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Emergence of Impurity-Doped Nanocrystal Light-Emitting Diodes

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Emergence of Impurity-Doped Nanocrystal Light-Emitting Diodes nanomaterials Review Emergence of Impurity-Doped Nanocrystal Light-Emitting Diodes Dongxiang Luo 1, Lin Wang 2, Ying Qiu 3,*, Runda Huang 4 and Baiquan Liu 5,* 1 Institute of Semiconductors, South China Normal University, Guangzhou 510631, China; [email protected] 2 Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore; [email protected] 3 Guangdong R&D Center for Technological Economy, Guangzhou 510000, China 4 School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China; [email protected] 5 State Key Laboratory of Optoelectronic Materials and Technologies and the Guangdong Province Key Laboratory of Display Material and Technology, School of Electronics and Information Technology, Sun Yat-sen University, Guangzhou 510275, China * Correspondence: [email protected] (Y.Q.); [email protected] (B.L.) Received: 26 May 2020; Accepted: 17 June 2020; Published: 24 June 2020 Abstract: In recent years, impurity-doped nanocrystal light-emitting diodes (LEDs) have aroused both academic and industrial interest since they are highly promising to satisfy the increasing demand of display, lighting, and signaling technologies. Compared with undoped counterparts, impurity-doped nanocrystal LEDs have been demonstrated to possess many extraordinary characteristics including enhanced efficiency, increased luminance, reduced voltage, and prolonged stability. In this review, recent state-of-the-art concepts to achieve high-performance impurity-doped nanocrystal LEDs are summarized. Firstly, the fundamental concepts of impurity-doped nanocrystal LEDs are presented. Then, the strategies to enhance the performance of impurity-doped nanocrystal LEDs via both material design and device engineering are introduced. In particular, the emergence of three types of impurity-doped nanocrystal LEDs is comprehensively highlighted, namely impurity-doped colloidal quantum dot LEDs, impurity-doped perovskite LEDs, and impurity-doped colloidal quantum well LEDs. At last, the challenges and the opportunities to further improve the performance of impurity-doped nanocrystal LEDs are described. Keywords: light-emitting diode; impurity doping; quantum dot; perovskite; quantum well 1. Introduction Nanocrystal light-emitting diodes (LEDs) have huge potential in display, lighting, and signaling applications because of their exceptional advantages including high efficiency, excellent luminance, low voltage, impressive power consumption, and long lifetime [1–5]. In 1994, Alivisatos et al. reported the first nanocrystal LED by using CdSe colloidal quantum dots (CQDs), achieving a maximum external quantum efficiency (EQE) of 0.01% [6]. Since then, plenty of endeavors have been taken to enhance the performance (e.g., EQE, current efficiency (CE), power efficiency (PE), voltage, luminance, and stability) of CQD-LEDs [7–11]. Nowadays, the performance of CQD-LEDs can be comparable to or even better than that of state-of-the-art organic LEDs (OLEDs) [12–16]. For example, the maximum EQE of CQD-LEDs exceeds 20% [1], while the maximum luminance of 2 CQD-LEDs overtakes 614,000 cd m− [17]. As a comparison, the maximum EQE of OLEDs is above 2 36% [13], but the maximum luminance of OLEDs is usually below 200,000 cd m− [15]. Benefiting from the understanding of CQD-LEDs, researchers have also explored other types of nanocrystal LEDs. As a representative class of optoelectronic materials, both organic-inorganic hybrid and all-inorganic Nanomaterials 2020, 10, 1226; doi:10.3390/nano10061226 www.mdpi.com/journal/nanomaterials Nanomaterials 2020, 10, 1226 2 of 40 perovskites have been intensively studied for LEDs in the recent years [18–23]. In 2014, Friend et al. realized the first successful organic-inorganic MAPbBr3 (MA= CH3NH3) perovskite LED (PeLED), yielding an EQE of 0.1% [18]. With the combined efforts from scientists worldwide, the performance of PeLEDs has been significantly enhanced [24]. So far, the maximum EQE of PeLEDs surpasses 2 20% [25–27], while the maximum luminance of PeLEDs surmounts 591,197 cd m− [28]. In addition, colloidal quantum wells (CQWs), also commonly nicknamed as semiconductor nanoplatelets, are considered to be another highly promising family of emitters for nanocrystal LEDs [29–33]. In 2014, Dubertret et al. developed the first CQW-LED by using CdSe/CdS core/shell heterostructures, obtaining a maximum EQE of 0.63% [34]. Over the past few years, the performance of CQW-LEDs has been improved step-by-step. Currently, the maximum EQE of CQW-LEDs is close to the theoretical limit of 20% [35]. These exciting facts demonstrate that the rapid development of nanocrystal LEDs will become real commercialization in the near future. Impurity doping is a broadly exploited strategy to endow nanocrystals exhibiting a multitude of novel electronic, optical, catalytic, transporting and magnetic properties [36–40]. By intentionally inserting atoms or ions of appropriate elements (e.g., transition metal, alkali metal, rare earth, and lanthanide impurities) into host lattices or nonstoichiometry-induced self-doping, various impurity-doped nanocrystals with desirable properties and functions can be achieved [41–45]. Since the self-quenching and reabsorption from enlarged Stokes shift can be eliminated, impurity-doped nanocrystals are much less sensitive than undoped ones to the chemical, thermal, and photochemical disturbances [46–50]. In particular, extra holes (p-type doping) or electrons (n-type doping) are provided with the utilization of impurities, enriching the electronic applications [51]. Doping levels and dopant positions are varied according to the synthesis schemes (e.g., reaction parameters, working temperatures, and doping agents), leading to the changed dopant luminescence and electronic impurities [52–55]. For instance, Norris et al. obtained p-type and n-type Ag doping through different doping levels by using the cation-exchange reaction between PbSe/CdSe and ethanolic Ag+ [56]. Klimov et al. incorporated Mn ions into CsPbX3 (X= Cl, Br, or I) perovskites through elucidating the function of bond strengths within the precursor and perovskite lattice, showing that the energy transfer between perovskites and Mn2+ played a key role in the intensity of band-edge and Mn emissions [57]. Eychmüller et al. observed that high-temperature synthesis methods (e.g., 240 ◦C) lead to a firm binding of Hg atoms within CQWs responsible for the single peak emission, while low-temperature means (e.g., 200 ◦C) caused both loosely (probably via interstitial incorporation) and firmly (substitutional) bound Hg atoms for double radiative recombination channels of lower and higher energies (i.e., two red PL signals) [58]. As a matter of fact, it has been demonstrated that impurities can afford CQDs, perovskites, and CQWs with new functionalities. Generally, impurity-doped nanocrystals can exhibit not only the intrinsic merits of nanocrystals but also additional advantages including enhanced thermal and chemical stability, improved photoluminescence quantum efficiency (PLQY), reduced Auger recombination, impurity-related emission, and tailored charge mobility [59–63]. Owing to these superiorities, impurity-doped nanocrystals have sparked efforts to satisfy the requirement of many optoelectronic applications. For example, Manoj et al. realized high-performance luminescent solar concentrators by using Cu-doped CQWs, whose quantum efficiency is near-unity (up to 97%) [64]. Huang et al. improved ≈ hole extraction through Ag doping (1% concentration) in PbS CQD solar cells, boosting the power conversion efficiency from 9.1% to 10.6% [65]. In the case of LEDs, impurity-doped nanocrystals have been extensively explored as versatile emitters. In general, impurity-doped nanocrystal LEDs can emit not only band-edge emissions but also impurity-related emissions [66–68]. As a consequence, three emission phenomena exist in impurity-doped nanocrystal LEDs (i.e., LEDs exhibit only host emissions, LEDs show only impurity emissions, and LEDs possess both host and dopant emissions). This is different from undoped nanocrystal LEDs, where only band-edge emissions can be observed [69–71]. Additionally, both the efficiency and luminance of impurity-doped nanocrystal LEDs can be enhanced compared with those of undoped counterparts. For example, nine times the EQE in CQW-LEDs [72] Nanomaterials 2020, 10, 1226 3 of 40 and ~10 times the luminance in PeLEDs [73] were accomplished via impurity doping. Furthermore, the stability of impurity-doped nanocrystal LEDs could be improved related to that of undoped ones [74]. Owing to the unique characteristics and impressive advantages (e.g., enhanced efficiency, improved luminance, lowered voltage, and increased stability), impurity-doped nanocrystal LEDs, especially for CQD-LEDs, PeLEDs and CQW-LEDs, are hugely promising for the new-generation display, lighting, and signaling technologies. Herein, the recent state-of-the-art concepts to achieve high-performance impurity-doped nanocrystal LEDs will be concluded. First, the fundamental concepts of impurity-doped nanocrystal LEDs will be presented. Second, the efforts to enhance the performance of impurity-doped nanocrystal LEDs via both material design and device engineering will be introduced. In particular, the emergence of various types of impurity-doped nanocrystal LEDs (e.g., CQD-LEDs, PeLEDs, and CQW-LEDs) will be comprehensively highlighted. Finally, the issues and ways to further improve the device performance
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