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Raman scattering is sensitive to local temperature and thus offers a convenient tool for non-contact and non-destructive optical thermometry at the nanoscale. In turn, all-dielectric nanostructures, such as silicon particles, exhibit strongly enhanced photothermal heating due to Mie resonances, which leads to the strong modulation of elastic Rayleigh scattering intensity through subsequent thermo-optical effects. However, the influence of the complex photo-thermo-optical effect on inelastic Raman scattering has yet to be explored for resonant dielectric nanostructures. In this work, we experimentally demonstrate that the strong photo-thermo-optical interaction results in the nonlinear dependence of the Raman scattering signal intensity from a crystalline silicon nanoparticle via the thermal reconfiguration of the resonant response. Our results reveal a crucial role of the Mie resonance spectral sensitivity to temperature, which modifies not only the conversion of the incident light into heat but also Raman scattering efficiency. The developed comprehensive model provides the mechanism for thermal modulation of Raman scattering, shedding light on the photon–phonon interaction physics of resonant material, which is essential for the validation of Raman nanothermometry in resonant silicon structures under a strong laser field.

In this paper, we theoretically and experimentally demonstrated photothermal nonlinearities of both forward and backward scattering intensities from quasi-perfect absorbing silicon-based metasurface with only λ/7 thickness. The metasurface is efficiently heated up by photothermal effect under laser irradiation, which in turn modulates the scattering spectra via thermo-optical effect. Under a few milliwatt continuous-wave excitation at the resonance wavelength of the metasurface, backward scattering cross-section doubles, and forward scattering cross-section reduces to half. Our study opens up the all-optical dynamical control of the scattering directionality, which would be applicable to silicon photonic devices.

Plasmonic structural color, in which vivid colors are generated via resonant nanostructures made of common plasmonic materials, such as noble metals have fueled worldwide interest in backlight-free displays. However, plasmonic colors that were withstanding ultrahigh temperatures without damage remain an unmet challenge due to the low melting point of noble metals. Here, we report the refractory hafnium nitride (HfN) plasmonic crystals that can generate full-visible color with a high image resolution of ∼63,500 dpi while withstanding a high temperature (900 °C). Plasmonic colors that reflect visible light could be attributed to the unique features in plasmonic HfN, a high bulk plasmon frequency of 3.1 eV, whichcould support localized surface plasmon resonance (LSPR) in the visible range. By tuning the wavelength of the LSPR, the reflective optical response can be controlled to generate the colors from blue to red across a wide gamut. The novel refractory plasmonic colors pave the way for emerging applications ranging from reflective displays to solar energy harvesting systems.

Silicon nanophotonics has attracted significant attention because of its unique optical properties such as efficient light confinement and low non-radiative loss. For practical applications such as all-optical switch, optical nonlinearity is a prerequisite, but the nonlinearity of silicon is intrinsically weak. Recently, we discovered a giant nonlinearity of scattering from a single silicon nanostructure by combining Mie resonance enhanced photo-thermal and thermo-optic effects. Since scattering and absorption are closely linked in Mie theory, we expect that absorption, as well as heating, of the silicon nanostructure shall exhibit similar nonlinear behaviors. In this work, we experimentally measure the temperature rise of a silicon nanoblock by in situ Raman spectroscopy, explicitly demonstrating the connection between nonlinear scattering and nonlinear heating. The results agree well with finite-element simulation based on the photo-thermo-optic effect, manifesting that the nonlinear effect is the coupled consequence of the red shift between scattering and absorption spectra. Our work not only unravels the nonlinear absorption in a silicon Mie-resonator but also offers a quantitative analytic model to better understand the complete photo-thermo-optic properties of silicon nanostructures, providing a new perspective toward practical silicon photonics applications. [ABSTRACT FROM AUTHOR]

Nonlinear optics, when combined with microscopy, is known to provide advantages including novel contrast, deep tissue observation, and minimal invasiveness. In addition, special nonlinearities, such as switch on/off and saturation, can enhance the spatial resolution below the diffraction limit, revolutionizing the field of optical microscopy. These nonlinear imaging techniques are extremely useful for biological studies on various scales from molecules to cells to tissues. Nevertheless, in most cases, nonlinear optical interaction requires strong illumination, typically at least gigawatts per square centimeter intensity. Such strong illumination can cause significant phototoxicity or even photodamage to fragile biological samples. Therefore, it is highly desirable to find mechanisms that allow the reduction of illumination intensity. Surface plasmon, which is the collective oscillation of electrons in metal under light excitation, is capable of significantly enhancing the local field around the metal nanostructures and thus boosting up the efficiency of nonlinear optical interactions of the surrounding materials or of the metal itself. In this mini-review, we discuss the recent progress of plasmonics in nonlinear optical microscopy with a special focus on biological applications. The advancement of nonlinear imaging modalities (including incoherent/coherent Raman scattering, two/three-photon luminescence, and second/third harmonic generations that have been amalgamated with plasmonics), as well as the novel subdiffraction limit imaging techniques based on nonlinear behaviors of plasmonic scattering, is addressed.

We solve the Maxwell and heat equations self-consistently for metal nanoparticles under intense continuous wave (CW) illumination. Unlike previous studies, we rely on experimentally-measured data for metal permittivity for increasing temperature and for the visible spectral range. We show that the thermal nonlinearity of the metal can lead to substantial deviations from the predictions of the linear model for the temperature and field distribution and, thus, can explain qualitatively the strong nonlinear scattering from such configurations observed experimentally. We also show that the incompleteness of existing data of the temperature dependence of the thermal properties of the system prevents reaching a quantitative agreement between the measured and calculated scattering data. This modeling approach is essential for the identification of the underlying physical mechanism responsible for the thermo-optical nonlinearity of the metal and should be adopted in all applications of high-temperature nonlinear plasmonics, especially for refractory metals, for both CW and pulsed illumination.

High‐index nanostructures are found to exhibit large nonlinearity of spectral responses under photoexcitation, which is applicable to all‐optical modulation. The nonlinearity stems from Mie‐type resonance shift due to photoinduced variation of refractive index. Here, amorphous silicon‐based Huygens' metasurface absorber and ultrafast excitation are used to demonstrate two orders of magnitude enhancement of modulation depth, both theoretically and experimentally, when electric dipole lattice resonance matches the magnetic dipole resonance. Within a few square micrometer spatial confinement and picosecond scale delay, over 100% photothermal modulation depth is experimentally achieved at matched resonance condition. This concept is not limited to photothermal modulation in the amorphous silicon but is applicable to dielectric materials with various mechanisms to achieve modulation of refractive index. This work opens the avenue toward all‐optical information processing via optimized modulation by careful spatiotemporal and spectral control over a metasurface. [ABSTRACT FROM AUTHOR]

In this paper, we theoretically and experimentally demonstrated photothermal nonlinearities of both forward and backward scattering intensities from quasi-perfect absorbing silicon-based metasurface with only λ/7 thickness. The metasurface is efficiently heated up by photothermal effect under laser irradiation, which in turn modulates the scattering spectra via thermo-optical effect. Under a few milliwatt continuous-wave excitation at the resonance wavelength of the metasurface, backward scattering cross-section doubles, and forward scattering cross-section reduces to half. Our study opens up the all-optical dynamical control of the scattering directionality, which would be applicable to silicon photonic devices. [ABSTRACT FROM AUTHOR]

Nonlinear silicon nano‐photonics has recently attracted significant attention due to the plethora of electric and magnetic Mie resonances that offer substantial enhancement of optical nonlinearities. Conventionally, the characterization of nonlinearity and its transient nature rely on intensity‐scan methods (z‐scan) in the spatial domain and pump‐probe techniques in the temporal domain. However, most studied ultrafast nonlinear effects are instantaneous, that is, strongest at zero pump‐probe delay, and have a solitary nonlinear power dependency (square, cubic, etc.). Here the authors found that when relaxation lifetime is dependent on pump fluence, transient nonlinearity appears. The effect is exemplified via Auger‐based nonlinear carrier dynamics of a nano‐silicon Mie‐resonator. The Auger‐induced transient nonlinearity not only locates at the time delay of several tens of picoseconds, but also displays diverse nonlinearities, including sub‐linear, super‐linear, and surprisingly full saturation, which features a "crossing point" where the probe scattering is pump‐fluence independent. The crossing point exists when the relaxation lifetime is inversely dependent to second power of carrier density. Combining confocal intensity‐scan (x‐scan) and pump‐probe temporal scan, the authors demonstrate that sub‐linearity and super‐linearity lead to swelled and reduced full‐width‐at‐half‐maximum (FWHM) of single‐nanostructure images, further confirming the nonlinearity as well as the potential of sub‐diffraction microscopy. The results open up a new avenue in nonlinear silicon nano‐photonics by adding new degrees of freedom in temporally tuning the types of transient nonlinearities, which are valuable in all‐optical signal processing and nano‐imaging. [ABSTRACT FROM AUTHOR]

Understanding how the brain functions is one of the grand challenges in modern scientific research. Similar to a computer, a functional brain is composed of hardware and software. The major bottleneck lies in the difficulty to directly observe the brain 'software', i.e. the rule and operating information used by the brain that might emerge from pan-neuron/synapse connectome. A recognized strategy for probing the functional connectome is to perform volumetric imaging in brains with high spatiotemporal resolution and deep brain penetration. Among various imaging technologies, optical imaging offers appealing combinations including spatial resolution of sub-micrometer to nanometer, temporal resolution of second to millisecond, penetration depth of millimeter or deeper, and molecular contrast based on the abundant choices of fluorescent indicators. Thus, it is ideal for enabling three-dimensional functional brain mapping of small animal models. In this review, we focus on recent technological advances in optical volumetric imaging, with an emphasis on the tools and methods for enhancing imaging speed, depth, and resolution. The review could serve as a quantitative reference for physicists and biologists to choose the techniques better suited for specific applications, as well as to stimulate novel technical developments to advance brain research. [ABSTRACT FROM AUTHOR]

Confocal pump-probe backscattering was used to study phonon dynamics of single nanoparticles, which can extend to confocal pump-probe microscopy for investigating carrier dynamics of single nanomaterials. Compared to previous pump-probe microscopy studies, in which nonlinear optical generation was widely utilized, spectral filters were employed in this work to separate the spectra from the optical pulses for pump/probe beams. This not only reduces the complexity of the experimental setup but can also circumvent the aberration issue. Phonon dynamics, including acoustic vibrations and heat diffusion, of a single gold nanoparticle were measured with a temporal delay of 8 ns, and a 0.5 K rise in the temperature of the surrounding media was resolved. The relative optical changes induced by the photoexcitation of the pump pulses in confocal reflection pump-probe traces were orders of magnitude larger than those in typical transmission-type pump probe traces. [ABSTRACT FROM AUTHOR]

We demonstrate a beam-scanning nonlinear light endoscope based on a flexible fiber bundle. Excited with a femtosecond Cr:Forsterite laser, the degradation in multiphoton multiharmonic excitation efficiency due to the pulse-broadening effect is significantly reduced without utilizing any external devices. The system resolution has been characterized to be 5.4 μm in the two-photon fluorescence endoscope, limited by the sampling theory. Finally, several image examples have been given. Microsc. Res. Tech., 2008. © 2008 Wiley-Liss, Inc. [ABSTRACT FROM AUTHOR]

In recent years, nonlinear laser scanning microscopy has gained much attention due to its unique ability of deep optical sectioning. Based on our previous studies, a 1,200-1,300-nm femtosecond laser can provide superior penetration capability with minimized photodamage possibility. However, with the longer wavelength excitation, three-photon-fluorescence (3PF) would be necessary for efficient use of intrinsic and extrinsic visible fluorophores. The three-photon process can provide much better spatial resolution than two-photon-fluorescence due to the cubic power dependency. On the other hand, third-harmonic-generation (THG), another intrinsic three-photon process, is interface-sensitive and can be used as a general structural imaging modality to show the exact location of cellular membranes. The virtual-transition characteristic of THG prevents any excess energy from releasing in bio-tissues and, thus, THG acts as a truly noninvasive imaging tool. Here we demonstrated the first combined 3PF and THG microscopy, which can provide three-dimensional high-resolution images with both functional molecule specificity and sub-micrometer structural mapping capability. The simultaneously acquired 3PF and THG images based on a 1,230-nm Cr:forsterite femtosecond laser are shown with a Hoechst-labeled hepatic cell sample. Strong 3PF around 450 nm from DNA-bounded Hoechst-33258 can be observed inside each nucleus while THG reveals the location of plasma membranes and other membrane-based organelles such as mitochondria. Considering that the maximum-allowable laser power in common nonlinear laser microscopy is less than 10 mW at 800 nm, it is remarkable that even with a 100-mW 1,230-nm incident power, there is no observable photo damage on the cells, demonstrating the noninvasiveness of this novel microscopy technique. Microsc. Res. Tech. 66:193-197, 2005. © 2005 Wiley-Liss, Inc. [ABSTRACT FROM AUTHOR]

Optical higher harmonic generation, including second harmonic generation and third harmonic generation, leaves no energy deposition to its interacted matters due to an energy-conservation characteristic, providing the “noninvasiveness” nature desirable for biological studies. Combined with its nonlinearity, higher harmonic generation microscopy provides excellent three-dimensional (3D) sectioning capability, offering new insights into the studies of embryonic morphological changes and complex developmental processes. By choosing a laser working in the biological penetration window, here we present a noninvasive in vivo light microscopy with sub-micron 3D resolution and millimeter penetration, utilizing endogenous higher harmonic generation signals in live specimens. Noninvasive imaging was performed in live zebrafish (Danio rerio) embryos. The complex developmental processes within >1-mm-thick zebrafish embryos can be observed in vivo without any treatment. No optical damage was found even with high illumination after long-term observations and the examined embryos all developed normally at least to the larval stage. The excellent 3D resolution of the demonstrated technology allows us to capture the subtle developmental information on the cellular or sub-cellular levels occurring deep inside the live embryos and larvae. This technique can not only provide in vivo observation of the cytoarchitecture dynamics during embryogenesis with submicron resolution and millimeter penetration depth, but would also make strong impact in developmental and structural biology studies. [Copyright &y& Elsevier]

We studied third harmonic generation (THG) of melanin solution with concentrations similar to melanocytes in human skin. In contrast to conventional observation of THG at interface, bulk THG was detected inside the solution due to the formation of melanin hydrocolloids. A linear relationship between melanin concentration and THG intensity was found, suggesting THG originated from high-order hyper-Rayleigh scattering. By fitting this linear relationship, third-order hyperpolarizability of melanin hydrocolloids was determined to be three orders larger than that of water. Our result will be useful for interpretation of THG signals in skin and other tissues containing colloidal particles. [ABSTRACT FROM AUTHOR]

Second-harmonic-generation (SHG) has proved itself as an important contrast mechanism in microscopic applications. Its noninvasiveness, optical sectioning capability, and high-penetrability provide attractive features in observation of thick biological tissues. Fibrous proteins, such as myosin and collagen, are dominant SHG harmonophores in vertebrates. Due to their biophotonic crystal nature, SHGs from these proteins are known to exhibit specific polarization dependencies, reflecting local molecule arrangements. Here the authors demonstrate a scheme to distinguish SHG from myosin-based muscle fibers and intertwined collagenous perimysium through polarization selection, without complicated staining or sample/image processing required. [ABSTRACT FROM AUTHOR]

By coinciding the plasmon frequency with the third-harmonic frequency of the excitation light, the authors determined the plasmon-resonance enhanced optical third-harmonic-generation (THG) susceptibility of a polyvinylpyrrolidone-coated Ag nanoparticle with a 5–7 nm diameter. With dispersed Ag nanoparticles on a quartz surface and through measuring the frequency dependent THG intensities, interface THG showed evident enhancement when the third harmonic of excitation matched the Ag-nanoparticle’s plasmon-resonant frequency. According to the effective medium theory and by analyzing the interface THG under focused Gaussian beams, the ensemble-averaged χ(3)(3ω:ω,ω,ω) of a Ag nanoparticle can be estimated to be on the order of 2×10-11 esu. [ABSTRACT FROM AUTHOR]