Abstract

The preparation and investigation of Fe(III) doped carbon nanodots (CNDs) with intense green photoluminescence and emission dependence on the dispersion medium are reported. Their unusual photoluminescence is especially highlighted in water where the initial blue emission is gradually shifted to intense deep green, while in other common solvents (chloroform, acetone etc.) this behavior has not been observed. Through embedding in a polymer matrix (e.g., PVA) the color transition becomes reversible and dependent on water content, ranging from a full blue emission, when completely dried, to an intense green emission, when wetted. The preparation path of the Fe(III) doped CNDs undergoes two main stages involving the initial obtaining of Fe(III)–N–Hydroxyphthalimide complex and then a thermal processing through controlled pyrolysis. Morphostructural investigations of the prepared Fe(III) doped CNDs were performed through TG, FT-IR, XPS, DLS, TEM and AFM techniques whereas absolute PLQY, steady state and lifetime fluorescence were used to highlight their luminescence properties. The results issued from structural and fluorescence investigations bring new insights on the particular mechanisms involved in CNDs photoluminescence, a topic still open to debate.

Highlights

  • The preparation and investigation of Fe(III) doped carbon nanodots (CNDs) with intense green photoluminescence and emission dependence on the dispersion medium are reported

  • Their unique feature of emission transition reversibility was tested by embedding the Fe(III) doped CNDs in a polymer matrix (PVA in this case, though not limited to) leading to color transition depending on water content, turning from a full blue emission when completely dried to intense green when wetted

  • Fe(III) doped CNDs with intense green photoluminescence and unusual emission dependence according to the dispersion medium were prepared through controlled pyrolytic processing of a Fe(III)–N–Hydroxyphthalimide complex

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Summary

Introduction

The preparation and investigation of Fe(III) doped carbon nanodots (CNDs) with intense green photoluminescence and emission dependence on the dispersion medium are reported Their unusual photoluminescence is especially highlighted in water where the initial blue emission is gradually shifted to intense deep green, while in other common solvents (chloroform, acetone etc.) this behavior has not been observed. A first approach is based on a behavior similar to that of semiconductor Quantum Dots, where the emission peaks are size dependent and rely on quantum confinement[11] while the second one highlights the radiative transitions occurring within or between the surface attached functional groups, with the graphitic core defects playing a key role over the entire process[12] The latter approach seems to gain more evidence as very recent studies revealed the importance of carbonyl or nitrogen containing groups and the influence of the dispersion medium on the emission characteristics of the CNDs13,14. The reported CNDs are the first to exhibit this type of behavior, opening several new perspectives in terms of potential applications and providing several new insights regarding their specific structure and luminescent mechanisms

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