Doris Reiter

Nanoscale Positioning of Single-Photon Emitters in Atomically Thin WSe2

Single-photon emitters in monolayer WSe2 are created at the nanoscale gap between two single-crystalline gold nanorods. The atomically thin semiconductor conforms to the metal nanostructure and is bent at the position of the gap. The induced strain leads to the formation of a localized potential well inside the gap. Single-photon emitters are localized there with a precision better than 140 nm.

The role of phonons for exciton and biexciton generation in an optically driven quantum dot

For many applications of semiconductor quantum dots in quantum technology, well-controlled state preparation of the quantum dot states is mandatory. Since quantum dots are embedded in the semiconductor matrix, their interaction with phonons often plays a major role in the preparation process. In this review, we discuss the influence of phonons on three basically different optical excitation schemes that can be used for the preparation of exciton, biexciton and superposition states: a resonant excitation leading to Rabi rotations in the excitonic system, an excitation with chirped pulses exploiting the effect of adiabatic rapid passage and an off-resonant excitation giving rise to a phonon-assisted state preparation. We give an overview of experimental and theoretical results, showing the role of phonons and compare the performance of the schemes for state preparation.

Impact of phonons on dephasing of individual excitons in deterministic quantum dot microlenses

Optimized light–matter coupling in semiconductor nanostructures is a key to understand their optical properties and can be enabled by advanced fabrication techniques. Using in situ electron beam lithography combined with a low-temperature cathodoluminescence imaging, we deterministically fabricate microlenses above selected InAs quantum dots (QDs), achieving their efficient coupling to the external light field. This enables performing four-wave mixing microspectroscopy of single QD excitons, revealing the exciton population and coherence dynamics. We infer the temperature dependence of the dephasing in order to address the impact of phonons on the decoherence of confined excitons. The loss of the coherence over the first picoseconds is associated with the emission of a phonon wave packet, also governing the phonon background in photoluminescence (PL) spectra. Using theory based on the independent boson model, we consistently explain the initial coherence decay, the zero-phonon line fraction, and the line shape of the phonon-assisted PL using realistic quantum dot geometries.

Biexciton state preparation in a quantum dot via adiabatic rapid passage: Comparison between two control protocols and impact of phonon-induced dephasing

We investigate theoretically under what conditions a stable and high-fidelity preparation of the biexciton state in a quantum dot can be realized by means of adiabatic rapid passage in the presence of acoustic phonon coupling. Our analysis is based on a numerically complete real-time path-integral approach and comprises two different schemes of optical driving using frequency-swept (chirped) pulses. We show that depending on the size of the biexciton binding energy, resonant two-photon excitations or two-color schemes can be favorable. It is demonstrated that the carrier-phonon interaction strongly affects the efficiency of both protocols and that a robust preparation of the biexciton is restricted to positive chirps and low temperatures. A considerable increase of the biexciton yield can be achieved realizing temperatures below 4 K.

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.

Lindblad approach to spatiotemporal quantum dynamics of phonon-induced carrier capture processes

In view of the ultrashort spatial and temporal scales involved, carrier capture processes in nanostructures are genuine quantum phenomena. To describe such processes, methods with different levels of approximations have been developed. By properly tailoring the Lindblad-based nonlinear single-particle density matrix equation provided by an alternative Markov approach, in this work we present a Lindblad superoperator to describe how the phonon-induced carrier capture affects the spatio-temporal quantum dynamics of a flying wave packet impinging on a quantum dot. We compare the results with non-Markovian quantum kinetics calculations and discuss the advantages and drawbacks of the two approaches.

Dynamics of excitons in individual InAs quantum dots revealed in four-wave mixing spectroscopy

A detailed understanding of the population and coherence dynamics in optically driven individual emitters in solids and their signatures in ultrafast nonlinear-optical signals is of prime importance for their applications in future quantum and optical technologies. In a combined experimental and theoretical study on exciton complexes in single semiconductor quantum dots we reveal a detailed picture of the dynamics employing three-beam polarization-resolved four-wave mixing (FWM) micro-spectroscopy. The oscillatory dynamics of the FWM signals in the exciton-biexciton system is governed by the fine-structure splitting and the biexciton binding energy in an excellent quantitative agreement between measurement and analytical description. The analysis of the excitation conditions exhibits a dependence of the dynamics on the specific choice of polarization configuration, pulse areas and temporal ordering of driving fields. The interplay between the transitions in the four-level exciton system leads to rich evolution of coherence and population. Using two-dimensional FWM spectroscopy we elucidate the exciton-biexciton coupling and identify neutral and charged exciton complexes in a single quantum dot. Our investigations thus clearly reveal that FWM spectroscopy is a powerful tool to characterize spectral and dynamical properties of single quantum structures.

Formulation of the twisted-light-matter interaction at the phase singularity: the twisted-light gauge

Twisted light is light carrying orbital angular momentum. The profile of such a beam is a ringlike structure with a node at the beam axis, where a phase singularity exists. Due to the strong spatial inhomogeneity the mathematical description of twisted-light--matter interaction is nontrivial, in particular close to the phase singularity, where the commonly used dipole-moment approximation cannot be applied. In this paper we show that, if the handedness of circular polarization and the orbital angular momentum of the twisted-light beam have the same sign, a specific gauge---the twisted-light gauge---can be used where the Hamiltonian takes a form similar to the dipole-moment approximation. However, if the signs differ, no such gauge can be found. Here in general the magnetic parts of the light beam become of significant importance and an interaction Hamiltonian which only accounts for electric fields is inappropriate. We discuss the consequences of these findings for twisted-light excitation of a semiconductor nanostructure, e.g., a quantum dot, placed at the phase singularity.

Optical control of exciton and spin states in a quantum dot by excitation with twisted light

We discuss how the excitation of a quantum dot can benefit from the special properties of twisted light beams. First we address the question of the appropriate theoretical description of the light-matter coupling in this system, i.e., of the most appropriate gauge. Then we discuss the optical transitions induced by different types of twisted light beams showing that both the envelope and the spin state of the exciton can be well controlled.

Energy transport and coherence properties of acoustic phonons generated by optical excitation of a quantum dot

The energy transport of acoustic phonons generated by the optical excitation of a quantum dot as well as the coherence properties of these phonons are studied theoretically both for the case of a pulsed excitation and for a continuous wave (CW) excitation switched on instantaneously. For a pulsed excitation, depending on pulse area and pulse duration, a finite number of phonon wave packets is emitted, while for the case of a CW excitation a sequence of wave packets with decreasing amplitude is generated after the excitation has been switched on. We show that the energy flow associated with the generated phonons is partly related to coherent phonon oscillations and partly to incoherent phonon emission. The efficiency of the energy transfer to the phonons and the details of the energy flow depend strongly and in a non-monotonic way on the Rabi frequency exhibiting a resonance behavior. However, in the case of CW excitation it turns out that the total energy transferred to the phonons is directly linked in a monotonic way to the Rabi frequency.