Roma Mulholland


Postgraduate Research Student

Academic and research departments

School of Chemistry and Chemical Engineering.

About

My research project

Publications

J O'Neill, J Ghosh, S Alghamdi, I Braddock, C Crean, R Dorey, R Mulholland, S Richards, M Wilson, H Salway, M Anaya, J Reiss, D Wolfe, P Sellin (2023)Hydrothermal and Mechanosynthesis of Mixed-Cation Double Perovskite Scintillators for Radiation Detection Wiley

Publication status: Published Funder: STFC; doi: http://dx.doi.org/10.13039/501100000271 Funder: Rutherford Appleton Laboratory; doi: http://dx.doi.org/10.13039/100014570 AbstractThis article details work performed on the synthesis and characterization of an inorganic mixed‐cation double halide perovskite, Cs2Ag.6Na.4In.85Bi.15Cl6 (CANIBIC). Single crystals have been created via a hydrothermal reaction, milled into a powder, and pressed into pellets, while nanocrystals have been directly synthesized via mechanosynthesis. A computational model is constructed to predict the X‐ray diffraction pattern of CANIBIC; this model aligns very well with the X‐ray diffraction pattern measured for CANIBIC crystal powder. This model can therefore be developed in the future as a tool to predict lattice parameters and crystal structures of other novel double‐halide perovskites. Photoluminescence spectra obtained from each format show broad emission centered at 630 nm, as is typical for self‐trapped exciton emission; self‐trapped exciton emission is also confirmed by investigating photoluminescence intensity as a function of laser power. Nanocomposites are produced via the loading of nanocrystals of CANIBIC into PMMA. Although nanocomposite disks consisting of a small proportion of CANIBIC nanocrystals in PMMA have a smaller mass attenuation coefficient than a pressed pellet of CANIBIC, these disks have comparatively bright radioluminescence due to their optical transparency. These nanocomposite disks are therefore a particularly useful format for the practical use of the CANIBIC scintillator.

Joseph O'Neill, Joydip Ghosh, Suad Alghamdi, Isabel Braddock, Carol Crean, Robert Dorey, Roma Mulholland, Sion Richards, Matthew Wilson, Hayden Salway, Miguel Anaya, Justin Reiss, Douglas Wolfe, Paul Sellin (2024)Hydrothermal and Mechanosynthesis of Mixed‐Cation Double Perovskite Scintillators for Radiation Detection, In: Advanced Optical Materials12(2)2301335 Wiley

This article details work performed on the synthesis and characterization of an inorganic mixed‐cation double halide perovskite, Cs 2 Ag .6 Na .4 In .85 Bi .15 Cl 6 (CANIBIC). Single crystals have been created via a hydrothermal reaction, milled into a powder, and pressed into pellets, while nanocrystals have been directly synthesized via mechanosynthesis. A computational model is constructed to predict the X‐ray diffraction pattern of CANIBIC; this model aligns very well with the X‐ray diffraction pattern measured for CANIBIC crystal powder. This model can therefore be developed in the future as a tool to predict lattice parameters and crystal structures of other novel double‐halide perovskites. Photoluminescence spectra obtained from each format show broad emission centered at 630 nm, as is typical for self‐trapped exciton emission; self‐trapped exciton emission is also confirmed by investigating photoluminescence intensity as a function of laser power. Nanocomposites are produced via the loading of nanocrystals of CANIBIC into PMMA. Although nanocomposite disks consisting of a small proportion of CANIBIC nanocrystals in PMMA have a smaller mass attenuation coefficient than a pressed pellet of CANIBIC, these disks have comparatively bright radioluminescence due to their optical transparency. These nanocomposite disks are therefore a particularly useful format for the practical use of the CANIBIC scintillator.

Isabel Helen Balbir Braddock, Maya Al Sid Cheikh, Joydip Ghosh, Roma Eve Mulholland, Joseph Gerard O'Neill, Vlad Stolojan, Carol Crean, Stephen Sweeney, Paul Jonathan Sellin (2022)Formamidinium Lead Halide Perovskite Nanocomposite Scintillators, In: Nanomaterials (Basel, Switzerland)12(13) Mdpi

While there is great demand for effective, affordable radiation detectors in various applications, many commonly used scintillators have major drawbacks. Conventional inorganic scintillators have a fixed emission wavelength and require expensive, high-temperature synthesis; plastic scintillators, while fast, inexpensive, and robust, have low atomic numbers, limiting their X-ray stopping power. Formamidinium lead halide perovskite nanocrystals show promise as scintillators due to their high X-ray attenuation coefficient and bright luminescence. Here, we used a room-temperature, solution-growth method to produce mixed-halide FAPbX(3) (X = Cl, Br) nanocrystals with emission wavelengths that can be varied between 403 and 531 nm via adjustments to the halide ratio. The substitution of bromine for increasing amounts of chlorine resulted in violet emission with faster lifetimes, while larger proportions of bromine resulted in green emission with increased luminescence intensity. By loading FAPbBr(3) nanocrystals into a PVT-based plastic scintillator matrix, we produced 1 mm-thick nanocomposite scintillators, which have brighter luminescence than the PVT-based plastic scintillator alone. While nanocomposites such as these are often opaque due to optical scattering from aggregates of the nanoparticles, we used a surface modification technique to improve transmission through the composites. A composite of FAPbBr(3) nanocrystals encapsulated in inert PMMA produced even stronger luminescence, with intensity 3.8 x greater than a comparative FAPbBr(3)/plastic scintillator composite. However, the luminescence decay time of the FAPbBr(3)/PMMA composite was more than 3 x slower than that of the FAPbBr(3)/plastic scintillator composite. We also demonstrate the potential of these lead halide perovskite nanocomposite scintillators for low-cost X-ray imaging applications.