All-Optical Noise Spectroscopy of a Solid-State Spin.

Noise spectroscopy elucidates the fundamental noise sources in spin systems, thereby serving as an essential tool toward developing spin qubits with long coherence times for quantum information processing, communication, and sensing. But existing techniques for noise spectroscopy that rely on microwave fields become infeasible when the microwave power is too weak to generate Rabi rotations of the spin. Here, we demonstrate an alternative all-optical approach to performing noise spectroscopy. Our approach utilizes coherent Raman rotations of the spin state with controlled timing and phase to implement Carr-Purcell-Meiboom-Gill pulse sequences. Analyzing the spin dynamics under these sequences enables us to extract the noise spectrum of a dense ensemble of nuclear spins interacting with a single spin in a quantum dot, which has thus far been modeled only theoretically. By providing spectral bandwidths of over 100 MHz, our approach enables studies of spin dynamics and decoherence for a broad range of solid-state spin qubits.

Optical Transparency Induced by a Largely Purcell Enhanced Quantum Dot in a Polarization-Degenerate Cavity.

Optically active spin systems coupled to photonic cavities with high cooperativity can generate strong light-matter interactions, a key ingredient in quantum networks. However, obtaining high cooperativities for quantum information processing often involves the use of photonic crystal cavities that feature a poor optical access from the free space, especially to circularly polarized light required for the coherent control of the spin. Here, we demonstrate coupling with a cooperativity as high as 8 of an InAs/GaAs quantum dot to a fabricated bullseye cavity that provides nearly degenerate and Gaussian polarization modes for efficient optical accessing. We observe spontaneous emission lifetimes of the quantum dot as short as 80 ps (an ∼15 Purcell enhancement) and a ∼80% transparency of light reflected from the cavity. Leveraging the induced transparency for photon switching while coherently controlling the quantum dot spin could contribute to ongoing efforts of establishing quantum networks.

Enhanced Spin Coherence of a Self-Assembled Quantum Dot Molecule at the Optimal Electrical Bias.

A pair of coupled dots with one electron in each dot can provide improvements in spin coherence, particularly at an electrical bias called the "sweet spot," but few measurements have been performed on self-assembled dots in this regime. Here, we directly measure the T_{2}^{*} coherence time of the singlet-triplet states in this system as a function of bias and magnetic field, obtaining a maximum T_{2}^{*} of 60 ns, more than an order of magnitude higher than an electron spin in a single quantum dot. Our results uncover two main dephasing mechanisms: electrical noise away from the sweet spot, and a magnetic field dependent interaction with nuclear spins due to a difference in g factors.

Coherent Population Trapping Combined with Cycling Transitions for Quantum Dot Hole Spins Using Triplet Trion States.

Optical spin rotations and cycling transitions for measurement are normally incompatible in quantum dots, presenting a fundamental problem for quantum information applications. Here we show that for a hole spin this problem can be addressed using a trion with one hole in an excited orbital, where strong spin-orbit interaction tilts the spin. Then, a particular trion triplet forms a double Λ system, even in a Faraday magnetic field, which we use to demonstrate fast hole spin initialization and coherent population trapping. The lowest trion transitions still strongly preserve spin, thus combining fast optical spin control with cycling transitions for spin readout.

Arrays of Si vacancies in 4H-SiC produced by focused Li ion beam implantation.

Point defects in SiC are an attractive platform for quantum information and sensing applications because they provide relatively long spin coherence times, optical spin initialization, and spin-dependent fluorescence readout in a fabrication-friendly semiconductor. The ability to precisely place these defects at the optimal location in a host material with nano-scale accuracy is desirable for integration of these quantum systems with traditional electronic and photonic structures. Here, we demonstrate the precise spatial patterning of arrays of silicon vacancy ([Formula: see text]) emitters in an epitaxial 4H-SiC (0001) layer through mask-less focused ion beam implantation of Li+. We characterize these arrays with high-resolution scanning confocal fluorescence microscopy on the Si-face, observing sharp emission lines primarily coming from the [Formula: see text] zero-phonon line (ZPL). The implantation dose is varied over 3 orders of magnitude, leading to [Formula: see text] densities from a few per implantation spot to thousands per spot, with a linear dependence between ZPL emission and implantation dose. Optically-detected magnetic resonance (ODMR) is also performed, confirming the presence of V2 [Formula: see text]. Our investigation reveals scalable and reproducible defect generation.

A Spin-Photon Interface Using Charge-Tunable Quantum Dots Strongly Coupled to a Cavity.

Charged quantum dots containing an electron or hole spin are bright solid-state qubits suitable for quantum networks and distributed quantum computing. Incorporating such quantum dot spin into a photonic crystal cavity creates a strong spin-photon interface in which the spin can control a photon by modulating the cavity reflection coefficient. However, previous demonstrations of such spin-photon interfaces have relied on quantum dots that are charged randomly by nearby impurities, leading to instability in the charge state, which causes poor contrast in the cavity reflectivity. Here we demonstrate a strong spin-photon interface using a quantum dot that is charged deterministically with a diode structure. By incorporating this actively charged quantum dot in a photonic crystal cavity, we achieve strong coupling between the cavity mode and the negatively charged state of the dot. Furthermore, by initializing the spin through optical pumping, we show strong spin-dependent modulation of the cavity reflectivity, corresponding to a cooperativity of 12. This spin-dependent reflectivity is important for mediating entanglement between spins using photons, as well as generating strong photon-photon interactions for applications in quantum networking and distributed quantum computing.

Tunable Coupling of a Double Quantum Dot Spin System to a Mechanical Resonator.

The interaction of quantum systems with mechanical resonators is of practical interest for applications in quantum information and sensing and also of fundamental interest as hybrid quantum systems. Achieving a large and tunable interaction strength is of great importance in this field as it enables controlled access to the quantum limit of motion and coherent interactions between different quantum systems. This has been challenging with solid state spins, where typically the coupling is weak and cannot be tuned. Here we use pairs of coupled quantum dots embedded within cantilevers to achieve a high coupling strength of the singlet-triplet spin system to mechanical motion through strain. Two methods of achieving strong, tunable coupling are demonstrated. The first is through different strain-induced energy shifts for the two QDs when the cantilever vibrates, resulting in changes to the exchange interaction. The second is through a laser-driven AC Stark shift that is sensitive to strain-induced shifts of the optical transitions. Both of these mechanisms can be tuned to zero with electrical bias or laser power, respectively, and give large spin-mechanical coupling strengths.

Scalable in operando strain tuning in nanophotonic waveguides enabling three-quantum-dot superradiance.

The quest for an integrated quantum optics platform has motivated the field of semiconductor quantum dot research for two decades. Demonstrations of quantum light sources, single photon switches, transistors and spin-photon interfaces have become very advanced. Yet the fundamental problem that every quantum dot is different prevents integration and scaling beyond a few quantum dots. Here, we address this challenge by patterning strain via local phase transitions to selectively tune individual quantum dots that are embedded in a photonic architecture. The patterning is implemented with in operando laser crystallization of a thin HfO2 film 'sheath' on the surface of a GaAs waveguide. Using this approach, we tune InAs quantum dot emission energies over the full inhomogeneous distribution with a step size down to the homogeneous linewidth and a spatial resolution better than 1 µm. Using these capabilities, we tune multiple quantum dots into resonance within the same waveguide and demonstrate a quantum interaction via superradiant emission from three quantum dots.

Direct excitation of a single quantum dot with cavity-SPDC photons.

The ability to generate mode-engineered single photons to interface with disparate quantum systems is of importance for building a quantum network. Here we report on the generation of a pulsed, heralded single photon source with a sub-GHz spectral bandwidth that couples to indium arsenide quantum dots centered at 942 nm. The source is built with a type-II PPKTP down-conversion crystal embedded in a semi-confocal optical cavity and pumped with a 76 MHz repetition rate pulsed laser to emit collinear, polarization-correlated photon pairs resonant with a single quantum dot. In order to demonstrate direct coupling, we use the mode-engineered cavity-SPDC single-photon source to resonantly excite an isolated single quantum dot.

Nonlocal Nuclear Spin Quieting in Quantum Dot Molecules: Optically Induced Extended Two-Electron Spin Coherence Time.

We demonstrate the extension of coherence between all four two-electron spin ground states of an InAs quantum dot molecule (QDM) via nonlocal suppression of nuclear spin fluctuations in two vertically stacked quantum dots (QDs), while optically addressing only the top QD transitions. Long coherence times are revealed through dark-state spectroscopy as resulting from nuclear spin locking mediated by the exchange interaction between the QDs. Line shape analysis provides the first measurement of the quieting of the Overhauser field distribution correlating with reduced nuclear spin fluctuations.

Spin-cavity interactions between a quantum dot molecule and a photonic crystal cavity.

The integration of InAs/GaAs quantum dots into nanophotonic cavities has led to impressive demonstrations of cavity quantum electrodynamics. However, these demonstrations are primarily based on two-level excitonic systems. Efforts to couple long-lived quantum dot electron spin states with a cavity are only now succeeding. Here we report a two-spin-cavity system, achieved by embedding an InAs quantum dot molecule within a photonic crystal cavity. With this system we obtain a spin singlet-triplet Λ-system where the ground-state spin splitting exceeds the cavity linewidth by an order of magnitude. This allows us to observe cavity-stimulated Raman emission that is highly spin-selective. Moreover, we demonstrate the first cases of cavity-enhanced optical nonlinearities in a solid-state Λ-system. This provides an all-optical, local method to control the spin exchange splitting. Incorporation of a highly engineerable quantum dot molecule into the photonic crystal architecture advances prospects for a quantum network.

Optophononics with coupled quantum dots.

Modern technology is founded on the intimate understanding of how to utilize and control electrons. Next to electrons, nature uses phonons, quantized vibrations of an elastic structure, to carry energy, momentum and even information through solids. Phonons permeate the crystalline components of modern technology, yet in terms of technological utilization phonons are far from being on par with electrons. Here we demonstrate how phonons can be employed to render a single quantum dot pair optically transparent. This phonon-induced transparency is realized via the formation of a molecular polaron, the result of a Fano-type quantum interference, which proves that we have accomplished making typically incoherent and dissipative phonons behave in a coherent and non-dissipative manner. We find the transparency to be widely tunable by electronic and optical means. Thereby we show amplification of weakest coupling channels. We further outline the molecular polaron's potential as a control element in phononic circuitry architecture.

Leveraging crystal anisotropy for deterministic growth of InAs quantum dots with narrow optical linewidths.

Crystal growth anisotropy in molecular beam epitaxy usually prevents deterministic nucleation of individual quantum dots when a thick GaAs buffer is grown over a nanopatterned substrate. Here, we demonstrate how this anisotropy can actually be used to mold nucleation sites for single dots on a much thicker buffer than has been achieved by conventional techniques. This approach greatly suppresses the problem of defect-induced line broadening for single quantum dots in a charge-tunable device, giving state-of-the-art optical linewidths for a system widely studied as a spin qubit for quantum information.

Persistent narrowing of nuclear-spin fluctuations in InAs quantum dots using laser excitation.

We demonstrate the suppression of nuclear-spin fluctuations in an InAs quantum dot and measure the timescales of the spin narrowing effect. By initializing for tens of milliseconds with two continuous wave diode lasers, fluctuations of the nuclear spins are suppressed via the hole-assisted dynamic nuclear polarization feedback mechanism. The fluctuation narrowed state persists in the dark (absent light illumination) for well over 1 s even in the presence of a varying electron charge and spin polarization. Enhancement of the electron spin coherence time (T2*) is directly measured using coherent dark state spectroscopy. By separating the calming of the nuclear spins in time from the spin qubit operations, this method is much simpler than the spin echo coherence recovery or dynamic decoupling schemes.

Three-dimensional control of self-assembled quantum dot configurations.

We demonstrate techniques for growing three-dimensional quantum dot configurations using molecular beam epitaxy on faceted template islands. Molecular beam shadowing leads to new geometries through selective nucleation of the dots on the template edges. Strain-induced stacking converts the planar configurations into three-dimensional structures. The resulting dot morphologies and their configurational uniformity are studied using cross sectional scanning tunneling microscopy and atomic force microscopy. Combining photoluminescence measurements with structural characterization allows interpretation of the ensemble photoluminescence spectrum. Bright spectra for the three-dimensional structures suggest an improved method for combining lithographic nucleation sites with self-assembled dot growth. These techniques can be applied to lithographic templates to fabricate complex quantum dot networks.

Optically controlled locking of the nuclear field via coherent dark-state spectroscopy.

A single electron or hole spin trapped inside a semiconductor quantum dot forms the foundation for many proposed quantum logic devices. In group III-V materials, the resonance and coherence between two ground states of the single spin are inevitably affected by the lattice nuclear spins through the hyperfine interaction, while the dynamics of the single spin also influence the nuclear environment. Recent efforts have been made to protect the coherence of spins in quantum dots by suppressing the nuclear spin fluctuations. However, coherent control of a single spin in a single dot with simultaneous suppression of the nuclear fluctuations has yet to be achieved. Here we report the suppression of nuclear field fluctuations in a singly charged quantum dot to well below the thermal value, as shown by an enhancement of the single electron spin dephasing time T(2)*, which we measure using coherent dark-state spectroscopy. The suppression of nuclear fluctuations is found to result from a hole-spin assisted dynamic nuclear spin polarization feedback process, where the stable value of the nuclear field is determined only by the laser frequencies at fixed laser powers. This nuclear field locking is further demonstrated in a three-laser measurement, indicating a possible enhancement of the electron spin T(2)* by a factor of several hundred. This is a simple and powerful method of enhancing the electron spin coherence time without use of 'spin echo'-type techniques. We expect that our results will enable the reproducible preparation of the nuclear spin environment for repetitive control and measurement of a single spin with minimal statistical broadening.

Optical spin initialization and nondestructive measurement in a quantum dot molecule.

The spin of an electron in a self-assembled InAs/GaAs quantum dot molecule is optically prepared and measured through the trion triplet states. A longitudinal magnetic field is used to tune two of the trion states into resonance, forming a superposition state through asymmetric spin exchange. As a result, spin-flip Raman transitions can be used for optical spin initialization, while separate trion states enable cycling transitions for nondestructive measurement. With two-laser transmission spectroscopy we demonstrate both operations simultaneously, something not previously accomplished in a single quantum dot.

Coherent optical spectroscopy of a strongly driven quantum dot.

Quantum dots are typically formed from large groupings of atoms and thus may be expected to have appreciable many-body behavior under intense optical excitation. Nonetheless, they are known to exhibit discrete energy levels due to quantum confinement effects. We show that, like single-atom or single-molecule two- and three-level quantum systems, single semiconductor quantum dots can also exhibit interference phenomena when driven simultaneously by two optical fields. Probe absorption spectra are obtained that exhibit Autler-Townes splitting when the optical fields drive coupled transitions and complex Mollow-related structure, including gain without population inversion, when they drive the same transition. Our results open the way for the demonstration of numerous quantum level-based applications, such as quantum dot lasers, optical modulators, and quantum logic devices.