Absorption of single photon

In Chap. 3, wave packet propagation could be observed for nearly all of the alkali dimer and trimer systems considered, over a rather long time compared to the wave packet oscillation period. The wave packet dynamics - a fingerprint of the excited molecule - definitely characterize the excited bound electronic state of these molecules. However, with the results on K3 (excited with A 800 nm), another phenomenon, which often governs ultrafast molecular and cluster dynamics, comes into the discussion photodissociation induced by the absorption of single photons. This photoinduced dissociation permits detailed study of molecular dynamics such as breaking of bonds, internal energy transfer, and radiationless transitions. The availability of laser sources with pulses of a few tens of femtoseconds today opens a direct, i.e. real-time, view on this phenomenon. 

Many molecules which have absorption bands in the wavelength region of existing laser lines can be excited by absorption of laser photons into single isolated rotational-vibrational levels of the electronic ground state 1W>-103) (jn the case of infrared laser lines) or of an excited electronic state (with visible or ultraviolet lines)... 

Figure 14.1 The singly excited state on the right may be qualitatively viewed as deriving from movement of an electron out of the ground-state HOMO into the indicated higher energy orbital (perhaps following absorption of a photon cairying the appropriate quantum of energy). Note, however, that the optimized orbitals of the ground state are at best approximations to those of the excited state...

PHOTONUCLEAR REACTION. A nuclear reaction induced by a photon. In some cases the reaction probably takes place via a compound nucleus formed by absorption of the photon followed by distribution of its energy among the nuclear constituents. One or more nuclear particles then "evaporate from the nuclear surface, or occasionally the nucleus undergoes pliotofissioii. In other cases the photon apparently interacts directly with a single nucleon, which is ejected as a photoneutron or photoproton without appreciable excitation of the rest of the nucleus. 

As o) increases further above 1 In3 a single photon drives the initially populated state closer and closer to the ionization limit, and ionization occurs with the absorption of fewer photons. Few photon processes are well described by lowest order perturbation theory, which shows that the rates are proportional to E2N, where N is the number of photons absorbed. For small N such processes are not well described by a threshold field, and it is not meaningful to discuss ionization threshold fields in this case. 

In atomic-molecular media the damping of plasmon states is due to the interaction of plasmon waves with electrons, lattice vibrations, and impurities. The electron-plasmon interaction is a long-range one. With absorption of a plasmon, the momentum q is transferred to the electron, resulting in a decay of the collective state into a single-particle one. The latter process is identical with absorption of a photon with the same energy. Wolff102 (see also Ref. 103) has shown that in this case the lifetime can be expressed in terms of two optical constants the absorption coefficient k and the refractive index nT, namely,... 

The selection rules will be mentioned briefly here. In general, the process of multiphoton absorption is similar to that of single-photon absorption. The multiple photons are absorbed simultaneously to a real excited state in the same quantum event, where the energy of the transition corresponds to the sum of the energies of the incident photons. Thus selection rules for these transitions may be derived from the selection rules for one-photon transitions as they can be considered multiple one-photon transitions [20]. 

This paper concentrates on a detailed description of the primary events occurring immediately after the absorption of a photon within a single titanium dioxide particle in an aqueous environment. This restriction was made, because 1) titanium dioxide seems to be the most active photocatalyst, and 2) the photocatalytic treatment of polluted water seems to be a promising application for an interfacial electron transfer serving the environment. 

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