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1. Ab initio nonadiabatic molecular dynamics of charge carriers in metal halide perovskites

   https://doi.org/10.1039/d1nr01990b  

   Li, Wei ; She, Yalan ; Vasenko, Andrey S. ; Prezhdo, Oleg V. ( June 2021 , Nanoscale)

   Photoinduced nonequilibrium processes in nanoscale materials play key roles in photovoltaic and photocatalytic applications. This review summarizes recent theoretical investigations of excited state dynamics in metal halide perovskites (MHPs), carried out using a state-of-the-art methodology combining nonadiabatic molecular dynamics with real-time time-dependent density functional theory. The simulations allow one to study evolution of charge carriers at the ab initio level and in the time-domain, in direct connection with time-resolved spectroscopy experiments. Eliminating the need for the common approximations, such as harmonic phonons, a choice of the reaction coordinate, weak electron–phonon coupling, a particular kinetic mechanism, and perturbative calculation of rate constants, we model full-dimensional quantum dynamics of electrons coupled to semiclassical vibrations. We study realistic aspects of material composition and structure and their influence on various nonequilibrium processes, including nonradiative trapping and relaxation of charge carriers, hot carrier cooling and luminescence, Auger-type charge–charge scattering, multiple excitons generation and recombination, charge and energy transfer between donor and acceptor materials, and charge recombination inside individual materials and across donor/acceptor interfaces. These phenomena are illustrated with representative materials and interfaces. Focus is placed on response to external perturbations, formation of point defects and their passivation, mixed stoichiometries, dopants, grain boundaries, and interfaces ofmore »MHPs with charge transport layers, and quantum confinement. In addition to bulk materials, perovskite quantum dots and 2D perovskites with different layer and spacer cation structures, edge passivation, and dielectric screening are discussed. The atomistic insights into excited state dynamics under realistic conditions provide the fundamental understanding needed for design of advanced solar energy and optoelectronic devices.« less
2. Conjugated molecule based 2D perovskites for high-performance perovskite solar cells

   https://doi.org/10.1039/d1ta05934c  

   Zhu, Tao ; Shen, Lening ; Chen, Hanlin ; Yang, Yongrui ; Zheng, Luyao ; Chen, Rui ; Zheng, Jie ; Wang, Junpeng ; Gong, Xiong ( October 2021 , Journal of Materials Chemistry A)

   Conjugated molecules have been typically utilized as either hole or electron extraction layers to boost the device performance of perovskite solar cells (PSCs), formed from three-dimensional (3D) perovskites, due to their high charge carrier mobility and electrical conductivity. However, the passivating role of conjugated molecules in creating two-dimensional (2D) perovskites has rarely been reported. In this study, we report novel conjugated aniline 3-phenyl-2-propen-1-amine (PPA) based 2D perovskites and further demonstrate efficient and stable PSCs containing a (PPA) x (MAPbI 3 ) 1− x /MAPbI 3 bilayer thin film (where MA is CH 3 NH 3 + ). The (PPA) x (MAPbI 3 ) 1− x /MAPbI 3 bilayer thin film possesses superior crystallinity and passivated trap states, resulting in enhanced charge transport and suppressed charge carrier recombination compared to those of a 3D MAPbI 3 thin film. As a result, PSCs containing the (PPA) x (MAPbI 3 ) 1− x /MAPbI 3 bilayer thin film exhibit a power conversion efficiency (PCE) of 21.98%, which is approximately a 25% enhancement compared to that of the MAPbI 3 thin film. Moreover, un-encapsulated PSCs containing the (PPA) x (MAPbI 3 ) 1− x /MAPbI 3 bilayer thin film retain 50% of their initialmore »PCE after 1200 hours in an ambient atmosphere (25 °C, and 30 ± 10 humidity), whereas PSCs with the 3D MAPbI 3 thin film show significant degradation after 100 hours and a degradation of more than 50% of their original PCE after 500 hours. These results demonstrate that the incorporation of conjugated molecules as organic spacer cations to create 2D perovskites on top of 3D perovskites is an effective way to approach high-performance PSCs.« less
3. Integration of a functionalized graphene nano-network into a planar perovskite absorber for high-efficiency large-area solar cells

   https://doi.org/10.1039/C8MH00511G  

   Wang, Yong ; Zhou, Yuanyuan ; Zhang, Taiyang ; Ju, Ming-Gang ; Zhang, Lin ; Kan, Miao ; Li, Yihui ; Zeng, Xiao Cheng ; Padture, Nitin. P. ; Zhao, Yixin ( January 2018 , Materials Horizons)

   Efficient charge collection is critical in large area (quasi-) planar configuration perovskite solar cells (PSCs) as the cell operation relies on the diffusion of photo-generated charge carriers to charge collector layers. Many defects/traps in the polycrystalline perovskite absorber layer strongly affect the charge collection efficiency because the 2D-like top charge collection layer barely penetrates into the 3D grain boundaries in the perovskite layer to efficiently collect the charge carrier. Inspired by blood capillaries for efficient mass exchange, a charge-collection nano-network for efficient charge collection was incorporated into the perovskite absorber using low-cost, stable amino-functionalized graphene (G-NH 2 ). The integration of such an unprecedented structure enables very efficient charge collection, leading to the significant enhancement of the power conversion efficiency of 1 × 1 cm 2 MAPbI 3 PSCs from 14.4 to 18.7% with higher reproducibility, smaller hysteresis and enhanced stability. The physicochemical mechanisms underlying the role of this nano charge-collection nano-network in boosting the charge collection in PSCs are elucidated comprehensively, using a combined experimental and theoretical approach, pointing to a new direction towards up-scaling of high-efficiency PSCs.
4. Interfacial charge-transfer doping of metal halide perovskites for high performance photovoltaics

   https://doi.org/10.1039/C9EE01773A  

   Noel, Nakita K. ; Habisreutinger, Severin N. ; Pellaroque, Alba ; Pulvirenti, Federico ; Wenger, Bernard ; Zhang, Fengyu ; Lin, Yen-Hung ; Reid, Obadiah G. ; Leisen, Johannes ; Zhang, Yadong ; et al ( October 2019 , Energy & Environmental Science)

   The remarkable optoelectronic properties of metal halide perovskites have generated intense research interest over the last few years. The ability to control and manipulate the crystallisation and stoichiometry of perovskite thin-films has allowed for impressive strides in the development of highly efficient perovskite solar cells. However, being able to effectively modify the interfaces of metal halide perovskites, and to controllably p- or n-type dope the surfaces, may be key to further improvements in the efficiency and long-term stability of these devices. In this study, we use surface doping of the mixed-cation, mixed-halide perovskite FA 0.85 MA 0.15 Pb(I 0.85 Br 0.15 ) 3 (FA – formamidinium; MA – methylammonium) to improve the hole extraction from the perovskite solar cell. By treating the surface of the perovskite film with a strongly oxidizing molybdenum tris(dithiolene) complex, we achieve a shift in the work function that is indicative of p-doping, and a twofold increase in the total conductivity throughout the film. We probe the associated interfacial chemistry through photoelectron and solid-state nuclear magnetic resonance spectroscopies and confirm that charge-transfer occurs between the perovskite and dopant complex. The resulting p-doped interface constitutes a homojunction with increased hole-selectivity. With charge-selective layers, we show that thismore »surface doping enhances the device performance of perovskite solar cells resulting in steady-state efficiencies approaching 21%. Finally, we demonstrate that a surface treatment with this dopant produces the same effect as the commonly employed additive 4- tert butylpyridine ( t BP), allowing us to achieve “ t BP-free” devices with steady-state efficiencies of over 20%, and enhanced thermal stability as compared to devices processed using t BP. Our findings therefore demonstrate that molecular doping is a feasible route to tune and control the surface properties of metal halide perovskites.« less
5. A multifunctional 2D black phosphorene-based platform for improved photovoltaics

   https://doi.org/10.1039/d1cs00847a  

   Zhang, Meng ; Biesold, Gill M. ; Lin, Zhiqun ( November 2021 , Chemical Society Reviews)

   As one of the latest additions to the 2D nanomaterials family, black phosphorene (BP, monolayer or few-layer black phosphorus) has gained much attention in various forms of solar cells. This is due largely to its intriguing semiconducting properties such as tunable direct bandgap (from 0.3 eV in the bulk to 2.0 eV in the monolayer), extremely high ambipolar carrier mobility, broad visible to infrared light absorption, etc. These appealing optoelectronic attributes make BP a multifunctional nanomaterial for use in solar cells via tailoring carrier dynamics, band energy alignment, and light harvesting, thereby promoting the rapid development of third-generation solar cells. Notably, in sharp contrast to the copious work on revealing the fundamental properties of BP, investigation into the utility of BP is comparatively less, particularly in the area of photovoltaics. Herein, we first identify and summarize an array of unique characteristics of BP that underpin its application in photovoltaics, aiming at providing inspiration to develop new designs and device architectures of photovoltaics. Subsequently, state-of-the-art synthetic routes ( i.e. , top-down and bottom-up) to scalable BP production that facilitates its applications in optoelectronic materials and devices are outlined. Afterward, recent advances in a diverse set of BP-incorporated solar cells, where BPmore »may impart electron and/or hole extraction and transport, function as a light absorber, provide dielectric screening for enhancing exciton dissociation, and modify the morphology of photoabsorbers, are discussed, including organic solar cells, dye-sensitized solar cells, heterojunction solar cells and perovskite solar cells. Finally, the challenges and opportunities in this rapidly evolving field are presented.« less