Ligang Yuan

Operationally stable mixed‐cation‐halide perovskite solar cells are fabricated by halogen‐engineering concept via a Br‐rich seeding growth method. Bromine anions are effectively incorporated into the final perovskite film with larger grains and better vertical columnar alignment. Photovoltaic devices based on the film show a power conversion efficiency (PCE) of 21.5% and significantly enhanced operational stability for over 500 h.

Abstract

The performance of perovskite solar cells (PSCs) relies on the synthesis method and chemical composition of the perovskite materials. So far, PSCs that have adopted two‐step sequential deposited perovskite with the state‐of‐art composition (FAPbI₃)_{1− x} (MAPbBr₃) _x (x < 0.05) have achieved record power conversion efficiency (PCE), while their one‐step antisolvent dripping counterparts with typical composition Cs_0.05FA_0.81MA_0.14Pb(I_0.85Br_0.15)₃ with more bromine have exhibited much better long‐term operational stability. Thus, halogen engineering that aims to elevate bromine content in sequential deposited perovskite film would push operational stability of PSCs toward that of antisolvent dripping deposited perovskite materials. Here, a Br‐rich seeding growth method is devised and perovskite seed solution with high bromine content is introduced into a PbI₂ precursor, leading to bromine incorporation in the resulting perovskite film. Photovoltaic devices fabricated by Br‐rich seeding growth method exhibit a PCE of 21.5%, similar to 21.6% for PSCs having lower bromine content. Whereas, the operational stability of PSCs with higher bromine content is significantly enhanced, with over 80% of initial PCE retained after 500 h tracking at maximum power point under 1‐sun illumination. This work highlights the vital importance of halogen composition for the operational stability of PSCs, and introduces an effective way to incorporate bromine into mixed‐cation‐halide perovskite film via sequential deposition method.

An efficient control of the film quality and thickness distribution of alternating cations in the interlayer space of 2D perovskite (GA)(MA) _n Pb _n I_{3 n +1} (〈n〉 = 3) quantum wells via incorporation of methylammonium chloride as an additive is demonstrated. The optimized device leads to more efficient charge transport and suppressed nonradiative charge recombination. Consequently, the optimized perovskite solar cell delivers an efficiency of 18.48%.

Abstract

2D perovskites stabilized by alternating cations in the interlayer space (ACI) represent a very new entry as highly efficient semiconductors for solar cells approaching 15% power conversion efficiency (PCE). However, further improvements will require understanding of the nature of the films, e.g., the thickness distribution and charge‐transfer characteristics of ACI quantum wells (QWs), which are currently unknown. Here, efficient control of the film quality of ACI 2D perovskite (GA)(MA) _n Pb _n I_{3 n +1} (〈n〉 = 3) QWs via incorporation of methylammonium chloride as an additive is demonstrated. The morphological and optoelectronic characterizations unambiguously demonstrate that the additive enables a larger grain size, a smoother surface, and a gradient distribution of QW thickness, which lead to enhanced photocurrent transport/extraction through efficient charge transfer between low‐n and high‐n QWs and suppressed nonradiative charge recombination. Therefore, the additive‐treated ACI perovskite film delivers a champion PCE of 18.48%, far higher than the pristine one (15.79%) due to significant improvements in open‐circuit voltage and fill factor. This PCE also stands as the highest value for all reported 2D perovskite solar cells based on the ACI, Ruddlesden–Popper, and Dion–Jacobson families. These findings establish the fundamental guidelines for the compositional control of 2D perovskites for efficient photovoltaics.

Various definitions of band gaps are used in the perovskite solar cell community as a reference to analyze losses in open‐circuit voltage. This essay proposes a band‐gap independent method to reference voltages that is easy to implement and a meta‐analysis of literature data to illustrate the state of the art and development of voltage losses in perovskite solar cells.

Abstract

Open‐circuit voltages of lead‐halide perovskite solar cells are improving rapidly and are approaching the thermodynamic limit. Since many different perovskite compositions with different bandgap energies are actively being investigated, it is not straightforward to compare the open‐circuit voltages between these devices as long as a consistent method of referencing is missing. For the purpose of comparing open‐circuit voltages and identifying outstanding values, it is imperative to use a unique, generally accepted way of calculating the thermodynamic limit, which is currently not the case. Here a meta‐analysis of methods to determine the bandgap and a radiative limit for open‐circuit voltage is presented. The differences between the methods are analyzed and an easily applicable approach based on the solar cell quantum efficiency as a general reference is proposed.

A‐site management by introducing an A‐site placeholder cation, NH₄ ⁺, during the perovskite crystallization process is proposed to balance the supersaturation discrepancy between AX and BX₂ so as to improve its crystal quality without any residue. Most importantly, the sharply decreased A‐site‐related defect I_MA indicates that it is responsible for such crystalline optimization.

Abstract

An in‐depth understanding and effective suppression of nonradiative recombination pathways in perovskites are crucial to their crystallization process, in which supersaturation discrepancies at different time scales between CH₃NH₃I (MAI, methylammonium iodide) and PbI₂ remain a key issue. Here, an A‐site management strategy via the introduction of an A‐site placeholder cation, NH₄ ⁺, to offset the deficient MA⁺ precipitation by occupying the cavity of Pb–I framework, is proposed. The temporarily remaining NH₄ ⁺ is substituted by subsequently precipitated MA⁺. The temperature‐dependent crystallization process with the generation and consumption of a transient phase is sufficiently demonstrated by the dynamic changes in crystal structure characteristic peaks through in situ grazing‐incidence X‐ray diffraction and the surface potential difference evolution through temperature‐dependent Kelvin probe force microscopy. A highly crystalline perovskite is consequently acquired, indicated by the enlarged grain size, lowered nonradiative defect density, prolonged carrier lifetime, and fluorescence lifetime imaging. Most importantly, it is identified that the A‐site I_MA defect is responsible for such crystal quality optimization based on theoretical calculations, transient absorption, and deep‐level transient spectroscopy. Furthermore, the universality of the proposed A‐site management strategy is demonstrated with other mixed‐cation perovskite systems, indicating that this methodology successfully provides guidance for synthesis route design of highly crystalline perovskites.

Here, a 3.19%‐external quantum efficiency all‐solution‐processed green perovskite light‐emitting diode is reported by employing 1,3,5‐tris(1‐phenyl‐1H‐benzimidazol‐2‐yl)benzene (TPBi) doped conjugated amino‐alkyl substituted polyfluorene poly[(9,9‐bis(3′‐(N,N‐dimethylamino)propyl)‐2,7‐fluorene)‐alt‐2,7‐(9,9‐dioctylfluorene)] (PFN) as electron injection layer. The doping of TPBi into PFN not only enhances the capability of electron injection, but also significantly suppresses the emission quenching of perovskite caused by the charge transfer between perovskite and PFN.

Abstract

Metal halide perovskites have attracted considerable attention in the field of light‐emitting diodes due to their high color purity and solution processability. However, most perovskite light‐emitting diodes (PeLEDs) employ thermally deposited charge transport layers (CTLs) on top of perovskite layers. In order to realize low‐cost and scalable fabrication of PeLEDs, all‐solution process is highly desired, but still remaining great challenges. Here, an efficient all‐solution‐processed green PeLEDs is reported by incorporating 1,3,5‐tris(1‐phenyl‐1H‐benzimidazol‐2‐yl)benzene (TPBi) doped conjugated amino‐alkyl substituted polyfluorene poly[(9,9‐bis(3′‐(N,N‐dimethylamino)propyl)‐2,7‐fluorene)‐alt‐2,7‐(9,9‐dioctylfluorene)] (PFN) electron injection layer, achieving a maximum luminance of 9875 cd m⁻², a high current efficiency of 10.41 cd A⁻¹, and an external quantum efficiency of 3.19%. Since the solvents used for perovskite precursors and PFN are orthogonal, the protected and complete interface of perovskite film and CTL is effectively obtained by solution processes. The doping of TPBi into PFN not only enhances the capability of electron injection, but also significantly suppresses the emission quenching of perovskite films caused by the charge transfer between perovskite and PFN due to the reduced difference in their work functions. This work provides an efficient approach for the development of all‐solution‐processed PeLEDs.

Optically pumped lasing is demonstrated in distributed feedback hybrid perovskite light emitting diodes fabricated on both glass and Si substrates. Thresholds as low as ≈6 µJ cm⁻² at room temperature are achieved and retained under ≈2 A cm⁻² of pulsed electrical excitation.

Abstract

Electrically pumped lasing from hybrid organic–inorganic metal‐halide perovskite semiconductors could lead to nonepitaxial diode lasers that are tunable throughout the visible and near‐infrared spectrum; however, a viable laser diode architecture has not been demonstrated to date. Here, an important step toward this goal is achieved by demonstrating two distinct distributed feedback light‐emitting diode architectures that achieve low threshold, optically pumped lasing. Bottom‐ and top‐emitting perovskite light‐emitting diodes are fabricated on glass and Si substrates, respectively, using a polydimethylsiloxane stamp in the latter case to nanoimprint a second‐order distributed feedback grating directly into the methylammonium lead iodide active layer. The devices exhibit room temperature thresholds as low as ≈6 µJ cm⁻², a peak external quantum efficiency of ≈0.1%, and a maximum current density of ≈2 A cm⁻² that is presently limited by degradation associated with excessive leakage current. In this low current regime, electrical injection does not adversely affect the optical pump threshold, leading to a projected threshold current density of ≈2 kA cm⁻². Operation at low temperature can significantly decrease this threshold, but must overcome extrinsic carrier freeze‐out in the doped organic transport layers to maintain a reasonable drive voltage.

A very high‐efficiency host material for blue single‐layer phosphorescent organic light‐emitting diode (OLED) (external quantum efficiency reaching 17.6%) is reported. This host is synthesized via an efficient approach, displays a high E _T, adequate highest occupied molecular orbital/lowest unoccupied molecular orbital energy levels, and suitable balance between hole and electron mobilities displaying all the required properties for reaching high‐performance single‐layer phosphorescent OLED.

Abstract

Herein, a high‐efficiency host material for single‐layer phosphorescent organic light‐emitting diodes (SL‐PhOLEDs) is reported. This host material is synthesized via an efficient approach and is constructed on the association of an electron‐rich phenylacridine unit connected by a spiro carbon atom to an electron‐deficient 2,7‐bis(diphenylphosphineoxide)‐fluorene. In addition to a high E _T value and adequate highest occupied molecular orbital/lowest unoccupied molecular orbital energy levels, the key point in this molecular design is the suitable balance between hole and electron mobilities, which leads to a high‐performance blue SL‐PhOLED with an external quantum efficiency of 17.6% (current efficiency = 37.8 cd A⁻¹ and power efficiency = 37.1 lm W⁻¹) and a low V _on of 2.5 V. This performance shows that the molecular design of the present host fulfills the criteria required for high‐efficiency SL‐PhOLEDs. The present performance is one of the highest reported to date for blue SL‐PhOLEDs and more importantly shows the potential of such a molecular design to reach very high‐performance single‐layer devices.

Over 2500 h operation lifetime at a high brightness of 1000 cd m⁻² light‐emitting diodes with high peak external quantum efficiency of 23.9%, current efficiency of 100.5 cd A⁻¹, and low efficiency roll‐off at high currents based on compositional graded ZnCdSe/ZnSe/ZnSeS/ZnS quantum dots are synthesized by a shell tailored strategy.

Abstract

Quantum dot light‐emitting diodes (QLEDs) are considered to be the candidate light sources with the most potential for applications in displays. Recent advances in luminance, external quantum efficiency (EQE), and even the operation lifetime of QLEDs have already satisfied the requirements for low‐light‐level displays. However, the short operation lifetime under high brightness limits the application of QLEDs for outdoor displays and lightings. Here, demonstrated are green QLEDs with a T ₉₅ operation lifetime reaching up to 2500 h at high brightness (1000 cd m⁻²) with a high peak EQE of 23.9%, current efficiency of 100.5 cd A⁻¹, and low efficiency roll‐off at high current. Both the EQE and lifetime of the QLEDs are superior to those reported to date for all solution‐processed green QLEDs. These major advances are qualitatively attributed to the use of a shell‐tailoring strategy for producing compositional graded CdZnSe/ZnSe/ZnSeS/ZnS quantum dots with a high photoluminescence quantum yield, suppressed nonradiative Förster resonant energy transfer and Auger recombination, and favorable valence band alignment for enhanced hole injection. Collectively, this work represents a huge step forward in eventually realizing QLEDs for high‐brightness display and lighting applications.

Based on mixed halide perovskites, a pure blue film with a photoluminescence quantum yield of 88% is obtained. Corresponding blue perovskite light‐emitting diode (LED) exhibits electroluminescence (EL) at 468 nm with an external quantum efficiency of 0.71%. By introducing the square‐wave alternate voltage for driving LED device, the EL spectrum of the device shows negligible shifts for 12 h.

Abstract

Perovskite light‐emitting diodes (PeLEDs) have attracted great research interests considering their excellent luminescent properties and solution processability. Despite rapid advances of green‐, red‐, and near‐infrared‐emitting PeLEDs, blue‐PeLEDs, as an essential part for full‐color display and solid‐state lighting, still remain challenging due to their low efficiency and spectral instability. Here, reported are spectrally stable blue‐PeLEDs biased by an alternating voltage. First, 2‐phenoxyethylamine‐passivated CsPbBr _x Cl_{3− x} is obtained as a blue emitter with a record photoluminescence quantum yield of 88%. Subsequently, constructed and optimized are pure blue‐emitting PeLEDs exhibiting electroluminescence (EL) at 468 nm with a high external quantum efficiency of 0.71%. Furthermore, driven are the devices by square‐wave alternating voltage and stabilized are the EL spectra for 12 h by suppressing the detrimental halide migration during operation. It is believed that this work provides an alternative way for the spectrally stable mixed halide blue PeLEDs.

The efficiency and stability of 2D perovskite solar cells are synergistically improved through metal ion doping. The hole extraction and transport abilities are significantly enhanced by Cu ion doping in the NiO _x layers, while the optoelectronic properties of the BA₂MA₃Pb₄I₁₃ (BA = butylamine; MA = methylammonium) layers are effectively improved with Cs ion doping.

Abstract

2D perovskites hold a great prospective to create highly efficient and stable solar cell devices. In order to explore their full potential, every component of 2D perovskite solar cells (PSCs) has to be carefully designed and engineered. Herein, the metal ion doping strategy is taken to optimize both the hole transport layers (HTLs) and the light absorbing layers of the BA₂MA₃Pb₄I₁₃ (BA = butylamine; MA = methylammonium) based 2D PSC devices. The hole extraction and transport abilities are significantly enhanced by Cu ion doping in the nickel oxide layers, while the optoelectronic properties of the BA₂MA₃Pb₄I₁₃ layers are effectively improved with Cs ion doping. The synergistic incorporations of Cu and Cs ions have boosted the device power conversion efficiency to 13.92%, the highest for 2D PSCs based on inorganic HTLs. In addition, the inorganic nature of the Cu doped nickel oxide film and the high quality of the Cs doped 2D perovskite film also endow the PSC device with extraordinary humidity and thermal stabilities.

The biaxial strains originating from the lattice mismatch endow the monolayer SnS an indirect‐to‐direct bandgap transition. Moreover, the interface effect in turn reduces the band offset of the CsPbI₃/SnS heterostructure and enhances its optical absorption ability. Therefore, forming heterostructure can promote the properties of CsPbI₃‐based devices.

Abstract

Different 2D materials can be stacked by the weak van der Waals (vdW) force, forming the vdW heterostructures and devices, which opens a new field of engineering regulation of electronic and optical properties at the atomic level. The asymmetric strain‐introduced interface effect is studied on the electronic and optical properties of CsPbI₃/SnS vdW heterostructure by employing first‐principles calculations. The biaxial strains deriving from the interface mismatch reduce the work function of the monolayer SnS to a low‐energy level, and lead to monolayer SnS an indirect‐to‐direct bandgap transition. The different charge transfer behaviors in the PbI₂‐ (CsI‐) surface indicate that monolayer SnS can act as the promising hole‐ (electron‐) transport material of perovskite solar cells (PSCs). Moreover, the interface effect causes the absorption spectrum of the CsPbI₃/SnS heterostructure an obvious redshift and enhances its absorption ability, which is more suitable for photovoltaic devices. This work suggests that the strain‐introduced interface effect plays a significant role in the interface engineering of the vdW heterostructure between perovskite and 2D materials, which provides a new way to fabricate the high performance perovskite/2D materials heterostructure‐based solar cells and optoelectronic devices.

A team has demonstrated that hybrid halide perovskites crystallize without an inversion center. Interactions between the organic molecules and adjacent iodine atoms can lead to the formation of ferroelectric domains, which, indirectly, can result in higher solar-cell efficiencies. The formation of these ferroelectric domains cannot occur in purely inorganic perovskites.

Publication date: February 2020

Source: Solar Energy Materials and Solar Cells, Volume 205

Author(s): Yu Kawano, Jakapan Chantana, Takahito Nishimura, Takashi Minemoto

In article https://doi.org/10.1002/aenm.2019020651902065, Doo Kyung Moon and co‐workers fabricate flexible organic solar modules, introducing a nonfullerene system via an evaporation‐free all‐solution process. This strategy enables the development of materials with balanced crystallinity, development of multifunctional hole transport layers and a printing method for evaporation‐free large‐area modules. As a result, these flexible organic solar modules exhibit high efficiency of 5.25% and they are potential candidates for industrial applications, for example, building‐integrated photovoltaics.

A general method is developed to synthesize four ternary metal oxides (TMO) with the idea of a proposed concept of constructing the hypocrystalline hydroxide intermediate. An example of the potential applications for the prepared TMOs is demonstrated by using TMO as the hole transport layer for organic solar cell and perovskite solar cells.

Abstract

Solution‐process fine metal‐oxide nanoparticles are promising carrier transport layer candidates for unlocking the full potential of solution process in solar cells, due to their low cost, good stability, and favorable electrical/optical properties. However, exotic organic ligands adopted for achieving small size and monodispersion can mostly cause poor conductivity, which thus impedes their electrical application. In this work, a concept of constructing a hypocrystalline intermediate is proposed to develop a general method for synthesizing various ternary metal oxide (TMO) nanoparticles with a sub‐ten‐nanometer size and good dispersibility without exotic ligands. Particularly, a guideline is summarized based on the understandings about the impact of metal ion intercalation as well as water and anion coordination on the hypocrystalline intermediate. A general method based on the proposed concept is developed to successfully synthesize various sub‐ten‐nanometer TMO nanoparticles with excellent ability for forming high‐quality (smooth and well‐coverage) films. As an application example, the high‐quality films are used as hole transport layers for achieving high‐performance (stability and efficiency) organic/perovskite solar cells. Consequently, this work will contribute to the development of TMO for large‐scale and high‐performance optoelectronic devices and the concept of tailoring intermediate can leverage the fundamental understandings of synthesis strategies for other metal oxides.

Low‐cost and efficient organic small molecules are desired as hole transporting materials for high‐performance perovskite solar cells. Two new molecules containing a benzodithiophene core and triphenylamine side chains are synthesized from cheap starting materials by a simple and low‐cost method. Lead‐free, tin‐based perovskite solar cells employing these new benzodithiophene‐based hole transporting materials achieve good efficiencies.

Abstract

Developing efficient interfacial hole transporting materials (HTMs) is crucial for achieving high‐performance Pb‐free Sn‐based halide perovskite solar cells (PSCs). Here, a new series of benzodithiophene (BDT)‐based organic small molecules containing tetra‐ and di‐triphenyl amine donors prepared via a straightforward and scalable synthetic route is reported. The thermal, optical, and electrochemical properties of two BDT‐based molecules are shown to be structurally and energetically suitable to serve as HTMs for Sn‐based PSCs. It is reported here that ethylenediammonium/formamidinium tin iodide solar cells using BDT‐based HTMs deliver a champion power conversion efficiency up to 7.59%, outperforming analogous reference solar cells using traditional and expensive HTMs. Thus, these BDT‐based molecules are promising candidates as HTMs for the fabrication of high‐performance Sn‐based PSCs.

Hole‐transport material based on dibenzo[b,d]thiophene (DBTMT) is synthesized with low costs. A champion power conversion efficiency of the optimized p–i–n planar perovskite solar cells based on dopant‐free DBTMT reaches 21.12% with a high fill factor of 83.25%, due to good hole‐transport properties and the passivation effect of DBTMT.

N ²,N ²,N ⁸,N ⁸‐tetrakis(4‐(methylthio)phenyl)dibenzo[b,d]thiophene‐2,8‐diamine (DBTMT) is synthesized from three commercial monomers for application as a promising dopant‐free hole‐transport material (HTM) in perovskite solar cells (pero‐SCs). The intrinsic properties (optical properties and electronic energy levels) of DBTMT are investigated, proving that DBTMT is a suitable HTM for the planar p–i–n pero‐SCs. The champion power conversion efficiency (PCE) of the optimized pero‐SCs (with structure as ITO/pristine DBTMT/MAPbI₃/C₆₀/BCP/Ag) reaches 21.12% with a fill factor (FF) of 83.25%, which is among the highest PCEs and FFs reported for planar p–i–n pero‐SCs based on dopant‐free HTMs. The Fourier‐transform infrared spectroscopy, X‐ray diffraction, and X‐ray photoelectron spectroscopy spectra of MAPbI₃ and DBTMT–MAPbI₃ films demonstrate that there is an interaction between DBTMT and MAPbI₃ at the interface through the sulfur atoms in DBTMT to passivate the defects, which is corresponding to the higher FF and PCE of the corresponding device.

Interfaces between the photoactive layer and electrodes play a critical role in ultimate device behaviors in organic bulk heterojunction solar cells (OSCs) and hybrid halide perovskite solar cells (PSCs). Recent progress in interface modification for OSCs and PSCs aimed at improving interfacial charge extraction and mitigating surface recombination, and at enhancing trap passivation and device stability is presented.

Abstract

Organic bulk heterojunction solar cells (OSCs) and hybrid halide perovskite solar cells (PSCs) are two promising photovoltaic techniques for next‐generation energy conversion devices. The rapid increase in the power conversion efficiency (PCE) in OSCs and PSCs has profited from synergetic progresses in rational material synthesis for photoactive layers, device processing, and interface engineering. Interface properties in these two types of devices play a critical role in dictating the processes of charge extraction, surface trap passivation, and interfacial recombination. Therefore, there have been great efforts directed to improving the solar cell performance and device stability in terms of interface modification. Here, recent progress in interfacial doping with biopolymers and ionic salts to modulate the cathode interface properties in OSCs is reviewed. For the anode interface modification, recent strategies of improving the surface properties in widely used PEDOT:PSS for narrowband OSCs or replacing it by novel organic conjugated materials will be touched upon. Several recent approaches are also in focus to deal with interfacial traps and surface passivation in emerging PSCs. Finally, the current challenges and possible directions for the efforts toward further boosts of PCEs and stability via interface engineering are discussed.

An ideal materials combination based on the electron donor BSFTR and acceptor Y6 is selected to construct small‐molecule solar cells (SMSCs). By morphology optimization, an extraordinary power conversion efficiency of 13.69% with a remarkably low energy loss of 0.48 eV is achieved, which is beneficial from the matched photoelectric properties, the favorable blend morphology, and is the best binary SMSC performance reported so far.

Abstract

Compared with the quick development of polymer solar cells, achieving high‐efficiency small‐molecule solar cells (SMSCs) remains highly challenging, as they are limited by the lack of matched materials and morphology control to a great extent. Herein, two small molecules, BSFTR and Y6, which possess broad as well as matched absorption and energy levels, are applied in SMSCs. Morphology optimization with sequential solvent vapor and thermal annealing makes their blend films show proper crystallinity, balanced and high mobilities, and favorable phase separation, which is conducive for exciton dissociation, charge transport, and extraction. These contribute to a remarkable power conversion efficiency up to 13.69% with an open‐circuit voltage of 0.85 V, a high short‐circuit current of 23.16 mA cm⁻² and a fill factor of 69.66%, which is the highest value among binary SMSCs ever reported. This result indicates that a combination of materials with matched photoelectric properties and subtle morphology control is the inevitable route to high‐performance SMSCs.

Ionic conduction in the perovskite oxide La_0.9Sr_0.1Ga_0.95Mg_0.05O_{3– δ} (LSGM) is found to be strongly correlated with crystal structure. A structural design with simultaneously large unit‐cell volume and octahedral rotations for fast ionic conduction is proposed and realized in LSGM superlattice thin films, where the ionic conductivity is tuned with structure alone by a factor of ≈2.5 at 600 °C.

Abstract

Solid‐oxide fuel/electrolyzer cells are limited by a dearth of electrolyte materials with low ohmic loss and an incomplete understanding of the structure–property relationships that would enable the rational design of better materials. Here, using epitaxial thin‐film growth, synchrotron radiation, impedance spectroscopy, and density‐functional theory, the impact of structural parameters (i.e., unit‐cell volume and octahedral rotations) on ionic conductivity is delineated in La_0.9Sr_0.1Ga_0.95Mg_0.05O_{3– δ} . As compared to the zero‐strain state, compressive strain reduces the unit‐cell volume while maintaining large octahedral rotations, resulting in a strong reduction of ionic conductivity, while tensile strain increases the unit‐cell volume while quenching octahedral rotations, resulting in a negligible effect on the ionic conductivity. Calculations reveal that larger unit‐cell volumes and octahedral rotations decrease migration barriers and create low‐energy migration pathways, respectively. The desired combination of large unit‐cell volume and octahedral rotations is normally contraindicated, but through the creation of superlattice structures both expanded unit‐cell volume and large octahedral rotations are experimentally realized, which result in an enhancement of the ionic conductivity. All told, the potential to tune ionic conductivity with structure alone by a factor of ≈2.5 at around 600 °C is observed, which sheds new light on the rational design of ion‐conducting perovskite electrolytes.

Publication date: Available online 6 November 2019

Source: Nano Energy

Author(s): Ligang Xu, Mengyuan Qian, Chi Zhang, Wenzhen Lv, Jibiao Jin, Jinshi Zhang, Chao Zheng, Mingguang Li, Runfeng Chen, Wei Huang

Graphical abstract

Publication date: Available online 5 November 2019

Source: Nano Energy

Author(s): Nabonswende Aida Nadege Ouedraogo, Yichuan Chen, Yue Yue Xiao, Qi Meng, Chang Bao Han, Hui Yan, Yongzhe Zhang

Graphical abstract

Publication date: Available online 2 November 2019

Source: Nano Energy

Author(s): Ying Yang, Tian Chen, Dequn Pan, Jing Gao, Congtan Zhu, Feiyu Lin, Conghua Zhou, Qidong Tai, Si Xiao, Yongbo Yuan, Qilin Dai, Yibo Han, Xie Haipeng, Xueyi Guo

Graphical abstract

An ultrathin functional polymer layer is used to enhance the nucleation of atomic layer deposited (ALD) SnO₂ contacts in metal‐halide perovskite solar cells. These nucleation‐enhanced ALD layers act as “built‐in” barriers to both internal and external degradation pathways, significantly improving the long‐term operational stability of high efficiency unencapsulated devices (>18%) in air.

Abstract

Metal‐halide perovskites show promise as highly efficient solar cells, light‐emitting diodes, and other optoelectronic devices. Ensuring long‐term stability is now a major priority. In this study, an ultrathin (2 nm) layer of polyethylenimine ethoxylated (PEIE) is used to functionalize the surface of C₆₀ for the subsequent deposition of atomic layer deposition (ALD) SnO₂, a commonly used electron contact bilayer for p–i–n devices. The enhanced nucleation results in a more continuous initial ALD SnO₂ layer that exhibits superior barrier properties, protecting Cs_0.25FA_0.75Pb(Br_0.20I_0.80)₃ films upon direct exposure to high temperatures (200 °C) and water. This surface modification with PEIE translates to more stable solar cells under aggressive testing conditions in air at 60 °C under illumination. This type of “built‐in” barrier layer mitigates degradation pathways not addressed by external encapsulation, such as internal halide or metal diffusion, while maintaining high device efficiency up to 18.5%. This nucleation strategy is also extended to ALD VO _x films, demonstrating its potential to be broadly applied to other metal oxide contacts and device architectures.

A simple perovskite solar cell architecture, which is based on dopant‐free electron and hole conductors and carbon back contact deposited at room temperature, is demonstrated. The resulting architecture leads to the fabrication of cheap and highly efficient perovskite solar cells exhibiting unprecedented long‐term operational and UV stability thus hold immense potential for large‐scale deployment.

Abstract

Today's perovskite solar cells (PSCs) mostly use components, such as organic hole conductors or noble metal back contacts, that are very expensive or cause degradation of their photovoltaic performance. For future large‐scale deployment of PSCs, these components need to be replaced with cost‐effective and robust ones that maintain high efficiency while ascertaining long‐term operational stability. Here, a simple and low‐cost PSC architecture employing dopant‐free TiO₂ and CuSCN as the electron and hole conductor, respectively, is introduced while a graphitic carbon layer deposited at room temperature serves as the back electrical contact. The resulting PSCs show efficiencies exceeding 18% under standard AM 1.5 solar illumination and retain ≈95% of their initial efficiencies for >2000 h at the maximum power point under full‐sun illumination at 60 °C. In addition, the CuSCN/carbon‐based PSCs exhibit remarkable stability under ultraviolet irradiance for >1000 h while under similar conditions, the standard spiro‐MeOTAD/Au based devices degrade severely.

The efficiencies of semitransparent perovskite device and four‐terminal perovskite/silicon multijunction/tandem solar cells rise to 18.3% and 27.0%, respectively. This is the highest recorded efficiency for semitransparent perovskite solar cells thus far. The high efficiencies originate from good transparency and high conductivity of the nanomesh‐structured gold top electrode.

Abstract

Multijunction/tandem solar cells have naturally attracted great attention because they are not subject to the Shockley–Queisser limit. Perovskite solar cells are ideal candidates for the top cell in multijunction/tandem devices due to the high power conversion efficiency (PCE) and relatively low voltage loss. Herein, sandwiched gold nanomesh between MoO₃ layers is designed as a transparent electrode. The large surface tension of MoO₃ effectively improves wettability for gold, resulting in Frank–van der Merwe growth to produce an ultrathin gold nanomesh layer, which guarantees not only excellent conductivity but also great optical transparency, which is particularly important for a multijunction/tandem solar cell. The top MoO₃ layer reduces the reflection at the gold layer to further increase light transmission. As a result, the semitransparent perovskite cell shows an 18.3% efficiency, the highest reported for this type of device. When the semitransparent perovskite device is mechanically stacked with a heterojunction silicon solar cell of 23.3% PCE, it yields a combined efficiency of 27.0%, higher than those of both the sub‐cells. This breakthrough in elevating the efficiency of semitransparent and multijunction/tandem devices can help to break the Shockley–Queisser limit.