Observation of Oscillatory Surface Reactions of Riboflavin, Trolox, and Singlet Oxygen Using Single Carbon Nanotube Fluorescence Spectroscopy

2012-12-01
Sen, Fatih
Boghossian, Ardemis A.
Sen, Selda
Ulissi, Zachary W.
Zhang, Jingqing
Strano, Michael S.
Show full item record
Creative Commons License
This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.
215
views
0
downloads
Single-molecule fluorescent microscopy allows semiconducting single-walled carbon nanotubes (SWCNTs) to detect the adsorption and desorption of single adsorbate molecules as a stochastic modulation of emission intensity. In this study, we identify and assign the signature of the complex decomposition and reaction pathways of riboflavin in the presence of the free radical scavenger Trolox using DNA-wrapped SWCNT sensors dispersed onto an aminopropyltriethoxysilane (APTES) coated surface. SWCNT emission is quenched by riboflavin-induced reactive oxygen species (ROS), but increases upon the adsorption of Trolox, which functions as a reductive brightening agent. Riboflavin has two parallel reaction pathways, a Trolox oxidizer and a photosensitizer for singlet oxygen and superoxide generation. The resulting reaction network can be detected in real time in the vicinity of a single SWCNT and can be completely described using elementary reactions and kinetic rate constants measured independently. The reaction mechanism results in an oscillatory fluorescence response from each SWCNT, allowing for the simultaneous detection of multiple reactants. A series-parallel kinetic model is shown to describe the critical points of these oscillations, with partition coefficients on the order of 10(6) - 10(4) for the reactive oxygen and excited state species. These results highlight the potential for SWCNTs to characterize complex reaction networks at the nanometer scale.
Single-walled carbon nanotube (SWCNT), Fluorescence, Deoxyribonucleic acid, (DNA AT15), Single molecule Trolox, Riboflavin, Singlet oxygen, Triplet state, Scavenging (scavenger), Sensor
https://hdl.handle.net/11511/68240
ACS NANO
Department of Chemistry, Article

Suggestions

Observation of long-range, near-side angular correlations in pPb collisions at the LHC
Chatrchyan, S.; et. al. (Elsevier BV, 2013-01-01)
Results on two-particle angular correlations for charged particles emitted in pPb collisions at a nucleon-nucleon center-of-mass energy of 5.02 TeV are presented. The analysis uses two million collisions collected with the CMS detector at the LHC. The correlations are studied over a broad range of pseudorapidity, eta, and full azimuth, phi, as a function of charged particle multiplicity and particle transverse momentum, p(T). In high-multiplicity events, a long-range (2 < vertical bar Delta eta vertical bar...
Analysis of vibrational spectra in relation to the thermodynamic quantities close to the phase transitions in ammonium halides (NH4F and NH4I)
Tari, O.; Yurtseven, Hasan Hamit (2017-01-01)
The pressure dependences of the vibrational frequencies of the TO and L modes are analyzed from the literature data and the thermodynamic quantities such as isothermal compressibility K gamma, thermal expansion alpha p and the specific heat C-p - C-v are calculated through the mode Grilneisen parameters of those modes in ammonium halides (NH4F and NH4I). For this calculation, the observed frequencies of the TO mode (238 cm(-1) at 1 bar) and the L mode (74.7 meV at 1.9 GPa) are used for the phases of I, II a...
Preparation and thermal characterization of poly(2-vinylpyridine) copolymers coordinated to Cr nanoparticles
Öztürk, Yurdagül; Kayran, Ceyhan; Hacaloğlu, Jale (2015-06-01)
In this study, polystyrene-block-poly(2-vinylpyridine), PS-b-P2VP, polyisoprene-block-poly(2-vinylpyridne), PI-b-P2VP and poly(methyl metacrylate)-block-poly(2-vinylpyridine), PMMA-b-P2VP, coordinated to Cr metal were synthesized and characterized by Fourier transform infrared, transmission electron microscopy and direct pyrolysis mass spectrometry techniques. Both thermal degradation mechanism and thermal stability of P2VP blocks were affected by the coordination of Cr nanoparticles to nitrogen of pyridine...
Synthesis of novel diketopyrrole and selenophene containing nir absorbing polymers and their application in bulk-heterojunction solar cells
Öklem, Gülce; Günbaş, Emrullah Görkem; Department of Polymer Science and Technology (2017)
DPP-based conjugated polymers are recently used in organic light emitting diodes, electrochromic devices, organic field effect transistor and organic solar cell applications. Their advantageous properties, such as broad optical absorption in Near Infra Red (NIR) region, high charge carrier mobility and good film forming ability make them an excellent choice for generation of highly efficient solar cells. In this thesis, using donor-acceptor approach (D-A) we aimed to synthesize novel polymers with furan bas...
Observation of Complex Time Structures in the Cosmic-Ray Electron and Positron Fluxes with the Alpha Magnetic Spectrometer on the International Space Station
Aguilar, M.; et. al. (2018-07-31)
We present high-statistics, precision measurements of the detailed time and energy dependence of the primary cosmic-ray electron flux and positron flux over 79 Bartels rotations from May 2011 to May 2017 in the energy range from 1 to 50 GeV. For the first time, the charge-sign dependent modulation during solar maximum has been investigated in detail by leptons alone. Based on 23.5 x 10(6) events, we report the observation of short-term structures on the timescale of months coincident in both the electron fl...
Citation Formats
F. Sen, A. A. Boghossian, S. Sen, Z. W. Ulissi, J. Zhang, and M. S. Strano, “Observation of Oscillatory Surface Reactions of Riboflavin, Trolox, and Singlet Oxygen Using Single Carbon Nanotube Fluorescence Spectroscopy,” ACS NANO, pp. 10632–10645, 2012, Accessed: 00, 2020. [Online]. Available: https://hdl.handle.net/11511/68240.
METU IIS - Integrated Information Service open@metu.edu.tr