Daniel Wigger

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.

Strain Control of Exciton–Phonon Coupling in Atomically Thin Semiconductors

Semiconducting transition metal dichalcogenide (TMDC) monolayers have exceptional physical properties. They show bright photoluminescence due to their unique band structure and absorb more than 10% of the light at their excitonic resonances despite their atomic thickness. At room temperature, the width of the exciton transitions is governed by the exciton-phonon interaction leading to strongly asymmetric line shapes. TMDC monolayers are also extremely flexible, sustaining mechanical strain of about 10% without breaking. The excitonic properties strongly depend on strain. For example, exciton energies of TMDC monolayers significantly redshift under uniaxial tensile strain. Here, we demonstrate that the width and the asymmetric line shape of excitonic resonances in TMDC monolayers can be controlled with applied strain. We measure photoluminescence and absorption spectra of the A exciton in monolayer MoSe2, WSe2, WS2, and MoS2 under uniaxial tensile strain. We find that the A exciton substantially narrows and becomes more symmetric for the selenium-based monolayer materials, while no change is observed for atomically thin WS2. For MoS2 monolayers, the line width increases. These effects are due to a modified exciton-phonon coupling at increasing strain levels because of changes in the electronic band structure of the respective monolayer materials. This interpretation based on steady-state experiments is corroborated by time-resolved photoluminescence measurements. Our results demonstrate that moderate strain values on the order of only 1% are already sufficient to globally tune the exciton-phonon interaction in TMDC monolayers and hold the promise for controlling the coupling on the nanoscale.

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.

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.

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.

Quantum dynamics of optical phonons generated by optical excitation of a quantum dot

The study of the fundamental properties of phonons is crucial to understand their role in applications in quantum information science, where the active use of phonons is currently highly debated. A genuine quantum phenomenon associated with the fluctuation properties of phonons is squeezing, which is achieved when the fluctuations of a certain variable drop below their respective vacuum values. We consider a semiconductor quantum dot (QD) in which the exciton is coupled to phonons. We review the fluctuation properties of the phonons, which are generated by optical manipulation of the QD, in the limiting case of ultra-short pulses. Then, we discuss the phonon properties for an excitation with finite pulses. Within a generating function formalism, we calculate the corresponding fluctuation properties of the phonons and show that phonon squeezing can be achieved by the optical manipulation of the QD exciton for certain conditions even for a single-pulse excitation where neither for short nor for long pulses squeezing occurs. To explain the occurrence of squeezing, we employ a Wigner function picture providing a detailed understanding of the induced quantum dynamics.

Picosecond control of quantum dot laser emission by coherent phonons

A picosecond acoustic pulse can be used to control the lasing emission from semiconductor nanostructures by shifting their electronic transitions. When the active medium, here an ensemble of (In,Ga)As quantum dots, is shifted into or out of resonance with the cavity mode, a large enhancement or suppression of the lasing emission can dynamically be achieved. Most interesting, even in the case when gain medium and cavity mode are in resonance, we observe an enhancement of the lasing due to shaking by coherent phonons. In order to understand the interactions of the nonlinearly coupled photon-exciton-phonon subsystems, we develop a semiclassical model and find an excellent agreement between theory and experiment.

Deterministic positioning of single-photon emitters in monolayer WSe 2 on the nanoscale

Single-photon sources are important building blocks for quantum technology. Recently, bright and stable single-photon emitters have been reported in the atomically thin semiconductor WSe2. However, the localized light sources appear at random positions at the edges of the material [1]. Here, we demonstrate the deterministic positioning of single-photon emitters in monolayer WSe2 on the nanoscale [2]. The monolayer is placed on top of a gapped single-crystalline gold rod. The atomically thin semiconductor folds around the metal nanostructure and is bent at the position of the gap (Fig. 1a).

Systematic study of the influence of coherent phonon wave packets on the lasing properties of a quantum dot ensemble

Coherent phonons can greatly vary light-matter interaction in semiconductor nanostructures placed inside an optical resonator on an ultrafast time scale. For an ensemble of quantum dots as active laser medium phonons are able to induce a large enhancement or attenuation of the emission intensity, as has been recently demonstrated. The physics of this coupled phonon-exciton-photon system consists of various effects, which in the experiment typically cannot be clearly separated, in particular because a rather complex strain pulse impinges on the quantum dot ensemble. Here we present a comprehensive theoretical study how the laser emission is affected by phonon pulses of various shapes as well as by ensembles with different spectral distributions of the quantum dots. This gives insight into the fundamental interaction dynamics of the coupled phonon-exciton-photon system, while it allows us to clearly discriminate between two prominent effects: the adiabatic shifting of the ensemble and the shaking effect. This paves the way to a tailored laser emission controlled by phonons.

Generating sequences of phonon wave packets by optical excitation of a quantum dot

Phonons can play an active role in controlling solid state systems or in the transport of energy and information. Thus, it is vital to understand generation processes and properties of phonons. By optical excitation of a semiconductor quantum dot, a sequence of phonon wave packets can be created. In this paper we focus on the fluctuation properties of lattice displacement and momentum of these phonon wave packets. For detuned excitation the fluctuations may fall below their respective vacuum values and squeezing occurs.