arXiv subjects

Malte Kremser

Publications and source records attributed to Malte Kremser.

8 recordsLinked to original sources

arXiv2022

Coherent Dynamics of the Swing-Up Excitation Technique

Developing coherent excitation methods for quantum emitters which enable high brightness, good single-photon purity and high indistinguishability of the emitted photons has been a key challenge in the past years. While many methods have been proposed and explored, they all have specific advantages and disadvantages. In this letter, we investigate the dynamics of the recent swing-up scheme as an excitation method for a two-level system and its performance in single-photon generation. By applying two far red-detuned laser pulses, the two-level system can be prepared in the excited state with near-unity fidelity. We demonstrate the successful functionality and the coherent character of this technique using semiconductor quantum dots. Moreover, we explore the multi-dimensional parameter space of the two laser pulses to study the impact on the excitation fidelity. Finally, we investigate the performance of the scheme as an excitation method for generation of high-quality single photons. We find that the swing-up scheme itself works well and exhibits nearly perfect single-photon purity, while the observed indistinguishability in our sample is limited by the influence of the inevitable high excitation powers on the semiconductor environment of the quantum dot.

quant-ph↗

arXiv2022

Twist-dependent intra- and interlayer excitons in moire MoSe2 homobilayers

Optoelectronic properties of van der Waals homostructures can be selectively engineered by the relative twist angle between layers. Here, we study the twist-dependent moire coupling in MoSe2 homobilayers. For small angles, we find a pronounced redshift of the K-K and Γ-K excitons accompanied by a transition from K-K to Γ-K emission. Both effects can be traced back to the underlying moire pattern in the MoSe2 homobilayers, as confirmed by our low-energy continuum model for different moire excitons. We identify two distinct intralayer moire excitons for R-stacking, while H-stacking yields two degenerate intralayer excitons due to inversion symmetry. In both cases, bright interlayer excitons are found at higher energies. The performed calculations are in excellent agreement with experiment and allow us to characterize the observed exciton resonances, providing insight about the layer composition and relevant stacking configuration of different moire exciton species.

cond-mat.mes-hall↗

arXiv2022

Tuning the Optical Properties of an MoSe$_2$ Monolayer Using Nanoscale Plasmonic Antennas

Nanoplasmonic systems combined with optically-active two-dimensional materials provide intriguing opportunities to explore and control light-matter interactions at extreme sub-wavelength lengthscales approaching the exciton Bohr radius. Here, we present room- and cryogenic-temperature investigations of light-matter interactions between an MoSe$_2$ monolayer and individual lithographically defined gold dipole nanoantennas having sub-10 nm feed gaps. By progressively tuning the nanoantenna size, their dipolar resonance is tuned relative to the A-exciton transition in a proximal MoSe$_2$ monolayer achieving a total tuning of $\sim 130\;\mathrm{meV}$. Differential reflectance measurements performed on $> 100$ structures reveal an apparent avoided crossing between exciton and dipolar mode and an exciton-plasmon coupling constant of $g= 55\;\mathrm{meV}$, representing $g/(\hbarω_X)\geq3\%$ of the transition energy. This places our hybrid system in the intermediate-coupling regime where spectra exhibit a characteristic Fano-like shape, indicative of the interplay between pronounced light-matter coupling and significant damping. We also demonstrate active control of the optical response by varying the polarization of the excitation light to programmably suppress coupling to the dipole mode. We further study the emerging optical signatures of the monolayer localized at dipole nanoantennas at $10\;\mathrm{K}$. Our findings represent a key step towards realizing non-linear photonic devices based on 2D materials with potential for low-energy and ultrafast performance.

cond-mat.mes-hall↗

arXiv2021

Raman spectrum of Janus transition metal dichalcogenide monolayers WSSe and MoSSe

Janus transition metal dichalcogenides (TMDs) lose the horizontal mirror symmetry of ordinary TMDs, leading to the emergence of additional features, such as native piezoelectricity, Rashba effect, and enhanced catalytic activity. While Raman spectroscopy is an essential nondestructive, phase- and composition-sensitive tool to monitor the synthesis of materials, a comprehensive study of the Raman spectrum of Janus monolayers is still missing. Here, we discuss the Raman spectra of WSSe and MoSSe measured at room and cryogenic temperatures, near and off resonance. By combining polarization-resolved Raman data with calculations of the phonon dispersion and using symmetry considerations, we identify the four first-order Raman modes and higher-order two-phonon modes. Moreover, we observe defect-activated phonon processes, which provide a route toward a quantitative assessment of the defect concentration and, thus, the crystal quality of the materials synthesized. Our work establishes a solid background for future research on material synthesis, study, and application of Janus TMD monolayers.

cond-mat.mes-hall↗

arXiv2021

High-resolution spectroscopy of a quantum dot driven bichromatically by two strong coherent fields

We present spectroscopic experiments and theory of a quantum dot driven bichromatically by two strong coherent lasers. In particular, we explore the regime where the drive strengths are substantial enough to merit a general non-perturbative analysis, resulting in a rich higher-order Floquet dressed-state energy structure. We show high resolution spectroscopy measurements with a variety of laser detunings performed on a single InGaAs quantum dot, with the resulting features well explained with a time-dependent quantum master equation and Floquet analysis. Notably, driving the quantum dot resonance and one of the subsequent Mollow triplet sidepeaks, we observe the disappearance and subsequent reappearance of the central transition and transition resonant with detuned-laser at high detuned-laser pump strengths and additional higher-order effects, e.g. emission triplets at higher harmonics and signatures of higher order Floquet states. For a similar excitation condition but with an off-resonant primary laser, we observe similar spectral features but with an enhanced inherent spectral asymmetry.

quant-ph↗

arXiv2020

Discrete Interactions between a few Interlayer Excitons Trapped at a MoSe$_2$-WSe$_2$ Heterointerface

Interlayer excitons (IXs) in hetero-bilayers of transition metal dichalcogenides (TMDs) represent an exciting emergent class of long-lived dipolar composite bosons in an atomically thin, near-ideal two-dimensional (2D) system. The long-range interactions that arise from the spatial separation of electrons and holes can give rise to novel quantum, as well as classical multi-particle correlation effects. In order to acquire a detailed understanding of the possible many-body effects, the fundamental interactions between individual IXs have to be studied. Here, we trap a tunable number of dipolar within a nanoscale confinement potential induced by placing a MoSe$_2$-WSe$_2$ hetero-bilayer (HBL) onto an array of SiO$_2$ nanopillars. We control the mean occupation of the IX trap via the optical excitation level and observe discrete sharp-line emission from different configurations of interacting IXs. We identify these features as different multiparticle states with $N_{IX}\sim1-5$ via their power dependencies and directly measure the hierarchy of dipolar and exchange interactions as $N_{IX}$ increases. The interlayer biexciton ($N_{IX}=2$) is found to be an emission doublet that is blue-shifted from the single exciton by $ΔE=(8.4\pm0.6)$ meV and split by $2J=(1.2\pm0.5)$ meV. The blueshift is even more pronounced for triexcitons ($(12.4\pm0.4)$ meV), quadexcitons ($(15.5\pm0.6)$ meV) and quintexcitons ($(18.2\pm0.8)$ meV). These values are shown to be mutually consistent with numerical modelling of dipolar excitons confined to a harmonic trapping potential having a confinement lengthscale in the range $\ell\approx 3$ nm. Our results contribute to the understanding of interactions between IXs in TMD HBLs at the discrete limit of only a few excitations and represent a key step towards exploring quantum correlations between them.

cond-mat.mes-hall↗

arXiv2017

Pulsed Rabi oscillations in quantum two-level systems: beyond the Area Theorem

The Area Theorem states that when a short optical pulse drives a quantum two-level system, it undergoes Rabi oscillations in the probability of scattering a single photon. In this work, we investigate the breakdown of the Area Theorem as both the pulse length becomes non-negligible and for certain pulse areas. Using simple quantum trajectories, we provide an analytic approximation to the photon emission dynamics of a two-level system. Our model provides an intuitive way to understand re-excitation, which elucidates the mechanism behind the two-photon emission events that can spoil single-photon emission. We experimentally measure the emission statistics from a semiconductor quantum dot, acting as a two-level system, and show good agreement with our simple model for short pulses. Additionally, the model clearly explains our recent results [K. Fischer and L. Hanschke, et al., Nature Physics (2017)] showing dominant two-photon emission from a two-level system for pulses with interaction areas equal to an even multiple of $π$.

quant-ph↗

arXiv2017

Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit

We demonstrate the reduction of the inhomogeneous linewidth of the free excitons in atomically thin transition metal dichalcogenides (TMDCs) MoSe$_{2}$, WSe$_{2}$ and MoS$_{2}$ by encapsulation within few nanometer thick hBN. Encapsulation is shown to result in a significant reduction of the 10K excitonic linewidths down to $\sim3.5 \text{ meV}$ for n-MoSe$_{2}$, $\sim5.0 \text{ meV}$ for p-WSe$_{2}$ and $\sim4.8 \text{ meV}$ for n-MoS$_{2}$. Evidence is obtained that the hBN environment effectively lowers the Fermi level since the relative spectral weight shifts towards the neutral exciton emission in n-doped TMDCs and towards charged exciton emission in p-doped TMDCs. Moreover, we find that fully encapsulated MoS$_{2}$ shows resolvable exciton and trion emission even after high power density excitation in contrast to non-encapsulated materials. Our findings suggest that encapsulation of mechanically exfoliated few-monolayer TMDCs within nanometer thick hBN dramatically enhances optical quality, producing ultra-narrow linewidths that approach the homogeneous limit.

cond-mat.mes-hall↗