Influence of Coulomb and Phonon Interaction on the Exciton Formation Dynamics in Semiconductor Heterostructures

A microscopic theory is developed to analyze the dynamics of exciton formation out of incoherent carriers in semiconductor heterostructures. The carrier Coulomb and phonon interaction is included consistently. A cluster expansion method is used to systematically truncate the hierarchy problem. By including all correlations up to the four-point (i.e. two-particle) level, the fundamental fermionic substructure of excitons is fully included. The analysis shows that the exciton formation is an intricate process where Coulomb correlations rapidly build up on a picosecond time scale while phonon dynamics leads to true exciton formation on a slow nanosecond time scale.Comment: 18 pages, 7 figure

Controlling Defect Formation of Nanoscale AlN: Toward Efficient Current Conduction of Ultrawide‐Bandgap Semiconductors

Ultrawide‐bandgap semiconductors such as AlN, BN, and diamond hold tremendous promise for high‐efficiency deep‐ultraviolet optoelectronics and high‐power/frequency electronics, but their practical application has been limited by poor current conduction. Through a combined theoretical and experimental study, it is shown that a critical challenge can be addressed for AlN nanostructures by using N‐rich epitaxy. Under N‐rich conditions, the p‐type Al‐substitutional Mg‐dopant formation energy is significantly reduced by 2 eV, whereas the formation energy for N‐vacancy related compensating defects is increased by ≈3 eV, both of which are essential to achieve high hole concentrations of AlN. Detailed analysis of the current−voltage characteristics of AlN p‐i‐n diodes suggests that current conduction is dominated by hole‐carrier tunneling at room temperature, which is directly related to the activation energy of Mg dopants. At high Mg concentrations, the dispersion of Mg acceptor energy levels leads to drastically reduced activation energy for a portion of Mg dopants, evidenced by the small tunneling energy of 67 meV, which explains the efficient current conduction and the very small turn‐on voltage (≈5 V) for the diodes made of nanoscale AlN. This work shows that nanostructures can overcome the dopability challenges of ultrawide‐bandgap semiconductors and significantly increase the efficiency of devices.Controlled defects formation and efficient current conduction of nanoscale AlN are realized. Under N‐rich epitaxy conditions, the formation energy for N‐vacancy related compensating defects is increased by nearly 3 eV, eliminating donor‐like compensating defects. Meanwhile, the p‐type Al‐substitutional Mg‐dopant formation energy is reduced by 2 eV, significantly enhancing Mg‐dopant incorporation and reducing hole carrier tunneling barrier.Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/162750/3/aelm202000337-sup-0001-SuppMat.pdfhttp://deepblue.lib.umich.edu/bitstream/2027.42/162750/2/aelm202000337_am.pdfhttp://deepblue.lib.umich.edu/bitstream/2027.42/162750/1/aelm202000337.pd

Controlling the polarization dynamics by strong THz fields in photoexcited germanium quantum wells

The interaction of strong single-cycle THz pulses with the optically induced polarization in germanium quantum wells is studied. With increasing THz field strength, it is observed that the excitonic resonances shift toward higher energy and broaden before weak signatures of a splitting of the exciton line occur. In comparison with high-quality GaAs-based quantum wells, where a much clearer Autler–Townes splitting is observed, the germanium system response is significantly more broadened and shows signatures of a quasi-steady-state behavior due to the intrinsic fast dephasing times dominated by intervalley scattering

Ultrafast Exciton Dynamics in the Atomically Thin van der Waals Magnet CrSBr

Among atomically thin semiconductors, CrSBr stands out as both its bulk and monolayer forms host tightly bound, quasi-one-dimensional excitons in a magnetic environment. Despite its pivotal importance for solid-state research, the exciton lifetime has remained unknown. While terahertz polarization probing can directly trace all excitons, independently of interband selection rules, the corresponding large far-field foci substantially exceed the lateral sample dimensions. Here, we combine terahertz polarization spectroscopy with near-field microscopy to reveal a femtosecond decay of paramagnetic excitons in a monolayer of CrSBr, which is 30 times shorter than the bulk lifetime. We unveil low-energy fingerprints of bound and unbound electron–hole pairs in bulk CrSBr and extract the nonequilibrium dielectric function of the monolayer in a model-free manner. Our results demonstrate the first direct access to the ultrafast dielectric response of quasi-one-dimensional excitons in CrSBr, potentially advancing the development of quantum devices based on ultrathin van der Waals magnets

Scalable high-repetition-rate sub-half-cycle terahertz pulses from spatially indirect interband transitions

Intense phase-locked terahertz (THz) pulses are the bedrock of THz lightwave electronics, where the carrier field creates a transient bias to control electrons on sub-cycle time scales. Key applications such as THz scanning tunnelling microscopy or electronic devices operating at optical clock rates call for ultimately short, almost unipolar waveforms, at megahertz (MHz) repetition rates. Here, we present a flexible and scalable scheme for the generation of strong phase-locked THz pulses based on shift currents in type-II-aligned epitaxial semiconductor heterostructures. The measured THz waveforms exhibit only 0.45 optical cycles at their centre frequency within the full width at half maximum of the intensity envelope, peak fields above 1.1 kV cm−1 and spectral components up to the mid-infrared, at a repetition rate of 4 MHz. The only positive half-cycle of this waveform exceeds all negative half-cycles by almost four times, which is unexpected from shift currents alone. Our detailed analysis reveals that local charging dynamics induces the pronounced positive THz-emission peak as electrons and holes approach charge neutrality after separation by the optical pump pulse, also enabling ultrabroadband operation. Our unipolar emitters mark a milestone for flexibly scalable, next-generation high-repetition-rate sources of intense and strongly asymmetric electric field transients

Microscopic Theory of Linear and Nonlinear Terahertz Spectroscopy of Semiconductors

This Thesis presents a fully microscopic theory to describe terahertz (THz)-induced processes in optically-excited semiconductors. The formation process of excitons and other quasi-particles after optical excitation has been studied in great detail for a variety of conditions. Here, the formation process is not modelled but a realistic initial many-body state is assumed. In particular, the linear THz response is reviewed and it is demonstrated that correlated quasi-particles such as excitons and plasmons can be unambiguously detected via THz spectroscopy. The focus of the investigations, however, is on situations where the optically-excited many-body state is excited by intense THz fields. While weak pulses detect the many-body state, strong THz pulses control and manipulate the quasi-particles in a way that is not accessible via conventional techniques. The nonlinear THz dynamics of exciton populations is especially interesting because similarities and differences to optics with atomic systems can be studied

Influence of Phonons on Semiconductor Quantum Emission

A microscopic theory of interacting charge carriers, lattice vibrations, and light modes in semiconductor systems is presented. The theory is applied to study quantum dots and phonon-assisted luminescence in bulk semiconductors and hetero structures

Microscopic Theory of Photon-Correlation Spectroscopy in Strong-Coupling Semiconductors

While many quantum-optical phenomena are already well established in the atomic systems, like the photon antibunching, squeezing, Bose-Einstein condensation, teleportation, the quantum-optical investigations in semiconductors are still at their beginning. The fascinating results observed in the atomic systems inspire physicists to demonstrate similar quantum-optical effects also in the semiconductor systems. In contrast to quantum optics with dilute atomic gases, the semiconductors exhibit a complicated many-body problem which is dominated by the Coulomb interaction between the electrons and holes and by coupling with the semiconductor environment. This makes the experimental observation of similar quantum-optical effects in semiconductors demanding. However, there are already experiments which have verified nonclassical effects in semiconductors. In particular, experiments have demonstrated that semiconductor quantum dots (QDs) can exhibit the single-photon emission and generation of polarization-entangled photon pairs. In fact, both atom and QD systems, embedded within a microcavity, have become versatile platforms where one can perform systematic quantum-optics investigations as well as development work toward quantum-information applications. Another interesting field is the strong-coupling regime in which the light-matter coupling exceeds both the decoherence rate of the atom or QD and the cavity resulting in a reversible dynamics between light and matter excitations. In the strong-coupling regime, the Jaynes-Cummings ladder is predicted and shows a photon-number dependent splitting of the new dressed strong-coupling states which are the polariton states of the coupled light-matter system. Although the semiclassical effect of the vacuum Rabi splitting has already been observed in QDs, the verification of the quantum-mechanical Jaynes-Cummings splitting is still missing mainly due to the dephasing. Clearly, the observation of the Jaynes-Cummings ladder in QDs would be a great contribution in the growing field of quantum optics in semiconductors. The efforts in QD systems are again driven by the atomic systems which not only have shown the vacuum Rabi splitting, but also the second rung, e.g. via direct spectroscopy and via photon-correlation measurements. In this thesis, it is shown that spectrally resolved photon-statistics measurements of the resonance fluorescence from realistic semiconductor quantum-dot systems allow for high contrast identification of the two-photon strong-coupling states. Using a microscopic theory, the second-rung resonance of Jaynes-Cummings ladder is analyzed and optimum excitation conditions are determined. The computed photon-statistics spectrum displays gigantic, experimentally robust resonances at the energetic positions of the second-rung emission. The resonance fluorescence equations are derived and solved for strong-coupling semiconductor quantum-dot systems using a fully quantized multimode theory and a cluster-expansion approach. A reduced model is developed to explain the origin of auto- and cross-correlation resonances in the two-photon emission spectrum of the fluorescent light. These resonances are traced back to the two-photon strong-coupling states of Jaynes-Cummings ladder. The accuracy of the reduced model is verified via numerical solution of the resonance fluorescence equations. The analysis reveals the direct relation between the squeezed-light emission and the strong-coupling states in optically excited semiconductor systems