Rebecca Momper1, Julian Steinbrecher2, Matthias Dorn3, Irina Rörich4, Simon Bretschneider5, Manuel Tonigold6, Charusheela Ramanan7, Sandra Ritz8, Volker Mailänder9, Katharina Landfester10, Markus B Bannwarth11. 1. Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany. Electronic address: momper@mpip-mainz.mpg.de. 2. Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany. Electronic address: stonebraker@gmx.net. 3. Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany. Electronic address: matthias.dorn1@gmx.net. 4. Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany. Electronic address: roerich@mpip-mainz.mpg.de. 5. Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany. Electronic address: bretschneider@mpip-mainz.mpg.de. 6. Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany; Dermatology Clinic, University Medical Center Mainz, Langenbeckstraße 1, 55131 Mainz, Germany. Electronic address: MTonigold85@gmx.de. 7. Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany. Electronic address: ramanan@mpip-mainz.mpg.de. 8. IMB gGmbH, Ackermannweg 4, 55128 Mainz, Germany. Electronic address: s.ritz@imb-mainz.de. 9. Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany; Dermatology Clinic, University Medical Center Mainz, Langenbeckstraße 1, 55131 Mainz, Germany. Electronic address: mailaend@mpip-mainz.mpg.de. 10. Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany. Electronic address: landfester@mpip-mainz.mpg.de. 11. Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany. Electronic address: bannwarth@mpip-mainz.mpg.de.
Abstract
HYPOTHESIS: Carbon dot systems are highly surface sensitive fluorescent nanomaterials. In the presence of specific molecules or ions, the fluorescence properties can be strongly influenced. Often their fluorescent properties are activated or strongly enhanced through passivation agents such as polymer coatings. While several passivating polymers have been directly attached to the carbon dot systems, the interaction of carbon dot systems with the polymer surface of colloids has not been investigated as a way to activate or enhance the photoluminescent properties. Here, we show for the first time that the interaction of carbon dot systems with polymer colloids can strongly enhance the fluorescent properties of the carbon dot systems. EXPERIMENTS: To introduce carbon dot - polymer nanoparticle interactions, carbon dots are either generated directly in a microwave assisted synthesis in the presence of negatively charged polystyrene nanoparticles (in situ) or synthesized in the microwave separately and mixed afterwards with polymer nanoparticles (mixing). For the carbon dot system synthesis, chitosan, 1,2-ethylenediamine, and acetic acid are used as precursors. The produced carbon dot - polymer nanoparticle system are characterized by scanning electron microscopy, transmission electron microscopy, and flow cytometry measurements, and their interaction is assessed by fluorescence spectroscopy and fluorescence lifetime measurements. FINDINGS: We show that depending on the synthesis route (in situ or mixing), the carbon dot systems are either covalently attached (in situ) or electrostatically bound (mixing) to the surface of the nanoparticles. Regardless of the preparation methods of the investigated carbon dot - polymer nanoparticle system and the interaction (chemical or physical) with the surface, the fluorescence intensity is strongly enhanced and the fluorescence lifetime prolonged. These findings indicate a stabilization of the radiative trap states of carbon dot systems through interaction with the surface of the particles.
HYPOTHESIS: Carbon dot systems are highly surface sensitive fluorescent nanomaterials. In the presence of specific molecules or ions, the fluorescence properties can be strongly influenced. Often their fluorescent properties are activated or strongly enhanced through passivation agents such as polymer coatings. While several passivating polymers have been directly attached to the carbon dot systems, the interaction of carbon dot systems with the polymer surface of colloids has not been investigated as a way to activate or enhance the photoluminescent properties. Here, we show for the first time that the interaction of carbon dot systems with polymer colloids can strongly enhance the fluorescent properties of the carbon dot systems. EXPERIMENTS: To introduce carbon dot - polymer nanoparticle interactions, carbon dots are either generated directly in a microwave assisted synthesis in the presence of negatively charged polystyrene nanoparticles (in situ) or synthesized in the microwave separately and mixed afterwards with polymer nanoparticles (mixing). For the carbon dot system synthesis, chitosan, 1,2-ethylenediamine, and acetic acid are used as precursors. The produced carbon dot - polymer nanoparticle system are characterized by scanning electron microscopy, transmission electron microscopy, and flow cytometry measurements, and their interaction is assessed by fluorescence spectroscopy and fluorescence lifetime measurements. FINDINGS: We show that depending on the synthesis route (in situ or mixing), the carbon dot systems are either covalently attached (in situ) or electrostatically bound (mixing) to the surface of the nanoparticles. Regardless of the preparation methods of the investigated carbon dot - polymer nanoparticle system and the interaction (chemical or physical) with the surface, the fluorescence intensity is strongly enhanced and the fluorescence lifetime prolonged. These findings indicate a stabilization of the radiative trap states of carbon dot systems through interaction with the surface of the particles.