Imperial College London

Dr Martyn A McLachlan

Faculty of EngineeringDepartment of Materials

Professor of Thin Films, Interfaces and Electronic Devices
 
 
 
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Contact

 

+44 (0)20 7594 9692martyn.mclachlan Website

 
 
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Location

 

RSM 2.03cRoyal School of MinesSouth Kensington Campus

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Summary

 

Publications

Publication Type
Year
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118 results found

Du T, Xu W, Xu S, Ratnasingham SR, Lin C-T, Kim J, Briscoe J, McLachlan MA, Durrant JRet al., 2020, Light-intensity and thickness dependent efficiency of planar perovskite solar cells: charge recombination versus extraction, Journal of Materials Chemistry C, Vol: 8, Pages: 12648-12655, ISSN: 2050-7526

Photoactive layer thickness is a key parameter for optimization of photovoltaic power conversion efficiency (PCE), yet its impact on charge extraction and recombination hasn’t been fully understood in perovskite solar cells (PSCs). Herein we find that in planar PSCs the perovskite thickness yielding maximal PCE is strongly light-intensity dependent. Whilst under 1 sun irradiation the PCE is relatively invariant for perovskite thicknesses between 250 to 750 nm, at lower light intensities (0.1–0.5 sun) the thickest devices yield strongly enhanced PCE, but at higher light intensities (>1 sun) the thinnest devices give optimal PCE. Our results unravel that increased perovskite thickness leads to enhanced light absorption, reduced interfacial recombination at open circuit but greater bimolecular recombination losses at short circuit thus is suitable for devices working under weak illumination, typical of many real-world applications. Reducing perovskite thickness, however, shows the contrast trend and is suitable for PSCs working under concentrated illumination.

Journal article

Mohan L, Ratnasingham SR, Panidi J, Anthopoulos TD, Binions R, McLachlan MA, Briscoe Jet al., 2020, Low Temperature Scalable Deposition of Copper(I) Thiocyanate Films via Aerosol-Assisted Chemical Vapor Deposition, Crystal Growth & Design, Vol: 20, Pages: 5380-5386, ISSN: 1528-7483

Copper(I) thiocyanate (CuSCN) is a stable, wide bandgap (>3.5 eV), low-cost p-type semiconductor widely used in a variety of optoelectronic applications, including thin film transistors, organic light-emitting diodes, and photovoltaic cells. For CuSCN to have impact in the commercial fabrication of such devices, large-area, low-cost deposition techniques are required. Here, we report a novel technique for deposition of CuSCN that addresses these challenges. Aerosol-assisted chemical vapor deposition (AACVD) is used to deposit highly crystalline CuSCN films at low temperature. AACVD is a commercially viable technique due to its low cost and inherent scalability. In this study, the deposition temperature, CuSCN concentration and carrier gas flow rate were studied and optimized, resulting in homogeneous films grown over areas approaching 30 cm2. At the optimized values, i.e., 60 °C using a 35 mg/mL solution and a carrier gas flow rate of 0.5 dm3/min, the film growth rate is around 100 nm/min. We present a thorough analysis of the film growth parameters and the subsequent morphology, composition, and structural and optical properties of the deposited thin films.

Journal article

Tang W, Zhang J, Ratnasingham S, Liscio F, Chen K, Liu T, Wan K, Galindez ES, Bilotti E, Reece M, Baxendale M, Milita S, McLachlan MA, Su L, Fenwick Oet al., 2020, Substitutional doping of hybrid organic-inorganic perovskite crystals for thermoelectrics, Journal of Materials Chemistry A, Vol: 8, Pages: 13594-13599, ISSN: 2050-7488

Hybrid organic–inorganic perovskites have generated considerable research interest in the field of optoelectronic devices. However, there have been significantly fewer reports of their thermoelectric properties despite some promising early results. In this article, we investigate the thermoelectric properties of bismuth-doped CH3NH3PbBr3 (MAPbBr3) single crystals. The high-quality Bi-doped crystals were synthesized by inverse temperature crystallization and it was found that Bi substitutes onto the B-site of the ABX3 perovskite lattice of MAPbBr3 crystals with very little distortion of the crystal structure. Bi doping does not significantly alter the thermal conductivity but dramatically enhances the electrical conductivity of MAPbBr3, increasing the charge carrier density by more than three orders of magnitude. We obtained a negative Seebeck coefficient of −378 μV K−1 for 15% (x = 0.15) Bi-doped MAPb(1−x)BixBr3 confirming n-type doping and also measured the figure of merit, ZT. This work highlights routes towards controlled substitutional doping of halide perovskites to optimise them for thermoelectric applications.

Journal article

Daboczi M, Kim J, Lee J, Kang H, Hamilton I, Lin C-T, Dimitrov SD, McLachlan MA, Lee K, Durrant JR, Kim J-Set al., 2020, Towards efficient integrated perovskite/organic bulk heterojunction solar cells: interfacial energetic requirement to reduce charge carrier recombination losses, Advanced Functional Materials, Vol: 30, Pages: 1-8, ISSN: 1616-301X

Integrated perovskite/organic bulk heterojunction (BHJ) solar cells have the potential to enhance the efficiency of perovskite solar cells by a simple one‐step deposition of an organic BHJ blend photoactive layer on top of the perovskite absorber. It is found that inverted structure integrated solar cells show significantly increased short‐circuit current (J sc) gained from the complementary absorption of the organic BHJ layer compared to the reference perovskite‐only devices. However, this increase in J sc is not directly reflected as an increase in power conversion efficiency of the devices due to a loss of fill factor. Herein, the origin of this efficiency loss is investigated. It is found that a significant energetic barrier (≈250 meV) exists at the perovskite/organic BHJ interface. This interfacial barrier prevents efficient transport of photogenerated charge carriers (holes) from the BHJ layer to the perovskite layer, leading to charge accumulation at the perovskite/BHJ interface. Such accumulation is found to cause undesirable recombination of charge carriers, lowering surface photovoltage of the photoactive layers and device efficiency via fill factor loss. The results highlight a critical role of the interfacial energetics in such integrated cells and provide useful guidelines for photoactive materials (both perovskite and organic semiconductors) required for high‐performance devices.

Journal article

Zhang J, Yang H, Zhang X, Morbidoni M, Burgess CH, Kilmurray R, Feng S, McLachlan MAet al., 2020, Effect of processing temperature on film properties of ZnO prepared by the aqueous method and related organic photovoltaics and LEDs, Inorganic Chemistry Frontiers, Vol: 7, Pages: 2809-2817, ISSN: 2052-1553

Here the influence of processing temperature on the properties of zinc oxide (ZnO) thin films fabricated using a carbon-free solution process is investigated. Our results show that the film processing temperature influences a wide range of structural and electro-optical properties. Films processed at 100 °C are shown to be formed of coalesced ZnO nanoparticles, whose dimensions increase with the processing temperature, accompanied by an increase in electron mobility. ZnO films processed at different temperatures were incorporated as electron transport layers (ETLs) in organic photovoltaic devices with PCDTBT:PC71BM as the active layer. We find that the ETLs processed at low temperature (100–200 °C) exhibit good device performance compared with those prepared at elevated temperatures, an effect we attribute to shifts in the work function and electrical conductivity. Interestingly a similar trend is observed when our ZnO is used as an electron injection layer in organic light emitting diodes, where the EILs processed at >200 °C show higher turn-on voltages and lower efficiencies than those annealed in the 100–200 °C range.

Journal article

Lin C-T, Ngiam J, Xu S, Chang Y-H, Du T, Macdonald TJ, Durrant J, McLachlan Met al., 2020, Enhancing the operational stability of unencapsulated perovskite solar cells through Cu-Ag bilayer electrode incorporation, Journal of Materials Chemistry A, Vol: 8, Pages: 8684-8691, ISSN: 2050-7488

We identify a facile strategy that significantly reduces electrode corrosion and device degradation in unencapsulated perovskite solar cells (PSCs) operating in ambient air. By employing Cu-Ag bilayer top electrodes PSCs, we show enhanced operational lifetime compared with devices prepared from single metal (Al, Ag and Cu) analogues. Time-of-flight secondary ion mass spectrometry depth profiles indicate that the insertion of the thin layer of Cu (10nm) below the Ag (100nm) electrode significantly reduces diffusion of species originating in the perovskite active layer into the electron transport layer and electrode. X-ray diffraction (XRD) analysis reveals the mutually beneficial relationship between the bilayer metals, whereby the thermally evaporated Ag inhibits Cu oxidation and the Cu prevents interfacial reactions between the perovskite and Ag. The results here not only demonstrate a simple approach to prevent the electrode and device degradation that enhance lifetime and stability but also give an insight into ageing related ion migration and structural reorganisation.

Journal article

Ambroz F, Sathasivam S, Lee R, Gadipelli S, Lin C-T, Xu S, Poduval RK, Mclachlan MA, Papakonstantinou I, Parkin IP, Macdonald TJet al., 2020, Corrigendum: Influence of lithium and lanthanum treatment on TiO2 nanofibers and their application in n-i-p solar cells, ChemElectroChem, Vol: 7, Pages: 2173-2173, ISSN: 2196-0216

Journal article

Wang S, Li W, Morbidoni M, McLachlan MA, Zhang Jet al., 2020, Building on soft hybrid perovskites: highly oriented metal oxides as electron transport and moisture resistant layers, APPLIED NANOSCIENCE, ISSN: 2190-5509

Journal article

Lin C-T, Lee J, Kim J, Macdonald TJ, Ngiam J, Xu B, Daboczi M, Xu W, Pont S, Park B, Kang H, Kim J-S, Payne DJ, Lee K, Durrant JR, McLachlan MAet al., 2020, Origin of open-circuit voltage enhancements in planar Perovskite solar cells induced by addition of bulky organic cations, Advanced Functional Materials, Vol: 30, ISSN: 1616-301X

The origin of performance enhancements in p‐i‐n perovskite solar cells (PSCs) when incorporating low concentrations of the bulky cation 1‐naphthylmethylamine (NMA) are discussed. A 0.25 vol % addition of NMA increases the open circuit voltage (Voc) of methylammonium lead iodide (MAPbI3) PSCs from 1.06 to 1.16 V and their power conversion efficiency (PCE) from 18.7% to 20.1%. X‐ray photoelectron spectroscopy and low energy ion scattering data show NMA is located at grain surfaces, not the bulk. Scanning electron microscopy shows combining NMA addition with solvent assisted annealing creates large grains that span the active layer. Steady state and transient photoluminescence data show NMA suppresses non‐radiative recombination resulting from charge trapping, consistent with passivation of grain surfaces. Increasing the NMA concentration reduces device short‐circuit current density and PCE, also suppressing photoluminescence quenching at charge transport layers. Both Voc and PCE enhancements are observed when bulky cations (phenyl(ethyl/methyl)ammonium) are incorporated, but not smaller cations (Cs/MA)—indicating size is a key parameter. Finally, it demonstrates that NMA also enhances mixed iodide/bromide wide bandgap PSCs (Voc of 1.22 V with a 1.68 eV bandgap). The results demonstrate a facile approach to maximizing Voc and provide insights into morphological control and charge carrier dynamics induced by bulky cations in PSCs.

Journal article

Georgiadou DG, Lin Y, Lim J, Ratnasingham S, McLachlan MA, Snaith HJ, Anthopoulos TDet al., 2020, High Responsivity and Response Speed Single‐Layer Mixed‐Cation Lead Mixed‐Halide Perovskite Photodetectors Based on Nanogap Electrodes Manufactured on Large‐Area Rigid and Flexible Substrates, Advanced Functional Materials, Vol: 30, Pages: 1909758-1909758, ISSN: 1616-301X

Journal article

Liu T, Yue S-Y, Ratnasingham S, Degousee T, Varsini P, Briscoe J, McLachlan MA, Hu M, Fenwick Oet al., 2019, Unusual Thermal Boundary Resistance in Halide Perovskites: A Way To Tune Ultralow Thermal Conductivity for Thermoelectrics, ACS APPLIED MATERIALS & INTERFACES, Vol: 11, Pages: 47507-47515, ISSN: 1944-8244

Journal article

Ambroz F, Xu W, Gadipelli S, Brett DJL, Lin C-T, Contini C, McLachlan MA, Durrant JR, Parkin IP, Macdonald TJet al., 2019, Room Temperature Synthesis of Phosphine-Capped Lead Bromide Perovskite Nanocrystals without Coordinating Solvents, PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION, Vol: 37, ISSN: 0934-0866

Journal article

Daboczi M, Hamilton I, Xu S, Luke J, Limbu S, Lee J, McLachlan MA, Lee K, Durrant JR, Baikie I, Kim J-Set al., 2019, The origin of open-circuit voltage losses in perovskite solar cells investigated by surface photovoltage measurement, ACS Applied Materials & Interfaces, Vol: 11, Pages: 46808-46817, ISSN: 1944-8244

Increasing the open circuit voltage (Voc) is one of the key strategies for further improvement of the efficiency of perovskite solar cells. It requires fundamental understanding of the complex optoelectronic processes related to charge carrier generation, transport, extraction and their loss mechanisms inside a device upon illumination. Herein we report the important origin of Voc losses in methylammonium lead iodide perovskite (MAPI) based solar cells, which results from undesirable positive charge (hole) accumulation at the interface between the perovskite photoactive layer and the PEDOT:PSS hole transport layer. We show strong correlation between the thickness-dependent surface photovoltage and device performance, unraveling that the interfacial charge accumulation leads to charge carrier recombination and results in a large decrease in Voc for the PEDOT:PSS/MAPI inverted devices (180 mV reduction in 50-nm-thick device compared to 230-nm-thick one). In contrast, accumulated positive charges at the TiO2/MAPI interface modify interfacial energy band bending, which leads to an increase in Voc for the TiO2/MAPI conventional devices (70 mV increase in 50-nm-thick device compared to 230-nm-thick one). Our results provide an important guideline for better control of interfaces in perovskite solar cells to improve device performance further.

Journal article

Macdonald TJ, Batmunkh M, Lin C-T, Kim J, Tune DD, Ambroz F, Li X, Xu S, Sol C, Papakonstantinou I, McLachlan MA, Parkin IP, Shapter JG, Durrant JRet al., 2019, Origin of performance enhancement in TiO2-carbon nanotube composite perovskite solar cells, Small Methods, Vol: 3, Pages: 1-10, ISSN: 2366-9608

Carbon nanotubes are shown to be beneficial additives to perovskite solar cells, and the inclusion of such nanomaterials will continue to play a crucial role in the push toward developing efficient and stable device architectures. Herein, titanium dioxide/carbon nanotube composite perovskite solar cells are fabricated, and device performance parameters are correlated with spectroscopic signatures of the materials to understand the origin of performance enhancement. By probing the charge carrier dynamics with photoluminescence and femtosecond transient absorption spectroscopy, the results indicate that charge transfer is not improved by the presence of the carbon nanotubes. Instead, carbon nanotubes are shown to passivate the electronic defect states within the titanium dioxide, which can lead to stronger radiative recombination in the titanium dioxide/carbon nanotube films. The defect passivation allows the perovskite solar cells made using an optimized titanium dioxide/carbon nanotube composite to achieve a peak power conversion efficiency of 20.4% (19% stabilized), which is one of the highest values reported for perovskite solar cells not incorporating a mixed cation light absorbing layer. The results discuss new fundamental understandings for the role of carbon nanomaterials in perovskite solar cells and present a significant step forward in advancing the field of high‐performance photovoltaics.

Journal article

Panidi J, Kainth J, Paterson AF, Wang S, Tsetseris L, Emwas AH, McLachlan MA, Heeney M, Anthopoulos TDet al., 2019, Introducing a nonvolatile N-type dopant drastically improves electron transport in polymer and small-molecule organic transistors, Advanced Functional Materials, Vol: 29, Pages: 1-10, ISSN: 1616-301X

KGaA, Weinheim Molecular doping is a powerful yet challenging technique for enhancing charge transport in organic semiconductors (OSCs). While there is a wealth of research on p-type dopants, work on their n-type counterparts is comparatively limited. Here, reported is the previously unexplored n-dopant (12a,18a)-5,6,12,12a,13,18,18a,19-octahydro-5,6-dimethyl- 13,18[1′,2′]-benzenobisbenzimidazo [1,2-b:2′,1′-d]benzo[i][2.5]benzodiazo-cine potassium triflate adduct (DMBI-BDZC) and its application in organic thin-film transistors (OTFTs). Two different high electron mobility OSCs, namely, the polymer poly[[N,N′-bis(2-octyldodecyl)-naphthalene-1,4,5,8- bis(dicarboximide)-2,6-diyl]-alt-5,5′-(2′-bithiophene)] and a small-molecule naphthalene diimides fused with 2-(1,3-dithiol-2-ylidene)malononitrile groups (NDI-DTYM2) are used to study the effectiveness of DMBI-BDZC as a n-dopant. N-doping of both semiconductors results in OTFTs with improved electron mobility (up to 1.1 cm2 V−1 s−1), reduced threshold voltage and lower contact resistance. The impact of DMBI-BDZC incorporation is particularly evident in the temperature dependence of the electron transport, where a significant reduction in the activation energy due to trap deactivation is observed. Electron paramagnetic resonance measurements support the n-doping activity of DMBI-BDZC in both semiconductors. This finding is corroborated by density functional theory calculations, which highlights ground-state electron transfer as the main doping mechanism. The work highlights DMBI-BDZC as a promising n-type molecular dopant for OSCs and its application in OTFTs, solar cells, photodetectors, and thermoelectrics.

Journal article

Du T, Xu W, Daboczi M, Kim J, Xu S, Lin C-T, Kang H, Lee K, Heeney MJ, Kim J-S, Durrant JR, McLachlan MAet al., 2019, p-Doping of organic hole transport layers in p–i–n perovskite solar cells: correlating open-circuit voltage and photoluminescence quenching, Journal of Materials Chemistry A, Vol: 7, Pages: 18971-18979, ISSN: 2050-7488

Doping is a widely implemented strategy for enhancing the inherent electronic properties of charge transport layers in photovoltaic (PV) devices. Here, in direct contrast to existing understanding, we find that a reduction in p-doping of the organic hole transport layer (HTL) leads to substantial improvements in PV performance in planar p–i–n perovskite solar cells (PSCs), driven by improvements in open circuit voltage (VOC). Employing a range of transient and steady state characterisation tools, we find that the improvements of VOC correlate with reduced surface recombination losses in less p-doped HTLs. A simple device model including screening of bulk electric fields in the perovskite layer is used to explain this observation. In particular, photoluminescence (PL) emission of complete solar cells shows that efficient performance is correlated to a high PL intensity at open circuit and a low PL intensity at short circuit. We conclude that desirable transport layers for p–i–n PSCs should be charge selective contacts with low doping densities.

Journal article

Cha H, Fish G, Luke J, Alraddadi A, Lee HH, Zhang W, Dong Y, Limbu S, Wadsworth A, Maria IP, Francas L, Sou HL, Du T, Kim J-S, McLachlan MA, McCulloch I, Durrant JRet al., 2019, Suppression of Recombination Losses in Polymer:Nonfullerene Acceptor Organic Solar Cells due to Aggregation Dependence of Acceptor Electron Affinity, ADVANCED ENERGY MATERIALS, Vol: 9, ISSN: 1614-6832

Journal article

Ambroz F, Sathasivam S, Lee R, Gadipelli S, Lin C, Xu S, Poduval RK, Mclachlan MA, Papakonstantinou I, Parkin IP, Macdonald TJet al., 2019, Influence of Lithium and Lanthanum Treatment on TiO 2 Nanofibers and Their Application in n‐i‐p Solar Cells, ChemElectroChem, Vol: 6, Pages: 3529-3529, ISSN: 2196-0216

Journal article

Ambroz F, Sathasivam S, Lee R, Gadipelli S, Lin C, Xu S, Poduval RK, Mclachlan MA, Papakonstantinou I, Parkin IP, Macdonald TJet al., 2019, Influence of lithium and lanthanum treatment on TiO2 nanofibers and their application in n‐i‐p solar cells, ChemElectroChem, Vol: 6, Pages: 3590-3598, ISSN: 2196-0216

The addition of cations to TiO2 photoelectrodes is routinely accepted as a route to enhance the performance of conventional n‐i‐p solar cells. However, this is typically achieved in multiple steps or by the incorporation of expensive and hydroscopic cationic precursors such as lithium bis(trifluoromethanesulfonyl)imide. In addition, it is often unclear as to whether the incorporation of such cation sources is inducing “doping” or simply transformed into cationic oxides on the surface of the photoelectrodes. In this study, TiO2 nanofibers were produced through a simple electrospinning technique and modified by introducing lithium and lanthanum precursors in one step. Our results show that the addition of both cations caused minimal substitutional or interstitial doping of TiO2. Brunauer‐Emmett‐Teller measurements showed that lanthanum‐treated TiO2 nanofibers had an increase in surface area, which even exceeded that of TiO2 P25 nanoparticles. Finally, treated and untreated TiO2 nanofibers were used in n‐i‐p solar cells. Photovoltaic characteristics revealed that lanthanum treatment was beneficial, whereas lithium treatment was found to be detrimental to the device performance for both dye‐sensitized and perovskite solar cells. The results discuss new fundamental understandings for two of the commonly incorporated cationic dopants in TiO2 photoelectrodes, lithium and lanthanum, and present a significant step forward in advancing the field of materials chemistry for photovoltaics.

Journal article

Georgiadou DG, Lin Y, Lim J, Ratnasingham S, McLachlan MA, Snaith HJ, Anthopoulos TDet al., 2019, High Responsivity and Response Speed Single‐Layer Mixed‐Cation Lead Mixed‐Halide Perovskite Photodetectors Based on Nanogap Electrodes Manufactured on Large‐Area Rigid and Flexible Substrates, Advanced Functional Materials, Vol: 29, Pages: 1901371-1901371, ISSN: 1616-301X

Journal article

Mehmood U, Harrabi K, Hussein IA, Shanmugam N, Mekki A, Mekki M, McLachlan MAet al., 2019, Correction to: A study on stability of active layer of polymer solar cells: effect of UV–visible light with different conditions, Polymer Bulletin, ISSN: 0170-0839

Journal article

Sun G, Shahid M, Fei Z, Xu S, Eisner FD, Anthopoulos TD, McLachlan MA, Heeney Met al., 2019, Highly-efficient semi-transparent organic solar cells utilising non-fullerene acceptors with optimised multilayer MoO3/Ag/MoO3 electrodes (vol 3, pg 450, 2019), MATERIALS CHEMISTRY FRONTIERS, Vol: 3, Pages: 955-955

Journal article

Sun G, Shahid M, Fei Z, Xu S, Eisner FD, Anthopolous TD, McLachlan MA, Heeney Met al., 2019, Highly-efficient semi-transparent organic solar cells utilising non-fullerene acceptors with optimised multilayer MoO3/Ag/MoO3 electrodes, Materials Chemistry Frontiers, Vol: 3, Pages: 450-455, ISSN: 2052-1537

We report the optimisation of a semi-transparent solar cell based on a blend of a recently reported high performance donor polymer (PFBDB-T) with a non-fullerene acceptor derivative (C8-ITIC). The performance is shown to strongly depend on the nature of the semi-transparent electrode, and we report the optimal fabrication conditions for a multilayer MoO3/Ag/MoO3 electrode. The effect of deposition rate and layer thickness of both the Ag and the outer MoO3 on transparency and sheet resistance is investigated, and is shown to have a significant impact on the overall device performance. The optimised PFBDB-T:C8-ITIC based devices exhibit an average power conversion efficiency (PCE) of 9.2% with an average visible transmittance (AVT) of 22%.

Journal article

Lin C-T, Rossi F, Kim J, Baker J, Ngiam J, Xu S, Pont S, Aristidou N, Haque S, Watson T, McLachlan M, Durrant Jet al., 2019, Evidence for surface defect passivation as the origin of the remarkable photostability of unencapsulated perovskite solar cells employing aminovaleric acid as a processing additive, Journal of Materials Chemistry A, Vol: 7, ISSN: 2050-7496

This study addresses the cause of enhanced stability of methyl ammonium lead iodide when processed with aminovaleric acid additives (AVA-MAPbI3) in screen printed, hole transport layer free perovskite solar cells with carbon top electrodes (c-PSC). Employing AVA as an additive in the active layer caused a 40-fold increase in device lifetime measured under full sun illumination in ambient air (RH ~15%). This stability improvement with AVA was also observed in optical photobleaching studies of planar films on glass, indicating this improvement is intrinsic to the perovskite film. Employing low-energy ion scattering spectroscopy, photoluminescence studies as a function of AVA and oxygen exposure, and a molecular probe for superoxide generation, we conclude that even though superoxide is generated in both AVA-MAPbI3 and MAPbI3 films, AVA located at grain boundaries is able to passivate surface defect sites, resulting in enhanced resistivity to oxygen induced degradation. These results are discussed in terms of their implications for the design of environmentally stable perovskite solar cells.

Journal article

Mehmood U, Harrabi K, Hussein IA, Shanmugam N, Mekki A, Mekki M, McLachlan MAet al., 2019, A study on stability of active layer of polymer solar cells: effect of UV–visible light with different conditions, Polymer Bulletin, Vol: 76, Pages: 525-537, ISSN: 0170-0839

© 2018, Springer-Verlag GmbH Germany, part of Springer Nature. Abstract: The objective of this study is to investigate the stability of the active layer of polymer solar cells from the effect of UV–visible light irradiation using different conditions with respect to time. The active layers were composed of poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl C61 butyric acid methyl ester (PCBM), deposited on conductive glass substrates through spin coating. These samples are placed in a UV–visible light exposure chamber using different conditions (heat and water) over the specific periods of time. The samples are analyzed by UV–visible absorption spectroscopy, X-ray photoelectron spectroscopy and Fourier transforms infrared spectroscopy (FTIR) measurements. The results indicate that after continuous exposure to UV irradiation for 72 and 120 h, the sample shows a significant decrease in absorption of the main peak. The sample shows around 25% loss in absorption (main peak) after 72 h of irradiation. The FTIR results illustrate a progressive decrease in intensities of all typical absorption peaks owing to P3HT ring scission, side chain oxidation as well as degradation of the side groups of PCBM. Graphical abstract: [Figure not available: see fulltext.].

Journal article

Kafizas A, Xing X, Selim S, Mesa CA, Ma Y, Burgess C, McLachlan MA, Durrant JRet al., 2019, Ultra-thin Al<inf>2</inf>O<inf>3</inf>coatings on BiVO<inf>4</inf>photoanodes: Impact on performance and charge carrier dynamics, Catalysis Today, Vol: 321-322, Pages: 59-66, ISSN: 0920-5861

Bismuth vanadate (BiVO 4 ) has emerged as one of the most promising photoanode materials for oxidising water due to its visible light activity and low cost. Recent studies have shown that the performance of BiVO 4 photoanodes can be remarkably improved when coated with ultra-thin passivation layers. In this article we investigate the use of ultra-thin Al 2 O 3 layers grown using atomic layer deposition (ALD). At an optimum thickness (~0.33nm, 3 ALD cycles), the Al 2 O 3 layer favourably shifted the onset potential by ~200mV and increased photocatalytic currents for the water oxidation reaction. When held at 1.23V RHE , we observe a remarkable increase in the theoretical solar photocurrent; from ~0.47mAcm -2 in uncoated BiVO 4 to ~3.0mAcm -2 in Al 2 O 3 -coated BiVO 4 . Using transient photocurrent (TPC) and transient absorption spectroscopy (TAS) the charge carrier dynamics in Al 2 O 3 -coated BiVO 4 photoanodes were examined for the first time. TPC showed that photogenerated electrons in the BiVO 4 layer were extracted within ~1ms. TAS showed that the remaining holes oxidised water from ~100ms to 1s. Ultra-thin Al 2 O 3 coatings did not improve the reaction kinetics towards water oxidation, but rather, suppressed bi-molecular recombination on the μs-ms timescale in BiVO 4 , and increased the yield of long-lived holes on the ms-s timescale required to oxidise water. This is attributed to an inhibition of surface recombination on BiVO 4 by Al 2 O 3 , which inhibited the early timescale recombination of charge carriers formed within the space charge layer.

Journal article

Lee HKH, Barbe J, Meroni SMP, Du T, Lin C-T, Pockett A, Troughton J, Jain SM, De Rossi F, Baker J, Carnie MJ, McLachlan MA, Watson TM, Durrant JR, Tsoi WCet al., 2019, Outstanding Indoor Performance of Perovskite Photovoltaic Cells - Effect of Device Architectures and Interlayers, SOLAR RRL, Vol: 3, ISSN: 2367-198X

Journal article

Du T, Burgess C, Lin C-T, Eisner F, Kim J, Xu S, Kang H, Durrant J, McLachlan Met al., 2018, Probing and controlling intra-grain crystallinity for improved low-temperature processed perovskite solar cells, Advanced Functional Materials, Vol: 28, ISSN: 1616-301X

Here, previously unobserved nanoscale defects residing within individual grains of solution‐processed methylammonium lead tri‐iodide (CH3NH3PbI3, MAPI) thin films are identified. Using scanning transmission electron microscopy (STEM), the defects inherently associated with the established solution‐processing methodology are identified, and a facile processing modification to eliminate these defects is introduced. Specifically, defect elimination is achieved by coannealing the as‐deposited MAPI layer with the electron transport layer (phenyl‐C61‐butyric acid methyl, PCBM) resulting in devices that significantly outperform devices prepared using the established methodology—with power conversion efficiencies increasing from 13.6% to 17.4%. The use of transmission electron microscopy allows the correlation of performance enhancements to improved intragrain crystallinity and shows that highly coherent crystallographic orientation results within individual grains when processing is modified. Detailed optoelectronic characterization reveals that the improved intragrain crystallinity drives an improvement of charge collection and a reduction of PEDOT:PSS/perovskite interfacial recombination. The study suggests that the microstructural defects in MAPI, owing to a lack of structural coherence throughout the thickness of thin film, are a significant cause of interfacial recombination.

Journal article

Kim J, Godin R, Dimitrov SD, Du T, Bryant D, McLachlan MA, Durrant JRet al., 2018, Excitation density dependent photoluminescence quenching and charge transfer efficiencies in hybrid perovskite/organic semiconductor bilayers, Advanced Energy Materials, Vol: 8, ISSN: 1614-6832

This study addresses the dependence of charge transfer efficiency between bilayers of methylammonium lead iodide (MAPI3) with PC61BM or poly(3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) charge transfer layers on excitation intensity. It analyzes the kinetic competition between interfacial electron/hole transfer and charge trapping and recombination within MAPI3 by employing a range of optical measurements including steady-state (SS) photoluminescence quenching (PLQ), and transient photoluminescence and absorption over a broad range of excitation densities. The results indicate that PLQ measurements with a typical photoluminescence spectrometer can yield significantly different transfer efficiencies to those measured under 1 Sun irradiation. Steady-state and pulsed measurements indicate low transfer efficiencies at low excitation conditions (<5E + 15 cm−3) due to rapid charge trapping and low transfer efficiencies at high excitation conditions (>5E + 17 cm−3) due to fast bimolecular recombination. Efficient transfer to PC61BM or PEDOT:PSS is only observed under intermediate excitation conditions (≈1 Sun irradiation) where electron and hole transfer times are determined to be 36 and 11 ns, respectively. The results are discussed in terms of their relevance to the excitation density dependence of device photocurrent generation, impact of charge trapping on this dependence, and appropriate methodologies to determine charge transfer efficiencies relevant to device performance.

Journal article

Loh AYY, Burgess CH, Tanase DA, Ferrari G, McLachlan MA, Cass AEG, Albrecht Tet al., 2018, Electric single-molecule hybridization detector for short DNA fragments, Analytical Chemistry, Vol: 90, Pages: 14063-14071, ISSN: 0003-2700

By combining DNA nanotechnology and high-bandwidth single-molecule detection in nanopipets, we demonstrate an electric, label-free hybridization sensor for short DNA sequences (<100 nucleotides). Such short fragments are known to occur as circulating cell-free DNA in various bodily fluids, such as blood plasma and saliva, and have been identified as disease markers for cancer and infectious diseases. To this end, we use as a model system an 88-mer target from the RV1910c gene in Mycobacterium tuberculosis, which is associated with antibiotic (isoniazid) resistance in TB. Upon binding to short probes attached to long carrier DNA, we show that resistive-pulse sensing in nanopipets is capable of identifying rather subtle structural differences, such as the hybridization state of the probes, in a statistically robust manner. With significant potential toward multiplexing and high-throughput analysis, our study points toward a new, single-molecule DNA-assay technology that is fast, easy to use, and compatible with point-of-care environments.

Journal article

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