Aluminum nanocrystals (AlNCs) are of increasing interest as sustainable, earth-abundant nanoparticles for visible wavelength plasmonics and as versatile nanoantennas for energy-efficient plasmonic photocatalysis. Here, we show that annealing AlNCs under various gases and thermal conditions induces substantial, systematic changes in their surface oxide, modifying crystalline phase, surface morphology, density, and defect type and concentration. Tailoring the surface oxide properties enables AlNCs to function as all-aluminum-based antenna-reactor plasmonic photocatalysts, with the modified surface oxides providing varying reactivities and selectivities for several chemical reactions.
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Free, publicly-accessible full text available March 12, 2025
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For the conversion of CO 2 into fuels and chemical feedstocks, hybrid gas/liquid-fed electrochemical flow reactors provide advantages in selectivity and production rates over traditional liquid phase reactors. However, fundamental questions remain about how to optimize conditions to produce desired products. Using an alkaline electrolyte to suppress hydrogen formation and a gas diffusion electrode catalyst composed of copper nanoparticles on carbon nanospikes, we investigate how hydrocarbon product selectivity in the CO 2 reduction reaction in hybrid reactors depends on three experimentally controllable parameters: (1) supply of dry or humidified CO 2 gas, (2) applied potential, and (3) electrolyte temperature. Changing from dry to humidified CO 2 dramatically alters product selectivity from C 2 products ethanol and acetic acid to ethylene and C 1 products formic acid and methane. Water vapor evidently influences product selectivity of reactions that occur on the gas-facing side of the catalyst by adding a source of protons that alters reaction pathways and intermediates.more » « less
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Abstract The synergy between topology and non-Hermiticity in photonics holds immense potential for next-generation optical devices that are robust against defects. However, most demonstrations of non-Hermitian and topological photonics have been limited to super-wavelength scales due to increased radiative losses at the deep-subwavelength scale. By carefully designing radiative losses at the nanoscale, we demonstrate a non-Hermitian plasmonic–dielectric metasurface in the visible with non-trivial topology. The metasurface is based on a fourth order passive parity-time symmetric system. The designed device exhibits an exceptional concentric ring in its momentum space and is described by a Hamiltonian with a non-Hermitian Z 3 ${\mathbb{Z}}_{3}$ topological invariant of V = −1. Fabricated devices are characterized using Fourier-space imaging for single-shot k -space measurements. Our results demonstrate a way to combine topology and non-Hermitian nanophotonics for designing robust devices with novel functionalities.more » « less
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Abstract Hybrid light–matter coupled states, or polaritons, in magnetic materials have attracted significant attention due to their potential for enabling novel applications in spintronics and quantum information processing. However, most magnon‐polariton studies in the strong coupling regime to date have been carried out for ferromagnetic materials with magnon excitations at gigahertz frequencies. Here, strong resonant photon–magnon coupling at frequencies above 1 terahertz is investigated for the first time in a prototypical room‐temperature antiferromagnetic insulator, NiO, inside a Fabry–Pérot cavity. The cavity is formed by the crystal itself with a thickness adjusted to an optimal value. Terahertz time‐domain spectroscopy measurements in magnetic fields up to 25 T reveal the evolution of the magnon frequency through Fabry–Pérot cavity modes with photon–magnon anticrossing behavior, demonstrating clear vacuum Rabi splittings exceeding the polariton linewidths. These results show that NiO is a promising platform for exploring antiferromagnetic spintronics and cavity magnonics in the terahertz frequency range.
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The terahertz region of the electromagnetic spectrum has been the least utilized owing to inadequacies of available sources. We introduce a compact, widely frequency-tunable, extremely bright source of terahertz radiation: a gas-phase molecular laser based on rotational population inversions optically pumped by a quantum cascade laser. By identifying the essential parameters that determine the suitability of a molecule for a terahertz laser, almost any rotational transition of almost any molecular gas can be made to lase. Nitrous oxide is used to illustrate the broad tunability over 37 lines spanning 0.251 to 0.955 terahertz, each with kilohertz linewidths. Our analysis shows that laser lines spanning more than 1 terahertz with powers greater than 1 milliwatt are possible from many molecular gases pumped by quantum cascade lasers.