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Register a new userCovalently Binding the Photosystem I to Carbon Nanotubes
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Added by
Alexander W. Holleitner
Publication date
2009
fields
Physics
and research's language is
English
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We present a chemical route to covalently couple the photosystem I (PS I) to carbon nanotubes (CNTs). Small linker molecules are used to connect the PS I to the CNTs. Hybrid systems, consisting of CNTs and the PS I, promise new photo-induced transport phenomena due to the outstanding optoelectronic properties of the robust cyanobacteria membrane protein PS I.
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We have calculated the binding energy of various nucleobases (guanine (G), adenine (A), thymine (T) and cytosine (C)) with (5,5) single-walled carbon nanotubes (SWNTs) using ab-initio Hartre-Fock method (HF) together with force field calculations. The gas phase binding energies follow the sequence G $>$ A $>$ T $>$ C. We show that main contribution to binding energy comes from van-der Wall (vdW) interaction between nanotube and nucleobases. We compare these results with the interaction of nucleobases with graphene. We show that the binding energy of bases with SWNTs is much lower than the graphene but the sequence remains same. When we include the effect of solvation energy (Poisson-Boltzman (PB) solver at HF level), the binding energy follow the sequence G $>$ T $>$ A $>$ C $>$, which explains the experimentcite{zheng} that oligonucleotides made of thymine bases are more effective in dispersing the SWNT in aqueous solution as compared to poly (A) and poly (C). We also demonstrate experimentally that there is differential binding affinity of nucleobases with the single-walled carbon nanotubes (SWNTs) by directly measuring the binding strength using isothermal titration (micro) calorimetry. The binding sequence of the nucleobases varies as thymine (T) $>$ adenine (A) $>$ cytosine (C), in agreement with our calculation.
We investigate the electronic structure of carbon nanotubes functionalized by adsorbates anchored with single C-C covalent bonds. We find that, despite the particular adsorbate, a spin moment with a universal value of 1.0 $mu_B$ per molecule is induced at low coverage. Therefore, we propose a mechanism of bonding-induced magnetism at the carbon surface. The adsorption of a single molecule creates a dispersionless defect state at the Fermi energy, which is mainly localized in the carbon wall and presents a small contribution from the adsorbate. This universal spin moment is fairly independent of the coverage as long as all the molecules occupy the same graphenic sublattice. The magnetic coupling between adsorbates is also studied and reveals a key dependence on the graphenic sublattice adsorption site.
One- and two-photon luminescence excitation spectroscopy showed a series of distinct excitonic states in single-walled carbon nanotubes. The energy splitting between one- and two-photon-active exciton states of different wavefunction symmetry is the fingerprint of excitonic interactions in carbon nanotubes. We determine exciton binding energies of 0.3-0.4 eV for different nanotubes with diameters between 0.7 and 0.9 nm. Our results, which are supported by ab-initio calculations of the linear and non-linear optical spectra, prove that the elementary optical excitations of carbon nanotubes are strongly Coulomb-correlated, quasi-one dimensionally confined electron-hole pairs, stable even at room temperature. This alters our microscopic understanding of both the electronic structure and the Coulomb interactions in carbon nanotubes, and has direct impact on the optical and transport properties of novel nanotube devices.
Vibrational energy transfer from photo-excited single-wall carbon nanotubes (SWCNTs) to coupled proteins is a key to engineer thermally induced biological reactions such as photothermal therapy. Here, we explored vibrational energy transfer from the photo-excited SWCNTs to different adsorbed biological materials by means of a femtosecond pump-probe technique. We show that the vibrational relaxation time of the radial breathing modes (RBMs) in SWCNTs significantly depends on the structure of coupled materials, i.e. proteins or biopolymers, indicating the vibrational energy transfer is governed by overlap of phonon density of states between the SWCNTs and coupled materials.
We develop two new amphiphilic molecules that are shown to act as efficient surfactants for carbon nanotubes in non-polar organic solvents. The active conjugated groups, which are highly attracted to graphene nanotube surface, are based on pyrene and porphyrin. We show that relatively short (C18) carbon tails are insufficient to provide stabilization. As our ultimate aim is to disperse and stabilize nanotubes in siloxane matrix (polymer and crosslinked elastomer), both surfactant molecules were made with long siloxane tails to facilitate solubility and steric stabilization. We show that pyrene-siloxane surfactant is very effective in dispersing multi-wall nanotubes, while the porphyrin-siloxane is making single-wall nanotubes soluble, both in petroleum ether and in siloxane matrix.
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