Hierarchical Nanostructures CuBi2O4 Integrated with Polyaniline Nanofibrous for Boosting Hole Extraction in Carbon-Based Perovskite Solar Cells.

Toward commercialization of carbon-based perovskite solar cells (C-PSCs), it is crucial to innovatively design inorganic hole transport layer materials that excel in extracting and transporting charge carriers to promote their photoelectric conversion efficiency (PCE). In this work, a novel and high-connectivity CuBi2O4-polyaniline nanofibrous (CuBi2O4-PN) reticular structure is created by integrating CuBi2O4 hierarchical microspheres (CuBi2O4 MS) with polyaniline nanofibrous. The introduction of CuBi2O4-PN as a hole transport layer (HTL) notably enhances the contact quality of the devices and substantially reduces the surface defects of C-PSCs. In a comparative analysis under identical experimental conditions, MAPbI3 devices incorporating CuBi2O4-PN HTL demonstrated a PCE of 14.79%, achieving a 44.3% increase over the reference device (10.25%). CuBi2O4-treated C-PSCs retained 89.9% of their original PCE after 45 days in storage, and they demonstrated improved stability over a longer time frame. This remarkable improvement in device performance can be attributed to the effective suppression of nonradiative recombination and the enhancement of the carrier transfer process in the device. Additionally, the unique interconnected reticular structure of CuBi2O4-PN provides efficient pathways for hole transfer, significantly contributing to the enhanced efficiency of the device.

Unraveling Differences in the Effects of Ammonium/Amine-Based Additives on the Performance and Stability of Inverted Perovskite Solar Cells.

Additive engineering, with its excellent ability to passivate bulk or surface perovskite defects, has become a common strategy to improve the performance and stability of perovskite solar cells (PVSCs). Among the various additives reported so far, ammonium salts are considered an important branch. It is worth noting that although both ammonium-based additives (R-NH3 +) and amine-based additives (R-NH2) are derivatives of ammonia (NH3), the functions of the two can be easily confused due to their structural similarities. Moreover, there is no comprehensive comparative analysis of them in the literature. Here, the differences between phenethylammonium iodide (PEA+) and phenethylamine (PEA) additives are revealed experimentally and theoretically. The results clearly show that PEA outperforms PEA+ in terms of device performance and stability based on the following three factors: i) PEA's defect passivation capability is superior to that of PEA+; ii) PEA has better hydrophobicity to hinder water ingress; and iii) PEA completely improves the stability of PVSCs by enhancing thermal stability and inhibiting iodide migration in perovskite more effectively than PEA+. As a result, the power conversion efficiency (PCE) of the inverted methylammonium triiodide (MAPbI3) device using PEA increases by ≈15% to over 21%. More importantly, this device exhibits greater ability to prevent water invasion, thermal-induce degradation, and inhibit iodide ion migration, resulting in better long-term stability.

Long-Term Comparisons of Photoluminescence Affected by Organic Cations of Formamidinium and Methylammonium in Monophasic Lead Iodide Perovskite Quantum Dots.

This study compared the photoluminescence (PL) stabilities of formamidinium (FA) and methylammonium (MA) in lead iodide perovskite quantum dots (QDs). To exclude other factors, such as size and purity, that may affect stability, MAPbI3 and FAPbI3 QDs with nearly identical sizes (~10.0 nm) were synthesized by controlling the ligand concentration and synthesis temperature. Transmission electron microscopy images and X-ray diffraction patterns confirmed homogeneous single-phase perovskite structures. Additionally, the bandgaps and sizes of the synthesized QDs closely matched those of the infinite quantum well model, which guaranteed that the photostability was solely caused by the different organic molecules in the two QDs. We analyzed the PL peak centers and full-width at half maximum of the QDs for 32 days. The enhanced stability of FAPbI3 was found to be caused by the nearly zero redshift (1.615 eV) of its PL peak, in contrast to the redshift (1.685→1.670 eV) of MAPbI3.

Interface Passivation of a Pyridine-Based Bifunctional Molecule for Inverted Perovskite Solar Cells.

Organic-inorganic hybrid perovskite solar cells (PSCs) have recently been demonstrated to be promising renewable harvesters because of their prominent photovoltaic power conversion efficiency (PCE), although their stability and efficiency still have not reached commercial criteria. Trouble-oriented analyses showcase that defect reduction among the grain boundaries and interfaces in the prepared perovskite polycrystalline films is a practical strategy, which has prompted researchers to develop functional molecules for interface passivation. Herein, the pyridine-based bifunctional molecule dimethylpyridine-3,5-dicarboxylate (DPDC) was employed as the interface between the electron-transport layer and perovskite layer, which achieved a champion PCE of 21.37% for an inverted MAPbI3-based PSC, which was greater than 18.64% for the control device. The mechanistic studies indicated that the significantly improved performance was mainly attributed to the remarkably enhanced fill factor with a value greater than 83%, which was primarily due to the nonradiative recombination suppression offered by the passivation effect of DPDC. Moreover, the promoted carrier mobility together with the enlarged crystal size contributed to a higher short-circuit current density. In addition, an increase in the open-circuit voltage was also observed in the DPDC-treated PSC, which benefited from the improved work function for reducing the energy loss during carrier transport. Furthermore, the DPDC-treated PSC showed substantially enhanced stability, with an over 80% retention rate of its initial PCE value over 300 h even at a 60% relative humidity level, which was attributed to the hydrophobic nature of the DPDC molecule and effective defect passivation. This work is expected not only to serve as an effective strategy for using a pyridine-based bifunctional molecule to passivate perovskite interfaces to enhance photovoltaic performance but also to shed light on the interface passivation mechanism.

Enhanced Piezoelectricity of MAPbI3 by the Introduction of MXene and Its Utilization in Boosting High-Performance Photodetectors.

Recently, perovskite photodetectors (PDs) are risen to prominence due to substantial research interest. Beyond merely tweaking the composition of materials, a cutting-edge advancement lies in leveraging the innate piezoelectric polarization properties of perovskites themselves. Here, the investigation shows utilizing Ti3C2Tx, a typical MXene, as an intermediate layer for significantly boosting the piezoelectric property of MAPbI3 thin films. This improvement is primarily attributed to the enhanced polarization of the methylammonium (MA+) groups within MAPbI3, induced by the OH groups present in Ti3C2Tx. A flexible PD based on the MAPbI3/MXene heterostructure is then fabricated. The new device is sensitive to a wide range of wavelengths, displays greatly enhanced performance owing to the piezo-phototronic coupling. Moreover, the device is endowed with a greatly reduced response time, down to millisecond level, through the pyro-phototronic effect. The characterization shows applying a -1.2% compressive strain on the PD leads to a remarkable 102% increase in the common photocurrent, and a 76% increase in the pyro-phototronic current. The present work reveals how the emerging piezo-phototronic and pyro-phototronic effects can be employed to design high-performance flexible perovskite PDs.

Interface engineering and defect passivation for enhanced hole extraction, ion migration, and optimal charge dynamics in both lead-based and lead-free perovskite solar cells.

The study elucidates the potential benefits of incorporating a BiI3 interfacial layer into perovskite solar cells (PSCs). Using MAPbI3 and MAGeI3 as active layers, complemented by the robust TiO2 and Spiro-OMeTAD as the charge-transport-layers, we employed the SCAPS-1D simulation tool for our investigations. Remarkably, the introduction of the BiI3 layer at the perovskite-HTL interface significantly enhanced hole extraction and effectively passivated defects. This approach minimized charge recombination and ion migration towards opposite electrodes, thus elevating device performance relative to conventional configurations. The efficiency witnessed a rise from 19.28 to 20.30% for MAPbI3 and from 11.90 to 15.57% for MAGeI3. Additionally, MAGeI3 based PSCs saw an improved fill-factor from 50.36 to 62.85%, and a better Jsc from 13.22 to 14.2 mA/cm2, signifying reduced recombination and improved charge extraction. The FF for MAPbI3 based PSCs saw a minor decline, while the Voc slightly ascended from 1.24 to 1.25 V and Jsc from 20.01 to 21.6 mA/cm2. A thorough evaluation of layer thickness, doping, and temperature further highlighted the critical role of the BiI3 layer for both perovskite variants. Our examination of bandgap alignments in devices with the BiI3 interfacial layer also offers valuable understanding into the mechanisms fueling the observed improvements.

PbS Quantum Dots Ink with Months-Long Shelf-Lifetime Enabling Scalable and Efficient Short-Wavelength Infrared Photodetectors.

The phase-transfer ligand exchange of PbS quantum dots (QDs) has substantially simplified device fabrication giving hope for future industrial exploitation. However, this technique when applied to QDs of large size (>4 nm) gives rise to inks with poor colloidal stability, thus hindering the development of QDs photodetectors in short-wavelength infrared range. Here, it is demonstrated that methylammonium lead iodide ligands can provide sufficient passivation of PbS QDs of size up to 6.7 nm, enabling inks with a minimum of ten-week shelf-life time, as proven by optical absorption and solution-small angle X-ray scattering. Furthermore, the maximum linear electron mobility of 4.7 × 10-2 cm2 V-1 s-1 is measured in field-effect transistors fabricated with fresh inks, while transistors fabricated with the same solution after ten-week storage retain 74% of the average starting electron mobility, demonstrating the outstanding quality both of the fresh and aged inks. Finally, photodetectors fabricated via blade-coating exhibit 76% external quantum efficiency at 1300 nm and 1.8 × 1012 Jones specific detectivity, values comparable with devices fabricated using ink with lower stability and wasteful methods such as spin-coating.

Strengthened Interficial Adhesive Fracture Energy by Young's Modulus Matching Degree Strategy in Carbon-Based HTM Free MAPbI3 Perovskite Solar Cell with Enhanced Mechanical Compatibility.

Carbon-based hole transport layer-free perovskite solar cells (PSCs) based on methylammonium lead triiodide (MAPbI3 ) have become one of the research focus due to low cost, easy preparation, and good optoelectronic properties. However, instability of perovskite under vacancy defects and stress-strain makes it difficult to achieve high-efficiency and stable power output. Here, a soft-structured long-chain 2D pentanamine iodide (abbreviated as "PI") is used to improve perovskite quality and interfacial mechanical compatibility. PI containing CH3 (CH2 )4 NH3 + and I- ions not only passivate defects at grain boundaries, but also effectively alleviate residual stress during high temperature annealing via decreasing Young's modulus of perovskite film. Most importantly, PI effectively increases matching degree of Young's modulus between MAPbI3 (47.1 GPa) and carbon (6.7 GPa), and strengthens adhesive fracture energy (Gc ) between perovskite and carbon, which is helpful for outward release of nascent interfacial stress generated under service conditions. Consequently, photoelectric conversion efficiency (PCE) of optimal device is enhanced from 10.85% to 13.76% and operational stability is also significantly improved. 83.1% output is maintained after aging for 720 h at room temperature and 25-60% relative humidity (RH). This strategy of regulation from chemistry and physics provides a strategy for efficient and stable carbon-based PSCs.

Role of Surface Features on the Initial Dissolution of CH3NH3PbI3 Perovskite in Liquid Water: An Ab Initio Molecular Dynamics Study.

The degradation of CH3NH3PbI3 (MAPbI3) hybrid organic inorganic perovskite (HOIP) by water has been the major issue hampering its use in commercial perovskites solar cells (PSCs), as MAPbI3 HOIP has been known to easily degrade in the presence of water. Even though there have been numerous studies investigating this phenomenon, there is still no consensus on the mechanisms of the initial stages of dissolution. Here, we attempt to consolidate differing mechanistic interpretations previously reported in the literature through the use of the first-principles constrained ab initio molecular dynamics (AIMD) to study both the energetics and mechanisms that accompany the degradation of MAPbI3 HOIP in liquid water. By comparing the dissolution free energy barrier between surface species of different surficial types, we find that the dominant dissolution mechanisms of surface species vary widely based on the specific surface features. The high sensitivity of the dissolution mechanism to surface features has contributed to the many dissolution mechanisms proposed in the literature. In contrast, the dissolution free energy barriers are mainly determined by the dissolving species rather than the type of surfaces, and the type of surfaces the ions are dissolving from is inconsequential toward the dissolution free energy barrier. However, the presence of surface defects such as vacancy sites is found to significantly lower the dissolution free energy barriers. Based on the estimated dissolution free energy barriers, we propose that the dissolution of MAPbI3 HOIP in liquid water originates from surface defect sites that propagate laterally along the surface layer of the MAPbI3 HOIP crystal.

Effect of Cs+ Doping on the Carrier Dynamics of MAPbI3 Perovskite.

Organic inorganic perovskite materials have received increasing attention in the optoelectronic field because of their unique properties. The ultrafast dynamics of photogenerated carriers determine photoelectric conversion efficiency, thus, it is feasible to influence the dynamics behavior of photogenerated carriers by regulating A-site cations. This paper mainly used transient absorption spectra (TAS) technology to study the photogenerated carriers relaxation processes of organic-inorganic perovskite CsxMA1-xPbI3 materials at different x values. Three sets of time constants were obtained by global fitting at different values of x. The experimental results showed that the crystal structure of perovskite could be affected by adjusting the Cs+ doping amount, thereby regulating the carrier dynamics. The appropriate amount of A-cation doping not only maintained the organic-inorganic perovskite crystal phase, but also prolonged the photogenerated carrier's lifetime. The 10% Cs+ doping CsxMA1-xPbI3 perovskite has potential for solar cell applications. We hope that our research can provide dynamics support for the development of organic-inorganic perovskite in solar cells.

Controllable Colloidal Synthesis of MAPbI3 Perovskite Nanocrystals for Dual-Mode Optoelectronic Applications.

This study demonstrates an acetate ligand (AcO-)-assisted strategy for the controllable and tunable synthesis of colloidal methylammonium lead iodide (MAPbI3) perovskite nanocrystals (PNCs) for efficient photovoltaic and photodetector devices. The size of colloidal MAPbI3 PNCs can be tuned from 9 to 20 nm by changing the AcO-/MA ratio in the reaction precursor. In situ observations and detailed characterization results show that the incorporation of the AcO- ligand alters the formation of PbI6 octahedral cages, which controls PNC growth. A well-optimized AcO-/MA ratio affords MAPbI3 PNCs with a low defect density, a long carrier lifetime, and unique solid-state isotropic properties, which can be used to fabricate solution-processed dual-mode photovoltaic and photodetector devices with a conversion efficiency of 13.34% and a detectivity of 2 × 1011 Jones, respectively. This study provides an avenue to further the precisely controllable synthesis of hybrid PNCs for multifunctional optoelectronic applications.

Multifunctional Thiophene Cascading SnO2/Perovskite Interfaces for Efficient and Stable MAPbI3 Photovoltaics.

The power conversion efficiency (PCE) and stability of n-i-p perovskite solar cells (PSCs) are significantly affected by inherent defects of SnO2 and perovskite layers. In this work, we incorporate 2-bromo-3-thiophenic acid (BrThCOOH) as a multifunctional passivant to simultaneously passivate the defects of SnO2 surface and perovskite layer. BrThCOOH permeates evenly into the MAPbI3 and coordinates with Pb2+ and iodine vacancies (VI+) to reduce surface defect density and inhibit the decomposition of MAPbI3. Carboxylic acid effectively passives the oxygen vacancy on the surface of SnO2 through coordination bonds, reducing the probability of electron capture by SnO2 surface defects, thus contributing to electron transport in device. The interaction of BrThCOOH with MAPbI3 and SnO2 surfaces leads to an upward shift in energy levels, reducing energy loss during charge migration. The optimal MAPbI3 device with BrThCOOH-modified SnO2 (T-SnO2) reveals an improved PCE of 21.12%, much higher than that of the control one (19.12%). The hydrophobicity of BrThCOOH-modified MAPbI3 is also improved, which is beneficial to the durability of the device. After 100 h of storage in the environment, the generated PSCs maintain their initial PCE of 75%, demonstrating excellent long-term stability without any encapsulation.

Promoting Photocatalytic H2 Evolution through Retarded Charge Trapping and Recombination by Continuously Distributed Defects in Methylammonium Lead Iodide Perovskite.

Inspired by its great success in the photovoltaic field, methylammonium lead iodide perovskite (MAPbI3 ) has recently been actively explored as photocatalysts in H2 evolution reactions. However, the practical application of MAPbI3 photocatalysts remains hampered by the intrinsically fast trapping and recombination of photogenerated charges. Herein, we propose a novel strategy of regulating the distribution of defective areas to promote charge-transfer dynamics of MAPbI3 photocatalysts. By deliberately designing and synthesizing the MAPbI3 photocatalysts featuring a unique continuation of defective areas, we demonstrate that such a feature enables retardation of charge trapping and recombination via lengthening the charge-transfer distance. As an outcome, such MAPbI3 photocatalysts turn out to achieve an impressive photocatalytic H2 evolution rate as high as 0.64 mmol ⋅ g-1 ⋅ h-1 , one order of magnitude higher than that of the conventional MAPbI3 photocatalysts. This work establishes a new paradigm for controlling charge-transfer dynamics in photocatalysis.

Direct Nanoscale Visualization of the Electric-Field-Induced Aging Dynamics of MAPbI3 Thin Films.

Perovskite solar cells represent the most attractive emerging photovoltaic technology, but their practical implementation is limited by solar cell devices' low levels of operational stability. The electric field represents one of the key stress factors leading to the fast degradation of perovskite solar cells. To mitigate this issue, one must gain a deep mechanistic understanding of the perovskite aging pathways associated with the action of the electric field. Since degradation processes are spatially heterogeneous, the behaviors of perovskite films under an applied electric field should be visualized with nanoscale resolution. Herein, we report a direct nanoscale visualization of methylammonium (MA+) cation dynamics in methylammonium lead iodide (MAPbI3) films during field-induced degradation, using infrared scattering-type scanning near-field microscopy (IR s-SNOM). The obtained data reveal that the major aging pathways are related to the anodic oxidation of I- and the cathodic reduction of MA+, which finally result in the depletion of organic species in the channel of the device and the formation of Pb. This conclusion was supported by a set of complementary techniques such as time-of-flight secondary ion mass spectrometry (ToF-SIMS), photoluminescence (PL) microscopy, scanning electron microscopy (SEM) and energy-dispersive X-ray (EDX) microanalysis. The obtained results demonstrate that IR s-SNOM represents a powerful technique for studying the spatially resolved field-induced degradation dynamics of hybrid perovskite absorbers and the identification of more promising materials resistant to the electric field.

Improved Power Conversion Efficiency and Stability of Perovskite Solar Cells Induced by Molecular Interaction with Poly(ionic liquid) Additives.

Ionic liquid (IL) additives proved to have a positive effect on the device efficiency and stability of perovskite solar cells. However, since ILs are small molecules and undergo Coulomb interactions, they can easily aggregate and evaporate over long times, which would cause instabilities during a long-term device operation. To overcome these problems, we polymerize ILs into macromolecules and incorporate them into perovskite films as well as into the corresponding solar cells. Both cations and anions of the used poly[1-(2-acryloylethyl)-3-methylimidazolium] bis (trifluoromethane) sulfonamides (PAEMI-TFSIs) are designed to coordinate with the Pb and I of PbI62- octahedra, respectively, which changes the crystallization behavior of the perovskite films. Importantly, the PAEMI-TFSI efficiently passivates electronic defects on the grain boundaries and thereby enhances the charge-carrier transport in the perovskite film. As a result, PAEMI-TFSI-modified MAPbI3 solar cells show a high power conversion efficiency of 22.4% and an excellent storage stability (92% of the initial efficiency remains after 1200 h operation in a nitrogen atmosphere for nonencapsulated devices).

Efficient Charge Transfer in MAPbI3 QDs/TiO2 Heterojunctions for High-Performance Solar Cells.

Methylammonium lead iodide (MAPbI3) perovskite quantum dots (QDs) have become one of the most promising materials for optoelectronics. Understanding the dynamics of the charge transfer from MAPbI3 QDs to the charge transport layer (CTL) is critical for improving the performance of MAPbI3 QD photoelectronic devices. However, there is currently less consensus on this. In this study, we used an ultrafast transient absorption (TA) technique to investigate the dynamics of charge transfer from MAPbI3 QDs to CTL titanium dioxide (TiO2), elucidating the dependence of these kinetics on QD size with an injection rate from 1.6 × 1010 to 4.3 × 1010 s-1. A QD solar cell based on MAPbI3/TiO2 junctions with a high-power conversion efficiency (PCE) of 11.03% was fabricated, indicating its great potential for application in high-performance solar cells.

Methylammonium lead triiodide perovskite-based solar cells efficiency: Insight from experimental and simulation.

This work deals with the growth investigation of the methylammonium lead triiodide (MAPbI3) thin films prepared by the spin coating technique. Firstly, MAPbI3 films were studied by X-ray diffraction (XRD) and scanning electron microscopy (SEM) and UV-Visible spectroscopy as well as photoluminescence techniques are used to calculate the band gap energy. Indeed, the high-quality MAPbI3 perovskite films were obtained by using Chlorobenzene as an antisolvent with good crystallinity, large grain sizes, and higher absorption compared to MAPbI3 treated by toluene. Secondly, the performance of FTO/TiO2/MAPbI3/Spiro OMeTAD/Au perovskite solar cell was evaluated using a numerical simulation of the Solar Cell by SCAPS simulator. The effect of the structural and physical parameters of MAPbI3 absorber layer and HTL with the different antisolvents, including thickness, defect density, total charge density, donor density and electron affinity. Obtained results are: Jsc of 25.96 mA/cm2, PCE of 30.70%, Voc of 1.259 V, FF of 88.93% of MAPbI3-based solar cells when MAPbI3 is treated by toluene. However, for MAPbI3- Chlorobenzene, the I-V characteristics are rather: Jsc of 28.18 mA/cm2, PCE of 31.81%, FF of 88.19% and Voc of 1.200 V. It is pointed out that the use of chlorobenzene may be of interest to improve the perovskites solar cells performances.

Optical Sensing Capability Evaluation for Methylammonium Based Perovskites for Explosive.

Here, we have synthesized methylammonium based two metal halide perovskites (MHP) such as MAPbBr3, and MAPbI3 using methylammonium bromide, methylammonium iodide, lead bromide, respective at room temperature under certain experimental conditions. All synthesized MHPs have been confirmed through X-ray diffraction technique (XRD), scanning electron microscope (SEM), Fourier transform infra-red (FTIR) and photoluminescence (PL) analysis. Afterward, comparative evaluation on optical sensing capability has been made for both MHPs using PL in different solvents. Importantly, we find out that MAPbBr3 exhibit an excellent optical feature over MAPbI3 in hexane only. Afterward, MAPbBr3 has also been explored to know the sensing capability for nitrobenzene sensing. Our model study confirms that MAPbBr3 is an excellent sensing material with R square (0.87), selectivity (16.9%) and Stern Volmer constant (Ksv=10- 2 × 0.464) for nitrobenzene in hexane.

Measurement of Optical Properties of CH3NH3PbX3 (X = Br, I) Single Crystals Using Terahertz Time-Domain Spectroscopy.

Organometallic lead bromide and iodide perovskite single crystals (PSCs) are potential candidates for terahertz applications. Herein, we performed terahertz time-domain spectroscopy (THz-TDS) in the frequency range of 0.1-3.0 THz on different thicknesses of MAPbBr3 (0.3, 0.6, and 0.8 mm) and MAPbI3 (0.6, 0.8, 0.9, 1.3, and 2.3 mm). The measurements were carried out with respect to the position (along the focal area), azimuthal rotation of the PSCs, and incidence angles of the reference THz pulse on the PSCs' surface. Based on the transmitted THz pulses from PSCs from the above measurements, we calculated the real and imaginary parts of the refractive index, dielectric constants, absorption coefficients, and dark conductivity. These optical parameters tend to increase with decreases in the PSCs' thicknesses. The transmission spectra of the terahertz electric field indicate that the measured optical properties do not vary significantly with the position and orientation of PSCs. The real parts of the refractive index and dielectric constants are higher than the imaginary values for both PSCs. On the other hand, a slight blueshift in the optical phonon vibrations corresponding to Pb-Br/I-Pb and Pb-Br/I bonds is observed with an increase in thickness. Interestingly, the phonon vibrations do not vary with the incidence angle of the THz pulses on the same crystal's surface. The optical parameters based on THz-TDS reveal that the PSCs satisfy the requirement for tunable THz devices which need suitable, sensitive, and stable absorption properties between 0.1 and 3 THz.

Anion-Dependent Polarization and Piezoelectric Power Generation in Hybrid Halide MAPbX3 (X = I, Br, and Cl) Thin Films with Out-of-Plane Structural Adjustments.

Anion-dependent differences in the electromechanical energy harvesting capability of perovskite halides have not been experimentally demonstrated thus far. Herein, anion-dependent piezoelectricity and bending-driven power generation in high-quality methylammonium lead halide MAPbX3 (X = I, Br, and Cl) thin films are explored; additionally, anisotropic in situ strain is imposed to improve energy harvesting under tensile bending. After applying the maximum in situ strain of -0.73% for all the halide thin films, the MAPbI3 thin-film harvester exhibited a peak voltage/current of ≈23.1 V/≈1703 nA as the best values, whereas MAPbBr3 and MAPbCl3 demonstrated ≈5.6 V/≈176 nA and ≈3.3 V/≈141 nA, respectively, under identical bending conditions. Apart from apparent ferroelectricity of tetragonal MAPbI3 , origin of the piezoelectricity in both cubic MAPbBr3 and MAPbCl3 is explored as being related to organic-inorganic hydrogen bonding, lattice distortion, and ionic migration, with experimental supports of effective piezoelectric coefficient and grain boundary potential. Conclusively, piezoelectricity of the cubic halides is assumed to be due to their soft polarity modes and relatively low elastic modulus with vacancies contributing to space-charge polarization. In the case of ferroelectric MAPbI3 , the distortion of PbI6 octahedra and atomic displacement within each octahedron are quantitatively estimated.