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Superconducting nanowire single-photon detectors (SNSPDs) are indispensable in fields such as quantum science and technology, astronomy, and biomedical imaging, where high detection efficiency, low dark count rates and high timing accuracy are required. Recently, helium (He) ion irradiation was shown to be a promising method to enhance SNSPD performance. Here, we study how changes in the underlying superconducting NbTiN film and the SiO2/Si substrate affect device performance. While irradiated and unirradiated NbTiN films show similar crystallinity, we observe He bubble formation below the SiO2/Si interface and an amorphization of the Si substrate. Both reduce the thermal conductance between the superconducting thin film and the substrate from 210 W/m^2/K^4 to 70 W/m^2/K^4 after irradiation with 2000 ions/nm^2. This effect, combined with the lateral straggle of He ions in the substrate, allows the modification of the superconductor-to-substrate thermal conductance of an SNSPD by selectively irradiating the regions around the nanowire. With this approach, we achieved an increased plateau width of saturating intrinsic detection efficiency of 9.8 uA compared to 3.7 uA after full irradiation. Moreover, the critical current remained similar to that of the unirradiated reference device (59 uA versus 60.1 uA), while full irradiation reduced it to 22.4 uA. Our results suggest that the irradiation-induced reduction of the thermal conductance significantly enhances SNSPD sensitivity, offering a novel approach to locally engineer substrate properties for improved detector performance., Comment: 18 pages, 11 figures

We investigate the coupling between an ensemble of individual emitters and multiple photons in a high-$Q$ cavity at the mesoscopic excitation level. The master equation theory is used to calculate the emission spectrum of the cavity QED system. The increasing excitation level not only pumps the system to the high-energy multi-emitter-photon states, but also introduces the pump-induced dephasing that suppresses the coherent energy exchange (coupling) between photons and emitters. When the emitter lifetime exceeds a threshold, we observe the mesoscopic excitation level i.e., the system is pumped to high energy states whilst the coherent couplings between these states are not yet suppressed. The mesoscopic excitation enables the couplings between multi-emitter-photon states, and thereby, paves the way to building quantum photonic devices based on multiple photons and nonlinear effects.

Single-photon emission from a two-level system offers promising perspectives for the development of quantum technologies, where multiphotons are generally regarded as accidental, undesired and should be suppressed. In quantum mechanics, however, multiphoton emission can turn out to be even more fundamental and interesting than the single-photon emission, since in a coherently driven system, the multiphoton suppression arises from quantum interferences between virtual multiphoton fluctuations and the mean field in a Poisson superposition of all number states. Here, we demonstrate how one can control the multiphoton dynamics of a two-level system by disrupting these quantum interferences through a precise and independent homodyne control of the mean field. We show that, counterintuitively, quantum fluctuations always play a major qualitative role, even and in fact especially, when their quantitative contribution is vanishing as compared to that of the mean field. Our findings provide new insights into the paradoxical character of quantum mechanics and open pathways for mean-field engineering as a tool for precision multiphoton control.

One-dimensional structures such as nanowires (NWs) show great promise in tailoring the rates of hot carrier thermalization in semiconductors with important implications for the design of efficient hot carrier absorbers. However, fabrication of high-quality, phase-pure crystal structures and control of their intrinsic electronic properties can be challenging, raising concerns about the role of competing radiative and non-radiative recombination mechanisms that govern hot carrier effects. Here, we elucidate the impact of crystal purity and altered electronic properties on the hot carrier properties by comparing two classes of III-V semiconductor NW arrays with similar band-gap energies and geometries, yet different crystal quality: one composed of GaAsSb NWs, free of planar stacking defects, and the other InGaAs NWs with a high density of stacking defects. Photoluminescence spectroscopy demonstrates distinct hot carrier effects in both NW arrays; however, the InGaAs NWs with lower crystal quality exhibit stronger hot carrier effects, as evidenced by increased carrier temperature under identical photoabsorptivity. This difference arises from higher rates of Auger recombination in the InGaAs NWs due to their increased n-type conductivity, as confirmed by excitation power-dependent measurements. Our findings suggest that while enhancing material properties is crucial for improving the performance of hot carrier absorbers, optimizing conditions to increase the rates of Auger recombination will further boost the efficiency of these devices., Comment: 13 pages, 4 figures

Quantum gases consisting of species with distinct quantum statistics, such as Bose-Fermi mixtures, can behave in a fundamentally different way than their unmixed constituents. This makes them an essential platform for studying emergent quantum many-body phenomena such as mediated interactions and unconventional pairing. Here, we realize an equilibrium Bose-Fermi mixture in a bilayer electron system implemented in a WS$_{2}$/WSe$_{2}$ moir\'e heterobilayer with strong Coulomb coupling to a nearby moir\'e-free WSe$_{2}$ monolayer. Absent the fermionic component, the underlying bosonic phase manifests as a dipolar excitonic insulator. By injecting excess charges into it, we show that the bosonic phase forms a stable mixture with added electrons but abruptly collapses upon hole doping. We develop a microscopic model to explain the unusual asymmetric stability with respect to electron and hole doping. By studying the Bose-Fermi mixture via monitoring excitonic resonances from both layers, we demonstrate gate-tunability over a wide range in the boson/fermion density phase space, in excellent agreement with theoretical calculations. Our results further the understanding of phases stabilized in moir\'e bilayer electron systems and demonstrate their potential for exploring the exotic properties of equilibrium Bose-Fermi mixtures., Comment: 13 pages, 4 figures. Extended Data: 6 figures. We welcome your feedback!

Combining a precise sputter etching method with subsequent AlO$_x$ growth within an atomic layer deposition chamber enables fabrication of atomically flat lateral patterns of SiO$_2$ and AlO$_x$. The transfer of MoSe$_2$ monolayers onto these dielectrically modulated substrates results in formation of lateral heterojunctions, with the flat substrate topography leading to minimal strain across the junction. Kelvin probe force microscopy (KPFM) measurements show significant variations in the contact potential difference (CPD) across the interface, with AlO$_x$ regions inducing a 230~mV increase in CPD. Spatially resolved photoluminescence spectroscopy reveals shifts in spectral weight of neutral and charged exciton species across the different dielectric regions. On the AlO$_x$ side, the Fermi energy moves closer to the conduction band, leading to a higher trion-to-exciton ratio, indicating a bandgap shift consistent with CPD changes. In addition, transient reflection spectroscopy highlights the influence of the dielectric environment on carrier dynamics, with the SiO$_2$ side exhibiting rapid carrier decay typical of neutral exciton recombination. In contrast, the AlO$_x$ side shows slower, mixed decay behavior consistent with conversion of trions back into excitons. These results demonstrate how dielectric substrate engineering can tune the electronic and optical characteristics of proximal two-dimensional materials, allowing scalable fabrication of advanced junctions for novel (opto)electronics applications., Comment: 24 pages, 5 figures. SI: 2 pages, 3 figures. We welcome your feedback!

We explore the optical dipole orientation of single photon emitters in monolayer MoS2 as produced by a focused helium ion beam. The single photon emitters can be understood as single sulfur vacancies. The corresponding far-field luminescence spectra reveal several photoluminescence lines below the dominating luminescence of the exciton in MoS2. These sub-bandgap emission lines were predicted by ab initio theory, but they have never been resolved in luminescence experiments because of their small amplitude. We reveal the lines by their dependence as a function of the photon energy and momentum as measured in the back focal plane of the optical circuitry. The agreement between theory and experiment suggests that the defect states interact strongly within the Brillouin zone.

We present time-resolved and CW optical spectroscopy studies of interlayer excitons (IXs) in 2$H-$ and 3$R-$stacked MoSe$_2$/WSe$_2$ heterobilayers and obtain evidence for the strong participation of hot phonons in the underlying photo-physics. Photoluminescence excitation spectroscopy reveals that excess energy associated with optical excitation of \textit{intra}-layer excitons and relaxation to IXs affects the overall IX-PL lineshape, while the spectrally narrow emission lines conventionally associated with moir\'e IXs are unaffected. A striking uniform line-spacing of the sharp emission lines is observed together with temperature and excitation level dependent spectra suggesting an entirely new picture that photo-generated phonons lead to phonon-replicas shaping the IX-emission. Excitation power and time resolved data indicate that these features are polaronic in nature. Our experimental findings modify our current understanding of the photophysics of IXs beyond current interpretations based on moir\'e-trapped IXs.

Detecting single photons is essential for applications such as dark matter detection, quantum science and technology, and biomedical imaging. Superconducting nanowire single-photon detectors (SNSPDs) excel in this task due to their near-unity detection efficiency, sub-Hz dark count rates, and picosecond timing jitter. However, a local increase of current density (current crowding) in the bends of meander-shaped SNSPDs limits these performance metrics. By locally irradiating the straight segments of SNSPDs with helium ions while leaving the bends unirradiated, we realize current-crowding-free SNSPDs with simultaneously enhanced sensitivity: after irradiation with 800 ions/nm$\unicode{xB2}$, locally irradiated SNSPDs showed a relative saturation plateau width of 37% while fully irradiated SNSPDs reached only 10%. This larger relative plateau width allows operation at lower relative bias currents, thereby reducing the dark count rate while still detecting single photons efficiently. We achieve an internal detection efficiency of 94% for a wavelength of 780 nm with a dark count rate of 7 mHz near the onset of saturating detection efficiency., Comment: 11 pages, 7 figures

InAs semiconductor quantum dots (QDs) emitting in the near infrared are promising platforms for on-demand single-photon sources and spin-photon interfaces. However, the realization of quantum-photonic nanodevices emitting in the second and third telecom windows with similar performance remains an open challenge. Here, we report an optimized heterostructure design for QDs emitting in the O- and C-bands grown by means of molecular beam epitaxy. The InAs QDs are grown on compositionally graded InGaAs buffers, which act as virtual substrates, and are embedded in mostly relaxed active regions. Reciprocal space maps of the indium profiles and optical absorption spectra are used to optimize In0.22Ga0.78As and In0.30Ga0.70As active regions, accounting for the chosen indium grading profile. This approach results in a tunable QD photoluminescence (PL) emission from 1200 up to 1600 nm. Power and polarization dependent micro-PL measurements performed at 4 K reveal exciton-biexciton complexes from quantum dots emitting in the telecom O- and C-bands. The presented study establishes a flexible platform that can be an essential component for advanced photonic devices based on InAs/GaAs that serve as building blocks for future quantum networks.

Understanding the origin of hot carrier relaxation in nanowires (NWs) with one-dimensional (1D) geometry is significant for designing efficient hot carrier solar cells with such nanostructures. Here, we study the influence of Auger heating and Shockley-Read-Hall recombination on hot carrier dynamics of catalyst-free InGaAs-InAlAs core-shell NWs. Using steady-state and time-resolved photoluminescence (PL) spectroscopy the dependencies of hot carrier effects on the degree of confinement of photo-generated carriers induced by the nanowire diameter are determined at different lattice temperatures. Analysis of excitation-power dependent data and temperature-dependent PL linewidth broadening reveal that at low temperatures, strong Auger recombination and phonon-bottleneck are responsible for hot carrier effects. Our analysis gives also insights into electron-phonon and ionized impurity scattering, showing opposing trends with NW diameter, and it allows to estimate the Fr\"ohlich coupling constant for the InGaAs NWs. Conversely, with increasing lattice temperature, hot carrier relaxation rates increase due to enhanced Shockley-Read Hall and surface recombination. Time-resolved spectroscopy reveals a fourfold increase in the rate of Shockley-Read-Hall recombination from 6 ns at 10 K to 1.5 ns at 150 K. The findings suggest that minimizing defect densities in the bulk and surfaces of these NWs will be key to enhance hot carrier effects towards higher temperatures., Comment: 15 pages, 5 figures

Coulomb interactions in atomically thin materials are uniquely sensitive to variations in the dielectric screening of the environment, which can be used to control quasiparticles and exotic quantum many-body phases. A static approximation of the dielectric response, where increased dielectric screening is predicted to cause an energy redshift of the exciton resonance, has been until now sufficient. Here, we use charge-tunable exciton resonances to study screening effects in transition metal dichalcogenide monolayers embedded in materials with dielectric constants ranging from 4 to more than 1000. In contrast to expectations, we observe a blueshift of the exciton resonance exceeding 30 meV for larger dielectric constant environments. By employing a dynamical screening model, we find that while the exciton binding energy remains mostly controlled by the static dielectric response, the exciton self-energy is dominated by the high-frequency response. Dielectrics with markedly different static and high-frequency screening enable the selective addressing of distinct many-body effects in layered materials and their heterostructures, expanding the tunability range and offering new routes to detect and control correlated quantum many-body states and to design optoelectronic and quantum devices., Comment: 10 pages, 4 figures. SI: 11 pages, 6 figures. We welcome your feedback!

Group IV vacancy color centers in diamond are promising spin-photon interfaces with strong potential for applications for photonic quantum technologies. Reliable methods for controlling and stabilizing their charge state are urgently needed for scaling to multi-qubit devices. Here, we manipulate the charge state of silicon vacancy (SiV) ensembles by combining luminescence and photo-current spectroscopy. We controllably convert the charge state between the optically active SiV$^-$ and dark SiV$^{2-}$ with MHz rates and 90% contrast by judiciously choosing the local potential applied to in-plane surface electrodes and the laser excitation wavelength. We observe intense SiV$^-$ photoluminescence under hole-capture, measure the intrinsic conversion time from the dark SiV$^{2-}$ to the bright SiV$^-$ to be 36.4(6.7)ms and demonstrate how it can be enhanced by a factor of $10^5$ via optical pumping. Moreover, we obtain new information on the defects that contribute to photo-conductivity, indicating the presence of substitutional nitrogen and divacancies., Comment: 5 figures

Radial Bragg gratings are commonly used to enhance light extraction from quantum emitters, but lack a well-suited, fast simulation method for optimization beyond periodic designs. To overcome this limitation, we propose and demonstrate an algorithm based on the transfer matrix model (TMM) to calculate the free-space emission of such gratings. Using finite difference time domain (FDTD) simulations, we characterize the free-space emission and transfer matrices of single grating components. Our TMM then combines any number of components to receive the total emission. Randomized benchmarks verify that results from our method agree within 98 % with FDTD while reducing simulation time by one to two orders of magnitude. The speed advantage of our approach is shown by maximizing emission of a fifteen-trench circular grating into a Gaussian mode. We expect that our novel algorithm will facilitate the optimization of radial gratings, enabling quantum light sources with unprecedented collection efficiencies., Comment: 9 pages, 5 figures, 2 pages supplemental, submitted to Optica

We report temperature-dependent spectroscopy on the layered (n=4) two-dimensional (2D) Ruddlesden-Popper perovskite (BA)(MA)PbI. Helicity-resolved steady-state photoluminescence (PL) reveals no optical degree of polarization. Time-resolved PL shows a photocarrier lifetime on the order of nanoseconds. From simultaneaously recorded time-resolved differential reflectivity (TR$\Delta$R) and time-resolved Kerr ellipticity (TRKE), a photocarrier lifetime of a few nanoseconds and a spin dephasing time on the order of picoseconds was found. This stark contrast in lifetimes clearly explains the lack of spin polarization in steady-state PL. While we observe clear temperature-dependent effects on the PL dynamics that can be related to structural dynamics, the spin dephasing is nearly T-independent. Our results highlight that spin dephasing in 2D (BA)(MA)PbI occurs at time scales faster than the exciton recombination time, which poses a bottleneck for applications aimingto utilize this degree of freedom.

We report a new dark exciton in monolayer MoS$_2$ using second harmonic generation spectroscopy. Hereby, the spectrally dependent second harmonic generation intensity splits into two branches, and an anticrossing is observed at $\sim$ 25 meV blue detuned from the bright neutral exciton. These observations are indicative of coherent quantum interference arising from strong two-photon light-matter interaction with an excitonic state that is dark for single photon interaction. The existence of the dark state is supported by engineering its relaxation to bright localized excitons, mediated by vibrational modes of a proximal nanobeam cavity. We show that two-photon light-matter interaction involving dark states has the potential to control relaxation pathways induced by nanostructuring the local environment. Moreover, our results indicate that dark excitons have significant potential for nonlinear quantum devices based on their nontrivial excitonic photophysics.

Electrically controllable quantum-dot molecules (QDMs) are a promising platform for deterministic entanglement generation and, as such, a resource for quantum-repeater networks. We develop a microscopic open-quantum-systems approach based on a time-dependent Bloch-Redfield equation to model the generation of entangled spin states with high fidelity. The state preparation is a crucial step in a protocol for deterministic entangled-photon-pair generation that we propose for quantum repeater applications. Our theory takes into account the quantum-dot molecules' electronic properties that are controlled by time-dependent electric fields as well as dissipation due to electron-phonon interaction. We quantify the transition between adiabatic and non-adiabatic regimes, which provides insights into the dynamics of adiabatic control of QDM charge states in the presence of dissipative processes. From this, we infer the maximum speed of entangled-state preparation under different experimental conditions, which serves as a first step towards simulation of attainable entangled photon-pair generation rates. The developed formalism opens the possibility for device-realistic descriptions of repeater protocol implementations., Comment: 12 pages, 11 figures

Two-dimensional (2D) heterostructures integrated into nanophotonic cavities have emerged as a promising approach towards novel photonic and opto-electronic devices. However, the thickness of the 2D heterostructure has a strong influence on the resonance frequency of the nanocavity. For a single cavity, the resonance frequency shifts approximately linearly with the thickness. Here, we propose to use the inherent non-linearity of the mode coupling to render the cavity mode insensitive to the thickness of the 2D heterostructure. Based on the coupled mode theory, we reveal that this goal can be achieved using either a homoatomic molecule with a filtered coupling or heteroatomic molecules. We perform numerical simulations to further demonstrate the robustness of the eigenfrequency in the proposed photonic molecules. Our results render nanophotonic structures insensitive to the thickness of 2D materials, thus owing appealing potential in energy- or detuning-sensitive applications such as cavity quantum electrodynamics.

The interaction of a resonant light field with a quantum two-level system is of key interest both for fundamental quantum optics and quantum technological applications employing resonant excitation. While emission under resonant continuous-wave excitation has been well-studied, the more complex emission spectrum of dynamically dressed states, a quantum two-level system driven by resonant pulsed excitation, has so far been investigated in detail only theoretically. Here, we present the first experimental observation of the complete resonance fluorescence emission spectrum of a single quantum two-level system, in form of an excitonic transition in a semiconductor quantum dot, driven by finite Gaussian pulses. We observe multiple emerging sidebands as predicted by theory with an increase of their number and spectral detuning with excitation pulse intensity and a dependence of their spectral shape and intensity on the pulse length. Detuning-dependent measurements provide additional insights into the emission features. The experimental results are in excellent agreement with theoretical calculations of the emission spectra, corroborating our findings.

Achieving homogeneous performance metrics between nominally identical pixels is challenging for the operation of arrays of superconducting nanowire single-photon detectors (SNSPDs). Here, we utilize local helium ion irradiation to post-process and tune single-photon detection efficiency, switching current, and critical temperature of individual devices on the same chip. For 12nm thick highly absorptive SNSPDs, which are barely single-photon sensitive prior to irradiation, we observe an increase of the system detection efficiency from $< 0.05\,\%$ to $(55.3 \pm 1.1)\,\%$ following irradiation. Moreover, the internal detection efficiency saturates at a temperature of 4.5 K after irradiation with $1800\, \mathrm{ions}\, \mathrm{nm}^{-2}$. For irradiated 10 nm thick detectors we observe a doubling of the switching current (to $20\, \mu\mathrm{A}$) compared to 8 nm SNSPDs of similar detection efficiency, increasing the amplitude of detection voltage pulses. Investigations of the scaling of superconducting thin film properties with irradiation up to a fluence of $2600\, \mathrm{ions}\, \mathrm{nm}^{-2}$ revealed an increase of sheet resistance and a decrease of critical temperature towards high fluences. A physical model accounting for defect generation and sputtering during helium ion irradiation is presented and shows good qualitative agreement with experiments., Comment: 12 pages, 11 Figures

Semiconductor quantum dot molecules are considered as 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 inter-dot 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 modelling on different levels of complexity we give an instructive explanation of the underlying coupling mechanism and dynamical processes.

The electron-hole exchange interaction is a fundamental mechanism that drives valley depolarization via intervalley exciton hopping in semiconductor multi-valley systems. Here, we report polarization-resolved photoluminescence spectroscopy of neutral excitons and negatively charged trions in monolayer MoSe$_2$ and WSe$_2$ under biaxial strain. We observe a marked enhancement(reduction) on the WSe$_2$ triplet trion valley polarization with compressive(tensile) strain while the trion in MoSe$_2$ is unaffected. The origin of this effect is shown to be a strain dependent tuning of the electron-hole exchange interaction. A combined analysis of the strain dependent polarization degree using ab initio calculations and rate equations shows that strain affects intervalley scattering beyond what is expected from strain dependent bandgap modulations. The results evidence how strain can be used to tune valley physics in energetically degenerate multi-valley systems.

Self-assembled optically active quantum dot molecules (QDMs) allow the creation of protected qubits via singlet-triplet spin states. The qubit energy splitting of these states is defined by the tunnel coupling strength and is, therefore, determined by the potential landscape and thus fixed during growth. Applying an in-plane magnetic field increases the confinement of the hybridized wave functions within the quantum dots, leading to a decrease of the tunnel coupling strength. We achieve a tuning of the coupling strength by $(53.4\pm1.7)$ %. The ability to fine-tune this coupling is essential for quantum network and computing applications that require quantum systems with near identical performance., Comment: Main: 6 pages, 3 figures, Supplemental: 4 pages, 2 figures

Janus transition metal dichalcogenides are an emerging class of atomically thin materials with engineered broken mirror symmetry that gives rise to long-lived dipolar excitons, Rashba splitting, and topologically protected solitons. They hold great promise as a versatile nonlinear optical platform due to their broadband harmonic generation tunability, ease of integration on photonic structures, and nonlinearities beyond the basal crystal plane. Here, we study second and third harmonic generation in MoSSe and WSSe Janus monolayers. We use polarization-resolved spectroscopy to map the full second-order susceptibility tensor of MoSSe, including its out-of-plane components. In addition, we measure the effective third-order susceptibility, and the second-order nonlinear dispersion close to exciton resonances for both MoSSe and WSSe at room and cryogenic temperatures. Our work sets a bedrock for understanding the nonlinear optical properties of Janus transition metal dichalcogenides and probing their use in the next-generation on-chip multifaceted photonic devices., Comment: 10 pages, 3 figures. SI: 8 pages, 5 figures

We report lasing of moir\'e trapped interlayer excitons (IXs) by integrating a pristine hBN-encapsulated MoSe$_2$/WSe$_2$ heterobilayer into a high-$Q$ ($>10^4$) nanophotonic cavity. We control the cavity-IX detuning using a magnetic field and measure their dipolar coupling strength to be $78 \pm 4\ \mathrm{\mu eV}$, fully consistent with the 82 $\mathrm{\mu eV}$ predicted by theory. The emission from the cavity mode shows clear threshold-like behavior as the transition is tuned into resonance with the cavity. We observe a superlinear power dependence accompanied by a narrowing of the linewidth as the distinct features of lasing. The onset and prominence of these threshold-like behaviors are pronounced at resonance while weak off-resonance. Our results show that a lasing transition can be induced in interacting moir\'e IXs with macroscopic coherence extending over the length scale of the cavity mode. Such systems raise interesting perspectives for low-power switching and synaptic nanophotonic devices using two-dimensional materials.

We report on scalable heterointegration of superconducting electrodes and epitaxial semiconductor quantum dots on strong piezoelectric and optically nonlinear lithium niobate. The implemented processes combine the sputter-deposited thin film superconductor niobium nitride and III-V compound semiconductor membranes onto the host substrate. The superconducting thin film is employed as a zero-resistivity electrode material for a surface acoustic wave resonator with internal quality factors $Q \approx 17000$ representing a three-fold enhancement compared to identical devices with normal conducting electrodes. Superconducting operation of $\approx 400\,\mathrm{MHz}$ resonators is achieved to temperatures $T>7\,\mathrm{K}$ and electrical radio frequency powers $P_{\mathrm{rf}}>+9\,\mathrm{dBm}$. Heterogeneously integrated single quantum dots couple to the resonant phononic field of the surface acoustic wave resonator operated in the superconducting regime. Position and frequency selective coupling mediated by deformation potential coupling is validated using time-integrated and time-resolved optical spectroscopy. Furthermore, acoustoelectric charge state control is achieved in a modified device geometry harnessing large piezoelectric fields inside the resonator. The hybrid quantum dot - surface acoustic wave resonator can be scaled to higher operation frequencies and smaller mode volumes for quantum phase modulation and transduction between photons and phonons via the quantum dot. Finally, the employed materials allow for the realization of other types of optoelectronic devices, including superconducting single photon detectors and integrated photonic and phononic circuits., Comment: submitted manuscript

Quantum dot molecules (QDMs) are one of the few quantum light sources that promise deterministic generation of one- and two-dimensional photonic graph states. The proposed protocols rely on coherent excitation of the tunnel-coupled and spatially indirect exciton states. Here, we demonstrate power-dependent Rabi oscillations of direct excitons, spatially indirect excitons, and excitons with a hybridized electron wave function. An off-resonant detection technique based on phonon-mediated state transfer allows for spectrally filtered detection under resonant excitation. Applying a gate voltage to the QDM-device enables a continuous transition between direct and indirect excitons and, thereby, control of the overlap of the electron and hole wave function. This does not only vary the Rabi frequency of the investigated transition by a factor of $\approx3$, but also allows to optimize graph state generation in terms of optical pulse power and reduction of radiative lifetimes., Comment: 6 pages, 3 figures

The valley Zeeman physics of excitons in monolayer transition metal dichalcogenides provides valuable insight into the spin and orbital degrees of freedom inherent to these materials. Being atomically-thin materials, these degrees of freedom can be influenced by the presence of adjacent layers, due to proximity interactions that arise from wave function overlap across the 2D interface. Here, we report 60 T magnetoreflection spectroscopy of the A- and B- excitons in monolayer WS$_2$, systematically encapsulated in monolayer graphene. While the observed variations of the valley Zeeman effect for the A- exciton are qualitatively in accord with expectations from the bandgap reduction and modification of the exciton binding energy due to the graphene-induced dielectric screening, the valley Zeeman effect for the B- exciton behaves markedly different. We investigate prototypical WS$_2$/graphene stacks employing first-principles calculations and find that the lower conduction band of WS$_2$ at the $K/K'$ valleys (the $CB^-$ band) is strongly influenced by the graphene layer on the orbital level. This leads to variations in the valley Zeeman physics of the B- exciton, consistent with the experimental observations. Our detailed microscopic analysis reveals that the conduction band at the $Q$ point of WS$_2$ mediates the coupling between $CB^-$ and graphene due to resonant energy conditions and strong coupling to the Dirac cone. Our results therefore expand the consequences of proximity effects in multilayer semiconductor stacks, showing that wave function hybridization can be a multi-step process with different bands mediating the interlayer interactions. Such effects can be exploited to resonantly engineer the spin-valley degrees of freedom in van der Waals and moir\'e heterostructures., Comment: 14 pages, 6 figures, 3 tables

Spin defects in hexagonal Boron Nitride (hBN) attract increasing interest for quantum technology since they represent optically-addressable qubits in a van der Waals material. In particular, negatively-charged boron vacancy centers (${V_B}^-$) in hBN have shown promise as sensors of temperature, pressure, and static magnetic fields. However, the short spin coherence time of this defect currently limits its scope for quantum technology. Here, we apply dynamical decoupling techniques to suppress magnetic noise and extend the spin coherence time by nearly two orders of magnitude, approaching the fundamental $T_1$ relaxation limit. Based on this improvement, we demonstrate advanced spin control and a set of quantum sensing protocols to detect electromagnetic signals in the MHz range with sub-Hz resolution. This work lays the foundation for nanoscale sensing using spin defects in an exfoliable material and opens a promising path to quantum sensors and quantum networks integrated into ultra-thin structures.

We utilize cavity-enhanced extinction spectroscopy to directly quantify the optical absorption of defects in MoS$_2$ 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 $10^{11}$ cm$^{-2}$. The corresponding spectra reveal a broad sub-gap absorption, being consistent with theoretical predictions related to sulfur vacancy-bound excitons in MoS$_2$. 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., Comment: 17 pages main manuscript, 7 pages supporting information

Developing coherent excitation methods for quantum emitters which enable high brightness, good single-photon purity and high indistinguishability of the emitted photons has been a key challenge in the past years. While many methods have been proposed and explored, they all have specific advantages and disadvantages. In this letter, we investigate the dynamics of the recent swing-up scheme as an excitation method for a two-level system and its performance in single-photon generation. By applying two far red-detuned laser pulses, the two-level system can be prepared in the excited state with near-unity fidelity. We demonstrate the successful functionality and the coherent character of this technique using semiconductor quantum dots. Moreover, we explore the multi-dimensional parameter space of the two laser pulses to study the impact on the excitation fidelity. Finally, we investigate the performance of the scheme as an excitation method for generation of high-quality single photons. We find that the swing-up scheme itself works well and exhibits nearly perfect single-photon purity, while the observed indistinguishability in our sample is limited by the influence of the inevitable high excitation powers on the semiconductor environment of the quantum dot., Comment: 11 pages, 11 figures

Optoelectronic properties of van der Waals homostructures can be selectively engineered by the relative twist angle between layers. Here, we study the twist-dependent moire coupling in MoSe2 homobilayers. For small angles, we find a pronounced redshift of the K-K and {\Gamma}-K excitons accompanied by a transition from K-K to {\Gamma}-K emission. Both effects can be traced back to the underlying moire pattern in the MoSe2 homobilayers, as confirmed by our low-energy continuum model for different moire excitons. We identify two distinct intralayer moire 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 moire exciton species.

Integrating quantum emitters into nanocavities which simultaneously couple to the photonic and mechanical modes is critical for interfacing electron spins, photons and phonons in the cavity QED system. Here, we investigate the interaction between the charged boron vacancy $V_B^-$, ultra-high-Q ($\sim10^5$) cavity photonic modes and local phonon modes. A pronounced asymmetry is observed in the emission spectrum for cavities with Q-factor above a threshold of 10$^4$. Similar asymmetries are not observed for cavities without $V_B^-$ centers. To explain our findings, we model the system with phonon-induced light-matter coupling based on $V_B^-$ centers, and compare to the Jaynes-Cummings model for usual emitters. Our results reveal that the multipartite interplay arises during the light-matter coupling of $V_B^-$ centers, illustrating that it is phonon-induced, rather than being caused by thermal population of phonon modes. Such emitter-optomechanical interaction between different photon ($V_B^-$ emission, cavity photonic) and phonon ($V_B^-$ phonon, cavity mechanical) modes provides a novel system to interface spin defects, photons and phonons in condensed matters.

Photonic bound states in the continuum (BICs) are a standout nanophotonic platform for strong light-matter coupling with transition metal dichalcogenides (TMDCs), but have so far mostly been employed as all-dielectric metasurfaces with adjacent TMDC layers, incurring limitations related to strain, mode overlap, and material integration. In this work, we experimentally demonstrate for the first time asymmetry-dependent BIC resonances in 2D arrays of monolithic metasurfaces composed solely of the nanostructured bulk TMDC WS$_2$ with BIC modes exhibiting sharp and tailored linewidths, ideal for selectively enhancing light-matter interactions. Geometrical variation enables the tuning of the BIC resonances across the exciton resonance in bulk WS$_2$, revealing the strong-coupling regime with an anti-crossing pattern and a Rabi splitting of 116 meV. The precise control over the radiative loss channel provided by the BIC concept is harnessed to tailor the Rabi splitting via a geometrical asymmetry parameter of the metasurface. Crucially, the coupling strength itself can be controlled and is shown to be independent of material-intrinsic losses. Our BIC-driven monolithic metasurface platform can readily incorporate other TMDCs or excitonic materials to deliver previously unavailable fundamental insights and practical device concepts for polaritonic applications., Comment: Main text and supporting information, 31 pages, 4 Figures manuscript + 8 Supporting Figures

Magnetic resonance imaging of spin systems combines scientific applications in medicine, chemistry and physics. Here, we investigate the pixel-wise coherent quantum dynamics of spins consisting of a 40 by 40 micron sized region of interest implanted with nitrogen vacancy centers (NV) coupled to a nano-magnetic flake of $\mathrm{CrTe_2}$. $\mathrm{CrTe_2}$ is an in-plane van der Waals ferromagnet, which we can probe quantitatively by the NV electron's spin signal even at room temperature. First, we combine the nano-scale sample shapes measured by atomic force microscope with the magnetic resonance imaging data. We then map out the coherent dynamics of the colour centers coupled to the van der Waals ferromagnet using pixel-wise coherent Rabi and Ramsey imaging of the NV sensor layer. Next, we fit the pixel-wise solution of the Hamiltonian to the quantum sensor data. Combining data and model, we can explore the detuning range of the spin oscillation with a quantum dynamic range of over $\left|\Delta_{max}\right|= 60 { }\mathrm{MHz} $ in the Ramsey interferometry mode. Finally, we show the effect of the $\mathrm{CrTe_2}$ van der Waals magnet on the coherence of the NV sensor layer and measure a 70 times increase in the maximum frequency of the quantum oscillation going from the Rabi to the Ramsey imaging mode.

Triangular cross-section SiC photonic devices have been studied as an efficient and scalable route for integration of color centers into quantum hardware. In this work, we explore efficient collection and detection of color center emission in a triangular cross-section SiC waveguide by introducing a photonic crystal mirror on its one side and a superconducting nanowire single photon detector (SNSPD) on the other. Our modeled triangular cross-section devices with a randomly positioned emitter have a maximum coupling efficiency of 89 % into the desired optical mode and a high coupling efficiency (> 75 %) in more than half of the configurations. For the first time, NbTiN thin films were sputtered on 4H-SiC and the electrical and optical properties of the thin films were measured. We found that the transport properties are similar to the case of NbTiN on SiO2 substrates, while the extinction coefficient is up to 50 % higher for 1680 nm wavelength. Finally, we performed Finite-Difference Time-Domain simulations of triangular cross-section waveguide integrated with an SNSPD to identify optimal nanowire geometries for efficient detection of light from TE and TM polarized modes., Comment: 31 pages, 8 figures

Two-dimensional transition metal di-chalcogenide semiconductors provide unique possibilities to investigate strongly confined excitonic physics and a plasmonic platform integrable to such materials constitutes a hybrid system that can be of interest to enable manipulation of their cumulative optical properties. Here we report tuning of excitonic emission from monolayer WSe2, mechanically exfoliated on top of a periodic two dimensional plasmonic array of elliptical gold (Au) nanodiscs. By exploiting the polarization-dependent nature of plasmonic resonance of the nano plasmonic array (NPA), the photoluminescence (PL) emission from the overlaid monolayer WSe2 could be significantly manipulated. PL is preferentially enhanced at the NPA covered regions of the ake when excited closer to the plasmonic resonant frequencies and previously unpolarized WSe2 PL emission gained ~ 20 up to 40 % degree of linear polarization at room temperature. Obtaining significant spectral overlap between the PL spectrum of WSe2 and the polarization tunable plasmonic resonance of the NPA plays a crucial role in this observation. The results demonstrate active tunability of optical emission from WSe2 by using an otherwise passive plasmonic environment and open the possibility of achieving atomically thin linearly polarized emitters at room temperature. In addition to fundamentally interesting physics of such interactions this can be highly desirable for ultrathin orientation sensitive opto-electronic device related applications., Comment: 9 pages, 3 Figures

Single spin defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2 and Q*) of He-ion induced sulfur vacancies in monolayer $\text{MoS}_2$. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wavefunction extent of $\sim$ 3.5 nm. The distinct valley-Zeeman splitting in out-of-plane $B$-fields and the brightening of dark states through in-plane $B$-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab-initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.

Tunnel-coupled pairs of optically active quantum dots - quantum dot molecules (QDMs) - offer the possibility to combine excellent optical properties such as strong light-matter coupling with two-spin singlet-triplet ($S-T_0$) qubits having extended coherence times. The $S-T_0$ basis formed using two spins is inherently protected against electric and magnetic field noise. However, since a single gate voltage is typically used to stabilize the charge occupancy of the dots and control the inter-dot orbital couplings, operation of the $S-T_0$ qubits under optimal conditions remains challenging. Here, we present an electric field tunable QDM that can be optically charged with one (1h) or two holes (2h) on demand. We perform a four-phase optical and electric field control sequence that facilitates the sequential preparation of the 2h charge state and subsequently allows flexible control of the inter-dot coupling. Charges are loaded via optical pumping and electron tunnel ionization. We achieve one- and two-hole charging efficiencies of 93.5 $\pm$ 0.8 % and 80.5 $\pm$ 1.3 %, respectively. Combining efficient charge state preparation and precise setting of inter-dot coupling allows control of few-spin qubits, as would be required for on-demand generation of two-dimensional photonic cluster states or quantum transduction between microwaves and photons., Comment: 4 figures

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.

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.

Entanglement swapping and heralding are at the heart of many protocols for distributed quantum information. For photons, this typically involves Bell state measurements based on two-photon interference effects. In this context, hybrid systems that combine high rate, ultra-stable and pure quantum sources with long-lived quantum memories are particularly interesting. Here, we develop a theoretical description of pulsed two-photon interference of photons from dissimilar sources to predict the outcomes of second-order cross-correlation measurements. These are directly related to, and hence used to quantify, photon indistinguishability. We study their dependence on critical system parameters such as quantum state lifetime and frequency detuning, and quantify the impact of emission time jitter, pure dephasing and spectral wandering. Our results show that for fixed lifetime of emitter one, for each frequency detuning there is an optimal lifetime of emitter two that leads to highest photon indistinguishability. Expectations for different hybrid combinations involving III-V quantum dots, color centers in diamond, 2D materials and atoms are quantitatively compared for real-world system parameters. Our work both provides a theoretical basis for the treatment of dissimilar emitters and enables assessment of which imperfections can be tolerated in hybrid photonic quantum networks.

We demonstrate that semiconductor quantum dots can be excited efficiently in a resonant three-photon process, whilst resonant two-photon excitation is highly suppressed. Time-dependent Floquet theory is used to quantify the strength of the multi-photon processes and model the experimental results. The efficiency of these transitions can be drawn directly from parity considerations in the electron and hole wavefunctions in semiconductor quantum dots. Finally, we exploit this technique to probe intrinsic properties of InGaN quantum dots. In contrast to non-resonant 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 non-resonant excitation., Comment: 6 pages, 3 figures

Rapid development in integrated optoelectronic devices and quantum photonic architectures creates a need for optical fiber to chip coupling with low losses. Here we present a fast and generic approach that allows temperature stable self-aligning connections of nanophotonic devices to optical fibers. We show that the attainable precision of our approach is equal to that of DRIE-process based couplings. Specifically, the initial alignment precision is $1.2\pm 0.4\mu m$, the average shift caused by mating $<0.5\mu m$, which is in the order of the precision of the concentricity of the employed fiber, and the thermal cycling stability is $<0.2\mu m$. From these values the expected overall alignment offset is calculated as $1.4 \pm 0.4\mu m$. These results show that our process offers an easy to implement, versatile, robust and DRIE-free method for coupling photonic devices to optical fibers. It can be fully automated and is therefore scalable for coupling to novel devices for quantum photonic systems., Comment: 9 pages, 4 figures

Atomic layer deposition (ALD) is a key technique for the continued scaling of semiconductor devices, which increasingly relies on reproducible and scalable processes for interface manipulation of 3D structured surfaces on the atomic scale. While ALD allows the synthesis of conformal films at low temperature with utmost control over the thickness, atomically-defined closed coatings and surface modifications are still extremely difficult to achieve because of three-dimensional growth during nucleation. Here, we present a route towards sub-nanometer thin and continuous aluminum oxide (AlOx) coatings on silicon (Si) substrates for the spatial control of the surface charge density and interface energetics. We use trimethylaluminum (TMA) in combination with remote hydrogen plasma instead of a gas-phase oxidant for the transformation of silicon oxide into alumina (AlOx). During the initial ALD cycles, TMA reacts with the surface oxide (SiO2) on silicon until there is a saturation of bindings sites, after which the oxygen from the underlying surface oxide is consumed, thereby transforming the silicon oxide into Si capped with AlOx. Depending on the number of ALD cycles, the SiO2 can be partially or fully transformed, which we exploit to create sub-nanometer thin and continuous AlOx layers deposited in selected regions defined by lithographic patterning. The resulting patterned surfaces are characterized by lateral AlOx/SiO2 interfaces possessing step heights as small as 0.3 nm and surface potential steps in excess of 0.4 V. In addition, the introduction of fixed negative charges of $9 \times 10^{12}$ cm$^{-2}$ enables modulation of the surface band bending, which is relevant to the field-effect passivation of Si and low-impedance charge transfer across contact interfaces., Comment: main manuscript: 16 pages, 5 figures; supporting information: 10 pages, 7 figures

We present a novel transparent conductive support structure for two-dimensional (2D) materials that provides an electronically passive 2D/3D interface while also enabling facile interfacial charge transport. This structure, which comprises an evaporated nanocrystalline carbon (nc-C) film beneath an atomic layer deposited alumina (ALD AlOx) layer, is thermally stable and allows direct chemical vapor deposition (CVD) of 2D materials onto the surface. When the nc-C/AlOx is deposited onto a 270 nm SiO2 layer on Si, strong optical contrast for monolayer flakes is retained. Raman spectroscopy reveals good crystal quality for MoS2 and we observe a ten-fold photoluminescence intensity enhancement compared to flakes on conventional Si/SiO2. Tunneling across the ultrathin AlOx enables interfacial charge injection, which we demonstrate by artifact-free scanning electron microscopy and photoemission electron microscopy. Thus, this combination of scalable fabrication and electronic conductivity across a weakly interacting 2D/3D interface opens up new application and characterization opportunities for 2D materials., Comment: 28 pages, 9 figures

We report magneto-photoluminescence spectroscopy of gated MoS$_2$ monolayers in high magnetic fields to 28 T. At B = 0T and electron density $n_s\sim 10^{12}cm^-2$, we observe three trion resonances that cannot be explained within a single-particle picture. Employing ab initio calculations that take into account three-particle correlation effects as well as local and non-local electron-hole exchange interaction, we identify those features as quantum superpositions of inter- and intravalley spin states. We experimentally investigate the mixed character of the trion wave function via the filling factor dependent valley Zeeman shift in positive and negative magnetic fields. Our results highlight the importance of exchange interactions for exciton physics in monolayer MoS$_2$ and provide new insights into the microscopic understanding of trion physics in 2D multi-valley semiconductors for low excess carrier densities., Comment: Main manuscript: 7 pages, 3 figures ; Supplemental material: 16 pages, 4 figures

Nanowire lasers can be monolithically and site-selectively integrated onto silicon photonic circuits. To assess their full potential for ultrafast opto-electronic devices, a detailed understanding of their lasing dynamics is crucial. However, the roles played by their resonator geometry and the microscopic processes that mediate energy exchange between the photonic, electronic, and phononic subsystems are largely unexplored. Here, we study the dynamics of GaAs-AlGaAs core-shell nanowire lasers at cryogenic temperatures using a combined experimental and theoretical approach. Our results indicate that these NW lasers exhibit sustained intensity oscillations with frequencies ranging from 160 GHz to 260 GHz. As the underlying physical mechanism, we identified self-induced electron-hole plasma temperature oscillations resulting from a dynamic competition between photoinduced carrier heating and cooling via phonon scattering. These dynamics are intimately linked to the strong interaction between the lasing mode and the gain material, which arises from the wavelength-scale dimensions of these lasers. We anticipate that our results could lead to new approaches for ultrafast intensity and phase modulation of chip-integrated nanoscale semiconductor lasers., Comment: Revised manuscript