Nonradiative Recombination Research Articles

Perovskite/silicon tandem solar cells with bilayer interface passivation.

Two-terminal monolithic perovskite/silicon tandem solar cells demonstrate huge advantages in power conversion efficiency compared with their respective single-junction counterparts1,2. However, suppressing interfacial recombination at the wide-bandgap perovskite/electron transport layer interface, without compromising its superior charge transport performance, remains a substantial challenge for perovskite/silicon tandem cells3,4. By exploiting the nanoscale discretely distributed lithium fluoride ultrathin layer followed by an additional deposition of diammonium diiodide molecule, we have devised a bilayer-intertwined passivation strategy that combines efficient electron extraction with further suppression of non-radiative recombination. We constructed perovskite/silicon tandem devices on a double-textured Czochralski-based silicon heterojunction cell, which featured a mildly textured front surface and a heavily textured rear surface, leading to simultaneously enhanced photocurrent and uncompromised rear passivation. The resulting perovskite/silicon tandem achieved an independently certified stabilized power conversion efficiency of 33.89%, accompanied by an impressive fill factor of 83.0% and an open-circuit voltage of nearly 1.97 V. To the best of our knowledge, this represents the first reported certified efficiency of a two-junction tandem solar cell exceeding the single-junction Shockley-Queisser limit of 33.7%.

Performance improvement of ZnO quantum dot-based white light-emitting diodes enabled by an insulating passivation interlayer

In this work, solution-processed white quantum dot light-emitting diodes (WQLEDs) were demonstrated by using the zinc oxide quantum dots (ZnO-QDs) as both a white fluorescent emitter as well as an effective electron injection layer. Meanwhile, a thin insulating passivation layer of polystyrene (PS) was inserted between the ZnO-QDs layer and aluminum cathode to optimize the electron injection into the device and reduce the non-radiative recombination at the interface between ZnO-QDs layer and cathode. Our findings reveal that strategically incorporating a thin PS insulating passivation interlayer between the ZnO-QDs and the aluminum cathode effectively reduces the surface defects of the ZnO-QDs as well as the infiltration of metal atoms into the ZnO-QD layer. Consequently, the WQLEDs with such an insulating PS interlayer exhibit a high brightness of 1076 cd/m2, showing a great improvement of∼40 % compared with that of WQLEDs without PS passivation interlayer (780 cd/m2). This work provides an efficient method to realize single component WQLEDs, thus bringing a feasible solution for next-generation solid-state lighting technologies.

Recycling Single‐Crystal Perovskite Solar Cells With Improved Efficiency and Stability

AbstractMetal halide perovskite single crystals are promising for photovoltaic applications due to their outstanding properties. However, the high surface trap density causes severe nonradiative recombination and ion migration, hindering device performance and stability. Herein, mitigation of the deficient crystal surface is reported by optimized polishing engineering, resulting in stoichiometric lead‐iodine ratio with reduced iodide ion vacancies, increased ion migration activation energy, and suppressed nonradiative recombination. As a result, Cs0.05FA0.95PbI3 (FA = formamidinium) devices exhibit an impressive efficiency of 23.1%, which is one of the highest values for single‐crystal perovskite solar cells (PSCs). Moreover, multiple recycling of the degraded single‐crystal PSCs with higher efficiency and stability is achieved by removing the deteriorated surface, validating crystal surface dominates device degradation while the role of bulk and buried interface is negligible, which is different from polycrystalline devices. The T85 lifetime (remain 85% of initial efficiency) of Cs0.05FA0.95PbI3 devices increases to 1150 h after the recycling process, which is much better than that of previously reported single‐crystal PSCs. Since deficient crystal surface and ion migration are universal issues of perovskite materials, this work will promote the development of stable single‐crystal PSCs and other optoelectronic devices, such as X‐ray detectors, light‐emitting diodes, etc.

Reconstruction and Solidification of Dion-Jacobson Perovskite Top and Buried Interfaces for Efficient and Stable Solar Cells.

Quasi-two-dimensional (Q-2D) perovskites show great potential in the field of photonic and optoelectronic device applications. However, defects and local lattice dislocation still limit performance and stability improvement by nonradiative recombination, unpreferred phase distribution, and unbonded amines. Here, a low-temperature synergistic strategy for both reconstructing and solidifying the perovskite top and buried interface is developed. By post-treating the 1,4-phenylenedimethanammonium (PDMA) based (PDMA)MA4Pb5I16 films with cesium acetate (CsAc) before thermal annealing, a condensation reaction between R-COO- and -NH2 and ion exchange between Cs+ and MA+ occur. It converts the unbonded amines to amides and passivates uncoordinated Pb2+. Meanwhile, it adjusts film composition and improves the phase distribution without changing the out-of-plane grain orientation. Consequently, performance of 18.1% and much-enhanced stability (e.g., stability for photo-oxygen increased over 10 times, light-thermal for T90 over 4 times, and reverse bias over 3 times) of (PDMA)MA4Pb5I16 perovskite solar cells are demonstrated.

Atomic Layer-Deposited Silane Coupling Agent for Interface Passivation of Quantum Dot Light-Emitting Diodes.

Inserting an insulating layer between the charge transport layer (CTL) and quantum dot emitting layer (QDL) is widely used in improving the performance of quantum dot light-emitting diodes (QLEDs). However, the additional layer inevitably leads to energy loss and joule heat. Herein, a monolayer silane coupling agent is used to modify the said interfaces via the self-limiting adsorption effect. Because the ultrathin layers induce negligible series resistance to the device, they can partially passivate the interfacial defects on the electron transport side and help confine the electrons within the QDL on the hole transport side. These interfacial modifications can not only suppress the nonradiative recombination but also slow down the aging of the hole transport layer. The findings here underline a low-temperature adsorption-based strategy for effective interfacial modification which can be used in any layer-by-layer device structures.

Multifaceted Design of Surface Passivator for Upgraded Charge Extraction in Perovskite Solar Cells

The nonradiative recombination arising from the interfaces of perovskite solar cells (PSCs) pose a hurdle, impacting both the efficiency and stability of devices. Functionalized organic molecules can passivate the perovskite surface to suppress the defects and can also fine‐tune the microstructure. This in turn promotes reliability and performance enhancement in solar cells. Using a design protocol, cyanoguanidine diiodide is synthesized and employed as a surface passivator for the fabrication of PSCs, and boosted performance from 20.44% to 23.04% is achieved. This improvement stems from an improved fill factor reaching up to 80.64%, together with the open‐circuit voltage (Voc) measuring 1119 mV. The steady‐state photoluminescence and microstructure of passivated perovskites display significant surface modification of the perovskite film which favorably impacts the charge carrier transfer at the interface of perovskite and Spiro‐OMeTAD. Our findings suggest that improved solar cell performance is due to the synergetic effect of amino and cyano functional groups along with the iodide reservoir in the organic passivator.

Frenkel and Charge-Transfer Excitonic Couplings Strengthened by Thiophene-Type Solvent Enables Binary Organic Solar Cells with 19.8 % Efficiency.

Overcoming the trade-off between short-circuited current (Jsc) and open-circuited voltage (Voc) is important to achieving high-efficiency organic solar cells (OSCs). Previous works modulated the energy gap between Frenkel local exciton (LE) and charge-transfer (CT) exciton, which served as the driving force of exciton splitting. Differently, our current work focuses on the modulation of LE-CT excitonic coupling (tLE-CT) via a simple but effective strategy that the 2-chlorothiophene (2Cl-Th) solvent utilizes in the treatment of OSC active-layer films. The results of our experimental measurements and theoretical simulations demonstrated that 2Cl-Th solvent initiates tighter intermolecular interactions with non-fullerene acceptor in comparison with that of traditional chlorobenzene solvent, thus suppressing the acceptor's over-aggregation and retarding the acceptor crystallization with reduced trap. Critically, the resulting shorter distances between donor and acceptor molecules in the 2Cl-Th treated blend efficiently strengthen tLE-CT, which not only promotes exciton splitting but also reduces non-radiative recombination. The champion efficiencies of 19.8 % (small-area) with superior operational reliability (T80: 586 hours) and 17.0 % (large-area) were yielded in 2Cl-Th treated cells. This work provided a new insight into modulating the exciton dynamics to overcome the trade-off between Jsc and Voc, which can productively promote the development of the OSC field.

Additive engineering for efficient wide-bandgap perovskite solar cells with low open-circuit voltage losses.

High-performance wide-bandgap (WBG) perovskite solar cells are used as top cells in perovskite/silicon or perovskite/perovskite tandem solar cells, which possess the potential to overcome the Shockley-Queisser limitation of single-junction perovskite solar cells (PSCs). However, WBG perovskites still suffer from severe nonradiative recombination and large open-circuit voltage (Voc) losses, which restrict the improvement of PSC performance. Herein, we introduce 3,3'-diethyl-oxacarbo-cyanine iodide (DiOC2(3)) and multifunctional groups (C=N, C=C, C-O-C, C-N) into perovskite precursor solutions to simultaneously passivate deep level defects and reduce recombination centers. The multifunctional groups in DiOC2(3) coordinate with free Pb2+ at symmetric sites, passivating Pb vacancy defects, effectively suppressing nonradiative recombination, and maintaining considerable stability. The results reveal that the power conversion efficiency (PCE) of the 1.68eV WBG perovskite solar cell with an inverted structure increases from 18.51% to 21.50%, and the Voc loss is only 0.487V. The unpackaged device maintains 95% of its initial PCE after 500h, in an N2 environment at 25°C.

An Optimization Path for Sb2(S,Se)3 Solar Cells to Achieve an Efficiency Exceeding 20.

Antimony selenosulfide, denoted as Sb2(S,Se)3, has garnered attention as an eco-friendly semiconductor candidate for thin-film photovoltaics due to its light-absorbing properties. The power conversion efficiency (PCE) of Sb2(S,Se)3 solar cells has recently increased to 10.75%, but significant challenges persist, particularly in the areas of open-circuit voltage (Voc) losses and fill factor (FF) losses. This study delves into the theoretical relationship between Voc and FF, revealing that, under conditions of low Voc and FF, internal resistance has a more pronounced effect on FF compared to non-radiative recombination. To address Voc and FF losses effectively, a phased optimization strategy was devised and implemented, paving the way for Sb2(S,Se)3 solar cells with PCEs exceeding 20%. By optimizing internal resistance, the FF loss was reduced from 10.79% to 2.80%, increasing the PCE to 12.57%. Subsequently, modifying the band level at the interface resulted in an 18.75% increase in Voc, pushing the PCE above 15%. Furthermore, minimizing interface recombination reduced Voc loss to 0.45 V and FF loss to 0.96%, enabling the PCE to surpass 20%. Finally, by augmenting the absorber layer thickness to 600 nm, we fully utilized the light absorption potential of Sb2(S,Se)3, achieving an unprecedented PCE of 26.77%. This study pinpoints the key factors affecting Voc and FF losses in Sb2(S,Se)3 solar cells and outlines an optimization pathway that markedly improves device efficiency, providing a valuable reference for further development of high-performance photovoltaic applications.

A Review on Suppressing Nonradiative Recombination Losses in Antimony Chalcogenide Thin‐Film Solar Cell

Antimony chalcogenide solar cells have captured considerable attention in recent years with an efficiency of over 10%, due to their use of Earth‐abundant materials and superior physical characteristics. Despite these achievements, significant nonradiative recombination processes within these solar cells present a substantial obstacle to further efficiency improvements. Therefore, this review delves into the primary mechanisms responsible for nonradiative recombination losses in antimony chalcogenide solar cells. Additionally, the latest advancements in addressing these losses are summarized. Finally, potential directions for future research efforts aimed at reducing nonrecombination losses and enhancing the overall performance of these devices are outlined.

Minimizing Interfacial Energy Loss and Volatilization of Formamidinium via Polymer-Assisted D-A supramolecular Self-Assembly Interface for Inverted Perovskite Solar Cells with 25.78% Efficiency.

2D perovskite passivation strategies effectively reduce defect-assisted carrier nonradiative recombination losses on the perovskite surface. Nonetheless, severe energy losses are causing by carrier thermalization, interfacial nonradiative recombination, and conduction band offset still persist at heterojunction perovskite/PCBM interfaces, which limits further performance enhancement of inverted heterojunction PSCs. Here, 5,10,15,20-tetrakis(pentafluorophenyl)porphyrin (5FTPP) is introduced between 3D/2D perovskite heterojunction and PCBM. Compared to tetraphenylporphyrin without electron-withdrawing fluoro-substituents, 5FTPP can self-assemble with PCBM at interface into donor-acceptor (D-A) complex with stronger supramolecular interaction and lower energy transfer losses. This rapid energy transfer from donor (5FTPP) to acceptor (PCBM) within femtosecond scale is demonstrated to enlarge hot carrier extraction rates and ranges, reducing thermalization losses. Furthermore, the incorporation of polystyrene derivative (PD) reinforces D-A interaction by inhibiting self-π-π stacking of 5FTPP, while fine-tuning conduction band offset and suppressing interfacial nonradiative recombination via Schottky barrier, dipole, and n-doping. Notably, the multidentate anchoring of PD-5FTPP with FA+, Pb2+, and I- mitigates the adverse effects of FA+ volatilization during thermal stress. Ultimately, devices with PD-5FTPP achieve a power conversion efficiency of 25.78% (certified: 25.36%), maintaining over 90% of initial efficiency after 1000 h of continuous illumination at the maximum power point (65°C) under ISOS-L-2 protocol.

Suppressed Defects by Functional Thermally Cross-Linked Fullerene for High-Efficiency Tin-Lead Perovskite Solar Cells.

Mixed tin-lead (Sn-Pb) perovskites have attracted the attention of the community due to their narrow bandgap, ideal for photovoltaic applications, especially tandem solar cells. However, the oxidation and rapid crystallization of Sn2+ and the interfacial traps hinder their development. Here, cross-linkable [6,6]-phenyl-C61-butyric styryl dendron ester (C-PCBSD) is introduced during the quenching step of perovskite thin film processing to suppress the generation of surface defects at the electron transport layer interface and improve the bulk crystallinity. The C-PCBSD has strong coordination ability with Sn2+ and Pb2+ perovskite precursors, which retards the crystallization process, suppresses the oxidation of Sn2+, and improves the perovskite bulk and surface crystallinity, yielding films with reduced nonradiative recombination and enhanced interface charge extraction. Besides, the C-PCBSD network deposited on the perovskite surface displays superior hydrophobicity and oxygen resistance. Consequently, the devices with C-PCBSD obtain PCEs of up to 23.4% and retained 97% of initial efficiency after 2000h of storage in a N2 atmosphere.

SnSe2 Quantum Dots and Chlorhexidine Acetate Suppress Synergistically Non-radiative Recombination Loss for High Efficiency and Stability Perovskite Solar Cells.

Non-radiative recombination losses limit the property of perovskite solar cells (PSCs). Here, a synergistic strategy of SnSe2QDs doping into SnO2 and chlorhexidine acetate (CA) coating on the surface of perovskite is proposed. The introduction of 2D SnSe2QDs reduces the oxygen vacancy defects and increases the carrier mobility of SnO2. The optimized SnO2 as a buried interface obviously improves the crystallization quality of perovskite. The CA containing abundant active sites of ─NH2/─NH─, ─C═N, CO, ─Cl groups passivate the defects on the surface and grain boundary of perovskite. The alkyl chain of CA also improves the hydrophobicity of perovskite. Moreover, the synergism of SnSe2QDs and CA releases the residual stress and regulates the energy level arrangement at the top and bottom interface of perovskite. Benefiting from these advantages, the bulk and interface non-radiative recombination loss is greatly suppressed and thereby increases the carrier transport and extraction in devices. As a result, the best power conversion efficiency (PCE) of 23.41% for rigid PSCs and the best PCE of 21.84% for flexible PSCs are reached. The rigid PSC maintains 89% of initial efficiency after storing nitrogen for 3100 h. The flexible PSCs retain 87% of the initial PCE after 5000 bending cycles at a bending radius of 5 mm.

Machine learning for screening and predicting the best surface modifiers for a rational optimization of efficient perovskite solar cells

The key to keep the rising slope of perovskite solar cell performances is to reduce non-radiative losses by minimizing defect density. To this end, a large variety of strategies have been adopted spanning from the use of interfacial layers, surface modifiers, to interface engineering. Although winning concepts have been demonstrated, they result from a mere trial and error approach, which is time consuming and operator-dependent. To face this challenge, in this work, we propose the use of a machine learning approach for an educated and rational material screening with optimal characteristics in terms of surface passivation. In particular, we applied Shapley additive explanation to extract the specific chemical features of the passivator, which directly impact the device parameters, specifically the open circuit voltage (Voc). By monitoring the different material parameters as input, we were able to list the most promising passivators and directly test them in working solar cells. By comparing the device performances with the results of the modeling and with additional optical and morphological characterization, we retrieved the most significant material properties linked to the highest efficiency, which are (i) the presence of chlorine and its strong binding capacity to positively charged defects on perovskite surface, reducing the non-radiative recombination and (ii) an increased flexibility of the molecule, resulting in better coverage of the surface. Finally, we tested the predictive power of the ML algorithm proposing a new passivator, which, implemented in a working device, leads to the predicted high Voc confirming the results of the modeling.

Investigation of the growth rate on optical and crystal quality of InGaAs/AlGaAs multi-quantum wells and InGaAs single layer grown by molecular beam epitaxy (MBE)

The impact of growth rate on the optical and crystal quality of InGaAs/AlGaAs multi-quantum wells (MQWs) and InGaAs single layer grown by molecular beam epitaxy (MBE) is studied. Photoluminescence (PL) and high-resolution X-ray diffraction (HRXRD) are applied for evaluation of the optical, crystal quality and interfaces smoothness. The room-temperature PL integral intensity increases by 220 % when the growth rate decreases from 2 to 1 Å/s. HRXRD analysis reveals the growth rate of 1 Å/s improves crystal and interface quality of MQWs, as well as significantly enhances PL intensity. But further reduce growth rate to 0.5 Å/s, the PL integral intensity decreases, instead. At lower growth rate, more impurities can incorporate into InGaN layer and act as nonradiative recombination centers. Growth rate can effectively control crystal quality, interfaces smoothness and impurity content and thus determine the optical quality of InGaAs/AlGaAs MQWs.

Elucidating the Role of Alkali Metal Carbonates in Impact on Oxygen Vacancies for Efficient and Stable Perovskite Solar Cells.

Effectively suppressing nonradiative recombination at the SnO2/perovskite interface is imperative for perovskite solar cells. Although the capabilities of alkali salts at the SnO2/perovskite interface have been acknowledged, the effects and optimal selection of alkali metal cations remain poorly understood. Herein, a novel approach for obtaining the optimal alkali metal cation (A-cation) at the interface is investigated by comparatively analyzing different alkali carbonates (A2CO3; Li2CO3, Na2CO3, K2CO3, Rb2CO3, and Cs2CO3). Theoretical calculations demonstrate that A2CO3 coordinates with undercoordinated Sn and O on the surface, effectively mitigating oxygen vacancy (VO) defects with increasing A-cation size, whereas Cs2CO3 exhibits diminished preferability owing to enhanced steric hindrance. The experimental results highlight the crucial role of Rb2CO3 in actively passivating VO defects, forming a robust bond with SnO2, and facilitating Rb+ diffusion into the perovskite layer, thereby enhancing charge extraction, alleviating deep-level trap states and structural distortion in the perovskite film, and significantly suppressing nonradiative recombination. X-ray absorption spectroscopy analyses further reveal the effect of Rb2CO3 on the local structure of the perovskite film. Consequently, a Rb2CO3-treated device with aperture area of 0.14 cm2 achieves a notable efficiency of 22.10%, showing improved stability compared to the 20.11% achieved for the control device.

Magnetic field-augmented photoelectrochemical water splitting in Co3O4 and NiO nanorod arrays

Effective charge separation is crucial for improving the sensitivity of photoelectrochemical studies. Here, we provide an immense magnetic field-based electron spin polarization approach for an efficient charge carrier separation. We have fabricated NiO and Co3O4 thin film and nanorod arrays by electron beam evaporation glancing angle method followed by annealing in a two-zone furnace. The photoelectrochemical performance was investigated for NiO and Co3O4 samples in the presence and absence of a magnetic field. The NiO and Co3O4 nanorods array samples exhibit better absorption compared with the thin film samples. The Co3O4 and NiO nanorod arrays showed the highest photocurrent density of 0.12 and 0.55 mA/cm2 in a magnetic field. The superior photoelectrochemical response of NiO and Co3O4 nanorods in a magnetic field could be ascribed to the limitation of non-radiative recombination of carriers manipulated by Lorentz force and spin polarization. Furthermore, the electrochemical impedance spectra of NiO and Co3O4 nanorod arrays in a magnetic field show the least charge transfer resistance. This study sheds light on the interaction process between external fields and radiative/non-radiative recombination of manipulating carriers. Thus, the application of a magnetic field presents an efficient and versatile approach to enhance the performance of photoelectrodes in solar water splitting.

Regulating thermal management by a CsPbClBr2/Ag hybrid microcavity for stable room temperature blue lasing with low threshold

Realization of long-term stable lasing from all-inorganic perovskite supercrystals is highly desirable for practical applications in optoelectronic devices. However, lasing from perovskite supercrystals excited by continuous wave laser light remains a challenge due to the photoluminescence degradation induced by thermal accumulation. Here, we report highly stable lasing with low threshold fom a CsPbClBr2 supercrystal placed on a thin Ag film, which form a CsPbClBr2/Ag microcavity, by managing the thermal distribution inside the CsPbClBr2 supercrystal. Combined numerical simulations and lifetime measurements, the localized electric field in such a hybrid microcavity leads to a spatially localized temperature distribution, which plays a crucial role in suppressing the thermal accumulation on the surface and in eliminating non-radiative recombination defects. The effective thermal management in the hybrid microcavity renders highly stable lasing with low threshold under the irradiation of continuouw wave laser light. Our findings provide a feasible and universal approach to the development of long-term stable perovskite laser.

Regulating Electron-Phonon Coupling by Solid Additive for Efficient Organic Solar Cells.

Strong electron-phonon couplingcan hinder excitontransport andinduce undesirable non-radiative recombination, resulting in a shortened exciton diffusion distance and constrainedexciton dissociation in organic solar cells (OSCs). Therefore, suppressingelectron-phonon coupling is crucially important for achieve high-performanceOSCs. Here, we employ the solid additive to regulating electron-phonon coupling in OSCs. The planar configuration of SA1 confers a significant advantage in suppressing lattice vibrations in the active layers, reducingthe scattering of excitons by phonons caused by lattice vibrations. Consequently, a slow but sustained hole transfer process is identified in the SA1-assisted film, indicating an enhancement in hole transfer efficiency.Prolongedexciton diffusion length and exciton lifetime are achieved in theblend film processed with SA1, attributed to a low non-radiative recombination rateand low energetic disorderfor charge carrier transport. As a result,a highefficiencyof20% was achieved for ternary device with a remarkable short-circuit current. This work highlights the important role of suppressing electron-phonon coupling in improving the photovoltaic performance of OSCs.

Propylammonium chloride passivation for efficient carbon-electrode FA0.1MA0.9PbI3 solar cells

Carbon-based perovskite solar cells (C-PSCs) are garnering considerable attention in the photovoltaic realm due to their cost-effectiveness, simplified fabrication processes, and improved long-term durability. Nonetheless, their efficiency often suffers from notable non-radiative recombination at the interface of the carbon electrode and the perovskite layer, as well as inherent film defects. This investigation adopts additive engineering to address these challenges by introducing propylammonium chloride (PACl) into FA0.1MA0.9PbI3 perovskite films. The resultant films exhibit larger grain sizes and smoother surface morphology, mitigating grain boundary defects and enhancing interface quality. Additionally, PACl-treated films demonstrate heightened photoluminescence intensity and prolonged carrier lifetimes, effectively suppressing non-radiative recombination. Comparative analysis with control devices showcases a noteworthy efficiency boost in PACl-treated devices, rising from 14.74 % to 16.57 %, alongside minimal hysteresis effects and exemplary long-term stability. This study presents a simple yet highly efficient approach to enhance film morphology and rectify defects in perovskite films, leading to superior efficiency and stability in hole transport layer free C-PSCs.