Energy Approach to Atoms in a Laser Field and Quantum Dynamics with Laser Pulses of Different Shapes 161 strong nonlinear coupling of radiation with atoms which can not fully explained by the modern theoretical models.In any case the problem requires a consistent quantum electrodynamic approach.Another important topic is a problem of governing and control of non-linear processes in a stochastic, multi-mode laser field (Grance, 1981;Lompre et al, 1981;Zoller, 1982; Glushkov & Ivanov, 1992).The principal aim of quantum coherent control is to steer a quantum system towards a desired final state through interaction with light while simultaneously inhibiting paths leading to undesirable outcomes.This type of quantum interference is inherent in non-linear multiphoton processes.Controlling mechanisms have been proposed and demonstrated for atomic, molecular and solid-state systems (Goldansky-Letokhov, 1974, Letokhov, 1977;Delone-Kraynov, 1984).Theoretical studies of the laser-atom nonlinear interactions are often based on solving the time-dependent Schrödinger equation or using the time-independent Floquet formalism or special perturbation theories (Brändas &
Energy Approach to Atoms in a Laser Field and Quantum Dynamics with Laser Pulses of Different Shapes 161 strong nonlinear coupling of radiation with atoms which can not fully explained by the modern theoretical models.In any case the problem requires a consistent quantum electrodynamic approach.Another important topic is a problem of governing and control of non-linear processes in a stochastic, multi-mode laser field (Grance, 1981;Lompre et al, 1981;Zoller, 1982; Glushkov & Ivanov, 1992).The principal aim of quantum coherent control is to steer a quantum system towards a desired final state through interaction with light while simultaneously inhibiting paths leading to undesirable outcomes.This type of quantum interference is inherent in non-linear multiphoton processes.Controlling mechanisms have been proposed and demonstrated for atomic, molecular and solid-state systems (Goldansky-Letokhov, 1974, Letokhov, 1977;Delone-Kraynov, 1984).Theoretical studies of the laser-atom nonlinear interactions are often based on solving the time-dependent Schrödinger equation or using the time-independent Floquet formalism or special perturbation theories (Brändas &
Quantum mechanics, though a probabilistic theory, gives a 'deterministic' answer to the question of how the present determines the future. In essence, in order to predict future probabilities, we need to (numerically) propagate the time-dependent Schrödinger equation from the present to the future. It is interesting to note that classical mechanics of macroscopic bodies, though reputed to be a deterministic theory, does not allow, due to chaos (which unfortunately is more prevalent than integrability), such clear insights into the future. In contrast, small (e.g., atomic, molecular and photonic) systems which are best understood using the tools of quantum mechanics, do not suffer from chaos, rendering the prediction of the probability-distributions of future events possible. The field of quantum control deals with an important modification of this task, namely, it asks: given a wave function in the present, what dynamics, i.e. what Hamiltonian, guarantees a desired outcome or 'objective' in the future? In practice one may achieve this goal of modifying and finding the desired Hamiltonian by introducing external fields, e.g. laser light. It is then possible to reach the objective in a 'trial-and-error' fashion, performed either numerically or in the laboratory. We can guess or build a Hamiltonian, do an experiment, or propagate the initial wave function to the future, compare the result with the desirable objective, and correct the guess for the Hamiltonian until satisfactory agreement with the objective is reached. A systematic way of executing this procedure is the sub-field called 'optimal control'. The trial-and-error method is often very time consuming and rarely provides mechanistic insight. There are situations where analytical solutions exist, rendering the control strategies more transparent. This is especially so when one can identify quantum interferences as the heart of quantum control, the essence of the field called 'coherent control'. The experience accumulated so far by many groups is that quantum interferences are the mechanism underlying most successful control scenarios and control experiments. The identification of the control mechanism is especially facile when the time-dependence of the Hamiltonian merely serves to prepare a state which then evolves in the absence of external fields. Analytical theories also exist when the explicit time dependence of the Hamiltonian can be treated adiabatically. Under these circumstances one can identify the quantum interfering pathways that lead to control, allowing for the simultaneous exploration of entire 'landscapes' (and not just a single 'desirable' objective) resulting from varying all the experimental 'knobs' at our disposal, e.g., relative- and envelope-phases, intensities, polarizations, and pulse-sequencing. Such 'pulse-shaping' knobs are now available down to the sub-femtosecond regime in broad spectral regions ranging from the UV to the IR. We expect that comprehensive investigations of the quantum interference required to control dynamical processes will result in a more detailed understanding of the dynamics themselves. Together with experimental progress---the stage is now set for many exciting applications in fundamental and applied sciences by 'tailoring' light--matter interactions essentially at will.
We study the general problem of matter-laser interaction within the framework of nonrelativistic quantum electrodynamics, with particular emphasis on strong laser field effects. Consequently, we formulate a well-defined approximation leading in a straightforward manner toward the conventional semiclassical mode of description. Namely, we arrive naturally to two coupled equations of motion: (i) the Schr\"odinger equation which governs the quantum dynamics of an atomic system driven by classically described radiation field (composed of an incoming laser pulse plus radiation emitted from the atom), and (ii) the classical Maxwell wave equation which describes the emission of radiation from the mentioned atomic source. Employing the formalism of adiabatic Floquet theory, we derive a simple criterion of validity of the just described semiclassical approach. It shows that the semiclassical treatment is justified in most situations. On the other hand, it turns out that the semiclassical approximation breaks down completely in certain special but realistic cases, regardless of the fact that the incoming laser pulse contains a huge number of photons. Under such special circumstances, we anticipate new effects arising due to the quantized nature of the radiation field, to be observable, for example, in harmonic generation spectra. Our considerations are illustrated more explicitly using a simple model of a two-level atom strongly driven by a laser. The quantum dynamics of this model problem is resolved within the framework of quantum electrodynamics while adopting well-defined and physically justifiable approximations. As an outcome, analytic formulas are found serving as a quantitative criterion of (non)applicability of the semiclassical approach and demonstrating the breakdown of semiclassical theory under well-defined conditions. An illustrative numerical calculation is provided.
In this chapter,we shall analyze the particular case of an atom interacting with a laser pulse whose duration is sufficiently long, so that the evolution of the atom in the laser field is adiabatic. When this condition is fulfilled, the atom can be considered to interact with a monochromatic laser field. As a consequence, the Hamiltonian of the system is periodic in time, and the Floquet theory [1] can be used to solve the time-dependent Schrödinger equation (TDSE) non-perturbatively. We begin in Section 4.1 by considering the Hermitian Floquet theory. We first derive the Floquet theorem for a monochromatic, spatially homogeneous laser field and show that the solutions of the TDSE correspond to dressed states having real quasi-energies , which can be obtained by solving an infinite system of time-independent coupled equations. We then generalize the Floquet theory to multicolor laser fields and to “non-dipole” laser fields which are not spatially homogeneous. In Section 4.2, the Floquet theory is applied to study the dynamics of a model atom having M discrete levels interacting with a monochromatic laser field. In this case, the coupling between the bound and continuum atomic states is neglected.We analyze the relationship between the Floquet theory and the rotating wave approximation, and examine the perturbative limit of the Floquet theory. We also consider the population transfer between Floquet dressed states.
The resonant multiphoton resonances shifts and widths and ionization cross-sections for multielectron atoms in a intense laser radiation field are studied. It is carried out a new consistent approach to atom in a strong realistic laser field, based on the relativistic energy formalism (S-matrix adiabatic formalism), relativistic Dirac equation Green function method and relativistic many-body perturbation theory with the Dirac-Kohn-Sham zeroth approximation. In relativistic theory, the Gell-Mann and Low adiabatic formula for energy shift is connected with electrodynamical scattering matrice, which includes interaction with as a laser field as a photon vacuum field (radiative decay). The optimized basis of the relativistic orbitals is generated with using a minimization procedure for the gauge-non-invariant contribution (the fourth-order of the QED perturbation theory) to the radiation width of atomic state. An approach to treating the multiphoton atomic processes is outlined on example of H, Cs, Kr,Mg etc. Analysis shows that the shift and width of the multi-photon resonance line for the interaction “atom- multimode laser pulse” is greater than the corresponding shift and width for a case of the “atom- single-mode pulse” (the Lorenz pulse model) interaction. From the physical point of view it is naturally provided by action of the photon-correlation effects and influence of the laser pulse multi-modity.
In this thesis, we present work on coherent control of multilevelquantum systems in the strong field limit using shaped ultrafastlaser pulses. In recent years there have been numerous multiphotonabsorption experiments in two,three, and four-level atomic/molecularsystems and many are performed in the limit of weak fields whereperturbation theory is valid. Here, we describe a series ofexperiments aimed at exploring and understanding multiphotontransitions when the exciting field is strong and perturbationtheory breaks down. Our approach to strong field control utilizesboth parameterized scans of various pulse shapes and closed-looplearning control to identify a pulse shape that is optimal forpopulating a target quantum state. With this we will highlight thedifference between sequential population transfer and adiabaticrapid passage in multilevel systems with multiphoton couplingbetween levels. Additionally, we examine strong field control of afour-level atomic interferometer and show how interference in atarget state changes from resonant pathways in the frequency domainto time-domain interference via a singe path.Further, we use shaped femtosecond pulses to demonstrate aphenomenon in which a three-level atom becomes a modulator of anultrafast pulse. The results are based on a pump-probe scheme thatis very similar to Electromagnetically Induced Transparency (EIT).Important dynamics associated with a time-dependent coupling fieldare examined. Lastly, we extend previous work on two-photon drivensuperfluorescence from a shaped ultrafast drive laser and show howstimulated emission near threshold can turn modest coherent controlyields into essentially perfect discrimination between systems wherea control factor of about 104 is achieved between atomic andmolecular species.
In this chapter we use the Langevin (Brownian motion) method of Chap. 19 to once again treat quantum mechanically both the field and the active atoms in a laser. The present treatment comprises a Heisenberg picture approach to the problem, as compared to the approach in Chap. 17, which represents the Schrodinger picture. The two methods are in complete agreement (as they should be!), a point discussed in some detail by Lax (1968). As before, the atoms are considered to comprise systems which interact with independent pumping and dissipation reservoirs, and the laser field is regarded as another system with reservoirs. The atom and field systems are then coupled by an electric-dipole perturbation energy, as depicted schematically in Fig. 20-1.