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Role of Emissive and Non‐Emissive Complex Formations in Photoinduced Electron Transfer Reaction of CdTe Quantum Dots
摘要： Bimolecular photoinduced electron transfer (PET) from excited state CdTe quantum dot (QD*) to an electron deficient molecule 2,4-dinitrotoluene (DNT) is studied in toluene. We observed two types of QD-DNT complex formations; (i) non-emissive complex, in which DNT is embedded deep inside the surface polymer layer of QD and (ii) emissive complex, in which DNT molecules are attached to QDs but approach to the QD core is shielded by polymer layer. Because of its non-emissive nature, the lifetime of QD is not affected by dark complex formation, though the steady-state emission is greatly quenched. However, emissive complex formation causes both, lifetime and steady-state emission quenching. In our fitting model, consideration of Poisson distribution of the attached quencher (DNT) molecules at QD surface enables a comprehensive fitting to our time resolved data. QD-DNT complex formation was confirmed by an isothermal titration calorimetry (ITC) study. Fitting to the time resolved data using a stochastic kinetic model shows moderate increase (0.05 ns(cid:2)1 to 0.072 ns(cid:2)1) of intrinsic quenching rate with increasing the QD particle size (from (cid:3) 3.2 nm to (cid:3) 5.2 nm). Our fitting also reveals that the number of DNT molecules attached to a single QD increases from (cid:3) 0.1–0.2 to (cid:3) 1.2–1.7, as the DNT concentration is increased from (cid:3) 1 mm to 17.5 mm. Complex formation at higher quencher concentration assures that the observed PET kinetics is a thermodynamically controlled process where solvent diffusion has no role on it.
关键词： CdTe quantum dot,photo-induced electron transfer,donor-acceptor complex,time-resolved spectroscopy,fluorescence quenching
更新于2025-09-19 17:13:59
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Non enzymatic fluorometric determination of glucose by using quenchable g-C3N4 quantum dots
摘要： A non-enzymatic fluorometric assay is described for the determination of glucose. The method is based on the use of g-C3N4 quantum dots (QDs) that have good water solubility. The QDs were synthesized by a one-step solvothermal process using formamide as precursor. The QDs possess an average size of ~5 nm, a band gap of 3.0~3.5 eV, and strong blue fluorescence (with excitation/emission maxima at 400/447 nm). Fluorescence is quenched by glucose (which acts as the electron acceptor) via an electron transfer mechanism. Comprehensive spectroscopy and density functional theory calculations show that the selectivity of the fluorescent probe can be attributed to the presence of N-H bonds that are formed between the QDs (mainly at plane edges) and glucose. The interaction forces lead to the formation of localized states for capturing hot electrons. This results in a decrease in the band gap and a reduction in fluorescence intensity. The probe is selective over some typical interfering species (such as cysteine and albumin) which often are present in the urine of diabetics. The method has a linear response in the 0.2 to 5.0 mM glucose concentration range and a 0.2 mM detection limit.
关键词： Density functional theory calculations,Fluorescent probe,Fluorescence quenching,Inorganic nanomaterials
更新于2025-09-16 10:30:52
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Understanding the excitation wavelength dependent spectral shift and large exciton binding energy of tungsten disulfide quantum dots and its interaction with single-walled carbon nanotubes
摘要： Herein, we investigate the origin of excitation wavelength dependent spectral features and high fluorescence quantum yield in fluorescent 2D tungsten disulfide (WS2) quantum dots (QDs) of average size 2.4 nm. The as-prepared WS2 QDs possess high optical bandgap and reasonably high fluorescence quantum yield ~15.4% in the green region without any functionalization. The broad photoluminescence (PL) spectrum consists of multiple peaks owing to emissions from excitonic transitions and surface defect-related transitions. The excitation wavelength-dependent spectral redshift and narrowing of line shape in the PL peak are analyzed carefully, and it is attributed to the selective excitation/recombination of carriers from different energy levels. The temperature-dependent PL analysis yields an exciton binding energy of ~301 meV in the QDs. Furthermore, we study the interaction between fluorescent WS2 QDs and single-walled carbon nanotubes (SWCNTs) and explore the mechanism of systematic quenching of PL of QDs by SWCNTs. The nature of the Stern–Volmer plot is found to be linear, and the time-resolved fluorescence measurements reveal that the quenching follows primarily the static behavior. Our study further reveals that defect sites in SWCNTs primarily act as the binding sites for WS2 QDs and form non-fluorescent complexes for effective quenching of the PL. The strong interaction between the WS2 QDs and the SWCNTs is evidenced from the spectral shift in the X-ray photoelectron spectroscopy and Raman peaks. Our study reveals the origin of excitation wavelength dependent PL emission from WS2 QDs and the nature of the interaction between WS2 QDs and SWCNTs, which are important for their applications in biomedical imaging and sensing, such as surface-enhanced Raman scattering, etc.
关键词： WS2 quantum dots,Fluorescence quenching,Defects,Carbon nanotubes,Exciton binding energy
更新于2025-09-16 10:30:52
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An eco-friendly imprinted polymer based on graphene quantum dots for fluorescent detection of <i>p</i> -nitroaniline
摘要： An eco-friendly fluorescent molecularly imprinted polymer anchored on the surface of graphene quantum dots (GQDs@MIP) was developed with an efficient sol–gel polymerization for highly sensitive and selective determination of p-nitroaniline (p-NA). The GQDs@MIP was characterized in detail by Fourier-transform infrared, fluorescence spectrometer, scanning electron microscope, transmission electron microscope and ultraviolet spectrophotometer. The results showed that the imprinted layer was successfully grafted on the surface of the GQDs. The fluorescence of the GQDs@MIP is efficiently quenched when p-NA recombines with the imprinting sites based on the photo-induced electron transfer fluorescence quenching mechanism. A good linear relationship was obtained between the fluorescence quenching efficiency of the GQDs@MIP and the concentration of p-NA in the range of 0–15.0 mM with a correlation coefficient of 0.99. The practicability of the proposed method in real samples was successfully evaluated through monitoring p-NA in water and fish samples with satisfactory recovery. The developed method provides a feasible and eco-friendly strategy to fabricate MIPs anchored on GQDs with good fluorescence properties for sensitive detection of organic pollutants in complex samples.
关键词： graphene quantum dots,fluorescent molecularly imprinted polymer,p-nitroaniline,fluorescence quenching,eco-friendly
更新于2025-09-16 10:30:52
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A novel optical fiber glucose biosensor based on carbon quantum dots-glucose oxidase/cellulose acetate complex sensitive film
摘要： A novel optical fiber glucose biosensor based on fluorescent carbon quantum dots (CQDs)-glucose oxidase (GOD)/cellulose acetate (CA) complex sensitive film was fabricated, in which the dip-coating method was adopted to immobilize the CQDs-GOD/CA complex sensitive film onto the end face of the optical fiber. The surface morphology, microstructure and optical performances of the sensitive film were characterized by field emission scanning electron microscope (FESEM), atomic force microscope (AFM), Zeiss Axiovert 25 inverted microscope, Fourier transform infrared spectroscopy (FTIR), Ultraviolet-visible spectrophotometer and fluorescence spectrophotometer, respectively. The developed fiber-optic biosensor exhibits high sensitivity and repeatability for continuous online detection of low concentration glucose, allowing visualization of real-time glucose fluctuations over a period of time. The change ratios in fluorescence intensity of the biosensor are linear with glucose concentration in various ranges including micromole and nanomole levels, and the relationship between relative fluorescence intensity ratio and glucose concentration complies well with the modified Stern-Volmer equation in the range of 10-200 μmol/L with the detection limit of 6.43 μM, and in the range of 10-100 nmol/L with the detection limit of 25.79 nM, respectively.
关键词： Optical fiber,Carbon quantum dots-glucose oxidase/cellulose acetate complex sensitive film,Glucose sensing,Fluorescence quenching
更新于2025-09-16 10:30:52
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Design of new Imidazole-derivative dye having donor-Π-acceptor moieties for highly efficient organic-dye-sensitized solar cells
摘要： In the present work, we have synthesised donors/acceptor substituted derivative of imidazole 4-(1-(3-chloro-4-nitrophenyl)-4,5-diphenyl-1H-imidazol-2-yl)benzoic acid (CNI) via one-pot synthetic method and has been characterized by spectroscopic methods such as IR, SEM and EDX. The photophysical properties like, solvatochromic shift and quantum yield of the CNI dye were found to be 1.85% and 0.57 respectively. The increase in absorbance and decrease in fluorescence spectra with different concentrations of TiO2 nanoparticles confirmed the possibility of interactions between dye and TiO2 nanoparticles. The Rehm-Weller relation suggests that, decrease in fluorescence of CNI dye was due to photo-induced electron transfer process and the Stern-Volmer studies suggest that, the fluorescence quenching mechanism was due to combined dynamic and static quenching process. The theoretical and experimental methods. Further, photosensitization of TiO2 nanoparticles from CNI dye has been investigated using absorption, steady state and time resolved fluorescence methods. Photovoltaic energy conversion efficiency and fill factor of fabricating CNI dye sensitized solar cell.
关键词： Dye sensitized solar cell (DSSC),TiO2 nanoparticles,Photo induced Electron transfer,Fluorescence quenching,Imidazoles derivatives
更新于2025-09-12 10:27:22
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Study on the preparation of water-soluble AgInS2 quantum dots and their application in the detection of ciprofloxacin
摘要： Water-soluble AgInS2 quantum dots (AIS QDs) were prepared by hot-injection method with thioglycolic acid (TGA) as the stabilizer. The fluorescence of as-prepared AIS QDs could be quenched effectively by ciprofloxacin. Herein, a method for the content determination of ciprofloxacin based on the fluorescence quenching effect was explored. The experimental results showed that the particle size of AIS QDs prepared at pH = 4 was about 3–8 nm, and the maximum fluorescence emission wavelength was centered at 626 nm at λex = 500 nm. The measured concentration range of ciprofloxacin could be adjusted by varying the amount of AIS QDs solution. When 0.40 mL AIS QDs solution was used for the content determination of ciprofloxacin, a good linearity relationship was achieved between the quenched efficiency of AIS QDs fluorescence and the concentration of ciprofloxacin in the range of 1.0–19.5 μg/mL, the correlation coefficient was 0.996, the detection limit of ciprofloxacin was 0.12 μg/mL, and the blank spike recoveries were in the range of 96.7–103.3%. The method is of wide detection range, excellent selectivity, high sensitivity and easy operability, could be applied for the content determination of ciprofloxacin in drugs.
关键词： AgInS2 quantum dots,Ciprofloxacin,Fluorescence quenching,Content determination
更新于2025-09-12 10:27:22
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CdTe Quantum Dots Modified with Cysteamine: A New Efficient Nanosensor for the Determination of Folic Acid
摘要： In this paper, we report the synthesis, characterization, and application of a new fluorescent nanosensor based on water-soluble CdTe quantum dots (QDs) coated with cysteamine (CA) for the determination of folic acid (FA). CdTe/CA QDs were characterized by high-resolution transmission electron microscopy, the zeta potential, and Fourier-transform infrared (FT-IR), UV-visible, and fluorescence spectroscopy. CdTe QDs coated with mercaptopropionic acid (MPA) and glutathione (GSH) were prepared for comparison purposes. The effect of FA on the photoluminescence intensity of the three thiol-capped QDs at pH 8 was studied. Only CdTe/CA QDs showed a notable fluorescence quenching in the presence of FA. Then, a nanosensor based on the fluorescence quenching of the CdTe QDs at pH 8 was explored. Under optimum conditions, the calibration curve showed a linear fluorescence quenching response in a concentration range of FA from 0.16 to 16.4 μM (R2 = 0.9944), with a detection limit of 0.048 μM. A probable mechanism of fluorescence quenching was proposed. The nanosensor showed good selectivity over other possible interferences. This method has been applied for FA quantification in orange beverage samples with excellent results (recoveries from 98.3 to 103.9%). The good selectivity, sensitivity, low cost, and rapidity make CdTe /CA QDs a suitable nanosensor for FA determination.
关键词： electron transfer,folic acid nanosensor,positive quantum dots,fluorescence quenching
更新于2025-09-12 10:27:22
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Fluorometric determination of aflatoxin B1 using a labeled aptamer and gold nanoparticles modified with a complementary sequence acting as a quencher
摘要： A fluorometric aptamer based assay is described for rapid and sensitive detection of aflatoxin B1 (AFB1). It is making use of a fluorescein (FAM) labeled anti-AFB1 aptamer and complementary DNA-modified gold nanoparticles (GNPs). In the absence of AFB1, the FAM-labeled aptamers hybridize with complementary DNA strands that were covalently immobilized on GNPs. This results in quenching of the green fluorescence (with excitation/emission peaks at 485/525 nm). In the presence of AFB1, the aptamer probe binds AFB1 and is released from the GNPs. Hence, fluorescence is restored. Under optimized conditions, AFB1 in the concentration range from 61 pM to 4.0 μM can be detected, and the detection limit is 61 pM. This assay is highly selective for AFB1. It was applied to the determination of AFB1 spiked into 50-fold diluted wine and 20-fold diluted beer.
关键词： Mycotoxin,Food safety,Environmental analysis,Fluorescence quenching,Fluorophore,Fluorescent probe,Nanomaterials,Nanoprobe
更新于2025-09-11 14:15:04
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Compact quantum dot surface modification to enable emergent behaviors in quantum dot-DNA composites
摘要： Quantum dot (QD) biological imaging and sensing applications often require surface modification with single-stranded deoxyribonucleic acid (ssDNA) oligonucleotides. Furthermore, ssDNA conjugation can be leveraged for precision QD templating via higher-order DNA nanostructures to exploit emergent behaviors in photonic applications. Use of ssDNA-QDs across these platforms requires compact, controlled conjugation that engenders QD stability over a wide pH range and in solutions of high ionic strength. However, current ssDNA-QD conjugation approaches suffer from limitations, such as the requirement for thick coatings, low control over ssDNA labeling density, requirement of large amounts of ssDNA, or low colloidal or photostability, restraining implementation in many applications. Here, we combine thin, multidentate, phytochelatin-3 (PC3) QD passivation techniques with strain-promoted copper-free alkyne-azide click chemistry to yield functional ssDNA-QDs with high stability. This process was broadly applicable across QD sizes (i.e., λem = 540, 560, 600 nm), ssDNA lengths (i.e., 10–16 base pairs, bps), and sequences (poly thymine, mixed bps). The resulting compact ssDNA-QDs displayed a fluorescence quenching efficiency of up to 89% by hybridization with complementary ssDNA-AuNPs. Furthermore, ssDNA-QDs were successfully incorporated with higher-order DNA origami nanostructure templates. Thus, this approach, combining PC3 passivation with click chemistry, generates ssDNA-PC3-QDs that enable emergent QD properties in DNA-based devices and applications.
关键词： ssDNA,click chemistry,DNA origami,quantum dots,fluorescence quenching
更新于2025-09-11 14:15:04