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We demonstrate scattering of laser light from two InAs quantum dots coupled to a photonic crystal waveguide, which is achieved by strain-tuning the optical transitions of the dots into mutual resonance. By performing measurements of the intensity and photon statistics of transmitted laser light before and after tuning the dots into resonance, we show that the nonlinearity is enhanced by collective scattering. In addition to providing a means of manipulating few-photon optical nonlinearities, our approach establishes new opportunities for multi-emitter quantum optics in a solid-state platform.

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.

Optically-active spin systems coupled to photonic cavities with high cooperativity can generate strong light-matter interactions, a key ingredient in quantum networks. But 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 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 (a $\approx 15$ Purcell enhancement) and a $\approx 80\%$ 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.

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 only been modeled theoretically. By providing spectral bandwidths of over 100 MHz, our approach enables the studies of spin dynamics and decoherence for a broad range of solid-state spin qubits.

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 $\Lambda$ 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., Comment: 30 pages, 13 figures

We report on the direct measurement of the electron spin splitting and the accompanying nuclear Overhauser (OH) field, and thus the underlying nuclear spin polarization (NSP) and fluctuation bandwidth, in a single InAs quantum dot under resonant excitation conditions with unprecedented spectral resolution. The electron spin splitting is measured directly via resonant spin-flip single photon Raman scattering detected by superconducting nanowires to generate excitation-emission energy maps. The observed two-dimensional maps reveal an OH field that has a non-linear dependence on excitation frequency. This study provides new insight into earlier reports of so-called avoidance and tracking, showing two distinct NSP responses directly by the addition of a emission energy axis. The data show that the polarization processes depend on which electron spin state is optically driven, with surprising differences in the polarization fluctuations for each case: in one case, a stabilized field characterized by a single-peaked distribution shifts monotonically with the laser excitation frequency resulting in a nearly constant optical interaction strength across a wide detuning range, while in the other case the previously reported avoidance behavior is actually the result of a nonlinear dependence on the laser excitation frequency near zero detuning leading to switching between two distinct mesoscopic nuclear spin states. The magnitude of the field, which is as large as 400 mT, is measured with sub-100 nuclear spin sensitivity. Stable/unstable points of the OH field distribution are observed, resulting from the non-linear feedback loop in the electron-trion-nuclear system. Nuclear spin polarization state switching occurs between fields differing by 160 mT at least as fast as 25 ms. Control experiments indicate that the strain-induced quadrupolar interaction may explain the measured OH fields.

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.

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.

A strong, far-detuned laser can shift the energy levels of an optically active quantum system via the AC Stark effect. We demonstrate that the polarization of the laser results in a spin-selective modification to the energy structure of a charged quantum dot, shifting one spin manifold but not the other. An additional shift occurs due to the Overhauser field of the nuclear spins, which are pumped into a partially polarized state. This mechanism offers a potentially rapid, reversible, and coherent control of the energy structure and polarization selection rules of a charged quantum dot., Comment: 5 pages, 4 figures

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 HfO$_{2}$ 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 $\mu $m. 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.

Due to their ability to strongly modify the local electromagnetic (EM) field through the excitation of surface plasmon polaritons (SPPs), plasmonic nanostructures have been often used to reshape the emission direction and enhance the radiative decay rate of quantum emitters, such as semiconductor quantum dots (QDs). These features are essential for quantum information processing, nanoscale photonic circuitry and optoelectronics. However, the modification and enhancement demonstrated thus far often drastically alter the local energy density of the emitters, and hence their intrinsic properties, leaving little room for active control. Here, we demonstrate dynamic tuning of the energy states of a single semiconductor QD by optically modifying its local dielectric environment with a nearby plasmonic structure, instead of directly coupling it to the QD. This method leaves the original intrinsic optical properties of the QD intact, enabling the opportunity of tuning its optical properties in real time. This capability is highly desired in applications requiring ultrafast switching and modulation mechanisms., Comment: manuscript + supplemental information

Generation and manipulation of the quantum state of a single photon is at the heart of many quantum information protocols. There has been growing interest in using phase modulators as quantum optics devices that preserve coherence. In this Letter, we have used an electro-optic phase modulator to shape the state vector of single photons emitted by a quantum dot to generate new frequency components (modes) and explicitly demonstrate that the phase modulation process agrees with the theoretical prediction at a single photon level. Through two-photon interference measurements we show that for an output consisting of three modes (the original mode and two sidebands), the indistinguishability of the mode engineered photon, measured through the secondorder intensity correlation (g2(0)) is preserved. This work demonstrates a robust means to generate a photonic qubit or more complex state (e.g., a qutrit) for quantum communication applications by encoding information in the sidebands without the loss of coherence.

We demonstrate the extension of coherence between all four two-electron spin ground states of an InAs quantum dot molecule (QDM) via non-local suppression of nuclear spin fluctuations in both constituent quantum dots (QDs), while optically addressing only the upper 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. Lineshape analysis provides the first measurement of the quieting of the Overhauser field distribution correlating with reduced nuclear spin fluctuations., Comment: Supplementary materials can be found on the publication page of our website. http://research.physics.lsa.umich.edu/dst/Publications.html

Solid state quantum emitters have shown strong potential for applications in quantum information, but spectral inhomogeneity of these emitters poses a significant challenge. We address this issue in a cavity-quantum dot system by demonstrating cavity-stimulated Raman spin flip emission. This process avoids populating the excited state of the emitter and generates a photon that is Raman shifted from the laser and enhanced by the cavity. The emission is spectrally narrow and tunable over a range of at least 125 GHz, which is two orders of magnitude greater than the natural linewidth. We obtain the regime in which the Raman emission is spin-dependent, which couples the photon to a long-lived electron spin qubit. This process can enable an efficient, tunable source of indistinguishable photons and deterministic entanglement of distant spin qubits in a photonic crystal quantum network.

Compared to electrons, holes in InAs quantum dots have a significantly weaker hyperfine interaction that leads to less dephasing from nuclear spins. Thus many recent studies have suggested that nuclear spins are unimportant for hole spin dynamics compared to electric field fluctuations. We show that the hole hyperfine interaction can have a strong effect on hole spin coherence measurements through a nuclear feedback effect. The nuclear polarization is generated through a unique process that is dependent on the anisotropy of the hole hyperfine interaction and the coherent precession of nuclear spins, giving rise to strong modulation at the nuclear precession frequency., Comment: 13 pages, 4 figures

A key ingredient for a quantum network is an interface between stationary quantum bits and photons, which act as flying qubits for interactions and communication. Photonic crystal architectures are promising platforms for enhancing the coupling of light to solid state qubits. Quantum dots can be integrated into a photonic crystal, with optical transitions coupling to photons and spin states forming a long-lived quantum memory. Many researchers have now succeeded in coupling these emitters to photonic crystal cavities, but there have been no demonstrations of a functional spin qubit and quantum gates in this environment. Here we have developed a coupled cavity-quantum dot system in which the dot is controllably charged with a single electron. We perform the initialization, rotation and measurement of a single electron spin qubit using laser pulses and find that the cavity can significantly improve these processes.

Monolayer fluctuations in the thickness of a semiconductor quantum well (QW) lead to three types of excitons, located in the narrower, average and thicker regions of the QW, which are clearly resolved in optical spectra. Whether or not these excitons are coherently coupled via Coulomb interactions is a long-standing debate. We demonstrate that different types of disorder in QWs distinctly affects the coherent coupling and that the coupling strength can be quantitatively measured using optical two-dimensional Fourier transform spectroscopy. We prove experimentally and theoretically that in narrow quantum wells the coherent coupling occurs predominantly between excitons residing in the disorder-free areas of the QWs and those residing in the plateau-type disorder. In contrast, excitons localized in the fault-type disorder potentials do not coherently couple to other excitons., Comment: 5 paages, 4 figures, journal submission

Spins confined in quantum dots are a leading candidate for solid-state quantum bits that can be coherently controlled by optical pulses. There are, however, many challenges to developing a scalable multibit information processing device based on spins in quantum dots, including the natural inhomogeneous distribution of quantum dot energy levels, the difficulty of creating all-optical spin manipulation protocols compatible with nondestructive readout, and the substantial electron-nuclear hyperfine interaction-induced decoherence. Here, we present a scalable qubit design and device architecture based on the spin states of single holes confined in a quantum dot molecule. The quantum dot molecule qubit enables a new strategy for optical coherent control with dramatically enhanced wavelength tunability. The use of hole spins allows the suppression of decoherence via hyperfine interactions and enables coherent spin rotations using Raman transitions mediated by a hole-spin-mixed optically excited state. Because the spin mixing is present only in the optically excited state, dephasing and decoherence are strongly suppressed in the ground states that define the qubits and nondestructive readout is possible. We present the qubit and device designs and analyze the wavelength tunability and fidelity of gate operations that can be implemented using this strategy. We then present experimental and theoretical progress toward implementing this design., Comment: 13 pages, 9 figures

Two electron spins in quantum dots coupled through coherent tunneling are generally acknowledged to approximately obey Heisenberg isotropic exchange. This has not been established for two holes. Here we measure the spectra of two holes and of two electrons in two vertically stacked self-assembled InAs quantum dots using optical spectroscopy as a function of electric and magnetic fields. We find that the exchange is approximately isotropic for both systems, but that significant asymmetric contributions, arising from spin-orbit and Zeeman interactions combined with spatial asymmetries, are required to explain large anticrossings and fine-structure energy splittings in the spectra. Asymmetric contributions to the isotropic Hamiltonian for electrons are of the order of a few percent while those for holes are an order of magnitude larger., Comment: 5 pages, 3 figures

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 one second 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.

A single hole spin in a semiconductor quantum dot has emerged as a quantum bit that is potentially superior to an electron spin. A key feature of holes is that they have a greatly reduced hyperfine interaction with nuclear spins, which is one of the biggest difficulties in working with an electron spin. It is now essential to show that holes are viable for quantum information processing by demonstrating fast quantum gates and scalability. To this end we have developed InAs/GaAs quantum dots coupled through coherent tunneling and charged with controlled numbers of holes. We report fast, single qubit gates using a sequence of short laser pulses. We then take the important next step toward scalability of quantum information by optically controlling two interacting hole spins in separate dots., Comment: 5 figures

We review spin properties of semiconductor quantum dots and their effect on optical spectra. Photoluminescence and other types of spectroscopy are used to probe neutral and charged excitons in individual quantum dots with high spectral and spatial resolution. Spectral fine structure and polarization reveal how quantum dot spins interact with each other and with their environment. By taking advantage of the selectivity of optical selection rules and spin relaxation, optical spin pumping of the ground state electron and nuclear spins is achieved. Through such mechanisms, light can be used to process spins for use as a carrier of information.

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 non-destructive measurement. With two-laser transmission spectroscopy we demonstrate both operations simultaneously, something not previously accomplished in a single quantum dot., Comment: Accepted for publication in Phys. Rev. Lett

Coherent population trapping (CPT) refers to the steady-state trapping of population in a coherent superposition of two ground states which are coupled by coherent optical fields to an intermediate state in a three-level atomic system. Recently, CPT has been observed in an ensemble of donor bound spins in GaAs and in single nitrogen vacancy centers in diamond by using a fluorescence technique. Here we report the demonstration of CPT of an electron spin in a single quantum dot (QD) charged with one electron., Comment: to be appeared in Nature Physics