t Father of Antoine-Henri Becquerel, the famous French physicist and discoverer of radioactivity. in .NET

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392 in detail by H. Gerischer. The photogalvanic effect was first interpreted in 1940 by E. Rabinowitch, and more recently studied by W. J. Albery, M. D. Archer and others. Besides the classification of photoelectrochemical effects (cells) according to the nature of the light-absorbing system, we can also distinguish them according to the effective Gibbs free energy change in the electrolyte, AG: 1. AG = 0: Regenerative photoelectrochemical cell. The reactants consumed during the photoredox process (either in homogeneous phase or at the semiconductor photoelectrode) are immediately regenerated by subsequent electrode reactions. The net output of the cell is an electrical current flowing through the cell and an external circuit, but no permanent chemical change in the electrolyte takes place. 2. AG = 0: Photoelectrosynthetic cell. The products of the homogeneous or heterogeneous photoredox process and the corresponding counterelectrode reactions are sufficiently stable to be collected for later use. Practically interesting is the endoergic photoelectrosynthesis (AG > 0 ) , producing species with stored chemical energy (fuel). The most important example is the splitting of water to oxygen and hydrogen. The exoergic process (AG<0) is also called photocatalytic, since the light provides only the activation energy for the reaction, which is otherwise thermodynamically possible even in the dark. Although no chemical energy is stored, useful products can sometimes result; an example is the synthesis of NH3 from N2 and H 2 . 5.10.2 Electrochemical photoemission
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In contrast to semiconductors, metals are usually not active as photoelectrodes owing to the fast thermal recombination of photogenerated charge carriers in the metal. The only light-stimulated charge transfer process at the electrolyte/metal electrode interface is photoemission of electrons. It is, in principle, similar to the conventional photoelectric effect in vacuum, i.e. it takes place under illumination with photons of sufficiently short wavelengths to overcome the binding energy of electron in the metal. Photoelectrons, emitted from the metal electrode into the electrolyte solution, are rapidly solvated and subsequently captured by a reducible solution species. The electrochemical photoemission was studied mostly at mercury electrode, first by M. Heyrovsky. The dependence of the photoemission current on the radiation frequency differs from that of a conventional vacuum photoemission. Gurevich et al. deduced the relationship: Ic = A(hv-hv0-eE)5/2 (5.10.1)
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where / c is the photocurrent, A is a constant, hv is the energy of the light quantum, hv0 is the threshold energy for photoemission at zero charge potential, e is the electron charge, and E is the electrode potential.
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393 5.10.3 Homogeneous photoredox reactions and photogalvanic effects The photogalvanic effects are initiated by a homogeneous photoredox reaction of an electrolyte redox system with a suitable photoexcited organic or organometallic substance (dye), S. The photon absorption produces a short-lived, electronically excited dye molecule, S*:
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whose structure and physicochemical properties are different. The conversion of 5* back to 5 proceeds by various radiative and non-radiative relaxation processes, which are characterized by a pseudo-first-order rate constant, kb. Its reciprocal value defines the lifetime of the excited state, r0: ro=l/kb (5.10.2)
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(the fraction of the S* molecules, deactivated during the time r 0 , equals 1 e~l 63%). Only excitations of electrons from the highest occupied molecular orbital (HOMO) to the lowest unoccupied molecular orbital (LUMO), which produce reasonably long-lived S* molecules are practically important. This is schematically depicted in Fig. 5.57. Most of the ground-state molecules contain all the electrons paired. (The 0 2 molecule is an important exception to this rule.) The excited molecule may occur in two states, either with none or two unpaired electrons; these states are called excited singlet, 5X, or excited triplet, Tx. The latter state is, according to the Pauli rule, energetically favoured and its lifetime is higher by orders of magnitude, since the reactions with singlet molecules as well as radiative relaxation (phosphorescence) are spin-forbidden. The photoexcited S*{TX) molecule may have a sufficiently long lifetime to diffuse some distance in the electrolyte solution and to take part in a
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