Author
Ajay Ram Srimath Kandada
Other affiliations: Istituto Italiano di Tecnologia, Georgia Institute of Technology, Université de Montréal ...read more
Bio: Ajay Ram Srimath Kandada is an academic researcher from Wake Forest University. The author has contributed to research in topics: Perovskite (structure) & Exciton. The author has an hindex of 31, co-authored 71 publications receiving 6644 citations. Previous affiliations of Ajay Ram Srimath Kandada include Istituto Italiano di Tecnologia & Georgia Institute of Technology.
Papers
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TL;DR: Optical spectroscopy is used to estimate the exciton binding energy in the mixed-halide crystal to be in the range of 50 meV, and it is shown that such a value is consistent with almost full ionization of the excitonic population under photovoltaic cell operating conditions.
Abstract: Excitonic solar cells, within which bound electron-hole pairs have a central role in energy harvesting, have represented a hot field of research over the last two decades due to the compelling prospect of low-cost solar energy. However, in such cells, exciton dissociation and charge collection occur with significant losses in energy, essentially due to poor charge screening. Organic-inorganic perovskites show promise for overcoming such limitations. Here, we use optical spectroscopy to estimate the exciton binding energy in the mixed-halide crystal to be in the range of 50 meV. We show that such a value is consistent with almost full ionization of the exciton population under photovoltaic cell operating conditions. However, increasing the total photoexcitation density, excitonic species become dominant, widening the perspective of this material for a host of optoelectronic applications.
1,473 citations
TL;DR: In this article, the authors show that planar perovskite solar cells using TiO2 are inherently limited due to conduction band misalignment and demonstrate, with a variety of characterization techniques, for the first time that SnO2 achieves a barrier-free energetic configuration, obtaining almost hysteresis-free power conversion efficiencies (PCEs).
Abstract: The simplification of perovskite solar cells (PSCs), by replacing the mesoporous electron selective layer (ESL) with a planar one, is advantageous for large-scale manufacturing. PSCs with a planar TiO2 ESL have been demonstrated, but these exhibit unstabilized power conversion efficiencies (PCEs). Herein we show that planar PSCs using TiO2 are inherently limited due to conduction band misalignment and demonstrate, with a variety of characterization techniques, for the first time that SnO2 achieves a barrier-free energetic configuration, obtaining almost hysteresis-free PCEs of over 18% with record high voltages of up to 1.19 V.
1,049 citations
TL;DR: The blue fluorescent CsPbCl3 NPLs represent a new member of the scarcely populated group of blue-emitting colloidal nanocrystals and the exciton dynamics were found to be independent of the extent of 2D confinement in these platelets, and this was supported by band structure calculations.
Abstract: We report a colloidal synthesis approach to CsPbBr3 nanoplatelets (NPLs). The nucleation and growth of the platelets, which takes place at room temperature, is triggered by the injection of acetone in a mixture of precursors that would remain unreactive otherwise. The low growth temperature enables the control of the plate thickness, which can be precisely tuned from 3 to 5 monolayers. The strong two-dimensional confinement of the carriers at such small vertical sizes is responsible for a narrow PL, strong excitonic absorption, and a blue shift of the optical band gap by more than 0.47 eV compared to that of bulk CsPbBr3. We also show that the composition of the NPLs can be varied all the way to CsPbBr3 or CsPbI3 by anion exchange, with preservation of the size and shape of the starting particles. The blue fluorescent CsPbCl3 NPLs represent a new member of the scarcely populated group of blue-emitting colloidal nanocrystals. The exciton dynamics were found to be independent of the extent of 2D confinement...
714 citations
TL;DR: It is demonstrated that larger crystallites present smaller band gap and longer lifetime, which correlates to a smaller radiative bimolecular recombination coefficient, and also shows that they present a higher optical gain, becoming preferred candidates for the realization of CW lasing devices.
Abstract: We report about the relationship between the morphology and luminescence properties of methylammonium lead trihalide perovskite thin films. By tuning the average crystallite dimension in the film from tens of nanometers to a few micrometers, we are able to tune the optical band gap of the material along with its photoluminescence lifetime. We demonstrate that larger crystallites present smaller band gap and longer lifetime, which correlates to a smaller radiative bimolecular recombination coefficient. We also show that they present a higher optical gain, becoming preferred candidates for the realization of CW lasing devices.
549 citations
TL;DR: In this paper, it was shown that ion segregation takes place via halide defects, resulting in iodide-rich lowbandgap regions close to the illuminated surface of the film, driven by the strong gradient in carrier generation rate through the thickness of these strongly absorbing materials.
Abstract: Solution-processable metal halide perovskites show immense promise for use in photovoltaics and other optoelectronic applications. The ability to tune their bandgap by alloying various halide anions (for example, in CH3NH3Pb(I1–xBrx)3, 0 < x < 1) is however hampered by the reversible photoinduced formation of sub-bandgap emissive states. We find that ion segregation takes place via halide defects, resulting in iodide-rich low-bandgap regions close to the illuminated surface of the film. This segregation may be driven by the strong gradient in carrier generation rate through the thickness of these strongly absorbing materials. Once returned to the dark, entropically driven intermixing of halides returns the system to a homogeneous condition. We present approaches to suppress this process by controlling either the internal light distribution or the defect density within the film. These results are relevant to stability in both single- and mixed-halide perovskites, leading the way toward tunable and stable p...
395 citations
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TL;DR: In this article, a review describes the rapid progress that has been made in hybrid organic-inorganic perovskite solar cells and their applications in the photovoltaic sector.
Abstract: Within the space of a few years, hybrid organic–inorganic perovskite solar cells have emerged as one of the most exciting material platforms in the photovoltaic sector. This review describes the rapid progress that has been made in this area.
5,463 citations
TL;DR: In this paper, the triple cation perovskite photovoltaics with inorganic cesium were shown to be thermally more stable, contain less phase impurities and are less sensitive to processing conditions.
Abstract: Today's best perovskite solar cells use a mixture of formamidinium and methylammonium as the monovalent cations. With the addition of inorganic cesium, the resulting triple cation perovskite compositions are thermally more stable, contain less phase impurities and are less sensitive to processing conditions. This enables more reproducible device performances to reach a stabilized power output of 21.1% and ∼18% after 250 hours under operational conditions. These properties are key for the industrialization of perovskite photovoltaics.
3,470 citations
TL;DR: This work shows that the small and oxidation-stable rubidium cation (Rb+) can be embedded into a “cation cascade” to create perovskite materials with excellent material properties and achieved stabilized efficiencies of up to 21.6% on small areas.
Abstract: All of the cations currently used in perovskite solar cells abide by the tolerance factor for incorporation into the lattice. We show that the small and oxidation-stable rubidium cation (Rb + ) can be embedded into a “cation cascade” to create perovskite materials with excellent material properties. We achieved stabilized efficiencies of up to 21.6% (average value, 20.2%) on small areas (and a stabilized 19.0% on a cell 0.5 square centimeters in area) as well as an electroluminescence of 3.8%. The open-circuit voltage of 1.24 volts at a band gap of 1.63 electron volts leads to a loss in potential of 0.39 volts, versus 0.4 volts for commercial silicon cells. Polymer-coated cells maintained 95% of their initial performance at 85°C for 500 hours under full illumination and maximum power point tracking.
3,034 citations
TL;DR: A solution-based hot-casting technique is demonstrated to grow continuous, pinhole-free thin films of organometallic perovskites with millimeter-scale crystalline grains that are applicable to several other material systems plagued by polydispersity, defects, and grain boundary recombination in solution-processed thin films.
Abstract: State-of-the-art photovoltaics use high-purity, large-area, wafer-scale single-crystalline semiconductors grown by sophisticated, high-temperature crystal growth processes. We demonstrate a solution-based hot-casting technique to grow continuous, pinhole-free thin films of organometallic perovskites with millimeter-scale crystalline grains. We fabricated planar solar cells with efficiencies approaching 18%, with little cell-to-cell variability. The devices show hysteresis-free photovoltaic response, which had been a fundamental bottleneck for the stable operation of perovskite devices. Characterization and modeling attribute the improved performance to reduced bulk defects and improved charge carrier mobility in large-grain devices. We anticipate that this technique will lead the field toward synthesis of wafer-scale crystalline perovskites, necessary for the fabrication of high-efficiency solar cells, and will be applicable to several other material systems plagued by polydispersity, defects, and grain boundary recombination in solution-processed thin films.
2,960 citations
TL;DR: The broad tunability and fabrication methods of these materials, the current understanding of the operation of state-of-the-art solar cells and the properties that have delivered light-emitting diodes and lasers are described.
Abstract: Metal-halide perovskites are crystalline materials originally developed out of scientific curiosity. Unexpectedly, solar cells incorporating these perovskites are rapidly emerging as serious contenders to rival the leading photovoltaic technologies. Power conversion efficiencies have jumped from 3% to over 20% in just four years of academic research. Here, we review the rapid progress in perovskite solar cells, as well as their promising use in light-emitting devices. In particular, we describe the broad tunability and fabrication methods of these materials, the current understanding of the operation of state-of-the-art solar cells and we highlight the properties that have delivered light-emitting diodes and lasers. We discuss key thermal and operational stability challenges facing perovskites, and give an outlook of future research avenues that might bring perovskite technology to commercialization.
2,513 citations