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arXiv:1612.07105

Nonlinearity in the sequential absorption of multiple photons

Christian Buth

Published Dec 21, 2016• 3 citations
arXivHTMLPDF

Abstract

I classify multiphoton absorption into separable, linked, and simultaneous processes. The first and second types can be distinguished when the rate-equation approximation is valid whereas the third type refers to the case when the full description of multiphoton absorption is essential. For this purpose, rate equations are solved analytically without decay processes which shows that even if many photons are absorbed the interaction with the light field is linear and one has the case of separable multiphoton absorption. Next a short-pulse approximation is investigated in which I first solve the rate equations without decay processes and then solve only rate equations for the ensuing decay. Finally, the full rate equations are examined and a successive approximation of the underlying Volterra integral equation of the second kind is derived leading to linked multiphoton absorption by the involved decay widths. The three methods are applied to a nitrogen atom in intense and ultrafast x rays from free-electron lasers (FELs). The linearity theorem barely approximates the results in the presence of decay processes which is also not satisfactorily corrected for by the short-pulse approximation. The successive approximation gives excellent agreement with the numerically-exact solution of the rate equations.

DOI
10.48550/arxiv.1612.07105

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I classify multiphoton absorption into separable, linked, and simultaneous processes. The first and second types can be distinguished when the rate-equation approximation is valid whereas the third type refers to the case when the full description of multiphoton absorption is essential. For this purpose, rate equations are solved analytically without decay processes which shows that even if many photons are absorbed the interaction with the light field is linear and one has the case of separable multiphoton absorption. Next a short-pulse approximation is investigated in which I first solve the rate equations without decay processes and then solve only rate equations for the ensuing decay. Finally, the full rate equations are examined and a successive approximation of the underlying Volterra integral equation of the second kind is derived leading to linked multiphoton absorption by the involved decay widths. The three methods are applied to a nitrogen atom in intense and ultrafast x rays from free-electron lasers (FELs). The linearity theorem barely approximates the results in the presence of decay processes which is also not satisfactorily corrected for by the short-pulse approximation. The successive approximation gives excellent agreement with the numerically-exact solution of the rate equations.
New generations of ultrashort and intense laser pulses as well ashigh power synchrotron radiation sources and x-ray free electronlasers have promoted fast developments in nonlinear optics andx-ray spectroscopy.The new experimental achievements and the appearance of varieties of novelnonlinear phenomena call for further development of theories. The objective of this thesis is to develop and apply thetheories to explain existing experimental data and to suggest new experiments. The first part of the thesis is devoted to nonlinear propagation of optical pulses. It is shown that the vibrational levels can be selectively populated by varying the duration, shape and intensity of the pump pulse. We obtained a strict analytical solution for the resonant two-photon interaction in a multilevel system beyond rotating wave approximation. Simulations show that the polarization anisotropy of the two-photon excitation affects strongly the anisotropy of photobleaching.The two-photon area theorem is reformulated with taking into account the dynamical Stark shift and the contribution from the permanent dipole moments. In general the dynamical Stark shift does not allow complete population of the excited state, but it can be compensated by detunings in atoms. A dynamical theory of the sequential two-photon absorption of microsecond pulses is developed to explore the role of transverse inhomogeneity of the light beam on optical limiting properties. The propagation of ultrashort laser pulses in nondipolar and dipolar media is investigated with special attention to the generation of superfluorescence and supercontinuum and the formation of attosecond pulses. The second part of the thesis addresses the interaction of molecules with x-ray radiation. We explore here the role of nuclear dynamics in resonant Auger scattering. Multimode simulations of the Auger spectra of ethylene molecule explain the main spectral features of the experimental spectra and show that the spectral profiles are formed mainly due to six vibrational modes. We predict the Doppler splitting of the atomic peak in resonant Auger scattering from SF6 molecule for circularly polarized x-rays. This effect is confirmed by the recent experiment. A new scheme of x-ray pump-probe spectroscopy, namely, resonant inelastic x-ray scattering accompanied by core-hole hopping induced by strong laser fields is suggested. The laser-induced promotion of core holes opens the symmetry forbidden scattering channels and gives rise to new spectral lines in the x-ray scattering spectrum. The strength of the symmetry forbidden lines becomes strong when the time of Rabi flopping is shorter than the lifetime of the core-excited state. We study the role of propagation of femtosecond x-ray free-electron pulses on the Auger process. Simulations show that there exists a strong competition between Auger decay and stimulated emission. The Auger yield and Auger branching ratio are strongly suppressed in the course of pulse propagation.
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The dependence of the multiphoton absorption probability for an atomic system on the statistical properties of the incident light is investigated. It is shown, by means of nthn\mathrm{th}nth-order time-dependent perturbation theory, that the multiphoton absorption probability depends on the (n,n)th(n, n)\mathrm{th}(n,n)th normally ordered correlation functions of the electromagnetic field. For stationary fields, the transition probability per unit time is constant and is directly related to the reduced cross-spectral correlation function of the electromagnetic field. This expression for the transition probability is then analyzed under various conditions of coherence. Explicit calculations are carried out for thermal light and for laser light, and the transition rates are compared when each has a Lorentzian spectrum. In particular, when the width of the final atomic level is much larger than the bandwidth of the field, the transition rate for thermal light is nnn! times higher than with laser light of the same mean intensity. The other extreme case, i.e., when the width of the final atomic level is much smaller than the bandwidth of the field, is also considered in detail. An equation for the density operator of the field is derived; this equation governs the change in the statistical properties of the photon system in nnn-photon absorption processes. On the basis of this equation, the time-dependent properties of the photon system are then studied and some physical consequences of these equations are discussed. Some numerical solutions relating to the time dependence of the factorial moments in two-photon absorption processes are presented.
The non linear interaction between an intense laser radiation and atoms leads to ionization through the absorption of N photons from the laser radiation via laser-induced virtual states. The multiphoton ionization rate varies as a function of the laser intensity I as IN. We discuss the two most important effects which govern multiphoton ionization processes : resonance effects and laser-coherence effects. In a moderate laser intensity range (107 - 109 W cm-2) corresponding to the two, three or four-photon ionization of atoms, resonance effects play a dominant role while the photon statistics of the laser radiation are relatively unimportant. On the contrary, in the very high intensity range (1012 - 1013 W cm-2) required to observe large Nth - order ionization processes, coherence effects play a dominant role through N! enhancement in the N-photon ionization rate, while resonance effects are completely damped due to the high laser intensity. We conclude by reviewing the possible applications of multiphoton absorption processes in other fields.
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