Solution-processed inorganic and organic materials have been pursued for more than a decade as low-threshold, high-gain lasing media, motivated in large part by their tunable optoelectronic properties and ease of synthesis and processing. Although both have demonstrated stimulated emission and lasing, they have not yet approached the continuous-wave pumping regime. Two-dimensional CdSe colloidal nanosheets combine the advantage of solution synthesis with the optoelectronic properties of epitaxial two-dimensional quantum wells. Here, we show that these colloidal quantum wells possess large exciton and biexciton binding energies of 132 meV and 30 meV, respectively, giving rise to stimulated emission from biexcitons at room temperature. Under femtosecond pulsed excitation, close-packed thin films yield an ultralow stimulated emission threshold of 6 μJ cm(-2), sufficient to achieve continuous-wave pumped stimulated emission, and lasing when these layers are embedded in surface-emitting microcavities.
Metal halide perovskite nanocrystals (NCs) possess high photoluminescence (PL) quantum yield (PL) and color tunability. Yet, until now, it has been difficult to maintain the high PL observed in solution in spin-coated films. Here, we report a novel CsPbBr3 NCs room-temperature synthesis based on Cs acetate, which displays near-unity PL in solid-state films upon post-synthetic treatment with lead bromide. The as-synthesized NCs show a PL of 80% in spincoated films but the post-synthesis treatment further enhances the efficiency >95%. The high PL is further confirmed by the monomolecular decay of the PL (5.8 ns) indicating a nearly complete suppression of non-radiative channels. The obtained films demonstrate high stability in air and require around 3 weeks to decrease to half the initial PL value.
We measured the intrinsic ground-state exciton dephasing and population dynamics in colloidal quasi-two-dimensional (2D) CdSe nanoplatelets at low temperature (5-50 K) using transient resonant four-wave mixing in heterodyne detection. Our results indicate that below 20 K the exciton dephasing is lifetime limited, with the exciton population lifetime being as fast as 1 ps. This is consistent with an exciton lifetime given by a fast radiative decay due to the large in-plane coherence area of the exciton center-of-mass motion in these quasi-2D systems compared to spherical nanocrystals. The radiative rate in such 2D platelet systems can be controlled by the platelet area over orders of magnitude
Current colloidal synthesis methods for CdSe nanoplatelets (NPLs) routinely yield samples that emit, in discrete steps, from 460 to 550 nm. A significant challenge lies with obtaining thicker NPLs, to further widen the emission range. This is at present typically achieved via colloidal atomic layer deposition onto CdSe cores, or by synthesizing NPL core/shell structures. Here, we demonstrate a novel reaction scheme, where we start from 4.5 monolayer (ML) NPLs and increase the thickness in a two-step reaction that switches from 2D to 3D growth. The key feature is the enhancement of the growth rate of basal facets by the addition of CdCl, resulting in a series of nearly monodisperse CdSe NPLs with thicknesses between 5.5 and 8.5 ML. Optical characterization yielded emission peaks from 554 nm up to 625 nm with a line width (fwhm) of 9-13 nm, making them one of the narrowest colloidal nanocrystal emitters currently available in this spectral range. The NPLs maintained a short emission lifetime of 5-11 ns. Finally, due to the increased red shift of the NPL band edge photoluminescence excitation spectra revealed several high-energy peaks. Calculation of the NPL band structure allowed us to identify these excited-state transitions, and spectral shifts are consistent with a significant mixing of light and split-off hole states. Clearly, chloride ions can add a new degree of freedom to the growth of 2D colloidal nanocrystals, yielding new insights into both the NPL synthesis as well as their optoelectronic properties.
Colloidal Quantum Dot (CQD) light emitting diodes (LEDs) have delivered compelling performance in the visible, yet infrared CQD LEDs underperform their visible-emitting counterparts, largely due to their low photoluminescence quantum efficiency (PLQE). Herein, we employ a ternary blend of CQD thin film comprising a binary host matrix that serves to electronically passivate as well as to cater for efficient and balanced carrier supply to the emitting QD species. In doing so, we report on infrared PbS CQD LEDs with external quantum efficiency of ~7.9% and power conversion efficiency of ~9.3%, thanks to their very low trap-state density on the order of 10 14 cm-3 and very high PLQE in electrically conductive QD solids of more than 60%. When these blend devices operate as solar cells they deliver VOC approaching their radiative limit thanks to the synergistic effect of reduced trap state density and the density of states modification in the nanocomposite. Near and shortwave infrared (NIR, SWIR) light emitting diodes serve a rather broad range of applications, including night vision 1 , surveillance 2 , remote sensing 3 , biological imaging 4 and spectroscopy 5. Recent progress in on-chip and wearable infrared spectroscopy for quality inspection, health and process monitoring also requires the development of highly efficient,
We report a comprehensive study on the two-photon absorption cross sections of colloidal CdSe nanoplatelets, -rods, and -dots of different sizes by the means of z-scan and two-photon excitation spectroscopy. Platelets combine large particle volumes with ultra strong confinement. In contrast to weakly confined nanocrystals, the TPA cross sections of CdSe nanoplatelets scale superlinearly with volume (V(∼2)) and show ten times more efficient two-photon absorption than nanorods or dots. This unexpectedly strong shape dependence goes well beyond the effect of local fields. The larger the particles' aspect ratio, the greater is the confinement related electronic contribution to the increased two-photon absorption. Both electronic confinement and local field effects favor the platelets and make them unique two-photon absorbers with outstanding cross sections of up to 10(7) GM, the largest ever reported for (colloidal) semiconductor nanocrystals and ideally suited for two-photon imaging and nonlinear optoelectronics. The obtained results are confirmed by two independent techniques as well as a new self-referencing method.
We evidence excited state emission from p states well below ground state saturation in CdSe nanoplatelets. Size-dependent exciton ground and excited state energies and population dynamics are determined by four independent methods: time-resolved PL, time-integrated PL, rate equation modeling, and Hartree renormalized k·p calculations-all in very good agreement. The ground state-excited state energy spacing strongly increases with the lateral platelet quantization. Depending on its detuning to the LO phonon energy, the PL decay of CdSe platelets is governed by a size tunable LO phonon bottleneck, related to the low exciton-phonon coupling, very large oscillator strength, and energy spacing of both states. This is, for instance, ideal to tune lasing properties. CdSe platelets are perfectly suited to control the exciton-phonon interaction by changing their lateral size while the optical transition energy is determined by their thickness.
The lateral dimensions of CdSe nanoplatelets have a strong and unique influence on their opto-electronic properties, with sizes that can be tuned from the weak to the strong exciton confinement regime. There are state-of-the-art reports on several nanoplatelet syntheses; however, at present only the thickness is well-controlled. We demonstrate here that we can achieve a control over the aspect ratio and overall nanoplate area by carefully adjusting the reagents that induce the in-plane growth. A variation of the fraction of hydrated Cd(OAc) in a Cd(OAc)/Cd(OAc)·2HO mixture tailors the nanoplatelet aspect ratio. This occurs independently of the reaction time, which can be used to fine-tune the overall length and width. An interpretation is given by the in situ formation of a small amount of hydroxide anions that alter the surface energy of specific planes.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
hi@scite.ai
10624 S. Eastern Ave., Ste. A-614
Henderson, NV 89052, USA
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.