We employ the Dynamical Projective Operatorial Approach (DPOA) to investigate the ultrafast optical excitations of germanium under intense, ultrashort pump pulses. The method has very low resource demand relative to many other available approaches and enables detailed calculation of the residual electron and hole populations induced by the pump pulse. It provides direct access to the energy distribution of excited carriers and to the total energy transferred to the system. By decomposing the response into contributions from different multi-photon resonant processes, we systematically study the dependence of excited-carrier density and absorbed energy on key pump-pulse parameters: duration, amplitude, and photon energy. Our results reveal a complex interplay between these parameters, governed by resonant Rabi-like dynamics and competition between different multi-photon absorption channels. For the studied germanium setup, we find that two-photon processes are generally dominant, while one- and three-photon channels become significant under specific conditions of pump-pulse frequency, duration, and intensity. This comprehensive analysis offers practical insights for optimizing ultrafast optical control in semiconductors by targeting specific multi-photon pathways.
We employ the Dynamical Projective Operatorial Approach (DPOA) to investigate the ultrafast optical excitations of germanium under intense, ultrashort pump pulses. The method has very low resource demand relative to many other available approaches and enables detailed calculation of the residual electron and hole populations induced by the pump pulse. It provides direct access to the energy distribution of excited carriers and to the total energy transferred to the system. By decomposing the response into contributions from different multi-photon resonant processes, we systematically study the dependence of excited-carrier density and absorbed energy on key pump-pulse parameters: duration, amplitude, and photon energy. Our results reveal a complex interplay between these parameters, governed by resonant Rabi-like dynamics and competition between different multi-photon absorption channels. For the studied germanium setup, we find that two-photon processes are generally dominant, while one- and three-photon channels become significant under specific conditions of pump-pulse frequency, duration, and intensity. This comprehensive analysis offers practical insights for optimizing ultrafast optical control in semiconductors by targeting specific multi-photon pathways.
Recent experimental advancements in ultrafast pump-probe setups drive a growing need for efficient and insightful theoretical methods. This study will delve into the intricacies of our newly developed approach, the Dynamical Projective Operatorial Approach (DPOA). DPOA stands out as a highly efficient model-Hamiltonian method capable of calculating a wide range of single/multi-time single/multi-particle properties, such as excitation populations, out-of-equilibrium Green's functions, TR-ARPES signals, and various response functions. When dealing with transient optical properties, utilizing the DPOA formulation and capitalizing on the weak intensity of the probe pulse, we efficiently compute the linear response of the pumped system to a generic probe pulse, significantly accelerating calculations. Alongside the theoretical framework, we present noteworthy results that experimentalists can utilize to establish connections between observed effects and their underlying physical phenomena.
Femtosecond-pulse propagation in resonantly excited semiconductors is investigated by numerically solving the semiconductor Maxwell-Bloch equations for plane waves. For excitation at the exciton resonance, it is shown that the pulse absorption exhibits a strongly nonlinear dependence on the input pulse area. Very long propagation distances for strong pulses are observed, but even when all dephasing processes have been neglected, no lossless propagation (self-induced transparency) was found. The influence of the electron-hole many-body effects, nonequilibrium carrier relaxation, and optical dephasing on the pulse-propagation dynamics is studied. The exchange interaction in the electron-hole plasma is shown to support large propagation distances. For excitation of the continuum states, the dependence of the absorption on the intensity of the input pulse is reduced due to the rapid carrier relaxation into quasiequilibrium distributions.
The coherent response of a semiconductor three-state system to one or two intense light pulses is investigated experimentally on a 100 fs time scale. Three experiments constitute this dissertation: observation of excitonic Rabi oscillations, measurement of two-exciton coupled Stark shifting, and an attempt to observe dark states. Basic concepts of time-resolved ultrafast semiconductor spectroscopy are explained, followed by an analysis of semiconductor two- and three-state systems. Pure two- and three-state dynamics are derived from first principles, followed by the development of the appropriate semiconductor Bloch equations (SBE). Two-color pump-probe, two-color pump-pump, and pump-pump-probe techniques are explained in the context of three-state semiconductor experiments. The experimental setup is explained in detail. Resonant two-color pump-probe measurements resulted in the first observation of multiple excitonic Rabi oscillations. The common conduction band shared by the light-hole and heavy-hole excitons of an InGaAs multiple quantum well allowed us to measure hh-exciton density (Rabi) oscillations by probing lh-exciton absorption. By studying the intensity dependence of the Rabi frequency, we showed the important role of many-body effects in renormalizing the dipole energy. The shared conduction band also causes the lh-exciton resonance to Stark shift when the hh exciton is Stark shifted. We measured a transient Stark shifting of both resonances due to virtual hh-exciton transitions. We observed that the ratio of the hh-exciton shift to lh-exciton shift was 2:1 at large pump-exciton detuning, as predicted from a simple three-state dressed exciton picture. For smaller detunings we saw an increase in the ratio and a redshift of the non-dipole coupled exciton state. Both of these observations are consistent with the most recent theories and experiments on excitonic Stark shifting. For strong near-resonant pumping of both lh- and hh-exciton transitions, an intervalence-band Raman-type coherence follows from the SBE that results in a transparent eigenstate (dark state) when both pumps are equally detuned from resonance. The existence of this coherence is well-known in atomic-optical systems, but has been elusive in semiconductors. Our inconclusive experimental result is presented along with an evaluation of experimental shortcomings. In brief, the expected change is absorption was too small to see.
Excitation-induced many-body effects play an important role in semiconductor quantum materials, where ultrafast processes determine the system properties. These effects occur when light excitations dynamically alter light absorption and emission, leading to nonlinear, excitation-induced changes in a semiconductor's optical response. This thesis theoretically investigates ultrafast excitation-induced effects in semiconductor nanostructures. Specifically, using a first-principles analysis based on quantum dynamic cluster expansion, we implement a systematic approach to describe the dynamics of microscopic polarizations and carrier occupations in semiconductor quantum materials precisely, with Coulomb-induced scattering fully included. We explore the dynamic buildup of excitation-induced effects, and develop a quantum memory model to precisely describe it. We also do a perturbative study on the third-order nonlinearities and propose a method based on it to measure the build-up time of excitation-induced effects via ultrafast experiments. Utilizing these theoretical tools, we successfully guided experiments to detect ultrafast processes. We successfully observed the time-delayed buildup of dephasing from the experiments and demonstrated a reversible ultrafast switching that can be switched within femtosecond time scale and is capable for hundreds of switching operations. We also identified nonperturbative ultrafast nonlinearities in the carbon nanotube, with the nonlinear refractive indices orders of magnitude higher than those found from other materials, explained by the strong excitation-induced effects. Our findings are crucial for quantum photonic applications. They offer significant insights into the fundamental quantum processes relevant to ultrafast photonics and open up new possibilities for quantum information and quantum optoelectronics technologies.
Quantitative control and measurement of quantum entanglement are essential for advancing quantum technologies. Photoionization induced by ultrashort laser pulses provides a unique platform for studying entanglement between photoelectrons and residual ions, representing one of the most intriguing quantum phenomena in attosecond physics. Although extensive studies have focused on the coherence properties within either the emitted electrons or the ions individually, the electron-ion entanglement has remained largely unexplored. In this work, we bridge this gap by investigating the resonance-enhanced multiphoton ionization of argon atoms driven by two time-delayed ultrashort ultraviolet pulses. Employing state-of-the-art first-principles multi-electron simulations, we demonstrate the ability to reconstruct and precisely manipulate the purity of electron quantum states through detailed analysis of the photoelectron angular distributions. Our results reveal distinct scattering-phase differences among various electron configurations within the same partial wave channel, providing unequivocal evidence of electron-ion correlation and entanglement. With the fast development of free-electron lasers, this study establishes an experimentally feasible framework for directly controlling quantum entanglement in ultrafast ionization processes, offering new insights and powerful methodologies for exploring complex electron dynamics in many-electron systems.
Within the framework of light-semiconductor interaction and the Lutting-Kohn model for the semiconductor band structure, we theoretically studied the mechanism of the polarization switch with coherent transient features. The result shows, in the coherent limitation, when the pump pulse Ep and signal pulse Es are orthogonal polarized, the third order polarization P(3), with first order of Es and second order of |Ep|, approach to zero, due to the destructive quantum interference, which results in an ultrafast pump-signal relative polarization dependent P(3), therewith a polarization switch. The study also shows that, when the light interacts with semiconductors coherently, the polarization state of the light is transferred to the relative phase of the electron spin, rather than the electron spin itself. The population of the polarization eigenstate excited by the pump pulse, do not origin from the Coulomb force of electrons, and should not thought phenomenologically as the exciton characterized by light polarization. This population will dephase to real carriers population, i.e. electron with exact spin |↑> or |↓>, by losing phase coefficients of the polarization eigenstates, in an ultrashort quantum dephase time.