Two-dimensional (2D) perovskites have attracted considerable interest for their promising applications for solar cells and other optoelectronics, such as light-emitting diodes, spintronics, and ...photodetectors. Here, we review the recent achievements of 2D perovskites for various optoelectronic applications. First, we discuss the basic structure and optoelectronic properties of 2D perovskites, including band structure, optical properties, and charge transport. We then highlight recent achievements using 2D perovskites in solar cells and beyond solar cells, including progress on various synthesis strategies and their impact on structural and optoelectronic properties. Finally, we discuss current challenges and future opportunities to further develop 2D perovskites for various applications.
Recent achievements of 2D perovskites for various optoelectronic applications along with their basic properties and future opportunities are discussed.
Perovskite solar cells (PSCs) with an inverted structure (often referred to as the p-i-n architecture) are attractive for future commercialization owing to their easily scalable fabrication, reliable ...operation and compatibility with a wide range of perovskite-based tandem device architectures
. However, the power conversion efficiency (PCE) of p-i-n PSCs falls behind that of n-i-p (or normal) structure counterparts
. This large performance gap could undermine efforts to adopt p-i-n architectures, despite their other advantages. Given the remarkable advances in perovskite bulk materials optimization over the past decade, interface engineering has become the most important strategy to push PSC performance to its limit
. Here we report a reactive surface engineering approach based on a simple post-growth treatment of 3-(aminomethyl)pyridine (3-APy) on top of a perovskite thin film. First, the 3-APy molecule selectively reacts with surface formamidinium ions, reducing perovskite surface roughness and surface potential fluctuations associated with surface steps and terraces. Second, the reaction product on the perovskite surface decreases the formation energy of charged iodine vacancies, leading to effective n-type doping with a reduced work function in the surface region. With this reactive surface engineering, the resulting p-i-n PSCs obtained a PCE of over 25 per cent, along with retaining 87 per cent of the initial PCE after over 2,400 hours of 1-sun operation at about 55 degrees Celsius in air.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
Multiple exciton generation in quantum dots (QDs) has been intensively studied as a way to enhance solar energy conversion by utilizing the excess energy in the absorbed photons. Among other useful ...properties, quantum confinement can both increase Coulomb interactions that drive the MEG process and decrease the electron–phonon coupling that cools hot excitons in bulk semiconductors. However, variations in the reported enhanced quantum yields (QYs) have led to disagreements over the role that quantum confinement plays. The enhanced yield of excitons per absorbed photon is deduced from a dynamical signature in the transient absorption or transient photoluminescence and is ascribed to the creation of biexcitons. Extraneous effects such as photocharging are partially responsible for the observed variations. When these extraneous effects are reduced, the MEG efficiency, defined in terms of the number of additional electron–hole pairs produced per additional band gap of photon excitation, is about two times better in PbSe QDs than that in bulk PbSe. Thin films of electronically coupled QDs have shown promise in simple photon-to-electron conversion architectures. If the MEG efficiency can be further enhanced and charge separation and transport can be optimized within QD films, then QD solar cells can lead to third-generation solar energy conversion technologies.
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IJS, KILJ, NUK, PNG, UL, UM
Cost-effective and efficient photocatalysis are highly desirable in chemical synthesis. Here we demonstrate that readily prepared suspensions of APbBr3 (A = Cs or methylammonium (MA)) type perovskite ...colloids (ca. 2–100 nm) can selectively photocatalyze carbon–carbon bond formation reactions, i.e., α-alkylations. Specifically, we demonstrate α-alkylation of aldehydes with a turnover number (TON) of over 52,000 under visible light illumination. Hybrid organic/inorganic perovskites are revolutionizing photovoltaic research and are now impacting other research fields, but their exploration in organic synthesis is rare. Our low-cost, easy-to-process, highly efficient and bandedge-tunable perovskite photocatalyst is expected to bring new insights in chemical synthesis.
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IJS, KILJ, NUK, PNG, UL, UM
Infrared technologies provide tremendous value to our modern-day society. The need for easy-to-fabricate, solution-processable, tunable infrared active optoelectronic materials has driven the ...development of infrared colloidal quantum dots, whose band gaps can readily be tuned by dimensional constraints due to the quantum confinement effect. In this Perspective, we summarize recent progress in the development of infrared quantum dots both as infrared light emitters (e.g., in light-emitting diodes, biological imaging, etc.) as well as infrared absorbers (e.g., in photovoltaics, solar fuels, photon up-conversion, etc.), focusing on how fundamental breakthroughs in synthesis, surface chemistry, and characterization techniques are facilitating the implementation of these nanostructures into exploratory device architectures as well as in emerging applications. We discuss the ongoing challenges and opportunities associated with infrared colloidal quantum dots.
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In traditional optoelectronic approaches, control over spin, charge, and light requires the use of both electrical and magnetic fields. In a spin-polarized light-emitting diode (spin-LED), charges ...are injected, and circularly polarized light is emitted from spin-polarized carrier pairs. Typically, the injection of carriers occurs with the application of an electric field, whereas spin polarization can be achieved using an applied magnetic field or polarized ferromagnetic contacts. We used chiral-induced spin selectivity (CISS) to produce spin-polarized carriers and demonstrate a spin-LED that operates at room temperature without magnetic fields or ferromagnetic contacts. The CISS layer consists of oriented, self-assembled small chiral molecules within a layered organic-inorganic metal-halide hybrid semiconductor framework. The spin-LED achieves ±2.6% circularly polarized electroluminescence at room temperature.
Organic-inorganic hybrid perovskites are attracting intense research effort due to their impressive performance in solar cells. While the carrier transport parameters such as mobility and bulk ...carrier lifetime shows sufficient characteristics, the surface recombination, which can have major impact on the solar cell performance, has not been studied. Here we measure surface recombination dynamics in CH3NH3PbBr3 perovskite single crystals using broadband transient reflectance spectroscopy. The surface recombination velocity is found to be 3.4±0.1 × 10(3) cm s(-1), ∼2-3 orders of magnitude lower than that in many important unpassivated semiconductors employed in solar cells. Our result suggests that the planar grain size for the perovskite thin films should be larger than ∼30 μm to avoid the influence of surface recombination on the effective carrier lifetime.
Incorporating chiral organic molecules into organic/inorganic hybrid 2D metal-halide perovskites results in a novel family of chiral hybrid semiconductors with unique spin-dependent properties. The ...embedded chiral organic moieties induce a chiroptical response from the inorganic metal–halide sublattice. However, the structural interplay between the chiral organic molecules and the inorganic sublattice, as well as their synergic effect on the resulting electronic band structure need to be explored in a broader material scope. Here we present three new layered tin iodide perovskites templated by chiral (R/S-)methylbenzylammonium (R/S-MBA), i.e., (R-/S-MBA)2SnI4, and their racemic phase (rac-MBA)2SnI4. These MBA2SnI4 compounds exhibit the largest level of octahedral bond distortion compared to any other reported layered tin iodide perovskite. The incorporation of chiral MBA cations leads to circularly polarized absorption from the inorganic Sn–I sublattice, displaying chiroptical activity in the 300–500 nm wavelength range. The bandgap and chiroptical activity are modulated by alloying Sn with Pb, in the series of (MBA)2Pb1–x Sn x I4. Finally, we show that vertical charge transport through oriented (R-/S-MBA)2SnI4 thin films is highly spin-dependent, arising from a chiral-induced spin selectivity (CISS) effect. We demonstrate a spin-polarization in the current–voltage characteristics as high as 94%. Our work shows the tremendous potential of these chiral hybrid semiconductors for controlling both spin and charge degrees of freedom.
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Understanding carrier recombination in semiconductors is a critical component when developing practical applications. Here we measure and compare the monomolecular, bimolecular, and trimolecular ...(Auger) recombination rate constants of CH3NH3PbBr3 and CH3NH3PbI3. The monomolecular and bimolecular recombination rate constants for both samples are limited by trap-assisted recombination. The bimolecular recombination rate constant for CH3NH3PbBr3 is ∼3.3 times larger than that for CH3NH3PbI3 and both are in line with that found for radiative recombination in other direct-gap semiconductors. The Auger recombination rate constant is 4 times larger in lead-bromide-based perovskite compared with lead-iodide-based perovskite and does not follow the reduced Auger rate when the bandgap increases. The increased Auger recombination rate, which is enhanced by Coulomb interactions, can be ascribed to the larger exciton binding energy, ∼40 meV, in CH3NH3PbBr3 compared with ∼13 meV in CH3NH3PbI3.
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We study the carrier dynamics in planar methyl ammonium lead iodide perovskite films using broadband transient absorption spectroscopy. We show that the sharp optical absorption onset is due to an ...exciton transition that is inhomogeneously broadened with a binding energy of 9 meV. We fully characterize the transient absorption spectrum by free-carrier-induced bleaching of the exciton transition, quasi-Fermi energy, carrier temperature and bandgap renormalization constant. The photo-induced carrier temperature is extracted from the transient absorption spectra and monitored as a function of delay time for different excitation wavelengths and photon fluences. We find an efficient hot-phonon bottleneck that slows down cooling of hot carriers by three to four orders of magnitude in time above a critical injection carrier density of ∼5 × 1017 cm-3 . Compared with molecular beam epitaxially grown GaAs, the critical density is an order of magnitude lower and the relaxation time is approximately three orders of magnitude longer.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, SBMB, UL, UM, UPUK
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