Vollrath M. Axt

Femtosecond spectroscopy in semiconductors: a key to coherences, correlations and quantum kinetics

The application of femtosecond spectroscopy to the study of ultrafast dynamics in semiconductor materials and nanostructures is reviewed with particular emphasis on the physics that can be learned from it. Excitation with ultrashort optical pulses in general results in the creation of coherent superpositions and correlated many-particle states. The review comprises a discussion of the dynamics of this correlated many-body system during and after pulsed excitation as well as its analysis by means of refined measurements and advanced theories. After an introduction of basic concepts—such as coherence, correlation and quantum kinetics—a brief overview of the most important experimental techniques and theoretical approaches is given. The remainder of this paper is devoted to specific results selected in order to highlight how femtosecond spectroscopy gives access to the physics of coherences, correlations and quantum kinetics involving charge, spin and lattice degrees of freedom.First examples deal with the dynamics of basic laser-induced coherences that can be observed, e.g. in quantum beat spectroscopy, in coherent control measurements or in experiments using few-cycle pulses. The phenomena discussed here are basic in the sense that they can be understood to a large extent on the mean-field level of the theory. Nevertheless, already on this level it is found that semiconductors behave substantially differently from atomic systems. Subsequent sections report on the occurrence of coherences and correlations beyond the mean-field level that are mediated either by carrier–phonon or carrier–carrier interactions. The corresponding analysis gives deep insight into fundamental issues such as the energy–time uncertainty, pure dephasing in quantum dot structures, the role of two-pair or even higher correlations and the build-up of screening. Finally results are presented concerning the ultrafast dynamics of resonantly coupled excitations, where a combination of different interaction mechanisms is involved in forming new types of correlations. Examples are coupled plasmon–phonon and Bloch–phonon oscillations.The results reviewed in this paper clearly reveal the central role of many-particle correlations and coherences for the ultrafast dynamics of dense semiconductor systems. Both the presence of strong correlation effects and the formation of coherences in a genuine many-particle system have important implications for the controllability of optical signals from this class of materials, which is of utmost importance for applications in present-day and future optoelectronic devices.

Reducing decoherence of the confined exciton state in a quantum dot by pulse-sequence control

We study the phonon-induced dephasing of the exciton state in a quantum dot excited by a sequence of ultra-short pulses. We show that the multiple-pulse control leads to a considerable improvement of the coherence of the optically excited state. For a fixed control time window, the optimized pulsed control often leads to a higher degree of coherence than the control by a smooth single Gaussian pulse. The reduction of dephasing is considerable already for 2-3 pulses.

Extended Ginzburg-Landau formalism : Systematic expansion in small deviation from the critical temperature

Based on the Gor’kov formalism for a clean s-wave superconductor, we develop an extended version of the single-band Ginzburg-Landau (GL) theory by means of a systematic expansion in the deviation from the critical temperature Tc, i.e., τ = 1 − T/T c. We calculate different contributions to the order parameter and the magnetic field: the leading contributions (∝ τ 1/2 in the order parameter and ∝ τ in the magnetic field) are controlled by the standard GL theory, while the next-to-leading terms (∝ τ 3/2 in the gap and ∝ τ 2 in the magnetic field) constitute the extended GL (EGL) approach. We derive the free-energy functional for the extended formalism and the corresponding expression for the current density. To illustrate the usefulness of our formalism, we calculate, in a semianalytical form, the temperature-dependent correction to the GL parameter at which the surface energy becomes zero, and analytically, the temperature dependence of the thermodynamic critical field. We demonstrate that the EGL formalism is not just a mathematical extension to the theory: variations of both the gap and the thermodynamic critical field with temperature calculated within the EGL theory are found in very good agreement with the full BCS results down to low temperatures, which dramatically improves the applicability of the formalism compared to its standard predecessor.

Atypical BCS-BEC crossover induced by quantum-size effects

Quantum-size oscillations of the basic physical characteristics of a confined fermionic condensate are a well-known phenomenon. Its conventional understanding is based on the single-particle physics, whereby the oscillations follow the size-dependent changes in the single-particle density of states. Here we present a study of a cigar-shaped ultracold superfluid Fermi gas, which demonstrates an important many-body aspect of the quantum-size effects, overlooked previously. The many-body physics is revealed in the atypical crossover from the Bardeen-Cooper-Schrieffer (BCS) superfluid to the Bose-Einstein condensate (BEC) induced by the size quantization of the particle motion. Quantized perpendicular spectrum results in the formation of single-particle subbands (shells) so that the aggregate fermionic condensate becomes a coherent mixture of subband condensates. Each time when the lower edge of a subband crosses the chemical potential, the BCS-BEC crossover is approached in this subband, and the aggregate condensate contains both the BCS and BEC-like components.

Many-body effects in intersubband transitions of modulation-doped quantum wells

Abstract Based on the time-dependent Hartree–Fock equations we study many-body effects in the absorption spectra as well as temporally and spectrally resolved four-wave-mixing signals of modulation-doped quantum well structures. For sufficiently long dephasing times we find a beating behavior in the time-reolved signals related to the Coulomb enhancement.

Optical signals of spin switching using the optical Stark effect in a Mn-doped quantum dot

The optically induced spin dynamics of a single Mn atom embedded into a single semiconductor quantum dot can be strongly influenced by using the optical Stark effect. The exchange interaction gives rise to simultaneous spin flips between the quantum dot electron and Mn. In the time domain these flips correspond to exchange induced Rabi oscillations, which are typically off-resonant. By applying a detuned laser pulse, the states involved in the flipping can be brought into resonance by means of the optical Stark effect increasing the amplitude of the Rabi oscillations to one. In this paper we study theoretically how this spin dynamics can be monitored in time-resolved spectroscopy. In the spectrum the exchange interaction leads to a splitting of the exciton line into six lines, each corresponding to one of the six Mn spin states. The dynamical behavior of the Mn spin is reflected by the strength of the individual lines as a function of time. When an off-resonant optical pulse is applied the spectral positions of the lines shift, but still the flipping dynamics is visible.

Relaxation Dynamics of Electron–Hole Pairs Studied by Spatiotemporal Pump and Probe Experiments

The temporal evolution of the ambipolar diffusivity of optically excited electron–hole pairs is investigated for a strained quantum well structure by temporally and spatially resolved pump and probe experiments. Dependent on the excitation conditions the diffusivity transients reflect the cooling and heating processes of excitons as well as the formation dynamics of excitons out of free electron–hole pairs within less than 10 ps. Diffusivity transients obtained by Monte Carlo simulations of a simplified excitonic Boltzmann equation display all features of the experimental curves and support our interpretation of the lateral propagation dynamics in terms of formation, cooling and heating of excitons.

Comparison between a quantum kinetic theory of spin transfer dynamics in Mn-doped bulk semiconductors and its Markov limit for nonzero Mn magnetization

We investigate the transfer between carrier and Mn spins due to the s-d-exchange interaction in a Mn doped bulk semiconductor within a microscopic quantum kinetic theory. We demonstrate that the spin transfer dynamics is qualitatively different for components of the carrier spin parallel and perpendicular to the Mn magnetization. From our quantum kinetic equations we have worked out the corresponding Markov limit which is equivalent to rate equations based on Fermis golden rule. The resulting equations resemble the widely used Landau-Lifshitz-Gilbert-equations, but also describe genuine spin transfer due to quantum corrections. Although it is known that the Markovian rate description works well for bulk systems when the initial Mn magnetization is zero, we find large qualitative deviations from the full quantum kinetic theory for finite initial Mn magnetizations. These deviations mainly reflect corrections of higher than leading order in the interaction which are not accounted for in golden rule-type rates.

Influence of higher Coulomb correlations on optical coherent-control signals from a ZnSe quantum well

The manipulation of the coherent optical polarization in a quantum well with a pair of phase-locked laser pulses is investigated by using wave-mixing signals. The measurements are performed in four- and six-wave-mixing geometries with different polarization states of the excitation pulses. Even at moderate excitation densities, the signals are modulated by higher harmonics that correspond to high-order optical nonlinearities. A significant effect of higher Coulomb correlations on the coherent-control signals is demonstrated by comparing the experiments with calculations based on a microscopic density-matrix theory. The theoretical approach makes use of the dynamics-controlled truncation scheme. The corresponding numerical results are in good agreement with the experiment.

Nonlinear cavity feeding and unconventional photon statistics in solid-state cavity QED revealed by many-level real-time path-integral calculations

The generation of photons in a microcavity coupled to a laser-driven quantum dot interacting with longitudinal acoustic (LA) phonons is studied in the regime of simultaneously strong driving and strong dot-cavity coupling. The stationary cavity photon number is found to depend in a non-trivial way on the detuning between the laser and the exciton transition in the dot. In particular, the maximal efficiency of the cavity feeding is obtained for detunings corresponding to transition energies between cavity-dressed states with excitation numbers larger than one. Phonons significantly enhance the cavity feeding at large detunings. In the strong-driving, strong-coupling limit, the photon statistics is highly non-Poissonian. While without phonons a double-peaked structure in the photon distribution is predicted, phonons make the photon statistics thermal-like with very high effective temperatures