Deterministic positioning of few aqueous colloidal quantum dots.

Emerging quantum technologies that critically require the integration of quantum emitters on photonic platforms are hindered by the control over their position, quantity, and scalability. Herein, we describe a facile strategy to deposit aqueous silica-coated quantum dots (QDs) in a template of polymethyl methacrylate (PMMA) nanoholes that leverages saturated ethanol vapor drop-casting and subsequent lift-off of the template. Ethanol vapor incorporation into water droplets during the drying process reduces the meniscus contact angle, which increases capillary forces and enhances particle confinement within the pinning contact region.

Demystifying Trion Emission in CdSe Nanoplatelets.

At cryogenic temperatures, the photoluminescence spectrum of CdSe nanoplatelets (NPLs) usually consists of multiple emission lines, the origin of which is still under debate. While there seems to be consensus that both neutral excitons and trions contribute to the NPL emission, the prominent role of trions is rather puzzling. In this work, we demonstrate that Förster resonant energy transfer in stacks of NPLs combined with hole trap states in specific NPLs within the stack trigger trion formation, while single NPL spectra are dominated by neutral excitonic emission.

Strongly polarized color conversion of isotropic colloidal quantum dots coupled to fano resonances.

Colloidal quantum dots (QDs) offer high color purity essential to high-quality liquid crystal displays (LCDs), which enables unprecedented levels of color enrichment in LCD-TVs today. However, for LCDs requiring polarized backplane illumination in operation, highly polarized light generation using inherently isotropic QDs remains a fundamental challenge. Here, we show strongly polarized color conversion of isotropic QDs coupled to Fano resonances of v-grooved surfaces compatible with surface-normal LED illumination for next-generation QD-TVs.

Orientation-Dependent Photoconductivity of Quasi-2D Nanocrystal Self-Assemblies: Face-Down, Edge-Up Versus Randomly Oriented Quantum Wells.

Here, strongly orientation-dependent lateral photoconductivity of a CdSe monolayer colloidal quantum wells (CQWs) possessing short-chain ligands is reported. A controlled liquid-air self-assembly technique is utilized to deliberately engineer the alignments of CQWs into either face-down (FO) or edge-up (EO) orientation on the substrate as opposed to randomly oriented (RO) CQWs prepared by spin-coating. Adapting planar configuration metal-semiconductor-metal (MSM) photodetectors, it is found that lateral conductivity spans ≈2 orders of magnitude depending on the orientation of CQWs in the film in the case of utilizing short ligands.

Weakly Confined Organic-Inorganic Halide Perovskite Quantum Dots as High-Purity Room-Temperature Single Photon Sources.

Colloidal perovskite quantum dots (PQDs) have emerged as highly promising single photon emitters for quantum information applications. Presently, most strategies have focused on leveraging quantum confinement to increase the nonradiative Auger recombination (AR) rate to enhance single-photon (SP) purity in all-inorganic CsPbBr QDs. However, this also increases the fluorescence intermittency.

"Giant" Colloidal Quantum Well Heterostructures of CdSe@CdS Core@Shell Nanoplatelets from 9.5 to 17.5 Monolayers in Thickness Enabling Ultra-High Gain Lasing.

Semiconductor colloidal quantum wells (CQWs) have emerged as a promising class of gain materials to be used in colloidal lasers. Although low gain thresholds are achieved, the required high gain coefficient levels are barely met for the applications of electrically-driven lasers which entails a very thin gain matrix to avoid charge injection limitations. Here, "giant" CdSe@CdS colloidal quantum well heterostructures of 9.

Photoinduced Transition from Quasi-Two-Dimensional Ruddlesden-Popper to Three-Dimensional Halide Perovskites for the Optical Writing of Multicolor and Light-Erasable Images.

Optical data storage, information encryption, and security labeling technologies require materials that exhibit local, pronounced, and diverse modifications of their structure-dependent optical properties under external excitation. Herein, we propose and develop a novel platform relying on lead halide Ruddlesden-Popper phases that undergo a light-induced transition toward bulk perovskite and employ this phenomenon for the direct optical writing of multicolor patterns. This transition causes the weakening of quantum confinement and hence a reduction in the band gap.

Dual-Resonance Nanostructures for Color Downconversion of Colloidal Quantum Emitters.

We present a dual-resonance nanostructure made of a titanium dioxide (TiO) subwavelength grating to enhance the color downconversion efficiency of CdZnSeS colloidal quantum dots (QDs) emitting at ∼530 nm when excited with a blue light at ∼460 nm. A large mode volume can be created within the QD layer by the hybridization of the grating resonances and waveguide modes, resulting in large absorption and emission enhancements. Particularly, we achieved polarized light emission with a maximum photoluminescence enhancement of ∼140 times at a specific angular direction and a total enhancement of ∼34 times within a 0.

Light-sensitive monolayer-thick nanocrystal skins of face-down self-oriented colloidal quantum wells.

Colloidal quantum wells (CQWs), a quasi-two-dimensional, atomically-flat sub-family of semiconductor nanocrystals, are well suited to produce excellent devices for photosensing applications thanks to their extraordinarily large absorption cross-sections. In this work, we propose and demonstrate a new class of light-sensitive nanocrystal skins (LS-NS) that employ a monolayer of face-down orientation-controlled self-assembled CQWs as the active absorbing layer in the UV-visible range. This CQW LS-NS platform enables non-conventional photosensing operation that relies on the strong optical absorption of the monolayered assembly of CQWs and the subsequent photogenerated potential build-up across the device, allowing for self-powered operation.

Near-Unity Emitting, Widely Tailorable, and Stable Exciton Concentrators Built from Doubly Gradient 2D Semiconductor Nanoplatelets.

The strength of electrostatic interactions (EIs) between electrons and holes within semiconductor nanocrystals profoundly affects the performance of their optoelectronic systems, and different optoelectronic devices demand distinct EI strength of the active medium. However, achieving a broad range and fine-tuning of the EI strength for specific optoelectronic applications is a daunting challenge, especially in quasi two-dimensional core-shell semiconductor nanoplatelets (NPLs), as the epitaxial growth of the inorganic shell along the direction of the thickness that solely contributes to the quantum confined effect significantly undermines the strength of the EI. Herein we propose and demonstrate a doubly gradient (DG) core-shell architecture of semiconductor NPLs for on-demand tailoring of the EI strength by controlling the localized exciton concentration via in-plane architectural modulation, demonstrated by a wide tuning of radiative recombination rate and exciton binding energy.

Optically detected magnetic resonance spectroscopic analyses on the role of magnetic ions in colloidal nanocrystals.

Incorporating magnetic ions into semiconductor nanocrystals has emerged as a prominent research field for manipulating spin-related properties. The magnetic ions within the host semiconductor experience spin-exchange interactions with photogenerated carriers and are often involved in the recombination routes, stimulating special magneto-optical effects. The current account presents a comparative study, emphasizing the impact of engineering nanostructures and selecting magnetic ions in shaping carrier-magnetic ion interactions.

Aqueous colloidal nanoplatelets for imaging and improved ALA-based photodynamic therapy of prostate cancer cells.

Fluorescent, CdSe/CdS core/crown heterostructured nanoplatelets (NPLs) were transferred to the water a simple, single-step ligand exchange using 2-mercaptopropionic acid in a simple extraction process. These stable, aqueous NPLs were loaded with a modal drug, 5-aminolevulinic acid (ALA). ALA-loaded NPLs emerged as a new class of theranostic nanoparticles for image-guided enhanced photodynamic therapy of both androgen-dependent and -independent human prostate cancer cells.

Vertically oriented self-assembly of colloidal CdSe/CdZnS quantum wells controlled hydrophilicity/lipophilicity balance: optical gain of quantum well stacks for amplified spontaneous emission and random lasing.

We propose and demonstrate vertically oriented self-assembly of colloidal quantum wells (CQWs) that allows for stacking CdSe/CdZnS core/shell CQWs in films for the purposes of amplified spontaneous emission (ASE) and random lasing. Here, a monolayer of such CQW stacks is obtained liquid-air interface self-assembly (LAISA) in a binary subphase by controlling the hydrophilicity/lipophilicity balance (HLB), a critical factor for maintaining the orientation of CQWs during their self-assembly. Ethylene glycol, as a hydrophilic subphase, orients the coalition of these CQWs into self-assembled multi-layers in the vertical direction.

On the Rational Design of Core/(Multi)-Crown Type-II Heteronanoplatelets.

Solution-processed two-dimensional nanoplatelets (NPLs) allowing lateral growth of a shell (crown) by not affecting the pure confinement in the vertical direction provide unprecedented opportunities for designing heterostructures for light-emitting and -harvesting applications. Here, we present a pathway for designing and synthesizing colloidal type-II core/(multi-)crown hetero-NPLs and investigate their optical properties. Stoke's shifted broad photoluminescence (PL) emission and long PL lifetime (∼few 100 ns) together with our wavefunction calculations confirm the type-II electronic structure in the synthesized CdS/CdSeTe core/crown hetero-NPLs.

Highly-Directional, Highly-Efficient Solution-Processed Light-Emitting Diodes of All-Face-Down Oriented Colloidal Quantum Well Self-Assembly.

Semiconductor colloidal quantum wells (CQWs) provide anisotropic emission behavior originating from their anisotropic optical transition dipole moments (TDMs). Here, solution-processed colloidal quantum well light-emitting diodes (CQW-LEDs) of a single all-face-down oriented self-assembled monolayer (SAM) film of CQWs that collectively enable a supreme level of IP TDMs at 92% in the ensemble emission are shown. This significantly enhances the outcoupling efficiency from 22% (of standard randomly-oriented emitters) to 34% (of face-down oriented emitters) in the LED.

High External Quantum Efficiency Light-Emitting Diodes Enabled by Advanced Heterostructures of Type-II Nanoplatelets.

Colloidal quantum wells (CQWs), also known as nanoplatelets (NPLs), are exciting material systems for numerous photonic applications, including lasers and light-emitting diodes (LEDs). Although many successful type-I NPL-LEDs with high device performance have been demonstrated, type-II NPLs are not fully exploited for LED applications, even with alloyed type-II NPLs with enhanced optical properties. Here, we present the development of CdSe/CdTe/CdSe core/crown/crown (multi-crowned) type-II NPLs and systematic investigation of their optical properties, including their comparison with the traditional core/crown counterparts.

High-Frequency EPR and ENDOR Spectroscopy of Mn Ions in CdSe/CdMnS Nanoplatelets.

Semiconductor colloidal nanoplatelets based of CdSe have excellent optical properties. Their magneto-optical and spin-dependent properties can be greatly modified by implementing magnetic Mn ions, using concepts well established for diluted magnetic semiconductors. A variety of magnetic resonance techniques based on high-frequency (94 GHz) electron paramagnetic resonance in continuous wave and pulsed mode were used to get detailed information on the spin structure and spin dynamics of Mn ions in core/shell CdSe/(Cd,Mn)S nanoplatelets.

Measuring the Ultrafast Spectral Diffusion and Vibronic Coupling Dynamics in CdSe Colloidal Quantum Wells using Two-Dimensional Electronic Spectroscopy.

We measure the ultrafast spectral diffusion, vibronic dynamics, and energy relaxation of a CdSe colloidal quantum wells (CQWs) system at room temperature using two-dimensional electronic spectroscopy (2DES). The energy relaxation of light-hole (LH) excitons and hot carriers to heavy-hole (HH) excitons is resolved with a time scale of ∼210 fs. We observe the equilibration dynamics between the spectroscopically accessible HH excitonic state and a dark state with a time scale of ∼160 fs.

Gradient Type-II CdSe/CdSeTe/CdTe Core/Crown/Crown Heteronanoplatelets with Asymmetric Shape and Disproportional Excitonic Properties.

Characterized by their strong 1D confinement and long-lifetime red-shifted emission spectra, colloidal nanoplatelets (NPLs) with type-II electronic structure provide an exciting ground to design complex heterostructures with remarkable properties. This work demonstrates the synthesis and optical characterization of CdSe/CdSeTe/CdTe core/crown/crown NPLs having a step-wise gradient electronic structure and disproportional wavefunction distribution, in which the excitonic properties of the electron and hole can be finely tuned through adjusting the geometry of the intermediate crown. The first crown with staggered configuration gives rise to a series of direct and indirect transition channels that activation/deactivation of each channel is possible through wavefunction engineering.

Observation of optical gain from aqueous quantum well heterostructures in water.

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@CdZnS core/crown@gradient-alloyed shell colloidal quantum wells (CQWs) with an ultralow threshold of ∼3.4 μJ cm and an ultralong gain lifetime of ∼2.

High-Performance Deep Red Colloidal Quantum Well Light-Emitting Diodes Enabled by the Understanding of Charge Dynamics.

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.