Singlet exciton fission has the potential to increase the efficiency of crystalline silicon solar cells beyond the conventional single junction limit. Perhaps the largest obstacle to achieving this enhancement is uncertainty about energy coupling mechanisms at the interfaces between silicon and exciton fission materials such as tetracene. Here, the previously reported silicon-hafnium oxynitride-tetracene structure is studied and a combination of magnetic-field-dependent silicon photoluminescence measurements and density functional theory calculations is used to probe the influence of the interlayer composition on the triplet transfer process across the hafnium oxynitride interlayer.
View Article and Find Full Text PDFPreventing ion migration in perovskite photovoltaics is key to achieving stable and efficient devices. The activation energy for ion migration is affected by the chemical environment surrounding the ions. Thus, the migration of organic cations in lead halide perovskites can be mitigated by engineering their local interactions, for example through hydrogen bonding.
View Article and Find Full Text PDFWe introduce a two-step silica-encapsulation procedure to optimize both the optical efficiency and structural robustness of 5,5',6,6'-tetrachloro-1,1'-diethyl-3,3'-di(4-sulfobutyl)-benzimidazolocarbocyanine (TDBC), a two-dimensional sheet-like J-aggregate. We report a fluorescence quantum yield of ∼98%, the highest quantum yield recorded for any J-aggregate structure at room temperature, and a fast, emissive lifetime of 234 ps. Silica, as an encapsulating matrix, provides optical transparency, chemical inertness, and robustness to dilution, while rigidifying the J-aggregate structure.
View Article and Find Full Text PDFThe development of many quantum optical technologies depends on the availability of single quantum emitters with near-perfect coherence. Systematic improvement is limited by a lack of understanding of the microscopic energy flow at the single-emitter level and ultrafast timescales. Here we utilize a combination of fluorescence correlation spectroscopy and ultrafast spectroscopy to capture the sample-averaged dynamics of defects with single-particle sensitivity.
View Article and Find Full Text PDFImposing quantum confinement has the potential to significantly modulate both the structural and optical parameters of interest in many material systems. In this work, we investigate strongly confined ultrathin perovskite nanoplatelets APbBr. We compare the all-inorganic and hybrid compositions with the A-sites cesium and formamidinium, respectively.
View Article and Find Full Text PDFSolid-state single-photon emitters (SPEs) are quantum light sources that combine atomlike optical properties with solid-state integration and fabrication capabilities. SPEs are hindered by spectral diffusion, where the emitter's surrounding environment induces random energy fluctuations. Timescales of spectral diffusion span nanoseconds to minutes and require probing single emitters to remove ensemble averaging.
View Article and Find Full Text PDFScalable fabrication of two-dimensional (2D) arrays of quantum dots (QDs) and quantum rods (QRs) with nanoscale precision is required for numerous device applications. However, self-assembly-based fabrication of such arrays using DNA origami typically suffers from low yield due to inefficient QD and QR DNA functionalization. In addition, it is challenging to organize solution-assembled DNA origami arrays on 2D device substrates while maintaining their structural fidelity.
View Article and Find Full Text PDFChemical bath deposition (CBD) is widely used to deposit tin oxide (SnO ) as an electron-transport layer in perovskite solar cells (PSCs). The conventional recipe uses thioglycolic acid (TGA) to facilitate attachments of SnO particles onto the substrate. However, nonvolatile TGA is reported to harm the operational stability of PSCs.
View Article and Find Full Text PDFQuantum photonic technologies such as quantum communication, sensing or computation require efficient, stable and pure single-photon sources. Epitaxial quantum dots (QDs) have been made capable of on-demand photon generation with high purity, indistinguishability and brightness, although they require precise fabrication and face challenges in scalability. By contrast, colloidal QDs are batch synthesized in solution but typically have broader linewidths, low single-photon purities and unstable emission.
View Article and Find Full Text PDFMany optoelectronic processes in colloidal semiconductor nanocrystals (NCs) suffer an efficiency decline under high-intensity excitation. This issue is caused by Auger recombination of multiple excitons, which converts the NC energy into excess heat, reducing the efficiency and life span of NC-based devices, including photodetectors, X-ray scintillators, lasers, and high-brightness light-emitting diodes (LEDs). Recently, semiconductor quantum shells (QSs) have emerged as a promising NC geometry for the suppression of Auger decay; however, their optoelectronic performance has been hindered by surface-related carrier losses.
View Article and Find Full Text PDFHybrid perovskites have emerged as a promising material candidate for exciton-polariton (polariton) optoelectronics. Thermodynamically, low-threshold Bose-Einstein condensation requires efficient scattering to the polariton energy dispersion minimum, and many applications demand precise control of polariton interactions. Thus far, the primary mechanisms by which polaritons relax in perovskites remains unclear.
View Article and Find Full Text PDFCesium lead halide perovskite nanocrystals (PNCs) have emerged as a potential next-generation single quantum emitter (QE) material for quantum optics and quantum information science. Optical dephasing processes at cryogenic temperatures are critical to the quality of a QE, making a mechanistic understanding of coherence losses of fundamental interest. We use photon-correlation Fourier spectroscopy (PCFS) to obtain a lower bound to the optical coherence times of single PNCs as a function of temperature.
View Article and Find Full Text PDFQuantum confined lead halide perovskite nanoplatelets are anisotropic materials displaying strongly bound excitons with spectrally pure photoluminescence. We report the controlled assembly of CsPbBr nanoplatelets through varying the evaporation rate of the dispersion solvent. We confirm the assembly of superlattices in the face-down and edge-up configurations by electron microscopy, as well as X-ray scattering and diffraction.
View Article and Find Full Text PDFWe demonstrate three general effective strategies to mitigate non-radiative losses in the superradiant emission from supramolecular assemblies. We focus on J-aggregates of 5,5',6,6'-tetrachloro-1,1'-diethyl-3,3'-di(4-sulfobutyl)-benzimidazolocarbocyanine (TDBC) and elucidate the nature of their nonradiative processes. We show that self-annealing at room temperature, photo-brightening, and the purification of the dye monomers all lead to substantial increases in emission quantum yields (QYs) and a concomitant lengthening of the emission lifetime, with purification of the monomers having the largest effect.
View Article and Find Full Text PDFLead halide perovskite nanocrystals (LHP NCs) are an emerging materials system with broad potential applications, including as emitters of quantum light. We apply design principles aimed at the structural optimization of surface ligand species for CsPbBr NCs, leading us to the study of LHP NCs with dicationic quaternary ammonium bromide ligands. Through the selection of linking groups and aliphatic backbones guided by experiments and computational support, we demonstrate consistently narrow photoluminescence line shapes with a full-width-at-half-maximum below 70 meV.
View Article and Find Full Text PDFInP quantum dots (QDs) are the material of choice for QD display applications and have been used as active layers in QD light-emitting diodes (QDLEDs) with high efficiency and color purity. Optimizing the color purity of QDs requires understanding mechanisms of spectral broadening. While ensemble-level broadening can be minimized by synthetic tuning to yield monodisperse QD sizes, single QD line widths are broadened by exciton-phonon scattering and fine-structure splitting.
View Article and Find Full Text PDFDetection of terahertz (THz) radiation has many potential applications, but presently available detectors are limited in many aspects of their performance, including sensitivity, speed, bandwidth and operating temperature. Most do not allow the characterization of THz polarization states. Recent observation of THz-driven luminescence in quantum dots offers a possible detection mechanism via field-driven interdot charge transfer.
View Article and Find Full Text PDFPurpose: The abnormal function of tumor blood vessels causes tissue hypoxia, promoting disease progression and treatment resistance. Although tumor microenvironment normalization strategies can alleviate hypoxia globally, how local oxygen levels change is not known because of the inability to longitudinally assess vascular and interstitial oxygen in tumors with sufficient resolution. Understanding the spatial and temporal heterogeneity should help improve the outcome of various normalization strategies.
View Article and Find Full Text PDFThe continuous and concerted development of colloidal quantum dot light-emitting diodes over the past two decades has established them as a bedrock technology for the next generation of displays. However, a fundamental issue that limits the performance of these devices is the quenching of photoluminescence due to excess charges from conductive charge transport layers. Although device designs have leveraged various workarounds, doing so often comes at the cost of limiting efficient charge injection.
View Article and Find Full Text PDFAuger decay of multiple excitons represents a significant obstacle to photonic applications of semiconductor quantum dots (QDs). This nonradiative process is particularly detrimental to the performance of QD-based electroluminescent and lasing devices. Here, we demonstrate that semiconductor quantum shells with an "inverted" QD geometry inhibit Auger recombination, allowing substantial improvements to their multiexciton characteristics.
View Article and Find Full Text PDFPhotoluminescence intermittency is a ubiquitous phenomenon, reducing the temporal emission intensity stability of single colloidal quantum dots (QDs) and the emission quantum yield of their ensembles. Despite efforts to achieve blinking reduction by chemical engineering of the QD architecture and its environment, blinking still poses barriers to the application of QDs, particularly in single-particle tracking in biology or in single-photon sources. Here, we demonstrate a deterministic all-optical suppression of QD blinking using a compound technique of visible and mid-infrared excitation.
View Article and Find Full Text PDFVolumetric optical imaging of magnetic fields is challenging with existing magneto-optical materials, motivating the search for dyes with strong magnetic field interactions, distinct emission spectra, and an ability to withstand high photon flux and incorporation within samples. Here, the magnetic field effect on singlet-exciton fission is exploited to demonstrate spatial imaging of magnetic fields in a thin film of rubrene. Doping rubrene with the high-quantum yield dye dibenzotetraphenylperiflanthene (DBP) is shown to enable optically pumped, slab waveguide lasing.
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