On-chip generation and dynamic piezo-optomechanical rotation of single photons.

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.

Sub-nanosecond acousto-electric carrier redistribution dynamics and transport in polytypic GaAs nanowires.

The authors report on a combined structural, optical and acousto-electric study of polytypic GaAs nanowires. Two types of nanowires with different zincblende and wurtzite crystal phase mixing are identified by transmission electron microscopy and photoluminescence spectroscopy. The nanowires exhibit characteristic recombination channels which are assigned to different types of spatially direct recombination (electron and hole within the same crystal phase segment) and spatially indirect recombination (electron and holes localized in different segments). Contact-free acousto-optoelectric spectroscopy is employed to resolve spatiotemporal charge carrier dynamics between different recombination channels induced by a piezoelectric surface acoustic wave. The observed suppression of the emission and its dynamic temporal modulation shows unambiguous fingerprints of the local bandedge variations induced by the crystal phase mixing. A nanowire, which exhibits a variation from a near-pristine zinc blende crystal structure to a highly mixed crystal phase, shows a clear dependence on the propagation direction of the acoustic wave. In contrast, no pronounced directionality is found for a nanowire with an extended near-pristine zincblende segment. The experimental findings are corroborated by solving the drift and diffusion equations of electrons and holes induced by the surface acoustic wave. The key characteristics observed in our experimental data are well reproduced in the numerical simulations by assuming two general bandedge modulations and realistic parameters for the bandedge discontinuities and transport mobilities of electrons and holes. This evidences that even all relevant physical processes are accounted for in the model.

Ultrafast electron cycloids driven by the transverse spin of a surface acoustic wave.

Spin-momentum locking is a universal wave phenomenon promising for applications in electronics and photonics. In acoustics, Lord Rayleigh showed that surface acoustic waves exhibit a characteristic elliptical particle motion strikingly similar to spin-momentum locking. Although these waves have become one of the few phononic technologies of industrial relevance, the observation of their transverse spin remained an open challenge. Here, we observe the full spin dynamics by detecting ultrafast electron cycloids driven by the gyrating electric field produced by a surface acoustic wave propagating on a slab of lithium niobate. A tubular quantum well wrapped around a nanowire serves as an ultrafast sensor tracking the full cyclic motion of electrons. Our acousto-optoelectrical approach opens previously unknown directions in the merged fields of nanoacoustics, nanophotonics, and nanoelectronics for future exploration.

Real-Time Electron and Hole Transport Dynamics in Halide Perovskite Nanowires.

For optoelectronic devices, high transport mobilities of electrons and holes are desirable, which, moreover, should be close to identical. Acousto-optoelectric spectroscopy is employed to probe the spatiotemporal dynamics of both electrons and holes inside CsPbI3 nanowires. These dynamics are induced without the need for electrical contacts simply by the piezoelectric field of a surface acoustic wave. Its radio frequency of fSAW = 324 MHz natively avoids spurious contributions from ion migration typically occurring in these materials. The observed dynamic modulation of the photoluminescence is faithfully reproduced by solving the drift and diffusion currents of electrons and holes induced by the surface acoustic wave. These calculations confirm that the mobilities of electrons and holes are equal and quantify them to be µe = µh = 3 ± 1 cm2 V-1 s-1. Additionally, carrier loss due to surface recombination is shown to be largely suppressed in CsPbI3 nanowires. Both findings mark significant advantages over traditional compound semiconductors, in particular, GaAs, for applications in future optoelectronic and photovoltaic devices. The demonstrated sublifetime modulation of the optical emission may find direct application in switchable perovskite light-emitting devices employing mature surface acoustic wave technology.

Breakdown of Corner States and Carrier Localization by Monolayer Fluctuations in Radial Nanowire Quantum Wells.

We report a comprehensive study of the impact of the structural properties in radial GaAs-Al0.3Ga0.7As nanowire-quantum well heterostructures on the optical recombination dynamics and electrical transport properties, emphasizing particularly the role of the commonly observed variations of the quantum well thickness at different facets. Typical thickness fluctuations of the radial quantum well observed by transmission electron microscopy lead to pronounced localization. Our optical data exhibit clear spectral shifts and a multipeak structure of the emission for such asymmetric ring structures resulting from spatially separated, yet interconnected quantum well systems. Charge carrier dynamics induced by a surface acoustic wave are resolved and prove efficient carrier exchange on native, subnanosecond time scales within the heterostructure. Experimental findings are corroborated by theoretical modeling, which unambiguously show that electrons and holes localize on facets where the quantum well is the thickest and that even minute deviations of the perfect hexagonal shape strongly perturb the commonly assumed 6-fold symmetric ground state.

Scalable and Transfer-Free Fabrication of MoS2/SiO2 Hybrid Nanophotonic Cavity Arrays with Quality Factors Exceeding 4000.

We report the fully-scalable fabrication of a large array of hybrid molybdenum disulfide (MoS2) - silicon dioxide (SiO2) one-dimensional, free-standing photonic-crystal cavities capable of enhancement of the MoS2 photoluminescence at the narrow cavity resonance. We demonstrate continuous tunability of the cavity resonance wavelength across the entire emission band of MoS2 simply by variation of the photonic crystal periodicity. Device fabrication started by substrate-scale growth of MoS2 using chemical vapor deposition (CVD) on non-birefringent thermal oxide on a silicon wafer; it was followed by lithographic fabrication of a photonic crystal nanocavity array on the same substrate at more than 50% yield of functional devices. Our cavities exhibit three dominant modes with measured linewidths less than 0.2 nm, corresponding to quality factors exceeding 4000. All experimental findings are found to be in excellent agreement with finite difference time domain (FDTD) simulations. CVD MoS2 provides scalable access to a direct band gap, inorganic, stable and efficient emitter material for on-chip photonics without the need for epitaxy and is at CMOS compatible processing parameters even for back-end-of-line integration; our findings suggest feasibility of cavity based line-narrowing in MoS2-based on-chip devices as it is required for instance for frequency-multiplexed operation in on-chip optical communication and sensing.

Thermochromic modulation of surface plasmon polaritons in vanadium dioxide nanocomposites.

We propose and implement a new concept for thermochromic plasmonic elements. It is based on vanadium dioxide (VO2) nanocrystals located in the near field of surface plasmon polaritons supported by an otherwise unstructured gold thin film. When the VO2 undergoes the metal-insulator phase transition, the coupling conditions for conversion of light into propagating surface plasmon polaritons change markedly. In particular, we realize thermochromic plasmonic grating couplers with substantial switching contrast as well as tunable plasmonic couplers in a Kretschmann configuration. The use of VO2 nanocrystals permits highly repetitive switching and room temperature operation. Simulations based on the actual dielectric function of our VO2 nanocrystals agree well with the experiment.

Dynamic acousto-optic control of a strongly coupled photonic molecule.

Strongly confined photonic modes can couple to quantum emitters and mechanical excitations. To harness the full potential in quantum photonic circuits, interactions between different constituents have to be precisely and dynamically controlled. Here, a prototypical coupled element, a photonic molecule defined in a photonic crystal membrane, is controlled by a radio frequency surface acoustic wave. The sound wave is tailored to deliberately switch on and off the bond of the photonic molecule on sub-nanosecond timescales. In time-resolved experiments, the acousto-optically controllable coupling is directly observed as clear anticrossings between the two nanophotonic modes. The coupling strength is determined directly from the experimental data. Both the time dependence of the tuning and the inter-cavity coupling strength are found to be in excellent agreement with numerical calculations. The demonstrated mechanical technique can be directly applied for dynamic quantum gate operations in state-of-the-art-coupled nanophotonic, quantum cavity electrodynamic and optomechanical systems.

Scalable fabrication of a hybrid field-effect and acousto-electric device by direct growth of monolayer MoS2/LiNbO3.

Lithium niobate is the archetypical ferroelectric material and the substrate of choice for numerous applications including surface acoustic wave radio frequencies devices and integrated optics. It offers a unique combination of substantial piezoelectric and birefringent properties, yet its lack of optical activity and semiconducting transport hamper application in optoelectronics. Here we fabricate and characterize a hybrid MoS2/LiNbO3 acousto-electric device via a scalable route that uses millimetre-scale direct chemical vapour deposition of MoS2 followed by lithographic definition of a field-effect transistor structure on top. The prototypical device exhibits electrical characteristics competitive with MoS2 devices on silicon. Surface acoustic waves excited on the substrate can manipulate and probe the electrical transport in the monolayer device in a contact-free manner. We realize both a sound-driven battery and an acoustic photodetector. Our findings open directions to non-invasive investigation of electrical properties of monolayer films.

Alloy Fluctuations Act as Quantum Dot-like Emitters in GaAs-AlGaAs Core-Shell Nanowires.

GaAs-AlxGa1-xAs (AlGaAs) core-shell nanowires show great promise for nanoscale electronic and optoelectronic devices, but the application of these nonplanar heterostructures in devices requires improved understanding and control of nanoscale alloy composition and interfaces. Multiple researchers have observed sharp emission lines of unknown origin below the AlGaAs band edge in photoluminescence (PL) spectra of core-shell nanowires; point defects, alloy composition fluctuations, and self-assembled quantum dots have been put forward as candidate structures. Here we employ laser-assisted atom probe tomography to reveal structural and compositional features that give rise to the sharp PL emission spectra. Nanoscale ellipsoidal Ga-enriched clusters resulting from random composition fluctuations are identified in the AlGaAs shell, and their compositions, size distributions, and interface characteristics are analyzed. Simulations of exciton transition energies in ellipsoidal quantum dots are used to relate the Ga nanocluster distribution with the distribution of sharp PL emission lines. We conclude that the Ga rich clusters can act as discrete emitters provided that the major diameter is ≥4 nm. Smaller clusters are under-represented in the PL spectrum, and spectral lines of larger clusters are broadened, due to quantum tunneling between clusters.

Fourier synthesis of radiofrequency nanomechanical pulses with different shapes.

The concept of Fourier synthesis is heavily used in both consumer electronic products and fundamental research. In the latter, pulse shaping is key to dynamically initializing, probing and manipulating the state of classical or quantum systems. In NMR, for instance, shaped pulses have a long-standing tradition and the underlying fundamental concepts have subsequently been successfully extended to optical frequencies and even to the implementation of quantum gate operations. Transferring these paradigms to nanomechanical systems requires tailored nanomechanical waveforms. Here, we report on an additive Fourier synthesizer for nanomechanical waveforms based on monochromatic surface acoustic waves. As a proof of concept, we electrically synthesize four different elementary nanomechanical waveforms from a fundamental surface acoustic wave at f1 ≈ 150 MHz using a superposition of up to three discrete harmonics. We use these shaped pulses to interact with an individual sensor quantum dot and detect their deliberately and temporally modulated strain component via the optomechanical quantum dot response. Importantly, and in contrast to direct mechanical actuation by bulk piezoactuators, surface acoustic waves provide much higher frequencies (>20 GHz; ref. 10) to resonantly drive mechanical motion. Thus, our technique uniquely allows coherent mechanical control of localized vibronic modes of optomechanical crystals, even in the quantum limit when cooled to the vibrational ground state.

Time-resolved coherent X-ray diffraction imaging of surface acoustic waves.

Time-resolved coherent X-ray diffraction experiments of standing surface acoustic waves, illuminated under grazing incidence by a nanofocused synchrotron beam, are reported. The data have been recorded in stroboscopic mode at controlled and varied phase between the acoustic frequency generator and the synchrotron bunch train. At each time delay (phase angle), the coherent far-field diffraction pattern in the small-angle regime is inverted by an iterative algorithm to yield the local instantaneous surface height profile along the optical axis. The results show that periodic nanoscale dynamics can be imaged at high temporal resolution in the range of 50 ps (pulse length).

Dynamic acoustic control of individual optically active quantum dot-like emission centers in heterostructure nanowires.

We probe and control the optical properties of emission centers forming in radial heterostructure GaAs-Al0.3Ga0.7As nanowires and show that these emitters, located in Al0.3Ga0.7As layers, can exhibit quantum-dot like characteristics. We employ a radio frequency surface acoustic wave to dynamically control their emission energy, and occupancy state on a nanosecond time scale. In the spectral oscillations, we identify unambiguous signatures arising from both the mechanical and electrical component of the surface acoustic wave. In addition, different emission lines of a single emission center exhibit pronounced anticorrelated intensity oscillations during the acoustic cycle. These arise from a dynamically triggered carrier extraction out of the emission center to a continuum in the radial heterostructure. Using finite element modeling and Wentzel-Kramers-Brillouin theory we identify quantum tunneling as the underlying mechanism. These simulation results quantitatively reproduce the observed switching and show that in our systems these emission centers are spatially separated from the continuum by >10.5 nm.

Site-selective ion beam synthesis and optical properties of individual CdSe nanocrystal quantum dots in a SiO2 matrix.

Cadmium selenide nanocrystal quantum dots (NC-QDs) are site-selectively synthesized by sequential ion beam implantation of selenium and cadmium ions in a SiO2 matrix through submicrometer apertures followed by a rapid thermal annealing step. The structural and optical properties of the NC-QDs are controlled by the ion fluence during implantation and the diameter of the implantation aperture. For low fluences and small apertures the emission of these optically active emitters is blue-shifted compared to that of the bulk material by >100 meV due to quantum confinement. The emission exhibits spectral diffusion and blinking on a second time scales as established also for solution-synthesized NC-QDs.

Surface acoustic wave mediated carrier injection into individual quantum post nano emitters.

Acousto-electric charge conveyance induced by a surface acoustic wave (SAW) is employed to dissociate photogenerated excitons. Over macroscopic distances, both electrons and holes are injected sequentially into a remotely positioned, isolated and high quality quantum emitter, a self-assembled quantum post. This process is found to be highly efficient and to exhibit improved stability at high acoustic powers when compared to direct optical pumping at the position of the quantum post. These characteristics are attributed to the wide matrix quantum well in which charge conveyance occurs and to the larger number of carriers available for injection in the remote configuration, respectively. The emission of such pumped quantum posts is dominated by recombination of neutral excitons and fully directional when the propagation direction of the SAW and the position of the quantum post are reversed.

Quantitative excited state spectroscopy of a single InGaAs quantum dot molecule through multi-million-atom electronic structure calculations.

Atomistic electronic structure calculations are performed to study the coherent inter-dot couplings of the electronic states in a single InGaAs quantum dot molecule. The experimentally observed excitonic spectrum by Krenner et al (2005) Phys. Rev. Lett. 94 057402 is quantitatively reproduced, and the correct energy states are identified based on a previously validated atomistic tight binding model. The extended devices are represented explicitly in space with 15-million-atom structures. An excited state spectroscopy technique is applied where the externally applied electric field is swept to probe the ladder of the electronic energy levels (electron or hole) of one quantum dot through anti-crossings with the energy levels of the other quantum dot in a two-quantum-dot molecule. This technique can be used to estimate the spatial electron-hole spacing inside the quantum dot molecule as well as to reverse engineer quantum dot geometry parameters such as the quantum dot separation. Crystal-deformation-induced piezoelectric effects have been discussed in the literature as minor perturbations lifting degeneracies of the electron excited (P and D) states, thus affecting polarization alignment of wavefunction lobes for III-V heterostructures such as single InAs/GaAs quantum dots. In contrast, this work demonstrates the crucial importance of piezoelectricity to resolve the symmetries and energies of the excited states through matching the experimentally measured spectrum in an InGaAs quantum dot molecule under the influence of an electric field. Both linear and quadratic piezoelectric effects are studied for the first time for a quantum dot molecule and demonstrated to be indeed important. The net piezoelectric contribution is found to be critical in determining the correct energy spectrum, which is in contrast to recent studies reporting vanishing net piezoelectric contributions.

Directional and dynamic modulation of the optical emission of an individual GaAs nanowire using surface acoustic waves.

We report on optical experiments performed on individual GaAs nanowires and the manipulation of their temporal emission characteristics using a surface acoustic wave. We find a pronounced, characteristic suppression of the emission intensity for the surface acoustic wave propagation aligned with the axis of the nanowire. Furthermore, we demonstrate that this quenching is dynamical as it shows a pronounced modulation as the local phase of the surface acoustic wave is tuned. These effects are strongly reduced for a surface acoustic wave applied in the direction perpendicular to the axis of the nanowire due to their inherent one-dimensional geometry. We resolve a fully dynamic modulation of the nanowire emission up to 678 MHz not limited by the physical properties of the nanowires.

Enhanced sequential carrier capture into individual quantum dots and quantum posts controlled by surface acoustic waves.

Individual self-assembled quantum dots and quantum posts are studied under the influence of a surface acoustic wave. In optical experiments we observe an acoustically induced switching of the occupancy of the nanostructures along with an overall increase of the emission intensity. For quantum posts, switching occurs continuously from predominantly charged excitons (dissimilar number of electrons and holes) to neutral excitons (same number of electrons and holes) and is independent of whether the surface acoustic wave amplitude is increased or decreased. For quantum dots, switching is nonmonotonic and shows a pronounced hysteresis on the amplitude sweep direction. Moreover, emission of positively charged and neutral excitons is observed at high surface acoustic wave amplitudes. These findings are explained by carrier trapping and localization in the thin and disordered two-dimensional wetting layer on top of which quantum dots nucleate. This limitation can be overcome for quantum posts where acoustically induced charge transport is highly efficient in a wide lateral matrix-quantum well.