Decaying atomic transitions, quantum

The interest in quantum interference stems from the early 1970s when Agarwal [4] showed that the ordinary spontaneous decay of an excited degenerate V-type three-level atom can be modified due to interference between the two atomic transitions. The analysis of quantum interference has since been extended to other configurations of three- and multilevel atoms and many interesting effects have been predicted, which can be used to control optical properties of quantum systems, such as high-contrast resonances [5,6], electro-magnetically induced transparency [7], amplification without population inversion [8], and enhancement of the index of refraction without absorption [9]. 

Another area of interest in quantum interference effects, which has been studied extensively, is the response of a V-type three-level atom to a coherent laser field directly coupled to the decaying transitions. This was studied by Cardimona et al. [36], who found that the system can be driven into a trapping state in which quantum interference prevents any fluorescence from the excited levels, regardless of the intensity of the driving laser. Similar predictions have been reported by Zhou and Swain [5], who have shown that ultrasharp spectral lines can be predicted in the fluorescence spectrum when the dipole moments of the atomic transitions are nearly parallel and the fluorescence can be completely quenched when the dipole moments are exactly parallel. 

Transition, Isomeric—The process by which a nuclide decays to an isomeric nuclide (i.e., one of the same mass number and atomic number) of lower quantum energy. Isomeric transitions (often abbreviated I.T.) proceed by gamma ray and/or internal conversion electron emission. 

Figure 14. (a) Potential-energy surfaces, with a trajectory showing the coherent vibrational motion as the diatom separates from the I atom. Two snapshots of the wavepacket motion (quantum molecular dynamics calculations) are shown for the same reaction at / = 0 and t = 600 fs. (b) Femtosecond dynamics of barrier reactions, IHgl system. Experimental observations of the vibrational (femtosecond) and rotational (picosecond) motions for the barrier (saddle-point transition state) descent, [IHgl] - Hgl(vib, rot) + I, are shown. The vibrational coherence in the reaction trajectories (oscillations) is observed in both polarizations of FTS. The rotational orientation can be seen in the decay of FTS spectra (parallel) and buildup of FTS (perpendicular) as the Hgl rotates during bond breakage (bottom). 

It is very important, in the theory of quantum relaxation processes, to understand how an atomic or molecular excited state is prepared, and to know under what circumstances it is meaningful to consider the time development of such a compound state. It is obvious, but nevertheless important to say, that an atomic or molecular system in a stationary state cannot be induced to make transitions to other states by small terms in the molecular Hamiltonian. A stationary state will undergo transition to other stationary states only by coupling with the radiation field, so that all time-dependent transitions between stationary states are radiative in nature. However, if the system is prepared in a nonstationary state of the total Hamiltonian, nonradiative transitions will occur. Thus, for example, in the theory of molecular predissociation4 it is not justified to prepare the physical system in a pure Born-Oppenheimer bound state and to force transitions to the manifold of continuum dissociative states. If, on the other hand, the excitation process produces the system in a mixed state consisting of a superposition of eigenstates of the total Hamiltonian, a relaxation process will take place. Provided that the absorption line shape is Lorentzian, the relaxation process will follow an exponential decay. 

As described in the main text of this section, the states of systems which undergo radiationless transitions are basically the same as the resonant scattering states described above. The terminology resonant scattering state is usually reserved for the case where a true continuum is involved. If the density of states in one of the zero-order subsystems is very large, but finite, the system is often said to be in a compound state. We show in the body of this section that the general theory of quantum mechanics leads to the conclusion that there is a set of features common to the compound states (or resonant scattering states) of a wide class of systems. In particular, the shapes of many resonances are very nearly the same, and the rates of decay of many different kinds of metastable states are of the same functional form. It is the ubiquity of these features in many atomic and molecular processes that we emphasize in this review. 

Since the radiative lifetime is nearly independent of v (852), it can be seen that the measured decay rate 1/t is proportional to kp, which in turn is proportional to the quantum yield of I atom production. Therefore, the wavelength dependence of decay rate follows approximately the quantum yield curve shown in Fig. V-22, that is, the decay rate is faster when the quantum yield of atom production is larger. However, the exact correspondence may not be expected, since both the B3n and ln states contribute to the 1 atom production, while only the B3n state gives rise to fluorescence. Then the percent absorption due to a transition to the B3fl state must be known at each wavelength. 

The finite lifetime of each excited state is the reflection of a fundamental law of nature - tendency towards minimum total energy of a system. The quantum mechanical system tends to occupy the state in which its total energy would be minimal. However, the transition of an atom to the lowest (ground) state depends on many circumstances (first of all, on the sort of excited configuration, on the presence of external fields, on the character of the matter itself - density of gas, vapours or plasma, etc.). There are two main channels of decay of the excited states radiative and radiationless. In the first case the electronic transition from the higher to the lower state is connected with the radiation of one or several quanta of... 

Turning to molecular physics, we note first papers by Ya.B. which are close to the problem of phase transition. We begin with the theory of interaction of an atom with a metal (11). By applying quantum-mechanical perturbation theory to the interaction of the virtual dipole moment of an atom with conducting electrons of the metal, the dependence on distance of the attractive force of the atom to the surface is obtained. The calculation led to a slow, r2, law for the potential energy decay with distance. This paper was published in 1935, and for many years remained essentially the only one devoted to the subject. 

Luminescence originates from electronically excited states in atoms and molecules and the emission process is governed by quantum mechanical selection rules. Forbidden transitions generally are slower than allowed optical transitions. Emission originating from allowed optical transitions, with decay times of the order of ps or faster is called fluorescence the term for emission with longer decay times is phosphorescence. The time in which the emission intensity decreases to 1/e or 1/10 (for exponential decay and hyperbolic decay, respectively) is called the decay time. 

The effect of quantum interference on spontaneous emission in atomic and molecular systems is the generation of superposition states that can be manipulated, to reduce the interaction with the environment, by adjusting the polarizations of the transition dipole moments, or the amplitudes and phases of the external driving fields. With a suitable choice of parameters, the superposition states can decay with controlled and significantly reduced rates. This modification can lead to subnatural linewidths in the fluorescence and absorption spectra [5,10]. Furthermore, as will be shown in this review, the superposition states can even be decoupled from the environment and the population can be trapped in these states without decaying to the lower levels. These states, known as dark or trapped states, were predicted in many configurations of multilevel systems [11], as well as in multiatom systems [12],... 

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