The empirical correlation between size and two-photon absorption cross section of CdSe and CdTe quantum dots

The tuning of CdSe quantum dot (QDs) sizes, and consequently their corresponding two-photon absorption (TPA) cross section, has been systematically investigated. As the size (diameter) of the quantum dots increases, the TPA cross section is found to be empirically related via a power-law proportionality of 3.5+/-0.5 and 5.6+/-0.7 to the diameters of CdSe and CdTe QDs, respectively. The results are tentatively rationalized via a theoretical model of two-photon excitation properties in a system incorporating excitons and defects.     

Red, green and blue lasing enabled by single-exciton gain in colloidal quantum dot films

Colloidal quantum dots exhibit efficient photoluminescence with widely tunable bandgaps as a result of quantum confinement effects. Such quantum dots are emerging as an appealing complement to epitaxial semiconductor laser materials, which are ubiquitous and technologically mature, but unable to cover the full visible spectrum (red, green and blue; RGB). However, the requirement for high colloidal-quantum-dot packing density, and losses due to non-radiative multiexcitonic Auger recombination, have hindered the development of lasers based on colloidal quantum dots. Here, we engineer CdSe/ZnCdS core/shell colloidal quantum dots with aromatic ligands, which form densely packed films exhibiting optical gain across the visible spectrum with less than one exciton per colloidal quantum dot on average. This single-exciton gain allows the films to reach the threshold of amplified spontaneous emission at very low optical pump energy densities of 90?μJ?cm(-2), more than one order of magnitude better than previously reported values. We leverage the low-threshold gain of these nanocomposite films to produce the first colloidal-quantum-dot vertical-cavity surface-emitting lasers (CQD-VCSEL). Our results represent a significant step towards full-colour single-material lasers.     

PbS量子点能级结构的尺寸和配体依赖性及其对异质结电池性能的影响

通过电化学循环伏安测试和吸收光谱测试, 确定了有机配体(油酸)和原子配体(四正丁基碘化铵, TBAI)钝化的不同粒径(2.6~4.5 nm)PbS量子点的导带和价带能级, 并研究了量子点尺寸对PbS/TiO₂异质结电池(空气气氛中制备)性能的影响。结果表明：PbS量子点的能级结构受其粒径大小和表面配体特性的影响。当PbS量子点尺寸从2.6 nm增加至4.5 nm时, 油酸包覆PbS量子点的导带底从-3.67 eV减小到-4.0 eV, 价带顶从-5.19 eV增加到-4.97 eV; 而对于TBAI配体置换的PbS量子点, 其导带底和价带顶则分别从-4.15 eV和-5.61 eV变化至-4.51 eV和-5.46 eV。粒径为3.9 nm的PbS量子点所制备的电池性能最优, 其能量转化效率达到2.32%, 这可归因于其适宜的禁带宽度、结晶质量和良好的PbS/TiO₂界面能级匹配度。     

Resonant infrared matrix-assisted pulsed laser evaporation of CdSe colloidal quantum dot/poly[2-methoxy-5-(2′-ethylhexyloxy)-1,4-(1-cyano vinylene)phenylene] hybrid nanocomposite thin films

CdSe colloidal quantum dot / poly[2-methoxy-5-(2′-ethylhexyloxy)-1,4-(1-cyano vinylene)phenylene] hybrid nanocomposite thin films were deposited using resonant infrared matrix-assisted pulsed laser evaporation. The distributions of CdSe colloidal quantum dots within the polymer matrices of as-grown films were evaluated using transmission electron microscopy, and the optical properties of these films were determined by photoluminescence spectroscopy. These measurements demonstrate that: i) depending upon the deposition parameters used, the CdSe colloidal quantum dot distribution can be tuned between two morphology extremes, i.e. clustering or homogenous dispersion; and ii) the constituent materials of the nanocomposite are not damaged in any way that affects structural or optical properties by the deposition process. The demonstrated ability to control nanoparticle distribution within organic films has not been achieved by other deposition techniques and could enhance the performance of optoelectronic devices based on these materials.     

MoS2–HgTe Quantum Dot Hybrid Photodetectors beyond 2 µm

Mercury telluride (HgTe) colloidal quantum dots (CQDs) have been developed as promising materials for the short and mid‐wave infrared photodetection applications because of their low cost, solution processing, and size tunable absorption in the short wave and mid‐infrared spectrum. However, the low mobility and poor photogain have limited the responsivity of HgTe CQD‐based photodetectors to only tens of mA W^?1. Here, HgTe CQDs are integrated on a TiO₂ encapsulated MoS₂ transistor channel to form hybrid phototransistors with high responsivity of ≈10⁶ A W^?1, the highest reported to date for HgTe QDs. By operating the phototransistor in the depletion regime enabled by the gate modulated current of MoS₂, the noise current is significantly suppressed, leading to an experimentally measured specific detectivity D* of ≈10¹² Jones at a wavelength of 2 µm. This work demonstrates for the first time the potential of the hybrid 2D/QD detector technology in reaching out to wavelengths beyond 2 µm with compelling sensitivity.     

Nanostructure assembly of indium sulphide quantum dots and their characterization

Nanocrystals (approximately 5 nm) of the semiconducting wide band gap material beta-In2S3 obtained by chemical synthesis through a hydrothermal route were characterized for phase and compositional purity. These nanoparticles exhibited quantum confinement characteristics as revealed by a blue-shifted optical absorption. These quantum dots of beta-In2S3 were electrically driven from a monodisperse colloidal suspension on to conducting glass substrates by Electophoretic Deposition (EPD) technique and nanostructural thin films were obtained. The crystalline and morphological structures of these deposits were investigated by X-ray diffraction and nanoscopic techniques. We report here that certain interesting nanostructural morphologies were observed in the two-dimensional quantum dot assemblies of beta-In2S3. The effect of the controlling parameters on the cluster growth and deposit integrity was also systematically studied through a series of experiments and the results are reported here.     

Electric field assisted growth of self-organized CdS films: size dependent structural and optical properties

This paper presents a systematic study of electric field assisted growth of self-organized cadmium sulphide (CdS) quantum dots (Q-CdS). CdS thin films of self-organized quantum dot like structure with different particle size have been successfully deposited simply by varying the concentration of surfactant in the reaction matrix. The model to describe the self-organization is also discussed. The size of CdS nanoparticles can be altered from 68 nm (corresponding to bulk) to 2 nm. The structural, optical, and morphological properties of Q-CdS films have been investigated. A blue shift has been observed in optical absorption and photoluminescence spectra. The strained growth of Q-CdS films has been observed. The microstructural strain calculated from peak broadening reveals an increase in strain with decreasing particle size. This study may provide a convenient method to deposit size selective and organized nanocrystalline semiconductor thin films.     

Bias-induced photoluminescence quenching of single colloidal quantum dots embedded in organic semiconductors

We demonstrate reversible quenching of the photoluminescence from single CdSe/ZnS colloidal quantum dots embedded in thin films of the molecular organic semiconductor N,N'-diphenyl-N,N'-bis(3-methylphenyl)-(1,1'-biphenyl)-4,4'-diamine (TPD) in a layered device structure. Our analysis, based on current and charge carrier density, points toward field ionization as the dominant photoluminescence quenching mechanism. Blinking traces from individual quantum dots reveal that the photoluminescence amplitude decreases continuously as a function of increasing forward bias even at the single quantum dot level. In addition, we show that quantum dot photoluminescence is quenched by aluminum tris(8-hydroxyquinoline) (Alq3) in chloroform solutions as well as in thin solid films of Alq3 whereas TPD has little effect. This highlights the importance of chemical compatibility between semiconductor nanocrystals and surrounding organic semiconductors. Our study helps elucidate elementary interactions between quantum dots and organic semiconductors, knowledge needed for designing efficient quantum dot organic optoelectronic devices.     

Interplay of confinement, strain, and piezoelectric effects in the optical spectrum of GaN quantum dots

We theoretically investigated excitonic states, energy and oscillator strength of optical transitions in GaN quantum dots characterized by different size, shape, interface, and substrate. On the basis of our multi-band model we determined that the piezoelectric field-induced red shift of the ground state transition, observed in recent experiments, can manifest itself only in strained GaN/AIN dots with the dot height larger than 3 nm. It was also established that the oscillator strength of the red-shifted transitions is small (< 0.05) and decreases fast with increasing the dot size, while the strength of ground state transitions in c-GaN/c-AIN and GaN/dielectric dots is large (approximately 0.4-0.7) and almost independent of the dot size.     

Lateral patterning of multilayer InAs/GaAs(001) quantum dot structures by in vacuo focused ion beam

We report on the effects of patterning and layering on multilayer InAs/GaAs(001) quantum dot structures laterally ordered using an in vacuo focused ion beam. The patterned hole size and lateral pattern spacing affected the quantum dot size and the fidelity of the quantum dots with respect to the lateral patterns. 100% pattern fidelity was retained after six layers of dots for a 9.0 ms focused ion beam dwell time and 2.0 μm lateral pattern spacing. Analysis of the change in quantum dot size as a function of pattern spacing provided a means of estimating the maximum average adatom surface diffusion length to be approximately 500 nm, and demonstrated the ability to alter the wetting layer thickness via pattern spacing. Increasing the number of layers from six to 26 resulted in mound formation, which destroyed the pattern fidelity at close pattern spacings and led to a bimodal quantum dot size distribution as measured by atomic force microscopy. The bimodal size distribution also affected the optical properties of the dots, causing a split quantum dot photoluminescence peak where the separation between the split peaks increased with increasing pattern spacing.     

Layer-by-layer assembly of multicolored semiconductor quantum dots towards efficient blue, green, red and full color optical films

Multicolored semiconductor quantum dots have shown great promise for construction of miniaturized light-emitting diodes with compact size, low weight and cost, and high luminescent efficiency. The unique size-dependent luminescent property of quantum dots offers the feasibility of constructing single-color or full-color output light-emitting diodes with one type of material. In this paper, we have demonstrated the facile fabrication of blue-, green-, red-?and full-color-emitting semiconductor quantum dot optical films via a layer-by-layer assembly technique. The optical films were constructed by alternative deposition of different colored quantum dots with a series of oppositely charged species, in particular, the new use of cationic starch on glass substrates. Semiconductor ZnSe quantum dots exhibiting blue emission were deposited for fabrication of blue-emitting optical films, while semiconductor CdTe quantum dots with green and red emission were utilized for construction of green-?and red-emitting optical films. The assembly of integrated blue, green and red semiconductor quantum dots resulted in full-color-emitting optical films. The luminescent optical films showed very bright emitting colors under UV irradiation, and displayed dense, smooth and efficient luminous features, showing brighter luminescence in comparison with their corresponding quantum dot aqueous colloid solutions. The assembled optical films provide the prospect of miniaturized light-emitting-diode applications.     

Multispectral and Circular Polarization-Sensitive Carbon Dot-Polydiacetylene Capacitive Photodetector (Small 31/2023)

Multispectral photodetectors (MSPs) and circularly polarized light (CPL) sensors are important in opto-electronics, photonics, and imaging. A capacitive photodetector consisting of an interdigitated electrode coated with carbon dot/anthraquinone-polydiacetylene is constructed. Photoexcitation of the carbon dots induces transient electron transfer to the anthraquinone moieties, and concomitant change in the film dielectric constant and recorded capacitance. This unique photodetection mechanism furnishes wavelength selectivity that is solely determined by the absorbance of the carbon dots incorporated in the anthraquinone-polydiacetylene matrix. Accordingly, employing an array of polymerized-anthraquinone photodetector films comprising carbon dots (C-dots) exhibiting different excitation wavelengths yielded optical “capacitive fingerprints” in a broad spectral range (350–650 nm). Furthermore, circular light polarization selectivity is achieved through chiral polymerization of the polydiacetylene framework. The carbon dot/anthraquinone-polydiacetylene capacitive photodetector features rapid photo-response, high fidelity, and recyclability as the redox reactions of anthraquinone are fully reversible. The carbon dot/anthraquinone-polydiacetylene platform is inexpensive, easy to fabricate, and consists of environmentally friendly materials.     

Nanoscale patterning of colloidal quantum dots on transparent and metallic planar surfaces

The patterning of colloidal quantum dots with nanometer resolution is essential for their application in photonics and plasmonics. Several patterning approaches, such as the use of polymer composites, molecular lock-and-key methods, inkjet printing and microcontact printing of quantum dots have been recently developed. Herein, we present a simple method of patterning colloidal quantum dots for photonic nanostructures such as straight lines, rings and dot patterns either on transparent or metallic substrates. Sub-10?nm width of the patterned line could be achieved with a well-defined sidewall profile. Using this method, we demonstrate a surface plasmon launcher from a quantum dot cluster in the visible spectrum.     

Photoluminescence imaging of focused ion beam induced individual quantum dots

We report on scanning microphotoluminescence measurements that spectrally and spatially resolve emission from individual InAs quantum dots that were induced by focused ion beam patterning. Multilayers of quantum dots were spaced 2 μm apart, with a minimum single dot emission line width of 160 μeV, indicating good optical quality for dots patterned using this technique. Mapping 16 array sites, at least 65% were occupied by optically active dots and the spectral inhomogeneity was within 30 meV.     

Investigations on the morphology,optical and photoresponse properties of PbS/CdS binary colloidal quantum dot thin film

Binary thin film exhibits not only the quantum features of the individual building blocks but also novel collective properties through coupling of colloidal quantum dot components. In this paper, lead sulfide (PbS) and cadmium sulfide (CdS) colloidal quantum dots (CQDs) were synthesized by using oleate and oleylamine as ligand. The as-synthesized PbS and CdS CQDs were monodispersity and well passivation. The average diameter of as-synthesized PbS and CdS CQDs were about 3 nm and 6 nm, respectively. By blending PbS with CdS CQDs and utilizing ethanedithiol for ligand passivation, the responsivity and detectivity of PbS CQDs thin film was enhanced with the weight ratio of CdS CQDs increased, the optimum responsivity and detectivity were 21.9 mA/W and 2.1 × 10¹⁰ Jones, respectively. The desirable properties of binary colloidal quantum dot thin films have important applications in future electronic and optoelectronic devices.     

CdS quantum dot sensitized nanocrystalline Gd-doped TiO2 thin films for photoelectrochemical solar cells

CdS quantum dot sensitized Gd-doped TiO₂ nanocrystalline thin films have been prepared by chemical method. X-ray diffraction analysis reveals that TiO₂ and Gd-doped TiO₂ nanocrystalline thin films are of anatase phase. The absorption spectra revealed that the absorption edge of CdS quantum dot sensitized Gd-doped TiO₂ thin films shifted towards longer wavelength side (red shift) when compared to that of CdS quantum dot sensitized TiO₂ films. CdS quantum dots with a size of 5 nm have been deposited onto Gd-doped TiO₂ film surface by successive ionic layer adsorption and reaction method and the assembly of CdS quantum dot with Gd-doped TiO₂ has been used as photo-electrode in quantum dot sensitized solar cells. CdS quantum dot sensitized Gd-doped TiO₂ based solar cell exhibited a power conversion efficiency of 1.18 %, which is higher than that of CdS quantum dot sensitized TiO₂ (0.91 %).     

Multiple exciton generation in films of electronically coupled PbSe quantum dots

We study multiple exciton generation (MEG) in electronically coupled films of PbSe quantum dots (QDs) employing ultrafast time-resolved transient absorption spectroscopy. We demonstrate that the MEG efficiency in PbSe does not decrease when the QDs are treated with hydrazine, which has been shown to greatly enhance carrier transport in PbSe QD films by decreasing the interdot distance. The quantum yield is measured and compared to previously reported values for electronically isolated QDs suspended in organic solvents at approximately 4 and 4.5 times the effective band gap. A slightly modified analysis is applied to extract the MEG efficiency and the absorption cross section of each sample at the pump wavelength. We compare the absorption cross sections of our samples to that of bulk PbSe. We find that both the biexciton lifetime and the absorption cross section increase in films relative to isolated QDs in solution.     

Highly efficient resonant coupling of optical excitations in hybrid organic/inorganic semiconductor nanostructures

The integration of organic and inorganic semiconductors on the nanoscale offers the possibility of developing new photonic devices that combine the best features of these two distinct classes of material. Such devices could, for example, benefit from the large oscillator strengths found in organic materials and the nonlinear optical properties of inorganic species. Here we describe a novel hybrid organic/inorganic nanocomposite in which alternating monolayers of J-aggregates of cyanine dye and crystalline semiconductor quantum dots are grown by a layer-by-layer self-assembly technique. We demonstrate near-field photon-mediated coupling of vastly dissimilar optical excitations in the two materials that can reach efficiencies of up to 98% at room temperature. By varying the size of the quantum dots and thus tuning their optical resonance for absorption and emission, we also show how the ability of J-aggregates to harvest light can be harnessed to increase the effective absorption cross section of the quantum dots by up to a factor of ten. Combining organic and inorganic semiconductors in this way could lead to novel nanoscale designs for light-emitting, photovoltaic and sensor applications.     

Enhanced 400-600 nm photoresponsivity of metal-oxide-semiconductor diodes with multi-stack germanium quantum dots

Metal-oxide-semiconductor (MOS) diodes with zero-, one-?or three-layer Ge quantum dots (QDs) embedded in the gate oxide are fabricated for visible to near-ultraviolet photodetection. Ge dots are formed by thermally oxidizing one or three stacks of amorphous Si (a-Si)/polycrystalline-Si(0.87)Ge(0.13)/a-Si multi-layers that are sandwiched by SiO(2) barriers. The current-voltage characteristics of Ge QD MOS diodes exhibit strong rectification in darkness and feature significant current enhancement in the inversion mode when illuminated. Increasing the number of Ge QD layers from zero through one to three in the gate oxide improves the responsivity from 4.64 through 482 to 812?mA?W(-1) and enhances the corresponding quantum efficiency from 1.42 through 148 to 245%, respectively. The spectral response reveals a considerable blueshift in peak energies as the Ge dot size decreases from 9.1 to 5.1?nm, suggesting that the light absorption originates from the quantum confinement effect of Ge QDs. The temperature and bias dependences of the dark current indicate that the carrier transport mechanism involves percolation hopping.     

Bright infrared quantum-dot light-emitting diodes through inter-dot spacing control

Infrared light-emitting diodes are currently fabricated from direct-gap semiconductors using epitaxy, which makes them expensive and difficult to integrate with other materials. Light-emitting diodes based on colloidal semiconductor quantum dots, on the other hand, can be solution-processed at low cost, and can be directly integrated with silicon. However, so far, exciton dissociation and recombination have not been well controlled in these devices, and this has limited their performance. Here, by tuning the distance between adjacent PbS quantum dots, we fabricate thin-film quantum-dot light-emitting diodes that operate at infrared wavelengths with radiances (6.4?W?sr(-1)?m(-2)) eight times higher and external quantum efficiencies (2.0%) two times higher than the highest values previously reported. The distance between adjacent dots is tuned over a range of 1.3?nm by varying the lengths of the linker molecules from three to eight CH(2) groups, which allows us to achieve the optimum balance between charge injection and radiative exciton recombination. The electroluminescent powers of the best devices are comparable to those produced by commercial InGaAsP light-emitting diodes. By varying the size of the quantum dots, we can tune the emission wavelengths between 800 and 1,850?nm.