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Two-dimensional (2D) materials have shown great promise as hosts for high-purity deterministic single-photon sources. In the last few years, the underlying physics of single photon emission in 2D materials have been uncovered, and their optical properties have been improved to meet criteria for a variety of quantum technologies and applications. In this work, we take advantage of the unique characteristics of dielectric nanoantennas in manipulating the electromagnetic response on a sub-wavelength scale to localize and control defect-based single-photon emitters (SPEs) in 2D layered materials. We show that dielectric nanoantennas are capable of inducing high Purcell enhancement >20 and therefore brighter single-photon emission, which is characterized by a reduction of the emitters’ radiative lifetimes and enhancement of their brightness by more than an order of magnitude. We demonstrate that the sub-wavelength-scale dielectric nanoantennas can be designed to also impose a predetermined strain profile that determines the confinement potential of the SPE, leading to robust control over the optical polarization with up to 94% extinction ratio. The combination of large Purcell enhancement, polarization orientation, and site control through strain engineering demonstrates the advantages and unique capabilities of dielectric nanoantennas for enhancing the quantum optical properties of 2D SPEs for quantum information technologies.

Single-photon emitters are an essential component of quantum networks, and defects or impurities in semiconductors are a promising platform to realize such quantum emitters. Here, we present a model that encapsulates the essential physics of coupling to phonons, which governs the behavior of real single-photon emitters, and critically evaluate several approximations that are commonly utilized. Emission in the telecom wavelength range is highly desirable, but our model shows that nonradiative processes are greatly enhanced at these low photon energies, leading to a decrease in efficiency. Our results suggest that reducing the phonon frequency is a fruitful avenue to enhance the efficiency. [ABSTRACT FROM AUTHOR]

Recent advances in the isolation and stacking of monolayers of van der Waals materials have provided approaches for the preparation of quantum materials in the ultimate two-dimensional limit.sup.1,2. In van der Waals heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moiré superlattice.sup.3. It is widely recognized that the moiré superlattice can modulate the electronic band structure of the material and lead to transport properties such as unconventional superconductivity.sup.4 and insulating behaviour driven by correlations.sup.5-7; however, the influence of the moiré superlattice on optical properties has not been investigated experimentally. Here we report the observation of multiple interlayer exciton resonances with either positive or negative circularly polarized emission in a molybdenum diselenide/tungsten diselenide (MoSe.sub.2/WSe.sub.2) heterobilayer with a small twist angle. We attribute these resonances to excitonic ground and excited states confined within the moiré potential. This interpretation is supported by recombination dynamics and by the dependence of these interlayer exciton resonances on twist angle and temperature. These results suggest the feasibility of engineering artificial excitonic crystals using van der Waals heterostructures for nanophotonics and quantum information applications. Multiple interlayer exciton resonances in a MoSe.sub.2/WSe.sub.2 heterobilayer with a small twist angle are attributed to excitonic ground and excited states confined within the moiré potential., Author(s): Kha Tran [sup.1] , Galan Moody [sup.2] , Fengcheng Wu [sup.3] , Xiaobo Lu [sup.4] , Junho Choi [sup.1] , Kyounghwan Kim [sup.5] , Amritesh Rai [sup.5] , Daniel [...]

An optical fibre-fed superconducting electro-optic modulator with gigahertz bandwidth and attojoule per bit electric power consumption offers a fast, efficient means to connect superconducting circuits to the room temperature environment. [ABSTRACT FROM AUTHOR]

We report on scalable heterointegration of superconducting electrodes and epitaxial semiconductor quantum dots (QDs) 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 ≈ 17 000 representing a three-fold enhancement compared to identical devices with normal conducting electrodes. Superconducting operation of ≈ 400 M H z resonators is achieved to temperatures T > 7 K and electrical radio frequency powers P r f > + 9 d B m . Heterogeneously integrated single QDs 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 QD—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 QD. 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. [ABSTRACT FROM AUTHOR]

We demonstrate a new method for multidimensional coherent spectroscopy of nanostructures. We use a heterodyne technique implemented with a confocal microscope to record the amplitude and phase of all degenerate third-order wave-mixing processes.

Two-dimensional (2D) materials have shown great promise as hosts for high-purity deterministic single-photon sources. In the last few years, the underlying physics of single photon emission in 2D materials have been uncovered, and their optical properties have been improved to meet criteria for a variety of quantum technologies and applications. In this work, we take advantage of the unique characteristics of dielectric nanoantennas in manipulating the electromagnetic response on a sub-wavelength scale to localize and control defect-based single-photon emitters (SPEs) in 2D layered materials. We show that dielectric nanoantennas are capable of inducing high Purcell enhancement >20 and therefore brighter single-photon emission, which is characterized by a reduction of the emitters' radiative lifetimes and enhancement of their brightness by more than an order of magnitude. We demonstrate that the sub-wavelength-scale dielectric nanoantennas can be designed to also impose a predetermined strain profile that determines the confinement potential of the SPE, leading to robust control over the optical polarization with up to 94% extinction ratio. The combination of large Purcell enhancement, polarization orientation, and site control through strain engineering demonstrates the advantages and unique capabilities of dielectric nanoantennas for enhancing the quantum optical properties of 2D SPEs for quantum information technologies. [ABSTRACT FROM AUTHOR]

Optical single- and double-quantum three-dimensional Fourier-transform spectra are obtained for atomic vapors. We show that three-dimensional spectra can be used to identify the Hamiltonian of complex systems and to reveal the nature of many-body interactions.

We review our recent work on multi-dimensional coherent optical spectroscopy (MDCS) of semiconductor nanostructures. Two approaches, appropriate for the study of semiconductor materials, are presented and compared. A first method is based on a non-collinear geometry, where the Four-Wave-Mixing (FWM) signal is detected in the form of a radiated optical field. This approach works for samples with translational symmetry, such as Quantum Wells (QWs) or large and dense ensembles of Quantum Dots (QDs). A second method detects the FWM in the form of a photocurrent in a collinear geometry. This second approach extends the horizon of MDCS to sub-diffraction nanostructures, such as single QDs, nanowires, or nanotubes, and small ensembles thereof. Examples of experimental results obtained on semiconductor QW structures are given for each method. In particular, it is shown how MDCS can assess coupling between excitons confined in separated QWs. [ABSTRACT FROM AUTHOR]

The search for an ideal single-photon source has generated significant interest in discovering emitters in materials as well as developing new manipulation techniques to gain better control over the emitters' properties. Quantum emitters in atomically thin two-dimensional (2D) materials have proven to be very attractive with high brightness, operation under ambient conditions, and the ability to be integrated with a wide range of electronic and photonic platforms. This Perspective highlights some of the recent advances in quantum light generation from 2D materials, focusing on hexagonal boron nitride and transition metal dichalcogenides. Efforts in engineering and deterministically creating arrays of quantum emitters in 2D materials, their electrical excitation, and their integration with photonic devices are discussed. Finally, we address some of the challenges the field is facing and the near-term efforts to tackle them. We provide an outlook toward efficient and scalable quantum light generation from 2D materials to controllable and addressable on-chip quantum sources. [ABSTRACT FROM AUTHOR]

We demonstrate cryogenic, all on-chip, single-photon-level photonic integrated circuits on a III-V platform with waveguide-coupled quantum-well sources and tungsten silicide superconducting nanowire single-photon detectors. We have measured the dark count rates below 10−3 counts/s and have reduced the cross talk to an adjacent waveguide by 30 dB. [ABSTRACT FROM AUTHOR]

We demonstrate cryogenic, electrically injected, waveguide-coupled Si light-emitting diodes (LEDs) operating at 1.22 μm. The active region of the LED consists of W centers implanted in the intrinsic region of a p-i-n diode. The LEDs are integrated on waveguides with superconducting nanowire single-photon detectors (SNSPDs). We demonstrate the scalability of this platform with an LED coupled to eleven SNSPDs in a single integrated photonic device. [ABSTRACT FROM AUTHOR]

We report charged exciton (trion) formation dynamics in doped monolayer transition metal dichalcogenides, specifically molybdenum diselenide (MoSe2), using resonant two-color pump-probe spectroscopy. When resonantly pumping the exciton transition, trions are generated on a picosecond time scale through excitonelectron interaction. As the pump energy is tuned from the high energy to low energy side of the inhomogeneously broadened exciton resonance, the trion formation time increases by ~50%. This feature can be explained by the existence of both localized and delocalized excitons in a disordered potential and suggests the existence of an exciton mobility edge in transition metal dichalcogenides. [ABSTRACT FROM AUTHOR]

We report the first direct spectroscopic evidence for coherent electronic coupling between excitons and trions in atomically thin transition metal dichalcogenides, specifically monolayer MoSe2. Signatures of coupling appear as isolated cross-peaks in two-color pump-probe spectra, and the line shape of the peaks reveals that the coherent coupling originates from many-body interactions. Excellent agreement between the experiment and density matrix calculations suggests that coherent exciton-trion coupling leads to the formation of a correlated state with a remarkably large binding energy. [ABSTRACT FROM AUTHOR]

We study an asymmetric double InGaAs quantum well using optical two-dimensional coherent spectroscopy. The collection of zero-quantum, one-quantum, and two-quantum two-dimensional spectra provides a unique and comprehensive picture of the double well coherent optical response. Coherent and incoherent contributions to the coupling between the two quantum well excitons are clearly separated. An excellent agreement with density matrix calculations reveals that coherent interwell coupling originates from many-body interactions. [ABSTRACT FROM AUTHOR]

The effects of confinement on biexciton renormalization in self-assembled InAs and interfacial GaAs quantum dot (QD) ensembles are studied using two-dimensional Fourier-transform spectroscopy. We find that in thermally annealed InAs QDs, changes in the biexciton transition energy are strongly correlated with those of the exciton and that the biexciton binding energy is similar for all QDs in the ensemble. These results are in contrast to those from GaAs QDs formed from interfacial fluctuations of a narrow quantum well (QW). In both the GaAs QW and QDs, correlation is reduced and the biexciton binding exhibits a strong dependence on localization. Comparison with simulations reveals how confinement and Coulomb interactions modify biexciton renormalization. [ABSTRACT FROM AUTHOR]

Optical 2-D Fourier transform spectroscopy is a powerful technique for studying resonant light-matter interactions, determining the transition structure and monitoring dynamics of optically created excitations. The ability to separate homogeneous and inhomogeneous broadening is one important capability. In this paper, we discuss the use of this technique to study excitonic transitions in semiconductor nanostructures. In quantum wells, the effects of structural disorder is observed as inhomogeneous broadening of the exciton resonances. In quantum dots, the temperature dependence of the homogeneous width gives insight into the nature of the dephasing processes. [ABSTRACT FROM PUBLISHER]

In atomically thin two-dimensional semiconductors such as transition metal dichalcogenides (TMDs), controlling the density and type of defects promises to be an effective approach for engineering light-matter interactions. We demonstrate that electron-beam irradiation is a simple tool for selectively introducing defect-bound exciton states associated with chalcogen vacancies in TMDs. Our first-principles calculations and time-resolved spectroscopy measurements of monolayer WSe2 reveal that these defect-bound excitons exhibit exceptional optical properties including a recombination lifetime approaching 200 ns and a valley lifetime longer than 1 μs. The ability to engineer the crystal lattice through electron irradiation provides a new approach for tailoring the optical response of TMDs for photonics, quantum optics, and valleytronics applications. [ABSTRACT FROM AUTHOR]

In atomically thin transition metal dichalcogenides (TMDs), reduced dielectric screening of the Coulomb interaction leads to strongly correlated many-body states, including excitons and trions, that dominate the optical properties. Higher-order states, such as bound biexcitons, are possible but are difficult to identify unambiguously using linear optical spectroscopy methods. Here, we implement polarization-resolved two-dimensional coherent spectroscopy (2DCS) to unravel the complex optical response of monolayer MoSe2 and identify multiple higher-order correlated states. Decisive signatures of neutral and charged inter-valley biexcitons appear in cross-polarized two-dimensional spectra as distinct resonances with respective ∼20 and ∼5 meV binding energies-similar to recent calculations using variational and Monte Carlo methods. A theoretical model considering the valley-dependent optical selection rules reveals the quantum pathways that give rise to these states. Inter-valley biexcitons identified here, comprising of neutral and charged excitons from different valleys, offer new opportunities for developing ultrathin biexciton lasers and polarization-entangled photon sources. [ABSTRACT FROM AUTHOR]

Predicting and controlling quantum mechanical phenomena require knowledge of the system Hamiltonian. A detailed understanding of the quantum pathways used to construct the Hamiltonian is essential for deterministic control and improved performance of coherent control schemes. In complex systems, parameters characterizing the pathways, especially those associated with inter-particle interactions and coupling to the environment, can only be identified experimentally. Quantitative insight can be obtained provided the quantum pathways are isolated and independently analysed. Here we demonstrate this possibility in an atomic vapour using optical three-dimensional Fourier-transform spectroscopy. By unfolding the system's nonlinear response onto three frequency dimensions, three-dimensional spectra unambiguously reveal transition energies, relaxation rates and dipole moments of each pathway. The results demonstrate the unique capacity of this technique as a powerful tool for resolving the complex nature of quantum systems. This experiment is a critical step in the pursuit of complete experimental characterization of a system's Hamiltonian. [ABSTRACT FROM AUTHOR]

Exciton transport in nanomaterials is sensitive to fluctuations in the confinement potential that are intrinsic to heterogeneous solid-state systems. Redistribution of exciton population manifests as spectral diffusion in which the exciton energy shifts. It is generally assumed that increase or decrease in the exciton energy are equally probable. We show that this assumption is not necessarily valid using two-dimensional coherent spectroscopy on a disordered GaAs quantum well. High-energy excitons relax into lower-energy localized states over a time scale of tens of picoseconds at low sample temperatures (~5K). A transition to uniform spectral diffusion of excitons is observed as the temperature is increased to ~20K. Numerical simulations reveal the contribution of exciton-phonon interactions to spectral diffusion of excitons. These results provide a perspective on the process of dynamic localization and the effect of the correlation length of disorder on spectral diffusion of excitons. [ABSTRACT FROM AUTHOR]

The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron-hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton-trion coupling and conversion phenomena. In this work, we reveal the coherent and incoherent nature of exciton-trion coupling and the relevant time scales in monolayer MoSe2 using optical two-dimensional coherent spectroscopy. Coherent interaction between excitons and trions is definitively identified as quantum beating of cross peaks in the spectra that persists for a few hundred femtoseconds. For longer times up to 10 ps, surprisingly, the relative intensity of the cross peaks increases, which is attributed to incoherent energy transfer likely due to phonon-assisted up-conversion and down-conversion processes that are efficient even at cryogenic temperature. [ABSTRACT FROM AUTHOR]

The homogeneous and inhomogeneous linewidths of the heavy-hole exciton resonance in a (110)-oriented GaAs multiple-quantum-well sample are measured using optical two-dimensional Fourier transform spectroscopy. By probing the optical nonlinear response for polarization along the in-plane crystal axes [110] and [110], we measure different homogeneous linewidths for the two orthogonal directions. This difference is found to be due to anisotropic excitation-induced dephasing, caused by a crystal-axis-dependent absorption coefficient. The extrapolated zero-excitation density homogeneous linewidth exhibits an activation-like temperature dependence. We find that the homogeneous linewidth extrapolated to zero excitation density and temperature is ∼34 μeV, while the inhomogeneous linewidth is 1.9 meV for both polarizations. [ABSTRACT FROM AUTHOR]

In van der Waals (vdW) heterostructures formed by stacking two monolayers of transition metal dichalcogenides, multiple exciton resonances with highly tunable properties are formed and subject to both vertical and lateral confinement. We investigate how a unique control knob, the twist angle between the two monolayers, can be used to control the exciton dynamics. We observe that the interlayer exciton lifetimes in MoSe2/WSe2 twisted bilayers (TBLs) change by one order of magnitude when the twist angle is varied from 1° to 3.5°. Using a low-energy continuum model, we theoretically separate two leading mechanisms that influence interlayer exciton radiative lifetimes. The shift to indirect transitions in the momentum space with an increasing twist angle and the energy modulation from the moiré potential both have a significant impact on interlayer exciton lifetimes. We further predict distinct temperature dependence of interlayer exciton lifetimes in TBLs with different twist angles, which is partially validated by experiments. While many recent studies have highlighted how the twist angle in a vdW TBL can be used to engineer the ground states and quantum phases due to many-body interaction, our studies explore its role in controlling the dynamics of optically excited states, thus, expanding the conceptual applications of "twistronics". [ABSTRACT FROM AUTHOR]

The exciton coherent signal decay rate in GaAs quantum wells, as measured in four-wave mixing experiments, depends on the polarization of the excitation pulses. Using polarization-dependent two-dimensional coherent spectroscopy, we show that this behavior is due to the bosonic character of excitons. Interference between two different quantum mechanical pathways results in a smaller decay rate for cocircular and colinear polarization of the optical excitation pulses. This interference does not exist for cross-linearly polarized excitation pulses resulting in a larger decay rate. Our result shows that the bosonic nature of excitons must be considered when interpreting ultrafast spectroscopic studies of exciton dephasing in semiconductors. This behavior should be considered while interpreting results of ultrafast spectroscopy experiments involving bosonlike excitations. [ABSTRACT FROM AUTHOR]

Studies have shown that many-body interactions among semiconductor excitons can produce distinct features in two-dimensional optical spectra. However, to the best of our knowledge, the dynamics of many-body interactions have not been measured in two-dimensional (2D) spectroscopy studies. Here we measure 2D spectra of GaAs quantum wells at many different "waiting" times and study the time dependence of the spectral features. Characteristic signatures of exciton polarization correlations manifest in the diagonal peaks decay at the exciton dephasing rate, consistent with theoretical predictions. Other many-body interactions manifest in off-diagonal features decay much more slowly. These persistent off-diagonal features must be due to many-body interactions involving exciton populations, and their persistence cannot be predicted by theoretical descriptions restricted to the coherent limit. [ABSTRACT FROM AUTHOR]