Search

Although achieving optical gain using aqueous solutions of colloidal nanocrystals as a gain medium is exceptionally beneficial for bio-optoelectronic applications, the realization of optical gain in an aqueous medium using solution-processed nanocrystals has been extremely challenging because of the need for surface modification to make nanocrystals water dispersible while still maintaining their gain. Here, we present the achievement of optical gain in an aqueous medium using an advanced architecture of CdSe/CdS@CdxZn1−xS core/crown@gradient-alloyed shell colloidal quantum wells (CQWs) with an ultralow threshold of ∼3.4 µJ cm−2 and an ultralong gain lifetime of ∼2.6 ns. This demonstration of optical gain in an aqueous medium is a result of the carefully heterostructured CQWs having large absorption cross-section and gain cross-section in addition to inherently slow Auger recombination in these CQWs. Furthermore, we show low-threshold in-water amplified spontaneous emission (ASE) from these aqueous CQWs with a threshold of 120 µJ cm−2 In addition, we demonstrate a whispering gallery mode laser with a low threshold of ∼30 µJ cm−2 obtained by incorporating films of CQWs by exploiting layerby-layer approach on a fiber. The observation of low-threshold optical gain with ultralong gain lifetime presents a significant step toward the realization of advanced optofluidic colloidal lasers and their continuous-wave pumping. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) National Research Foundation (NRF) Submitted/Accepted version The authors gratefully acknowledge the financial support in part from Singapore National Research Foundation under the programs of NRF-NRFI2016-08, the Science and the Singapore Agency for Science, Technology and Research (A*STAR) SERC Pharos Program under grant number 152-73-00025 and Agency for Science, Technology and Research (A*STAR) MTC program under grant number M21J9B0085, Ministry of Education Tier 1 under grant number MOE-RG62/20 (Singapore), and in part from TUBITAK 119N343, 120N076, 121N395 and 20AG001.

Novel, vertically oriented self-assembly of core/shell CdSe/CdZnS colloidal quantum wells stacked in film via the control of hydrophilicity/lipophilicity is shown for optical gain media, allowing amplified spontaneous emission and random lasing.

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 light-emitting 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 CdSe1-xSx 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. Ministry of Education (MOE) National Research Foundation (NRF) Accepted version This research is supported by the National Research Foundation, Prime Minister’s Office, Singapore under its NRF Investigatorship Award program (NRF-NRFI2016-08) and the Ministry of Education Tier 1 grant (MOE-RG62/20). H.V.D. also gratefully acknowledges the support from TUBA

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. Agency for Science, Technology and Research (A*STAR) National Research Foundation (NRF) The authors gratefully acknowledge the financial support in part from Singapore National Research Foundation under the programs of NRF-NRFI2016-08, NRF-CRP14-2014-03 and the Science and Engineering Research Council, Agency for Science, Technology and Research (A*STAR) of Singapore and in part from TUBITAK 115F297, 117E713, and 119N343. H.V.D. also acknowledges support from TUBA.

We demonstrate amplified spontaneous emission (ASE) in solution with ultralow thresholds of 30 μJ/cm2 in red and of 44 μJ/cm2 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@CdxZn1–xS core/crown@gradient-alloyed shell CQWs, further tuned to reach the red region by shell alloying, were employed to achieve high-performance 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 cm2 in the green and ≥1.3 × 10–14 cm2 in the red, which are two orders of magnitude larger compared to those of CQDs. Agency for Science, Technology and Research (A*STAR) National Research Foundation (NRF) Accepted version The authors gratefully acknowledge the financial support in part from Singapore National Research Foundation under the programs of NRF-NRFI2016-08, NRF-CRP14-2014-03 and the Science and the Singapore Agency for Science, Technology and Research (A*STAR) SERC Pharos Program under Grant No. 152-73-00025 and in part from TUBITAK 115F297, 117E713, and 119N343. H.V.D. also gratefully acknowledges support from TUBA. O.E. acknowledges support from TUBITAK BIDEB. S.D. and O.E contributed equally. The authors declare no competing financial interest.

Self-assembly of colloidal nanocrystals into ordered superlattices is a powerful approach to enable novel collective properties which are not available in individual colloids. However, to date, it remains a major challenge to develop a practical route to modulate such collective properties for potential photonic applications. Herein, it is shown that the collective emission properties in colloidal quantum well (CQW) superlattices, including emission color and anisotropy, can be effectively modulated in a binary host–guest architecture. The experimental and theoretical results reveal that excitons of the host (i.e., the undoped CQWs) generated by photoexcitation can be controllably harvested by the guest (i.e., the Cu-doped CQWs) for light emission, owing to an exciton hopping assisted exciton trapping process. Such a nano-building block with tunable collective optical properties may enlighten novel colloidal material-based photonic applications, including optical anti-counterfeiting, next-generation liquid crystal displays, and multifunctional biological markers. Ministry of Education (MOE) National Research Foundation (NRF) Accepted version The authors would like to acknowledge the financial support from Singapore National Research Foundation under the program of NRF-NRFI2016-08, the Competitive Research Program NRF-CRP14-2014-03, and the Singapore Ministry of Education AcRF Tier-1 grant (MOE2019-T1-002-087). H.V.D. is also grateful to acknowledge additional financial support from the TUBA.

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 ) accompanied with a large net modal gain coefficient of 360 cm 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 demonstrated. The synthesized QRs with controlled crown size outperform the best reported ASE thresholds and net modal gain coefficients from the solution-processed materials by ≈2.5- and ≈4-fold, respectively, in the similar blue spectral window. Utilizing this QR architecture, it is also shown that the ASE peak can be spectrally tuned by controlling the lateral size of the crown and hence quantum confinement in the lateral direction. These outstanding results support the prospects of these solution-processed QRs made of 2D hetero-NPLs in the challenging blue region as colloidal gain. Agency for Science, Technology and Research (A*STAR) National Research Foundation (NRF) Accepted version