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Durham Research Online Durham Research Online Deposited in DRO: 07 May 2019 Version of attached le: Accepted Version Peer-review status of attached le: Peer-reviewed Citation for published item: Chaudhry, Mujeeb Ullah and Wang, Nana and Tetzner, Kornelius and Seitkhan, Akmaral and Miao, Yanfeng and Sun, Yan and Petty, Michael C. and Anthopoulos, Thomas D. and Wang, Jianpu and Bradley, Donal D. C. (2019) 'Lightemitting transistors based on solutionprocessed heterostructures of selforganized multiplequantumwell perovskite and metaloxide semiconductors.', Advanced electronic materials., 5 (7). p. 1800985. Further information on publisher's website: https://doi.org/10.1002/aelm.201800985 Publisher's copyright statement: This is the accepted version of the following article: Chaudhry, Mujeeb Ullah, Wang, Nana, Tetzner, Kornelius, Seitkhan, Akmaral, Miao, Yanfeng, Sun, Yan, Petty, Michael C., Anthopoulos, Thomas D., Wang, Jianpu Bradley, Donal D. C. (2019). LightEmitting Transistors Based on SolutionProcessed Heterostructures of SelfOrganized MultipleQuantumWell Perovskite and MetalOxide Semiconductors. Advanced Electronic Materials 5(7): 1800985, which has been published in nal form at https://doi.org/10.1002/aelm.201800985. This article may be used for non-commercial purposes in accordance With Wiley Terms and Conditions for self-archiving. Additional information: Use policy The full-text may be used and/or reproduced, and given to third parties in any format or medium, without prior permission or charge, for personal research or study, educational, or not-for-prot purposes provided that: • a full bibliographic reference is made to the original source • a link is made to the metadata record in DRO • the full-text is not changed in any way The full-text must not be sold in any format or medium without the formal permission of the copyright holders. Please consult the full DRO policy for further details. Durham University Library, Stockton Road, Durham DH1 3LY, United Kingdom Tel : +44 (0)191 334 3042 | Fax : +44 (0)191 334 2971 https://dro.dur.ac.uk Light-emitting transistors based on solution processed heterostructures of self-organized multiple quantum well perovskite and metal-oxide semiconductors Mujeeb Ullah Chaudhry,*1 Nana Wang,2 Kornelius Tetzner,3 Akmaral Seitkhan,4 Yanfeng Miao,2 Yan Sun,2 Michael C. Petty,1 Thomas D. Anthopoulos,*3, 4 Jianpu Wang,*2 Donal D.C. Bradley*5 1 Department of Engineering, Durham University, Lower Mount Joy, South Road, Durham, DH1 3LE, United Kingdom. 2 Key Laboratory of Flexible Electronics (KLOFE) & Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing Tech University (NanjingTech), 30 South Puzhu Road, Nanjing 211816, P.R. China. 3Department of Physics and Centre for Plastic Electronics, Blackett Laboratory, Imperial College London, London SW7 2BW, United Kingdom. 4 King Abdullah University of Science and Technology (KAUST), KAUST Solar Center, Physical Science and Engineering Division, Thuwal 23955, Saudi Arabia. 5 Departments of Physics and Engineering Science, Division of Mathematical, Physical and Life Sciences, University of Oxford, 9 Parks Road, Oxford OX1 3PD, United Kingdom. *Address correspondence to: [email protected]; [email protected]; [email protected]; [email protected] 1 Abstract Solution-processed hybrid organic-inorganic perovskite semiconductors have demonstrated remarkable performance for both photovoltaic and light-emitting-diode applications in recent years, launching a new field of condensed matter physics. However, their use in additional emerging opto-electronic applications such as light-emitting field effect (LEFET) transistors has been surprisingly limited with only a few exceptions with low performance. We report the development of hybrid light-emitting field-effect transistors (LEFETs) consisting of a solution processed self-organized multiple quantum well (MQW) lead iodide perovskite layer grown onto an electron transporting In2O3/ZnO heterojunction channel. The multi-layer transistors offer bi-functional characteristics, namely transistor function with high electron mobility (>20 cm2/Vs) and a large current On/Off ratio (>106), combined with near infrared (NIR) light 2 emission (max = 783 nm) with a promising external quantum efficiency (≈ 0.2 % at 18 cd/m ). A further interesting feature of these hybrid LEFETs, in comparison to previously reported structures, is their highly uniform and stable emission characteristics, which make them attractive for smart-pixel-format display applications. 2 Organometal halide perovskite semiconductors possess highly attractive optoelectronic properties,1-10 which combined with cost-effective solution processing have fuelled growing interest in photovoltaic,5-13 water splitting,14 light-emitting diode (LED),15-18 optically-pumped laser,19-21 and X-ray detector22, 23 applications. The combination of high photoluminescence quantum efficiency2 (PLQE), high ambipolar charge carrier mobility24-26 and widely tuneable optical gaps (spanning the visible to near infrared spectrum)26 is of especial interest for LEDs,15- 18 light-emitting field effect transistors (LEFETs)27-29 and lasers.30,31 LEFETs, in particular, integrate the switching functionality of FETs with the light emission properties of an LED.32 Although LEFETs demand simultaneous optimisation of multiple electrical and optical device characteristics,32-34 they are highly attractive for applications in optical communications and high-definition displays due to their potential for simplifying and maximising the emissive aperture ratio of the pixel.32-38 In the case of perovskite LEFETs (PeLEFETs), there has been rather little progress since 27 the first report in 2015 of methylammonium lead iodide (CH3NH3PbI3) devices. Light emission was observed only at temperatures ≤ 178 K, with charge carrier mobilities limited to ≈10-5 cm2/Vs. Subsequent AC driving at high frequency allows room temperature emission by suppressing ion migration but with low (unquantified) intensity.28 At low temperature the emission is stronger and quantifiable, but only reaches a luminance of 0.94 cd/m2 at 78K for 100kHz driving.29 This is despite the remarkable progress achieved in the area of perovskite- 39 2 based LEDs (EQEs >14%) and the predictions for ultra-high electron (µe ≈ 1,500 cm /Vs) 2 24,25,26 and hole (µh ≈ 3,100 cm /Vs) mobility. This limited progress is likely due to the microstructure of the three-dimensional (3D) perovskite layers15-16 which have often been employed, and the adverse effects of ion migration and polarization disorder.40 3 More recently, a new class of self-organized multiple quantum well (MQW) perovskite has been demonstrated.18,36 This class of perovskite combines high photoluminescence quantum efficiency, PLQE ( ≈ 60 %) with superior layer uniformity manifested as low surface roughness (rms ≈ 2.6 nm). Red/near-infrared (max = 791 nm) and green (max = 532 nm) MQWs perovskite LEDs have been reported, with state-of-the-art external quantum efficiency (EQE) values of 12.7% and 15.5%, respectively.41-44 Sky-blue LED devices have also been reported with EQE up to 1.5%.45 In comparison to lead halide perovskites, solution- processed metal-oxide semiconductors are known to yield high performance transistors and integrated circuits,46-48 with electron mobilities reaching ≈ 50 cm2/Vs for structures based on oxide-oxide heterojunctions which promote the formation of a two-dimensional-like electron gas.47 These latter materials do not, however, give efficient light emission and so are not suited on their own to LEFET use. Herein we report the development of an innovative strategy that combines these two classes of material in a heterostructure PeLEFET architecture. This heterostructure consists of a self-organized NFPI7 (vide infra) MQW perovskite as the light-emitting and hole- transporting layer, together with a high electron mobility In2O3/ZnO heterostructure in a layered channel configuration. The combination yields relatively efficient (0.2% EQE at 18 cd/m2) PeLEFETs operating at room temperature, with effective electron mobilities of the order of ~ 20 cm2/Vs and a high channel current On/Off ratio >106. Light emission emerges uniformly from the entire drain electrode region (hole injecting contact) and peaks in the near infra-red at 783 nm (a wavelength widely used for fluorescence-free Raman spectroscopy)49, with a full-width-at-half-maximum linewidth = 50 nm that ensures enough visible red light for it to be readily observable by eye. The electrical and optical performance of the PeLEFETs studied here is orders of magnitude better than previously reported and offers encouragement for further progress towards a variety of solution processed inorganic optoelectronic devices. 4 A schematic of the perovskite MQW structure, referred to hereafter as NFPI7, is shown in Fig. 1(a). NFPI7 films were deposited by spin-coating a precursor solution comprising 1- naphthylmethylamine iodide (NMAI), formamidinium iodide (FAI) and PbI2 in molar ratio 2:1:2 dissolved in N,N-dimethylformamide (DMF) (7 wt.%) and annealed at 100 oC for 10 min (see Experimental Methods for details). Atomic force microscopy (AFM) measurements on typical 20 nm thickness NFPI7 films show uniform surface coverage with 2 nm root-mean- square roughness (see Fig. 1(b)). To investigate further the film structure, X-ray diffraction (XRD) measurements (see Fig. 1(c)) were performed on NFPI7 films deposited on ZnO/PEIE coated
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