Improvement of Thermal Stability and Photoelectric Performance of Cs2PbI2Cl2/CsPbI2.5Br0.5 Perovskite Solar Cells by Triple-Layer Inorganic Hole Transport Materials.

Conventional hole transport layer (HTL) Spiro-OMeTAD requires the addition of hygroscopic dopants due to its low conductivity and hole mobility, resulting in a high preparation cost and poor device stability. Cuprous thiocyanate (CuSCN) is a cost-effective alternative with a suitable energy structure and high hole mobility. However, CuSCN-based perovskite solar cells (PSCs) are affected by environmental factors, and the solvents of an HTL can potentially corrode the perovskite layer. In this study, a Co3O4/CuSCN/Co3O4 sandwich structure was proposed as an HTL for inorganic Cs2PbI2Cl2/CsPbI2.5Br0.5 PSCs to address these issues. The Co3O4 layers can serve as buffer and encapsulation layers, protecting the perovskite layer from solvent-induced corrosion and enhancing hole mobility at the interface. Based on this sandwich structure, the photovoltaic performances of the Cs2PbI2Cl2/CsPbI2.5Br0.5 PSCs are significantly improved, with the power conversion efficiency (PCE) increasing from 9.87% (without Co3O4) to 11.06%. Furthermore, the thermal stability of the devices is also significantly enhanced, retaining 80% of its initial PCE after 40 h of continuous aging at 60 °C. These results indicate that the Co3O4/CuSCN/Co3O4 sandwich structure can effectively mitigate the corrosion of the perovskite layer by solvents of an HTL and significantly improves the photovoltaic performance and thermal stability of devices.

Fabrication and Characterization of a Lead-Free Cesium Bismuth Iodide Perovskite through Antisolvent-Assisted Crystallization.

Cesium bismuth iodide perovskite material offers good stability toward ambient conditions and has potential optoelectronic characteristics. However, wide bandgap, absorber surface roughness, and poor surface coverage with pinholes are among the key impediments to its adoption as a photovoltaic absorber material. Herein, bandgap modification and the tailoring of surface morphology have been performed through molar ratio variation and antisolvent treatment, whereby type III antisolvent (toluene) based on Hansen space has been utilized. XRD and Raman spectroscopy analyses confirm the formation of a 0D/2D mixed dimensional structure with improved optoelectronic properties when the molar ratio of CsI/BiI3 was adjusted from 1.5:1 to 1:1.5. The absorption results and Tauc plot determination show that the fabricated film has a lower bandgap of 1.80 eV. TRPL analysis reveals that the film possesses a very low charge carrier lifetime of 0.94 ns, suggesting deep defects. Toluene improves the charge carrier lifetime to 1.89 ns. The average grain size also increases from 323.26 nm to 444.3 nm upon toluene addition. Additionally, the inclusion of toluene results in a modest improvement in PCE, from 0.23% to 0.33%.

Anti-Solvent-Free Fabrication of Stable FA0.9Cs0.1PbI3 Perovskite Solar Cells with Efficiency Exceeding 24.0% through a Naphthalene-Based Passivator.

The anti-solvent-free fabrication of high-efficiency perovskite solar cells (PSCs) holds immense significance for the transition from laboratory-scale to large-scale commercial applications. However, the device performance is severely hindered by the increased occurrence of surface defects resulting from the lack of control over nucleation and crystallization of perovskite using anti-solvent methods. In this study, 2-(naphthalen-2-yl)ethylamine hydriodide (NEAI) is employed as the surface passivator for perovskite films without using any anti-solvent. Naphthalene demonstrates strong π-π conjugation, which aids in the efficient extraction of charge carriers. Additionally, the naphthalene-ring moieties form a tight attachment to the perovskite surface. After NEAI treatment, FA and I vacancies are selectively occupied by NEA+ and I- in NEAI respectively, thus effectively passivating the surface defects and isolating the surface from moisture. Ultimately, the optimized NEAI-treated device achieves a promising power conversion efficiency (PCE) of 24.19% (with a certified efficiency of 23.94%), featuring a high fill factor of 83.53%. It stands out as one of the reported high PCEs achieved for PSCs using the spin-coating technique without the need for any anti-solvent so far. Furthermore, the NEAI-treated device can maintain ≈87% of its initial PCE after 2000 h in ambient air with a relative humidity of 30% ± 5%.

Interfacial Engineering for Efficient Low-Temperature Flexible Perovskite Solar Cells.

Photovoltaic technology with low weight, high specific power in cold environments, and compatibility with flexible fabrication is highly desired for near-space vehicles and polar region applications. Herein, we demonstrate efficient low-temperature flexible perovskite solar cells by improving the interfacial contact between electron-transport layer (ETL) and perovskite layer. We find that the adsorbed oxygen active sites and oxygen vacancies of flexible tin oxide (SnO2 ) ETL layer can be effectively decreased by incorporating a trace amount of titanium tetrachloride (TiCl4 ). The effective defects elimination at the interfacial increases the electron mobility of flexible SnO2 layer, regulates band alignment at the perovskite/SnO2 interface, induces larger perovskite crystal growth, and improves charge collection efficiency in a complete solar cell. Correspondingly, the improved interfacial contact transforms into high-performance solar cells under one-sun illumination (AM 1.5G) with efficiencies up to 23.7 % at 218 K, which might open up a new era of application of this emerging flexible photovoltaic technology to low-temperature environments such as near-space and polar regions.

Mixed-Cation Halide Perovskite Doped with Rb+ for Highly Efficient Photodetector.

Photodetectors are widely employed as fundamental devices in optical communication, automatic control, image sensors, night vision, missile guidance, and many other industrial or military fields. Mixed-cation perovskites have emerged as promising optoelectronic materials for application in photodetectors due to their superior compositional flexibility and photovoltaic performance. However, their application involves obstacles such as phase segregation and poor-quality crystallization, which introduce defects in perovskite films and adversely affect devices' optoelectronic performance. The application prospects of mixed-cation perovskite technology are significantly constrained by these challenges. Therefore, it is necessary to investigate strategies that combine crystallinity control and defect passivation to obtain high-quality thin films. In this study, we incorporated different Rb+ ratios in triple-cation (CsMAFA) perovskite precursor solutions and studied their effects on crystal growth. Our results show that a small amount of Rb+ was enough to induce the crystallization of the α-FAPbI3 phase and suppress the formation of the yellow non-photoactive phase; the grain size increased, and the product of the carrier mobility and the lifetime (µτ) improved. As a result, the fabricated photodetector exhibited a broad photo-response region, from ultraviolet to near-infrared, with maximum responsivity (R) up to 11.8 mA W-1 and excellent detectivity (D*) values up to 5.33 × 1011 Jones. This work provides a feasible strategy to improve photodetectors' performance via additive engineering.

Highly Efficient 2D/3D Mixed-Dimensional Cs2PbI2Cl2/CsPbI2.5Br0.5 Perovskite Solar Cells Prepared by Methanol/Isopropanol Treatment.

All-inorganic perovskite solar cells are attractive photovoltaic devices because of their excellent optoelectronic performance and thermal stability. Unfortunately, the currently used efficient inorganic perovskite materials can spontaneously transform into undesirable phases without light-absorption properties. Studies have been carried out to stabilize all-inorganic perovskite by mixing low-dimensional perovskite. Compared with organic two-dimensional (2D) perovskite, inorganic 2D Cs2PbI2Cl2 shows superior thermal stability. Our group has successfully fabricated 2D/3D mixed-dimensional Cs2PbI2Cl2/CsPbI2.5Br0.5 films with increasing phase stability. The high boiling point of dimethyl sulfoxide (DMSO) makes it a preferred solvent in the preparation of Cs2PbI2Cl2/CsPbI2.5Br0.5 inorganic perovskite. When the perovskite films are prepared by the one-step solution method, it is difficult to evaporate the residual solvent molecules from the prefabricated films, resulting in films with rough surface morphology and high defect density. This study used the rapid precipitation method to control the formation of perovskite by treating it with methanol/isopropanol (MT/IPA) mixed solvent to produce densely packed, smooth, and high-crystallized perovskite films. The bulk defects and the carrier transport barrier of the interface were effectively reduced, which decreased the recombination of the carriers in the device. As a result, this effectively improved photoelectric performance. Through treatment with MT/IPA, the photoelectric conversion efficiency (PCE) of solar cells prepared in the N2 atmosphere increased from 13.44% to 14.10%, and the PCE of the device prepared in the air increased from 3.52% to 8.91%.

A 0D Additive for Flexible All-Inorganic Perovskite Solar Cells to Go Beyond 60 000 Flexible Cycles.

All-inorganic cesium lead halide flexible perovskite solar cells (f-PSCs) exhibit superior thermal stability compared to their organic-inorganic hybrid counterparts. However, their flexibility and efficiency are still below-par for practical viability. Herein, a design using a 0D Cs4 Pb(IBr)6 additive to transform tensile stress into compressive stress in the perovskite film, effectively preventing expansion of cracks for significantly improved mechanical durability, is reported. It is found that not only is improved flexibility obtained, but also the cell efficiency is increased for the all-inorganic flexible 3D CsPbI3- x Brx solar cells. The CsPbI2.81 Br0.19 f-PSC retains over 97% of its initial efficiency even after 60 000 flexing cycles at a curvature radius of 5 mm (R = 5 mm). Simultaneously, 0D Cs4 Pb(IBr)6 enhances the crystallinity of the CsPbI2.81 Br0.19 film and passivates the defects along the grain boundaries, effectively improving the photovoltaic performance of the all-inorganic f-PSCs. The highest power-conversion efficiency obtained is 14.25% with a short-circuit current density of 18.47 mA cm-2 , open-circuit voltage of 1.09 V, and fill factor of 70.67%. This strategy paves the way for further improvement of the mechanical durability of all-inorganic f-PSCs.

Stabilization of FAPbI3 with Multifunctional Alkali-Functionalized Polymer.

The defects located at the interfaces and grain boundaries (GBs) of perovskite films are detrimental to the photovoltaic performance and stability of perovskite solar cells. Manipulating the perovskite crystallization process and tailoring the interfaces with molecular passivators are the main effective strategies to mitigate performance loss and instability. Herein, a new strategy is reported to manipulate the crystallization process of FAPbI3 -rich perovskite by incorporating a small amount of alkali-functionalized polymers into the antisolvent solution. The synergic effects of the alkali cations and poly(acrylic acid) anion effectively passivate the defects on the surface and GBs of perovskite films. As a result, the rubidium (Rb)-functionalized poly(acrylic acid) significantly improves the power conversion efficiency of FAPbI3 perovskite solar cells to approaching 25% and reduces the risk of lead ion (Pb2+ ) leakage continuously via the strong interaction between CO bonds and Pb2+ . In addition, the unencapsulated device shows enhanced operational stability, retaining 80% of its initial efficiency after 500 h operation at maximum power point under one-sun illumination.

Dopant-free NiOx Nanocrystals: A Low-cost and Stable Hole Transport Material for Commercializing Perovskite Optoelectronics.

Advancing inverted (p-i-n) perovskite solar cells (PSCs) is critical for commercial applications given their compatibility with different bottom cells for tandem photovoltaics, low-temperature processability (≤100 °C), and promising operational stability. Although inverted PSCs have achieved an efficiency of over 25 % using doped or expensive organic hole transport materials (HTMs), their synthesis cost and stability still cannot meet the requirements for their commercialization. Recently, dopant-free and low-cost non-stoichiometric nickel oxide nanocrystals (NiOx NCs) have been extensively studied as a low-cost and effective HTM in perovskite optoelectronics. In this minireview, we summarize the synthesis and surface-functionalization methods of NiOx NCs. Then, the applications of NiOx NCs in other perovskite optoelectronics beyond photovoltaics are discussed. Finally, we provide a perspective for the future development of NiOx NCs for the commercialization of perovskite optoelectronics.

Dye-Sensitized Solar Cell Based on TiO2 Anode Thin Film with Three-Dimensional Web-like Structure.

TiO2 films with a three-dimensional web-like porous structure were prepared using the photo polymerization-induced phase separation method integrated with the pulling coating process. By adjusting the ratio of the substance in the precursor sol and the coating times, the relationships between the sol ratio, the coating times, the film structure, and the performance of the DSC were studied. The optimal film structure was found and a detailed description is given. The performance of the DSC was further improved by introducing the barrier layer and the surface-modified layer of the TiO2 coating. This promoted the short-circuit current density and the photoelectric conversion efficiency of the DSC, the mechanism of which was also investigated. Ultimately, the photoelectric conversion efficiency of the DSC based on the TiO2 anode films with a three-dimensional web-like structure was stabilized at a higher level as a result of the structural improvement.

Two-Dimensional Cs3Sb2I9-xClx Film with (201) Preferred Orientation for Efficient Perovskite Solar Cells.

All-inorganic Sb-perovskite has become a promising material for solar cell applications owing to its air stability and nontoxic lead-free constitution. However, the poor morphology and unexpected (001) orientation of Sb-based perovskite films strongly hinder the improvement of efficiency. In this work, two-dimensional Cs3Sb2ClxI9-x with (201) preferred orientation has been successfully fabricated by introducing thiourea (TU) to the precursor solution. The presence of the C=S functional group in TU regulates the crystallization dynamics of Cs3Sb2I9-xClx films and generates the (201) preferred orientation of Cs3Sb2ClxI9-x films, which could effectively improve the carrier transport and film morphology. As a result, the Cs3Sb2I9-xClx perovskite solar cells (PSCs) delivered a power conversion efficiency (PCE) of 2.22%. Moreover, after being stored in nitrogen at room temperature for 60 days, the devices retained above 87.69% of their original efficiency. This work demonstrates a potential pathway to achieve high-efficiency Sb-based PSCs.

0D/2D Mixed Dimensional Lead-Free Caesium Bismuth Iodide Perovskite for Solar Cell Application.

Bismuth-based perovskites are potentially a promising alternative for lead-free perovskites. During bond formation, however, trivalent ions on Cs3Bi2I9 with CsI/BiI3 ratio of 1.5/1 form 0D-neutral charged compounds with higher bandgap (>2.0 eV) and poor absorption capacity. Mixed 0/2-dimensional structures are potentially suitable substitutes due to their low bandgap. So far, the reported CsI/BiI3 ratios for 0D/2D structures are 1:1, 1:2 and 1:3. Herein, a new ratio of 1/1.5 is reported. Caesium bismuth iodide at a ratio of CsI/BiI3 of 1/1.5 was synthesised using a one-step processing method with/without solvent vapour annealing. During solvent annealing, a 1/4 (v/v) mixture of DMF/methanol was used as a solvent. The crystal structure formed at a ratio of 1/1.5 is more similar to 1.5/1 than to 1/3. The XRD pattern revealed additional characteristics peaks at 009, 012, 209 and 300, indicating the growth of another phase. The formed heterogeneous mixed 0D/2D structure has an extended light absorption capacity greater than 720 nm. Solvent vapour annealing improved film morphology by enhancing grain size and packing density. When cells with and without solvent vapour annealing are compared, the power conversion efficiency of caesium bismuth iodide increases from 0.26% without solvent annealing to 0.98% with solvent vapour annealing. This study establishes a new route for future research on crystal configuration, nomenclature, film and morphology, quality tailoring and applications toward the goal of lead-free perovskite solar cells.

A descriptor for the structural stability of organic-inorganic hybrid perovskites based on binding mechanism in electronic structure.

The poor stability of organic-inorganic hybrid perovskites hinders its commercial application, which motivates a need for greater theoretical insight into its binding mechanism. To date, the binding mode of organic cation and anion inside organic-inorganic hybrid perovskites is still unclear and even contradictory. Therefore, in this work based on density functional theory (DFT), the binding mechanism between organic cation and anion was systematically investigated through electronic structure analysis including an examination of the electronic localization function (ELF), electron density difference (EDD), reduced density gradient (RDG), and energy decomposition analysis (EDA). The binding strength is mainly determined by Coulomb effect and orbital polarization. Based on the above analysis, a novel 2D linear regression descriptor that Eb = - 9.75Q2/R0 + 0.00053 V∙EHL - 6.11 with coefficient of determination R2 = 0.88 was proposed to evaluate the binding strength (the units for Q, R0, V, and EHL are |e|, Å, bohr3, and eV, respectively), revealing that larger Coulomb effect (Q2/R0), smaller volume of perovskite (V), and narrower energy difference (EHL) between the lowest unoccupied molecular orbital (LUMO) of organic cation and the highest occupied molecular orbital (HOMO) of anion correspond to the stronger binding strength, which guides the design of highly stable organic-inorganic hybrid perovskites.

Exploring the Effects of Ionic Defects on the Stability of CsPbI3 with a Deep Learning Potential.

Inorganic metal halide perovskites, such as CsPbI3 , have recently drawn extensive attention due to their excellent optical properties and high photoelectric efficiencies. However, the structural instability originating from inherent ionic defects leads to a sharp drop in the photoelectric efficiency, which significantly limits their applications in solar cells. The instability induced by ionic defects remains unresolved due to its complicated reaction process. Herein, to explore the effects of ionic defects on stability, we develop a deep learning potential for a CsPbI3 ternary system based upon density functional theory (DFT) calculated data for large-scale molecular dynamics (MD) simulations. By exploring 2.4 million configurations, of which 7,730 structures are used for the training set, the deep learning potential shows an accuracy approaching DFT-level. Furthermore, MD simulations with a 5,000-atom system and a one nanosecond timeframe are performed to explore the effects of bulk and surface defects on the stability of CsPbI3 . This deep learning potential based MD simulation provides solid evidence together with the derived radial distribution functions, simulated diffraction of X-rays, instability temperature, molecular trajectory, and coordination number for revealing the instability mechanism of CsPbI3 . Among bulk defects, Cs defects have the most significant influence on the stability of CsPbI3 with a defect tolerance concentration of 0.32 %, followed by Pb and I defects. With regards to surface defects, Cs defects have the largest impact on the stability of CsPbI3 when the defect concentration is less than 15 %, whereas Pb defects act play a dominant role for defect concentrations exceeding 20 %. Most importantly, this machine-learning-based MD simulation strategy provides a new avenue to explore the ionic defect effects on the stability of perovskite-like materials, laying a theoretical foundation for the design of stable perovskite materials.

High throughput screening of promising lead-free inorganic halide double perovskites via first-principles calculations.

Perovskite solar cells (PSCs) have been intensively investigated and made great progress due to their high photoelectric conversion efficiency and low production cost. However, poor stability and the toxicity of Pb limit their commercial applications. It is particularly important to search for new non-toxic, high-stability perovskite materials. In this study, 760 Cs2B2+B'2+X6 (X = F, Cl, Br, I) inorganic halide double perovskites are screened based on high-throughput first-principles calculations to obtain an ideal perovskite material. The band gaps of this type of double perovskite are mainly determined by the elements X and B2+, decreasing monotonously with the increase in the atomic number of X (from F to I). We obtain 14 optimal and unreported materials with suitable band gaps as potential alternative materials for Pb-based photovoltaic absorbers in PSCs. This theoretical investigation can provide theoretical guidance for developing novel lead-free PSC materials.

Unraveling Passivation Mechanism of Imidazolium-Based Ionic Liquids on Inorganic Perovskite to Achieve Near-Record-Efficiency CsPbI2Br Solar Cells.

The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells (PSCs). However, the detailed mechanisms behind the improvement remain mysterious. Herein, a series of imidazolium-based ionic liquids (IILs) with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites. It is found that IILs display the following advantages: (1) They form ionic bonds with Cs+ and Pb2+ cations on the surface and at the grain boundaries of perovskite films, which could effectively heal/reduce the Cs+/I- vacancies and Pb-related defects; (2) They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer; and (3) They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI2Br PSCs. The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI2Br PSCs and an impressive power conversion efficiency of 17.02%. Additionally, the CsPbI2Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability. Our results provide guidance for an in-depth understanding of the passivation mechanism of IILs in inorganic perovskites.

A new perspective for evaluating the photoelectric performance of organic-inorganic hybrid perovskites based on the DFT calculations of excited states.

The high efficiency of organic-inorganic hybrid perovskites has attracted the attention of many scholars all over the world, the chemical formula of which is ABX3, where A is an organic cation, B is a metal cation, and X is a halogen ion. In addition, the micro-mechanism behind the efficient photoelectric conversion needs more in-depth exploration. Therefore, in this work, based on time-dependent density functional theory (TD-DFT), the electron transfer mechanism from the ground state to the first singlet excited state was systematically investigated by electron and hole analysis and an inter-fragment charge transfer amount method (IFCT). In this work, we optimized and analyzed 99 different perovskite cluster configurations, where A sites are CH3NH3+ (MA+), NH2CHNH2+ (FA+), CH3CH2NH3+ (EA+), NH2CHOH+ (JA+), NH3OH+ (BA+), N(CH3)4+ (DA+), CH3CH2CH2NH3+ (KB+), CH3CH2CH2CH2NH3+ (KC+), C3N2H5+ (RA+), CH(CH3)2+ (TA+), and CH3NH(CH3)2+ (UA+), B sites are Ge2+, Sn2+ and Pb2+, and X sites are Cl-, Br- and I-. According to the analysis of a series of perovskite clusters of the hole-electron distribution, the distribution is mainly concentrated on BX, and electrons and holes are respectively distributed on B and X sites. The exciton binding energy decreases when the metal element changes from Ge to Pb and the halogen element changes from Cl to I. A radar chart including the exciton binding energy, excited energy, amount of net charge transfer, electron and hole overlap index, distance between the centroid of holes and electrons, and the hole and electron separation index was proposed to intuitively describe the electron transmission characteristics of perovskites. Based on that, a comprehensive score index was innovatively proposed to evaluate the photoelectric property of perovskites, providing foundational guidance for the design of high-efficiency organic-inorganic hybrid perovskites.

An in-situ defect passivation through a green anti-solvent approach for high-efficiency and stable perovskite solar cells.

Surface and grain boundary defects in halide perovskite solar cells are highly detrimental, reducing efficiencies and stabilities. Widespread halide anion and organic cation defects usually aggravate ion diffusion and material degradation on the surfaces and at the grain boundaries of perovskite films. In this study, we employ an in-situ green method utilizing nontoxic cetyltrimethylammonium chloride (CTAC) and isopropanol (IPA) as anti-solvents to effectively passivate both surface and grain boundary defects in hybrid perovskites. Anion vacancies can be readily passivated by the chloride group due to its high electronegativity, and cation defects can be synchronously passivated by the more stable cetyltrimethylammonium group. The results show that the charge trap density was significantly reduced, while the carrier recombination lifetime was markedly extended. As a result, the power conversion efficiency of the cell can reach 23.4% with this in-situ green method. In addition, the device retains 85% of its original power conversion efficiency after 600 h of operation under illumination, showing that the stability of perovskite solar cells is improved with this in-situ passivation strategy. This work may provide a green and effective route to improve both the stability and efficiency of perovskite solar cells.

Non-stoichiometric molybdenum sulfide clusters and their reactions with the hydrogen molecule.

Structures of non-stoichiometric MoxSy clusters (x = 2-4; y = 2-10) were studied by density functional calculations with global optimization. Besides 1T phase like structures, a novel regular grid structure in which Mo atoms are well separated by S atoms was found, which might be used as a building-block to construct a new type of two-dimensional molybdenum sulfide monolayer. The hydrogen molecule prefers to be adsorbed onto Mo atoms rather than S atoms, and Mo atoms with less S coordination have a higher ability to adsorb H2. In addition, the reaction pathways for H2 dissociation were studied on two clusters with the highest H2 adsorption energy (Mo2S4 and Mo3S3). The vacant bridge site of Mo-Mo in S-deficient clusters, which corresponds to the sulfur vacancy in the bulk phase MoS2, is favored by H atom adsorption and plays an important role in the H atom transfer on MoxSy clusters. Our results provide a new aspect to understand the reason why S defect in MoS2 and MoS2 with an Mo-edge could enhance the catalytic performance in the hydrogen evolution reaction.

High Performance Tandem Solar Cells with Inorganic Perovskite and Organic Conjugated Molecules to Realize Complementary Absorption.

All-inorganic halide perovskite solar cells (PerSCs) have achieved rapid development in recent years. However, limited by narrow absorption bands, the power conversion efficiency (PCE) of all-inorganic halide PerSCs lag behind the organic-inorganic hybrid ones. In this contribution, to expand their absorption spectra and enhance the PCE, tandem solar cells (TSCs) with inorganic perovskite and organic conjugated molecules are constructed, utilizing CsPbI2Br as an ultraviolet-visible light absorber and a PTB7-Th:IEICO-4F bulk-heterojunction (BHJ) active layer as a near-infrared light absorber. To physically and electronically connect the front and rear subcells, P3HT/MoO3/Ag/PFN-Br is introduced as an interconnecting junction. Finally, the TSCs exhibit a remarkably higher PCE of 17.24% compared to that of the single junction PerSCs (12.09%) and organic solar cells (OSCs) (10.89%). These results indicate that the combination of all-inorganic perovskite and a low bandgap organic active layer for TSCs is a feasible approach to realize broad spectra utilization and efficiency enhancement.