Coherent Dynamics in Quantum Emitters under Dichromatic Excitation.

We characterize the coherent dynamics of a two-level quantum emitter driven by a pair of symmetrically detuned phase-locked pulses. The promise of dichromatic excitation is to spectrally isolate the excitation laser from the quantum emission, enabling background-free photon extraction from the emitter. While excitation is not possible without spectral overlap between the exciting pulse and the quantum emitter transition for ideal two-level systems due to cancellation of the accumulated pulse area, we find that any additional interactions that interfere with cancellation of the accumulated pulse area may lead to a finite stationary population inversion. Our spectroscopic results of a solid-state two-level system show that, while coupling to lattice vibrations helps to improve the inversion efficiency up to 50% under symmetric driving, coherent population control and a larger amount of inversion are possible using asymmetric dichromatic excitation, which we achieve by adjusting the ratio of the intensities between the red- and blue-detuned pulses. Our measured results, supported by simulations using a real-time path-integral method, offer a new perspective toward realizing efficient, background-free photon generation and extraction.

Highly energy-tunable quantum light from moiré-trapped excitons.

Photon antibunching, a hallmark of quantum light, has been observed in the correlations of light from isolated atomic and atomic-like solid-state systems. Two-dimensional semiconductor heterostructures offer a unique method to create a quantum light source: Moiré trapping potentials for excitons are predicted to create arrays of quantum emitters. While signatures of moiré-trapped excitons have been observed, their quantum nature has yet to be confirmed. Here, we report photon antibunching from single moiré-trapped interlayer excitons in a heterobilayer. Via magneto-optical spectroscopy, we demonstrate that the discrete anharmonic spectra arise from bound band-edge electron-hole pairs trapped in moiré potentials. Last, we exploit the large permanent dipole of interlayer excitons to achieve large direct current (DC) Stark tuning up to 40 meV. Our results confirm the quantum nature of moiré-confined excitons and open opportunities to investigate their inhomogeneity and interactions between the emitters or energetically tune single emitters into resonance with cavity modes.

Fundamental Limits to Coherent Photon Generation with Solid-State Atomlike Transitions.

Coherent generation of indistinguishable single photons is crucial for many quantum communication and processing protocols. Solid-state realizations of two-level atomic transitions or three-level spin-Λ systems offer significant advantages over their atomic counterparts for this purpose, albeit decoherence can arise due to environmental couplings. One popular approach to mitigate dephasing is to operate in the weak-excitation limit, where the excited-state population is minimal and coherently scattered photons dominate over incoherent emission. Here we probe the coherence of photons produced using two-level and spin-Λ solid-state systems. We observe that the coupling of the atomiclike transitions to the vibronic transitions of the crystal lattice is independent of the driving strength, even for detuned excitation using the spin-Λ configuration. We apply a polaron master equation to capture the non-Markovian dynamics of the vibrational manifolds. These results provide insight into the fundamental limitations to photon coherence from solid-state quantum emitters.

Screening Nuclear Field Fluctuations in Quantum Dots for Indistinguishable Photon Generation.

A semiconductor quantum dot can generate highly coherent and indistinguishable single photons. However, intrinsic semiconductor dephasing mechanisms can reduce the visibility of two-photon interference. For an electron in a quantum dot, a fundamental dephasing process is the hyperfine interaction with the nuclear spin bath. Here, we directly probe the consequence of the fluctuating nuclear spins on the elastic and inelastic scattered photon spectra from a resident electron in a single dot. We find the in-plane component of the nuclear Overhauser field leads to detuned Raman scattered photons, broadened over experimental time scales by field fluctuations, which are distinguishable from both the elastic and incoherent components of the resonance fluorescence. This significantly reduces two-photon interference visibility. However, we demonstrate successful screening of the nuclear spin noise, which enables the generation of coherent single photons that exhibit high visibility two-photon interference.

Strain-Induced Spatial and Spectral Isolation of Quantum Emitters in Mono- and Bilayer WSe2.

Two-dimensional transition metal dichalcogenide semiconductors are intriguing hosts for quantum light sources due to their unique optoelectronic properties. Here, we report that strain gradients, either unintentionally induced or generated by substrate patterning, result in spatially and spectrally isolated quantum emitters in mono- and bilayer WSe2. By correlating localized excitons with localized strain variations, we show that the quantum emitter emission energy can be red-tuned up to a remarkable ∼170 meV. We probe the fine-structure, magneto-optics, and second-order coherence of a strained emitter. These results raise the prospect of strain-engineering quantum emitter properties and deterministically creating arrays of quantum emitters in two-dimensional semiconductors.

Highly directional emission from a quantum emitter embedded in a hemispherical cavity.

We report the design of a solid-state, micron-sized hemispherical cavity that yields significantly enhanced extraction efficiency with modest Purcell enhancement from embedded quantum emitters. A simple analytical model provides a guideline for the design and optimization of the structure, while finite-difference time-domain simulations are used for full analysis of the optimum structure. Cavity modes with up to 90% extraction efficiency, a Purcell enhancement factor >2, and a quality factor of ≈50 are achieved. In addition, Gaussian-like far-field beam profiles with low divergence are exhibited for several modes. These monolithic cavities are promising for solid-state emitters buried in a high dielectric environment, such as self-assembled quantum dots and optically active defects in diamond.

Probing single-charge fluctuations at a GaAs/AlAs interface using laser spectroscopy on a nearby InGaAs quantum dot.

We probe local charge fluctuations in a semiconductor via laser spectroscopy on a nearby self-assembled quantum dot. We demonstrate that the quantum dot is sensitive to changes in the local environment at the single-charge level. By controlling the charge state of localized defects, we are able to infer the distance of the defects from the quantum dot with ±5 nm resolution. The results identify and quantify the main source of charge noise in the commonly used optical field-effect devices.

Controlling the interaction of electron and nuclear spins in a tunnel-coupled quantum dot.

We present a technique for manipulating the nuclear spins and the emission polarization from a single optically active quantum dot. When the quantum dot is tunnel coupled to a Fermi sea, we have discovered a natural cycle in which an electron spin is repeatedly created with resonant optical excitation. The spontaneous emission polarization and the nuclear spin polarization exhibit a bistability. For a σ(+) pump, the emission switches from σ(+) to σ(-) at a particular detuning of the laser. Simultaneously, the nuclear spin polarization switches from positive to negative. Away from the bistability, the nuclear spin polarization can be changed continuously from negative to positive, allowing precise control via the laser wavelength.

Optically induced hybridization of a quantum dot state with a filled continuum.

We present an optical signature of a hybridization between a localized quantum dot state and a filled continuum. Radiative recombination of the negatively charged trion in a single quantum dot leaves behind a single electron. We show that in two regions of vertical electric field, the electron hybridizes with a continuum through a tunneling interaction. The hybridization manifests itself through an unusual voltage dependence of the emission energy and a non-Lorentzian line shape, features which we reproduce with a theory based on the Anderson Hamiltonian.

The nonlinear Fano effect.

The Fano effect is ubiquitous in the spectroscopy of, for instance, atoms, bulk solids and semiconductor heterostructures. It arises when quantum interference takes place between two competing optical pathways, one connecting the energy ground state and an excited discrete state, the other connecting the ground state with a continuum of energy states. The nature of the interference changes rapidly as a function of energy, giving rise to characteristically asymmetric lineshapes. The Fano effect is particularly important in the interpretation of electronic transport and optical spectra in semiconductors. Whereas Fano's original theory applies to the linear regime at low power, at higher power a laser field strongly admixes the states and the physics becomes rich, leading, for example, to a remarkable interplay of coherent nonlinear transitions. Despite the general importance of Fano physics, this nonlinear regime has received very little attention experimentally, presumably because the classic autoionization processes, the original test-bed of Fano's ideas, occur in an inconvenient spectral region, the deep ultraviolet. Here we report experiments that access the nonlinear Fano regime by using semiconductor quantum dots, which allow both the continuum states to be engineered and the energies to be rescaled to the near infrared. We measure the absorption cross-section of a single quantum dot and discover clear Fano resonances that we can tune with the device design or even in situ with a voltage bias. In parallel, we develop a nonlinear theory applicable to solid-state systems with fast relaxation of carriers. In the nonlinear regime, the visibility of the Fano quantum interferences increases dramatically, affording a sensitive probe of continuum coupling. This could be a unique method to detect weak couplings of a two-level quantum system (qubits), which should ideally be decoupled from all other states.

Fine structure of negatively and positively charged excitons in semiconductor quantum dots: electron-hole asymmetry.

We present new understanding of excitonic fine structure in close-to-symmetric InAs/GaAs and InGaAs/GaAs quantum dots. We demonstrate excellent agreement between spectroscopy and many-body pseudopotential theory in the energy splittings, selection rules and polarizations of the optical emissions from doubly charged excitons. We discover a marked difference between the fine structure of the doubly negatively and doubly positively charged excitons. The features in the doubly charged emission spectra are shown to arise mainly from the lack of inversion symmetry in the underlying crystal lattice.

Entangled photon pairs from semiconductor quantum dots.

Tomographic analysis demonstrates that the polarization state of pairs of photons emitted from a biexciton decay cascade becomes entangled when spectral filtering is applied. The measured density matrix of the photon pair satisfies the Peres criterion for entanglement by more than 3 standard deviations of the experimental uncertainty and violates Bell's inequality. We show that the spectral filtering erases the "which path" information contained in the photons' color and that the remanent information in the quantum dot degrees of freedom is negligible.

Voltage control of the spin dynamics of an exciton in a semiconductor quantum dot.

We report the observation of a spin-flip process in a quantum dot whereby a dark exciton with total angular momentum L = 2 becomes a bright exciton with L = 1. The spin-flip process is revealed in the decay dynamics following nongeminate excitation. We are able to control the spin-flip rate by more than an order of magnitude simply with a dc voltage. The spin-flip mechanism involves a spin exchange with the Fermi sea in the back contact of our device and corresponds to the high temperature Kondo regime. We use the Anderson Hamiltonian to calculate a spin-flip rate, and we find excellent agreement with the experimental results.

Fine structure of highly charged excitons in semiconductor quantum dots.

An exciton in a symmetric semiconductor quantum dot has two possible states, one dark and one bright, split in energy by the electron-hole exchange interaction. We demonstrate that for a doubly charged exciton, there are also two states split by the electron-hole exchange, but both states are now bright. We also uncover a fine structure in the emission from the triply charged exciton. By measuring these splittings, and also those from the singly charged and doubly charged biexcitons, all on the same quantum dot, we show how the various electron-hole exchange energies can be measured without having to break the symmetry of the dot.