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Register a new userGiant nonlinear optical responses from photon avalanching nanoparticles
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Avalanche phenomena leverage steeply nonlinear dynamics to generate disproportionately high responses from small perturbations and are found in a multitude of events and materials, enabling technologies including optical phase-conjugate imaging, infrared quantum counting, and efficient upconverted lasing. However, the photon avalanching (PA) mechanism underlying these optical innovations has been observed only in bulk materials and aggregates, and typically at cryogenic temperatures, limiting its utility and impact. Here, we report the realization of PA at room temperature in single nanostructures--small, Tm-doped upconverting nanocrystals--and demonstrate their use in superresolution imaging at near-infrared (NIR) wavelengths within spectral windows of maximal biological transparency. Avalanching nanoparticles (ANPs) can be pumped by continuous-wave or pulsed lasers and exhibit all of the defining features of PA. These hallmarks include excitation power thresholds, long rise time at threshold, and a dominant excited-state absorption that is >13,000x larger than ground-state absorption. Beyond the avalanching threshold, ANP emission scales nonlinearly with the 26th power of pump intensity. This enables the realization of photon-avalanche single-beam superresolution imaging (PASSI), achieving sub-70 nm spatial resolution using only simple scanning confocal microscopy and before any computational analysis. Pairing their steep nonlinearity with existing superresolution techniques and computational methods, ANPs allow for imaging with higher resolution and at ca. 100-fold lower excitation intensities than is possible with other probes. The low PA threshold and exceptional photostability of ANPs also suggest their utility in a diverse array of applications including sub-wavelength bioimaging, IR detection, temperature and pressure transduction, neuromorphic computing, and quantum optics.
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Nonlinear optical (NLO) phenomena such as harmonic generation, Kerr, and Pockels effects are of great technological importance for lasers, frequency converters, modulators, switches, etc. Recently, two-dimensional (2D) materials have drawn significant attention due to their strong and unique NLO properties. Here, we describe an efficient first-principles workflow for calculating the quadratic optical response and apply it to 375 non-centrosymmetric semiconductor monolayers from the Computational 2D Materials Database (C2DB). Sorting the non-resonant nonlinearities with respect to bandgap $E_g$ reveals an upper limit proportional to $E_g^{-4}$, which is neatly explained by two distinct generic models. We identify multiple promising candidates with giant nonlinearities and bandgaps ranging from 0.4 to 5 eV, some of which approach the theoretical upper limit and greatly outperform known materials. Our comprehensive library of ab initio NLO spectra for all 375 monolayers is freely available via the C2DB website. We expect this work to pave the way for highly efficient and compact opto-electronic devices based on 2D materials.
The optical properties of some nanomaterials can be controlled by an external magnetic field, providing active functionalities for a wide range of applications, from single-molecule sensing to nanoscale nonreciprocal optical isolation. Materials with broadband tunable magneto-optical response are therefore highly desired for various components in next-generation integrated photonic nanodevices. Concurrently, hyperbolic metamaterials received a lot of attention in the past decade since they exhibit unusual properties that are rarely observed in nature and provide an ideal platform to control the optical response at the nanoscale via careful design of the effective permittivity tensor, surpassing the possibilities of conventional systems. Here, we experimentally study magnetic circular dichroism in a metasurface made of type-II hyperbolic nanoparticles on a transparent substrate. Numerical simulations confirm the experimental findings, and an analytical model is established to explain the physical origin of the observed magneto-optical effects, which can be described in terms of the coupling of fundamental electric and magnetic dipole modes with an external magnetic field. Our system paves the way for the development of nanophotonic active devices combining the benefits of sub-wavelength light manipulation in hyperbolic metamaterials supporting a large density of optical states with the ability to freely tune the magneto-optical response via control over the anisotropic permittivity of the system.
Nonlinear optical (NLO) responses of topological materials are under active research in recent years. Yet by far most studies focused on the bulk properties, whereas the surface effects and the difference between surface and bulk responses have not been systematically studied. In this work, we develop a generic Greens function framework to investigate the surface NLO properties of topological materials. The Greens function framework can naturally incorporate many body effects and can be easily extended to high order NLO responses. Using $rm T_d WTe_2$ as an example, we reveal that the surface can behave disparately from the bulk under light illumination. Remarkably, the shift and circular current on the surface can flow in opposite directions to that in the bulk. Moreover, the light induced spin current on the surface can be orders of magnitude stronger than that in the bulk. We also study the responses under inhomogeneous field and higher order NLO effect, which are all distinct on the surface. These anomalous surface NLO responses suggest that light can be a valuable tool for probing the surface states of topological materials, while on the other hand, the surface effects shall be prudently considered when investigating the optical properties of topological materials.
We predict the simultaneous occurrence of two fundamental phenomena for metal nanoparticles possessing sharp corners: First, the main plasmonic dipolar mode experiences strong red shift with decreasing corner curvature radius; its resonant frequency is controlled by the apex angle of the corner and the normalized (to the particle size) corner curvature. Second, the split-off plasmonic mode experiences strong localization at the corners. Altogether, this paves the way for tailoring of metal nano-structures providing wavelength-selective excitation of localized plasmons and a strong near-field enhancement of linear and nonlinear optical phenomena.
We introduce the concept of nonlinear graphene metasurfaces employing the controllable interaction between a graphene layer and a planar metamaterial. Such hybrid metasurfaces support two types of subradiant resonant modes, asymmetric modes of structured metamaterial elements (metamolecules) and graphene plasmons exhibiting strong mutual coupling and avoided dispersion crossing. High tunability of graphene plasmons facilitates strong interaction between the subradiant modes, modifying the spectral position and lifetime of the associated Fano resonances. We demonstrate that strong resonant interaction, combined with the subwavelength localization of plasmons, leads to the enhanced nonlinear response and high efficiency of the second-harmonic generation.
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