Ultrafast Coherent Exciton Couplings and Many-Body Interactions in Monolayer WS.

Transition metal dichalcogenides (TMDs) are quantum confined systems with interesting optoelectronic properties, governed by Coulomb interactions in the monolayer (1L) limit, where strongly bound excitons provide a sensitive probe for many-body interactions. Here, we use two-dimensional electronic spectroscopy (2DES) to investigate many-body interactions and their dynamics in 1L-WS at room temperature and with sub-10 fs time resolution. Our data reveal coherent interactions between the strongly detuned A and B exciton states in 1L-WS.

Phonon-driven intra-exciton Rabi oscillations in CsPbBr halide perovskites.

Coupling electromagnetic radiation with matter, e.g., by resonant light fields in external optical cavities, is highly promising for tailoring the optoelectronic properties of functional materials on the nanoscale.

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.

Electron Dynamics in a Two-Dimensional Nanobubble: A Two-Level System Based on Spatial Density.

Nanobubbles formed in monolayers of transition metal dichalcogenides (TMDCs) on top of a substrate feature localized potentials in which electrons can be captured. We show that the captured electronic density can exhibit a nontrivial spatiotemporal dynamics, whose movements can be mapped to states in a two-level system illustrated as points of an electronic Poincaré sphere. These states can be fully controlled, i.

The role of chalcogen vacancies for atomic defect emission in MoS.

For two-dimensional (2D) layered semiconductors, control over atomic defects and understanding of their electronic and optical functionality represent major challenges towards developing a mature semiconductor technology using such materials. Here, we correlate generation, optical spectroscopy, atomic resolution imaging, and ab initio theory of chalcogen vacancies in monolayer MoS. Chalcogen vacancies are selectively generated by in-vacuo annealing, but also focused ion beam exposure.

Twist Angle-Dependent Interlayer Exciton Lifetimes in van der Waals Heterostructures.

In van der Waals (vdW) heterostructures formed by stacking two monolayers of transition metal dichalcogenides, multiple exciton resonances with highly tunable properties are formed and subject to both vertical and lateral confinement. We investigate how a unique control knob, the twist angle between the two monolayers, can be used to control the exciton dynamics. We observe that the interlayer exciton lifetimes in MoSe_{2}/WSe_{2} twisted bilayers (TBLs) change by one order of magnitude when the twist angle is varied from 1° to 3.

Gate-Switchable Arrays of Quantum Light Emitters in Contacted Monolayer MoS van der Waals Heterodevices.

We demonstrate electrostatic switching of individual, site-selectively generated matrices of single photon emitters (SPEs) in MoS van der Waals heterodevices. We contact monolayers of MoS in field-effect devices with graphene gates and hexagonal boron nitride as the dielectric and graphite as bottom gates. After the assembly of such gate-tunable heterodevices, we demonstrate how arrays of defects, that serve as quantum emitters, can be site-selectively generated in the monolayer MoS by focused helium ion irradiation.

Imaging strain-localized excitons in nanoscale bubbles of monolayer WSe at room temperature.

In monolayer transition-metal dichalcogenides, localized strain can be used to design nanoarrays of single photon sources. Despite strong empirical correlation, the nanoscale interplay between excitons and local crystalline structure that gives rise to these quantum emitters is poorly understood. Here, we combine room-temperature nano-optical imaging and spectroscopic analysis of excitons in nanobubbles of monolayer WSe with atomistic models to study how strain induces nanoscale confinement potentials and localized exciton states.

Mahan excitons in room-temperature methylammonium lead bromide perovskites.

In a seminal paper, Mahan predicted that excitonic bound states can still exist in a semiconductor at electron-hole densities above the insulator-to-metal Mott transition. However, no clear evidence for this exotic quasiparticle, dubbed Mahan exciton, exists to date at room temperature. In this work, we combine ultrafast broadband optical spectroscopy and advanced many-body calculations to reveal that organic-inorganic lead-bromide perovskites host Mahan excitons at room temperature.

Optical generation of high carrier densities in 2D semiconductor heterobilayers.

Controlling charge density in two-dimensional (2D) materials is a powerful approach for engineering new electronic phases and properties. This control is traditionally realized by electrostatic gating. Here, we report an optical approach for generation of high carrier densities using transition metal dichalcogenide heterobilayers, WSe/MoSe, with type II band alignment.

Ultrafast Charge Carrier Relaxation in Inorganic Halide Perovskite Single Crystals Probed by Two-Dimensional Electronic Spectroscopy.

Halide perovskites are promising optoelectronic materials. Despite impressive device performance, especially in photovoltaics, the femtosecond dynamics of elementary optical excitations and their interactions are still debated. Here we combine ultrafast two-dimensional electronic spectroscopy (2DES) and semiconductor Bloch equations (SBEs) to probe the room-temperature dynamics of nonequilibrium excitations in CsPbBr crystals.

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.

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.

Emission from quantum-dot high-β microcavities: transition from spontaneous emission to lasing and the effects of superradiant emitter coupling.

Measured and calculated results are presented for the emission properties of a new class of emitters operating in the cavity quantum electrodynamics regime. The structures are based on high-finesse GaAs/AlAs micropillar cavities, each with an active medium consisting of a layer of InGaAs quantum dots (QDs) and the distinguishing feature of having a substantial fraction of spontaneous emission channeled into one cavity mode (high β-factor). This paper demonstrates that the usual criterion for lasing with a conventional (low β-factor) cavity, that is, a sharp non-linearity in the input-output curve accompanied by noticeable linewidth narrowing, has to be reinforced by the equal-time second-order photon autocorrelation function to confirm lasing.

A quantum optical study of thresholdless lasing features in high-β nitride nanobeam cavities.

Exploring the limits of spontaneous emission coupling is not only one of the central goals in the development of nanolasers, it is also highly relevant regarding future large-scale photonic integration requiring energy-efficient coherent light sources with a small footprint. Recent studies in this field have triggered a vivid debate on how to prove and interpret lasing in the high-β regime. We investigate close-to-ideal spontaneous emission coupling in GaN nanobeam lasers grown on silicon.

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.

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.

Long-Lived Direct and Indirect Interlayer Excitons in van der Waals Heterostructures.

We report the observation of a doublet structure in the low-temperature photoluminescence of interlayer excitons in heterostructures consisting of monolayer MoSe and WSe. Both peaks exhibit long photoluminescence lifetimes of several tens of nanoseconds up to 100 ns verifying the interlayer nature of the excitons. The energy and line width of both peaks show unusual temperature and power dependences.

Observation of Exciton Redshift-Blueshift Crossover in Monolayer WS.

We report a rare atom-like interaction between excitons in monolayer WS, 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.

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

We demonstrate pronounced electric-field-induced second-harmonic generation in naturally inversion symmetric 2H stacked bilayer MoS embedded into microcapacitor devices. By applying strong external electric field perturbations (|F| = ±2.6 MV cm) perpendicular to the basal plane of the crystal, we control the inversion symmetry breaking and, hereby, tune the nonlinear conversion efficiency.

Giant photon bunching, superradiant pulse emission and excitation trapping in quantum-dot nanolasers.

Light is often characterized only by its classical properties, like intensity or coherence. When looking at its quantum properties, described by photon correlations, new information about the state of the matter generating the radiation can be revealed. In particular the difference between independent and entangled emitters, which is at the heart of quantum mechanics, can be made visible in the photon statistics of the emitted light.

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.

Modulating the Substrate Selectivity of DNA Aptamers Using Surfactants.

Nucleic acid aptamers have a number of advantages compared to antibodies, including greater ease of production and increased thermal stability. We hypothesized that aptamers may also be capable of functioning in the presence of high concentrations of surfactants, which readily denature antibodies and other protein-based affinity reagents. Here we report the first systematic investigation into the compatibility of DNA aptamers with surfactants.

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.

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.