15 research outputs found

    Characteristic Excitation Wavelength Dependence of Fluorescence Emissions in Carbon "quantum" Dots

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    Carbon "quantum" dots (CDots), generally defined as small carbon nanoparticles with various surface passivation schemes, have emerged to represent a rapidly advancing and expanding research field. CDots are known for their bright and colorful fluorescence emissions, where the colorfulness is associated with the emissions being excitation wavelength dependent. In this work, CDots with 2,2′-(ethylenedioxy)bis(ethylamine) (EDA) for surface functionalization were studied systematically by using steady-state and time-resolved fluorescence methods. The observed fluorescence quantum yields are strongly excitation wavelength dependent, and the dependence apparently tracks closely the observed absorption profile of the EDA-CDots, whereas the excitation wavelength dependence of observed fluorescence lifetimes is much weaker, obviously decoupled from the quantum yields. Mechanistically, the presence of two sequential processes immediately following the photoexcitation of CDots leading to fluorescence is used to rationalize these effects, and the experimental results seem better explained by attributing one of the two processes to be primarily responsible for the characteristic excitation wavelength dependence. Significant implications of the mechanistic probing to the understanding of CDots as a new class of quantum dot-like fluorescent nanomaterials are discussed, and so are further challenges and opportunities

    Functionalization of Carbon Nanoparticles and DefunctionalizationToward Structural and Mechanistic Elucidation of Carbon “Quantum” Dots

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    Small carbon nanoparticles were functionalized by low-molecular weight amino compound 3-ethoxypropylamine (EPA) for ultracompact carbon dots of bright fluorescence emissions. The results from solution-phase NMR characterization support the expected dot structure of carbon nanoparticles surface-attached with EPA species. The optical properties of the EPA-carbon dots share many features with those found in carbon dots of other surface functionalities, but there is an extra absorption shoulder in the blue spectral region, into which the excitation results in much enhanced green fluorescence emissions. The EPA-carbon dots were defunctionalized by gradually removing the EPA species from the carbon nanoparticles, along with spectroscopic characterizations on the samples of different degrees of defunctionalization. The outcomes further confirm the critical role of surface functionalization in the superior optical properties of carbon dots. Results from systematic measurements of fluorescence quantum yields and decays at different excitation wavelengths for the EPA-carbon dots and their gradually defunctionalized samples are presented, and their mechanistic implications are discussed
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