Polarized light is crucial in numerous applications, including liquid crystal display (LCD) backlights
Opto-Electronic Advances, Volume. 7, Issue 3, 230210-1(2024)
Self-polarized RGB device realized by semipolar micro-LEDs and perovskite-in-polymer films for backlight applications
In backlighting systems for liquid crystal displays, conventional red, green, and blue (RGB) light sources that lack polarization properties can result in a significant optical loss of up to 50% when passing through a polarizer. To address this inefficiency and optimize energy utilization, this study presents a high-performance device designed for RGB polarized emissions. The device employs an array of semipolar blue μLEDs with inherent polarization capabilities, coupled with mechanically stretched films of green-emitting CsPbBr3 nanorods and red-emitting CsPbI3-Cs4PbI6 hybrid nanocrystals. The CsPbBr3 nanorods in the polymer film offer intrinsic polarization emission, while the aligned-wire structures formed by the stable CsPbI3-Cs4PbI6 hybrid nanocrystals contribute to substantial anisotropic emissions, due to their high dielectric constant. The resulting device achieved RGB polarization degrees of 0.26, 0.48, and 0.38, respectively, and exhibited a broad color gamut, reaching 137.2% of the NTSC standard and 102.5% of the Rec. 2020 standard. When compared to a device utilizing c-plane LEDs for excitation, the current approach increased the intensity of light transmitted through the polarizer by 73.6%. This novel fabrication approach for polarized devices containing RGB components holds considerable promise for advancing next-generation display technologies.
Introduction
Polarized light is crucial in numerous applications, including liquid crystal display (LCD) backlights
Light must be polarized in red, green, and blue (RGB) to be applied in applications such as backlights for LCDs and polarizer-tunable multiplexed color displays. Halide perovskite nanocrystals are promising color conversion materials due to their high photoluminescence quantum yield, high color purity, and controlled photovoltaic properties
Micro-LEDs (μLEDs) are anticipated to exhibit high dynamic range characteristics when employed in LCD backlights, owing to their capability for local dimming. These ultra-small pixels are also capable of achieving a more homogeneous light distribution compared to traditional LED backlights
This article introduces a high-performance, stable device designed for RGB polarized emission. The architecture of the device incorporates an array of blue semipolar μLEDs with intrinsic polarization emission that excite stretched composite films of green CsPbBr3 NRs and red CsPbI3-Cs4PbI6 hybrid nanocrystals (NCs), acting as the color-conversion layers (
Figure 1.
Results and discussion
Fabrication of CsPbBr3 NRs and CsPbI3-Cs4PbI6 hybrid NCs
CsPbBr3 NRs were synthesized under ambient conditions at room temperature (see Methods). The Cs precursor (Cs-oleate) was prepared by dissolving Cs2CO3 in an ODE solution containing oleic acid and heating it. Compared to other works, the proportion of oleic acid was increased to ensure that Cs-oleate remained completely soluble at room temperature. After synthesizing NWs, the formation of NRs during dilution can be explained by kinetic model
Morphology and optical properties of CsPbBr3 NRs
The resulting CsPbBr3 NRs emitted green luminescence under UV irradiation (
Figure 2.(
Polarized photoluminescence of CsPbBr3 NR stretched composite film
The green NR color-conversion layer was fabricated by mixing NRs with an EVA polymer and spin-coating the mixture onto a glass substrate to form a thin film (
Figure 3.(
The DOLP can be determined by calculating the difference between the intensities emitted in two orthogonal directions:
For the unstretched films, weakly polarized emission with a DOLP of approximately 0.12 was observed with unpolarized 405 nm light excitation. In contrast, the stretched composite film exhibited significantly polarized PL emission with a DOLP of approximately 0.44 (
For NRs with an anisotropic arrangement, PL polarization can be attributed to the depolarizing field generated by the dielectric confinement effect, which weakens the electric field perpendicular to the long axes of the NRs
where E// and E⊥ represent the parallel and perpendicular components of the external electric field, respectively; ε is the dielectric constant of nanomaterials; and ε0 is the dielectric constant of the polymer. The dielectric confinement of the electric field causes emission anisotropy and aligns the transition dipole moments along the long axis of the NRs, leading to anisotropic excitons contributing to the anisotropy of optical absorption
Morphology and optical properties of CsPbI3-Cs4PbI6 hybrid NCs
The susceptibility of CsPbI3 black polycrystals to environmental degradation poses a significant challenge for obtaining stable iodine-containing perovskite NRs
CsPbI3-Cs4PbI6 hybrid NCs displayed red-emission properties closely resembling those of unadulterated CsPbI3 NCs (
Figure 4.(
Similarly, CsPbI3-Cs4PbI6 composite films were fabricated based on EVA polymer. The stability of the CsPbI3 QDs was enhanced when they were embedded in Cs4PbI6. Moreover, to compare the stability of the CsPbI3-Cs4PbI6 hybrid NC film with that of pure γ-CsPbI3 QDs (corresponding TEM images are presented in
Polarized photoluminescence of hybrid NC stretched composite film
As CsPbI3 was embedded within Cs4PbI6 in the hybrid NCs, growing them into nanorods was challenging. The perovskite NCs in the composite film can be oriented into wires along the stretching direction, and this NC-aligned wire (NC-AW) structure also can exhibit polarized emission
Figure 5.(
The NC-AWs in this study mainly consisted of CsPbI3, Cs4PbI6, and polymers. Thus, a combination of these three substances is required to calculate the dielectric constants. The relative dielectric constant of Cs4PbI6 was 9.6, which is higher than that of CsPbI3 (5.9
No emission polarization was observed in the composite films before stretching, whereas the DOLP of the stretched composite films reached 0.37 with unpolarized 405 nm light excitation (
The PL polarization characteristics of the hybrid NC-stretched films under linearly polarized optical excitation were measured (
RGB polarized device based on semipolar μLEDs and stretched perovskite films
A LCD backlight system was developed using a semipolar blue LED array and perovskite composite films. A schematic cross-section of the semipolar 2×2 µLED array with a diameter of 30 µm is shown in
Figure 6.(
The process for fabricating the RGB polarized system is depicted in
Figure 7.(
The RGB polarized μLED device described in this study utilizes CsPbBr3 NRs and CsPbI3-Cs4PbI6 hybrid NC composite films with anisotropic emission properties to provide the green and red components, respectively. In addition, the semipolar blue LED array provides the blue component of polarized emission, enabling the device to emit polarized light containing RGB trichrome. For effective transmission through the first polarizer within the LCD backplane, the polarization direction of the blue light is parallel to the stretching direction of the composite film.
The DOLP of the blue light decreased from 0.37 to 0.29 after the excitation of the green NR composite film alone (
Figure 8.(
To elucidate the advantages of utilizing semipolar blue LEDs as excitation sources in RGB polarized devices, we conducted experiments by replacing the semipolar blue μLED arrays with c-plane μLEDs in our system and measuring the optical properties (
These observations further validate the high efficiency of the RGB polarized device delineated in this study for polarized backlight applications. Currently, the industrial film bidirectional synchronous tensile equipment is capable of manufacturing large-scale stretched polymer films. The perovskite-EVA films in this work were malleable and easy to stretch with high stability. Therefore, it is capable of realizing large-scale manufacturing of perovskite quantum dot color enhanced color conversion stretched film for backlighting of LCD TVs or displays.
Conclusions
This study has demonstrated the potential of a highly efficient and stable RGB polarized device that is well-suited for backlights for LCD and polarizer-adjustable multiplexed color displays. The proposed device incorporates an array of blue semipolar μLEDs with inherent polarization properties as the excitation source. These μLEDs illuminate stretched composite films, composed of green CsPbBr3 NRs and red CsPbI3-Cs4PbI6 hybrid NCs, which serve as the color-conversion layers. In addition to the inherent polarized emission of the CsPbBr3 NRs within the polymer film, the device benefits from strong anisotropic emissions generated by the AWs structures in the CsPbI3-Cs4PbI6 hybrid NCs. These AWs structures have exhibited exceptional stability upon prolonged exposure to blue radiation. The integration of these elements results in high degrees of polarization for the device: 0.26, 0.48, and 0.38 for blue, green, and red emissions, respectively. Furthermore, the device manifests a broad and stable color gamut, fulfilling 137.2% of the NTSC standard and 102.5% of the Rec.2020 specification. In comparison to devices that employ c-plane LEDs for excitation, our approach, which utilizes semipolar μLEDs with intrinsic polarization characteristics, enhances the light intensity passing through the polarizer by 73.6%. In summary, this investigation offers a novel framework for the development of RGB polarized optoelectronic devices, employing anisotropically structured building blocks encased in polymer matrices and μLED technology.
Methods
Fabrication of array of blue semipolar μLEDs
First, indium tin oxide (ITO) was deposited as the p-contact layer. A mesa with a depth of approximately 1 µm was then etched into the ITO layer using a hydrochloric acid solution and an inductively coupled plasma reactive ion etching (ICP-RIE) machine. Subsequently, Ti/Al/Ti/Au metal contacts were deposited using photolithography and an electron gun. Next, 30-nm-thick aluminum oxide and SiO2 passivation layers were deposited via atomic layer deposition and plasma-enhanced chemical vapor deposition, respectively. Finally, Ni/Au was deposited as the p-metal electrode using ICP-RIE, and a distributed Bragg reflector was deposited on the back surface of the wafer to improve the light output efficiency.
Synthesis of Cs-Oleate
To prepare a Cs-precursor, 0.55 g of Cs2CO3 powder in the mixed solution of 20 mL of Oct and 2 mL of OlAc at 130 °C in a vacuum.
Synthesis of CsPbBr3 NRs
Here, 0.1395 g PbBr2, 12 mL of ODE, 1 mL of OAm, and 0.7 mL of OlAc were poured into a three-necked round-bottom flask, heated to 120 °C in a vacuum, and then cooled to room temperature. Afterward, 0.6 mL of Cs source precursor was injected into Pb precursor, and the mixture was allowed to react for 2 h. The sample was centrifuged at 12000 r/min for 3 min and the precipitate formed nanowires. The precipitate was diluted into 2 mL of hexane, and the solution was left to react for 48 h to form the nanorods.
Synthesis of γ-CsPbI3 QDs
In this step, 0.092 g PbI2, 10 mL of ODE, 1 mL of OlAc, and 1 mL of OlAm were degassed in a three-necked flask for approximately 1 h at 120 °C. Then, 0.6 mL of Cs-oleate was injected into the Pb precursor at 155 °C under a vacuum. After 7–8 s, the reaction was quenched in an ice bath. The obtained NCs were centrifuged at 8000 rpm for 5 min. The supernatant was discarded, and 10 mL of hexane was added. Lastly, the obtained hexane solution was centrifuged at 6000 rpm for 5 min.
Synthesis of CsPbI3-Cs4PbI6 NCs
In particular, 0.058 g PbI2, 10 mL of ODE, 1 mL of OlAc, 1 mL of OlAm, and 80 μL of HI were degassed in a three-necked flask for approximately 1 h at 120 °C. Subsequently, 1.7 mL of Cs source precursor was injected into Pb precursor at 155 °C under vacuum. After 7–8 s, the reaction was quenched in an ice-bath. The obtained NCs were centrifuged at 7300 rpm for 5 min. The supernatant was discarded, and 10 mL of hexane was added to the precipitate. The obtained hexane solution was then centrifuged at 4900 rpm for 5 min.
Preparation of tensile polymer films
For typical film preparation, nanorods or hybrid NCs were added to a solution of 5% wt. EVA polymer in toluene. The solutions were added to the glass substrate to cover the entire area, and the sample was placed under vacuum at room temperature for 12 h. The resulting polymer composites were peeled off after a complete evaporation of the solvent. The separated films were stretched to 300% of their original length using a stretching machine.
Measurement of polarization emission
Unpolarized light or // and ⊥ polarized light at 405 nm was used as the excitation source in the polarization characterization of the individual green or red perovskite stretched films. The unpolarized 405 nm light is generated by xenon lamp and monochromator; the // and ⊥ polarized light is generated by a 405 nm laser diode after passing through a polarizer in the corresponding direction. For the subsequent final RGB polarized devices, the excitation sources were semipolar blue μLED array or c-plane blue μLED array, respectively. The transmitted emission was collected and filtered through a polarizer and an appropriate bandpass filter. The collected light was further filtered by a suitable h-bandpass filter and sent to a spectrometer (QE65 Pro, Ocean Optics) to measure its intensity at varying angles through the rotation of the polarizer. Finally, the excitation polarization was regulated by another polarizer situated in the excitation beam path.
Aging test
As the light sources, 450 nm blue LEDs under an injected current of 20 mA were employed. The distance between the blue-LED and color conversion layer was 1 cm. After the corresponding aging time, the PL spectra of the films were measured under the excitation of 356 nm LEDs using a spectrometer (QE65 Pro, Ocean Optics).
Characterizations
A SmartLab SE (Rigaku, Japan) instrument was used to perform the XRD measurements of the samples for a 2θ range of 10°–60°. TEM images were acquired using a JEM 2100 (JEOL, Japan) and a Talos F200X (Thermo Fisher, USA). The samples were prepared using a focused ion beam by a Helios 660 (Thermo Fisher, USA). The absolute PLQYs (λex = 450 nm) were measured in a steady-state/transient fluorescence spectrometer (FLS1000).
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Tingwei Lu, Yue Lin, Tianqi Zhang, Yue Huang, Xiaotong Fan, Shouqiang Lai, Yijun Lu, Hao-Chung Kuo, Zhong Chen, Tingzhu Wu, Rong Zhang. Self-polarized RGB device realized by semipolar micro-LEDs and perovskite-in-polymer films for backlight applications[J]. Opto-Electronic Advances, 2024, 7(3): 230210-1
Category: Research Articles
Received: Nov. 12, 2023
Accepted: Dec. 31, 2023
Published Online: May. 24, 2024
The Author Email: Wu Tingzhu (TZWu)