J. Semicond. > 2022, Volume 43 > Issue 9 > 090201

RESEARCH HIGHLIGHTS

Perovskite nanocrystals for light-emitting diodes

Xinyi Mei1, Lixiu Zhang2, Xiaoliang Zhang1, and Liming Ding2,

+ Author Affiliations

 Corresponding author: Xiaoliang Zhang, xiaoliang.zhang@buaa.edu.cn; Liming Ding, ding@nanoctr.cn

DOI: 10.1088/1674-4926/43/9/090201

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With superior photoluminescence quantum yields (PLQYs), tunable bandgap, high color purity and solution processibility[1, 2], metal halide perovskite nanocrystals (PNCs) with a general formula of ABX3 (A = CH3NH3+ (MA+), CH(NH2)2+ (FA+) and Cs+, B = Pb2+, Sn2+ and Mn2+, X = Cl–, Br– and I–) emerge as promising luminescent materials in light-emitting diodes (LEDs) and solid-state lighting[2-4]. Since electroluminescence (EL) of PNCs was first observed in CsPbBr3 PNC-based LEDs with an external quantum efficiency (EQE) of 0.07% in 2015[5], the efficiencies for different LEDs have been significantly boosted. The red and green LEDs demonstrated an EQE of >23% and the highest EQE for blue LEDs reached 13.8%[6-8], comparable to conventional LEDs based on organic emitters or metal chalcogenide (II–VI) quantum dots (QDs)[9, 10].

Compared to traditional emitters, the ionic bonding and relatively low formation energy of perovskite lattice enabled the facile formation of PNCs through liquid-phase synthesis[11, 12] (e.g. hot-injection (Fig. 1(a))[1], ligand-assisted reprecipitation[13] and ultrasonic-assisted synthesis[14]). Thanks to the great efforts in regulating the types and ratios of precursors, modifying the reaction temperature and adjusting the solvents and anti-solvents, near-unity PLQYs have been demonstrated for as-synthesized PNCs[15-17]. However, the luminescence properties for fresh PNCs would always be impaired during the subsequent purification, assembly process and storage in ambient conditions. The highly dynamic binding between the capping ligands and PNC surface induced the surface ligand desorption and subsequent generation of surface defects[18, 19]. In particular, the facilely formed halide ion (X–) vacancies and uncoordinated Pb2+ ions on PNC surface would yield carrier trapping centers and also provide sites for the invasion of external water and oxygen[20, 21], seriously deteriorating the performance of PNCs[22-25]. Chiba et al. utilized ammonium iodine salts, oleylammonium iodide (OAM-I) and aniline hydroiodide (An-HI), for post-treatment of CsPbBr3 PNCs to fill in the surface Br– vacancies and red-shift their PL emission (Fig. 1(a)), leading to pure red PNC-LEDs with an EQE of 21.3%[26]. Similarly, didodecyldimethylammonium fluoride (DDAF) endowed CsPbBr3 PNCs with well-passivated surface and improved resistance to thermal quenching of PL[27]. As a result, the LEDs presented an EQE of 19.3% with a low efficiency roll-off and enhanced thermal stability. Dong et al. proposed an ordinal surface-passivating strategy involving short-chain isopropylammonium bromide (IPABr) and NaBr to coat CsPbBr3 PNCs with a relatively stable bipolar shell, while also enhancing inter-dot charge coupling due to adequate removal of insulating OA and OAm ligands[28]. This strategy yielded blue and green CsPbBr3 PNC-LEDs with EQEs of 12.3% and 22%, respectively, as well as improved operational stability. Zheng et al. used n-dodecylammonium thiocyanate (DAT) to eliminate the surface defects of mix-halide PNCs without affecting their PL spectra, yielding pure blue PNC-LEDs with an EQE of 6.3% and stabilized EL spectra[29].

Fig. 1.  (Color online) (a) Surface-treating and anion-exchange process of CsPbBr3 PNCs by using OAm-I or An-HI. Reproduced with permission[26], Copyright 2018, Nature Publishing Group. (b) Schematic for PNC-LED with bilateral passivation and the corresponding sectional TEM image. Reproduced with permission[31], Copyright 2020, Nature Publishing Group. (c) Treating PNCs with glutathione and EDTA to remove excess surface Pb2+. Reproduced with permission[34], Copyright 2021, Nature Publishing Group.
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Lewis bases containing carbonyl (C=O), carboxylate (–COO–), phosphate (P=O) or sulfonate (–SO3–) groups can also passivate uncoordinated surface Pb2+ and suppress nonradiative recombination in PNCs[30-33]. Zeng et al. employed phosphine oxide molecules to passivate both top and bottom surfaces of CsPbBr3 PNC film to suppress trap-assisted nonradiative recombination (Fig. 1(b)). The LEDs gave an EQE of 18.7% and a prolonged half-life of 15.8 h[31]. Zhao et al. used 2-naphthalenesulfonic acid (NSA) to passivate the uncoordinated surface Pb2+ in FAPbBr3 PNCs, and the green LEDs offered a luminance of 67115 cd/m2 and an EQE of 19.2%[32]. The removal of redundant Pb2+ from PNC surface is an effective strategy to keep the high efficiency. Hassan et al. reported that ethylenediaminetetraacetic acid (EDTA) and the reduced L-glutathione could eliminate excess surface Pb2+ in MAPb(Br/I)3 PNCs due to their strong interaction with Pb2+ (Fig. 1(c))[34]. The PNCs with flattened surfaces presented boosted PLQY and suppressed phase separation, yielding an EQE of >20% for the LEDs with a stable EL peak at 620 nm. Bi et al. utilized hydrogen bromide (HBr) to facilitate the desorption of OA ligands and induce the removal of imperfect [PbBr6]4− octahedra from CsPbBr3 PNC surface. By using didodecylamine (DDDAM) and phenethylamine (PEA) passivating ligands, the damaged PNC surface was recovered with reduced trap density, yielding a pure-blue LED with enhanced stability and a luminance of 3850 cd/m2[35].

In addition to surface engineering, composition adjustment of PNCs is also a feasible strategy. Kim et al. introduced guanidinium cations (GA+) to occupy A sites in FAPbBr3 PNCs (Fig. 2(a)), which can well passivate surface-exposed Pb2+ due to extra amino groups and the well distributed positive charges on GA+[9]. Because of high PLQY (93.3%) and structural stability of GA+-doped FAPbBr3 PNCs, the LEDs offered an EQE of 23.4% (Fig. 2(b)) and a current efficiency of 108 cd/A. By contrast, doping cations on B-site modulates the energy band of PNCs (e.g. Mn2+, Cu2+, Sn2+ and Sr2+)[36-39]. Shen et al. converted CsPbI3 PNC from n-type semiconductor to nearly ambipolar semiconductor via doping Zn2+ (Fig. 2(c)), leading to more balanced carrier transport within LEDs[40]. The resulting red LEDs achieved brighter EL emission with a luminance of 2202 cd/m2 and an EQE of 15.1% (Fig. 2(d)). Besides, doping Mn2+ into perovskite lattice induced a second emission peak at ~600 nm, which resulted from the energy transfer from perovskite to Mn2+ (Fig. 2(e)). Doping Sr2+ in CsPbI3 PNCs caused new trap states near the conduction band edge but simultaneously generating an excitonic state at a lower energy level, which prevented the trap-assisted non-radiative recombination, yielding a PLQY of ~95%[39]. Such PNCs showed enhanced stability, due to the increased formation energy of cubic CsPbI3 after being doped with Sr2+. Based on Sr2+-doped CsPbI3 PNCs, Chen et al. realized efficient and stable red LEDs with an EQE of 17.1%[41].

Fig. 2.  (Color online) (a) Schematic for GA+-doped FAPbBr3 PNCs. (b) EQE–V curves for LEDs based on GA+-doped FAPbBr3 PNCs with different GA+ doping content. (a, b) Reproduced with permission[9], Copyright 2021, Nature Publishing Group. (c) Energy level diagram showing the change in the energy band of Zn2+-doped CsPbI3 PNCs. (d) J–V–L curves for LEDs based on CsPbI3 and Zn2+-doped CsPbI3 PNCs. Insets show the working LEDs. (c, d) Reproduced with permission[40], Copyright 2019, American Chemical Society. (e) Energy transfer in Mn2+-doped nanocrystal. Reproduced with permission[36], Copyright 2018, Elsevier.
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Several issues impede the application of PNC-LEDs. (1) Poor stability. More conductive capping matrix can facilitate charge injection into PNC emitters, e.g. 3D perovskite and metal of frame (MOF)[42, 43]. Besides, balanced charge transport favors to combat the efficiency roll-off and enhance device stability[44]. (2) Lead toxicity. Lead-free PNCs always present inferior luminescent properties, e.g. relatively low PLQY and wide emission spectra[45]. More studies on bandgap structure, surface properties and carrier dynamics of lead-free PNCs are needed. In addition, effective encapsulation of lead-halide PNCs may also be a solution.

This work was supported by the National Natural Science Foundation of China (51872014), the Recruitment Program for Global Experts, the Fundamental Research Funds for the Central Universities and the “111” project (B17002). L. Ding thanks the open research fund of Songshan Lake Materials Laboratory (2021SLABFK02), the National Key Research and Development Program of China (2017YFA0206600) and the National Natural Science Foundation of China (51922032, 21961160720).



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Fig. 1.  (Color online) (a) Surface-treating and anion-exchange process of CsPbBr3 PNCs by using OAm-I or An-HI. Reproduced with permission[26], Copyright 2018, Nature Publishing Group. (b) Schematic for PNC-LED with bilateral passivation and the corresponding sectional TEM image. Reproduced with permission[31], Copyright 2020, Nature Publishing Group. (c) Treating PNCs with glutathione and EDTA to remove excess surface Pb2+. Reproduced with permission[34], Copyright 2021, Nature Publishing Group.

DownLoad: Full-Size Img PowerPoint
Fig. 2.  (Color online) (a) Schematic for GA+-doped FAPbBr3 PNCs. (b) EQE–V curves for LEDs based on GA+-doped FAPbBr3 PNCs with different GA+ doping content. (a, b) Reproduced with permission[9], Copyright 2021, Nature Publishing Group. (c) Energy level diagram showing the change in the energy band of Zn2+-doped CsPbI3 PNCs. (d) J–V–L curves for LEDs based on CsPbI3 and Zn2+-doped CsPbI3 PNCs. Insets show the working LEDs. (c, d) Reproduced with permission[40], Copyright 2019, American Chemical Society. (e) Energy transfer in Mn2+-doped nanocrystal. Reproduced with permission[36], Copyright 2018, Elsevier.

DownLoad: Full-Size Img PowerPoint
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    Xinyi Mei, Lixiu Zhang, Xiaoliang Zhang, Liming Ding. Perovskite nanocrystals for light-emitting diodes[J]. Journal of Semiconductors, 2022, 43(9): 090201. doi: 10.1088/1674-4926/43/9/090201
    X Y Mei, L X Zhang, X L Zhang, L M Ding. Perovskite nanocrystals for light-emitting diodes[J]. J. Semicond, 2022, 43(9): 090201. doi: 10.1088/1674-4926/43/9/090201
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    Received: 12 June 2022 Revised: Online: Accepted Manuscript: 15 June 2022Uncorrected proof: 15 June 2022Published: 02 September 2022

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      Article Navigation >  Journal of Semiconductors  > 2022  >  43(9): 090201
      Xinyi Mei, Lixiu Zhang, Xiaoliang Zhang, Liming Ding. Perovskite nanocrystals for light-emitting diodes[J]. Journal of Semiconductors, 2022, 43(9): 090201. doi: 10.1088/1674-4926/43/9/090201 ****X Y Mei, L X Zhang, X L Zhang, L M Ding. Perovskite nanocrystals for light-emitting diodes[J]. J. Semicond, 2022, 43(9): 090201. doi: 10.1088/1674-4926/43/9/090201
      Citation:
      Xinyi Mei, Lixiu Zhang, Xiaoliang Zhang, Liming Ding. Perovskite nanocrystals for light-emitting diodes[J]. Journal of Semiconductors, 2022, 43(9): 090201. doi: 10.1088/1674-4926/43/9/090201 ****
      X Y Mei, L X Zhang, X L Zhang, L M Ding. Perovskite nanocrystals for light-emitting diodes[J]. J. Semicond, 2022, 43(9): 090201. doi: 10.1088/1674-4926/43/9/090201
      shu

      Perovskite nanocrystals for light-emitting diodes

      DOI: 10.1088/1674-4926/43/9/090201
      • 1.

        School of Materials Science and Engineering, Beihang University, Beijing 100191, China

      • 2.

        Center for Excellence in Nanoscience (CAS), Key Laboratory of Nanosystem and Hierarchical Fabrication (CAS), National Center for Nanoscience and Technology, Beijing 100190, China

      More Information
      • Xinyi Mei：got her BS from Central South University in 2019. She is now pursuing her PhD degree in Materials Physics and Chemistry at Beihang University under the supervision of Prof. Xiaoliang Zhang. Her research focuses on low-dimensional optoelectronic materials, such as quantum dots, and their application in light-emitting devices
      • Lixiu Zhang：got her BS from Soochow University in 2019. Now she is a PhD student at University of Chinese Academy of Sciences under the supervision of Prof. Liming Ding. Her research focuses on perovskite solar cells
      • Xiaoliang Zhang：is a professor at Beihang University. He received his PhD in Materials Physics and Chemistry from Beihang University in 2013. Then, he joined Uppsala University as a postdoc and subsequently was promoted as a Senior Researcher there. He joined Beihang University as a full professor in 2018. His research focuses on semiconducting quantum dots and their application in optoelectronic devices
      • Liming Ding：got his PhD from University of Science and Technology of China (was a joint student at Changchun Institute of Applied Chemistry, CAS). He started his research on OSCs and PLEDs in Olle Inganäs Lab in 1998. Later on, he worked at National Center for Polymer Research, Wright-Patterson Air Force Base and ArgonneNational Lab (USA). He joined Konarka as a Senior Scientist in 2008. In 2010, he joined National Center for Nanoscience and Technology as a full professor. His research focuses on innovative materials and devices. He is RSC Fellow, the nominator for Xplorer Prize, and the Associate Editor for Journal of Semiconductors
      • Corresponding author: xiaoliang.zhang@buaa.edu.cn; ding@nanoctr.cn
      • Received Date: 2022-06-12
        Available Online: 2022-06-15

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