Recently, there has been tremendous interest in the synthesis and optoelectronic applications of quasi-two-dimensional colloidal nanoplatelets (NPLs). Thanks to the ultranarrow emission linewidth, high-extinction coefficient, and high photostability, NPLs offer an exciting opportunity for high-performance optoelectronics. However, until now, the applications of these NPLs are limited to available discrete emission ranges, limiting the full potential of these exotic materials as efficient light emitters. Here, we introduce a detailed systematic study on the synthesis of NPLs based on the alloying mechanisms in core/shell, core/alloyed shell, alloyed core/shell, and alloyed core/alloyed shell heterostructures. Through the engineering of the band gap supported by the theoretical calculations, we carefully designed and successfully synthesized the NPL emitters with continuously tunable emission. Unlike conventional NPLs showing discrete emission, here, we present highly efficient core/shell NPLs with fine spectral tunability from green to deep-red spectra. As an important demonstration of these efficient emitters, the first-time implementation of yellow NPL light-emitting diodes (LEDs) has been reported with record device performance, including the current efficiency surpassing 18.2 cd A −1 , power efficiency reaching 14.8 lm W −1 , and record luminance exceeding 46 900 cd m −2 . This fine and wide-range color tunability in the visible range from stable and efficient core/shell NPLs is expected to be extremely important for the optoelectronic applications of the family of colloidal NPL emitters.
Colloidal quantum wells (CQWs) have emerged as a promising family of two-dimensional (2D) optoelectronic materials with outstanding properties, including ultranarrow luminescence emission, nearly unity quantum yield, and large extinction coefficient. However, the performance of CQWs-based light-emitting diodes (CQW-LEDs) is far from satisfactory, particularly for deep red emissions (≥660 nm). Herein, high efficiency, ultra-low-efficiency roll-off, high luminance, and extremely saturated deep red CQW-LEDs are reported. A key feature for the high performance is the understanding of charge dynamics achieved by introducing an efficient electron transport layer, ZnMgO, which enables balanced charge injection, reduced nonradiative channels, and smooth films. The CQW-LEDs based on (CdSe/CdS)@(CdS/CdZnS) ((core/crown)@(colloidal atomic layer deposition shell/hot injection shell)) show an external quantum efficiency of 9.89%, which is a record value for 2D nanocrystal LEDs with deep red emissions. The device also exhibits an ultra-low-efficiency roll-off and a high luminance of 3853 cd m −2 . Additionally, an exceptional color purity with the CIE coordinates of (0.719, 0.278) is obtained, indicating that the color gamut covers 102% of the International Telecommunication Union Recommendation BT 2020 (Rec. 2020) standard in the CIE 1931 color space, which is the best for CQW-LEDs. Furthermore, an active-matrix CQW-LED pixel circuit is demonstrated. The findings imply that the understanding of charge dynamics not only enables high-performance CQW-LEDs and can be further applied to other kinds of nanocrystal LEDs but also is beneficial to the development of CQW-LEDs-based display technology and related integrated optoelectronics.
Here, the first account of self-resonant fully colloidal μ-lasers made from colloidal quantum well (CQW) solution is reported. A deep patterning technique is developed to fabricate well-defined high aspect-ratio on-chip CQW resonators made of grating waveguides and in-plane reflectors. The fabricated waveguide-coupled laser, enabling tight optical confinement, assures in-plane lasing. CQWs of the patterned layers are closedpacked with sharp edges and residual-free lifted-off surfaces. Additionally, the method is successfully applied to various nanoparticles including colloidal quantum dots and metal nanoparticles. It is observed that the patterning process does not affect the nanocrystals (NCs) immobilized in the attained patterns and the different physical and chemical properties of the NCs remain pristine. Thanks to the deep patterning capability of the proposed method, patterns of NCs with subwavelength lateral feature sizes and micron-scale heights can possibly be fabricated in high aspect ratios.
with tight 1D exciton confinement, demonstrating highly promising properties by their possible design of heterostructures. [1][2][3] The size-and shape-dependent properties of these materials alongside with various electronic structures enable them for a vast range of optoelectronic applications [4] including light-emitting diodes (LEDs), [5,6] luminescent solar concentrator, [7] photodetectors, [8] lasers, [9][10][11] and photocatalysts. [12] These NPLs offer such advantages over their spherical counterparts, colloidal quantum dots (CQDs), as they possess giant oscillator strengths, [13,14] larger absorption crosssections, [15][16][17] and enhanced molar extinction coefficients. [18] While inhomogeneous broadening is a major drawback of CQDs, NPLs with constant ensemble thickness, exhibit much narrower emission bandwidth. [19,20] CdSe NPLs are among the most studied CQWs, offering a suitable platform as a base material to further design and synthesize complex heterostructures. In its zinc blend crystalline structure, increasing the thickness along [001] direction, normal to the basal planes, [21] can be performed mainly through one of the two strategies: i) One/two-pot synthesis of thick NPLs [22,23] Extending the emission peak wavelength of quasi-2D colloidal quantum wells has been an important quest to fully exploit the potential of these materials, which has not been possible due to the complications arising from the partial dissolution and recrystallization during growth to date. Here, the synthetic pathway of (CdSe/CdS)@(1-4 CdS/CdZnS) (core/crown)@(colloidal atomic layer deposition shell/hot injection shell) hetero-nanoplatelets (NPLs) using multiple techniques, which together enable highly efficient emission beyond 700 nm in the deep-red region, is proposed and demonstrated. Given the challenges of using conventional hot injection procedure, a method that allows to obtain sufficiently thick and passivated NPLs as the seeds is developed. Consequently, through the final hot injection shell coating, thick NPLs with superior optical properties including a high photoluminescence quantum yield of 88% are achieved. These NPLs emitting at 701 nm exhibit a full-width-at-half-maximum of 26 nm, enabled by the successfully maintained quasi-2D shape and minimum defects of the resulting heterostructure. The deep-red light-emitting diode (LED) device fabricated with these NPLs has shown to yield a high external quantum efficiency of 6.8% at 701 nm, which is on par with other types of LEDs in this spectral range.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smll.202106115.
We demonstrate amplified spontaneous emission (ASE) in solution with ultralow thresholds of 30 μJ/cm 2 in red and of 44 μJ/cm 2 in green from engineered colloidal quantum well (CQW) heterostructures. For this purpose, CdSe/CdS core/crown CQWs, designed to hit the green region, and CdSe/CdS@Cd x Zn 1−x S core/crown@gradient-alloyed shell CQWs, further tuned to reach the red region by shell alloying, were employed to achieve highperformance ASE in the visible range. The net modal gain of these CQWs reaches 530 cm −1 for the green and 201 cm −1 for the red, 2−3 orders of magnitude larger than those of colloidal quantum dots (QDs) in solution. To explain the root cause for ultrahigh gain coefficient in solution, we show for the first time that the gain cross sections of these CQWs is ≥3.3 × 10 −14 cm 2 in the green and ≥1.3 × 10 −14 cm 2 in the red, which are two orders of magnitude larger compared to those of CQDs.
Colloidal nanoplatelets (NPLs) have emerged as the last class of semiconductor nanocrystals for their potential optoelectronic applications. The heterostructures of these nanocrystals can achieve high photoluminescence quantum yield and enhanced photostability, along with color purity. Such advantages make them a promising candidate for solution-processable lightemitting diodes (LEDs). However, to date, blue-emitting CdSe nanoplatelets (NPLs) exhibit poor photoluminescence quantum yield and also typically suffer from a rolled-up morphology. To mitigate these problems in this work, we propose and demonstrate efficient alloyed 4 ML CdSe 1−x S x nanoplatelets having a CdS crown with enhanced photoluminescence quantum yields (up to 60%) in the blue region (462−487 nm). We successfully used these NPLs as an electrically driven active emitter in the blue-emitting NPL-LEDs with a low turn-on voltage of ∼4 V. The Commission Internationale de L'Eclairage (CIE) coordinates of (0.23, 0.14) were obtained for these blue-emitting NPL-LEDs. These emitters could potentially open up the opportunity for full-color displays using these NPL-based blue LEDs in conjunction with the red and green ones.
light-emitting diodes and lasing, [1] as a result of their unique optical and electronic properties such as giant oscillator strength, [2] exceptional color purity owing to their magic-size vertical thickness, [3] photoluminescence (PL) quantum yields reaching near-unity, [4][5][6] directed emission profile, [7][8][9] switchable excitonic polarization, [10] and spectral tunability as a result of their lateral size and thickness control at monolayer (ML) precision. [11][12][13] These quasi-2D structures further enable unique opportunities for the design of novel heterostructures as a result of the possibilities of isotropically growing a shell around the entire core seed with atomic layer precision [12,14,15] and/or anisotropically only a crown [16][17][18] with an identical number of monolayers fixes vertical thickness as the seed core, as an purely lateral extension (wings) which is otherwise not possible at such a level of selectivity for other types of solution-processed nanocrystals in different geometries, for example quantum dots (QDs). Using heterostructures of NPLs, amplified spontaneous emission (ASE) with ultralow thresholds, [19][20][21][22][23] large modal gain, [19,21] long gain lifetime, [21,24] and stable ASE [21,25] and lasing [26] have been recently reported in the green and red regions of the visible spectrum using 4 ML CdSe/CdS core/crown, CdSe/Cd 1-x Zn x S core/shell, and CdSe/CdS/Cd 1-x Zn x S core/crown/shell NPLs. However, these have not been achieved using hetero-NPLs in the blue region to date.Since blue emission characteristically necessitates smaller nanocrystals which exhibit faster Auger rates and an increased density of trap surface traps states compared to larger ones in general and, therefore, achieving low threshold ASE and lasing in the blue region is unambiguously difficult for nanocrystals. [27] However, it was demonstrated that NPLs display reduced Auger rates compared to QDs having a comparable bandgap as a result of the reduced exciton density due to the large lateral area of these 2D structures, [28][29][30] which makes them suitable candidates for optical gain studies in the blue region. Yet, there are very few reports on optical gain of NPLs in the blue region compared to heavily studied green and red regions. This is largely due to the poor optical properties of 3 and 2 ML CdSe NPLs that are in the form of Achieving low-threshold optical gain for solution-processed materials is crucial for their real-life applications and deployment as gain media. However, the realization of low gain threshold in the blue region has shown to be technically an extremely challenging task using colloidal nanocrystals as a result of fast nonradiative Auger rates in smaller nanocrystals. Here, ultralow-threshold blue amplified spontaneous emission (ASE) (≈2.7 µJ cm −2 ) accompanied with a large net modal gain coefficient of 360 cm −1 in the blue enabled by blue-emitting (≈455-465 nm) colloidal quantum rings (QRs) of inverted type-I CdS/CdSe core/crown nanoplatelets (NPLs) is proposed and dem...
Functionalization of TiO2 (P25) with oleic acid‐capped CdSe(core)/CdSeTe(crown) quantum‐well nanoplatelets (NPL) yielded remarkable activity and selectivity toward nitrate formation in photocatalytic NOx oxidation and storage (PHONOS) under both ultraviolet (UV‐A) and visible (VIS) light irradiation. In the NPL/P25 photocatalytic system, photocatalytic active sites responsible for the NO(g) photo‐oxidation and NO2 formation reside mostly on titania, while the main function of the NPL is associated with the photocatalytic conversion of the generated NO2 into the adsorbed NO3− species, significantly boosting selectivity toward NOx storage. Photocatalytic improvement in NOx oxidation and storage upon NPL functionalization of titania can also be associated with enhanced electron‐hole separation due to a favorable Type‐II heterojunction formation and photo‐induced electron transfer from the CdSeTe crown to the CdSe core of the quantum well system, where the trapped electrons in the CdSe core can later be transferred to titania. Re‐usability of NPL/P25 system was also demonstrated upon prolonged use of the photocatalyst, where NPL/P25 catalyst surpassed P25 benchmark in all tests.
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