Disentangling Thermal from Electronic Contributions in the Spectral Response of Photoexcited Perovskite Materials.

Disentangling electronic and thermal effects in photoexcited perovskite materials is crucial for photovoltaic and optoelectronic applications but remains a challenge due to their intertwined nature in both the time and energy domains. In this study, we employed temperature-dependent variable-angle spectroscopic ellipsometry, density functional theory calculations, and broadband transient absorption spectroscopy spanning the visible to mid-to-deep-ultraviolet (UV) ranges on MAPbBr3 thin films. The use of deep-UV detection opens a new spectral window that enables the exploration of high-energy excitations at various symmetry points within the Brillouin zone, facilitating an understanding of the ultrafast responses of the UV bands and the underlying mechanisms governing them. Our investigation reveals that the photoinduced spectral features remarkably resemble those generated by pure lattice heating, and we disentangle the relative thermal and electronic contributions and their evolutions at different delay times using combinations of decay-associated spectra and temperature-induced differential absorption. The results demonstrate that the photoinduced transients possess a significant thermal origin and cannot be attributed solely to electronic effects. Following photoexcitation, as carriers (electrons and holes) transfer their energy to the lattice, the thermal contribution increases from ∼15% at 1 ps to ∼55% at 500 ps and subsequently decreases to ∼35-50% at 1 ns. These findings elucidate the intricate energy exchange between charge carriers and the lattice in photoexcited perovskite materials and provide insights into the limited utilization efficiency of photogenerated charge carriers.

Recent Advances in the Inverted Planar Structure of Perovskite Solar Cells.

Inorganic-organic hybrid perovskite solar cells research could be traced back to 2009, and initially showed 3.8% efficiency. After 6 years of efforts, the efficiency has been pushed to 20.1%. The pace of development was much faster than that of any type of solar cell technology. In addition to high efficiency, the device fabrication is a low-cost solution process. Due to these advantages, a large number of scientists have been immersed into this promising area. In the past 6 years, much of the research on perovskite solar cells has been focused on planar and mesoporous device structures employing an n-type TiO2 layer as the bottom electron transport layer. These architectures have achieved champion device efficiencies. However, they still possess unwanted features. Mesoporous structures require a high temperature (>450 °C) sintering process for the TiO2 scaffold, which will increase the cost and also not be compatible with flexible substrates. While the planar structures based on TiO2 (regular structure) usually suffer from a large degree of J-V hysteresis. Recently, another emerging structure, referred to as an "inverted" planar device structure (i.e., p-i-n), uses p-type and n-type materials as bottom and top charge transport layers, respectively. This structure derived from organic solar cells, and the charge transport layers used in organic photovoltaics were successfully transferred into perovskite solar cells. The p-i-n structure of perovskite solar cells has shown efficiencies as high as 18%, lower temperature processing, flexibility, and, furthermore, negligible J-V hysteresis effects. In this Account, we will provide a comprehensive comparison of the mesoporous and planar structures, and also the regular and inverted of planar structures. Later, we will focus the discussion on the development of the inverted planar structure of perovskite solar cells, including film growth, band alignment, stability, and hysteresis. In the film growth part, several methods for obtaining high quality perovskite films are reviewed. In the interface engineering parts, the effect of hole transport layer on subsequent perovskite film growth and their interface band alignment, and also the effect of electron transport layers on charge transport and interface contact will be discussed. As concerns stability, the role of charge transport layers especially the top electron transport layer in the devices stability will be concluded. In the hysteresis part, possible reasons for hysteresis free in inverted planar structure are provided. At the end of this Account, future development and possible solutions to the remaining challenges facing the commercialization of perovskite solar cells are discussed.

Water/alcohol soluble electron injection material containing azacrown ether groups: synthesis, characterization and application to enhancement of electroluminescence.

Using an environmentally stable metal as the cathode in a polymer light-emitting diode (PLED) is an essential requirement for its practical application. We present the preparation of a water/alcohol soluble copoly(p-phenylene) (P1) containing pendant azacrown ether and ethylene glycol ether groups as a highly efficient electron injection layer (EIL) for PLEDs, allowing the use of environmentally stable aluminum as the cathode. Multilayer PLEDs [ITO/PEDOT:PSS/PF-Green-B/EIL/Al] using P1 as EIL exhibit significantly enhanced device performance, particularly in the presence of K2CO3 or Cs2CO3. The maximum luminous power efficiency and maximum luminance of the device with Cs2CO3-doped P1 as EIL were enhanced to 9.16 lm W(-1) and 17,050 cd m(-2), respectively, compared with those without EIL (0.16 lm W(-1), 890 cd m(-2)). The turn-on voltage was also significantly reduced from 5.7 V to 3.7 V simultaneously. The performance enhancement has been attributed to improved electron injection which has been confirmed by the rise in open-circuit voltage (Voc) obtained from photovoltaic measurements. The incorporation of such an electron injection layer significantly enhances device performance for PLEDs with an environmentally stable metal as the cathode.

High voltage and efficient bilayer heterojunction solar cells based on an organic-inorganic hybrid perovskite absorber with a low-cost flexible substrate.

A low temperature (<100 °C), flexible solar cell based on an organic-inorganic hybrid CH3NH3PbI3 perovskite-fullerene planar heterojunction (PHJ) is successfully demonstrated. In this manuscript, we study the effects of energy level offset between a solar absorber (organic-inorganic hybrid CH3NH3PbI3 perovskite) and the selective contact materials on the photovoltaic behaviors of the planar organometallic perovskite-fullerene heterojunction solar cells. We find that the difference between the highest occupied molecular orbital (HOMO) level of CH3NH3PbI3 perovskite and the Fermi level of indium-tin-oxide (ITO) dominates the voltage output of the device. ITO films on glass or on the polyethylene terephthalate (PET) flexible substrate with different work functions are investigated to illustrate this phenomenon. The higher work function of the PET/ITO substrate decreases the energy loss of hole transfer from the HOMO of perovskite to ITO and minimizes the energy redundancy of the photovoltage output. The devices using the high work function ITO substrate as contact material show significant open-circuit voltage enhancement (920 mV), with the power conversion efficiency of 4.54%, and these types of extra-thin planar bilayer heterojunction solar cells have the potential advantages of low-cost and lightweight.

Femtosecond excitonic relaxation dynamics of perovskite on mesoporous films of Al2O3 and NiO nanoparticles.

The excitonic relaxation dynamics of perovskite adsorbed on mesoporous thin films of Al2O3 and NiO upon excitation at 450 nm were investigated with femtosecond optical gating of photoluminescence (PL) via up-conversion. The temporal profiles of emission observed in spectral region 670-810 nm were described satisfactorily with a composite consecutive kinetic model and three transient components representing one hot and two cold excitonic relaxations. All observed relaxation dynamics depend on the emission wavelength, showing a systematic time-amplitude correlation for all three components. When the NiO film was employed, we observed an extent of relaxation proceeding through the non-emissive surface state larger than through the direct electronic relaxation channel, which quenches the PL intensity more effectively than on the Al2O3 film. We conclude that perovskite is an effective hole carrier in a p-type electrode for NiO-based perovskite solar cells showing great performance.

Band Gap Renormalization at Different Symmetry Points in Perovskites.

Using ultrafast broad-band transient absorption (TA) spectroscopy of photoexcited MAPbBr3 thin films with probe continua in the visible and the mid- to deep-ultraviolet (UV) ranges, we capture the ultrafast renormalization at the fundamental gap at the R symmetry point of the Brillouin zone (BZ) and a higher energy gap at the M symmetry point. Advanced global lifetime analysis and lifetime density distribution analysis are applied to extract quantitative information. Our work confirms the similarity of the response at both high-symmetry points, which indicates a band edge renormalization that rises within the instrument response function (IRF, ∼250 fs) and decays in ca. 400-600 fs, undergoing an energy red shift of 90-150 meV. The reported time scale corresponds to the decay of free carriers into neutral excitons. The ability to monitor different high-symmetry points in photoexcited perovskites opens exciting prospects for the characterization of a large class of materials and for photonic applications.

A large-scale sub-100 nm Au nanodisk array fabricated using nanospherical-lens lithography: a low-cost localized surface plasmon resonance sensor.

Large-scale Au nanodisk arrays are successfully fabricated using nanospherical-lens lithography (NLL). By incorporating both rotational oblique-angle deposition and oxygen plasma treatment, the improved NLL is capable of fabricating Au nanodisks with diameters as small as 75 nm that cover an area larger than 1 cm(2). The fabricated nanodisk arrays are investigated as sensitive localized surface plasmon resonance (LSPR) sensors. The extinction spectra of the Au nanodisk arrays reveal a narrower LSPR peak when the diameter becomes smaller. The shape imperfection severely limits the minimum obtainable linewidth, especially when the nanodisk diameter is smaller than 200 nm. The imperfection is found to be improved by thermal annealing at high temperatures. The maximum theoretically predicted and experimentally obtained figure-of-merit for Au nanodisk arrays whose periodicities are 500 nm are around 15 and 9, respectively. Further optimization of the periodicity and thickness of the nanodisks will further improve their sensitivity and lead to more novel applications.

Suppressing phase disproportionation in quasi-2D perovskite light-emitting diodes.

Electroluminescence efficiencies and stabilities of quasi-two-dimensional halide perovskites are restricted by the formation of multiple-quantum-well structures with broad and uncontrollable phase distributions. Here, we report a ligand design strategy to substantially suppress diffusion-limited phase disproportionation, thereby enabling better phase control. We demonstrate that extending the π-conjugation length and increasing the cross-sectional area of the ligand enables perovskite thin films with dramatically suppressed ion transport, narrowed phase distributions, reduced defect densities, and enhanced radiative recombination efficiencies. Consequently, we achieved efficient and stable deep-red light-emitting diodes with a peak external quantum efficiency of 26.3% (average 22.9% among 70 devices and cross-checked) and a half-life of ~220 and 2.8 h under a constant current density of 0.1 and 12 mA/cm2, respectively. Our devices also exhibit wide wavelength tunability and improved spectral and phase stability compared with existing perovskite light-emitting diodes. These discoveries provide critical insights into the molecular design and crystallization kinetics of low-dimensional perovskite semiconductors for light-emitting devices.

Manipulation of micro-particles by flexible polymer-based optically-induced dielectrophoretic devices.

This study presents a novel technology to manipulate micro-particles with the assistance from flexible polymer-based optically-induced dielectrophoretic (ODEP) devices. Bending the flexible ODEP devices downwards or upwards to create convex or concave curvatures, respectively, enables the more effective separation or collection of micro-particles with different diameters. The travel distances of the polystyrene beads of 40 µm diameter, as induced by the projected light in a given time period was increased by ~100%, which were 43.0 ± 5.0 and 84.6 ± 4.0 µm for flat and convex ODEP devices, respectively. A rapid separation or collection of micro-particles can be achieved with the assistance of gravity because the falling polystyrene beads followed the inclination of the downward and upward bent ODEP devices.

Lead-Free Organic-Perovskite Hybrid Quantum Wells for Highly Stable Light-Emitting Diodes.

Two-dimensional perovskites that could be regarded as natural organic-inorganic hybrid quantum wells (HQWs) are promising for light-emitting diode (LED) applications. High photoluminescence quantum efficiencies (approaching 80%) and extremely narrow emission bandwidth (less than 20 nm) have been demonstrated in their single crystals; however, a reliable electrically driven LED device has not been realized owing to inefficient charge injection and extremely poor stability. Furthermore, the use of toxic lead raises concerns. Here, we report Sn(II)-based organic-perovskite HQWs employing molecularly tailored organic semiconducting barrier layers for efficient and stable LEDs. Utilizing femtosecond transient absorption spectroscopy, we demonstrate the energy transfer from organic barrier to inorganic perovskite emitter occurs faster than the intramolecular charge transfer in the organic layer. Consequently, this process allows efficient conversion of lower-energy emission associated with the organic layer into higher-energy emission from the perovskite layer. This greatly broadened the candidate pool for the organic layer. Incorporating a bulky small bandgap organic barrier in the HQW, charge transport is enhanced and ion migration is greatly suppressed. We demonstrate a HQW-LED device with pure red emission, a maximum luminance of 3466 cd m-2, a peak external quantum efficiency up to 3.33%, and an operational stability of over 150 h, which are significantly better than previously reported lead-free perovskite LEDs.

Surface plasmon-enhanced and quenched two-photon excited fluorescence.

This study investigated theoretically and experimentally that two-photon excited fluorescence is enhanced and quenched via surface plasmons (SPs) excited by total internal reflection with a silver film. The fluorescence intensity is fundamentally affected by the local electromagnetic field enhancement and the quantum yield change according to the surrounding structure and materials. By utilizing the Fresnel equation and classical dipole radiation modeling, local electric field enhancement, fluorescence quantum yield, and fluorescence emission coupling yield via SPs were theoretically analyzed at different dielectric spacer thicknesses between the fluorescence dye and the metal film. The fluorescence lifetime was also decreased substantially via the quenching effect. A two-photon excited total internal reflection fluorescence (TIRF) microscopy with a time-correlated single photon counting device has been developed to measure the fluorescence lifetimes, photostabilities, and enhancements. The experimental results demonstrate that the fluorescence lifetimes and the trend of the enhancements are consistent with the theoretical analysis. The maximum fluorescence enhancement factor in the surface plasmon-total internal reflection fluorescence (SP-TIRF) configuration can be increased up to 30 fold with a suitable thickness SiO(2) spacer. Also, to compromise for the fluorescence enhancement and the fluorophore photostability, we find that the SP-TIRF configuration with a 10 nm SiO(2) spacer can provide an enhanced and less photobleached fluorescent signal via the assistance of enhanced local electromagnetic field and quenched fluorescence lifetime, respectively.

High-Performance Perovskite-Based Light-Emitting Diodes from the Conversion of Amorphous Spin-Coated Lead Bromide with Phenethylamine Doping.

Large-grained and well-oriented methylammonium lead tribromide (MAPbBr3) perovskite was formed from the conversion of amorphous lead bromide (PbBr2) doped with phenethylamine (PEA). The addition of PEA ions (with an optimized molar ratio of 0.008%) to the PbBr2 solution assisted the formation of a smooth PEA-doped PbBr2 layer by spin-coating. Then, the PEA-doped PbBr2 thin film would convert into large-grained and well-oriented MAPbBr3 with the help of a solid-vapor reaction under a vaporized methylammonium bromide (MABr) and choline chloride (CC) atmosphere. Furthermore, both PEA and CC would passivate the defects of perovskite to improve the crystal quality of perovskite. By applying this perovskite layer in perovskite light-emitting diodes (PeLEDs), the maximum luminance and current efficiency of PeLEDs could reach 20,869 cd/m2 and 3.99 cd/A, respectively; these values are approximately five and three times larger than those of PeLEDs without PEA. The perovskite converted from spin-coated PbBr2 with a PEA dopant remarkably improved the luminance and current efficiency of its PeLEDs.

White-emissive tandem-type hybrid organic/polymer diodes with (0.33, 0.33) chromaticity coordinates.

This study reports fabrication of white-emissive, tandem-type, hybrid organic/polymer light-emitting diodes (O/PLED). The tandem devices are made by stacking a blue-emissive OLED on a yellow-emissive phenyl-substituted poly(para-phenylene vinylene) copolymer-based PLED and applying an organic oxide/Al/molybdenum oxide (MoO(3)) complex structure as a connecting structure or charge-generation layer (CGL). The organic oxide/Al/MoO(3) CGL functions as an effective junction interface for the transport and injection of opposite charge carriers through the stacked configuration. The electroluminescence (EL) spectra of the tandem-type devices can be tuned by varying the intensity of the emission in each emissive component to yield the visible-range spectra from 400 to 750 nm, with Commission Internationale de l'Eclairage chromaticity coordinates of (0.33, 0.33) and a high color rendering capacity as used for illumination. The EL spectra also exhibit good color stability under various bias conditions. The tandem-type device of emission with chromaticity coordinates, (0.30, 0.31), has maximum brightness and luminous efficiency over 25,000 cd/m(2) and approximately 4.2 cd/A, respectively.

Bulk-heterojunction polymers in optically-induced dielectrophoretic devices for the manipulation of microparticles.

This paper presents a decent polymer material for fabricating optically-induced dielectrophoretic (ODEP) devices, which can manipulate microparticles or cells by using moving light patterns. A thin film of a bulk-heterojunction (BHJ) polymer, a mixture of regioregular poly(3-hexylthiophene) and [6,6]-phenyl C61-butyric acid methyl ester, is used as a light-activated layer. When illuminated by a projected light beam, the photo-induced charge carriers created by the electron transfer of excitons at a donor/acceptor interface in the BHJ layer, disturbs the uniformly-distributed electric field applied on the ODEP devices. A negative DEP force is then generated by virtual electrodes defined by the optical images from a computer-programmable projector to manipulate microparticles, thus providing a functionalized platform for particle manipulation. The effect of the polymer thickness and composition on the magnitude of the generated DEP force has been extensively investigated. The maximum particle drag velocity and the force applied on 20.0 mum diameter polystyrene beads are measured to be approximately 202.2 mum/s and 38.2 pN, respectively, for a device with a 497.3-nm thick BHJ layer. The lifetime of the developed device is also explored (~5 hours), which is sufficient for applications of disposable ODEP devices. Therefore, the BHJ polymer may provide a promising candidate for future ODEP devices capable of nanoparticle and cell manipulation.

Lead-Free Antimony-Based Light-Emitting Diodes through the Vapor-Anion-Exchange Method.

Hybrid lead halide perovskites continue to attract interest for use in optoelectronic devices such as solar cells and light-emitting diodes. Although challenging, the replacement of toxic lead in these systems is an active field of research. Recently, the use of trivalent metal cations (Bi3+ and Sb3+) that form defect perovskites A3B2X9 has received great attention for the development of solar cells, but their light-emissive properties have not previously been studied. Herein, an all-inorganic antimony-based two-dimensional perovskite, Cs3Sb2I9, was synthesized using the solution process. Vapor-anion-exchange method was employed to change the structural composition from Cs3Sb2I9 to Cs3Sb2Br9 or Cs3Sb2Cl9 by treating CsI/SbI3 spin-coated films with SbBr3 or SbCl3, respectively. This novel method facilitates the fabrication of Cs3Sb2Br9 or Cs3Sb2Cl9 through solution processing without the need of using poorly soluble precursors (e.g., CsCl and CsBr). We go on to demonstrate electroluminescence from a device employing Cs3Sb2I9 emitter sandwiched between ITO/PEDOT:PSS and TPBi/LiF/Al as the hole and electron injection electrodes, respectively. A visible-infrared radiance of 0.012 W·Sr-1·m-2 was measured at 6 V when Cs3Sb2I9 was the active emitter layer. These proof-of-principle devices suggest a viable path toward low-dimensional, lead-free A3B2X9 perovskite optoelectronics.

Surfactant-Enriched ZnO Surface via Sol-Gel Process for the Efficient Inverted Polymer Solar Cell.

In this study, we demonstrate that the top surface is enriched by surfactants, tetraoctylammonium bromide, and cetylpyridinium bromide (CPB), in the sol-gel ZnO, being evidenced by the Br depth profile of electron spectroscopy for chemical analysis data. X-ray photoelectron spectroscopy results showed the formation of Zn-Br bonding due to the oxygen defects occupied by Br at the surfactant-enriched ZnO surface. The surfactant-enriched ZnO surface possessed a smoother surface and more hydrophobicity than the pristine ZnO from the experimental results of atomic force microscopy and contact angle, respectively. On the basis of ultraviolet photoelectron spectroscopy data, the work function slightly reduced due to the dipole built-up by the electrostatic force between Br- and N+ to enhance the electron extraction ability. The improved properties benefited the power conversion efficiency (PCE) of bulk-heterojunction polymer solar cells (PSCs) by spin-coating the active layer on the surfactant-enriched ZnO surface. The inverted PSCs with the surfactant-enriched ZnO surface showed the highest PCE of 9.55% for the CPB case, in comparison with the pristine ZnO surface (8.08% PCE). This study discloses that turning the ZnO surface is easily achieved by the addition of surfactants with different molecular structures in the sol-gel ZnO for high performance polymer solar cells.

Enhancement of Inverted Polymer Solar Cells Performances Using Cetyltrimethylammonium-Bromide Modified ZnO.

In this study, the performance and stability of inverted bulk heterojunction (BHJ) polymer solar cells (PSCs) is enhanced by doping zinc oxide (ZnO) with 0-6 wt % cetyltrimethylammonium bromide (CTAB) in the sol-gel ZnO precursor solution. The power conversion efficiency (PCE) of the optimized 3 wt % CTAB-doped ZnO PSCs was increased by 9.07%, compared to a PCE of 7.31% for the pristine ZnO device. The 0-6 wt % CTAB-doped ZnO surface roughness was reduced from 2.6 to 1 nm and the number of surface defects decreased. The X-ray photoelectron spectroscopy binding energies of Zn 2p3/2 (1021.92 eV) and 2p1/2 (1044.99 eV) shifted to 1022.83 and 1045.88 eV, respectively, which is related to strong chemical bonding via bromide ions (Br-) that occupy oxygen vacancies in the ZnO lattice, improving the PCE of PSCs. The concentration of CTAB in ZnO significantly affected the work function of PSC devices; however, excessive CTAB increased the work function of the ZnO layer, resulting from the aggregation of CTAB molecules. In addition, after a 120-hour stability test in the atmosphere with 40% relative humidity, the inverted device based on CTAB-doped ZnO retained 92% of its original PCE and that based on pristine ZnO retained 68% of its original PCE. The obtained results demonstrate that the addition of CTAB into ZnO can dramatically influence the optical, electrical, and morphological properties of ZnO, enhancing the performance and stability of BHJ PSCs.

Highly Efficient 2D/3D Hybrid Perovskite Solar Cells via Low-Pressure Vapor-Assisted Solution Process.

The fabrication of multidimensional organometallic halide perovskite via a low-pressure vapor-assisted solution process is demonstrated for the first time. Phenyl ethyl-ammonium iodide (PEAI)-doped lead iodide (PbI2 ) is first spin-coated onto the substrate and subsequently reacts with methyl-ammonium iodide (MAI) vapor in a low-pressure heating oven. The doping ratio of PEAI in MAI-vapor-treated perovskite has significant impact on the crystalline structure, surface morphology, grain size, UV-vis absorption and photoluminescence spectra, and the resultant device performance. Multiple photoluminescence spectra are observed in the perovskite film starting with high PEAI/PbI2 ratio, which suggests the coexistence of low-dimensional perovskite (PEA2 MAn-1 Pbn I3n+1 ) with various values of n after vapor reaction. The dimensionality of the as-fabricated perovskite film reveals an evolution from 2D, hybrid 2D/3D to 3D structure when the doping level of PEAI/PbI2 ratio varies from 2 to 0. Scanning electron microscopy images and Kelvin probe force microscopy mapping show that the PEAI-containing perovskite grain is presumably formed around the MAPbI3 perovskite grain to benefit MAPbI3 grain growth. The device employing perovskite with PEAI/PbI2 = 0.05 achieves a champion power conversion efficiency of 19.10% with an open-circuit voltage of 1.08 V, a current density of 21.91 mA cm-2 , and a remarkable fill factor of 80.36%.

Roller-Induced Bundling of Long Silver Nanowire Networks for Strong Interfacial Adhesion, Highly Flexible, Transparent Conductive Electrodes.

Silver nanowires (AgNWs) have been the most promising electrode materials for fabrication of flexible transparent touch panel, displays and many other electronics because of their excellent electrical properties, cost effectiveness, synthesis scalability, and suitability for mass production. Although a few literature reports have described the use of short Ag NWs in fabrication of randomly oriented Ag NW network-based electrode, their electrical conductivities are still far lower than that of Ag films. So far, no any literature report was able to provide any simple solution to fabrication of large-area and mass-manufactural ability to address the issues, such as, conductivity, transparency, electrical current withstand, bending stability, and interfacial adhesion. In the current work, we provide a simple solution to conquer the above-mentioned challenges, and report the development of long Ag NW bundle network electrodes on large area PET films that were coated, aligned, and bundled quickly and simply using a steel roller. Our developed AgNWs-bundle networks had superior performance in optoelectronic properties (sheet resistance 5.8 Ω sq-1; optical transmittance 89% at 550 nm wavelength), electrical current withstand up to 500 mA, and bending stability over 5000 bending cycles, and strong interfacial adhesion.

Robust and Recyclable Substrate Template with an Ultrathin Nanoporous Counter Electrode for Organic-Hole-Conductor-Free Monolithic Perovskite Solar Cells.

A robust and recyclable monolithic substrate applying all-inorganic metal-oxide selective contact with a nanoporous (np) Au:NiOx counter electrode is successfully demonstrated for efficient perovskite solar cells, of which the perovskite active layer is deposited in the final step for device fabrication. Through annealing of the Ni/Au bilayer, the nanoporous NiO/Au electrode is formed in virtue of interconnected Au network embedded in oxidized Ni. By optimizing the annealing parameters and tuning the mesoscopic layer thickness (mp-TiO2 and mp-Al2O3), a decent power conversion efficiency (PCE) of 10.25% is delivered. With mp-TiO2/mp-Al2O3/np-Au:NiOx as a template, the original perovskite solar cell with 8.52% PCE can be rejuvenated by rinsing off the perovskite material with dimethylformamide and refilling with newly deposited perovskite. A renewed device using the recycled substrate once and twice, respectively, achieved a PCE of 8.17 and 7.72% that are comparable to original performance. This demonstrates that the novel device architecture is possible to recycle the expensive transparent conducting glass substrates together with all the electrode constituents. Deposition of stable multicomponent perovskite materials in the template also achieves an efficiency of 8.54%, which shows its versatility for various perovskite materials. The application of such a novel NiO/Au nanoporous electrode has promising potential for commercializing cost-effective, large scale, and robust perovskite solar cells.