arXiv subjects

Matthias Florian

Publications and source records attributed to Matthias Florian.

32 records · Page 2Linked to original sources

arXiv2020

Scalable single-photon sources in atomically thin MoS2

Real-world quantum applications, eg. on-chip quantum networks and quantum cryptography, necessitate large scale integrated single-photon sources with nanoscale footprint for modern information technology. While on-demand and high fidelity implantation of atomic scale single-photon sources in conventional 3D materials suffer from uncertainties due to the crystals dimensionality, layered 2D materials can host point-like centers with inherent confinement to a sub-nm plane. However, previous attempts to truly deterministically control spatial position and spectral homogeneity while maintaining the 2D character have not been realized. Here, we demonstrate the on-demand creation and precise positioning of single-photon sources in atomically thin MoS2 with very narrow ensemble broadening and near-unity fabrication yield. Focused ion beam irradiation creates 100s to 1000s of mono-typical atomistic defects with anti-bunched emission lines with sub-10 nm lateral and 0.7 nm axial positioning accuracy. Our results firmly establish 2D materials as a scalable platform for single-photon emitters with unprecedented control of position as well as photophysical properties owing to the all-interfacial nature.

cond-mat.mes-hall↗

arXiv2019

Dynamical screening effects of substrate phonons on two-dimensional excitons

Atomically thin materials are exceedingly susceptible to their dielectric environment. For transition metal dichalcogenides, sample placement on a substrate or encapsulation in hexagonal boron nitride (hBN) are frequently used. In this paper we show that the dielectric response due to optical phonons of adjacent materials influences excitons in 2d crystals. We provide an analytic model for the coupling of 2d charge carriers to optical substrate phonons, which causes polaron effects similar to that of intrinsic 2d phonons. We apply the model to hBN-encapsulated WSe2, finding a significant reduction of the exciton binding energies due to dynamical screening effects.

cond-mat.mes-hall↗

arXiv2019

Quantum-dot-like states in molybdenum disulfide nanostructures due to the interplay of local surface wrinkling, strain, and dielectric confinement

The observation of quantum light emission from atomically thin transition metal dichalcogenides has opened a new field of applications for these material systems. The corresponding excited charge-carrier localization has been linked to defects and strain, while open questions remain regarding the microscopic origin. We demonstrate that the bending rigidity of these materials leads to wrinkling of the two-dimensional layer. The resulting strain field facilitates strong carrier localization due to its pronounced influence on the band gap. Additionally, we consider charge carrier confinement due to local changes of the dielectric environment and show that both effects contribute to modified electronic states and optical properties. The interplay of surface wrinkling, strain-induced confinement, and local changes of the dielectric environment is demonstrated for the example of nanobubbles that form when monolayers are deposited on substrates or other two-dimensional materials.

cond-mat.mes-hall↗

arXiv2019

Atomistic defect states as quantum emitters in monolayer MoS$_2$

Quantum light sources in solid-state systems are of major interest as a basic ingredient for integrated quantum device technologies. The ability to tailor quantum emission through deterministic defect engineering is of growing importance for realizing scalable quantum architectures. However, a major difficulty is that defects need to be positioned site-selectively within the solid. Here, we overcome this challenge by controllably irradiating single-layer MoS$_{2}$ using a sub-nm focused helium ion beam to deterministically create defects. Subsequent encapsulation of the ion bombarded MoS$_{2}$ flake with high-quality hBN reveals spectrally narrow emission lines that produce photons at optical wavelengths in an energy window of one to two hundred meV below the neutral 2D exciton of MoS$_{2}$. Based on ab-initio calculations we interpret these emission lines as stemming from the recombination of highly localized electron-hole complexes at defect states generated by the helium ion bombardment. Our approach to deterministically write optically active defect states in a single transition metal dichalcogenide layer provides a platform for realizing exotic many-body systems, including coupled single-photon sources and exotic Hubbard systems.

cond-mat.mes-hall↗

arXiv2018

Prospects and limitations of transition-metal dichalcogenide laser gain materials

Nanolasers operate with a minimal amount of active material and low losses. In this regime, single layers of transition-metal dichalcogenides (TMDs) are being investigated as next generation gain materials due to their high quantum efficiency. We provide results from microscopic gain calculations of highly excited TMD monolayers and specify requirements to achieve lasing with four commonly used TMD semiconductors. Our approach includes band-structure renormalizations due to excited carriers that trigger a direct-to-indirect band-gap transition. As a consequence, we predict a rollover for the gain that limits the excitation regime where laser operation is possible. A parametrization of the peak gain is provided that is used in combination with a rate-equation theory to discuss consequences for experimentally accessible laser characteristics.

cond-mat.mes-hall↗

arXiv2018

Polariton hyperspectral imaging of two-dimensional semiconductor crystals

Atomically thin crystals of transition metal dichalcogenides (TMDs) host excitons with strong binding energies and sizable light-matter interactions. Coupled to optical cavities, monolayer TMDs routinely reach the regime of strong light-matter coupling, where excitons and photons admix coherently to form quasiparticles known as polaritons up to room temperature. Here, we explore the two-dimensional nature of TMD polaritons with cavity-assisted hyperspectral imaging. Using extended WS$_2$ monolayers, we establish the regime of strong coupling with a scanning microcavity to map out polariton properties and correlate their spatial features with intrinsic and extrinsic effects. We find a high level of homogeneity, and show that polariton splitting variations are correlated with intrinsic exciton properties such as oscillator strength and linewidth. Moreover, we observe a deviation from thermal equilibrium in the resonant polariton population, which we ascribe to non-perturbative polariton-phonon coupling. Our measurements reveal a promisingly consistent polariton landscape, and highlight the importance of phonons for future polaritonic devices.

physics.optics↗

arXiv2018

Biexciton fine structure in monolayer transition metal dichalcogenides

The optical properties of atomically thin transition metal dichalcogenide (TMDC) semiconductors are shaped by the emergence of correlated many-body complexes due to strong Coulomb interaction. Exceptional electron-hole exchange predestines TMDCs to study fundamental and applied properties of Coulomb complexes such as valley depolarization of excitons and fine-structure splitting of trions. Biexcitons in these materials are less understood and it has been established only recently that they are spectrally located between exciton and trion. Here we show that biexcitons in monolayer TMDCs exhibit a distinct fine structure on the order of meV due to electron-hole exchange. Ultrafast pump-probe experiments on monolayer WSe$_2$ reveal decisive biexciton signatures and a fine structure in excellent agreement with a microscopic theory. We provide a pathway to access biexciton spectra with unprecedented accuracy, which is valuable beyond the class of TMDCs, and to understand even higher Coulomb complexes under the influence of electron-hole exchange.

cond-mat.mtrl-sci↗

arXiv2017

Strong light-matter coupling in the presence of lasing

The regime of strong light-matter coupling is typically associated with weak excitation. With current realizations of cavity-QED systems, strong coupling may persevere even at elevated excitation levels sufficient to cross the threshold to lasing. In the presence of stimulated emission, the vacuum-Rabi doublet in the emission spectrum is modified and the established criterion for strong coupling no longer applies. We provide a generalized criterion for strong coupling and the corresponding emission spectrum, which includes the influence of higher Jaynes-Cummings states. The applicability is demonstrated in a theory-experiment comparison of a few-emitter quantum-dot--micropillar laser as a particular realization of the driven dissipative Jaynes-Cummings model. Furthermore, we address the question if and for which parameters true single-emitter lasing can be achieved, and provide evidence for the coexistence of strong coupling and lasing in our system in the presence of background emitter contributions.

physics.optics↗

arXiv2017

Excitons versus electron-hole plasma in monolayer transition metal dichalcogenide semiconductors

When electron-hole pairs are excited in a semiconductor, it is a priori not clear if they form a fermionic plasma of unbound particles or a bosonic exciton gas. Usually, the exciton phase is associated with low temperatures. In atomically thin transition metal dichalcogenide semiconductors, excitons are particularly important even at room temperature due to strong Coulomb interaction and a large exciton density of states. Using state-of-the-art many-body theory including dynamical screening, we show that the exciton-to-plasma ratio can be efficiently tuned by dielectric substrate screening as well as charge carrier doping. Moreover, we predict a Mott transition from the exciton-dominated regime to a fully ionized electron-hole plasma at excitation densities between $3\times10^{12}$ cm$^{-2}$ and $1\times10^{13}$ cm$^{-2}$ depending on temperature, carrier doping and dielectric environment. We propose the observation of these effects by studying excitonic satellites in photoemission spectroscopy and scanning tunneling microscopy.

cond-mat.mtrl-sci↗

arXiv2017

Electric-field switchable second-harmonic generation in bilayer MoS$_{2}$ by inversion symmetry breaking

We demonstrate pronounced electric-field-induced second-harmonic generation in naturally inversion symmetric 2H stacked bilayer MoS$_{2}$ embedded into microcapacitor devices. By applying strong external electric field perturbations ($|F| = \pm 2.6 MVcm^{-1}$) perpendicular to the basal plane of the crystal we control the inversion symmetry breaking and, hereby, tune the nonlinear conversion efficiency. Strong tunability of the nonlinear response is observed throughout the energy range ($E_ω \sim 1.25 eV - 1.47 eV$) probed by measuring the second-harmonic response at $E_{2ω}$, spectrally detuned from both the A- and B-exciton resonances. A 60-fold enhancement of the second-order nonlinear signal is obtained for emission at $E_{2ω} = 2.49 eV$, energetically detuned by $ΔE = E_{2ω} - E_C = -0.26 eV$ from the C-resonance ($E_{C} = 2.75 eV$). The pronounced spectral dependence of the electric-field-induced second-harmonic generation signal reflects the bandstructure and wave function admixture and exhibits particularly strong tunability below the C-resonance, in good agreement with Density Functional Theory calculations. Moreover, we show that the field-induced second-harmonic generation relies on the interlayer coupling in the bilayer. Our findings strongly suggest that the strong tunability of the electric-field-induced second-harmonic generation signal in bilayer transition metal dichalcogenides may find applications in miniaturized electrically switchable nonlinear devices.

cond-mat.mes-hall↗

arXiv2016

Nonequilibrium Carrier Dynamics in Transition Metal Dichalcogenide Semiconductors

When exploring new materials for their potential in (opto)electronic device applications, it is important to understand the role of various carrier interaction and scattering processes. Research on transition metal dichalcogenide (TMD) semiconductors has recently progressed towards the realisation of working devices, which involve light-emitting diodes, nanocavity lasers, and single-photon emitters. In these two-dimensional atomically thin semiconductors, the Coulomb interaction is known to be much stronger than in quantum wells of conventional semiconductors like GaAs, as witnessed by the 50 times larger exciton binding energy. The question arises, whether this directly translates into equivalently faster carrier-carrier Coulomb scattering of excited carriers. Here we show that a combination of ab-initio band-structure and many-body theory predicts carrier relaxation on a 50-fs time scale, which is less than an order of magnitude faster than in quantum wells. These scattering times compete with the recently reported sub-ps exciton recombination times, thus making it harder to achieve population inversion and lasing.

cond-mat.mtrl-sci↗

arXiv2013

Coulomb-assisted cavity feeding in the non-resonant optical emission from a quantum dot

Recent experiments have demonstrated that for a quantum dot in an optical resonator off-resonant cavity mode emission can occur even for detunings of the order of 10 meV. We show that Coulomb mediated Auger processes based on additional carriers in delocalized states can facilitate this far off-resonant emission. Using a novel theoretical approach for a non-perturbative treatment of the Auger-assisted quantum-dot carrier recombination, we present numerical calculations of the far off-resonant cavity feeding rate and cavity mean photon number confirming efficient coupling at higher densities of carriers in the delocalized states. In comparison to fast Auger-like intraband scattering processes, we find a reduced overall efficiency of Coulomb-mediated interband transitions due the required electron-hole correlations for the recombination processes.

cond-mat.mes-hall↗

arXiv2012

Pronounced Purcell enhancement of spontaneous emission in CdTe/ZnTe quantum dots embedded in micropillar cavities

The coupling of CdTe/ZnTe quantum dot (QD) emission to micropillar cavity eigenmodes in the weak coupling regime is demonstrated. We analyze photoluminescence spectra of QDs embedded in monolithic micropillar cavities based on Bragg mirrors which contain MgSe/ZnTe/MgTe superlattices as low-index material. The pillar emission shows pronounced cavity eigenmodes and their spectral shape is in good agreement with simulations. QD emission in resonance with the cavity mode is shown to be efficiently guided toward the detector and an experimental Purcell enhancement by a factor of 5.7 is determined, confirming theoretical expectations.

cond-mat.mes-hall↗

arXiv2007

Poynting's theorem and energy conservation in the propagation of light in bounded media

Starting from the Maxwell-Lorentz equations, Poynting's theorem is reconsidered. The energy flux vector is introduced as S_e=(E x B)/mu_0 instead of E x H, because only by this choice the energy dissipation can be related to the balance of the kinetic energy of the matter subsystem. Conservation of the total energy as the sum of kinetic and electromagnetic energy follows. In our discussion, media and their microscopic nature are represented exactly by their susceptibility functions, which do not necessarily have to be known. On this footing, it can be shown that energy conservation in the propagation of light through bounded media is ensured by Maxwell's boundary conditions alone, even for some frequently used approximations. This is demonstrated for approaches using additional boundary conditions and the dielectric approximation in detail, the latter of which suspected to violate energy conservation for decades.

cond-mat.str-el↗