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Plasmonic perovskite light-emitting diodes based on Ag-CsPbBr3 system Xiaoli Zhang, Bing Xu, Weigao Wang, Sheng Liu, Yuanjin Zheng, Shuming Chen, Kai Wang, and Xiao Wei Sun ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.6b12450 • Publication Date (Web): 16 Jan 2017 Downloaded from http://pubs.acs.org on January 16, 2017

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ACS Applied Materials & Interfaces

Plasmonic perovskite light-emitting diodes based on Ag-CsPbBr3 system Xiaoli Zhang†,‡*, Bing Xu†,§, Weigao Wang†, Sheng Liu§, Yuanjin Zheng‡, Shuming Chen†,*, Kai Wang†, Xiao Wei Sun†,* †

Department of Electrical & Electronic Engineering, Southern University of Science and

Technology, Shenzhen, 518055, China ‡

School of Electrical & Electronic Engineering, Nanyang Technological University, 50 Nanyang

Avenue, 639798, Singapore §

School of Power and Mechanical Engineering, Wuhan University, Wuhan, 430072, China

ABSTRACT: The enhanced luminescence through semiconductor-metal interactions suggests the great potential of device performance improvement via properly tailored plasmonic nanostructures. Surface plasmon enhanced electroluminescence in all-inorganic CsPbBr3 perovskite light-emitting diode (LED) is fabricated by decorating the hole transport layer with the synthesized Ag nanorods. An increase of 42% and 43.3% in the luminance and efficiency are demonstrated for devices incorporated with Ag nanorods. The device with Ag introduction indicates identical optoelectronic properties to the controlled device without Ag nanostructures. The increased spontaneous emission rate caused by the Ag-induced plasmonic near-field effect is responsible to the performance enhancement. Therefore, plasmonic Ag-CsPbBr3 nanostructure studied here provides a novel strategy on the road to the future development of perovskite LEDs.

KEYWORDS: all-inorganic, perovskite, light-emitting diode, plasmonic, silver nanostructures

ACS Paragon Plus Environment


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Introduction The recent hot research on metal halide perovskite has demonstrated tremendous advances in photovoltaics by showing a significant enhancement of power conversion efficiency above 20%.1-5 As a new class of optoelectronic semiconductor, the perovskite has also been widely used in LED, lasing, photodetectors, x-ray diffraction detection and plasmonics.6-9 Specially, the organic-inorganic hybrid perovskite CH3NH3PbBr3 thin film applied in LED has been reported to exhibit record activity, such as a current efficiency (CE) as high as 42.9 cd A-1 and an external quantum efficiency (EQE) of 8.53%.10 However, organic cation CH3NH3 or HC(NH2)2 based perovskites are often criticized for their inherent instability, such as high sensitivity to the oxygen and moisture.11 In contrast, the recent success on the alternative inorganic Cs cation based perovskite has witnessed its outstanding stability and excellent photoelectric properties,1214

whereas the inferior performance in LEDs represents a fundamental challenge for this material

system. The reported CsPbBr3 nanocrystals (NCs) LED exhibited luminance of 946~2335 cd m-2 and current efficiency (CE) of 0.19~0.43 cd A-1,15-16 while the CsPbBr3 thin film perovskite LEDs was rarely reported and exhibited inferior performance.17 Therefore, it is highly eager to find an effective method to achieve the desired perovskite CsPbBr3 LED with efficient performance. The all-inorganic perovskite CsPbBr3 NCs behave like quantum dots (QDs), which present high efficiency quantum yield, tunable bandgap, and narrow-band emission.18-19 Therefore, the extensive research on QDs LED with superior performance could afford effective reference and guidance for perovskite LEDs. Metallic nanostructures induced localized surface plasmon (SP) effect is an attractive and effective approach for light emission enhancement in QDs LED. The noble metal nanostructures enhanced photoluminescence (PL) and


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electroluminescence (EL) have been widely achieved in the past few years,20-29 indicating the great potential of enhancing the LEDs performance through properly tailored plasmonic nanostructures in perovskite NCs. Surface plasmon resonance (SPR) is the strong interaction between plasmonic metallic nanostructures and resonant photons, through which photon-induced collective oscillations can be achieved among free electrons. SPR could facilitate the effective energy transfer, improving LEDs performance through enhanced radiative recombination rate. The necessary prerequisite to promote the coupling effect between excitons and SP is overlapping their local electromagnetic field, which is related to the nature of selected metallic nanostructures.30-34 Therefore, it is crucial to effectively manipulate the morphology of plasmonic nanoparticles to realize SPR maximization. Here, we report the first account of plamonic perovskite CsPbBr3 NCs on the strength of Ag nanostructures. In detail, we fabricated Ag nanorods, and the maximum SPR induced between Ag nanorods and CsPbBr3 NCs has been achieved. The resulting plasmonic perovskite LEDs exhibit the improved luminance and efficiency, which is increased up to 42% and 43.3%, respectively, with compare to the controlled LEDs without Ag-rod. Therefore, plasmonic perovskite LEDs has great potential for the improved performance through perovskite-metal nanostructure interactions. Results and discussion The as-prepared all-inorganic CsPbBr3 NCs are monodispersed with cubic shape of 10 nm, as investigated by the transmission electronic microscopy (TEM) in Figure 1. The Ag nanostructures were prepared through the standard sodium citrate reduction method as reported previously.35 The synthesis procedure of Ag nanoparticles is based on the silver salt precursor



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Figure 1. (a) TEM images of CsPbBr3 nanocrystals. (b) Photographs of Ag nanorods and CsPbBr3 NCs. (c) TEM image of Ag nanorods and (d) the corresponding SEM images of Ag nanorods dispersed on PEDOT:PSS this film. and NaBH4 as a reducing agent. By adjusting the concentration of reduction agent and additives in the precursor, we can get Ag nanostructures with different shapes. As displayed in Figure 1b, the argent colloid implies the resultant Ag nanorods. For comparison, under the fixed process procedure with little revision, the resulting yellow and bule colloid are obtained, indicating a dramatic shape evolution into spherical Ag nanoparticles and triangle Ag nanoprisms, respectively (see supporting information Figure S1 and S2). The as-prepared Ag nanostructures are denoted as Ag-sphere, Ag-triangle and Ag-rod, respectively. The solution-processed Ag nanostructures with the same concentration were subjected to spin-coating on the surface of poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT:PSS) thin film, followed by the evaporation of N,N’-bis(1-naphtalenyl)-N-N’-bis(phenylbenzidine) (NPB) of about 9 nm (± 1 nm) as barrier layer covered on its surface. From Figure 1d, we can see that Ag nanorods are uniformly dispersed on the surface of PEDOT:PSS layer.


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Figure 2. (a) Absorption spectra of different Ag nanorods. (b) Absorption and PL plots of CsPbBr3 nanocrystals. (c) Absorption spectrum of the Ag-rod and PL spectrum of the CsPbBr3 nanocrystals. (d) TEM image of cross section of device and corresponding schematic diagram of device structure. The optical response of CsPbBr3 NCs to the as-obtained Ag nanostructures is studied, which is prerequisite condition for the maximum SPR. As the morphology of Ag nanostructures are evolved from sphere to triangle and rod, the absorption peak redshifts from 413 to 526 nm with widened full width at half maximum (FWHM) (see Figure S2). Optical properties of CsPbBr3 NCs are shown in Figure 2b. The perovskite CsPbBr3 NC displays a typical absorption band edge of 518 nm and PL emission of 527 nm. It has been found that the absorption peak of Ag-rod well match the PL emission peak of the CsPbBr3 NCs, as indicated in Figure 2c. The overlap of two spectra indicates the possible resonance between radiated light generated in perovskite and localized SPs excited by Ag-rod, which will result in an effective energy transfer



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and therefore the enhanced emission intensity. Therefore, plasmonic enhanced perovskite LEDs is expected to realize through a maximum coupling between emitting layer and the SP of Ag-rod. In contract, the referential Ag-sphere and Ag-triangle show mismatched optical properties for SPR. Therefore, herein, the plasmonic perovskite LEDs have been fabricated based on Ag-rod to investigate the capability of Ag-CsPbBr3 system for enhancing the device performance. The typical device configuration consists of spin-coated layers of Ag-rod on the surface of PEDOT:PSS layer, barrier layer NPB (N-N’-bis(1-naphtalenyl)-N-N’-bis(phenylbenzidine)), provskite CsPbBr3 NCs, and evaporated layers of 1,3,5-Tris(1-phenyl-1H-benzimidazol-2yl)benzene (TPBi) and LiF/Al, as shown in the schematic diagram in Figure 2d. To avoid the fluorescence quenching, the NPB thin film here is employed as a dielectric spacer placing between CsPbBr3 NCs and Ag-rod. The distance between emitting layer and metal cathode Al in LED is large enough to avoid the influence of SP losses. In this study, the TPBi thickness of 40 nm is used, which almost totally drops off the SP disturbance caused by Al electrode.


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Figure 3. (a) Luminance and current density of the devices as a function of the driving voltage. (b) EL spectra of plasmonic and reference perovskite LEDs. The inset is the photographic image of plasmonic perovskite LED driven at voltage of 4 V. (c) CE and (d) EQE for the devices with and without Ag-rod. Figure 3 displays the EL characteristics of the perovskite LEDs with and without Ag-rod. The plasmonic perovskite LED with Ag-rod exhibits a higher luminance (8911 cd m-2), about 42 % enhancement, in comparison with the controlled device without Ag-rod (6274 cd m-2) (Figure 3a). A significant EL enhancement is detected in the resulting plamonic device, which is attributed to the excitons mode matching of SP with that of CsPbBr3 nanocrystals in the plasmonic perovskite LED. It is worth pointing out that the incorporation of Ag-rod in perovskite LED leads to negligible influence on EL spectra, revealing no connection of spectra and the introduced Ag-rod. A uniform and bright green emission of plasmonic LED driven at voltage of 4 V is displayed in the inset. With Ag-rod mixed in PEDOT:PSS layer, the efficiency of the plasmonic LED is dramatically improved, with a maximum CE (current efficiency) and EQE (external quantum efficiency) of 1.42 cd A-1 and 0.43%, respectively, 43.4% and 43.3% higher than that of the controlled device (0.99 cd A-1 and 0.30%). The similar turn-on voltage demonstrated that the electrical property of the corresponding devices remain almost identical. To illustrate the influence of Ag incorporation on electrical properties, hole-only device with and without Ag-rod was made, which indicates that that the presence of Ag-rod in HTL (hole transport layer) has no influence on the hole injection. As illustrated in the reported results,36,37 it is reasonable to infer that the EL enhancement as observed in Figure 3 is associated with the SP effect, as deduced from SP penetration depth of about 30-40 nm near TPBi and perovskite layer. The EL characteristics of perovskite LEDs with and without Ag-rod are summarized in Table S1.



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Figure 4. (a) FILM image of CsPbBr3 thin films with and without Ag-rod. The film without Agrod shows bright color while CsPbBr3 nanocrystals with Ag-rod displays dark color. (b) PL intensity of CsPbBr3 nanocrystals with and without Ag-rod. (c) The lifetime distribution of different samples. (d) PL lifetime of perovskite CsPbBr3 nanocrystals layer with and without Agrod. It has been reported that the decreased exciton lifetime in SP-enhanced structure is related to the faster coupling process between SPs and radiated light than spontaneous recombination.38,

39

The localized SPR effect induced by Ag-rod on the fluorescence from

CsPbBr3 NCs layer in LEDs is investigated by fluorescence-lifetime imaging microscopy (FLIM) and time-resolved PL spectroscopy. The measurement was conducted on the CsPbBr3 film spincoated on PEDOT:PSS layer with or without Ag-rod. Figure 4a plots the FILM images of different samples, which indicates the right image with Ag-rod is color dim compared to the reference sample, which is mainly due to the excitons coupling induced decrease of excited state


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lifetime of CsPbBr3 NCs. Meanwhile, the PL intensity for plamonic perovskite CsPbBr3 NCs is accordingly increased compared to that of reference sample, indicative of the effective excitation of excitons from CsPbBr3 NCs with Ag-rod. The main lifetime distribution regions in two different samples are shown in Figure 4c, from which we can see the decreased lifetime from 1.66 to 1.56 ns as Ag-rod is embedded in the system. The PL lifetime demonstrates the shortened lifetime from 1.62 to 1.50 ns in the presence of Ag-rod in the structure (Figure 4d). Therefore, the localized SPR on Ag-rod is responsible to the enhancement of spontaneous emission rate. In addition, the enhanced EL can be ascribed to extracted SP energy in the form of light in view of the improved electromagnetic field intensity and the scattered SPs. Conclusion In summary, we have demonstrated the enhanced electroluminescence of perovskite CsPbBr3 LEDs with Ag nanorods, which exhibit an emission enhancement up to 42% compared to the reference device. The maximum EQE of 0.43% for the plasmonic perovskite LEDs has been achieved, about 43.3% increase than that of the controlled device without Ag-rod. The enhanced radiative decay rate is ascribed to the enhanced plasmonic perovskite CsPbBr3 LED. Supporting Information The Supporting Information is available free of charge on the ACS Publications websites. TEM images and optical properties of Ag nanostructures; The summary of device performance; Hole only device with and without Ag-rod. Corresponding Authors *

E-mail: [email protected], [email protected], [email protected]



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Notes Authors Xiaoli Zhang and Bing Xu are contributed equally to this work. The authors declare no competing financial interest. Acknowledgements This research is supported by the National Research Foundation, Prime Minister’s Office, Singapore under its Competitive Research Programme (NRF-CRP11-2012-01) and administered by Nanyang Technological University. This work is also supported by National Science and Technology Major Project of the Ministry of Science and Technology of China (No. 2016YFB0401702), National Natural Science Foundation of China (No. 51402148), Shenzhen Innovation

Project

(No.

JCYJ20160301113356947,

KC2014JSQN0011A

and

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