Thomas J. Macdonald

Dr. Thomas J. Macdonald

Department of Chemistry and Centre for Plastic Electronics, Imperial College London, London, W12 0BZ, United Kingdom
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Research Focus & Metrics

Academic Career Length

16Years (2011-Present)

(Calculated once Scilit publication data is synced: current year − year of first publication + 1)

Representative Publications

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25 August 2021 in Energy & Environmental Science
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Journal Article
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FRFlorine M. Rombach
Florine M. Rombach
SHSaif A. Haque
Saif A. Haque
TMThomas J. Macdonald
Thomas J. Macdonald
Organic semiconductors have become essential parts of thin-film electronic devices, particularly as hole transport layers (HTLs) in perovskite solar cells (PSCs) where they represent one of the major bottlenecks to further enhancements in both device stability and efficiency. Small molecule 2,2′,7,7′-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9′-spirobifluorene (spiro-OMeTAD) and polymer poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) are two of the first successful HTLs used in PSCs, and have remained at the forefront of developing high efficiency devices for almost a decade. Since their first application, many investigations into the properties of spiro-OMeTAD and PTAA have contributed to a growing understanding of the mechanisms that enable their success as HTLs. This review summarizes and discusses the key electronic and morphological properties, doping strategies and mechanisms, and degradation pathways of both spiro-OMeTAD and PTAA. A critical comparison between the two materials is provided, highlighting both the similarities which explain their enduring popularity as well as key differences in electrical and morphological properties. From this analysis emerges an improved understanding of the fundamental properties that enable the persistent success of HTL materials, which are found to include not only hole conductivity, band gap, and morphology, but also interactions with dopants, the perovskite, and environmental stressors. The knowledge about these properties, which are critically summarized in this review, is also applicable to the many other types of organic electronic devices now employing spiro-OMeTAD and PTAA. A detailed examination of the properties of materials reveals a clear set of guiding principles for the development of future generation HTLs. Applying these design strategies to produce more advanced HTLs will be essential to further improve the stability, efficiency, and commercialization of PSCs.

16 August 2018 in Small Methods
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FAFilip Ambroz
Filip Ambroz
TMThomas J. Macdonald
Thomas J. Macdonald
VMVladimir Martis
Vladimir Martis
IPIvan Parkin
Ivan Parkin
Surface area determination with the Brunauer–Emmett–Teller (BET) method is a widely used characterization technique for metal–organic frameworks (MOFs). Since these materials are highly porous, the use of the BET theory can be problematic. Several researchers have evaluated the BET method to gain insights into the usefulness of the obtained results and interestingly, their findings are not always consistent. In this review, the suitability of the BET method is discussed for MOFs that have a diverse range of pore widths below the diameters of N2 or Ar and above 20 Å. In addition, the surface area of MOFs that are obtained by implementing different approaches, such as grand canonical Monte Carlo simulations, calculations from the crystal structures or based on experimental N2, Ar, or CO2 adsorption isotherms, are compared and evaluated. Inconsistencies in the state‐of‐the‐art are also noted. Based on the current literature, an overview is provided of how the BET method can give useful estimations of the surface areas for the majority of MOFs, but there are some crucial and specific exceptions which are highlighted in this review.

14 May 2021 in Nature Communications
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LLLuis Lanzetta
Luis Lanzetta
TWThomas Webb
Thomas Webb
NZNourdine Zibouche
Nourdine Zibouche
XLXinxing Liang
Xinxing Liang
DDDong Ding
Dong Ding
SHSaif A. Haque
Saif A. Haque
Tin perovskites have emerged as promising alternatives to toxic lead perovskites in next-generation photovoltaics, but their poor environmental stability remains an obstacle towards more competitive performances. Therefore, a full understanding of their decomposition processes is needed to address these stability issues. Herein, we elucidate the degradation mechanism of 2D/3D tin perovskite films based on (PEA)0.2(FA)0.8SnI3(where PEA is phenylethylammonium and FA is formamidinium). We show that SnI4, a product of the oxygen-induced degradation of tin perovskite, quickly evolves into iodine via the combined action of moisture and oxygen. We identify iodine as a highly aggressive species that can further oxidise the perovskite to more SnI4, establishing a cyclic degradation mechanism. Perovskite stability is then observed to strongly depend on the hole transport layer chosen as the substrate, which is exploited to tackle film degradation. These key insights will enable the future design and optimisation of stable tin-based perovskite optoelectronics.

11 December 2021 in Advanced Materials
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TDTian Du
Tian Du
TMThomas J. Macdonald
Thomas J. Macdonald
RYRuoxi Yang
Ruoxi Yang
Meng LiMeng Li
Meng Li
ZJZhongyao Jiang
Zhongyao Jiang
JBJoe Briscoe
Joe Briscoe
Formamidinium lead triiodide (FAPbI3) is attractive for photovoltaic devices due to its optimal bandgap at around 1.45 eV and improved thermal stability compared with methylammonium‐based perovskites. Crystallization of phase‐pure α‐FAPbI3 conventionally requires high‐temperature thermal annealing at 150 °C whilst the obtained α‐FAPbI3 is metastable at room temperature. Here, aerosol‐assisted crystallization (AAC) is reported, which converts yellow δ‐FAPbI3 into black α‐FAPbI3 at only 100 °C using precursor solutions containing only lead iodide and formamidinium iodide with no chemical additives. The obtained α‐FAPbI3 exhibits remarkably enhanced stability compared to the 150 °C annealed counterparts, in combination with improvements in film crystallinity and photoluminescence yield. Using X‐ray diffraction, X‐ray scattering, and density functional theory simulation, it is identified that relaxation of residual tensile strains, achieved through the lower annealing temperature and post‐crystallization crystal growth during AAC, is the key factor that facilitates the formation of phase‐stable α‐FAPbI3. This overcomes the strain‐induced lattice expansion that is known to cause the metastability of α‐FAPbI3. Accordingly, pure FAPbI3 p–i–n solar cells are reported, facilitated by the low‐temperature (≤100 °C) AAC processing, which demonstrates increases of both power conversion efficiency and operational stability compared to devices fabricated using 150 °C annealed films.

17 September 2020 in Communications Chemistry
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CCClaudia Contini
Claudia Contini
JHJames W Hindley
James W Hindley
TMThomas J. Macdonald
Thomas J. Macdonald
JBJoseph D. Barritt
Joseph D. Barritt
OCOscar Ces
Oscar Ces
NQNick Quirke
Nick Quirke
The rapid development of nanotechnology has led to an increase in the number and variety of engineered nanomaterials in the environment. Gold nanoparticles (AuNPs) are an example of a commonly studied nanomaterial whose highly tailorable properties have generated significant interest through a wide range of research fields. In the present work, we characterise the AuNP-lipid membrane interaction by coupling qualitative data with quantitative measurements of the enthalpy change of interaction. We investigate the interactions between citrate-stabilised AuNPs ranging from 5 to 60 nm in diameter and large unilamellar vesicles acting as a model membrane system. Our results reveal the existence of two critical AuNP diameters which determine their fate when in contact with a lipid membrane. The results provide new insights into the size dependent interaction between AuNPs and lipid bilayers which is of direct relevance to nanotoxicology and to the design of NP vectors.

18 September 2020 in Small Methods
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Journal Article
Open access
YZYuan Zhang
Yuan Zhang
AKAshleigh Kirs
Ashleigh Kirs
FAFilip Ambroz
Filip Ambroz
CLChieh‐Ting Lin
Chieh‐Ting Lin
ABAbdulaziz S. R. Bati
Abdulaziz S. R. Bati
TMThomas J. Macdonald
Thomas J. Macdonald
Organic–inorganic hybrid perovskite solar cells (PSCs) have attracted significant attention in recent years due to their high‐power conversion efficiency, simple fabrication, and low material cost. However, due to their high sensitivity to moisture and oxygen, high efficiency PSCs are mainly constructed in an inert environment. This has led to significant concerns associated with the long‐term stability and manufacturing costs, which are some of the major limitations for the commercialization of this cutting‐edge technology. Over the past few years, excellent progress in fabricating PSCs in ambient conditions has been made. These advancements have drawn considerable research interest in the photovoltaic community and shown great promise for the successful commercialization of efficient and stable PSCs. In this review, after providing an overview to the influence of an ambient fabrication environment on perovskite films, recent advances in fabricating efficient and stable PSCs in ambient conditions are discussed. Along with discussing the underlying challenges and limitations, the most appropriate strategies to fabricate efficient PSCs under ambient conditions are summarized along with multiple roadmaps to assist in the future development of this technology.