Moderate Humidity Delays Electron–Hole Recombination in Hybrid Organic–Inorganic Perovskites: Time-Domain Ab Initio Simulations Rationalize Experiments

Long, Run; Fang, Wei‐Hai; Prezhdo, Oleg V.

doi:10.1021/acs.jpclett.6b01412

Cited by 141 publications

(153 citation statements)

References 68 publications

(163 reference statements)

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“…Ab initio NAMD combined with TDDFT were performed to investigate the influence of different levels of humidity on nonradiative electron‐hole recombination at the MAPbI 3 (001) surface with a varying number of adsorbed water molecules . The study demonstrated that moderate humidity extends the excited‐state lifetime, while heavy humidity reduces the lifetime, in agreement with experiments.…”

Section: Photoexcitation Dynamicssupporting

confidence: 60%

“…We show why a grain boundary accelerates charge recombination in the CH 3 NH 3 PbI 3 (MAPbI 3 ) perovskite, and why chlorine passivation of the boundary extends the excited‐state lifetime . We demonstrate that moderate humidity delays electron‐hole recombination in MAPbI 3 and that heavy humidity accelerates the recombination . We analyze in detail how dopants control electron‐hole recombination at a MAPbI 3 /TiO 2 interface and suggest a route to suppress the charge and energy losses via a rational choice of dopants .…”

Section: Photoexcitation Dynamicsmentioning

confidence: 93%

“…The nonadiabatic coupling is larger and the decay is faster when water maintains a continuous hydrogen‐bonded network, e.g., 8H 2 O. Adapted from Ref . J Phys Chem Lett 7 , 3215 (2016).…”

Section: Photoexcitation Dynamicsmentioning

confidence: 99%

“…The present review introduces briefly the computational methodologies underlying the time‐domain ab initio calculations of the photo‐induced dynamics in nanoscale materials and interfaces, and then discusses charge separation and recombination in a variety of systems . In particular, focusing on charge separation, we show that metallic graphene can be used as a light harvester, and that the photoexcited hot electron can be extracted from PbSe QDs into TiO 2 before cooling .…”

Section: Introductionmentioning

confidence: 99%

“…Focusing on charge recombination, we show how grain boundaries (GBs) accelerate electron‐hole recombination in perovskite CH 3 NH 3 PbI 3 (MAPbI 3 ), and how humidity can have both positive and negative influence on perovskite MAPbI 3 excited state properties . We demonstrate how dopants can be used to control electron‐hole recombination across a MAPbI 3 /TiO 2 interface, and how defects slow down electron‐hole recombination in black phosphorus (BP) .…”

Section: Introductionmentioning

confidence: 99%

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Nonadiabatic charge dynamics in novel solar cell materials

Long

Prezhdo

Fang

2017

WIREs Comput Mol Sci

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The review describes recent research into the nonequilibrium phenomena in nanoscale materials, with focus on charge separation and recombination, that form the basis for photovoltaic and photocatalytic devices. Nonadiabatic molecular dynamics combined with ab initio real-time time-dependent density functional theory enable us to model time-resolved laser experiments at the atomistic level, emphasizing realistic aspects of the materials, such as defects, dopants, boundaries, chemical bonding, etc. A variety of systems have been considered, including bulk semiconductors sensitized by semiconducting/metallic nanoparticles and graphene, nanocrystal/molecule junctions, polymer interfaces with carbon nanotubes and nanoclusters, van der Waals heterojunctions, black phosphorus, and hybrid organic-inorganic perovskites. The detailed atomistic knowledge obtained from the explicit time-domain modeling generates comprehensive understanding of electron-vibrational dynamics in complex multicomponent systems, provides critical insights into quantum mechanical transport of energy and charge, and leads to valuable guidelines for improvement of solarto-electric power conversion in photovoltaic and photocatalytic applications and for efficient performance of transport devices. FIGURE 14 | Decay of populations of the first excited state in bilayer black phosphorus (BP) and at the BP/MoS 2 interface. BP/MoS 2 shows slower decay because of electron-hole separation across the interface.

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Section: Photoexcitation Dynamicssupporting

confidence: 60%

Section: Photoexcitation Dynamicsmentioning

confidence: 93%

“…The nonadiabatic coupling is larger and the decay is faster when water maintains a continuous hydrogen‐bonded network, e.g., 8H 2 O. Adapted from Ref . J Phys Chem Lett 7 , 3215 (2016).…”

Section: Photoexcitation Dynamicsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Nonadiabatic charge dynamics in novel solar cell materials

Long

Prezhdo

Fang

2017

WIREs Comput Mol Sci

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Heavy Water Additive in Formamidinium: A Novel Approach to Enhance Perovskite Solar Cell Efficiency

Solanki

Tavakoli

et al. 2020

Advanced Materials

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Heavy water or deuterium oxide (D2O) comprises deuterium, a hydrogen isotope twice the mass of hydrogen. Contrary to the disadvantages of deuterated perovskites, such as shorter recombination lifetimes and lower/invariant efficiencies, the serendipitous effect of D2O as a beneficial solvent additive for enhancing the power conversion efficiency (PCE) of triple‐A cation (cesium (Cs)/methylammonium (MA)/formaminidium (FA)) perovskite solar cells from ≈19.2% (reference) to 20.8% (using 1 vol% D2O) with higher stability is reported. Ultrafast optical spectroscopy confirms passivation of trap states, increased carrier recombination lifetimes, and enhanced charge carrier diffusion lengths in the deuterated samples. Fourier transform infrared spectroscopy and solid‐state NMR spectroscopy validate the N–H2 group as the preferential isotope exchange site. Furthermore, the NMR results reveal the induced alteration of the FA to MA ratio due to deuteration causes a widespread alteration to several dynamic processes that influence the photophysical properties. First‐principles density functional theory calculations reveal a decrease in PbI6 phonon frequencies in the deuterated perovskite lattice. This stabilizes the PbI6 structures and weakens the electron–LO phonon (Fröhlich) coupling, yielding higher electron mobility. Importantly, these findings demonstrate that selective isotope exchange potentially opens new opportunities for tuning perovskite optoelectronic properties.

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Quantum Dots Encapsulated by ZrO₂ Enhance the Stability of Perovskite Solar Cells

Wang

Yao

Shen

et al. 2021

Adv Materials Inter

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rier recombination [15][16][17][18][19][20] thereby restricting PSCs performance. In addition, water and oxygen in the ambient degrades the performance of PSCs devices through the defects. Therefore, passivation surface defects are one of the methods to improve the stability and device performance of PSCs simply and efficiently. [21][22][23][24] Interface engineering is an effective way to overcome interfacial recombination and improve the performance of PSCs devices. The size and quality of perovskite grain are urgent problems, Lewis acid, [25,26] Lewis base, [20,27] and organic materials [28,29] were developed for passivating the defects through regulating the grain size as the passivation agents. Recently, quantum dots (QDs) passivation has been applied to PSCs to reduce interface defects by filling holes. [30][31][32] QDs were introduced into the PSCs interface engineering as a significant passivation method that can reduce the non-radiative recombination. But the stability of QDs is still an important factor that plagues modification strategies. They are easily decomposed in harsh environments such as humid air. Commonly, polymers, shells, and semiconductors were introduced into the QDs structure to increase the stability and optical properties. Later, the structure of composite QDs compounds was developed. Composite CsPbBr 3 /MoS 2 [33] has been fabricated, corresponding to similar compounds which have also been reported such as CsPbBr 3 /TiO 2 [34,35] and CsPbBr 3 / SiO 2 . [36,37] Zheng et al. [38] construed the CsPbI 3 /Mg x Zn 1-x Te the high-quality, functional nanocomposites. This strategy was proved to improve charge diffusion and separation causing better optical properties. Recently, ZrO 2 has been introduced to composite QDs due to its chemical stability and easy solution processing. Thereby the combination of QDs and ZrO 2 attracts attention ascribed to boosting the performance of the device of composite QDs/ZrO 2 structure. [39] In this study, we use ZrO 2 , as the interface modification layer, to encapsulate the QDs. We obtain the ZrO 2 sol by hydrolysis reaction. [40] Zirconium n-propoxide is hydrolyzed by trace water in n-propanol and toluene to get ZrOH and ZrOC 3 H 7 which interact to form ZrO 2 sol. Acetic acid was added to prevent precipitation. The ZrO 2 sol formed mesh interpenetration structure to encapsulate QDs. The CsPbBr 1.5 I 1.5 /ZrO 2 nanostructure improved the performance and stability of PSCs device with the functions of surface passivation and withstanding harsh environments. The QDs can also modify the morphology and passivating the surface defect. The champion performance of the device based on CsPbBr 1.5 I 1.5 /ZrO 2 achieves a significantly PCE of 21.23%, in contrast to the control device with a PCE In the last several years, perovskite solar cells (PSCs) are faced with big problems in the stability issues, which also occur in the Interface modification materials. Herein, CsPbBr 1.5 I 1.5 quantum dots (QDs) encapsulated in ZrO 2 sol is introduced to improve device stabili...

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Moderate Humidity Delays Electron–Hole Recombination in Hybrid Organic–Inorganic Perovskites: Time-Domain Ab Initio Simulations Rationalize Experiments

Cited by 141 publications

References 68 publications

Nonadiabatic charge dynamics in novel solar cell materials

Nonadiabatic charge dynamics in novel solar cell materials

Heavy Water Additive in Formamidinium: A Novel Approach to Enhance Perovskite Solar Cell Efficiency

Quantum Dots Encapsulated by ZrO₂ Enhance the Stability of Perovskite Solar Cells

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Moderate Humidity Delays Electron–Hole Recombination in Hybrid Organic–Inorganic Perovskites: Time-Domain Ab Initio Simulations Rationalize Experiments

Cited by 141 publications

References 68 publications

Nonadiabatic charge dynamics in novel solar cell materials

Nonadiabatic charge dynamics in novel solar cell materials

Heavy Water Additive in Formamidinium: A Novel Approach to Enhance Perovskite Solar Cell Efficiency

Quantum Dots Encapsulated by ZrO2 Enhance the Stability of Perovskite Solar Cells

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Quantum Dots Encapsulated by ZrO₂ Enhance the Stability of Perovskite Solar Cells