A solvent-based surface cleaning and passivation technique for suppressing ionic defects in high-mobility perovskite field-effect transistors

Abstract

Organometal halide perovskite semiconductors could potentially be used to create field-effect transistors (FETs) with high carrier mobilities. However, the performance of these transistors is currently limited by the migration of ionic surface defects. Here, we show that a surface cleaning and passivation technique, which is based on a sequence of three solution-based steps, can reduce the concentration of ionic surface defects in halide-based perovskites without perturbing the crystal lattice. The approach consists of an initial cleaning step using a polar/nonpolar solvent, a healing step to remove surface organic halide vacancies and a second cleaning step. The surface treatment is shown to restore clean, near hysteresis-free transistor operation, even if the perovskite films are formed under non-optimized conditions, and can improve room-temperature FET mobility by two to three orders of magnitude compared to untreated films. Our methylammonium lead iodide (MAPbI3) FETs exhibit high n- and p-type mobilities of 3.0 cm2 V−1 s−1 and 1.8 cm2 V−1 s−1, respectively, at 300 K, and higher values (9.2 cm2 V−1 s−1; n-type) at 80 K. We also show that the approach can be used to transform PbI2 single crystals into high-quality, two-dimensional perovskite single crystals.

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Fig. 1: Design of the cleaning–healing–cleaning surface passivation process.
Fig. 2: SKPM characterization of ion migration.
Fig. 3: Film microstructure before and after surface passivation.
Fig. 4: Performance of perovskite FETs prepared with C–H–C surface treatment.
Fig. 5: Transformation of PbI2 into MAPbI3 micro-platelet single crystals.

Data availability

The data supporting this paper are available at https://www.data.cam.ac.uk/repository.

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Acknowledgements

X.-J.S. thanks the Cambridge Trust and China Scholarship Council for financial support. H.S. thanks the Engineering and Physical Sciences Research Council (EPSRC) for support through a programme grant (EP/M005143/1). L.C. and B.Z. were also supported by the EPSRC grant. We thank R. Chakalov and R. Beadle for technical support. X.-J.S. is grateful to R.D. Pietro for discussions on early-stage SKPM measurements, to N. Berdunov for resolving experimental problems with the SKPM set-up and to D. Venkateshvaran for LabVIEW programming discussions. J.F.O. acknowledges the EPSRC Nano Doctoral Training Centre (EP/L015978/1) for support.

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X.-J.S. conceived the idea, designed the measurements, conducted and led the majority of the research experiments. X.-J.S. and C.C. fabricated the SKPM samples and FET devices, with B.Z., W.X. and J.P. contributing to the optimization of perovskite fabrications and J.W. contributing to the investigations on electrode selection. Y.L. performed the atomic layer deposition growth. X.-J.S. performed the SKPM and FET studies with assistance from C.C. B.Z. and X.-J.S. performed the XRD investigations. J.F.O., L.C. and X.-J.S. performed SEM studies with discussions from G.D. about the measurements. A.S. performed the PDS characterizations. S.W. contributed to the electrostatic potential simulations. X.-J.S. interpreted the results and established the model. H.S. directed and supervised the project. H.S. and X.-J.S. wrote the manuscript. All authors discussed the results and revised the manuscript.

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Correspondence to Henning Sirringhaus.

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Supplementary Figs. 1–31 and Discussion sections 1–17.

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She, XJ., Chen, C., Divitini, G. et al. A solvent-based surface cleaning and passivation technique for suppressing ionic defects in high-mobility perovskite field-effect transistors. Nat Electron 3, 694–703 (2020). https://doi.org/10.1038/s41928-020-00486-5

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