Publications by authors named "Maria A Loi"

In recent years, metal halide perovskite-based light-emitting diodes (LEDs) have garnered significant attention as they display high quantum efficiency, good spectral tunability, and are expected to have low processing costs. When the peak emission wavelength is beyond 900 nm the interest is even higher because of the critical importance of this wavelength for biomedical imaging, night vision, and sensing. However, many challenges persist in fabricating these high-performance NIR LEDs, particularly for wavelengths above 950 nm, which appear to be limited by low radiance and poor stability.

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Metal halide perovskites have shown exceptionally slow hot-carrier cooling, which has been attributed to various physical mechanisms without reaching a consensus. Here, experiment and theory are combined to unveil the carrier cooling process in formamidinium (FA) and caesium (Cs) tin triiodide thin films. Through impulsive vibrational spectroscopy and molecular dynamics, much shorter phonon dephasing times of the hybrid perovskite, which accounts for the larger blueshift in the photoluminescence seen at high excitation density for FASnI compared to CsSnI is reported.

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Tin halide perovskites are promising for optoelectronics, although their sensitivity to ambient conditions due to Sn(II) oxidation presents a challenge. Encapsulation techniques can mitigate degradation and facilitate advanced studies of the intrinsic properties. To study and improve the ambient stability of CsSnBr and CsSnI nanocrystal (NC) thin films, we explored various encapsulation methods: organic, inorganic, and hybrid.

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  • Researchers have tackled the challenge of crystal growth alignment in low-dimensional perovskites (LDPs) used for solar cells, specifically those with wide band gaps that hinder charge flow.
  • By adding chlorine to the precursor solution, they induced vertical crystal growth which enhances efficiency.
  • This method led to a significant power conversion efficiency of 9.4% and an open circuit voltage of 1.4V, paving the way for innovative solar applications in buildings and indoor energy solutions.
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  • Metalloporphyrins with open-shell transition metals like Ni(II) have a fast excited-state relaxation mechanism, which is explored in a nanographene-Ni(II) porphyrin conjugate.
  • Using variable temperature transient absorption and global fit analysis, the study reveals that after photoexcitation, vibrational cooling occurs in 1.6 ps, followed by a brief 20 ps window where some excited states decay radiatively before intersystem crossing.
  • At low temperatures, two relaxation pathways from the lowest triplet state to the ground state are identified: a slow process over 1.6 ns and a faster route influenced by a conical intersection, important for applications in energy harvesting and optoelectronics.
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Colloidal perovskite nanoplatelets (NPLs) have shown promise in tackling blue light-emitting diode challenges based on their tunable band gap and high photoluminescence efficiencies. However, high quality and large area dense NPL films have been proven to be very hard to prepare because of their chemical and physical fragility during the liquid phase deposition. Herein, we report a perovskite-polymer composite film deposition strategy with fine morphology engineering obtained using the blade coating method.

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Lead chalcogenide colloidal quantum dots are one of the most promising materials to revolutionize the field of short-wavelength infrared optoelectronics due to their bandgap tunability and strong absorption. By self-assembling these quantum dots into ordered superlattices, mobilities approaching those of the bulk counterparts can be achieved while still retaining their original optical properties. The recent literature focused mostly on PbSe-based superlattices, but PbS quantum dots have several advantages, including higher stability.

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Chemical doping is an important approach to manipulating charge-carrier concentration and transport in organic semiconductors (OSCs) and ultimately enhances device performance. However, conventional doping strategies often rely on the use of highly reactive (strong) dopants, which are consumed during the doping process. Achieving efficient doping with weak and/or widely accessible dopants under mild conditions remains a considerable challenge.

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  • The surface chemistry of colloidal semiconductor nanocrystals, particularly InP QDs, significantly affects their properties and applications, especially in optoelectronics.
  • Replacing insulating organic ligands with shorter inorganic alternatives improves charge mobility and stability, making them suitable for devices like LEDs and photodetectors.
  • The study investigates the ligand exchange using group III metal salts and reveals that these salts create stable metal-solvent complexes, enhancing the colloidal stability of InP QDs in polar solvents for extended periods.
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Slow hot-carrier cooling may potentially allow overcoming the maximum achievable power conversion efficiency of single-junction solar cells. For formamidinium tin triiodide, an exceptional slow cooling time of a few nanoseconds was reported. However, a systematic study of the cation influence, as is present for lead compounds, is lacking.

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The phase-transfer ligand exchange of PbS quantum dots (QDs) has substantially simplified device fabrication giving hope for future industrial exploitation. However, this technique when applied to QDs of large size (>4 nm) gives rise to inks with poor colloidal stability, thus hindering the development of QDs photodetectors in short-wavelength infrared range. Here, it is demonstrated that methylammonium lead iodide ligands can provide sufficient passivation of PbS QDs of size up to 6.

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  • The optical response of 2D layered perovskites features closely spaced spectral signatures, interpreted as phonon replicas, with an energy separation ranging from 12 to 40 meV, depending on the material.
  • These materials also show a strong scattering response in resonant Raman spectroscopy above roughly 200 cm (or 25 meV), which is linked to the presence of polarons, exhibiting a distinctive spectral pattern deviating from the Rayleigh line.
  • A significant Huang-Rhys factor (S > 6) suggests strong coupling between charge carriers and the lattice, with polaron binding energies between 20-35 meV, influencing the optical properties critical for future opto-electronic applications.
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The integration of organic electronic circuits into real-life applications compels the fulfillment of a range of requirements, among which the ideal operation at a low voltage with reduced power consumption is paramount. Moreover, these performance factors should be achieved via solution-based fabrication schemes in order to comply with the promise of cost- and energy-efficient manufacturing offered by an organic, printed electronic technology. Here, we propose a solution-based route for the fabrication of low-voltage organic transistors, encompassing ideal device operation at voltages below 5 V and exhibiting n-type unipolarization.

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An introduction to the Nanoscale themed collection on halide perovskite nanomaterials for optoelectronic applications, featuring a variety of articles that highlight the latest developments to address ongoing challenges in the field.

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Metal halide perovskites show the capability of performing structural transformation, allowing the formation of functional heterostructures. Unfortunately, the elusive mechanism governing these transformations limits their technological application. Herein, the mechanism of 2D-3D structural transformation is unraveled as catalyzed by solvents.

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Two terminal passive devices are regarded as one of the promising candidates to solve the processor-memory bottleneck in the Von Neumann computing architectures. Many different materials are used to fabricate memory devices, which have the potential to act as synapses in future neuromorphic electronics. Metal halide perovskites are attractive for memory devices as they display high density of defects with a low migration barrier.

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  • Transport layers are crucial for enhancing the efficiency and stability of thin-film solar cells, especially as they move towards mass production.
  • This study showcases organic solar cells (OSCs) with a power conversion efficiency (PCE) of 17.26% using tin oxide (SnO) as an electron transport layer, deposited via atomic layer deposition (ALD).
  • The ALD-SnO exhibits superior performance over traditional solutions like SnO nanoparticles and sol-gel ZnO, thanks to reduced charge recombination and improved stability under light exposure.
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  • Researchers created blue LEDs that emit light at a specific peak wavelength of 481 nm and achieved a color purity of 88%, along with a luminance of 8260 cd/m² and an external quantum yield of 5.2%.
  • The LEDs are made from a material called quasi-2D PEA(CsMA)PbBr, with an additive (isopropylammonium or iPAm) that helps prevent unwanted bulk-like phase formations.
  • The study also shows that by managing energy transfer within the material, the researchers improved the efficiency of these blue-emitting LEDs, achieving a photoluminescence quantum yield over 60% and suggesting a potential for better optoelectronic devices using tailored
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The development of an environmentally friendly fabrication process for non-fullerene acceptor organic solar cells is an essential condition for their commercialization. However, devices fabricated by processing the active layer with green solvents still struggle to reach, in terms of efficiency, the same performance as those fabricated with halogenated solvents. The reason behind this is the non-optimal nanostructure of the active layer obtained with green solvents.

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Scarce information is available on the thin film morphology of Dion-Jacobson halide perovskites. However, the microstructure can have a profound impact on a material's photophysics and its potential for optoelectronic applications. The microscopic mechanisms at play in the prototypical 1,4-phenylenedimethanammonium lead iodide (PDMAPbI) Dion-Jacobson compound are here elucidated through a combination of hyperspectral photoluminescence and Raman spectro-microscopy supported by x-ray diffraction.

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2D metal halide perovskites can show narrow and broad emission bands (BEs), and the latter's origin is hotly debated. A widespread opinion assigns BEs to the recombination of intrinsic self-trapped excitons (STEs), whereas recent studies indicate they can have an extrinsic defect-related origin. Here, we carry out a combined experimental-computational study into the microscopic origin of BEs for a series of prototypical phenylethylammonium-based 2D perovskites, comprising different metals (Pb, Sn) and halides (I, Br, Cl).

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  • 3D superlattices of colloidal quantum dots have potential for next-gen optoelectronic devices due to their tunable optical properties and coherent electrical transport.
  • Previous research mostly focused on 2D arrays, which struggled with long-range order and transport issues.
  • Controlled nanoscale ordering of 3D quantum dots has achieved record electron mobilities and demonstrates the possibility of highly tunable optical properties, paving the way for advanced optoelectronic materials.
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Conjugated polymers with narrow band gaps are particularly useful for sorting and discriminating semiconducting single-walled carbon nanotubes (s-SWCNT) due to the low charge carrier injection barrier for transport. In this paper, we report two newly synthesized narrow-band-gap conjugated polymers ( and ) based on naphthalene diimide (NDI) and thienylennevinylene (TVT) building blocks, decorated with different polar side chains that can be used for dispersing and discriminating s-SWCNT. Compared with the mid-band-gap conjugated polymer , which is composed of naphthalene diimide (NDI) and head-to-head bithiophene building blocks, the addition of a vinylene linker eliminates the steric congestion present in head-to-head bithiophene, which promotes backbone planarity, extending the π-conjugation length and narrowing the band gap.

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Given their comparatively narrow band gap, mixed Pb-Sn iodide perovskites are interesting candidates for bottom cells in all-perovskite tandems or single junction solar cells, and their luminescence around 900 nm offers great potential for near-infrared optoelectronics. Here, we investigate mixed FAPbSnI offering the first accurate determination of the crystal structure over a temperature range from 293 to 100 K. We demonstrate that all compositions exhibit a cubic structure at room temperature and undergo at least two transitions to lower symmetry tetragonal phases upon cooling.

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