Time-Correlated Single-Photon Counting (TCSPC) is an excellent technique used in a great variety of scientific experiments to acquire exceptionally fast and faint light signals. Above all, in Fluorescence Lifetime Imaging (FLIM), it is widely recognized as the gold standard to record sub-nanosecond transient phenomena with picosecond precision. Unfortunately, TCSPC has an intrinsic limitation: to avoid the so-called pile-up distortion, the experiments have been historically carried out, limiting the acquisition rate below 5% of the excitation frequency. In 2017, we demonstrated that such a limitation can be overcome if the detector dead time is exactly matched with the excitation period, thus paving the way to unprecedented speedup of FLIM measurements. In this paper, we present the first single-channel system that implements the novel proposed methodology to be used in modern TCSPC experimental setups. To achieve this goal, we designed a compact detection head, including a custom single-photon avalanche diode externally driven by a fully integrated Active Quenching Circuit (AQC), featuring a finely tunable dead time and a short reset time. The output timing signal is extracted by using a picosecond precision Pick-Up Circuit (PUC) and fed to a newly developed timing module consisting of a mixed-architecture Fast Time to Amplitude Converter (F-TAC) followed by high-performance Analog-to-Digital Converters (ADCs). Data are transmitted in real-time to a Personal Computer (PC) at USB 3.0 rate for specific and custom elaboration. Preliminary experimental results show that the new TCSPC system is suitable for implementing the proposed technique, achieving, indeed, high timing precision along with a count rate as high as 40 Mcps.
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J Phys Chem A
January 2025
Advanced Membranes and Porous Materials Center, Division of Physical Science and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900, Kingdom of Saudi Arabia.
Understanding how structural modifications affect the photophysics of organic linkers is crucial for their integration into metal-organic frameworks (MOFs) for light-driven applications. This study explores the impact of varying the amine functional group position on two terephthalic acid derivatives─linker and linker ─by investigating their photophysics through a combination of steady-state and ultrafast laser spectroscopy and time-dependent density functional theory (TD-DFT) calculations. With tetrahydrofuran as the solvent, time-correlated single-photon counting revealed a 2-fold increase in the S excited-state lifetime of the molecule with the amine group at the meta position compared with that of the molecule with the amine group at the ortho position.
View Article and Find Full Text PDFAdv Sci (Weinh)
January 2025
Institute of Molecular Science, University of Valencia, c/Catedrático José Beltrán Martínez 2, Paterna, 46980, Valencia, Spain.
Energy transfer processes in nanohybrids are at the focal point of conceptualizing, designing, and realizing novel energy-harvesting systems featuring nanocrystals that absorb photons and transfer their energy unidirectionally to surface-immobilized functional dyes. Importantly, the functionality of these dyes defines the ultimate application. Herein, CsPbBr perovskite nanocrystals (NCs) are interfaced with zinc phthalocyanine (ZnPc) dyes featuring carboxylic acid.
View Article and Find Full Text PDFJ Phys Chem A
January 2025
Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, United States.
Time-resolved single molecule localization microscopy (TR-SMLM) with a 2 × 2 pixel fiber optic array camera was combined with time-correlated single photon counting (TCSPC) to obtain super-resolved fluorescence lifetime images of individual Cy3 dye molecules and individual colloidal CdSe/CdS/ZnS core/shell/shell semiconductor quantum dots (QDs). The characteristic blinking and bleaching behavior of the Cy3 and the blinking behavior of the QD emitters were used as distinguishing optical characteristics to isolate them and determine their centroid locations with spatial resolution below the optical diffraction limit. TCSPC was used to characterize the fluorescence lifetime and intensity corresponding to each emitter location.
View Article and Find Full Text PDFJ Phys Chem B
January 2025
Surfactant Chemistry Laboratory, Department of Chemistry, The University of Burdwan, Burdwan 713104, West Bengal, India.
The oxidation kinetics of phenylalanine (Phe) by Ce(IV) have been examined in both the absence and presence of aqueous micellar media with asymmetric tails, specifically using sodium dodecyl sulfate (SDS) and sodium tetradecyl sulfate (STS) surfactants. The reaction progress was monitored by observing a decrease in absorbance using UV-vis spectroscopy. Interestingly, the kinetic profile revealed a consistent increase in the observed rate constant values as the concentration of the surfactant increased.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
December 2024
BU-DRDO Center for Life Science, Bharathiar University, Coimbatore 641046, Tamilnadu, India.
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