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Metal Halide Perovskite Light Emitters SPECIAL FEATURE: PERSPECTIVE Young-Hoon Kima,B,1, Himchan Choa,B,1, and Tae-Woo Leea,B,2

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Metal Halide Perovskite Light Emitters SPECIAL FEATURE: PERSPECTIVE Young-Hoon Kima,B,1, Himchan Choa,B,1, and Tae-Woo Leea,B,2 SPECIAL FEATURE: PERSPECTIVE Metal halide perovskite light emitters SPECIAL FEATURE: PERSPECTIVE Young-Hoon Kima,b,1, Himchan Choa,b,1, and Tae-Woo Leea,b,2 Edited by John A. Rogers, University of Illinois, Urbana, IL, and approved August 16, 2016 (received for review May 10, 2016) Twenty years after layer-type metal halide perovskites were successfully developed, 3D metal halide perovskites (shortly, perovskites) were recently rediscovered and are attracting multidisciplinary interest from physicists, chemists, and material engineers. Perovskites have a crystal structure composed of five atoms per unit cell (ABX3) with cation A positioned at a corner, metal cation B at the center, and halide anion X at the center of six planes and unique optoelectronic properties determined by the crystal structure. Because of very narrow spectra (full width at half-maximum ≤20 nm), which are insensitive to the crystallite/grain/particle dimension and wide wavelength range (400 nm ≤ λ ≤ 780 nm), perovskites are expected to be promising high-color purity light emitters that overcome inherent problems of conventional organic and inorganic quantum dot emitters. Within the last 2 y, perovskites have already demonstrated their great potential in light-emitting diodes by showing high electroluminescence efficiency comparable to those of organic and quantum dot light-emitting diodes. This article reviews the progress of perovskite emitters in two directions of bulk perovskite polycrystalline films and perovskite nanoparticles, describes current challenges, and suggests future research directions for researchers to encourage them to collabo- rate and to make a synergetic effect in this rapidly emerging multidisciplinary field. organic–inorganic hybrid perovskite | light-emitting diodes | polycrystalline film | nanoparticle | vivid display As human civilization went through the information They were expected to be novel hybrid materials that revolution, display technology has been designated as a had both advantages of organic materials (e.g., solu- core technology to increase convenience in daily human tion processability and low material costs) and inor- life. In an information society, the desire of humans to see ganic materials (e.g., high charge carrier mobility) (7). the materials more vividly in displays has significantly Especially, perovskites with high color purity, easy increased. In this aspect, major trend of the display wavelength tuning, and efficient charge injection/ technology is changing from high resolution and high transport property have been intensively studied as efficiency to high color purity for realizing vivid natural promising candidates for future light emitters (8–10). colors (Fig. 1). Therefore, research on new emitting mate- Furthermore, stable and environmentally benign perov- rials that can emit light with narrow full width at half- skites, which were recently reported, further raise the maximum (FWHM) have been attempted. Inorganic possibility of perovskites as future emitters in display quantum dot (QD) emitters with narrow spectra (FWHM technology (11–19). ∼30 nm) have been significantly studied following organic However, early works on layer-type (i.e., 2D) perovskite emitters (FWHM >40 nm); however, size-sensitive color emitters, in the 1990s, did not gain much attention (1–5). purity, difficult size uniformity control, and expensive ma- The layer-type perovskite emitters incorporating long- terial costs of inorganic QD emitters retard the progress chain organic ammoniums can generate stable excitons for wide use in industry. Therefore, new emitters with at low temperature, but the photoluminescence (PL) in- size-insensitively high color purity (FWHM <20 nm) tensity dramatically decreased as temperature increased, and low material cost should be developed. Among so the perovskite light-emitting diodes (PeLEDs) exhibited many candidates, metal halide perovskites (hereafter, electroluminescence (EL) only at low temperature “perovskites”) have gained great attentions and shown (<110 K) (1–5). The PeLEDs that exhibited EL at room the possibility for future high-color purity emitters. temperature (RT) were first fabricated in 1999 using a layer- The first perovskites were layer-type thin films (A2MX4) type perovskite incorporating an organic dye molecule (A = organic cation; M = divalent metal; X = Cl, Br, I) (1–6). (H2NC2H4C16H8S4–C2H4NH2) and exhibited a maximum aDepartment of Materials Science and Engineering, Pohang University of Science and Technology, Pohang, Gyungbuk 790-784, Republic of Korea; and bDepartment of Materials Science and Engineering, Seoul National University, Gwanak-gu, Seoul 08826, Republic of Korea Author contributions: Y.-H.K., H.C., and T.-W.L. wrote the paper. The authors declare no conflict of interest. This article is a PNAS Direct Submission. 1Y.-H.K. and H.C. contributed equally to this work. 2To whom correspondence should be addressed. Email: [email protected]. www.pnas.org/cgi/doi/10.1073/pnas.1607471113 PNAS Early Edition | 1of9 Downloaded by guest on September 28, 2021 Fig. 1. Major trend of display technology. Data are taken from references as follows: OLEDs, refs. 30–41; QD LEDs, refs. 20–29;andPeLEDs,refs.8–10. external quantum efficiency (EQEmax) of 0.11% (7). However, this emis- relatively narrow (FWHM ∼30 nm) but size-sensitive spectra in lim- sion originated not from the inorganic frameworks but from the or- ited dimension (≤10 nm) (Fig. 2C). ganic dye ligands; thus, PeLEDs showed very low color purity The polar lead–halide bonds in perovskite crystal induce the (FWHM ≥ 100 nm) compared with inorganic QD LEDs (20–29), Fröhlich interaction between charge carriers and longitudinal and inferior EL efficiency compared with organic LEDs (OLEDs) optical (LO) phonons, which results in LO phonon scattering and (30–41). As a result, the development of these perovskite emitters has electron–phonon coupling; these predominantly determine the been retarded, whereas organic emitters and inorganic QD emitters linewidth of emission spectrum (FWHM ∼20 nm) (44). Further- have been intensively studied for 27 y and 22 y, respectively (20–41). more, the traps and impurities in perovskites, which can arise from In 2012, the first 3D perovskite emitters, CH3NH3PbBr3 nano- the low crystallinity, do not make a significant effect on the FWHM particles (NPs) in porous alumina (42), were reported, and the pos- because trap-assisted recombination is mostly nonradiative decay sibility of perovskites as emitters was rediscovered. As a result, since and impurity-contributed linewidth broadening is negligible, re- 2014, the research on 3D perovskite emitters has intensively grown spectively (44, 45). Thus, perovskites showed the size-insensitive and focused on achieving high efficiency in PL and EL. Within the FWHM, which is only affected by the crystal structure rather than last 2 y, more than 72 papers on perovskite emitters were published, quality and dimension of perovskite crystal. and EQEmax of 8.53% and photoluminescence quantum efficiency In general, photoexcitation or charge carrier injection by external (PLQE) of more than 90% were reported (10, 43). field forms geminate electron–hole pairs, which can (i)bedissoci- In this Perspective, we highlight the potential of perovskites as ated into free charge carriers or (ii) form excitons (46, 47). The Eb promising emitters that can be mainstream in the research field of reflecting the strength with which geminate electron–hole pairs are displays and solid-state lightings. In addition, we present our bound and the excitation density affecting the frequency with which perspectives on the progress of perovskite emitters in two direc- tions: bulk perovskite polycrystalline films (PePCs) and perovskite nanoparticles (PeNPs). Finally, we suggest future research directions of perovskite emitters that may engage a researcher’s attention in this research field. Fundamental Properties of Perovskite Emitters Three-dimensional perovskites have an ABX3 crystal structure com- posed of five atoms per unit cell, with cation A positioned at a corner, metal cation B at the center, and six nearest-neighbor anions X with octahedral corner sharing at the center of six planes (Fig. 2A). +1 + Generally, perovskites consist of organic ammonium (CnH2n NH3 ) + or organic amidinium [e.g., CH(NH2) ]oralkalimetalssuchasCsat + + + + the A site, divalent transition metals (e.g., Pb2 ,Eu2 ,Sn2 ,Cu2 )at − − − the B site, and halide anions (I ,Br ,Cl ) at the X site. Perovskite emitters show size-insensitively very narrow spectra (FWHM ∼20 nm) in wide wavelength range (400 nm ≤ λ ≤ 780 nm) according to their inherent crystal structure (Fig. 2B). Therefore, they can have a very wide color gamut in Commission Inter- nationale de l’Eclairage´ diagram. This highlights that perovskites can be promising emitters especially in display fields. On the other Fig. 2. (A) Schematic of crystal structure, (B) schematic of emission ≥ hand, organic emitters showed broad spectra (FWHM 40 nm) of metal halide perovskites, and (C) FWHM and dimension of in large dimension (≥10 nm) and inorganic QD emitters showed perovskite, inorganic QD, and organic emitters. 2of9 | www.pnas.org/cgi/doi/10.1073/pnas.1607471113 Kim et al. Downloaded by guest on September 28, 2021 −2 electrons and holes meet together determine the ratio of free car- (EQEmax = 0.125% and Lmax = 417 cd·m ) by using modified riers and excitons (nfc/ne-h, where nfc is the number of free carriers interlayers (9). These works demonstrated
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