Ferroelectric Modulation of Quantum Emitters in Monolayer WS2.

Quantum photonics promises significant advances in secure communications, metrology, sensing, and information processing/computation. Single-photon sources are fundamental to this endeavor. However, the lack of high-quality single photon sources remains a significant obstacle. We present here a paradigm for the control of single photon emitters (SPEs) and single photon purity by integrating monolayer WS2 with the organic ferroelectric polymer poly(vinylidene fluoride-co-trifluoroethylene) (P(VDF-TrFE)). We demonstrate that the ferroelectric domains in the P(VDF-TrFE) film control the purity of single photon emission from the adjacent WS2. By switching the ferroelectric polarization, we reversibly tune the single photon purity between the semiclassical and quantum light regimes, with single photon purities as high as 94%. This demonstrates a method for modulating and encoding quantum photonic information, complementing more complex approaches. This multidimensional heterostructure introduces an approach for control of quantum emitters by combining the nonvolatile ferroic properties of a ferroelectric with the radiative properties of the zero-dimensional atomic-scale emitters embedded in the two-dimensional WS2 semiconductor monolayer.

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.

Enabling remote quantum emission in 2D semiconductors via porous metallic networks.

Here we report how two-dimensional crystal (2DC) overlayers influence the recrystallization of relatively thick metal films and the subsequent synergetic benefits this provides for coupling surface plasmon-polaritons (SPPs) to photon emission in 2D semiconductors. We show that annealing 2DC/Au films on SiO2 results in a reverse epitaxial process where initially nanocrystalline Au films gain texture, crystallographically orient with the 2D crystal overlayer, and form an oriented porous metallic network (OPEN) structure in which the 2DC can suspend above or coat the inside of the metal pores. Both laser excitation and exciton recombination in the 2DC semiconductor launch propagating SPPs in the OPEN film. Energy in-/out- coupling occurs at metal pore sites, alleviating the need for dielectric spacers between the metal and 2DC layer. At low temperatures, single-photon emitters (SPEs) are present across an OPEN-WSe2 film, and we demonstrate remote SPP-mediated excitation of SPEs at a distance of 17 µm.

Optical charge state control of spin defects in 4H-SiC.

Defects in silicon carbide (SiC) have emerged as a favorable platform for optically active spin-based quantum technologies. Spin qubits exist in specific charge states of these defects, where the ability to control these states can provide enhanced spin-dependent readout and long-term charge stability. We investigate this charge state control for two major spin qubits in 4H-SiC, the divacancy and silicon vacancy, obtaining bidirectional optical charge conversion between the bright and dark states of these defects. We measure increased photoluminescence from divacancy ensembles by up to three orders of magnitude using near-ultraviolet excitation, depending on the substrate, and without degrading the electron spin coherence time. This charge conversion remains stable for hours at cryogenic temperatures, allowing spatial and persistent patterning of the charge state populations. We develop a comprehensive model of the defects and optical processes involved, offering a strong basis to improve material design and to develop quantum applications in SiC.

Helicity dependent photocurrent in electrically gated (Bi1-x Sb x )2Te3 thin films.

Circularly polarized photons are known to generate a directional helicity-dependent photocurrent in three-dimensional topological insulators at room temperature. Surprisingly, the phenomenon is readily observed at photon energies that excite electrons to states far above the spin-momentum locked Dirac cone and the underlying mechanism for the helicity-dependent photocurrent is still not understood. Here we show a comprehensive study of the helicity-dependent photocurrent in (Bi1-x Sb x )2Te3 thin films as a function of the incidence angle of the optical excitation, its wavelength and the gate-tuned chemical potential. Our observations allow us to unambiguously identify the circular photo-galvanic effect as the dominant mechanism for the helicity-dependent photocurrent. Additionally, we use an analytical model to relate the directional nature of the photocurrent to asymmetric optical transitions between the topological surface states and bulk bands. The insights we obtain are important for engineering opto-spintronic devices that rely on optical steering of spin and charge currents.

Local optical control of ferromagnetism and chemical potential in a topological insulator.

Many proposed experiments involving topological insulators (TIs) require spatial control over time-reversal symmetry and chemical potential. We demonstrate reconfigurable micron-scale optical control of both magnetization (which breaks time-reversal symmetry) and chemical potential in ferromagnetic thin films of Cr-(Bi,Sb)2Te3 grown on SrTiO3 By optically modulating the coercivity of the films, we write and erase arbitrary patterns in their remanent magnetization, which we then image with Kerr microscopy. Additionally, by optically manipulating a space charge layer in the underlying SrTiO3 substrates, we control the local chemical potential of the films. This optical gating effect allows us to write and erase p-n junctions in the films, which we study with photocurrent microscopy. Both effects are persistent and may be patterned and imaged independently on a few-micron scale. Dynamic optical control over both magnetization and chemical potential of a TI may be useful in efforts to understand and control the edge states predicted at magnetic domain walls in quantum anomalous Hall insulators.

Persistent optical gating of a topological insulator.

The spin-polarized surface states of topological insulators (TIs) are attractive for applications in spintronics and quantum computing. A central challenge with these materials is to reliably tune the chemical potential of their electrons with respect to the Dirac point and the bulk bands. We demonstrate persistent, bidirectional optical control of the chemical potential of (Bi,Sb)2Te3 thin films grown on SrTiO3. By optically modulating a space-charge layer in the SrTiO3 substrates, we induce a persistent field effect in the TI films comparable to electrostatic gating techniques but without additional materials or processing. This enables us to optically pattern arbitrarily shaped p- and n-type regions in a TI, which we subsequently image with scanning photocurrent microscopy. The ability to optically write and erase mesoscopic electronic structures in a TI may aid in the investigation of the unique properties of the topological insulating phase. The gating effect also generalizes to other thin-film materials, suggesting that these phenomena could provide optical control of chemical potential in a wide range of ultrathin electronic systems.