Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 4, Pages 5368-5378Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c17655
Keywords
hybrid organic-inorganic lead halide perovskites; perovskite light-emitting electrochemical cells; nanoimprint lithography; grain growth mechanism; crystallographic orientations; crystallinity; morphology; surface energy
Funding
- Welch Foundation [AT-1992-20190330, AT-1617]
- National Science Foundation (NSF) CAREER Award [ECCS-1941629]
- University of Texas at Dallas Office of Research through the SPIRe Grant Program
- Nano Materials Technology Development Program [2016M3A7B4909942]
- Louis Beecherl, Jr. endowment fund
- National Research Foundation (NRF) of Korea by Creative Materials Discovery Program [2015M3D1A1068062]
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The study revealed that surface energy-driven preferential grain growth during NIL is the key factor in enhancing the material properties of perovskites. An optimized NIL process was developed and successfully applied in a PeLEC architecture, resulting in a fourfold enhancement in maximum current efficiency and twofold enhancement in luminance compared to a PeLEC without NIL.
Hybrid organic-inorganic lead halide perovskites have attracted much attention in the field of optoelectronic devices because of their desirable properties such as high crystallinity, smooth morphology, and well-oriented grains. Recently, it was shown that thermal nanoimprint lithography (NIL) is an effective method not only to directly pattern but also to improve the morphology, crystallinity, and crystallographic orientations of annealed perovskite films. However, the underlining mechanisms behind the positive effects of NIL on perovskite material properties have not been understood. In this work, we study the kinetics of perovskite grain growth with surface energy calculations by first-principles density functional theory (DFT) and reveal that the surface energy-driven preferential grain growth during NIL, which involves multiplex processes of restricted grain growth in the surface-normal direction, abnormal grain growth, crystallographic reorientation, and grain boundary migration, is the enabler of the material quality enhancement. Moreover, we develop an optimized NIL process and prove its effectiveness by employing it in a perovskite light-emitting electrochemical cell (PeLEC) architecture, in which we observe a fourfold enhancement of maximum current efficiency and twofold enhancement of luminance compared to a PeLEC without NIL, reaching a maximum current efficiency of 0.07598 cd/A at 3.5 V and luminance of 1084 cd/m(2) at 4 V.
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