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1.
Sci Adv ; 10(20): eadn8465, 2024 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-38758786

RESUMO

Deep-blue perovskite light-emitting diodes (PeLEDs) of high purity are highly sought after for next-generation displays complying with the Rec. 2020 standard. However, mixed-halide perovskite materials designed for deep-blue emitters are prone to halide vacancies, which readily occur because of the low formation energy of chloride vacancies. This degrades bandgap instability and performance. Here, we propose a chloride vacancy-targeting passivation strategy using sulfonate ligands with different chain lengths. The sulfonate groups have a strong affinity for lead(II) ions, effectively neutralizing vacancies. Our strategy successfully suppressed phase segregation, yielding color-stable deep-blue PeLEDs with an emission peak at 461 nanometers and a maximum luminance (Lmax) of 2707 candela per square meter with external quantum efficiency (EQE) of 3.05%, one of the highest for Rec. 2020 standard-compliant deep-blue PeLEDs. We also observed a notable increase in EQE up to 5.68% at Lmax of 1978 candela per square meter with an emission peak at 461 nanometers by changing the carbon chain length.

2.
Adv Sci (Weinh) ; 11(13): e2306798, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38240455

RESUMO

Solution-processed low-bandgap semiconductors are crucial to next-generation infrared (IR) detection for various applications, such as autonomous driving, virtual reality, recognitions, and quantum communications. In particular, III-V group colloidal quantum dots (CQDs) are interesting as nontoxic bandgap-tunable materials and suitable for IR absorbers; however, the device performance is still lower than that of Pb-based devices. Herein, a universal surface-passivation method of InAs CQDs enabled by intermediate phase transfer (IPT), a preliminary process that exchanges native ligands with aromatic ligands on the CQD surface is presented. IPT yields highly stable CQD ink. In particular, desirable surface ligands with various reactivities can be obtained by dispersing them in green solvents. Furthermore, CQD near-infrared (NIR) photodetectors are demonstrated using solution processes. Careful surface ligand control via IPT is revealed that enables the modulation of surface-mediated photomultiplication, resulting in a notable gain control up to ≈10 with a fast rise/fall response time (≈12/36 ns). Considering the figure of merit (FOM), EQE versus response time (or -3 dB bandwidth), the optimal CQD photodiode yields one of the highest FOMs among all previously reported solution-processed nontoxic semiconductors comprising organics, perovskites, and CQDs in the NIR wavelength range.

3.
ACS Appl Mater Interfaces ; 15(33): 39408-39416, 2023 Aug 23.
Artigo em Inglês | MEDLINE | ID: mdl-37555937

RESUMO

Hybrid colloidal quantum dot (CQD)/organic architectures are promising candidates for emerging optoelectronic devices having high performance and inexpensive fabrication. For unlocking the potential of CQD/organic hybrid devices, enhancing charge extraction properties at electron transport layer (ETL)/CQD interfaces is crucial. Hence, we carefully adjust the interface properties between the ETL and CQD layer by incorporating an interfacial layer for the ETL (EIL) using several types of cinnamic acid ligands. The EIL having a cascading band offset (ΔEC) between the ETL and CQD layer suppresses the potential barrier and the local charge accumulation at ETL/CQD interfaces, thereby reducing the bimolecular recombination. An optimal EIL effectively expands the depletion region that facilitates charge extraction between the ETL and CQD layer while preventing the formation of shallow traps. Representative devices with an EIL exhibit a maximum power conversion efficiency of 14.01% and retain over 80% of initial performances after 300 h under continuous maximum power point operation.

4.
Small ; 19(41): e2302195, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37300352

RESUMO

Lead sulfide (PbS) colloidal quantum dots (CQDs) are promising materials for next-generation flexible solar cells because of near-infrared absorption, facile bandgap tunability, and superior air stability. However, CQD devices still lack enough flexibility to be applied to wearable devices owing to the poor mechanical properties of CQD films. In this study, a facile approach is proposed to improve the mechanical stability of CQDs solar cells without compromising the high power conversion efficiency (PCE) of the devices. (3-aminopropyl)triethoxysilane (APTS) is introduced on CQD films to strengthen the dot-to-dot bonding via QD-siloxane anchoring, and as a result, crack pattern analysis reveals that the treated devices become robust to mechanical stress. The device maintains 88% of the initial PCE under 12 000 cycles at a bending radius of 8.3 mm. In addition, APTS forms a dipole layer on CQD films, which improves the open circuit voltage (VOC ) of the device, achieving a PCE of 11.04%, one of the highest PCEs in flexible PbS CQD solar cells.

5.
Adv Sci (Weinh) ; 9(13): e2200073, 2022 May.
Artigo em Inglês | MEDLINE | ID: mdl-35233994

RESUMO

Although post-synthetic anion exchange allows halide perovskite quantum dots to easily change the optical bandgap of materials, additional exchange of shorter ligands is required to use them as active materials in optoelectronic devices. In this study, a novel all-in-one process exchanging ligands and halide anions in film-state for facile color tuning and patterning of cesium lead halide perovskite colloidal quantum dot (PeQD) light-emitting diodes (LEDs) is proposed. The proposed all-in-one process significantly enhances the performances of PeQD LEDs by passivating the PeQD with shorter ligands. In addition, the all-in-one process is repeated more stably in the film state. Red, green, and blue LEDs with extremely narrow emission spectra using cesium lead bromide PeQDs and appropriate butylammonium halide solutions are fabricated. Furthermore, the proposed all-in-one process in film-state facilitated rapid color change in localized areas, thereby aiding in realizing fine patterns of narrow widths (300 µm) using simple contact masks. Consequently, various paint-over red/green/blue patterns in PeQD LEDs by applying halide solutions additively are fabricated.

6.
ACS Appl Mater Interfaces ; 12(52): 57840-57846, 2020 Dec 30.
Artigo em Inglês | MEDLINE | ID: mdl-33320537

RESUMO

Colloidal quantum dots (CQDs) have large surface-to-volume ratios; thus, surface control is critical, especially when CQDs are utilized in optoelectronic devices. Layer-by-layer solid-state ligand exchange is a facile and applicable process for the formation of conductive CQD solids through various ligands; however, achieving complete ligand exchange on the CQD surface without dangling bonds is challenging. Herein, we demonstrate that CQDs can be further passivated through two-step annealing; air annealing forms sulfonate bonding at (111) Pb-rich surfaces, and subsequent N2 annealing removes insulating oxygen layers from the (100) surfaces of CQDs. By subsequently conducting annealing treatment in two different environments, traps on the surface of CQDs could be significantly reduced. We achieved a 40.8% enhancement of the power conversion efficiency by optimizing each two-step annealing process.

7.
Adv Mater ; 30(25): e1707224, 2018 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-29748976

RESUMO

A novel self-charging platform is proposed using colloidal-quantum-dot (CQD) photovoltaics (PVs) via the near-infrared (NIR) band for low-power electronics. Low-bandgap CQDs can convert invisible NIR light sources to electrical energy more efficiently than wider spectra because of reduced thermalization loss. This energy-conversion strategy via NIR photons ensures an enhanced photostability of the CQD devices. Furthermore, the NIR wireless charging system can be concealed using various colored and NIR-transparent fabric or films, providing aesthetic freedom. Finally, an NIR-driven wireless charging system is demonstrated for a wearable healthcare bracelet by integrating a CQD PVs receiver with a flexible lithium-ion battery and entirely embedding them into a flexible strap, enabling permanent self-charging without detachment.

8.
Sci Rep ; 7(1): 17393, 2017 12 12.
Artigo em Inglês | MEDLINE | ID: mdl-29234046

RESUMO

Bandgap tunability and broadband absorption make quantum-dot (QD) photovoltaic cells (PVs) a promising candidate for future solar energy conversion systems. Approaches to improving the electrical properties of the active layer increase efficiency in part. The present study focuses on optical room for enhancement in QD PVs over wide spectrum in the near-infrared (NIR) region. We find that ray-optical light trapping schemes rather than the nanophotonics approach may be the best solution for enhancing broadband QD PVs by suppressing the escape probability of internal photons without spectral dependency. Based on the theoretical study of diverse schemes for various bandgaps, we apply a V-groove structure and a V-groove textured compound parabolic trapper (VCPT) to PbS-based QD PVs along with the measurement issues for PVs with a light scattering layer. The efficiency of the best device is improved from 10.3% to 11.0% (certified to 10.8%) by a V-groove structure despite the possibility of underestimation caused by light scattering in small-area devices (aperture area: 0.0625 cm2). By minimizing such underestimation, even greater enhancements of 13.6% and 15.6% in short circuit current are demonstrated for finger-type devices (0.167 cm2 without aperture) and large-area devices (2.10 cm2 with an aperture of 0.350 cm2), respectively, using VCPT.

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