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Meng, Dong

Publications and source records attributed to Meng, Dong.

Suppressing ion migration in metal halide perovskite via interstitial doping with a trace amount of multivalent cations

Cations with suitable sizes to occupy an interstitial site of perovskite crystals have been widely used to inhibit ion migration and promote the performance and stability of perovskite optoelectronics. However, such interstitial doping inevitably leads to lattice microstrain that impairs the long-range ordering and stability of the crystals, causing a sacrificial trade-off. Here, we unravel the evident influence of the valence states of the interstitial cations on their efficacy to suppress the ion migration. Incorporation of a trivalent neodymium cation (Nd 3+ ) effectively mitigates the ion migration in the perovskite lattice with a reduced dosage (0.08%) compared to a widely used monovalent cation dopant (Na + , 0.45%). As a result, the photovoltaic performances and operational stability of the prototypical perovskite solar cells are enhanced with a trace amount of Nd 3+ doping while minimizing the sacrificial trade-off.

36 MATERIALS SCIENCE↗

Stability-limiting heterointerfaces of perovskite photovoltaics

Optoelectronic devices consist of heterointerfaces formed between dissimilar semiconducting materials. The relative energy level alignment between contacting semiconductors determinately affects the heterointerface charge injection and extraction dynamics. For perovskite solar cells (PSCs), the heterointerface between the top perovskite surface and a charge-transporting material (CTM) is often treated for defect passivation to improve PSC stability and performance. However, such surface treatments could also affect the heterointerface energetics. Here we show that surface treatments may induce a negative work function shift (i.e. more n-type), which activates halide migration to aggravate PSC instability. Therefore, despite the beneficial effects of surface passivation, this detrimental side effect limits the maximum stability improvement attainable for PSCs treated in these ways. Furthermore, this trade-off between the beneficial and detrimental effects should guide further work on improving PSC stability via surface treatments.

14 SOLAR ENERGY↗

Wide-Gap Perovskite via Synergetic Surface Passivation and Its Application toward Efficient Stacked Tandem Photovoltaics

Superior bandgap tunability enables solution-processed halide perovskite a promising candidate for multi-junction photovoltaics (PVs). Particularly, optically coupling wide-gap perovskite by stacking with commercially available PVs such as silicon and CIGS (also known as 4-terminal tandem) simplifies the technology transfer process, and further advances the commercialization potential of perovskite technology. However, compared with matured PV materials and the phase-pure FAPbI 3 , wide-gap perovskite still suffers from huge voltage deficits. Here, the authors take advantage of the synergetic effect behind a sequential fluoride and organic ammonium salt surface passivation strategy to control non-radiative energy losses, and obtained a 17.7% efficiency in infrared-transparent wide-gap perovskite solar cells (21.1% for opaque device), and achieved efficiencies of over 25% when stacked with commercial Si and CIGS products with original PCEs of 18–20% under a 4-terminal working condition.

36 MATERIALS SCIENCE↗

Reconfiguring the band-edge states of photovoltaic perovskites by conjugated organic cations

The band edges of metal-halide perovskites with a general chemical structure of ABX 3 (A, usually a monovalent organic cation; B, a divalent cation; and X, a halide anion) are constructed mainly of the orbitals from B and X sites. Hence, the structural and compositional varieties of the inorganic B–X framework are primarily responsible for regulating their electronic properties, whereas A-site cations are thought to only help stabilize the lattice and not to directly contribute to near-edge states. We report a π-conjugation–induced extension of electronic states of A-site cations that affects perovskite frontier orbitals. The π-conjugated pyrene-containing A-site cations electronically contribute to the surface band edges and influence the carrier dynamics, with a properly tailored intercalation distance between layers of the inorganic framework. Lastly, the ethylammonium pyrene increased hole mobilities, improved power conversion efficiencies relative to that of a reference perovskite, and enhanced device stability.

36 MATERIALS SCIENCE↗

Molecular Interaction Regulates the Performance and Longevity of Defect Passivation for Metal Halide Perovskite Solar Cells

Defect passivation constitutes one of the most commonly used strategies to fabricate highly efficient perovskite solar cells (PSCs). However, the durability of the passivation effects under harsh operational conditions has not been extensively studied regardless of the weak and vulnerable secondary bonding between the molecular passivation agents and perovskite crystals. Here, we incorporated strategically designed passivating agents to investigate the effect of their interaction energies on the perovskite crystals and correlated these with the performance and longevity of the passivation effects. We unraveled that the passivation agents with a stronger interaction energy are advantageous not only for effective defect passivation but also to suppress defect migration. The prototypical PSCs treated with the optimal passivation agent exhibited superior performance and operational stability, retaining 81.9 and 85.3% of their initial performance under continuous illumination or nitrogen at 85 °C after 1008 h, respectively, while the reference device completely degraded during that time. Furthermore, this work provides important insights into designing operationally durable defect passivation agents for perovskite optoelectronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗