Magnetism in two-dimensional materials reveals phenomena distinct from bulk magnetic crystals, with sensitivity to charge doping and electric fields in monolayer and bilayer van der Waals magnet CrI3. Within the class of layered magnets, semiconducting CrSBr stands out by featuring stability under ambient conditions, correlating excitons with magnetic order and thus providing strong magnon-exciton coupling, and exhibiting peculiar magneto-optics of exciton-polaritons. Here, we demonstrate that both exciton and magnetic transitions in bilayer and trilayer CrSBr are sensitive to voltage-controlled field-effect charging, exhibiting bound exciton-charge complexes and doping-induced metamagnetic transitions. Moreover, we demonstrate how these unique properties enable optical probes of local magnetic order, visualizing magnetic domains of competing phases across metamagnetic transitions induced by magnetic field or electrostatic doping. Our work identifies few-layer CrSBr as a rich platform for exploring collaborative effects of charge, optical excitations, and magnetism. CrSBr is a van der Waals layered antiferromagnet. Unlike many other van der Waals magnetic materials it is air stable, and in addition hosts a rich array of magneto-optical responses. Here, Tabataba-Vakili et al demonstrate that the magnetic and optical response of CrSBr is sensitive to gating, allowing electrical control of the magneto-optical properties.

Indistinguishable single photons in the telecom-bandwidth of optical fibers are indispensable for long-distance quantum communication. Solid-state single photon emitters have achieved excellent performance in key benchmarks, however, the demonstration of indistinguishability at room-temperature remains a major challenge. Here, we report room-temperature photon indistinguishability at telecom wavelengths from individual nanotube defects in a fiber-based microcavity operated in the regime of incoherent good cavity-coupling. The efficiency of the coupled system outperforms spectral or temporal filtering, and the photon indistinguishability is increased by more than two orders of magnitude compared to the free-space limit. Our results highlight a promising strategy to attain optimized non-classical light sources. Carbon nanotube-based single photon emitters allow for room-temperature operation, but suffer from vanishing indistinguishability due to strong dephasing. Following a theoretical proposal, the authors tackle the problem experimentally by using a cavity to enhance the photon coherence time and the emission spectral density in the regime of incoherent good cavity-coupling.

We report experimental and theoretical studies of MoTe2-MoSe2 heterobilayers with rigid moiré superlattices controlled by the twist angle. Using an effective continuum model that combines resonant interlayer electron tunneling with stacking-dependent moiré potentials, we identify the nature of moiré excitons and the dependence of their energies, oscillator strengths, and Landé g-factors on the twist angle. Within the same framework, we interpret distinct signatures of bound complexes among electrons and moiré excitons in nearly collinear heterostacks. Our work provides a fundamental understanding of hybrid moiré,. excitons and trions in MoTe2-MoSe2 heterobilayers and establishes the material system as a prime candidate for optical studies of correlated phenomena in moiré lattices.

We study experimentally and theoretically the hybridization among intralayer and interlayer moire excitons in a MoSe2/WS2 heterostructure with antiparallel alignment. Using a dual -gate device and cryogenic white light reflectance and narrow-band laser modulation spectroscopy, we subject the moire excitons in the MoSe2/WS2 heterostack to a perpendicular electric field, monitor the field-induced dispersion and hybridization of intralayer and interlayer moire exciton states, and induce a crossover from type I to type II band alignment. Moreover, we employ perpendicular magnetic fields to map out the dependence of the corresponding exciton Land e g factors on the electric field. Finally, we develop an effective theoretical model combining resonant and nonresonant contributions to moire potentials to explain the observed phenomenology, and highlight the relevance of interlayer coupling for structures with close energetic band alignment as in MoSe2/WS2.

Interlayer exciton diffusion is studied in atomically reconstructed MoSe2/WSe2 heterobilayers with suppressed disorder. Local atomic registry is confirmed by characteristic optical absorption, circularly polarized photoluminescence, and g -factor measurements. Using transient microscopy we observe propagation properties of interlayer excitons that are independent from trapping at moire '- or disorderinduced local potentials. Confirmed by characteristic temperature dependence for free particles, linear diffusion coefficients of interlayer excitons at liquid helium temperature and low excitation densities are almost 1000 times higher than in previous observations. We further show that exciton-exciton repulsion and annihilation contribute nearly equally to nonlinear propagation by disentangling the two processes in the experiment and simulations. Finally, we demonstrate effective shrinking of the light emission area over time across several hundreds of picoseconds at the transition from exciton- to the plasma -dominated regimes. Supported by microscopic calculations for band gap renormalization to identify the Mott threshold, this indicates transient crossing between rapidly expanding, short-lived electron -hole plasma and slower, long-lived exciton populations.

Moire interference effects influence profoundly the optoelectronic properties of vertical van der Waals structures. Here we systematically establish secondary electron imaging in a scanning electron microscope as a powerful technique for visualizing reconstruction of moire lattices into registry-contrasting domains in vertical homobilayers and heteorbilayers of transition metal dichalcogenides (TMDs) with parallel and antiparallel alignment. With optimal parameters for contrast-maximizing imaging of high-symmetry registries, we identify distinct crystal realizations of WSe2 homobilayers and MoSe2-WSe2 heterostructures synthesized by chemical vapor deposition. In particular, we find evidence for a mutually exclusive competition between RhX and RhM registries, manifesting in complete reconstruction of bilayer crystals into one distinct registry or alternating large-area domains in RhX and RhM stacking. Our results have immediate implications for the optical properties of registry-specific excitons in layered stacks of TMDs, and demonstrate the general potential of secondary electron imaging for van der Waals twistronics.

Their outstanding electrical and optical properties make semiconducting single-walled carbon nanotubes (SWCNTs) highly suitable for charge transport and emissive layers in near-infrared optoelectronic devices. However, the luminescence spectra of SWCNT thin films on commonly used glass and Si/SiO2 substrates are often compromised by broadening of the main excitonic emission and unwanted low-energy sidebands. Surface passivation with a commercially available, low dielectric constant, cross-linked bis-benzocyclobutene-based polymer (BCB) enhances the emission properties of SWCNTs to the same level as hexagonal boron nitride (h-BN) flakes do. The presence of BCB suppresses sideband emission, especially from the Y-1 band, which is attributed to defects introduced by the interaction of the nanotube lattice with oxygen-containing terminal groups of the substrate surface. The facile and reproducible deposition of homogeneous BCB films over large areas combined with their resistance against common solvents and chemicals employed during photolithography make them compatible with standard semiconductor device fabrication. Utilizing this approach, light-emitting (6,5) SWCNT network field-effect transistors are fabricated on BCB-treated glass substrates with excellent electrical characteristics and near-intrinsic electroluminescence. Hence, passivation with BCB is proposed as a standard treatment for substrates used for spectroscopic investigations of and optoelectronic devices with SWCNTs and other low-dimensional emitters.

Moire effects in vertical stacks of two-dimensional crystals give rise to new quantum materials with rich transport and optical phenomena that originate from modulations of atomic registries within moire supercells. Due to finite elasticity, however, the superlattices can transform from moire-type to periodically reconstructed patterns. Here we expand the notion of such nanoscale lattice reconstruction to the mesoscopic scale of laterally extended samples and demonstrate rich consequences in optical studies of excitons in MoSe2-WSe2 heterostructures with parallel and antiparallel alignments. Our results provide a unified perspective on moire excitons in near-commensurate semiconductor heterostructures with small twist angles by identifying domains with exciton properties of distinct effective dimensionality, and establish mesoscopic reconstruction as a compelling feature of real samples and devices with inherent finite size effects and disorder. Generalized to stacks of other two-dimensional materials, this notion of mesoscale domain formation with emergent topological defects and percolation networks will instructively expand the understanding of fundamental electronic, optical and magnetic properties of van der Waals heterostructures. Moire lattice reconstruction on mesoscopic length scales gives rise to diverse exciton signatures within emergent domains of different dimensionality.

Vertical van der Waals heterostructures of semiconducting transition metal dichalcogenides realize moire systems with rich correlated electron phases and moire exciton phenomena. For material combinations with small lattice mismatch and twist angles as in MoSe2-WSe2, however, lattice reconstruction eliminates the canonical moire pattern and instead gives rise to arrays of periodically reconstructed nanoscale domains and mesoscopically extended areas of one atomic registry. Here, we elucidate the role of atomic reconstruction in MoSe2-WSe2 heterostructures synthesized by chemical vapor deposition. With complementary imaging down to the atomic scale, simulations, and optical spectroscopy methods, we identify the coexistence of moire-type cores and extended moire-free regions in heterostacks with parallel and antiparallel alignment. Our work highlights the potential of chemical vapor deposition for applications requiring laterally extended heterosystems of one atomic registry or exciton-confining heterostack arrays.

Chirality is a fundamental asymmetry phenomenon, with chiral optical elements exhibiting asymmetric response in reflection or absorption of circularly polarized light. Recent realizations of such elements include nanoplasmonic systems with broken-mirror symmetry and polarization-contrasting optical absorption known as circular dichroism. An alternative route to circular dichroism is provided by spin-valley polarized excitons in atomically thin semiconductors. In the presence of magnetic fields, they exhibit an imbalanced coupling to circularly polarized photons and thus circular dichroism. Here, we demonstrate that polarization-contrasting optical transitions associated with excitons in monolayer WSe2 can be transferred to proximal plasmonic nanodisks by coherent coupling. The coupled exciton-plasmon system exhibits magneto induced circular dichroism in a spectrally narrow window of Fano interference, which we model in a master equation framework. Our work motivates the use of exciton-plasmon interfaces as building blocks of chiral metasurfaces for applications in information processing, nonlinear optics, and sensing.

We report the implementation of energy-dispersive x-ray spectroscopy for high-resolution inspection of layered semiconductors in the form of atomically thin transition metal dichalcogenides down to the monolayer limit. The technique is based on a scanning electron microscope equipped with a silicon drift detector for energy-dispersive x-ray analysis. By optimizing operational parameters in numerical simulations and experiments, we achieve layer-resolving sensitivity for few-layer crystals down to the monolayer, and demonstrate elemental composition profiling in vertical and lateral heterobilayers of transition metal dichalcogenides. The technique can be straightforwardly applied to other layered two-dimensional materials and van der Waals heterostructures, thus expanding the experimental toolbox for quantitative characterization of layer number, atomic composition, or alloy gradients for atomically thin materials and devices.

We utilize cavity-enhanced extinction spectroscopy to directly quantify the optical absorption of defects in MoS2 generated by helium ion bombardment. We achieve hyperspectral imaging of specific defect patterns with a detection limit below 0.01% extinction, corresponding to a detectable defect density below 1 x 10(11) cm(-2). The corresponding spectra reveal a broad subgap absorption, being consistent with theoretical predictions related to sulfur vacancy-bound excitons in MoS2. Our results highlight cavity-enhanced extinction spectroscopy as efficient means for the detection of optical transitions in nanoscale thin films with weak absorption, applicable to a broad range of materials.

Twisted layers of atomically thin two-dimensional materials realize a broad range of quantum materials with engineered optical and transport phenomena arising from spin and valley degrees of freedom and strong electron correlations in hybridized interlayer bands. Here, we report on experimental and theoretical studies of WSe2 homobilayers obtained in two stable configurations of 2H (60?? twist) and 3R (0?? twist) stackings by controlled chemical vapor synthesis of high-quality large-area crystals. Using optical absorption and photoluminescence (PL) spectroscopy at cryogenic temperatures, we uncover marked differences in the optical characteristics of 2H and 3R bilayer WSe2 which we explain on the basis of beyond-density functional theory calculations. Our results highlight the role of layer stacking for the spectral multiplicity of momentum-direct intralayer exciton transitions in absorption and relate the multiplicity of phonon sidebands in the PL to momentum-indirect excitons with different spin valley and layer character. Our comprehensive study generalizes to other layered homobilayer and heterobilayer semiconductor systems and highlights the role of crystal symmetry and stacking for interlayer hybrid states.

We report an experimental study of temperature-dependent spectral line shapes of phonon sideband emission stemming from dark excitons in monolayer and bilayer WSe2. Using photoluminescence spectroscopy in the range from 4 to 100 K, we observe a pronounced asymmetry in the phonon-assisted luminescence from momentum-indirect exciton reservoirs. We demonstrate that the corresponding spectral profiles are distinct from those of bright excitons with direct radiative decay pathways. The line-shape asymmetry reflects thermal distribution of exciton states with finite center-of-mass momenta, characteristic for phonon sideband emission. The extracted temperature of the exciton reservoirs is found to generally follow that of the crystal lattice, with deviations reflecting overheated populations. The latter are most pronounced in the bilayer case and at lowest temperatures. Our results add to the understanding of phonon-assisted recombination of momentum-dark excitons and, more generally, establish means to access the thermal distribution of finite-momentum excitons in atomically thin semiconductors with indirect band gaps.

The introduction of an optical resonator can enable efficient and precise interaction between a photon and a solid-state emitter. It facilitates the study of strong light-matter interaction, polaritonic physics and presents a powerful interface for quantum communication and computing. A pivotal aspect in the progress of light-matter interaction with solid-state systems is the challenge of combining the requirements of cryogenic temperature and high mechanical stability against vibrations while maintaining sufficient degrees of freedom for in situ tunability. Here, we present a fiber-based open Fabry-Perot cavity in a closed-cycle cryostat exhibiting ultrahigh mechanical stability while providing wide-range tunability in all three spatial directions. We characterize the setup and demonstrate the operation with the root-mean-square cavity-length fluctuation of less than 90 pm at temperature of 6.5 K and integration bandwidth of 100 kHz. Finally, we benchmark the cavity performance by demonstrating the strong-coupling formation of exciton polaritons in monolayer WSe2 with a cooperativity of 1.6. This set of results manifests the open cavity in a closed-cycle cryostat as a versatile and powerful platform for low-temperature cavity QED experiments.

The controlled functionalization of single-walled carbon nanotubes with luminescent sp(3)-defects has created the potential to employ them as quantum-light sources in the near-infrared. For that, it is crucial to control their spectral diversity. The emission wavelength is determined by the binding configuration of the defects rather than the molecular structure of the attached groups. However, current functionalization methods produce a variety of binding configurations and thus emission wavelengths. We introduce a simple reaction protocol for the creation of only one type of luminescent defect in polymer-sorted (6,5) nanotubes, which is more red-shifted and exhibits longer photoluminescence lifetimes than the commonly obtained binding configurations. We demonstrate single-photon emission at room temperature and expand this functionalization to other polymer-wrapped nanotubes with emission further in the near-infrared. As the selectivity of the reaction with various aniline derivatives depends on the presence of an organic base we propose nucleophilic addition as the reaction mechanism. Covalent functionalization of single-walled carbon nanotubes with luminescent sp(3)-defects generally produces a variety of binding configurations and emission wavelengths. The authors propose a base-mediated nucleophilic functionalization approach to selectively achieve configurations for E-11* and E-11*(-) or purely E-11*(-) defect emission.

The functionalization of single-walled carbon nanotubes (SWCNTs) with luminescent sp(3) defects has greatly improved their performance in applications such as quantum light sources and bioimaging. Here, we report the covalent functionalization of purified semiconducting SWCNTs with stable organic radicals (perchlorotriphenylmethyl, PTM) carrying a net spin. This model system allows us to use the near-infrared photoluminescence arising from the defect-localized exciton as a highly sensitive probe for the short-range interaction between the PTM radical and the SWCNT. Our results point toward an increased triplet exciton population due to radical-enhanced intersystem crossing, which could provide access to the elusive triplet manifold in SWCNTs. Furthermore, this simple synthetic route to spin-labeled defects could enable magnetic resonance studies complementary to in vivo fluorescence imaging with functionalized SWCNTs and facilitate the scalable fabrication of spintronic devices with magnetically switchable charge transport.

Layered two-dimensional materials exhibit rich transport and optical phenomena in twisted or lattice-incommensurate heterostructures with spatial variations of interlayer hybridization arising from moire interference effects. Here, we report experimental and theoretical studies of excitons in twisted heterobilayers and heterotrilayers of transition metal dichalcogenides. Using MoSe2-WSe2 stacks as representative realizations of twisted van der Waals bilayer and trilayer heterostructures, we observe contrasting optical signatures and interpret them in the theoretical framework of interlayer moire excitons in different spin and valley configurations. We conclude that the photoluminescence of MoSe2-WSe2 heterobilayer is consistent with joint contributions from radiatively decaying valley-direct interlayer excitons and phonon-assisted emission from momentum-indirect reservoirs that reside in spatially distinct regions of moire supercells, whereas the heterotrilayer emission is entirely due to momentum-dark interlayer excitons of hybrid-layer valleys. Our results highlight the profound role of interlayer hybridization for transition metal dichalcogenide heterostacks and other realizations of multi-layered semiconductor van der Waals heterostructures. Here, the authors show that the photoluminescence of MoSe2/WSe2 heterobilayers is dominated by valley-direct excitons, whereas, in heterotrilayers, interlayer hybridization turns momentum-indirect interlayer excitons into energetically lowest states with phonon-assisted emission.

In monolayers of transition metal dichalcogenides the nonlocal nature of the effective dielectric screening leads to large binding energies of excitons. Additional lateral confinement gives rise to exciton localization in quantum dots. By assuming parabolic confinement for both the electron and the hole, we derive model wave functions for the relative and the center-of-mass motions of electronhole pairs, and investigate theoretically resonant energy transfer among excitons localized in two neighboring quantum dots. We quantify the probability of energy transfer for a direct- gap transition by assuming that the interaction between two quantum dots is described by a Coulomb potential, which allows us to include all relevant multipole terms of the interaction. We demonstrate the structural control of the valley-selective energy transfer between quantum dots.

The optical properties of monolayer and bilayer transition metal dichalcogenide semiconductors are governed by excitons in different spin and valley configurations, providing versatile aspects for van der Waals heterostructures and devices. Here, we present experimental and theoretical studies of exciton energy splittings in external magnetic field in neutral and charged WSe2 monolayer and bilayer crystals embedded in a field effect device for active doping control. We develop theoretical methods to calculate the exciton g-factors from first principles for all possible spin-valley configurations of excitons in monolayer and bilayer WSe2 including valley-indirect excitons. Our theoretical and experimental findings shed light on some of the characteristic photoluminescence peaks observed for monolayer and bilayer WSe2. In more general terms, the theoretical aspects of our work provide additional means for the characterization of single and few-layer transition metal dichalcogenides, as well as their heterostructures, in the presence of external magnetic fields.

Trions, charged excitons that are reminiscent of hydrogen and positronium ions, have been intensively studied for energy harvesting, light-emitting diodes, lasing, and quantum computing applications because of their inherent connection with electron spin and dark excitons. However, these quasi-particles are typically present as a minority species at room temperature making it difficult for quantitative experimental measurements. Here, we show that by chemically engineering the well depth of sp3 quantum defects through a series of alkyl functional groups covalently attached to semiconducting carbon nanotube hosts, trions can be efficiently generated and localized at the trapping chemical defects. The exciton-electron binding energy of the trapped trion approaches 119 meV, which more than doubles that of “free” trions in the same host material (54 meV) and other nanoscale systems (2–45 meV). Magnetoluminescence spectroscopy suggests the absence of dark states in the energetic vicinity of trapped trions. Unexpectedly, the trapped trions are approximately 7.3-fold brighter than the brightest previously reported and 16 times as bright as native nanotube excitons, with a photoluminescence lifetime that is more than 100 times larger than that of free trions. These intriguing observations are understood by an efficient conversion of dark excitons to bright trions at the defect sites. This work makes trions synthetically accessible and uncovers the rich photophysics of these tricarrier quasi-particles, which may find broad implications in bioimaging, chemical sensing, energy harvesting, and light emitting in the short-wave infrared.

Defect-decorated single-wall carbon nanotubes have shown rapid growing potential for imaging, sensing, and the development of room-temperature single-photon sources. The key to the highly nonclassical emission statistics is the discrete energy spectrum of defect-localized excitons. However, variations in defect configurations give rise to distinct spectral bands that may compromise single-photon efficiency and purity in practical devices, and experimentally it has been challenging to study the exciton population distribution among the various defect-specific states. Here, we performed photon correlation spectroscopy on hexyl-decorated single-wall carbon nanotubes to unravel the dynamics and competition between neutral and charged exciton populations. With autocorrelation measurements at the single-tube level, we prove the nonclassical photon emission statistics of defect-specific exciton and trion photoluminescence and identify their mutual exclusiveness in photoemissive events with cross-correlation spectroscopy. Moreover, our study reveals the presence of a dark state with population-shelving time scales between 10 and 100 ns. These new insights will guide further development of chemically tailored carbon nanotube states for quantum photonics applications.

Monolayer transition metal dichalcogenides integrated in optical microcavities host exciton-polaritons as a hallmark of the strong light-matter coupling regime. Analogous concepts for hybrid light-matter systems employing spatially indirect excitons with a permanent electric dipole moment in heterobilayer crystals promise realizations of exciton-polariton gases and condensates with inherent dipolar interactions. Here, we implement cavity-control of interlayer excitons in vertical MoSe2-WSe2 heterostructures. Our experiments demonstrate the Purcell effect for heterobilayer emission in cavity-modified photonic environments, and quantify the light-matter coupling strength of interlayer excitons. The results will facilitate further developments of dipolar exciton-polariton gases and condensates in hybrid cavity - van der Waals heterostructure systems.

We report the observation of ubiquitous contamination of dielectric substrates and poly(methyl methacrylate) matrices by organic molecules with optical transitions in the visible spectral range. Contamination sites of individual solvent-related fluorophores in thin films of poly(methyl methacrylate) constitute fluorescence hotspots with quantum emission statistics and quantum yields approaching 30% at cryogenic temperatures. Our findings not only resolve prevalent puzzles in the assignment of spectral features to various nanoemitters on bare dielectric substrates or in polymer matrices but also identify the means for the simple and cost-efficient realization of single-photon sources in the visible spectral range.

Charge carriers in semiconducting transition metal dichalcogenides possess a valley degree of freedom that allows for optoelectronic applications based on the momentum of excitons. At elevated temperatures, scattering by phonons limits valley polarization, making a detailed knowledge about strength and nature of the interaction of excitons with phonons essential. In this work, we directly access exciton-phonon coupling in charge tunable single layer MoS2 devices by polarization resolved Raman spectroscopy. We observe a strong defect mediated coupling between the long-range oscillating electric field induced by the longitudinal optical phonon in the dipolar medium and the exciton. This so-called Frohlich exciton phonon interaction is suppressed by doping. The suppression correlates with a distinct increase of the degree of valley polarization up to 20% even at elevated temperatures of 220 K. Our result demonstrates a promising strategy to increase the degree of valley polarization towards room temperature valleytronic applications.