Protein Nanoparticle Interactions: Opportunities and Challenges Morteza Mahmoudi,* Iseult Lynch, Mohammad Reza Ejtehadi, Marco P. Monopoli, Francesca Baldelli Bombelli, and Sophie Laurent National Cell Bank, Pasteur Institute of Iran, Tehran, Iran Nanotechnology Research Center, Faculty of Pharmacy, Tehran University of Medical Sciences, Tehran, Iran School of Chemistry and Chemical Biology & Conway Institute for Biomolecular and Biomedical Research, University College Dublin, Belfield, Dublin 4, Ireland Department of Physics, Sharif University of Technology, Tehran, Iran School of Pharmacy, UEA, Norwich Research Park, Norwich,U.K. Department of General, Organic, and Biomedical Chemistry, NMR and Molecular Imaging Laboratory, University of Mons, Avenue Maistriau 19, B-7000 Mons, Belgium

Protein-nanoparticle interactions: opportunities and challenges.

The current state of understanding of molecular resonance energy transfer (RET) and recent developments in the field are reviewed. The development of more general theoretical approaches has uncovered some new principles underlying RET processes. This review brings many of these important new concepts together into a generalization of Forster's original theory. The conclusions of studies investigating the various approximations in Forster theory are summarized. Areas of present and future activity are discussed. The review covers Forster theory for donor-acceptor pairs and electronic coupling for singlet-singlet, triplet-triplet, and superexchange-mediated energy transfer. This includes the transition density picture of Coulombic coupling as well as electronic coupling between molecular aggregates (excitons). Spectral overlaps and ensemble energy transfer rates in disordered aggregates, the role of dielectric properties of the medium, weak versus strong coupling, and new models for energy transfer in complex molecular assemblies are also described.

/pdf/long-range-resonance-energy-transfer-in-molecular-systems-2t0z5zlmj8.pdf

Long-Range Resonance Energy Transfer in Molecular Systems

Peptide nucleic acids (PNA): synthesis, properties and potential applications

The attainment of a better understanding of the dependence of photoinduced electron transfer reaction rates on the molecular structures of the donor and acceptor entities results in improving the capture and storage of solar energy. Here, the intermolecular and supramolecular electron transfer processes from electron donors (porphyrins (P), chlorophylls (Chl), phthalocyanines (Pc) and naphthalocyanines (Nc)) and their metal derivatives to electron acceptors (fullerenes such as C 60 and C 70 ) studied by nanosecond and picosecond laser flash photolysis techniques in polar and nonpolar solvents are reviewed. For intermolecular systems in polar solvents, photoinduced electron transfer takes place via the excited triplet states of C 60 /C 70 or via the excited triplet states of P/Pc/Nc, yielding solvated radical ions in polar solvents; thus, the back electron transfer rates are generally slow. In the case of the supramolecular dyads and triads formed by axial coordination, hydrogen bonding, crown ether complexation, or rotaxane formation, the photoinduced charge separation takes place mainly from the excited singlet state of the donor; however, the back electron transfer rates are generally quite fast. The relations between structures and photochemical reactivities of these novel supramolecular systems are discussed in relation to the efficiency of charge separation and charge recombination.

Intermolecular and supramolecular photoinduced electron transfer processes of fullerene–porphyrin/phthalocyanine systems

The rate of energy transfer from B800 to B850 in the peripheral light harvesting complex LH2 is modeled in detail. A method for determining ensemble average energy transfer rates in complex, coupled multichromophoric systems is reported and is employed to investigate the interplay of electron−phonon coupling (fast fluctuations of the protein) and site energy disorder (slow fluctuations) on the spectral overlap between donor and acceptor, and therefore the energy transfer rate. A series of model calculations for Rb. sphaeroides is reported. The disorder is found to have a marked influence on the calculated rate of energy transfer and is responsible for a faster energy transfer time than would occur in its absence and furthermore accounts for the weak temperature dependence observed in experiment. The excitonic nature of the acceptor (albeit dynamically localized) also has impact in terms of how B850 functions as an energy acceptor. These conclusions are further elucidated by calculations of Rps. acidophila...

/pdf/on-the-mechanism-of-light-harvesting-in-photosynthetic-12mjgbv21s.pdf

On the Mechanism of Light Harvesting in Photosynthetic Purple Bacteria: B800 to B850 Energy Transfer

Photoinduced electron transfer in donor-bridge-acceptor systems with zinc porphyrin (or its pyridine complex) as the donor and gold(III) porphyrin as the acceptor has been studied. The porphyrin moieties were covalently linked with geometrically similar bridging chromophores which vary only in electronic structure. Three of the bridges are fully conjugated pi -systems and in a fourth, the conjugation is broken. For systems with this bridge, the quenching rate of the singlet excited state of the donor was independent of solvent and corresponded to the rate of singlet energy transfer expected for a Forster mechanism. In contrast, systems with a rr-conjugated bridging chromophore show a solvent-dependent quenching rate that suggests electron transfer in the Marcus normal region. This is supported by picosecond transient absorption measurements, which showed formation of the zinc porphyrin radical cation only in systems with pi -conjugated bridging chromophores. On the basis of the Marcus and Rehm-Weller equations, an electronic coupling of 5-20 cm(-1) between the donor and acceptor is estimated for these systems. The largest coupling is found for the systems with the smallest energy gap between the donor and bridge singlet excited states. This is in good agreement with the coupling calculated with quantum mechanical methods, as is the prediction of an almost zero coupling in the systems with a nonconjugated bridging chromophore.

Bridge-dependent electron transfer in porphyrin-based donor-bridge-acceptor systems.

https://febs.onlinelibrary.wiley.com/doi/pdf/10.1016/0014-5793%2895%2900409-3

Phospholipid membrane permeability of peptide nucleic acid

We have studied singlet electronic energy transfer (EET) in two donor-bridge-acceptor series (D-B -A), in which the donor (zinc porphyrin or its pyridine complex) and the acceptor (free base porphyrin) were covalently connected by a geometrically well-defined bridging chromophore. We have investigated how the medium between a donor and an acceptor influences EET by separating the influence of the electronic structure of the bridging chromophore from other effects known to influence the energy transfer. The electronic structure of the bridging chromophore was varied by changing the central unit (bicyclo[2.2.2]octane, benzene, naphthalene, or anthracene) in the bridging chromophore. In all systems the excited state energy separation donor-bridge and bridge-acceptor is large enough to prevent stepwise singlet energy transfer. In addition, the systems were designed to minimize conjugation to preserve the identity of the separate chromophores (donor, bridge, acceptor). Compared with the rate constant expected from the Forster theory, the bridging chromophore with bicyclo[2.2.2]octane as the central unit did not significantly enhance the energy transfer rate constant. However, the bridging chromophores with benzene and naphthalene as the central unit showed a moderate increase, whereas the bridging chromophore with anthracene as the central unit showed the largest increase in energy transfer rate constant. This increase is ascribed to a mediating effect of the bridging chromophore and it is proposed to be strongly correlated to the energy splitting between the singlet excited states of donor and bridging chromophores.

Mediated electronic coupling: Singlet energy transfer in porphyrin dimers enhanced by the bridging chromophore

Donor−acceptor systems where the rate of radiationless electronic energy transfer is influenced by the electronic structure of the intervening medium are studied. In this paper we report the observation of mediated energy transfer in a series of geometrically well-defined porphyrin dimers. The dimers consist of a free base porphyrin (5,15-diphenyl-α,β-octaalkylporphyrin, H2P) and the corresponding zinc porphyrin (ZnP) as acceptor and donor, respectively, connected by aryl chromophores with varying energies of the lowest excited states.

Mediated energy transfer in covalently linked porphyrin dimers

Triplet energy transfer in porphyrin dimers: Comparison between pi- and sigma-chromophore bridged systems

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