Polarization Dynamics of Solid-State Quantum Emitters.

Quantum emitters in solid-state crystals have recently attracted a great deal of attention due to their simple applicability in optical quantum technologies. The polarization of single photons generated by quantum emitters is one of the key parameters that plays a crucial role in various applications, such as quantum computation, which uses the indistinguishability of photons. However, the degree of single-photon polarization is typically quantified using the time-averaged photoluminescence intensity of single emitters, which provides limited information about the dipole properties in solids. In this work, we use single defects in hexagonal boron nitride and nanodiamond as efficient room-temperature single-photon sources to reveal the origin and temporal evolution of the dipole orientation in solid-state quantum emitters. The angles of the excitation and emission dipoles relative to the crystal axes were determined experimentally and then calculated using density functional theory, which resulted in characteristic angles for every specific defect that can be used as an efficient tool for defect identification and understanding their atomic structure. Moreover, the temporal polarization dynamics revealed a strongly modified linear polarization visibility that depends on the excited-state decay time of the individual excitation. This effect can potentially be traced back to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further improve the performance of polarization-sensitive experiments, particularly that for quantum communication with single-photon emitters.

Sol-Gel Barium Titanate Nanohole Array as a Nonlinear Metasurface and a Photonic Crystal.

The quest of a nonlinear optical material that can be easily nanostructured over a large surface area is still ongoing. Here, we demonstrate a nanoimprinted nonlinear barium titanate 2D nanohole array that shows the optical properties of a 2D photonic crystal and a metasurface, depending on the direction of the optical axis. The challenge of nanostructuring the inert metal-oxide is resolved by direct soft nanoimprint lithography with sol-gel derived barium titanate enabling critical dimensions of 120 nm with aspect ratios of five. The nanohole array exhibits a photonic bandgap in the infrared range when probed along the slab axis, while lattice resonant states are observed in out-of-plane transmission configuration. The enhanced light-matter interaction from the resonant structure enables to increase in the second-harmonic generation in the near-ultraviolet by a factor of 18 illustrating the potential in the flexible fabrication technique for barium titanate photonic devices.

Background-Free Near-Infrared Biphoton Emission from Single GaAs Nanowires.

The generation of photon pairs from nanoscale structures with high rates is still a challenge for the integration of quantum devices, as it suffers from parasitic signals from the substrate. In this work, we report type-0 spontaneous parametric down-conversion at 1550 nm from individual bottom-up grown zinc-blende GaAs nanowires with lengths of up to 5 µm and diameters of up to 450 nm. The nanowires were deposited on a transparent ITO substrate, and we measured a background-free coincidence rate of 0.05 Hz in a Hanbury-Brown-Twiss setup. Taking into account transmission losses, the pump fluence, and the nanowire volume, we achieved a biphoton generation of 60 GHz/Wm, which is at least 3 times higher than that of previously reported single nonlinear micro- and nanostructures. We also studied the correlations between the second-harmonic generation and the spontaneous parametric down-conversion intensities with respect to the pump polarization and in different individual nanowires.

Second-harmonic generation tuning by stretching arrays of GaAs nanowires.

We present a wearable device with III-V nanowires in a flexible polymer, which is used for active mechanical tuning of the second-harmonic generation intensity. An array of vertical GaAs nanowires was grown with metalorganic vapour-phase epitaxy, then embedded in polydimethylsiloxane and detached from the rigid substrate with mechanical peel off. Experimental results show a tunability of the second-harmonic generation intensity by a factor of two for 30% stretching which matches the simulations including the distribution of sizes. We studied the impact of different parameters on the band dispersion and tunability of the second-harmonic generation, such as the pitch, the length, and the diameter. We predict at least three orders of magnitude active mechanical tuning of the nonlinear signal intensity for nanowire arrays. The flexibility of the array together with the resonant wavelength engineering make such structures perspective platforms for future bendable or stretchable nanophotonic devices as light sources or sensors.

Gallium Phosphide Nanowires in a Free-Standing, Flexible, and Semitransparent Membrane for Large-Scale Infrared-to-Visible Light Conversion.

Engineering of nonlinear optical response in nanostructures is one of the key topics in nanophotonics, as it allows for broad frequency conversion at the nanoscale. Nevertheless, the application of the developed designs is limited by either high cost of their manufacturing or low conversion efficiencies. This paper reports on the efficient second-harmonic generation in a free-standing GaP nanowire array encapsulated in a polymer membrane. Light coupling with optical resonances and field confinement in the nanowires together with high nonlinearity of GaP material yield a strong second-harmonic signal and efficient near-infrared (800-1200 nm) to visible upconversion. The fabricated nanowire-based membranes demonstrate high flexibility and semitransparency for the incident infrared radiation, allowing utilizing them for infrared imaging, which can be easily integrated into different optical schemes without disturbing the visualized beam.

Forward and Backward Switching of Nonlinear Unidirectional Emission from GaAs Nanoantennas.

High-index III-V semiconductor nanoantennas have gained great attention for enhanced nonlinear light-matter interactions, in the past few years. However, the complexity of nonlinear emission profiles imposes severe constraints on practical applications, such as in optical communications and integrated optoelectronic devices. These complexities include the lack of unidirectional nonlinear emission and the severe challenges in switching between forward and backward emissions, due to the structure of the susceptibility tensor of the III-V nanoantennas. Here, we propose a solution to both issues via engineering the nonlinear tensor of the nanoantennas. The special nonlinear tensorial properties of zinc-blende material can be used to engineer the nonlinear characteristics via growing the nanoantennas along different crystalline orientations. Based on the nonlinear multipolar effect, we have designed and fabricated (110)-grown GaAs nanoantennas, with engineered tensorial properties, embedded in a transparent low-index material. Our technique provides an approach not only for unidirectional second-harmonic generation (SHG) forward or backward emission but also for switching from one to another. Importantly, switching the SHG emission directionality is obtained only by rotating the polarization of the incident light, without the need for physical variation of the antennas or the environment. This characteristic is an advantage, as compared to other nonlinear nanoantennas, including (100)- and (111)-grown III-V counterparts or silicon and germanium nanoantennas. Indeed, (110)-GaAs nanoantennas allow for engineering the nonlinear nanophotonic systems including nonlinear "Huygens metasurfaces" and offer exciting opportunities for various nonlinear nanophotonics technologies, such as nanoscale light routing and light sources, as well as multifunctional flat optical elements.

Image-based autofocusing system for nonlinear optical microscopy with broad spectral tuning.

We present an image-based autofocusing system applied in nonlinear microscopy and spectroscopy with a wide range of excitation wavelengths. The core of the developed autofocusing system consists of an adapted two-step procedure maximizing an image score with six different image scorings algorithms implemented to cover different types of focusing scenarios in automated regime for broad wavelength region. The developed approach is combined with an automated multi-axis alignment procedure. We demonstrate the key abilities of the autofocusing procedure on different types of structures: single nanoparticles, nanowires and complex 3D nanostructures. Based on these experiments, we determine the optimal autofocusing algorithms for different types of structures and applications.