Professor Robert Taylor

Abstract:

Mixed halide perovskites exhibit promising optoelectronic properties for next-generation light-emitting diodes due to their tunable emission wavelength that covers the entire visible light spectrum. However, these materials suffer from severe phase segregation under continuous illumination, making long-term stability for pure red emission a significant challenge. In this study, we present a comprehensive analysis of the role of halide oxidation in unbalanced ion migration (I/Br) within CsPbI₂Br nanocrystals and thin films. We also introduce a new approach using cyclic olefin copolymer (COC) to encapsulate CsPbI₂Br perovskite nanocrystals (PNCs), effectively suppressing ion migration by increasing the corresponding activation energy. Compared with that of unencapsulated samples, we observe a substantial reduction in phase separation under intense illumination in PNCs with a COC coating. Our findings show that COC enhances phase stability by passivating uncoordinated surface defects (Pb²⁺ and I^-), increasing the formation energy of halide vacancies, improving the charge carrier lifetime, and reducing the nonradiative recombination density.

Abstract:

Silicon belongs to group 14 elements along with carbon, germanium, tin, and lead in the periodic table. Similar to carbon, silicon is capable of forming a wide range of stable compounds, including silicon hydrides, organosilicons, silicic acids, silicon oxides, and silicone polymers. These materials have been used extensively in optoelectronic devices, sensing, catalysis, and biomedical applications. In recent years, silicon compounds have also been shown to be suitable for stabilizing delicate halide perovskite structures. These composite materials are now receiving a lot of interest for their potential use in various real‐world applications. Despite exhibiting outstanding performance in various optoelectronic devices, halide perovskites are susceptible to breakdown in the presence of moisture, oxygen, heat, and UV light. Silicon compounds are thought to be excellent materials for improving both halide perovskite stability and the performance of perovskite‐based optoelectronic devices. In this work, a wide range of silicon compounds that have been used in halide perovskite research and their applications in various fields are discussed. The interfacial stability, structure–property correlations, and various application aspects of perovskite and silicon compounds are also analyzed at the molecular level. This study also explores the developments, difficulties, and potential future directions associated with the synthesis and application of perovskite‐silicon compounds. image

Abstract:

<jats:title>Abstract</jats:title><jats:p>Photocatalytic splitting of seawater for hydrogen evolution has attracted a great deal of attention in recent years. However, the poor energy conversion efficiency and stability of photocatalysts in a salty environment have greatly hindered further applications of this technology. Moreover, the effects of electrolytes in seawater remain controversial. Here we present electrolyte-assisted charge polarization over an N-doped TiO<jats:sub>2</jats:sub> photocatalyst, which demonstrates the stoichiometric evolution of H<jats:sub>2</jats:sub> and O<jats:sub>2</jats:sub> from the thermo-assisted photocatalytic splitting of seawater. Our extensive characterizations and computational studies show that ionic species in seawater can selectively adsorb on photo-polarized facets of the opposite charge, which can prolong the charge-carrier lifetime by a factor of five, leading to an overall energy conversion efficiency of 15.9 ± 0.4% at 270 °C. Using a light-concentrated furnace, a steady hydrogen evolution rate of 40 mmol g<jats:sup>−1</jats:sup> h<jats:sup>−1</jats:sup> is demonstrated, which is of the same order of magnitude as laboratory-scale electrolysers.</jats:p>

Abstract:

Lead Mixed Halide Perovskites (LMHPs), CsPbBrI₂, have attracted significant interest as promising candidates for wide bandgap absorber layers in tandem solar cells due to their relative stability and red-light emission with a bandgap ∼1.7 eV. However, these materials segregate into Br-rich and I-rich domains upon continuous illumination, affecting their optical properties and compromising the operational stability of devices. Herein, we track the microscopic processes occurring during halide segregation by using combined spectroscopic measurements at room and cryogenic temperatures. We also evaluate a passivation strategy to mitigate the halide migration of Br/I ions in the films by overcoating with cyclic olefin copolymer (COC). Our results explain the correlation between grain size, intensity dependencies, phase segregation, activation energy barrier, and their influence on photoinduced carrier lifetimes. Importantly, COC treatment increases the lifetime charge carriers in mixed halide thin films, improving efficient charge transport in perovskite solar cell applications.

Abstract:

Ultranarrow bandwidth single-photon sources operating at room-temperature are of vital importance for viable optical quantum technologies at scale, including quantum key distribution, cloud-based quantum information processing networks, and quantum metrology. Here we show a room-temperature ultranarrow bandwidth single-photon source generating single-mode photons at a rate of 5 MHz based on an inorganic CsPbI₃ perovskite quantum dot embedded in a tunable open-access optical microcavity. When coupled to an optical cavity mode, the quantum dot room-temperature emission becomes single-mode, and the spectrum narrows down to just ∼1 nm. The low numerical aperture of the optical cavities enables efficient collection of high-purity single-mode single-photon emission at room-temperature, offering promising performance for photonic and quantum technology applications. We measure 94% pure single-photon emission in a single-mode under pulsed and continuous-wave (CW) excitation.