Controlled Coherent Coupling in a Quantum Dot Molecule Revealed by Ultrafast Four-Wave Mixing Spectroscopy.

Semiconductor quantum dot molecules are considered promising candidates for quantum technological applications due to their wide tunability of optical properties and coverage of different energy scales associated with charge and spin physics. While previous works have studied the tunnel-coupling of the different excitonic charge complexes shared by the two quantum dots by conventional optical spectroscopy, we here report on the first demonstration of a coherently controlled interdot tunnel-coupling focusing on the quantum coherence of the optically active trion transitions. We employ ultrafast four-wave mixing spectroscopy to resonantly generate a quantum coherence in one trion complex, transfer it to and probe it in another trion configuration. With the help of theoretical modeling on different levels of complexity, we give an instructive explanation of the underlying coupling mechanism and dynamical processes.

Coupling of MoS_{2} Excitons with Lattice Phonons and Cavity Vibrational Phonons in Hybrid Nanobeam Cavities.

We report resonant Raman spectroscopy of neutral excitons X^{0} and intravalley trions X^{-} in hBN-encapsulated MoS_{2} monolayer embedded in a nanobeam cavity. By temperature tuning the detuning between Raman modes of MoS_{2} lattice phonons and X^{0}/X^{-} emission peaks, we probe the mutual coupling of excitons, lattice phonons and cavity vibrational phonons. We observe an enhancement of X^{0}-induced Raman scattering and a suppression for X^{-}-induced, and explain our findings as arising from the tripartite exciton-phonon-phonon coupling. The cavity vibrational phonons provide intermediate replica states of X^{0} for resonance conditions in the scattering of lattice phonons, thus enhancing the Raman intensity. In contrast, the tripartite coupling involving X^{-} is found to be much weaker, an observation explained by the geometry-dependent polarity of the electron and hole deformation potentials. Our results indicate that phononic hybridization between lattice and nanomechanical modes plays a key role in the excitonic photophysics and light-matter interaction in 2D-material nanophotonic systems.

Three-Photon Excitation of InGaN Quantum Dots.

We demonstrate that semiconductor quantum dots can be excited efficiently in a resonant three-photon process, while resonant two-photon excitation is highly suppressed. Time-dependent Floquet theory is used to quantify the strength of the multiphoton processes and model the experimental results. The efficiency of these transitions can be drawn directly from parity considerations in the electron and hole wave functions in semiconductor quantum dots. Finally, we exploit this technique to probe intrinsic properties of InGaN quantum dots. In contrast to nonresonant excitation, slow relaxation of charge carriers is avoided, which allows us to measure directly the radiative lifetime of the lowest energy exciton states. Since the emission energy is detuned far from the resonant driving laser field, polarization filtering is not required and emission with a greater degree of linear polarization is observed compared to nonresonant excitation.

Sb-Mediated Tuning of Growth- and Exciton Dynamics in Entirely Catalyst-Free GaAsSb Nanowires.

Vapor-liquid-solid (VLS) growth is the mainstream method in realizing advanced semiconductor nanowires (NWs), as widely applied to many III-V compounds. It is exclusively explored also for antimony (Sb) compounds, such as the relevant GaAsSb-based NW materials, although morphological inhomogeneities, phase segregation, and limitations in the supersaturation due to Sb strongly inhibit their growth dynamics. Fundamental advances are now reported here via entirely catalyst-free GaAsSb NWs, where particularly the Sb-mediated effects on the NW growth dynamics and physical properties are investigated in this novel growth regime. Remarkably, depending on GaAsSb composition and nature of the growth surface, both surfactant and anti-surfactant action is found, as seen by transitions between growth acceleration and deceleration characteristics. For threshold Sb-contents up to 3-4%, adatom diffusion lengths are increased ≈sevenfold compared to Sb-free GaAs NWs, evidencing the significant surfactant effect. Furthermore, microstructural analysis reveals unique Sb-mediated transitions in compositional structure, as well as substantial reduction in twin defect density, ≈tenfold over only small compositional range (1.5-6% Sb), exhibiting much larger dynamics as found in VLS-type GaAsSb NWs. The effect of such extended twin-free domains is corroborated by ≈threefold increases in exciton lifetime (≈4.5 ns) due to enlarged electron-hole pair separation in these phase-pure NWs.

Twist-Dependent Intra- and Interlayer Excitons in Moiré MoSe_{2} 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 moiré coupling in MoSe_{2} 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 moiré pattern in the MoSe_{2} homobilayers, as confirmed by our low-energy continuum model for different moiré excitons. We identify two distinct intralayer moiré 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 moiré exciton species.

The dependence of timing jitter of superconducting nanowire single-photon detectors on the multi-layer sample design and slew rate.

We investigated the timing jitter of superconducting nanowire single-photon detectors (SNSPDs) and found a strong dependence on the detector response. By varying the multi-layer structure, we observed changes in pulse shape which are attributed to capacitive behaviour affecting the pulse heights, rise times and consequently timing jitter. Moreover, we developed a technique to predict the timing jitter of a single device within certain limits by capturing only a single detector pulse, eliminating the need for detailed jitter measurement using a pulsed laser when a rough estimate of the timing jitter is sufficient.

Real-Time Investigation of Sulfur Vacancy Generation and Passivation in Monolayer Molybdenum Disulfide via in situ X-ray Photoelectron Spectromicroscopy.

Understanding the chemical and electronic properties of point defects in two-dimensional materials, as well as their generation and passivation, is essential for the development of functional systems, spanning from next-generation optoelectronic devices to advanced catalysis. Here, we use synchrotron-based X-ray photoelectron spectroscopy (XPS) with submicron spatial resolution to create sulfur vacancies (SVs) in monolayer MoS2 and monitor their chemical and electronic properties in situ during the defect creation process. X-ray irradiation leads to the emergence of a distinct Mo 3d spectral feature associated with undercoordinated Mo atoms. Real-time analysis of the evolution of this feature, along with the decrease of S content, reveals predominant monosulfur vacancy generation at low doses and preferential disulfur vacancy generation at high doses. Formation of these defects leads to a shift of the Fermi level toward the valence band (VB) edge, introduction of electronic states within the VB, and formation of lateral pn junctions. These findings are consistent with theoretical predictions that SVs serve as deep acceptors and are not responsible for the ubiquitous n-type conductivity of MoS2. In addition, we find that these defects are metastable upon short-term exposure to ambient air. By contrast, in situ oxygen exposure during XPS measurements enables passivation of SVs, resulting in partial elimination of undercoordinated Mo sites and reduction of SV-related states near the VB edge. Correlative Raman spectroscopy and photoluminescence measurements confirm our findings of localized SV generation and passivation, thereby demonstrating the connection between chemical, structural, and optoelectronic properties of SVs in MoS2.

3D Bragg Coherent Diffraction Imaging of Extended Nanowires: Defect Formation in Highly Strained InGaAs Quantum Wells.

InGaAs quantum wells embedded in GaAs nanowires can serve as compact near-infrared emitters for direct integration onto Si complementary metal oxide semiconductor technology. While the core-shell geometry in principle allows for a greater tuning of composition and emission, especially farther into the infrared, the practical limits of elastic strain accommodation in quantum wells on multifaceted nanowires have not been established. One barrier to progress is the difficulty of directly comparing the emission characteristics and the precise microstructure of a single nanowire. Here we report an approach to correlating quantum well morphology, strain, defects, and emission to understand the limits of elastic strain accommodation in nanowire quantum wells specific to their geometry. We realize full 3D Bragg coherent diffraction imaging (BCDI) of intact quantum wells on vertically oriented epitaxial nanowires, which enables direct correlation with single-nanowire photoluminescence. By growing In0.2Ga0.8As quantum wells of distinct thicknesses on different facets of the same nanowire, we identified the critical thickness at which defects are nucleated. A correlation with a traditional transmission electron microscopy analysis confirms that BCDI can image the extended structure of defects. Finite element simulations of electron and hole states explain the emission characteristics arising from strained and partially relaxed regions. This approach, imaging the 3D strain and microstructure of intact nanowire core-shell structures with application-relevant dimensions, can aid the development of predictive models that enable the design of new compact infrared emitters.

On-chip generation and dynamic piezo-optomechanical rotation of single photons.

Integrated photonic circuits are key components for photonic quantum technologies and for the implementation of chip-based quantum devices. Future applications demand flexible architectures to overcome common limitations of many current devices, for instance the lack of tuneabilty or built-in quantum light sources. Here, we report on a dynamically reconfigurable integrated photonic circuit comprising integrated quantum dots (QDs), a Mach-Zehnder interferometer (MZI) and surface acoustic wave (SAW) transducers directly fabricated on a monolithic semiconductor platform. We demonstrate on-chip single photon generation by the QD and its sub-nanosecond dynamic on-chip control. Two independently applied SAWs piezo-optomechanically rotate the single photon in the MZI or spectrally modulate the QD emission wavelength. In the MZI, SAWs imprint a time-dependent optical phase and modulate the qubit rotation to the output superposition state. This enables dynamic single photon routing with frequencies exceeding one gigahertz. Finally, the combination of the dynamic single photon control and spectral tuning of the QD realizes wavelength multiplexing of the input photon state and demultiplexing it at the output. Our approach is scalable to multi-component integrated quantum photonic circuits and is compatible with hybrid photonic architectures and other key components for instance photonic resonators or on-chip detectors.

Ultra-Sensitive Extinction Measurements of Optically Active Defects in Monolayer MoS2.

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 × 1011 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.

Nonlocal Exciton-Photon Interactions in Hybrid High-Q Beam Nanocavities with Encapsulated MoS_{2} Monolayers.

Atomically thin semiconductors can be readily integrated into a wide range of nanophotonic architectures for applications in quantum photonics and novel optoelectronic devices. We report the observation of nonlocal interactions of "free" trions in pristine hBN/MoS_{2}/hBN heterostructures coupled to single mode (Q>10^{4}) quasi 0D nanocavities. The high excitonic and photonic quality of the interaction system stems from our integrated nanofabrication approach simultaneously with the hBN encapsulation and the maximized local cavity field amplitude within the MoS_{2} monolayer. We observe a nonmonotonic temperature dependence of the cavity-trion interaction strength, consistent with the nonlocal light-matter interactions in which the extent of the center-of-mass (c.m.) wave function is comparable to the cavity mode volume in space. Our approach can be generalized to other optically active 2D materials, opening the way toward harnessing novel light-matter interaction regimes for applications in quantum photonics.

Unveiling the Zero-Phonon Line of the Boron Vacancy Center by Cavity-Enhanced Emission.

Negatively charged boron vacancies (VB-) in hexagonal boron nitride (hBN) exhibit a broad emission spectrum due to strong electron-phonon coupling and Jahn-Teller mixing of electronic states. As such, the direct measurement of the zero-phonon line (ZPL) of VB- has remained elusive. Here, we measure the room-temperature ZPL wavelength to be 773 ± 2 nm by coupling the hBN layer to the high-Q nanobeam cavity. As the wavelength of cavity mode is tuned, we observe a pronounced intensity resonance, indicating the coupling to VB-. Our observations are consistent with the spatial redistribution of VB- emission. Spatially resolved measurements show a clear Purcell effect maximum at the midpoint of the nanobeam, in accord with the optical field distribution of the cavity mode. Our results are in good agreement with theoretical calculations, opening the way to using VB- as cavity spin-photon interfaces.

Stimulated Generation of Indistinguishable Single Photons from a Quantum Ladder System.

We propose a scheme for the generation of highly indistinguishable single photons using semiconductor quantum dots and demonstrate its performance and potential. The scheme is based on the resonant two-photon excitation of the biexciton followed by stimulation of the biexciton to selectively prepare an exciton. Quantum-optical simulations and experiments are in good agreement and show that the scheme provides significant advantages over previously demonstrated excitation methods. The two-photon excitation of the biexciton suppresses re-excitation and enables ultralow multiphoton errors, while the precisely timed stimulation pulse results in very low timing jitter of the photons, and consequently, high indistinguishability. In addition, the polarization of the stimulation pulse allows us to deterministically program the polarization of the emitted photon (H or V). This ensures that all emission of interest occurs in the polarization of the detection channel, resulting in higher brightness than cross-polarized resonant excitation.

Tuning the Optical Properties of a MoSe2 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 subwavelength length scales approaching the exciton Bohr radius. Here, we present room- and cryogenic-temperature investigations of a MoSe2 monolayer on individual gold dipole nanoantennas. By controlling nanoantenna size, the dipolar resonance is tuned relative to the exciton achieving a total tuning of ∼130 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 meV, representing g/(ℏωX) ≥ 3% of the transition energy. This places our hybrid system in the intermediate-coupling regime where spectra exhibit a characteristic Fano-like shape. We demonstrate active control 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 K.

Efficient Optomechanical Mode-Shape Mapping of Micromechanical Devices.

Visualizing eigenmodes is crucial in understanding the behavior of state-of-the-art micromechanical devices. We demonstrate a method to optically map multiple modes of mechanical structures simultaneously. The fast and robust method, based on a modified phase-lock loop, is demonstrated on a silicon nitride membrane and shown to outperform three alternative approaches. Line traces and two-dimensional maps of different modes are acquired. The high quality data enables us to determine the weights of individual contributions in superpositions of degenerate modes.

Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites.

Materials combining semiconductor functionalities with spin control are desired for the advancement of quantum technologies. Here, we study the magneto-optical properties of novel paramagnetic Ruddlesden-Popper hybrid perovskites Mn:(PEA)2PbI4 (PEA = phenethylammonium) and report magnetically brightened excitonic luminescence with strong circular polarization from the interaction with isolated Mn2+ ions. Using a combination of superconducting quantum interference device (SQUID) magnetometry, magneto-absorption and transient optical spectroscopy, we find that a dark exciton population is brightened by state mixing with the bright excitons in the presence of a magnetic field. Unexpectedly, the circular polarization of the dark exciton luminescence follows the Brillouin-shaped magnetization with a saturation polarization of 13% at 4 K and 6 T. From high-field transient magneto-luminescence we attribute our observations to spin-dependent exciton dynamics at early times after excitation, with first indications for a Mn-mediated spin-flip process. Our findings demonstrate manganese doping as a powerful approach to control excitonic spin physics in Ruddlesden-Popper perovskites, which will stimulate research on this highly tuneable material platform with promise for tailored interactions between magnetic moments and excitonic states.

3D Deep Learning Enables Accurate Layer Mapping of 2D Materials.

Layered, two-dimensional (2D) materials are promising for next-generation photonics devices. Typically, the thickness of mechanically cleaved flakes and chemical vapor deposited thin films is distributed randomly over a large area, where accurate identification of atomic layer numbers is time-consuming. Hyperspectral imaging microscopy yields spectral information that can be used to distinguish the spectral differences of varying thickness specimens. However, its spatial resolution is relatively low due to the spectral imaging nature. In this work, we present a 3D deep learning solution called DALM (deep-learning-enabled atomic layer mapping) to merge hyperspectral reflection images (high spectral resolution) and RGB images (high spatial resolution) for the identification and segmentation of MoS2 flakes with mono-, bi-, tri-, and multilayer thicknesses. DALM is trained on a small set of labeled images, automatically predicts layer distributions and segments individual layers with high accuracy, and shows robustness to illumination and contrast variations. Further, we show its advantageous performance over the state-of-the-art model that is solely based on RGB microscope images. This AI-supported technique with high speed, spatial resolution, and accuracy allows for reliable computer-aided identification of atomically thin materials.

Charged Exciton Kinetics in Monolayer MoSe2 near Ferroelectric Domain Walls in Periodically Poled LiNbO3.

Monolayer semiconducting transition metal dichalcogenides are a strongly emergent platform for exploring quantum phenomena in condensed matter, building novel optoelectronic devices with enhanced functionalities. Because of their atomic thickness, their excitonic optical response is highly sensitive to their dielectric environment. In this work, we explore the optical properties of monolayer thick MoSe2 straddling domain wall boundaries in periodically poled LiNbO3. Spatially resolved photoluminescence experiments reveal spatial sorting of charge and photogenerated neutral and charged excitons across the boundary. Our results reveal evidence for extremely large in-plane electric fields of ≃4000 kV/cm at the domain wall whose effect is manifested in exciton dissociation and routing of free charges and trions toward oppositely poled domains and a nonintuitive spatial intensity dependence. By modeling our result using drift-diffusion and continuity equations, we obtain excellent qualitative agreement with our observations and have explained the observed spatial luminescence modulation using realistic material parameters.

Gate-Switchable Arrays of Quantum Light Emitters in Contacted Monolayer MoS2 van der Waals Heterodevices.

We demonstrate electrostatic switching of individual, site-selectively generated matrices of single photon emitters (SPEs) in MoS2 van der Waals heterodevices. We contact monolayers of MoS2 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 MoS2 by focused helium ion irradiation. The SPEs are sensitive to the charge carrier concentration in the MoS2 and switch on and off similar to the neutral exciton in MoS2 for moderate electron doping. The demonstrated scheme is a first step for producing scalable, gate-addressable, and gate-switchable arrays of quantum light emitters in MoS2 heterostacks.

Growth dynamics and compositional structure in periodic InAsSb nanowire arrays on Si (111) grown by selective area molecular beam epitaxy.

We report a comprehensive study of the growth dynamics in highly periodic, composition tunable InAsSb nanowire (NW) arrays using catalyst-free selective area molecular beam epitaxy. Employing periodically patterned SiO2-masks on Si (111) with various mask opening sizes (20-150 nm) and pitches (0.25-2 µm), high NW yield of >90% (irrespective of the InAsSb alloy composition) is realized by the creation of an As-terminated 1 × 1-Si(111) surface prior to NW nucleation. While the NW aspect ratio decreases continually with increasing Sb content (x Sb from 0% to 30%), we find a remarkable dependence of the aspect ratio on the mask opening size yielding up to ∼8-fold increase for openings decreasing from 150 to 20 nm. The effects of the interwire separation (pitch) on the NW aspect ratio are strongest for pure InAs NWs and gradually vanish for increasing Sb content, suggesting that growth of InAsSb NW arrays is governed by an In surface diffusion limited regime even for the smallest investigated pitches. Compositional analysis using high-resolution x-ray diffraction reveals a substantial impact of the pitch on the alloy composition in homogeneous InAsSb NW arrays, leading to much larger x Sb as the pitch increases due to decreasing competition for Sb adatoms. Scanning transmission electron microscopy and associated energy-dispersive x-ray spectroscopy performed on the cross-sections of individual NWs reveal an interesting growth-axis dependent core-shell like structure with a discontinuous few-nm thick Sb-deficient coaxial boundary layer and six Sb-deficient corner bands. Further analysis evidences the presence of a nanoscale facet at the truncation of the (111)B growth front and {1-10} sidewall surfaces that is found responsible for the formation of the characteristic core-shell structure.