-based carrier transport layers, specifically PEDOT:PSS, an inherently conductive polymer, as an HTL, and PFN, a semiconducting polymer, as an ETL. The simulation is performed on the connected initial cells for two cases. The first case is for inverted (p-i-n)/(p-i-n) cells and the second is for the conventional (n-i-p)/(n-i-p) configuration. Both tandems are investigated in terms of the most important layer materials and parameters. After designing the current matching condition, the tandem PCEs are boosted to 21.52% and 19.14% for the inverted and conventional tandem cells, respectively. All TCAD device simulations are made by employing the Atlas device simulator given an illumination of AM1.5G (100 mW/cm2). This present study can offer design principles and valuable suggestions for eco-friendly solar cells made entirely of thin films, which can achieve flexibility for prospective use in wearable electronics.

Investigation of Polymer/Si Thin Film Tandem Solar Cell Using TCAD Numerical Simulation.

The current study introduces a two-terminal (2T) thin-film tandem solar cell (TSC) comprised of a polymer-based top sub cell and a thin crystalline silicon (c-Si) bottom sub cell. The photoactive layer of the top sub cell is a blend of PDTBTBz-2F as a polymer donor and PC71BM as a fullerene acceptor. Initially, a calibration of the two sub cells is carried out against experimental studies, providing a power conversion efficiency (PCE) of 9.88% for the top sub cell and 14.26% for the bottom sub cell. Upon incorporating both sub cells in a polymer/Si TSC, the resulting cell shows a PCE of 20.45% and a short circuit current density (Jsc) of 13.40 mA/cm2. Then, we optimize the tandem performance by controlling the valence band offset (VBO) of the polymer top cell. Furthermore, we investigate the impact of varying the top absorber defect density and the thicknesses of both absorber layers in an attempt to obtain the maximum obtainable PCE. After optimizing the tandem cell and at the designed current matching condition, the Jsc and PCE of the tandem cell are improved to 16.43 mA/cm2 and 28.41%, respectively. Based on this TCAD simulation study, a tandem configuration established from an all thin-film model may be feasible for wearable electronics applications. All simulations utilize the Silvaco Atlas package where the cells are subjected to standard one Sun (AM1.5G, 1000 W/m2) spectrum illumination.

Investigation on Preparation and Performance of High Ga CIGS Absorbers and Their Solar Cells.

Tandem solar cells usually use a wide band gap absorber for top cell. The band gap of CuIn(1-x)GaxSe2 can be changed from 1.04 eV to 1.68 eV with the ratio of Ga/(In+Ga) from 0 to 1. When the ratio of Ga/(In+Ga) is over 0.7, the band gap of CIGS absorber is over 1.48 eV. CIGS absorber with a high Ga content is a possible candidate one for the top cell. In this work, CuInGa precursors were prepared by magnetron sputtering with CuIn and CuGa targets, and CIGS absorbers were prepared by selenization annealing. The Ga/(In+Ga) is changed by changing the thickness of CuIn and CuGa layers. Additionally, CIGS solar cells were prepared using CdS buffer layer. The effects of Ga content on CIGS thin film and CIGS solar cell were studied. The band gap was measured by PL and EQE. The results show that using structure of CuIn/CuGa precursors can make the band gap of CIGS present a gradient band gap, which can obtain a high open circuit voltage and high short circuit current of the device. With the decrease in Ga content, the efficiency of the solar cell increases gradually. Additionally, the highest efficiency of the CIGS solar cells is 11.58% when the ratio of Ga/(In+Ga) is 0.72. The value of Voc is 702 mV. CIGS with high Ga content shows a great potential for the top cell of the tandem solar cell.

Proposal and Design of Flexible All-Polymer/CIGS Tandem Solar Cell.

Tandem solar cells (TSCs) have attracted prodigious attention for their high efficiency, which can surmount the Shockley-Queisser limit for single-junction solar cells. Flexible TSCs are lightweight and cost-effective, and are considered a promising approach for a wide range of applications. In this paper, a numerical model, based on TCAD simulation, is presented to assess the performance of a novel two-terminal (2T) all-polymer/CIGS TSC. To confirm the model, the obtained simulation results were compared with standalone fabricated all-polymer and CIGS single solar cells. Common properties of the polymer and CIGS complementary candidates are their non-toxicity and flexibility. The initial top all-polymer solar cell had a photoactive blend layer (PM7:PIDT), the optical bandgap of which was 1.76 eV, and the initial bottom cell had a photoactive CIGS layer, with a bandgap of 1.15 eV. The simulation was then carried out on the initially connected cells, revealing a power conversion efficiency (PCE) of 16.77%. Next, some optimization techniques were applied to enhance the tandem performance. Upon treating the band alignment, the PCE became 18.57%, while the optimization of polymer and CIGS thicknesses showed the best performance, reflected by a PCE of 22.73%. Moreover, it was found that the condition of current matching did not necessarily meet the maximum PCE condition, signifying the essential role of full optoelectronic simulations. All TCAD simulations were performed via an Atlas device simulator, where the light illumination was AM1.5G. The current study can offer design strategies and effective suggestions for flexible thin-film TSCs for potential applications in wearable electronics.

Theoretical study of highly efficient all-inorganic Sb2S3-on-Si monolithically integrated (2-T) and mechanically stacked (4-T) tandem solar cells using SCAPS-1D.

The power conversion efficiency of all-inorganic Sb2S3-on-Si two-terminal (2-T) monolithically integrated and four-terminal (4-T) mechanically stacked tandem solar cells are investigated. A one-dimensional solar cell capacitance simulator (SCAPS-1D) has been used to simulate the stand-alone antimony trisulfide (Sb2S3) top sub-cell, silicon (Si) bottom sub-cell, 2-T monolithic, and 4-T mechanically stacked tandem solar cells. The stand-alone sub-cells are optimized by extensive studies, including interface defects density, bulk defects density, absorber layer thickness, and series resistance. The power conversion efficiency (PCE) of simulated stand-alone sub-cells is compared and verified with the existing literature. A current matching condition is established to characterize the 2-T monolithic Sb2S3-on-Si tandem cell. A filtered spectrum has been utilized for bottom sub-cell measurement in the tandem solar cells. The best-simulated PCE of Sb2S3-on-Si 2-T monolithic and 4-T tandem cells is 30.22% and 29.30%, respectively. The simulation results presented in this paper open an opportunity for the scientific community to consider Sb2S3 as a potential top sub-cell material in Sb2S3-on-Si tandem solar cells with high PCE.

Impermeable Atomic Layer Deposition for Sputtering Buffer Layer in Efficient Semi-Transparent and Tandem Solar Cells via Activating Unreactive Substrate.

Atomic layer deposition (ALD) turns out to be particularly attractive technology for the sputtering buffer layer when preparing the semi-transparent (ST) perovskite solar cells (PSCs) and the tandem solar cells. ALD process turns to be island growth when the substrate is unreactive with the ALD reactants, resulting in the pin-hole layer, which causes an adverse effect on anti-sputtering. Here, p-i-n structured PSCs with ALD SnOx as sputtering buffer layer are conducted. The commonly used electron transportation layer (ETL) PCBM in the p-i-n structured PVK solar cell is an unreactive substrate that prevents the layer-by-layer growth for the ALD SnOx . PCBM layer is activated by introducing reaction sites to form impermeable ALD layers. By introducing reaction sites/ALD SnOx as sputtering buffer layer, the authors succeed to fabricate ST-PSCs and perovskite/silicon (double-side polished) tandem solar cells with power conversion efficiency (PCE) of 20.25% and 23.31%, respectively. Besides, the unencapsulated device with reaction sites maintains more than 99% of the initial PCE after aging over 5100 h. This work opens a promising avenue to prepare impermeable layer for stable PSCs, ST-PSCs, tandem solar cells, and the related scale-up solar cells.

New Method for Preparing ZnO Layer for Efficient and Stable Organic Solar Cells.

Owing to outstanding optoelectronic properties and simple preparation, zinc oxide (ZnO) has widely been used in organic solar cells (OSCs). Although versatile cathode interface materials have been designed in past, ZnO remains indispensable owing to its excellent overall performance. Therefore, solving the persistent problem of residual amine reacting with non-fullerene acceptors will make ZnO superior over other materials, and thus improve the performance and energy budget of OSCs. Herein, a simple, effective, and economical method for removing residual amine in ZnO without distorting ZnO is reported. By accurately comparing the alkalinities of ZnO and residual amine, boric acid (BA) is selected as the amine-removing agent because of its suitable acidic dissociation constant. Moreover, the high water solubility of BA ensures that the post-cleaning process can be easily performed. The work function, electron extraction, and stability of cathode interface layer are optimized through rinsing them with BA. Consequently, the power conversion efficiency (PCE) and stability of OSCs under long-term illumination are significantly improved. The optimal 0.04 and 1.00 cm2  single-junction OSCs are based on PBDB-TF:HDO-4Cl:BTP-eC9 bulk heterojunction output 18.40% and 17.42% efficiencies, respectively. Furthermore, tandem OSCs based on the BA-treated ZnO exhibit a 19.56% PCE, demonstrating the reliability of this method.

Improvement Strategies for Stability and Efficiency of Perovskite Solar Cells.

Recently, perovskites have garnered great attention owing to their outstanding characteristics, such as tunable bandgap, rapid absorption reaction, low cost and solution-based processing, leading to the development of high-quality and low-cost photovoltaic devices. However, the key challenges, such as stability, large-area processing, and toxicity, hinder the commercialization of perovskite solar cells (PSCs). In recent years, several studies have been carried out to overcome these issues and realize the commercialization of PSCs. Herein, the stability and photovoltaic efficiency improvement strategies of perovskite solar cells are briefly summarized from several directions, such as precursor doping, selection of hole/electron transport layer, tandem solar cell structure, and graphene-based PSCs. According to reference and analysis, we present our perspective on the future research directions and challenges of PSCs.

F-Type Pseudo-Halide Anions for High-Efficiency and Stable Wide-Band-Gap Inverted Perovskite Solar Cells with Fill Factor Exceeding 84.

The quality of wide-band-gap (WBG) perovskite films plays an important role in tandem solar cells. Therefore, it is necessary to improve the performance of WBG perovskite films for the development of tandem solar cells. Here, we employ F-type pseudo-halogen additives (PF6- or BF4-) into perovskite precursors. The perovskite films with F-type pseudo-halogen additives have a larger grain size and higher crystal quality with lower defect density. At the same time, the perovskite lattice increases due to substitution of F-type pseudo-halogen anions for I-/Br-, and the stress distortion in the film is released, which effectively suppresses the recombination of carriers, reduces the charge transfer loss, and inhibits the phase separation. Finally, the power conversion efficiency (PCE) of the inverted 1.67 eV perovskite devices is significantly improved to over 20% with an impressive fill factor of 84.02% and excellent device stability. In addition, the PCE of the four-terminal (4T) perovskite/silicon tandem solar cells reached 27.35% (PF6-) and 27.11% (BF4-), respectively. This provides important guidance for further improving WBG perovskite solar cell performance.

Enhanced Efficiency of Semitransparent Perovskite Solar Cells via Double-Sided Sandwich Evaporation Technique for Four Terminal Perovskite-Silicon Tandem Application.

Halide perovskite based solar cells (PSC's) have shown tremendous potential based on its facile fabrication technique, and the low cost of perovskite thin film formation with efficiency passing through an unmatched growth in recent years. High quality film along with morphology and crystallinity of the perovskite layer influences the efficiency and other properties of the perovskite solar cell (PSC). Furthermore, semitransparent perovskite solar cells (ST-PSC) are an area of attraction due to its application in tandem solar cells, although various factors like suitable transparent rear electrodes and optimized technique limit the power conversion efficiency (PCE). In this article, we fabricated perovskite film using a technique termed Double-sided sandwich evaporation technique (DS-SET) resulting in high quality perovskite film (MAPbI3 and MAPbIxCl3-x). Using this fabrication approach as compared to the traditional spin-coating method, we reported an enhanced photovoltaic performance of the PSC with a better surface morphology and homogeneity. The best parameter via DS-SET was found to be SET 30 min, which demonstrated a PCE (%) up to 14.8% for MAPbI3 and 16.25% for MAPbIxCl3-x, respectively. Addressing the tandem solar cell, incorporating thin Ag as a transparent electrode with a thickness of 20 nm onto the PSC's as the top cell and further combining with the Si solar cell results in the four terminal (4T) tandem solar cell exhibiting a PCE (%) of 24.43%.

Layered Dion-Jacobson-Type Chalcogenide Perovskite CsLaM2X7 (M = Ta/Nb; X = S/Se) with a Narrow Band Gap of ∼1 eV as a Promising Rear Cell for All-Perovskite Tandem Solar Cells.

Perovskite-perovskite tandem solar cells have bright prospects to improve the power conversion efficiency (PCE) beyond the Shockley-Queisser (SQ) limit of single-junction solar cells. The star lead-based halide perovskites are well-recognized as suitable candidates for the front cell, thanks to their suitable band gap (∼1.8 eV), strong optical absorption, and high certified PCE. However, the toxicity of lead for the front cell and the lack of a narrow band gap (∼1.1 eV) for the rear cell seriously restrict the development of the two-junction tandem cell. To break through this bottleneck, a novel Dion-Jacobson (DJ)-type (n = 2) chalcogenide perovskite CsLaM2X7 (M = Ta, Nb; X = S, Se) has been found based on the powerful first-principles and advanced many-body perturbation GW calculations. Their excellent electronic, transport, and optical properties can be summarized as follows. (1) They are stable and environmentally friendly lead-free materials. (2) The direct band gap of CsLaTa2Se7 (0.96-1.10 eV) is much smaller than those of lead-based halide perovskites and very suitable for the rear cell in the two-junction tandem cell. (3) The carrier mobility in CsLaTa2Se7 reaches 1.6 × 103 cm2 V-1 s-1 at room temperature. (4) The absorption coefficients (3-5 × 105 cm-1) are 1 order higher than that of Si (104 cm-1). (5) The estimated PCEs of the Cs2Sb2Br8-CsLaTa2Se7 tandem cell (33.3%) and the concentrator solar cell (35.8% in 100 suns) are higher than those of the best recorded GaAs-Si tandem cell (32.8%) and the perovskite-perovskite tandem solar cell (24.8%). These energetic results strongly demonstrate that the novel lead-free chalcogenide perovskites CsLaM2X7 are good candidates for the rear cell of tandem cells.

Tuning of the Interconnecting Layer for Monolithic Perovskite/Organic Tandem Solar Cells with Record Efficiency Exceeding 21.

The photovoltaic performance of inorganic perovskite solar cells (PSCs) still lags behind the organic-inorganic hybrid PSCs due to limited light absorption of wide bandgap CsPbI3-xBrx under solar illumination. Constructing tandem devices with organic solar cells can effectively extend light absorption toward the long-wavelength region and reduce radiative photovoltage loss. Herein, we utilize wide-bandgap CsPbI2Br semiconductor and narrow-bandgap PM6:Y6-BO blend to fabricate perovskite/organic tandem solar cells with an efficiency of 21.1% and a very small tandem open-circuit voltage loss of 0.06 V. We demonstrate that the hole transport material of the interconnecting layers plays a critical role in determining efficiency, with polyTPD being superior to PBDB-T-Si and D18 due to its low parasitic absorption, sufficient hole mobility and quasi-Ohmic contact to suppress charge accumulation and voltage loss within the tandem device. These perovskite/organic tandem devices also display superior storage, thermal and ultraviolet stabilities.

Surface-Orientation Elimination of Vapor-Deposited PbI2 Flakes for Efficient Perovskite Synthesis on Curved Solar Cells.

Vapor deposition of perovskite solar cells (PSCs) has attracted considerable interest for its dry processing characteristics. However, a two-step sequential vapor deposition method suffers from ineffective conversion of PbI2 to perovskite with reasons still unclear. In this report, we carefully investigated the crystallization orientation of PbI2 films deposited by physical vapor deposition via synchrotron grazing-incidence wide-angle X-ray scattering (GIWAXS) and observed an asymmetric scattering pattern with respect to the qz-axis. The observed oriented morphology and texture hinder the diffusion of MAI molecules in the PbI2 films synthesized by vapor deposition, resulting in over 15% PbI2 remaining at the buried interface after reaction with MAI vapor. As a result, the MAPbI3 synthesized in this way was also highly oriented, especially in the surface layers. Surface fumigation (SF) step was introduced to decrease the orientational anisotropy of PbI2, which successfully breaks the diffusion barriers of MAI molecules by forming a complex layer on the PbI2 surface with polar solvent vapors, like dimethyl sulfoxide or 1,3-dimethyl-2-imidazolidinone. We infer that the SF treatment changes the vapor-solid reaction mechanism from reaction-crystallization to dissolution-recrystallization, which largely promotes the conversion of PbI2 to perovskite. Defects were reduced in perovskite synthesized in this way, and a p-i-n device with 19.56% efficiency was fabricated, which is among the highest efficiencies reported for sequential-vapor-deposited PSCs. Notably, this method enables the fabrication of conformal perovskite layers on uneven substrates. An exemplary PSC showing efficiency of 8.93% was fabricated on a precurved substrate. We believe that the method is applicable to the fabrication of tandem or curved PSCs that are compatible with wearable or building/autocar-integrated photovoltaics in the future.

Enhanced Optical Absorption in Perovskite/Si Tandem Solar Cells with Nanoholes Array.

Perovskite solar cells are used in silicon-based tandem solar cells due to their tunable band gap, high absorption coefficient and low preparation cost. However, the relatively large optical refractive index of bottom silicon, in comparison with that of top perovskite absorber layers, results in significant reflection losses in two-terminal devices. Therefore, light management is crucial to improve photocurrent absorption in the Si bottom cell. In this paper, nanoholes array filled with TiO2 is introduced into bottom cells design. By finite-difference time-domain methods, the absorption efficiency and photocurrent density in the range of 300-1100 nm has been analyzed, and the structural parameters have been also optimized. Our calculations show the photocurrent density which tends to be saturated with the increase in the height of the nanoholes. The absorption enhancement modes of photons at different wavelengths have been analyzed intuitively by the distribution of electric field. These results enable a viable and convenient route toward high efficiency design of perovskite/Si tandem solar cells.