Surface plasmon-mediated photoluminescence boost in graphene-covered CsPbBr3 quantum dots

Applied Surface Science Elsevier 681 (2024) 161601

Authors:

Youngsin Park, Elham Oleiki, Guanhua Ying, Atanu Jana, Mutibah Alanazi, Vitaly Osokin, Sangeun Cho, Robert A Taylor, Geunsik Lee

Abstract:

The optical properties of graphene (Gr)-covered CsPbBr3 quantum dots (QDs) were investigated using micro-photoluminescence spectroscopy, revealing a remarkable three orders of magnitude enhancement in photoluminescence (PL) intensity compared to bare CsPbBr3 QDs. To elucidate the underlying mechanisms, we combined experimental techniques with density functional theory (DFT) calculations. DFT simulations showed that the graphene layer generates interfacial electrostatic potential barriers when in contact with the CsPbBr3 surface, impeding carrier leakage from perovskite to graphene and enhancing radiative recombination. Additionally, graphene passivates CsPbBr3 surface defect states, suppressing nonradiative recombination of photo-generated carriers. Our study also revealed that graphene becomes n-doped upon contact with CsPbBr3 QDs, activating its plasmon mode. This mode resonantly couples with photo-generated excitons in the perovskite. The momentum mismatch between graphene plasmons and free-space photons is resolved through plasmon scattering at Gr/CsPbBr3 interface corrugations, facilitating the observed super-bright emission. These findings highlight the critical role of graphene as a top contact in dramatically enhancing CsPbBr3 QDs’ PL. Our work advances the understanding of graphene-perovskite interfaces and opens new avenues for designing high-efficiency optoelectronic devices. The multifaceted enhancement mechanisms uncovered provide valuable insights for future research in nanophotonics and materials science, potentially leading to breakthroughs in light-emitting technologies.

Thermally activated delayed fluorophore and plasmonic structures integrated with perovskites for X-ray scintillation and imaging

Matter Cell Press 7:10 (2024) 3256-3289

Authors:

Atanu Jana, Sangeun Cho, Kandasamy Sasikumar, Heongkyu Ju, Hyunsik Im, Robert A Taylor

Abstract:

The development of inexpensive and easily processable X-ray-sensitive materials is of great importance because a number of commercial scintillators, such as LaBr3(Ce), Gd3Al3Ga2O12(Ce), Cs2HfCl6, NaI:Tl, CsI:Tl, and LiI:Eu, are fabricated using highly toxic or rare-earth elements via high-temperature synthesis. This has spurred research into radioluminescence-enhancing mechanisms and solution-processable scintillating materials made from earth-abundant elements that have excellent optoelectronic properties, including high quantum yields and a low afterglow effect. In recent years, a range of metal halide perovskite (MHP) integrated with thermally activated delayed fluorescence (TADF) materials have been developed, exhibiting excellent scintillation properties and a high spatial resolution. Meanwhile, plasmonic technologies are reported to exploit light-energy confinement capabilities beyond the diffraction limit that produces local-field enhancement. This enhancement has subsequently improved the performance of small-sized optoelectronic devices such as solar cells and diagnostic optical sensors. This perspective summarizes the current development of innovative MHP, TADF, and plasmonic materials for use in scintillators and their integrated moieties while also identifying the relevant challenges. Following a thorough evaluation of the efforts made to improve the X-ray scintillation efficiency of these materials, we propose an outlook for future research in order to further enhance their scintillation properties and spatial resolution.

Inhibiting the Appearance of Green Emission in Mixed Lead Halide Perovskite Nanocrystals for Pure Red Emission.

Nano letters American Chemical Society (ACS) 24:39 (2024) 12045-12053

Authors:

Mutibah Alanazi, Ashley R Marshall, Yincheng Liu, Jinwoo Kim, Shaoni Kar, Henry J Snaith, Robert A Taylor, Tristan Farrow

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 CsPbI<sub>2</sub>Br nanocrystals and thin films. We also introduce a new approach using cyclic olefin copolymer (COC) to encapsulate CsPbI<sub>2</sub>Br 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 (Pb<sup>2+</sup> and I<sup>-</sup>), increasing the formation energy of halide vacancies, improving the charge carrier lifetime, and reducing the nonradiative recombination density.

Boosting biomolecular switch efficiency with quantum coherence

Physical Review A American Physical Society (APS) 110:1 (2024) 012411

Authors:

Mattheus Burkhard, Onur Pusuluk, Tristan Farrow

Stabilization of halide perovskites with silicon compounds for optoelectronic, catalytic, and bioimaging applications

InfoMat Wiley Open Access (2024) e12559

Authors:

Atanu Jana, Sangeun Cho, Abhishek Meena, Abu Talha Aqueel Ahmed, Vijaya Gopalan Sree, Youngsin Park, Hyungsang Kim, Hyunsik Im, Robert A Taylor

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