Biexciton properties strongly affect the usability of a light emitter in quantum photon sources and lasers but are difficult to measure for single fluorophores at room temperature due to luminescence intermittency and bleaching at the high excitation fluences usually required. Here, we observe the biexciton (BX) to exciton (X) to ground photoluminescence cascade of single colloidal semiconductor nanocrystals (NCs) under weak excitation in a g((2)) photon correlation measurement and show that the normalized amplitude of the cascade feature is equal to the ratio of the BX to X fluorescence quantum yields. This imposes a limit on the attainable depth of photon antibunching and provides a robust means to study single emitter biexciton physics. In NC samples, we show that the BX quantum yield is considerably inhomogeneous, consistent with the defect sensitivity expected of the Auger nonradiative recombination mechanism. The method can be extended to study X,BX spectral and polarization correlations.
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http://dx.doi.org/10.1021/nl104054t | DOI Listing |
Magn Reson Chem
January 2025
Laboratório de Química Computacional e Modelagem Molecular (LQC-MM), Departamento de Química Inorgânica, Instituto de Química, Universidade Federal Fluminense (UFF), Niterói, Rio de Janeiro, Brazil.
We present a DFT-PCM NMR study of 3-indoleacetic acid (3-IAA), used as a working example, including explicit solvent molecules, named PCM-nCHCl, PCM-nDMSO (n = 0, 2, 4, 8, 14, 20, and 25), to investigate the dimer formation in solution. Apart from well-known cyclic (I) and open (II) acetic acid (AA) dimers, two new structures were located on DFT-PCM potential energy surface (PES) for 3-IAA named quasicyclic A (III) and quasicyclic B (IV), the last one having N-H…O hydrogen bond (instead of O-H…O). In addition, four other structures having π-π type interactions named V, VI, VII, and VIII were also obtained completing the sample on the PES.
View Article and Find Full Text PDFChemSusChem
January 2025
CSIR Central Glass & Ceramic Research Institute, EMDD, 196 Raja S C Mullick Road, 700032, Kolkata, INDIA.
The advancement of photocatalytic technology for solar-driven hydrogen (H2) production remains hindered by several challenges in developing efficient photocatalysts. A key issue is the rapid recombination of charge carriers, which significantly limits the light-harvesting ability of materials like BiOCl and Cu2SnS3 quantum dots (CTS QDs), despite the faster charge mobility and quantum confinement effect, respectively. Herein, a BiOCl/CTS (BCTS) heterostructure was synthesized by loading CTS QDs onto BiOCl 2D nanosheets (NSs), that demonstrated excellent photocatalytic activity under visible light irradiation.
View Article and Find Full Text PDFJ Colloid Interface Sci
January 2025
State Key Laboratory of Bio-Fibers and Eco-Textiles, Qingdao University, No. 308 Ningxia Road, Qingdao 266071 PR China. Electronic address:
Luminescent solar concentrators (LSCs) are large scale sunlight collector and can be used for building-integrated photovoltaics (BIPV). Achieving high-performance LSCs requires fluorophores with broad absorption, high quantum yield and a large Stokes shift. Nevertheless, conventional high-efficiency LSCs typically rely on heavy metal-based quantum dots as fluorophores.
View Article and Find Full Text PDFJ Phys Chem A
January 2025
Department of Chemistry and Supercomputing Institute, University of Minnesota, Minneapolis, Minnesota 55455-0431, United States.
The energy gaps, spin-orbit coupling (SOC), and admixture coefficients over a series of the configurations are evaluated by the SA-CASSCF/6-31G, SA-CASSCF/6-31G*, SA-CASSCF/ANO-RCC-VDZP, and MS-CASPT2/ANO-RCC-VDZP to reveal the extent of the inaccuracy of the SA-CASSCF. By comparing the mean absolute errors for the energy gaps and the admixture coefficient magnitudes (ACMs) measured between the SA-CASSCF/6-31G, SA-CASSCF/6-31G*, or SA-CASSCF/ANO-RCC-VDZP and the MS-CASPT2/ANO-RCC-VDZP, the SA-CASSCF/6-31G is selected as the electronic structure method in the nonadiabatic molecular dynamics simulation. The major components of the ACMs of the SA-CASSCF/6-31G and MS-CASPT2/ANO-RCC-VDZP are identified and compared; we find that the ACMs are underestimated by the SA-CASSCF/6-31G, which is verified by the reasonable triplet quantum yield simulated by the trajectory surface hopping and the calibrated SA-CASSCF/6-31G.
View Article and Find Full Text PDFSci Bull (Beijing)
January 2025
Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, China; Macao Institute of Materials Science and Engineering (MIMSE), MUST-SUDA Joint Research Center for Advanced Functional Materials, Zhuhai MUST Science and Technology Research Institute, Macau University of Science and Technology, Macao 999078, China; Institute of Organic Optoelectronics (IOO), Jiangsu Industrial Technology Research Institute (JITRI), Suzhou 215200, China. Electronic address:
High-quality quantum dots (QDs) possess superior electroluminescent efficiencies and ultra-narrow emission linewidths are essential for realizing ultra-high definition QD light-emitting diodes (QLEDs). However, the synthesis of such QDs remains challenging. In this study, we present a facile high-temperature successive ion layer adsorption and reaction (HT-SILAR) strategy for the growth of precisely tailored ZnCdSe/ZnSe shells, and the consequent production of high-quality, large-particle, alloyed red CdZnSe/ZnCdSe/ZnSe/ZnS/CdZnS QDs.
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