Rationalization of passivation strategies toward high-performance perovskite solar cells

Chemical Society Reviews, Год журнала: 2022, Номер 52(1), С. 163 - 195

Опубликована: Дек. 1, 2022

Lead halide perovskite solar cells (PSCs) have shown unprecedented development in efficiency and progressed relentlessly improving stability. All the achievements been accompanied by diverse passivation strategies to circumvent pervasive defects materials, which play crucial roles process of charge recombination, ion migration, component degradation. Among tremendous efforts made solve these issues achieve high-performance PSCs, we classify review both well-established burgeoning provide further guidance for protocols including chemical eliminate formation bonds, physical strain relaxation or treatments, energetic improve stability toward light oxygen, field-effect regulate interfacial carrier behavior. The subtle but non-trivial consequences from various need advanced characterization techniques combining synchrotron-based X-ray analysis, capacitance-based measurements, spatially resolved imaging, fluorescent molecular probe, Kelvin probe force microscope, etc., scrutinize mechanisms. In end, challenges prospective research directions on advancing are proposed. Judicious combinations among chemical, physical, energetic, deserve more attention future high-efficiency stable photovoltaics.

Язык: Английский

---

Structural Disorder in Higher-Temperature Phases Increases Charge Carrier Lifetimes in Metal Halide Perovskites

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(41), С. 19137 - 19149

Опубликована: Окт. 7, 2022

Solar cells and optoelectronic devices are exposed to heat that degrades performance. Therefore, elucidating temperature-dependent charge carrier dynamics is essential for device optimization. Charge lifetimes decrease with temperature in conventional semiconductors. The opposite, anomalous trend observed some experiments performed MAPbI3 (MA = CH3NH3+) other metal halide perovskites. Using ab initio quantum simulation, we establish the atomic mechanisms responsible nonradiative electron-hole recombination orthorhombic-, tetragonal-, cubic MAPbI3. We demonstrate structural disorder arising from phase transitions as important due heating same phase. grow both increasing upon transition higher-temperature phases. increased lifetime rationalized by induces partial localization, decreases nonadiabatic coupling, shortens coherence. Inelastic elastic electron-vibrational interactions exhibit opposite dependence on localization arise thermal motions of inorganic lattice organic cations depend significantly deformations induced fluctuations order defects, hence, plays a very role. Since increases but inhibits transport, an optimal regime maximizing diffusion can be designed, depending phase, temperature, material morphology, architecture. atomistic enhanced at elevated temperatures provide guidelines design improved solar energy materials.

Язык: Английский

---

A brief review on metal halide perovskite photocatalysts: History, applications and prospects

Journal of Alloys and Compounds, Год журнала: 2022, Номер 911, С. 165062 - 165062

Опубликована: Апрель 19, 2022

Язык: Английский

---

Mechanistic Understanding of Oxidation of Tin‐based Perovskite Solar Cells and Mitigation Strategies

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(45)

Опубликована: Авг. 1, 2023

Abstract Tin (Sn)‐based perovskites as the most promising absorber materials for lead‐free perovskite solar cells (PSCs) have achieved record efficiency of over 14 %. Although suppressing oxidation Sn‐based is a frequently concerned topic PSCs, many studies given vague explanations and mechanisms are still under debate. This in principal due to lack an in‐depth understanding various complex intrinsic extrinsic factors causing process. In this context, we critically review chemical mechanism facile differentiate its detrimental effects at material‐ device‐level. More importantly, classify introduce (raw solvent precursors) (exposure neutral oxygen superoxide) with their corresponding anti‐oxidation improvement methods. The presented comprehensive prospect provide insightful guidance PSCs “from beginning end”.

Язык: Английский

---

Twist Angle-Dependent Intervalley Charge Carrier Transfer and Recombination in Bilayer WS₂

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(41), С. 22826 - 22835

Опубликована: Окт. 5, 2023

A twist angle at a van der Waals junction provides handle to tune its optoelectronic properties for variety of applications, and comprehensive understanding how the modulates electronic structure, interlayer coupling, carrier dynamics is needed. We employ time-dependent density functional theory nonadiabatic molecular elucidate angle-dependent intervalley transfer recombination in bilayer WS2. Repulsion between S atoms twisted configurations weakens increases distance, softens layer breathing modes. Twisting has minor influence on K valleys while it lowers Γ raises Q because their wave functions are delocalized layers. Consequently, reduced energy gaps accelerate hole structures. Intervalley electron proceeds nearly an order magnitude faster than transfer. The more localized values larger bandgaps result smaller couplings recombination, making 3-4 times slower high-symmetry B2g breathing, E2g in-plane, A1g out-of-plane modes most active during recombination. extended lifetimes junctions favorable device performance.

Язык: Английский

---

Indium Iodide Additive Realizing Efficient Mixed Sn─Pb Perovskite Solar Cells

Advanced Energy Materials, Год журнала: 2024, Номер 14(17)

Опубликована: Янв. 28, 2024

Abstract Low‐bandgap mixed tin (Sn)‐lead (Pb) perovskite solar cells promise efficiency beyond the pure‐Pb ones. However, difference in interaction rate of SnI 2 and PbI with organic salts causes spatial distribution heterogeneity Sn 2+ Pb Sn─Pb layers. This a Sn‐rich surface, which can trigger more severe oxidation nonradiative recombination. A strategy, introducing indium ion (In 3+ ) into precursor solution to compete when reacting is developed. Therefore, nucleation crystallization films are well‐controlled, leading improved film quality balanced Sn/Pb ratio on surface. Additionally, In has lower reduction potential compared generate an extra energy barrier for oxidation. The reduced surface result accelerated electron transfer carrier recombination rate. modified devices achieve power conversion (PCE) 23.34%, representing one highest PCEs made PCBM.

Язык: Английский

---

Compression of Organic Molecules Coupled with Hydrogen Bonding Extends the Charge Carrier Lifetime in BA₂SnI₄

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(23), С. 16314 - 16323

Опубликована: Май 30, 2024

Two-dimensional (2D) metal halide perovskites, such as BA2SnI4 (BA═CH3(CH2)3NH3), exhibit an enhanced charge carrier lifetime in experiments under strain. Experiments suggest that significant compression of the BA molecule, rather than inorganic lattice, contributes to this enhancement. To elucidate underlying physical mechanism, we apply a moderate compressive strain entire system and subsequently introduce molecules. We then perform ab initio nonadiabatic molecular dynamics simulations nonradiative electron–hole recombination. observe overall lattice reduces atomic motions decreases coupling, thereby delaying Additionally, molecules enhances hydrogen bonding between iodine atoms, which lengthens Sn–I bonds, distorts [SnI6]4– octahedra, suppresses further, thus reducing coupling. Also, elongated bonds weakened antibonding interactions increase band gap. Altogether, delays recombination by more factor 3. Our provide new valuable insights into how strain, accommodated primarily organic ligands, positively influences optoelectronic properties 2D layered offering promising pathway for further performance improvements.

Язык: Английский

---

Reducing Nonradiative Recombination in Halide Perovskites through Appropriate Band Gaps and Heavy Atomic Masses

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер unknown, С. 1253 - 1260

Опубликована: Янв. 26, 2025

Halide perovskite optoelectronic devices achieve high energy conversion efficiencies. However, their efficiency decreases significantly with an increase in temperature. This decline is likely caused by changes nonradiative recombination and electron-phonon coupling, which remain underexplored. When the lattice temperature increases, anharmonicity induces level fluctuation band gap narrowing modulating interactions. As vibrations intensify, high-frequency phonons progressively dominate carrier dynamic processes halide perovskites, thereby strengthening coupling between electronic subsystem phonons. The increased overlap of electron wave functions strengthens non-adiabatic accelerating process. On basis these findings, we propose introduction appropriate materials heavy atoms at B-site X-site to modulate mitigating enhancing solar cell performance.

Язык: Английский

---

Extending Carrier Lifetimes of Metal Halide Perovskites by Defect Passivation with Alkaline Earth Metals: A Time-Domain Study

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер 16(9), С. 2438 - 2444

Опубликована: Фев. 27, 2025

Intrinsic defects that serve as non-radiative recombination centers significantly accelerate charge and energy losses in hybrid organic-inorganic perovskites. The defect IMA, formed by replacing an MA with I MAPbI3 (MA = CH3NH3+), creates trimer produces a deep electron trap state. Non-adiabatic (NA) molecular dynamics simulations demonstrate excited conduction band is rapidly captured this within 100 ps, followed valence hole 1 ns, which 3 times faster than the pristine system. Doping interstitial Sr Ba eliminates state breaking trimer, thereby restoring electron-hole across bandgap to durations up 3.20 4.36 respectively. delayed attributed decreased NA coupling shortened decoherence time. These findings provide critical insights into perovskite passivation strategies alkaline earth metals.

Язык: Английский

---

Ultrafast Charge Transfer and Delayed Recombination in Graphitic-CN/WTe₂ van der Waals Heterostructure: A Time Domain Ab Initio Study

The Journal of Physical Chemistry Letters, Год журнала: 2022, Номер 13(34), С. 7898 - 7905

Опубликована: Авг. 18, 2022

In search of an efficient solar energy harvester, we herein performed a time domain density functional study coupled with nonadiabatic molecular dynamics (NAMD) simulation to gain atomistic insight into the charge carrier graphitic carbon nitride (g-CN)-tungsten telluride (WTe2) van der Waals heterostructure. Our NAMD predicted ultrafast electron (589 fs) and hole-transfer (807 in g-CN/WTe2 heterostructure delayed electron-hole recombination process (2.404 ns) as compared that individual g-CN (3 ps) WTe2 (0.55 monolayer. The transfer is due strong electron-phonon coupling during charge-transfer while comparatively weak coupling, sufficient band gap, lower (NAC), fast decoherence slow down process. results exciton relaxation are valuable for insightful understanding designing photovoltaic devices based on organic-inorganic 2D heterostructures.

Язык: Английский

---