High-Resolution Cryogenic Spectroscopy of Single Molecules in Nanoprinted Crystals.

We perform laser spectroscopy at liquid helium temperatures (T = 2 K) to investigate single dibenzoterrylene (DBT) molecules doped in anthracene crystals of nanoscopic height fabricated by electrohydrodynamic dripping. Using high-resolution fluorescence excitation spectroscopy, we show that zero-phonon lines of single molecules in printed nanocrystals are nearly as narrow as the Fourier-limited transitions observed for the same guest-host system in the bulk. Moreover, the spectral instabilities are comparable to or less than one line width. By recording super-resolution images of DBT molecules and varying the polarization of the excitation beam, we determine the dimensions of the printed crystals and the orientation of the crystals' axes. Electrohydrodynamic printing of organic nano- and microcrystals is of interest for a series of applications, where controlled positioning of quantum emitters with narrow optical transitions is desirable.

Third Harmonic Generation Enhancement and Wavefront Control Using a Local High-Q Metasurface.

High quality factor optical nanostructures provide a great opportunity to enhance nonlinear optical processes such as third harmonic generation. However, the field enhancement in these high quality factor structures is typically accompanied by optical mode nonlocality. As a result, the enhancement of nonlinear processes comes at the cost of their local control as needed for nonlinear wavefront shaping, imaging, and holography. Here we show simultaneous strong enhancement and spatial control over third harmonic generation with a local high-Q metasurface relying on higher-order Mie resonant modes. Our results demonstrate third harmonic generation at an efficiency of up to 3.25 × 10-5, high quality wavefront shaping as illustrated by a third harmonic metalens, and a flatband, angle independent, third harmonic response up to ±11° incident angle. The demonstrated high level of local control and efficient frequency conversion offer promising prospects for realizing novel nonlinear optical devices.

High quality factor metasurfaces for two-dimensional wavefront manipulation.

The strong interaction of light with micro- and nanostructures plays a critical role in optical sensing, nonlinear optics, active optical devices, and quantum optics. However, for wavefront shaping, the required local control over light at a subwavelength scale limits this interaction, typically leading to low-quality-factor optical devices. Here, we demonstrate an avenue towards high-quality-factor wavefront shaping in two spatial dimensions based on all-dielectric higher-order Mie-resonant metasurfaces. We design and experimentally realize transmissive band stop filters, beam deflectors and high numerical aperture radial lenses with measured quality factors in the range of 202-1475 at near-infrared wavelengths. The excited optical mode and resulting wavefront control are both local, allowing versatile operation with finite apertures and oblique illumination. Our results represent an improvement in quality factor by nearly two orders of magnitude over previous localized mode designs, and provide a design approach for a new class of compact optical devices.

Excitonic Beam Steering in an Active van der Waals Metasurface.

Two-dimensional transition metal dichalcogenides (2D TMDCs) are promising candidates for ultrathin active nanophotonic elements due to the strong tunable excitonic resonances that dominate their optical response. Here, we demonstrate dynamic beam steering by an active van der Waals metasurface that leverages large complex refractive index tunability near excitonic resonances in monolayer molybdenum diselenide (MoSe2). Through varying the radiative and nonradiative rates of the excitons, we can dynamically control both the reflection amplitude and phase profiles, resulting in an excitonic phased array metasurface. Our experiments show reflected light steering to angles between -30° and 30° at different resonant wavelengths corresponding to the A exciton and B exciton. This active van der Waals metasurface relies solely on the excitonic resonances of the monolayer MoSe2 material rather than geometric resonances of patterned nanostructures, suggesting the potential to harness the tunability of excitonic resonances for wavefront shaping in emerging photonic applications.

Refractive Index Modulation in Monolayer Molybdenum Diselenide.

Two-dimensional transition metal dichalcogenides are promising candidates for ultrathin light modulators due to their highly tunable excitonic resonances at visible and near-infrared wavelengths. At cryogenic temperatures, large excitonic reflectivity in monolayer molybdenum diselenide (MoSe2) has been shown, but the permittivity and index modulation have not been studied. Here, we demonstrate large gate-tunability of complex refractive index in monolayer MoSe2 by Fermi level modulation and study the doping dependence of the A and B excitonic resonances for temperatures between 4 and 150 K. By tuning the charge density, we observe both temperature- and carrier-dependent epsilon-near-zero response in the permittivity and transition from metallic to dielectric near the A exciton energy. We attribute the dynamic control of the refractive index to the interplay between radiative and non-radiative decay channels that are tuned upon gating. Our results suggest the potential of monolayer MoSe2 as an active material for emerging photonics applications.

Colloidal HgTe Quantum Dot/Graphene Phototransistor with a Spectral Sensitivity Beyond 3 µm.

Infrared light detection enables diverse technologies ranging from night vision to gas analysis. Emerging technologies such as low-cost cameras for self-driving cars require highly sensitive, low-cost photodetector cameras with spectral sensitivities up to wavelengths of 10 µm. For this purpose, colloidal quantum dot (QD) graphene phototransistors offer a viable alternative to traditional technologies owing to inexpensive synthesis and processing of QDs. However, the spectral range of QD/graphene phototransistors is thus far limited to 1.6 µm. Here, HgTe QD/graphene phototransistors with spectral sensitivity up to 3 µm are presented, with specific detectivities of 6 × 108 Jones at a wavelength of 2.5 µm and a temperature of 80 K. Even at kHz light modulation frequencies, specific detectivities exceed 108 Jones making them suitable for fast video imaging. The simple device architecture and QD film patterning in combination with a broad spectral sensitivity manifest an important step toward low-cost, multi-color infrared cameras.

Temperature-Dependent Charge Carrier Transfer in Colloidal Quantum Dot/Graphene Infrared Photodetectors.

Colloidal PbS quantum dot (QD)/graphene hybrid photodetectors are emerging QD technologies for affordable infrared light detectors. By interfacing the QDs with graphene, the photosignal of these detectors is amplified, leading to high responsivity values. While these detectors have been mainly operated at room temperature, low-temperature operation is required for extending their spectral sensitivity beyond a wavelength of 3 µm. Here, we unveil the temperature-dependent response of PbS QD/graphene phototransistors by performing steady-state and time-dependent measurements over a large temperature range of 80-300 K. We find that the temperature dependence of photoinduced charge carrier transfer from the QD layer to graphene is (i) not impeded by freeze-out of the (Schottky-like) potential barrier at low temperatures, (ii) tremendously sensitive to QD surface states (surface oxidation), and (iii) minimally affected by the ligand exposure time and QD layer thickness. Moreover, the specific detectivity of our detectors increases with cooling, with a maximum measured specific detectivity of at least 1010 Jones at a wavelength of 1280 nm and a temperature of 80 K, which is an order of magnitude larger compared to the corresponding room temperature value. The temperature- and gate voltage-dependent characterization presented here constitutes an important step in expanding our knowledge of charge transfer at interfaces of low-dimensional materials and toward the realization of next-generation optoelectronic devices.

A Plasmonic Painter's Method of Color Mixing for a Continuous Red-Green-Blue Palette.

The ability of mixing colors with remarkable results had long been exclusive to the talents of master painters. By finely combining colors in different amounts on the palette, intuitively, they obtain smooth gradients with any given color. Creating such smooth color variations through scattering by the structural patterning of a surface, as opposed to color pigments, has long remained a challenge. Here, we borrow from the painter's approach and demonstrate color mixing generated by an optical metasurface. We propose a single-layer plasmonic color pixel and a method for nanophotonic structural color mixing based on the additive red-green-blue (RGB) color model. The color pixels consist of plasmonic nanorod arrays that generate vivid primary colors and enable independent control of color brightness without affecting chromaticity by simply varying geometric in-plane parameters. By interleaving different nanorod arrays, we combine up to three primary colors on a single pixel. Based on this, two- and three-color mixing is demonstrated, enabling the continuous coverage of a plasmonic RGB color gamut and yielding a palette with a virtually unlimited number of colors. With this multiresonant color pixel, we show the photorealistic printing of color and monochrome images at the nanoscale, with ultrasmooth transitions in color and brightness. Our color-mixing approach can be applied to a broad range of scatterer designs and materials and has the potential to be used for multiwavelength color filters and dynamic photorealistic displays.

Nanoprinting organic molecules at the quantum level.

Organic compounds present a powerful platform for nanotechnological applications. In particular, molecules suitable for optical functionalities such as single photon generation and energy transfer have great promise for complex nanophotonic circuitry due to their large variety of spectral properties, efficient absorption and emission, and ease of synthesis. Optimal integration, however, calls for control over position and orientation of individual molecules. While various methods have been explored for reaching this regime in the past, none satisfies requirements necessary for practical applications. Here, we present direct non-contact electrohydrodynamic nanoprinting of a countable number of photostable and oriented molecules in a nanocrystal host with subwavelength positioning accuracy. We demonstrate the power of our approach by writing arbitrary patterns and controlled coupling of single molecules to the near field of optical nanostructures. Placement precision, high yield and fabrication facility of our method open many doors for the realization of novel nanophotonic devices.

Metasurfaces Leveraging Solar Energy for Icephobicity.

Inhibiting ice accumulation on surfaces is an energy-intensive task and is of significant importance in nature and technology where it has found applications in windshields, automobiles, aviation, renewable energy generation, and infrastructure. Existing methods rely on on-site electrical heat generation, chemicals, or mechanical removal, with drawbacks ranging from financial costs to disruptive technical interventions and environmental incompatibility. Here we focus on applications where surface transparency is desirable and propose metasurfaces with embedded plasmonically enhanced light absorption heating, using ultrathin hybrid metal-dielectric coatings, as a passive, viable approach for de-icing and anti-icing, in which the sole heat source is renewable solar energy. The balancing of transparency and absorption is achieved with rationally nanoengineered coatings consisting of gold nanoparticle inclusions in a dielectric (titanium dioxide), concentrating broadband absorbed solar energy into a small volume. This causes a > 10 °C temperature increase with respect to ambient at the air-solid interface, where ice is most likely to form, delaying freezing, reducing ice adhesion, when it occurs, to negligible levels (de-icing) and inhibiting frost formation (anti-icing). Our results illustrate an effective unexplored pathway toward environmentally compatible, solar-energy-driven icephobicity, enabled by respectively tailored plasmonic metasurfaces, with the ability to design the balance of transparency and light absorption.