All-perovskite Tandem Solar Cells Research Articles

Advances in Mixed Tin-Lead Narrow-Bandgap Perovskites for Single-Junction and All-Perovskite Tandem Solar Cells.

Organic-inorganic metal-halide perovskites have received great attention for photovoltaic (PV) applications owing to their superior optoelectronic properties and the unprecedented performance development. For single-junction PV devices, although lead (Pb)-based perovskite solar cells (PSCs) have achieved 26.1% efficiency, the mixed tin-lead (Sn-Pb) perovskites offer more ideal bandgap tuning capability to enable an even higher performance. The Sn-Pb perovskite (with a bandgap tuned to approximately 1.2eV) is also attractive as the bottom subcell for a tandem configuration to further surpass the Shockley-Queisser radiative limit for the single-junction devices. The performance of the all-perovskite tandem solar cells has gained rapid development and achieved a certified efficiency up to 29.1%. In this article, we review the properties and recent development of state-of-the-art mixed Sn-Pb perovskites and their application in single-junction and all-perovskite tandem solar cells. We highlight recent advances in various approaches covering additives, solvents, interfaces, and perovskite growth. We also provide our perspective and outlook on the challenges and strategies for further development of mixed Sn-Pb perovskites in both efficiency and stability for PV applications. This article is protected by copyright. All rights reserved.

Buried Interface Passivation of Sn–Pb Narrow‐Bandgap Perovskite for Highly Efficient All‐Perovskite Tandem Solar Cells

All‐perovskite tandem solar cells (ATSCs) present a remarkable opportunity to overcome the Shockley–Queisser efficiency limit of single‐junction solar cells. However, the stability of ATSCs significantly lags that of their pure Pb‐based single‐junction counterparts. Recent studies have identified that the widely used poly(3,4‐ethylenedioxythiophene)‐poly(styrenesulfonate) (PEDOT:PSS) hole transport layer in narrow‐bandgap (NBG) tin–lead (Sn–Pb) perovskite solar cells (PSCs) hinders the efficiency and stability. Herein, a patching strategy to optimize the interface between perovskite and PEDOT:PSS is proposed. Both theoretical and experimental studies reveal that PenA+ and Ac− can decrease defect states at the interface and strengthen the binding between PEDOT:PSS and Sn–Pb perovskite. Furthermore, the pentylammonium acetate (PenAAc) interlayer improves carrier extraction and suppresses the oxidation of Sn2+ to Sn4+. With the PenAAc buried layer, the fabricated NBG PSCs obtain an impressive power conversion efficiency (PCE) of 21.86%, along with significantly enhanced device stability. By integrating the buried passivated NBG Sn–Pb perovskite with a 1.75 eV wide‐bandgap PSC, the two‐terminal ATSC achieves a PCE of 26.54%. This work provides a valuable approach to fabricate efficient and stable NBG PSCs.

Sustainable thermal regulation improves stability and efficiency in all-perovskite tandem solar cells

Mixed Sn-Pb perovskites have emerged as promising photovoltaic materials for both single- and multi-junction solar cells. However, achieving their scale-up and practical application requires further enhancement in stability. We identify that their poor thermal conductivity results in insufficient thermal transfer, leading to heat accumulation within the absorber layer that accelerates thermal degradation. A thermal regulation strategy by incorporating carboranes into perovskites is developed; these are electron-delocalized carbon-boron molecules known for their efficient heat transfer capability. We specifically select ortho-carborane due to its low thermal hysteresis. We observe its existence through the perovskite layer showing a decreasing trend from the buried interface to the top surface, effectively transferring heat and lowering the surface temperature by around 5 °C under illumination. o-CB also facilitates hole extraction at the perovskite/PEDOT:PSS interface and reduces charge recombination. These enable mixed Sn-Pb cells to exhibit improved thermal stability, retaining 80% of their initial efficiencies after aging at 85 °C for 1080 hours. When integrated into monolithic all-perovskite tandems, we achieve efficiencies of over 27%. A tandem cell maintains 87% of its initial PCE after 704 h of continuous operation under illumination.

Custom-tailored hole transport layer using oxalic acid for high-quality tin-lead perovskites and efficient all-perovskite tandems.

All-perovskite tandem solar cells (TSCs) have exhibited higher efficiencies than single-junction perovskite solar cells (PSCs) but still suffer from the unsatisfactory performance of low-bandgap (LBG) tin-lead (Sn-Pb) subcells. The inherent properties of PEDOT:PSS are crucial to high-performance Sn-Pb perovskite films and devices; however, the underlying mechanism has not been fully explored and revealed. Here, we report a facile oxalic acid treatment of PEDOT:PSS (OA-PEDOT:PSS) to precisely regulate its work function and surface morphology. OA-PEDOT:PSS shows a larger work function and an ordered reorientation and fiber-shaped film morphology with efficient hole transport pathways, leading to the formation of more ideal hole-selective contact with Sn-Pb perovskite for suppressing interfacial nonradiative recombination losses. Moreover, OA-PEDOT:PSS induces (100) preferred orientation growth of perovskite for higher-quality Sn-Pb films. Last, the OA-PEDOT:PSS-tailored LBG PSC yields an impressive efficiency of up to 22.56% (certified 21.88%), enabling 27.81% efficient all-perovskite TSC with enhanced operational stability.

Enhancing the Efficiency and Stability of Tin-Lead Perovskite Solar Cells via Sodium Hydroxide Dedoping of PEDOT:PSS.

Tin-lead (Sn-Pb) perovskite solar cells (PSCs) have gained interest as candidates for the bottom cell of all-perovskite tandem solar cells due to their broad absorption of the solar spectrum. A notable challenge arises from the prevalent use of the hole transport layer, PEDOT:PSS, known for its inherently high doping level. This high doping level can lead to interfacial recombination, imposing a significant limitation on efficiency. Herein, NaOH is used to dedope PEDOT:PSS, with the aim of enhancing the efficiency of Sn-Pb PSCs. Secondary ion mass spectrometer profiles indicate that sodium ions diffuse into the perovskite layer, improving its crystallinity and enlarging its grains. Comprehensive evaluations, including photoluminescence and nanosecond transient absorption spectroscopy, confirm that dedoping significantly reduces interfacial recombination, resulting in an open-circuit voltage as high as 0.90V. Additionally, dedoping PEDOT:PSS leads to increased shunt resistance and high fill factor up to 0.81. As a result of these improvements, the power conversion efficiency is enhanced from 19.7% to 22.6%. Utilizing NaOH to dedope PEDOT:PSS also transitions its nature from acidic to basic, enhancing stability and exhibiting less than a 7% power conversion efficiency loss after 1176h of storage in N2 atmosphere.

Phase-stable wide-bandgap perovskites enabled by suppressed ion migration

Wide-bandgap (>1.7 eV) perovskites suffer from severe light-induced phase segregation due to high bromine content, causing irreversible damage to devices stability. However, the strategies of suppressing photoinduced phase segregation and related mechanisms have not been fully disclosed. Here, we report a new passivation agent 4-aminotetrahydrothiopyran hydrochloride (4-ATpHCl) with multifunctional groups for the interface treatment of a 1.77-eV wide-bandgap perovskite film. 4-ATpH+ impeded halogen ion migration by anchoring on the perovskite surface, leading to the inhibition of phase segregation and thus the passivation of defects, which is ascribed to the interaction of 4-ATpH+ with perovskite and the formation of low-dimensional perovskites. Finally, the champion device achieved an efficiency of 19.32% with an open-circuit voltage (VOC) of 1.314 V and a fill factor of 83.32%. Moreover, 4-ATpHCl modified device exhibited significant improved stability as compared with control one. The target device maintained 80% of its initial efficiency after 519 h of maximum power output (MPP) tracking under 1 sun illumination, however, the control device showed a rapid decrease in efficiency after 267 h. Finally, an efficiency of 27.38% of the champion 4-terminal all-perovskite tandem solar cell was achieved by mechanically stacking this wide-bandgap top subcell with a 1.25-eV low-bandgap perovskite bottom subcell.

Narrow Bandgap Metal Halide Perovskites for All-Perovskite Tandem Photovoltaics.

All-perovskite tandem solar cells are attracting considerable interest in photovoltaics research, owing to their potential to surpass the theoretical efficiency limit of single-junction cells, in a cost-effective sustainable manner. Thanks to the bandgap-bowing effect, mixed tin-lead (Sn-Pb) perovskites possess a close to ideal narrow bandgap for constructing tandem cells, matched with wide-bandgap neat lead-based counterparts. The performance of all-perovskite tandems, however, has yet to reach its efficiency potential. One of the main obstacles that need to be overcome is the─oftentimes─low quality of the mixed Sn-Pb perovskite films, largely caused by the facile oxidation of Sn(II) to Sn(IV), as well as the difficult-to-control film crystallization dynamics. Additional detrimental imperfections are introduced in the perovskite thin film, particularly at its vulnerable surfaces, including the top and bottom interfaces as well as the grain boundaries. Due to these issues, the resultant device performance is distinctly far lower than their theoretically achievable maximum efficiency. Robust modifications and improvements to the surfaces of mixed Sn-Pb perovskite films are therefore critical for the advancement of the field. This Review describes the origins of imperfections in thin films and covers efforts made so far toward reaching a better understanding of mixed Sn-Pb perovskites, in particular with respect to surface modifications that improved the efficiency and stability of the narrow bandgap solar cells. In addition, we also outline the important issues of integrating the narrow bandgap subcells for achieving reliable and efficient all-perovskite double- and multi-junction tandems. Future work should focus on the characterization and visualization of the specific surface defects, as well as tracking their evolution under different external stimuli, guiding in turn the processing for efficient and stable single-junction and tandem solar cell devices.

Mixed tin-lead perovskites with balanced crystallization and oxidation barrier for all-perovskite tandem solar cells

Mixed tin-lead perovskite solar cells have driven a lot of passion for research because of their vital role in all-perovskite tandem solar cells, which hold the potential for achieving higher efficiencies compared to single-junction counterparts. However, the pronounced disparity in crystallization processes between tin-based perovskites and lead-based perovskites, coupled with the easy Sn2+ oxidation, has long been a dominant factor contributing to high defect densities. In this study, we propose a multidimensional strategy to achieve efficient tin-lead perovskite solar cells by employing a functional N-(carboxypheny)guanidine hydrochloride molecule. The tailored N-(carboxypheny)guanidine hydrochloride molecule plays a pivotal role in manipulating the crystallization and grain growth of tin-lead perovskites, while also serving as a preservative to effectively inhibit Sn2+ oxidation, owing to the strong binding between N-(carboxypheny)guanidine hydrochloride and tin (II) iodide and the elevated energy barriers for oxidation. Consequently, single-junction tin-lead cells exhibit a stabilized power conversion efficiency of 23.11% and can maintain 97.45% of their initial value even after 3500 h of shelf storage in an inert atmosphere without encapsulation. We further integrate tin-lead perovskites into two-terminal monolithic all-perovskite tandem cells, delivering a certified efficiency of 27.35%.

Synergetic Near- and Far-Field Plasmonic Effects for Optimal All-Perovskite Tandem Solar Cells with Maximized Infrared Absorption.

The efficiency and reliability of perovskite solar cells have rapidly increased in conjunction with the proposition of advanced single-junction and multi-junction designs that allow light harvesting to be maximized. However, Sn-based compositions required for optimized all-perovskite tandem devices have reduced absorption coefficients, as opposed to pure Pb perovskites. To overcome this, we investigate near- and far-field plasmonic effects to locally enhance the light absorption of infrared photons. Through optimization of the metal type, particle size, and volume concentration, we maximize effective light harvesting while minimizing parasitic absorption in all-perovskite tandem devices. Interestingly, incorporating 240 nm silver particles into the Pb-Sn perovskite layer with a volume concentration of 3.1% indicates an absolute power conversion efficiency enhancement of 2% in the tandem system. We present a promising avenue for experimentalists to realize ultrathin all-perovskite tandem devices with optimized charge carrier collection, diminishing the weight and the use of Pb.

Homogeneous crystallization and buried interface passivation for perovskite tandem solar modules.

Scalable fabrication of all-perovskite tandem solar cells is challenging because the narrow-bandgap subcells made of mixed lead-tin (Pb-Sn) perovskite films suffer from nonuniform crystallization and inferior buried perovskite interfaces. We used a dopant from Good's list of biochemical buffers, aminoacetamide hydrochloride, to homogenize perovskite crystallization and used it to extend the processing window for blade-coating Pb-Sn perovskite films and to selectively passivate defects at the buried perovskite interface. The resulting all-perovskite tandem solar module exhibited a certified power conversion efficiency of 24.5% with an aperture area of 20.25 square centimeters.

Design and simulation of three-junction all perovskite tandem solar cells: A path to enhanced photovoltaic performance

Despite numerous publications on two-junction tandems using SCAPS-1D simulation, there is a gap in research regarding three-junction tandems. This paper explores the advantages of three junction all-perovskite tandem solar cells (3J-APTSC) where we introduce a new methodology utilizing two-step filtered spectrum and current matching techniques in SCAPS-1D to design realistic tandem solar cells. Crucial steps involve determining filtered spectrum and current matching points among sub-cells for tandem optimization. Our designed three-terminal tandem solar cell exhibits promising photovoltaic parameters, including VOC: 3.76 V, JSC: 10.70 mA/cm2, FF: 69.00 %, and PCE: 26.24 %, achieved through optimized active layer thicknesses. This thorough examination of 3J-APTSC offers insights that could drive the future development of highly efficient tandem solar cells.

Surface repair of wide-bandgap perovskites for high-performance all-perovskite tandem solar cells

Wide-bandgap (WBG) perovskite solar cells (PSCs) play a fundamental role in perovskite-based tandem solar cells. However, the efficiency of WBG PSCs is limited by significant open-circuit voltage losses, which are primarily caused by surface defects. In this study, we present a novel method for modifying surfaces using the multifunctional S-ethylisothiourea hydrobromide (SEBr), which can passivate both Pb-I and FA-I terminated surfaces. Moreover, the SEBr upshifted the Fermi level at the perovskite interface, thereby promoting carrier collection. This proposed method was effective for both 1.67 and 1.77 eV WBG PSCs, achieving power conversion efficiencies (PCEs) of 22.47% and 19.90%, respectively, with VOC values of 1.28 and 1.33 V, along with improved film and device stability. With this advancement, we were able to fabricate monolithic all-perovskite tandem solar cells with a champion PCE of 27.10%. This research offers valuable insights for passivating the surface trap states of WBG perovskite through rational multifunctional molecular engineering.

Hot-Carrier Cooling Regulation for Mixed Sn-Pb Perovskite Solar Cells.

The rapid relaxation of hot carriers leads to energy loss in the form of heat and consequently restricts the theoretical efficiency of single-junction solar cells; However, this issue has not received much attention in tin-lead perovskites solar cells. Herein, tin(II) oxalate (SnC2O4) is introduced into tin-lead perovskite precursor solution to regulate hot-carrier cooling dynamics. The addition of SnC2O4 increases the length of carrier diffusion, extends the lifetime of carriers, and simultaneously slows down the cooling rate of carriers. Furthermore, SnC2O4 can bond with uncoordinated Sn2+ and Pb2+ ions to regulate the crystallization of perovskite and enable large grains. The strongly reducing properties of the C2O4 2- can inhibit the oxidation of Sn2+ to Sn4+ and minimize the formation of Sn vacancies in the resulting perovskite films. Additionally, as a substitute for tin(II) fluoride, the introduction of SnC2O4 avoids the carrier transport issues caused by the aggregation of F- ions at the interface. As a result, the SnC2O4-treated Sn-Pb cells show a champion efficiency of 23.36%, as well as 27.56% for the all-perovskite tandem solar cells. Moreover, the SnC2O4-treated devices show excellent long-term stability. This finding is expected to pave the way toward stable and highly efficient all-perovskite tandem solar cells.

Electron-withdrawing organic ligand for high-efficiency all-perovskite tandem solar cells

Electron-withdrawing organic ligand for high-efficiency all-perovskite tandem solar cells

Enhanced efficiency in two-terminal all-perovskite tandem solar cells via binary functional high polymer doping strategy

An enhanced power conversion efficiency (PCE) of 26.1 % has been achieved in two-terminal (2T) all-perovskite tandem perovskite solar cells (TPSCs) via a binary functional high polymer doping strategy. By incorporating methylene diphenyl diisocyanate polyurethane (MDI-PU) and PJ71 into the wide bandgap (WBG) and narrow bandgap (NBG) perovskite layers, respectively, the perovskite crystalline quality of them was significantly improved. The optimized PCE of the WBG top cell and the NBG bottom cell achieved 17.6 % and 20.9 %, respectively. After continuous dark storage of 150 days in nitrogen-filled glovebox, the PCE of optimized TPSC remained 94.2 % of initial. TPSCs on flexible substrates of polyethylene naphthalate (PEN) and silk-derived substrate (SDS) were also studied. With the binary polymer doping strategy, the PEN-based TPSC achieved a champion PCE of 22.2 %, and exhibited excellent anti-bending ability compared with control. The champion SDS-based TPSC achieved the PCE of 11.6 %, and showed enhanced anti-stretching ability. We demonstrate that strong coordinate bonding formed between the O atom in the carbonyl group of MDI-PU and the Pb2+ ions at the grain boundaries (GBs) in WBG perovskite. For the NBG layer, the S atoms in the thiophene structure of PJ71 interact with the Pb2+ and Sn2+ ions in the NBG perovskite and effectively passivate the GB defects. The study suggests the potential for developing new generation multi-functional optoelectronic high polymers to further boost the performance of 2T all-perovskite TPSCs.

All-perovskite tandem solar cells from fundamentals to technological progress

Organic-inorganic perovskite materials have gradually progressed from single-junction solar cells to tandem (double) or even multi-junction (triple-junction) solar cells as all-perovskite tandem solar cells (APTSCs) have advantages: (1) the tunable...

Numerical Simulation of Lead-Free Tin and Germanium Based All Perovskite Tandem Solar Cell

The ability to customize the materials bandgaps makes perovskite solar cells a promising candidate for hybrid-tandem applications. This allows them to effectively utilize parts of the solar spectrum that silicon-based solar cells cannot efficiently capture, resulting in higher absorption coefficients. However, there is a lack of research on lead-free all-perovskite tandem solar cells, and secondary data on materials is limited. One of the main challenges in previous studies is the high cost and solid structure of traditional silicon-based solar cells, which require significant storage space. Additionally, lead-based perovskite solar cells pose environmental concerns due to their water solubility and potential harmful effects upon consumption. To address these issues, thin-film perovskite solar cells with liquid solvents are employed in the solar cell design. Lead is replaced with germanium and tin-based perovskites, which exhibit comparable photovoltaic performance to silicon. In the present work, the OghmaNano simulation tool was utilized to conduct numerical simulation of the perovskite design. The perovskite solar cell layers were structured as follows: FTO/ZnO/MAGeI3/Spiro-OMeTAD/FAMASnGeI3/Cu2O/Au. The variables considered included optimum layer thicknesses and bandgaps, as well as the most suitable materials for the ETL and HTL, aiming to obtain the highest efficiency. Based on the simulation results, the proposed perovskite structure shows remarkable photovoltaic parameters. The Voc was measured at 0.84 V Jsc of 16.1 mA/cm2, FF of 0.825, and PCE that reached 11.12%. This project contributes to future research on materials for the ETL and HTL of lead-free, tin and germanium based APTSCs.

Minimizing Interfacial Recombination in 1.8eVTriple-Halide Perovskites for 27.5% Efficient All-Perovskite Tandems.

All-perovskite tandem solar cells show great potential to enable the highest performance at reasonable costs for a viable market entry in the near future. In particular, wide-bandgap (WBG) perovskites with higher open-circuit voltage (VOC ) are essential to further improve the tandem solar cells' performance. Here, a new 1.8eV bandgap triple-halide perovskite composition in conjunction with a piperazinium iodide (PI) surface treatment is developed. With structural analysis, it is found that the PI modifies the surface through a reduction of excess lead iodide in the perovskite and additionally penetrates the bulk. Constant light-induced magneto-transport measurements are applied to separately resolve charge carrier properties of electrons and holes. These measurements reveal a reduced deep trap state density, and improved steady-state carrier lifetime (factor 2.6) and diffusion lengths (factor 1.6). As a result, WBG PSCs achieve 1.36V VOC , reaching 90% of the radiative limit. Combined with a 1.26eV narrow bandgap (NBG) perovskite with a rubidium iodide additive, this enables a tandem cell with a certified scan efficiency of 27.5%.

Insights into efficiency deviation from current-mismatch for tandem photovoltaics

For tandem solar cells (TSCs), the highest efficiency is generally believed to occur when the top and bottom sub-cells obtain an identical photocurrent, i.e., the current-match condition. However, the real situation is that there is a slight deviation from the matching point, which is an interesting phenomenon, but lacks a clear explanation. Here, we report a coupled photoelectric investigation on the intrinsic mechanisms within TSCs under various current configurations. Taking an all-perovskite TSC as an example, we find that the efficiency deviation originates from the current reduction and fill factor (FF) compensation; moreover, the optimal efficiency depends primarily on the sub-cells with higher FF. Our analysis further reveals that the higher FF and efficiency are achieved under current-mismatch condition due to the differentiated voltage assignments among the sub-cells, i.e., the sub-cells with higher currents require larger voltages in order to effectively recombine the surplus currents. We also find that the impact of sub-cell leakage on TSC performance can be partially alleviated by increasing the current of the affected sub-cell. Such an optoelectronic insight offers a valuable guidance for designing high-efficiency TSCs.

Hole Transport Layer-Free Low-Bandgap Perovskite Solar Cells for Efficient All-Perovskite Tandems.

Low-bandgap (LBG,Eg ≈1.25eV)tin-lead (Sn-Pb) perovskite solar cells (PSCs) play critical roles inconstructing efficient all-perovskite tandem solar cells (TSCs) that can surpass the efficiency limit of single-junction solar cells. However, the traditional poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) hole transport layer (HTL) in LBG PSCs usually restricts device efficiency and stability. Here, a strategy of employing 2-aminoethanesulfonic acid (i.e., taurine) as the interface bridge to fabricate efficient HTL-free LBG PSCs with improved optoelectronic properties of the perovskite absorbers at the buried contacts is reported. Taurine-modified ITO substrate has lower optical losses, better energy level alignment, and higher charge transfer capability than PEDOT:PSS HTL, leading to significantly improved open-circuit voltage (VOC ) and short-circuit current density of corresponding devices. The best-performing LBG PSC with a power conversion efficiency (PCE) of 22.50% and an impressive VOC of 0.911V is realized, enabling all-perovskite TSCs with an efficiency of 26.03%. The taurine-based HTL-free TSCs have highly increased stability, retaining more than 90% and 80% of their initial PCEs after constant operation under 1-sun illumination for 600h and under 55°C thermal stress for 950h, respectively. This work provides a facile strategy for fabricating efficient and stable perovskite devices with a simplified HTL-free architecture.