Inverted Perovskite Solar Cells Research Articles

Controllable Heavy n–type Behaviours in Inverted Perovskite Solar Cells with Non‐Conjugated Passivants

AbstractInterfacial issues between the perovskite film and electron transport layer greatly limit the efficiency and stability of inverted (p‐i‐n) perovskite solar cells (PSCs). Despite organic ammonium passivants have been widely established as interfacial layers, they failed to improve electron extraction. Here, we reported that the heavy n‐type characteristics in a low band gap perovskite film could be modulated by incorporating non‐conjugated ammonium passivants with strong electron‐withdrawing abilities. This resulted in a significant enhancement of electron extraction in the heavily n‐type doped perovskite. The passivant‐treated PSCs exhibited a power conversion efficiency of 25.74 % with an excellent fill factor of 85.4 % and a high open‐circuit voltage of 1.166 V, which are significantly higher than that of the control device. The unencapsulated devices maintained 88 % of their initial PCEs after 1,200 hours at 85 °C.

Stable Surface Contact with Tailored Alkylamine Pyridine Derivatives for High-Performance Inverted Perovskite Solar Cells.

Formamidinium-cesium lead triiodide (FA1-xCsxPbI3) perovskite holds great promise for perovskite solar cells (PSCs) with both high efficiency and stability. However, the defective perovskite surfaces induced by defects and residual tensile strain largely limit the photovoltaic performance of the corresponding devices. Here, the passivation capability of alkylamine-modified pyridine derivatives for the surface defects of FA1-xCsxPbI3 perovskite is systematically studied. Among the studied surface passivators, 3-(2-aminoethyl)pyridine (3-PyEA) with the suitable size is demonstrated to be the most effective in reducing surface iodine impurities and defects (VI and I2) through its strong coordination with Npyridine. Additionally, the tail amino group (─NH2) from 3-PyEA can react with FA+ cations to reduce the surface roughness of perovskite films, and the reaction products can also passivate FA vacancies (VFA), and further strengthen their binding interaction to perovskite surfaces. These merits lead to suppressed nonradiative recombination loss, the release of residual tensile stress for the perovskite films, and a favorable energy-level alignment at the perovskite/[6,6]-phenyl-C61-butyric acid methyl ester interface. Consequently, the resulting inverted FA1-xCsxPbI3 PSCs obtain an impressive power conversion efficiency (PCE) of 25.65% (certified 25.45%, certified steady-state efficiency 25.06%), along with retaining 96.5% of the initial PCE after 1800 h of 1-sun operation at 55 °C in air.

A Polymeric Hole Transporter with Dual-Interfacial Interactions Enables 25%-Efficiency Blade-Coated Perovskite Solar Cells.

Self-assembly monolayer (SAM) hole transporters, consisting of anchoring, spacer, and terminal groups, have played a significant role in the development of inverted perovskite solar cells (PSCs). However, the weak interaction between perovskite and hydrophobic terminal group of SAMs limits surface wettability and interface stability. To address this issue, two novel hole transporters (named DBPP and Poly-DBPP) with centrosymmetric biphosphonic acid groups are developed. Unlike conventional SAM hole transporters, the biphosphonic acid groups in DBPP and Poly-DBPP can anchor to the underlying conductive substrate and interact with the perovskite layer simultaneously, improving surface wettability and suppressing interface recombination. Furthermore, compared to the small-molecular DBPP, Poly-DBPP exhibits higher conductance and excellent uniformity. This translates to a remarkable power conversion efficiency of 25.1% for blade-coated PSCs and 22.0% for large-area modules, respectively. Additionally, the PSCs based on Poly-DBPP demonstrate impressive operational stability, retaining 92% of their initial PCE after 1,600 h of light soaking. This work presents a promising strategy for designing multifunctional hole transporters, paving the way for highly efficient and stable PSCs.

Polymeric Charge-Transporting Materials for Inverted Perovskite Solar Cells.

Inverted perovskite solar cells (PSCs) hold exceptional promise as next-generation photovoltaic technology, where both perovskite absorbers and charge-transporting materials (CTMs) play critical roles in cell performance. In recent years, polymeric CTMs have played an important role in developing efficient, stable, and large-area inverted PSCs due to their unique properties of high conductivity, tunable structures, and mechanical flexibility. This review provides a comprehensive overview of polymeric CTMs used in inverted PSCs, encompassing polymeric hole transport materials (HTMs) and electron transport materials (ETMs). the relationship between their molecular structures, modification strategies are systematically summarized and analyzed for adjusting energy levels, and improving charge extraction, enabling a deep understanding of these widely used materials. The review also explores effective strategies for designing even more efficient polymeric CTMs. Finally, an outlook is proposed on the exciting research of novel polymeric CTMs, paving the way for their commercialized applications in PSCs.

Cross‐Linkable Fullerene Electron Transport Layer with Internal Encapsulation Capability for Efficient and Stable Inverted Perovskite Solar Cells

AbstractA stable and compact fullerene electron transport layer (ETL) is crucial for high‐performance inverted perovskite solar cells (PSCs). However, traditional fullerene‐based ETLs like C60 and PCBM are prone to aggregate under operational conditions, a challenge recently recognized by academic and industrial researchers. Here, we designed and synthesized a novel cross‐linkable fullerene molecule, bis((3‐methyloxetan‐3‐yl)methyl) malonate‐C60 monoadduct (BCM), for use as an ETL in PSCs. Upon a low‐temperature annealing at 100 °C, BCM undergoes in situ cross‐linking to form a robust cross‐linked BCM (CBCM) film, which demonstrates excellent electron mobility and a suitable band structure for efficient PSCs. Our results show that PSCs incorporating CBCM‐based ETL achieve an impressive efficiency of 25.89 % (certified: 25.36 %), significantly surpassing the 23.25 % efficiency of PCBM‐based devices. The intramolecular covalent interactions within CBCM films effectively prevent aggregation and enhance film compactness, creating an internal encapsulation layer that mitigates the decomposition and ion migration of perovskite components. Consequently, CBCM‐based PSCs show exceptional stability, maintaining 97.8 % of their initial efficiency after 1000 hours of maximum power point tracking, compared to only 78.6 % retention in PCBM‐based devices after less than 820 hours.

Enhancing the Efficiency and Stability of Inverted Perovskite Solar Cells and Modules through Top Interface Modification with N‐type Semiconductors

The interface modification between perovskite and electron transport layer (ETL) plays a crucial role in achieving high performance inverted perovskite photovoltaics (i‐PPVs). Herein, non‐fullerene acceptors (NFAs), known as Y6‐BO and Y7‐BO, were utilized to modify the perovskite/ETL interface in i‐PPVs. Non‐polar solvent‐soluble NFAs can effectively passivate surface defects without structural damage of the underlying perovskite films. Additionally, the improved PCBM ETL induced by NFAs modification significantly accelerates the electrons extraction. As a result, both Y6‐BO and Y7‐BO exhibit more effective interface modification effects compared to traditional PI molecules. The power conversion efficiency (PCE) of the inverted perovskite solar cell (i‐PSC) modified with Y7‐BO reaches 25.82%. Moreover, the adoption of non‐polar solvents and the superior semiconductor properties of Y7‐BO molecules also enable perovskite solar modules (i‐PSM) with effective areas of 50 cm2, 400 cm2, and 1160 cm2 to achieve record efficiencies of 23.05%, 22.32%, and 21.1% (certified PCE), respectively, making them the best PCE reported in the literature. Importantly, enhanced interface mechanical strength between the perovskite and PCBM layer results in significantly improved environmental and operational stability of the cells. The cells modified with Y7‐BO maintained 94.4% of the initial efficiency after 1522 hours of maximum power point aging.

Enhancing the Efficiency and Stability of Inverted Perovskite Solar Cells and Modules through Top Interface Modification with N-type Semiconductors.

The interface modification between perovskite and electron transport layer (ETL) plays a crucial role in achieving high performance inverted perovskite photovoltaics (i-PPVs). Herein, non-fullerene acceptors (NFAs), known as Y6-BO and Y7-BO, were utilized to modify the perovskite/ETL interface in i-PPVs. Non-polar solvent-soluble NFAs can effectively passivate surface defects without structural damage of the underlying perovskite films. Additionally, the improved PCBM ETL induced by NFAs modification significantly accelerates the electrons extraction. As a result, both Y6-BO and Y7-BO exhibit more effective interface modification effects compared to traditional PI molecules. The power conversion efficiency (PCE) of the inverted perovskite solar cell (i-PSC) modified with Y7-BO reaches 25.82%. Moreover, the adoption of non-polar solvents and the superior semiconductor properties of Y7-BO molecules also enable perovskite solar modules (i-PSM) with effective areas of 50 cm2, 400 cm2, and 1160 cm2 to achieve record efficiencies of 23.05%, 22.32%, and 21.1% (certified PCE), respectively, making them the best PCE reported in the literature. Importantly, enhanced interface mechanical strength between the perovskite and PCBM layer results in significantly improved environmental and operational stability of the cells. The cells modified with Y7-BO maintained 94.4% of the initial efficiency after 1522 hours of maximum power point aging.

Stereo-Hindrance Induced Conformal Self-Assembled Monolayer for High Efficiency Inverted Perovskite Solar Cells.

Self-assembled monolayers (SAMs) are employed as hole-selective contacts in inverted perovskite solar cells (PSCs) and have achieved record power conversion efficiency (PCE) over 26%. However, the tendency of extensively employed SAM [2-(3,6-Dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid to aggregate leads to its uneven coverage to the transparent conducting oxide substrate, which subsequently compromises the photovoltaic performance. Herein, a novel tert-butyl functionalized phosphonic acid carbazole SAM is developed, i.e., (4-(3,6-di-tert-butyl-9H-carbazol-9-yl)butyl)phosphonic acid (tBu-4PACz), and introduced to a mixed SAM system as the hole-extraction layer in inverted PSCs. The stereo-hindrance of the bulky tert-butyl group prevents undesired aggregation and leads to better conformality, which facilitates more efficient hole-extraction and suppresses interfacial recombination losses. The tBu-4PACz SAM-based inverted PSC has achieved record level PCE of 26.25% (26.21%, certificated) with outstanding fill factors over 86%. Moreover, the mixed SAM based inverted PSC devices maintained over 94.7% of their initial efficiency after 500h continuous maximum power-point tracking under simulation 1-sun irradiation.

Investigation of internal thermal distribution in inverted perovskite solar cell and improvement of its heat dissipation performance

Abstract COMSOL Multiphysics software was used to construct a numerical opto-electro-thermal coupling model to investigate the mechanisms of internal heat generation, conduction, and dissipation in inverted (p-i-n architecture) perovskite solar cells (PSCs). The research results indicate that Joule heating and Shockley-Read-Hall (SRH) recombination are the primary sources of heat, leading to significant accumulation of heat at the interfaces between the perovskite and the electron transport layer (ETL), as well as between the ETL and the electrode. This concentration of heat not only affects the performance of the device but also poses challenges for overall thermal management. Therefore, we compared four different top electrode materials (Ag, Cu, Al, and reduced graphene oxide) to assess their performance in terms of heat dissipation efficiency. The results showed that reduced graphene oxide (RGO) performed exceptionally well in heat dissipation efficiency, primarily due to its high thermal conductivity, which enables it to effectively reduce heat accumulation at the interfaces, thereby improving performance of PSCs. This finding provides important material selection criteria for optimizing the thermal management of PSCs.

Enhancing Efficiency and Stability of Inverted Perovskite Solar Cells through Solution‐Processed and Structurally Ordered Fullerene

AbstractThe electron transporting layer (ETL) used in high performance inverted perovskite solar cells (PSCs) is typically composed of C60, which requires time‐consuming and costly thermal evaporation deposition, posing a significant challenge for large‐scale production. To address this challenge, herein, we present a novel design of solution‐processible electron transporting material (ETM) by grafting a non‐fullerene acceptor fragment onto C60. The synthesized BTPC60 exhibits an exceptional solution processability and well‐organized molecular stacking pattern, enabling the formation of uniform and structurally ordered film with high electron mobility. When applied as ETL in inverted PSCs, BTPC60 not only exhibits excellent interfacial contact with the perovskite layer, resulting in enhanced electron extraction and transfer efficiency, but also effectively passivates the interfacial defects to suppress non‐radiative recombination. Resultant BTPC60‐based inverted PSCs deliver an impressive power conversion efficiency (PCE) of 25.3 % and retain almost 90 % of the initial values after aging at 85 °C for 1500 hours in N2. More encouragingly, the solution‐processed BTPC60 ETL demonstrates remarkable film thickness tolerance, and enables a high PCE up to 24.8 % with the ETL thickness of 200 nm. Our results highlight BTPC60 as a promising solution‐processed fullerene‐based ETM, opening an avenue for improving the scalability of efficient and stable inverted PSCs.

Polymerized non-fullerene small molecular acceptor as a versatile electron-transport material for 24.50 % efficiency inverted perovskite solar cells with extended spectral response

Development of novel non-fullerene electron-transport materials (ETMs) with excellent optoelectronic properties, good thermal and chemical stability, and defect passivation capability is of great significance for improving the device performance of inverted perovskite solar cells (PSCs). In this work, a polymerized non-fullerene small molecular acceptor with narrow bandgap named PY-DFT is rationally designed and synthesized. The resultant materials not only exhibits great hydrophobicity, thermal and chemical stability, but also maintains the excellent electron-transport properties of Y-type small molecule. Moreover, the electron-rich units in PY-DFT finely passivates the surface defects in perovskite. Consequently, an exceptional PCE of 24.50 % has been achieved for the champion device based on PY-DFT ETM, which is the highest efficiency for inverted PSCs based on non-fullerene ETMs to date. Notably, PY-DFT provides an extra current density of 0.25 mA/cm2 in the near-infrared light response region, where the intrinsic perovskite film has no spectral response, demonstrating attractive advantages in rationally utilization of solar spectrum. The target device without encapsulation also demonstrates good long-term operational stability. This work paves a new avenue for designing photo-active non-fullerene electron-acceptor towards efficient and stable inverted PSCs.

Tuning anchoring groups of “Y-Type” self-assembled hole transport materials for interface passivation in inverted perovskite solar cells

Tuning anchoring groups of “Y-Type” self-assembled hole transport materials for interface passivation in inverted perovskite solar cells

Controllable Heavy n-type Behaviours in Inverted Perovskite Solar Cells with Non-Conjugated Passivants.

Interfacial issues between the perovskite film and electron transport layer greatly limit the efficiency and stability of inverted (p-i-n) perovskite solar cells (PSCs). Despite organic ammonium passivants have been widely established as interfacial layers, they failed to improve electron extraction. Here, we reported that the heavy n-type characteristics in a low bandgap perovskite film could be modulated by incorporating non-conjugated ammonium passivants with strong electron-withdrawing abilities. This resulted in a significant enhancement of electron extraction in the heavily n-type doped perovskite. The passivant-treated PSCs exhibited a power conversion efficiency of 25.74% with an excellent fill factor of 85.4% and a high open-circuit voltage of 1.166 V, which are significantly higher than that of the control device. The unencapsulated devices maintained 88% of their initial PCEs after 1,200 hours at 85 °C.

Interface modification based on norfloxacin for enhancing the performance of the inverted perovskite solar cells

Interface modification based on norfloxacin for enhancing the performance of the inverted perovskite solar cells

Synergistic strain engineering of the perovskite films for improving flexible inverted perovskite solar cells under convex bending

Synergistic strain engineering of the perovskite films for improving flexible inverted perovskite solar cells under convex bending

Double-side Integration of the Fluorinated Self-Assembling Monolayers for Enhanced Stability of Inverted Perovskite Solar Cells

Double-side Integration of the Fluorinated Self-Assembling Monolayers for Enhanced Stability of Inverted Perovskite Solar Cells

Self‐Induced Bi‐interfacial Modification via Fluoropyridinic Acid For High‐Performance Inverted Perovskite Solar Cells

AbstractThe uncontrolled crystallization of perovskite generates a significant number of internal and interfacial defects, posing a major challenge to the performance of perovskite solar cells (PSCs). In this paper, a novel bi‐interfacial modification strategy utilizing 5‐fluoropyridinic acid (FPA) is proposed to modulate crystal growth and provide defect passivation. It is demonstrated that FPA is self‐deposited at both the top and bottom interfaces of perovskite films during thermal annealing. The CO and N functional groups in FPA serve as chelating agents, binding closely to uncoordinated Pb2+/Pb clusters, thereby passivating defects and reducing charge recombination at the interfaces. The strong chemical interactions between FPA and Pb further stabilize the Pb‐I framework, promoting the formation of high‐quality perovskite films, as confirmed by in situ photoluminescence measurements. Consequently, the modified inverted PSCs achieved an exceptional power conversion efficiency (PCE) of 25.37%. Moreover, the devices retained over 93.17% of initial efficiency after 3000 h of continuous illumination under one‐sun equivalent conditions in a nitrogen atmosphere. This paper presents a promising pathway for enhancing the performance and stability of inverted PSCs through a self‐induced bi‐interfacial modification approach.

Computational Screening Two-Dimensional Conjugated Microporous Polymer Applied in Perovskite Solar Cells.

A two-dimensional (2D) conjugated microporous polymer with a structure of 2D nanosheets has been synthesized. Theoretical calculations and experimental results reveal that the Fermi level of this 2D polymer aligns well with perovskite absorber, and its conduction band is high enough to block electron transport into the anode. This 2D polymer is used to modify the hole transport layer, significantly improving its photoelectric properties, including enhanced hole mobility, matched energy level, and reduced recombination. Furthermore, the 2D polymer exhibits a mesoporous structure, allowing perovskite to fill into its loose framework, increasing the hole export area and providing a large hole transport flux. As a result, the efficiency of inverted perovskite solar cells enhances to 24.64 % from 21.17 % of control device without 2D conjugated microporous polymer. Given that this material can be synthesized on a large scale, this work has significant implications for the future development of 2D polymers in perovskite solar cells, potentially accelerating industrialization.

Synergistic Passivation of Bulk and Interfacial Defects Improves Efficiency and Stability of Inverted Perovskite Solar Cells

Defects both in bulk and at the interfaces serve as charge trapping sites for nonradiative recombination and as ion migration pathways, resulting in degradation of perovskite solar cell efficiency and stability. In this work, a strategy for simultaneous passivation of both bulk and interfacial defects is reported. For bulk passivation polystyrene (PS) is used as an additive in the perovskite precursor which reduces the structural defects by forming larger defect‐free grains. While the F‐PEAI cation is used to passivate the interfacial defects, present at both perovskite HTL/ETL interfaces. Furthermore, by conducting control measurements with just bulk modification (PS), just interface modification (F‐PEAI), and a combination of both, the role of individual defect passivation strategies is decoupled. As a result of simultaneous bulk as well as interfacial passivation, the modified perovskite solar cell shows the highest efficiency of 22.32% with a high Voc of 1.14 V and fill factor of 80%. Moreover, the cells have excellent stability retaining 92% and 99% of their initial efficiency after 1008 h and 560 h under ISOS‐ D1 and D2 storage conditions. These results highlight the importance of simultaneous bulk and interfacial passivation for improving solar cell efficiency and stability.

Bimolecular Passivation-Dipole Bridge for Highly Efficient Inverted Perovskite Solar Cells with Low Nonradiative Recombination Loss.

Constructing charge-selective heterointerface with minimized defect state and matched energy level alignment is essential to reduce nonradiative recombination for achieving high-performance perovskite solar cells (PSCs). Herein, a bimolecular passivation-dipole bridge comprised of sodium phenylmethanesulfonate (SPM) and 2-phenylethylammonium iodide (PEAI) is carefully developed to regulate perovskite heterointerface. SPM passivates defect states and upshifts Fermi level (EF) of perovskite surface, and subsequent PEAI further induces additional negative dipole and causes the surface EF of perovskite pinning to negative polaron transport state of electron transport layer PCBM, which significantly promotes electron extraction at the perovskite electron-selective contact. These advantages are confirmed by a remarkably improved efficiency from 21.74% for control to 25.12% for treated PSC with excellent stability. Moreover, corresponding nonradiative recombination loss impressively diminishes from 123 to 70 meV, and charge transport-induced fill factor loss is only 3.00%. This work provides a promising approach via passivation-energetic synergy for engineering perovskite heterointerface toward highly efficient and stable PSCs.