Canonical Transformation Approach to the Ultrafast Non-linear Optical Dynamics of Semiconductors

We develop a theory describing the effects of many-particle Coulomb correlations on the coherent ultrafast nonlinear optical response of semiconductors and metals. Our approach is based on a mapping of the nonlinear optical response of the ``bare'' system onto the linear response of a ``dressed'' system. The latter is characterized by effective time-dependent optical transition matrix elements, electron/hole dispersions, and interaction potentials, which in undoped semiconductors are determined by the single-exciton and two-exciton Green functions in the absence of optical fields. This mapping is achieved by eliminating the optically-induced charge fluctuations from the Hamiltonian using a Van Vleck canonical transformation. It takes into account all many-body contributions up to a given order in the optical fields as well as important Coulomb-induced quantum dynamics to all orders in the optical field. Our approach allows us to distinguish between optical nonlinearities of different origins and provides a physically-intuitive interpretation of their manifestations in ultrafast coherent nonlinear optical spectroscopy.Comment: 24 page

Adsorption and desorption of hydrogen at nonpolar GaN(1-100) surfaces: Kinetics and impact on surface vibrational and electronic properties

The adsorption of hydrogen at nonpolar GaN(1-100) surfaces and its impact on the electronic and vibrational properties is investigated using surface electron spectroscopy in combination with density functional theory (DFT) calculations. For the surface mediated dissociation of H2 and the subsequent adsorption of H, an energy barrier of 0.55 eV has to be overcome. The calculated kinetic surface phase diagram indicates that the reaction is kinetically hindered at low pressures and low temperatures. At higher temperatures ab-initio thermodynamics show, that the H-free surface is energetically favored. To validate these theoretical predictions experiments at room temperature and under ultrahigh vacuum conditions were performed. They reveal that molecular hydrogen does not dissociatively adsorb at the GaN(1-100) surface. Only activated atomic hydrogen atoms attach to the surface. At temperatures above 820 K, the attached hydrogen gets desorbed. The adsorbed hydrogen atoms saturate the dangling bonds of the gallium and nitrogen surface atoms and result in an inversion of the Ga-N surface dimer buckling. The signatures of the Ga-H and N-H vibrational modes on the H-covered surface have experimentally been identified and are in good agreement with the DFT calculations of the surface phonon modes. Both theory and experiment show that H adsorption results in a removal of occupied and unoccupied intragap electron states of the clean GaN(1-100) surface and a reduction of the surface upward band bending by 0.4 eV. The latter mechanism largely reduces surface electron depletion

Nonmonotonic Decay of Nonequilibrium Polariton Condensate in Direct-Gap Semiconductors

Time evolution of a nonequilibrium polariton condensate has been studied in the framework of a microscopic approach. It has been shown that due to polariton-polariton scattering a significant condensate depletion takes place in a comparatively short time interval. The condensate decay occurs in the form of multiple echo signals. Distribution-function dynamics of noncondensate polaritons have been investigated. It has been shown that at the initial stage of evolution the distribution function has the form of a bell. Then oscillations arise in the contour of the distribution function, which further transform into small chaotic ripples. The appearance of a short-wavelength wing of the distribution function has been demonstrated. We have pointed out the enhancement and then partial extinction of the sharp extra peak arising within the time interval characterized by small values of polariton condensate density and its relatively slow changes.Comment: 20 pages, LaTeX 2.09; in press in PR

A Cantor set of tori with monodromy near a focus-focus singularity

We write down an asymptotic expression for action coordinates in an integrable Hamiltonian system with a focus-focus equilibrium. From the singularity in the actions we deduce that the Arnol'd determinant grows infinitely large near the pinched torus. Moreover, we prove that it is possible to globally parametrise the Liouville tori by their frequencies. If one perturbs this integrable system, then the KAM tori form a Whitney smooth family: they can be smoothly interpolated by a torus bundle that is diffeomorphic to the bundle of Liouville tori of the unperturbed integrable system. As is well-known, this bundle of Liouville tori is not trivial. Our result implies that the KAM tori have monodromy. In semi-classical quantum mechanics, quantisation rules select sequences of KAM tori that correspond to quantum levels. Hence a global labeling of quantum levels by two quantum numbers is not possible.Comment: 11 pages, 2 figure

Pump Built-in Hamiltonian Method for Pump-Probe Spectroscopy

We propose a new method of calculating nonlinear optical responses of interacting electronic systems. In this method, the total Hamiltonian (system + system-pump interaction) is transformed into a different form that (apparently) does not have a system-pump interaction. The transformed Hamiltonian, which we call the pump built-in Hamiltonian, has parameters that depend on the strength of the pump beam. Using the pump built-in Hamiltonian, we can calculate nonlinear responses (responses to probe beams as a function of the pump beam) by applying the {\em linear} response theory. We demonstrate the basic idea of this new method by applying it to a one-dimensional, two-band model, in the case the pump excitation is virtual (coherent excitation). We find that the exponent of the Fermi edge singularity varies with the pump intensity.Comment: 6 page

Ultrafast Coulomb-induced dynamics of 2D magnetoexcitons

We study theoretically the ultrafast nonlinear optical response of quantum well excitons in a perpendicular magnetic field. We show that for magnetoexcitons confined to the lowest Landau levels, the third-order four-wave-mixing (FWM) polarization is dominated by the exciton-exciton interaction effects. For repulsive interactions, we identify two regimes in the time-evolution of the optical polarization characterized by exponential and {\em power law} decay of the FWM signal. We describe these regimes by deriving an analytical solution for the memory kernel of the two-exciton wave-function in strong magnetic field. For strong exciton-exciton interactions, the decay of the FWM signal is governed by an antibound resonance with an interaction-dependent decay rate. For weak interactions, the continuum of exciton-exciton scattering states leads to a long tail of the time-integrated FWM signal for negative time delays, which is described by the product of a power law and a logarithmic factor. By combining this analytic solution with numerical calculations, we study the crossover between the exponential and non-exponential regimes as a function of magnetic field. For attractive exciton-exciton interaction, we show that the time-evolution of the FWM signal is dominated by the biexcitonic effects.Comment: 41 pages with 11 fig

Pseudogap phase formation in the crossover from Bose-Einstein condensation to BCS superconductivity

A phase diagram for a 2D metal with variable carrier density has been derived. It consists of a normal phase, where the order parameter is absent; a so-called ``abnormal normal'' phase where this parameter is also absent but the mean number of composite bosons (bound pairs) exceeds the mean number of free fermions; a pseudogap phase where the absolute value of the order parameter gradually increases but its phase is a random value, and finally a superconducting (here Berezinskii-Kosterlitz-Thouless) phase. The characteristic transition temperatures between these phases are found. The chemical potential and paramagnetic susceptibility behavior as functions of the fermion density and the temperature are also studied. An attempt is made to qualitatively compare the resulting phase diagram with the features of underdoped high-$T_{c}$ superconducting compounds above their critical temperature.Comment: 26 pages, revtex, 5 EMTeX figures; more discussion and references added; to be published in JET

Theory of exciton-exciton correlation in nonlinear optical response

We present a systematic theory of Coulomb interaction effects in the nonlinear optical processes in semiconductors using a perturbation series in the exciting laser field. The third-order dynamical response consists of phase-space filling correction, mean-field exciton-exciton interaction, and two-exciton correlation effects expressed as a force-force correlation function. The theory provides a unified description of effects of bound and unbound biexcitons, including memory-effects beyond the Markovian approximation. Approximations for the correlation function are presented.Comment: RevTex, 35 pages, 10 PostScript figs, shorter version submitted to Physical Review

Optical absorption in semiconductor quantum dots: Nonlocal effects

The optical absorption of a single spherical semiconductor quantum dot in an electrical field is studied taking into account the nonlocal coupling between the field of the light and the polarizability of the semiconductor. These nonlocal effects lead to a small size anf field dependent shift and broadening of the excitonic resonance which may be of interest in future high precision experiments.Comment: 6 pages, 4 figure

Effective Hamiltonian for Excitons with Spin Degrees of Freedom

Starting from the conventional electron-hole Hamiltonian ${\cal H}_{eh}$, we derive an effective Hamiltonian $\tilde{\cal H}_{1s}$ for $1s$ excitons with spin degrees of freedom. The Hamiltonian describes optical processes close to the exciton resonance for the case of weak excitation. We show that straightforward bosonization of ${\cal H}_{eh}$ does not give the correct form of $\tilde{\cal H}_{1s}$, which we obtain by a projection onto the subspace spanned by the $1s$ excitons. The resulting relaxation and renormalization terms generate an interaction between excitons with opposite spin. Moreover, exciton-exciton repulsive interaction is greatly reduced by the renormalization. The agreement of the present theory with the experiment supports the validity of the description of a fermionic system by bosonic fields in two dimensions.Comment: 12 pages, no figures, RevTe