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Engineering Directionality in Quantum Dot Shell Lasing Using Plasmonic Lattices
摘要： We report how the direction of quantum dot (QD) lasing can be engineered by exploiting high-symmetry points in plasmonic nanoparticle (NP) lattices. The nanolaser architecture consists of CdSe?CdS core?shell QD layers conformally coated on two-dimensional square arrays of Ag NPs. Using waveguide-surface lattice resonances (W-SLRs) near the Δ point in the Brillouin zone as optical feedback, we achieved lasing from the gain in CdS shells at off-normal emission angles. Changing the periodicity of the plasmonic lattices enables other high-symmetry points (Γ or M) of the lattice to overlap with the QD shell emission, which facilitates tuning of the lasing direction. We also increased the thickness of the QD layer to introduce higher-order W-SLR modes with additional avoided crossings in the band structure, which expands the selection of cavity modes for any desired lasing emission angle.
关键词： band structure engineering,laser directionality,surface lattice resonances,colloidal quantum dots,lattice plasmons,waveguide
更新于2025-09-16 10:30:52
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Acquisition of Hyperspectral Data with Colloidal Quantum Dots
摘要： Hyperspectral sensors, combining the functions of photon detection with ultrahigh spectral resolution in a single device, have emerged as a new class of devices with significant potential for applications that rely on the input of optical information. Despite continued advancement, the widespread use of infrared hyperspectral sensors is still limited primarily due to the high cost associated with the growth and processing of epitaxial semiconductors, such as HgCdTe, InSb, and superlattices. Here, it is shown that colloidal quantum dots (CQDs) provide a promising route toward low-cost, compact, and sensitive infrared hyperspectral sensors with tunable sensing ranges. In total, 64 narrowband channels with full-width at half-maxima down to ≈30 cm?1 can be realized by directly integrating CQDs sensors with a distributed Bragg mirror filter array. The results of high-resolution spectra measurement with resolving power up to 180 and acquisition of a hyperspectral image cube in the short-wave infrared range, benefiting from the fast (≈120 ns) and sensitive (>1010 Jones) performance of the CQDs sensors, are experimentally demonstrated.
关键词： colloidal quantum dots,Fabry–Perot filters,hyperspectral sensors,infrared detectors
更新于2025-09-12 10:27:22
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Dielectric response function for colloidal semiconductor quantum dots
摘要： We calculate the optical properties of InP and CdSe colloidal quantum dots (QDs) within the framework of the atomic effective pseudopotential approach and the screened configuration interaction theory. We obtain an excellent agreement with experiment with our microscopic and space-dependent screening function where the dielectric constant varies in real space with a sharp transition (width of ≈0.18 nm) from the QD material high-frequency bulk value inside the QD to the solvent or passivant high-frequency value outside. We obtain a reasonable agreement (with deviations less than 140 meV) for a computationally less demanding solvent-independent screening using the full high-frequency bulk screening, in contrast to the more commonly used reduced QD radius-dependent screening constant. We show theoretically that for QDs passivated with long-chained organic molecules, the influence of the solvent on the optical gap is in the range of 10 meV, while QDs passivated with short ligands can experience shifts in the order of 100 meV. Experiments on CdSe QDs passivated with octadecylphosphonic acid (ODPA, long-chained ligand) in two different solvents (toluene and chloroform) confirm the bandgap dependence. While the optical gap is weakly affected by the environment, the quasiparticle gap and the exciton binding energy show a strong environmental dependence. Finally, we show that the optical bandgap does not depend significantly on the crystal structure (wurtzite or zincblende) or the morphological details (faceted or “spherical” shape).
关键词： optical properties,dielectric response function,screened configuration interaction theory,pseudopotential approach,colloidal quantum dots
更新于2025-09-12 10:27:22
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Ultrafast hole extraction from photoexcited colloidal CdSe quantum dots coupled to nitroxide free radicals
摘要： Organic free radicals related to the 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) radical are known as photoluminescence-quenchers when coupled to group II-chalcogenide colloidal quantum dots (QDs), but the mechanism responsible for this phenomenon has so far remained unresolved. Using a combination of time-resolved photoluminescence and transient absorption spectroscopies, we demonstrate that photoexcited colloidal CdSe QDs coupled to 4-amino-TEMPO undergo highly efficient reductive quenching, that is, hole transfer from the valence band of the quantum dot to the organic paramagnetic species. Interestingly, the process is shown to occur on a subpicosecond time scale for bound 4AT; such a large rate constant for the extraction of holes from photoexcited CdSe QD by a molecular species is rare and underlines the potential that TEMPO derivatives can play in mediating efficient redox processes involving colloidal CdSe QDs.
关键词： TEMPO,photoluminescence quenching,ultrafast spectroscopy,colloidal quantum dots,hole transfer
更新于2025-09-12 10:27:22
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Machine Learning Accelerates Discovery of Optimal Colloidal Quantum Dot Synthesis
摘要： Colloidal quantum dots (CQDs) allow broad tuning of the bandgap across the visible and near-infrared spectral regions. Recent advances in applying CQDs in light sensing, photovoltaics, and light emission have heightened interest in achieving further synthetic improvements. In particular, improving monodispersity remains a key priority in order to improve solar cells’ open-circuit voltage, decrease lasing thresholds, and improve photodetectors’ noise-equivalent power. Here we utilize machine-learning-in-the-loop to learn from available experimental data, propose experimental parameters to try, and, ultimately, point to regions of synthetic parameter space that will enable record-monodispersity PbS quantum dots. The resultant studies reveal that adding a growth-slowing precursor (oleylamine) allows nucleation to prevail over growth, a strategy that enables record-large-bandgap (611 nm exciton) PbS nanoparticles with a well-defined excitonic absorption peak (half width at half max (HWHM) of 145 meV). At longer wavelengths, we also achieve improved monodispersity, with HWHM of 55 meV at 950 nm and 24 meV at 1500 nm, compared to the best published to date values of 75 meV and 26 meV, respectively.
关键词： machine learning,PbS,Bayesian optimization,synthesis,nanocrystals,colloidal quantum dots
更新于2025-09-12 10:27:22
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All-solution-processed UV-IR broadband trilayer photodetectors with CsPbBr3 colloidal nanocrystals as carriers-extracting layer
摘要： Colloidal quantum dots (CQDs) are very promising nanomaterials for optoelectronics due to their tunable bandgap and quantum confinement effect. Especially, all-inorganic CsPbX3 (X=Br, Cl and I) perovskite nanocrystals (NCs) have attracted enormous interests owing to their promising and exciting applications in photovoltaic devices. In this paper, all-solution-processed broadband photodetectors ITO/ZnO/CsPbBr3/PbS/Au with high-performance were presented. The role of CsPbBr3 QDs layer as the carriers-extracting layer in the trilayer devices was discussed. As compared with bilayer device ITO/ZnO/PbS/Au, both the dark currents and photocurrents under illumination from UV-IR broadband trilayer photodetector ITO/ZnO(80nm)/PbS(150nm)/CsPbBr3(50nm)/Au are enhanced, but the trilayer photodetector ITO/ZnO(80nm)/CsPbBr3(50nm)/PbS(150nm)/Au showed a maximum specific detectivity (D*) of 1.73×1012 Jones with a responsivity (R) of 5.31 A/W under 6.8 mW/cm2 405 nm illumination. However, another trilayer photodetector ITO/ZnO(80nm)/PbS(150nm)/CsPbBr3(50nm)/Au showed a maximum D* of 8.3×1012 Jones with a R of 35 A/W under 1.6 mW/cm2 980 nm illumination. Further, the underlying mechanism for the enhanced performance of trilayer photodetectors was discussed. Thus, this strategy of all-solution-processed heterojunction configuration paves a facile way for broadband photodetectors with high-performance.
关键词： broadband photodetectors,all-solution-processed heterojunction,Colloidal quantum dots (CQDs),CsPbBr3 perovskite nanocrystals,carrier-extraction layer
更新于2025-09-12 10:27:22
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Contribution of electron-phonon coupling to the luminescence spectra of single colloidal quantum dots
摘要： Luminescence spectroscopy experiments were realized for single colloidal quantum dots CdSe/ZnS in a broad temperature range above room temperature in a nitrogen atmosphere. Broadening and shifts of spectra due to the temperature change as well as due to spectral diffusion processes were detected and analyzed. A linear correlation between the positions of maxima and the squared linewidths of the spectra was found. This dependence was explained by a model that takes into account the slow variation of the electron-phonon coupling strength.
关键词： temperature dependence,spectral diffusion,luminescence spectroscopy,electron-phonon coupling,colloidal quantum dots
更新于2025-09-12 10:27:22
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Stable Colloidal Quantum Dot Inks Enable Inkjet-Printed High-Sensitivity Infrared Photodetectors
摘要： Colloidal Quantum Dots (CQDs) have recently gained attention as materials for manufacturing optoelectronic devices in view of their tunable light absorption and emission properties and compatibility with low-temperature thin-film manufacture. The realization of CQD inkjet-printed infrared photodetectors has thus far been hindered by incompatibility between the chemical processes that produce state-of-art CQD solution-exchanged inks; and the requirements of ink formulations for inkjet materials processing. To achieve inkjet-printed CQD solids with a high degree of reproducibility, as well as with the needed morphological and optoelectronic characteristics, we sought to overcome the mismatch among these processing conditions. In this study, we design CQD inks by simultaneous evaluation of requirements regarding ink colloidal stability, jetting conditions and film morphology for different dots and solvents. The new inks remain colloidally stable, achieved through a design that suppresses the reductant properties of amines on the dots’ surface. After drop ejection from the nozzle, the quantum dot material is immobilized on the substrate surface due to the rapid evaporation of the low boiling point amine-based compound. Concurrently, the high boiling point solvent allows for the formation of a thin film of high uniformity, as is required for the fabrication of high-performance IR photodetectors. We fabricate inkjet-printed photodetectors exhibiting the highest specific detectivities reported to date (above 1012 Jones across the IR) in an inkjet-printed quantum dot film. As a patternable CMOS-compatible process, the work offers routes to integrated sensing devices and systems.
关键词： CQD,infrared,printing,ink-jet,inkjet,colloidal quantum dots,photodetectors
更新于2025-09-12 10:27:22
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Simultaneous Existence of Confined and Delocalized Vibrational Modes in Colloidal Quantum Dots
摘要： Coupling to phonon modes is a primary mechanism of excitonic dephasing and energy loss in semiconductors. However, low-energy phonons in colloidal quantum dots and their coupling to excitons are poorly understood, since their experimental signatures are weak and usually obscured by unavoidable inhomogeneous broadening of colloidal dot ensembles. We use multi-dimensional coherent spectroscopy at cryogenic temperatures to extract the homogeneous nonlinear optical response of excitons in a CdSe/CdZnS core/shell colloidal quantum dot ensemble. Comparison to simulation provides evidence that the observed lineshapes arise from the co-existence of confined and delocalized vibrational modes, both of which couple strongly to excitons in CdSe/CdZnS colloidal quantum dots.
关键词： multi-dimensional coherent spectroscopy,exciton,colloidal quantum dots,CdSe/CdZnS,phonon modes
更新于2025-09-12 10:27:22
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Anomalous Stokes shift of colloidal quantum dots and their influence on solar cell performance
摘要： We report an anomalous Stokes shift effect observed in colloidal solutions containing down-shifting Carbon quantum dots (CQDs) of different sizes that is expected to have a positive in?uence on the power conversion ef?ciency of photovoltaic structures. Speci?cally, with an excitation wavelength of 390 nm, individual colloidal solutions of CQDs whose diameter was determined by the applied current during synthesis, exhibited photoluminescent (PL) emission wavelength peaks centered at 420 nm. However, the colloidal solution comprising the mixture of all the previously synthesized CQDs of different diameters was observed to have an anomalous PL Stokes shift centered at 515 nm. Furthermore, the afore-mentioned anomalous SSE was also observed in CdTe QDs when added to the CQD mixed-solution (CMS). Thus, whereas a mixture of CdTe QDs of different sizes, exhibited a down-shifted photoluminescence centered at 555 nm, the peak was observed to have an anomalous Stokes shift centered at 580 nm when combined with the CMS. Quantum dot characterization included crystal structure analysis as well as photon absorption and photoluminescence wavelengths. Subsequently, the synthesized QDs were dispersed in a polymeric layer of PMMA and incorporated on functional and previously characterized solar cells, to quantify their in?uence in the electrical performance of the photovoltaic devices. The observations indicate an improvement in the PCE of 4.6% when incorporating Carbon QDs, 2.9% with CdTe QDs and 4.8% when employing both C and CdTe QDs.
关键词： solar cell performance,photoluminescence,Carbon quantum dots,Anomalous Stokes shift,colloidal quantum dots,CdTe quantum dots,power conversion efficiency
更新于2025-09-11 14:15:04