Control of structure and spin texture in the van der Waals layered magnet CrSBr.

Controlling magnetism at nanometer length scales is essential for realizing high-performance spintronic, magneto-electric and topological devices and creating on-demand spin Hamiltonians probing fundamental concepts in physics. Van der Waals (vdW)-bonded layered magnets offer exceptional opportunities for such spin texture engineering. Here, we demonstrate nanoscale structural control in the layered magnet CrSBr with the potential to create spin patterns without the environmental sensitivity that has hindered such manipulations in other vdW magnets. We drive a local phase transformation using an electron beam that moves atoms and exchanges bond directions, effectively creating regions that have vertical vdW layers embedded within the initial horizontally vdW bonded exfoliated flakes. We calculate that the newly formed two-dimensional structure is ferromagnetically ordered in-plane with an energy gap in the visible spectrum, and weak antiferromagnetism between the planes, suggesting possibilities for creating spin textures and quantum magnetic phases.

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.

Exciton fission 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 plasma of unbound fermionic particles or a gas of composite bosons called excitons. 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, we show that the thermodynamic fission-fusion balance of excitons and electron-hole plasma can be efficiently tuned via the dielectric environment as well as charge carrier doping. We propose the observation of these effects by studying exciton satellites in photoemission and tunneling spectroscopy, which present direct solid-state counterparts of high-energy collider experiments on the induced fission of composite particles.

A few-emitter solid-state multi-exciton laser.

We report on non-conventional lasing in a photonic-crystal nanocavity that operates with only four solid-state quantum-dot emitters. In a comparison between microscopic theory and experiment, we demonstrate that irrespective of emitter detuning, lasing with [Formula: see text] is facilitated by means of emission from dense-lying multi-exciton states. In the spontaneous-emission regime we find signatures for radiative coupling between the quantum dots. The realization of different multi-exciton states at different excitation powers and the presence of electronic inter-emitter correlations are reflected in a pump-rate dependence of the ß-factor.

Observation of Exciton Redshift-Blueshift Crossover in Monolayer WS2.

We report a rare atom-like interaction between excitons in monolayer WS2, measured using ultrafast absorption spectroscopy. At increasing excitation density, the exciton resonance energy exhibits a pronounced redshift followed by an anomalous blueshift. Using both material-realistic computation and phenomenological modeling, we attribute this observation to plasma effects and an attraction-repulsion crossover of the exciton-exciton interaction that mimics the Lennard-Jones potential between atoms. Our experiment demonstrates a strong analogy between excitons and atoms with respect to interparticle interaction, which holds promise to pursue the predicted liquid and crystalline phases of excitons in two-dimensional materials.

Electric-Field Switchable Second-Harmonic Generation in Bilayer MoS2 by Inversion Symmetry Breaking.

We demonstrate pronounced electric-field-induced second-harmonic generation in naturally inversion symmetric 2H stacked bilayer MoS2 embedded into microcapacitor devices. By applying strong external electric field perturbations (|F| = ±2.6 MV cm-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 (Eω ∼ 1.25-1.47 eV) probed by measuring the second-harmonic response at E2ω, 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 E2ω = 2.49 eV, energetically detuned by ΔE = E2ω - EC = -0.26 eV from the C-resonance (EC = 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.

Two-Dimensional Heterojunctions from Nonlocal Manipulations of the Interactions.

We propose to create lateral heterojunctions in two-dimensional materials based on nonlocal manipulations of the Coulomb interaction using structured dielectric environments. By means of ab initio calculations for MoS2 as well as generic semiconductor models, we show that the Coulomb interaction-induced self-energy corrections in real space are sufficiently nonlocal to be manipulated externally, but still local enough to induce spatially sharp interfaces within a single homogeneous monolayer to form heterojunctions. We find a type-II heterojunction band scheme promoted by a laterally structured dielectric environment, which exhibits a sharp band gap crossover within less than 5 unit cells.

Efficient Excitonic Photoluminescence in Direct and Indirect Band Gap Monolayer MoS2.

We discuss the photoluminescence (PL) of semiconducting transition metal dichalcogenides on the basis of experiments and a microscopic theory. The latter connects ab initio calculations of the single-particle states and Coulomb matrix elements with a many-body description of optical emission spectra. For monolayer MoS2, we study the PL efficiency at the excitonic A and B transitions in terms of carrier populations in the band structure and provide a quantitative comparison to an (In)GaAs quantum well-structure. Suppression and enhancement of PL under biaxial strain is quantified in terms of changes in the local extrema of the conduction and valence bands. The large exciton binding energy in MoS2 enables two distinctly different excitation methods: above-band gap excitation and quasi-resonant excitation of excitonic resonances below the single-particle band gap. The latter case creates a nonequilibrium distribution of carriers predominantly in the K-valleys, which leads to strong emission from the A-exciton transition and a visible B-peak even if the band gap is indirect. For above-band gap excitation, we predict a strongly reduced emission intensity at comparable carrier densities and the absence of B-exciton emission. The results agree well with PL measurements performed on monolayer MoS2 at excitation wavelengths of 405 nm (above) and 532 nm (below the band gap).

Influence of excited carriers on the optical and electronic properties of MoS2.

We study the ground-state and finite-density optical response of molybdenum disulfide by solving the semiconductor Bloch equations, using ab initio band structures and Coulomb interaction matrix elements. Spectra for excited carrier densities up to 10(13) cm(-2) reveal a redshift of the excitonic ground-state absorption, whereas higher excitonic lines are found to disappear successively due to Coulomb-induced band gap shrinkage of more than 500 meV and binding-energy reduction. Strain-induced band variations lead to a redshift of the lowest exciton line by ∼110 meV/% and change the direct transition to indirect while maintaining the magnitude of the optical response.

Emission properties and photon statistics of a single quantum dot laser.

A theoretical description for a single quantum-dot emitter in a microcavity is developed.We analyze for increasing steady-state pump rate the transition from the strong-coupling regime with photon antibunching to the weak-coupling regime with coherent emission. It is demonstrated how Coulomb interaction of excited carriers and excitation-induced dephasing can strongly modify the emission properties. Our theoretical investigations are based on a direct solution of the Liouville-von Neumann equation for the coupled carrier-photon system. We include multiple carrier excitations in the quantum dot, their Coulomb interaction, as well as excitation-induced dephasing and screening. Similarities and differences to atomic systems are discussed and results in the regime of recent experiments are interpreted.

Direct observation of correlations between individual photon emission events of a microcavity laser.

Lasers are recognized for coherent light emission, the onset of which is reflected in a change in the photon statistics. For many years, attempts have been made to directly measure correlations in the individual photon emission events of semiconductor lasers. Previously, the temporal decay of these correlations below or at the lasing threshold was considerably faster than could be measured with the time resolution provided by the Hanbury Brown/Twiss measurement set-up used. Here we demonstrate a measurement technique using a streak camera that overcomes this limitation and provides a record of the arrival times of individual photons. This allows us to investigate the dynamical evolution of correlations between the individual photon emission events. We apply our studies to micropillar lasers with semiconductor quantum dots as the active material, operating in the regime of cavity quantum electrodynamics. For laser resonators with a low cavity quality factor, Q, a smooth transition from photon bunching to uncorrelated emission with increasing pumping is observed; for high-Q resonators, we see a non-monotonic dependence around the threshold where quantum light emission can occur. We identify regimes of dynamical anti-bunching of photons in agreement with the predictions of a microscopic theory that includes semiconductor-specific effects.

Photon statistics of semiconductor microcavity lasers.

We present measurements of first- and second-order coherence of quantum-dot micropillar lasers together with a semiconductor laser theory. Our results show a broad threshold region for the observed high-beta microcavities. The intensity jump is accompanied by both pronounced photon intensity fluctuations and strong coherence length changes. The investigations clearly visualize a smooth transition from spontaneous to predominantly stimulated emission which becomes harder to determine for high beta. In our theory, a microscopic approach is used to incorporate the semiconductor nature of quantum dots. The results are in agreement with the experimental intensity traces and the photon statistics measurements.

Unified picture of polariton propagation in bulk GaAs semiconductors

High-resolution amplitude and phase linear spectroscopy of high-quality bulk GaAs are reported. The detailed structure of the observed full complex transmission is consistently explained by polariton effects on the basis of microscopic calculations. The coupled equations for the excitonic polarization and the light field in the slab configuration are evaluated using appropriate boundary conditions for the electromagnetic field and the excitonic wave function without reference to additional boundary conditions for the macroscopic polarization.

Quantum correlations in the nonperturbative regime of semiconductor microcavities.

The nonlinear optical response of semiconductor microcavities in the nonpertubative regime is studied in resonant single-beam-transmission and pump-probe experiments. In both cases a pronounced third transmission peak lying spectrally between the two normal modes is observed. A fully quantized theory is essential for the agreement with the experimental observations, demonstrating that quantum fluctuations leading to intraband polarizations are responsible for this effect.

Spontaneous emission lifetime of carriers in a semiconductor microcavity measured by photoluminescence without distortion by reabsorption.

A theory for carrier decay rates and a technique for measuring them are reported. Modification of the spontaneous emission rate of carriers by a semiconductor microcavity is investigated with 100-nm-thick bulk GaAs. Reabsorption makes the cavity-mode photoluminescence (PL) decay much faster than the square of the carrier density. Here reabsorption distortion is avoided by collecting PL that escapes the microcavity directly without multiple reflections: a ZnSe prism glued to the top mirror allows PL to escape at angles beyond the cutoff angle for total internal reflection without the prism. At these steep angles, the stop band of the top mirror has shifted to higher energy, so that it does not impede PL emission. Removal of most of the bottom mirror decreases the true carrier decay rate by only 25%, showing that the large enhancements deduced from cavity-mode PL are incorrect. Fully quantum mechanical computation including guided modes corroborates this conclusion. The prism technique could be used to study carrier dynamics and competition between guided and cavity modes in microcavities below and near threshold.

Pump geometry for resonant and quasi-resonant optical excitation of microcavity lasers.

A simple new pump geometry for optical excitation of microcavities and vertical-cavity surface-emitting lasers is presented. The technique circumvents the high reflectivity of the cavity stop band by excitation through the substrate at a large angle of incidence. Under these conditions, the reflectivity of the bottom Bragg reflector is small, and optical pumping at any desired photon energy becomes possible. Experimental results for optical excitation with this new geometry are compared with resonant optical pumping through the cavity mode.