[Show abstract][Hide abstract] ABSTRACT: We report our recent development in pursuing high Quality-Factor (high-Q factor) plasmonic resonances, with vertically aligned two dimensional (2-D) periodic nanorod arrays. The 2-D vertically aligned nano-antenna array can have high-Q resonances varying arbitrarily from near infrared to terahertz regime, as the antenna resonances of the nanorod are highly tunable through material properties, the length of the nanorod, and the orthogonal polarization direction with respect to the lattice surface,. The high-Q in combination with the small optical mode volume gives a very high Purcell factor, which could potentially be applied to various enhanced nonlinear photonics or optoelectronic devices. The 'hot spots' around the nanorods can be easily harvested as no index-matching is necessary. The resonances maintain their high-Q factor with the change of the environmental refractive index, which is of great interest for molecular sensing.
SPIE NanoScience & Engineering, San Diego; 09/2014
[Show abstract][Hide abstract] ABSTRACT: Diffractively coupled plasmonic resonances possess both ultra-sharp linewidths and giant electric field enhancement around plasmonic nanostructures. They can be applied to create a new generation of sensors, detectors, and nano-optical devices. However, all current designs require stringent index-matching at the resonance condition that limits their applicability. Here, we propose and demonstrate that it is possible to relieve the index-matching requirement and to induce ultra-sharp plasmon resonances in an ordered vertically aligned optical nano-antenna phased array by transforming a dipole resonance to a monopole resonance with a mirror plane. Due to the mirror image effect, the monopole resonance not only retained the dipole features but also enhanced them. The engineered resonances strongly suppressed the radiative decay channel, resulting in a four-order of magnitude enhancement in local electric field and a Q-factor greater than 200.
[Show abstract][Hide abstract] ABSTRACT: Periodic dielectric structures are typically integrated with a planar waveguide to create photonic band-edge modes for feedback in one-dimensional distributed feedback lasers and two-dimensional photonic-crystal lasers. Although photonic band-edge lasers are widely used in optics and biological applications, drawbacks include low modulation speeds and diffraction-limited mode confinement. In contrast, plasmonic nanolasers can support ultrafast dynamics and ultrasmall mode volumes. However, because of the large momentum mismatch between their nanolocalized lasing fields and free-space light, they suffer from large radiative losses and lack beam directionality. Here, we report lasing action from band-edge lattice plasmons in arrays of plasmonic nanocavities in a homogeneous dielectric environment. We find that optically pumped, two-dimensional arrays of plasmonic Au or Ag nanoparticles surrounded by an organic gain medium show directional beam emission (divergence angle <1.5° and linewidth <1.3 nm) characteristic of lasing action in the far-field, and behave as arrays of nanoscale light sources in the near-field. Using a semi-quantum electromagnetic approach to simulate the active optical responses, we show that lasing is achieved through stimulated energy transfer from the gain to the band-edge lattice plasmons in the deep subwavelength vicinity of the individual nanoparticles. Using femtosecond-transient absorption spectroscopy, we verified that lattice plasmons in plasmonic nanoparticle arrays could reach a 200-fold enhancement of the spontaneous emission rate of the dye because of their large local density of optical states.
[Show abstract][Hide abstract] ABSTRACT: Plasmonic lasers exploit strong electromagnetic field confinement at dimensions well below the diffraction limit. However, lasing from an electromagnetic hot spot supported by discrete, coupled metal nanoparticles (NPs) has not been explicitly demonstrated to date. We present a new design for a room-temperature nanolaser based on three-dimensional (3D) Au bowtie NPs supported by an organic gain material. The extreme field compression, and thus ultrasmall mode volume, within the bowtie gaps produced laser oscillations at the localized plasmon resonance gap mode of the 3D bowties. Transient absorption measurements confirmed ultrafast resonant energy transfer between photoexcited dye molecules and gap plasmons on the picosecond time scale. These plasmonic nanolasers are anticipated to be readily integrated into Si-based photonic devices, all-optical circuits, and nanoscale biosensors.
[Show abstract][Hide abstract] ABSTRACT: This article describes the angle-dependent optical responses of 2D metal–insulator–metal (MIM) nanocavity arrays. Through a combination of soft nanolithography and template stripping, we fabricated arrays of plasmonic MIM nanostructures with subwavelength spacings over square centimeter areas. We controlled the coupling between the localized surface plasmon and guided modes as well as engineered the optical band structure by tuning the insulator thickness. Rabi splitting of hybridized modes strongly depended on the spatial overlap of the near-fields of the localized and guided modes.
The Journal of Physical Chemistry C. 09/2012; 117(6):2541–2546.
[Show abstract][Hide abstract] ABSTRACT: This paper describes a new nanofabrication method, moiré nanolithography, that can fabricate subwavelength lattices with high-rotational symmetries. By exposing elastomeric photomasks sequentially at multiple offset angles, we created arrays with rotational symmetries as high as 36-fold, which is three times higher than quasiperiodic lattices (≤12-fold) and six times higher than two-dimensional periodic lattices (≤6-fold). Because these moiré nanopatterns can be generated over wafer-scale areas, they are promising for a range of photonic applications, especially those that require broadband, omnidirectional absorption of visible light.
[Show abstract][Hide abstract] ABSTRACT: This paper reports the manipulation of surface plasmon polaritons (SPPs) in a liquid plasmonic metal by changing its physical phase. Dynamic properties were controlled by solid-to-liquid phase transitions in 1D Ga gratings that were fabricated using a simple molding process. Solid and liquid phases were found to exhibit different plasmonic properties, where light coupled to SPPs more efficiently in the liquid phase. We exploited the supercooling characteristics of Ga to access plasmonic properties associated with the liquid phase over a wider temperature range (up to 30 °C below the melting point of bulk Ga). Ab initio density functional theory-molecular dynamic calculations showed that the broadening of the solid-state electronic band structure was responsible for the superior plasmonic properties of the liquid metal.
[Show abstract][Hide abstract] ABSTRACT: This paper reports the experimental and theoretical investigation of the Talbot effect beyond the paraxial limit at optical frequencies. Au hole array films with periodicity a(0) comparable to the wavelength of coherent illumination λ were used to study the non-paraxial Talbot effect. Significant differences from the paraxial (classical) Talbot effect were observed. Depending on the ratio of a(0)/λ, the interference pattern in the direction perpendicular to the hole array was not necessarily periodic, and the self-image distances deviated from the paraxial Talbot distances. Defects within the hole array film or above the film were healed in the self-images as the light propagated from the surface.
[Show abstract][Hide abstract] ABSTRACT: This Letter describes how out-of-plane lattice plasmon (OLP) resonances in 2D Au nanoparticle (NP) arrays show dispersive quality factors. These quality factors can be tailored simply by controlling NP height. Numerical calculations of near-field optical properties and band diagrams were performed to understand the measured dispersion effects of the OLPs. The results revealed that delocalized OLPs are a type of surface Bloch mode composed of many Bloch harmonics. As the OLP dispersion evolves from a stationary state to a propagating state, the nonradiative loss decreases because of weak local field confinement, whereas the radiative loss increases because of strong coupling to the leaky zero-order harmonic.
[Show abstract][Hide abstract] ABSTRACT: This paper reports the fabrication and characterization of three-dimensional (3D) multiscale Au particles with different aspect ratios. Increasing the length of the particles resulted in excitation of a longitudinal mode and two different transverse modes having different multipolar orders. The multipolar orders increased for both longitudinal and transverse modes as the aspect ratio increased. Finite-difference time-domain calculations revealed that the structural asymmetry of the 3D anisotropic particles were the reason for the two distinct transverse plasmon resonances. When the 3D structural change occurred at the ends of the multiscale particle, however, the optical response showed two resonances in the longitudinal direction and only a single resonance in the transverse direction.
[Show abstract][Hide abstract] ABSTRACT: This paper reports that arrays of three-dimensional (3D), bowtie-shaped Au nanoparticle dimers can exhibit extremely high nonlinear absorption. Near-field interactions across the gap of the 3D bowties at the localized surface plasmon resonance wavelengths resulted in an increase of more than 4 orders of magnitude in local field intensity. The imaginary part of the third-order nonlinear susceptibility (Im χ((3))) for the 3D bowtie arrays embedded in a dielectric material was measured to be 10(-4) esu, more than 2 orders of magnitude higher than reported for other metal nanoparticle-dielectric composites. Moreover, 3D dimers with increased nanoscale structure (such as folding) exhibited increased optical nonlinearity. These 3D nanoantennas can be used as critical elements for nanoscale nonlinear optical devices.
[Show abstract][Hide abstract] ABSTRACT: This article reports the study of infrared plasmonics with both random and periodic arrays of indium-tin-oxide (ITO) nanorods (NR). A description is given on the synthesis, patterning, and characterization of physical properties of the ITO NR arrays. A classical scattering model, along with a 3-D finite-element-method and a 3-D finite-difference-time-domain numerical simulation method has been used to interpret the unique light scattering phenomena. It is also shown that the intrinsic plasma frequency can be varied through careful postsynthesis processing of the ITO NRs. Examples are given on how coupled plasmon resonances can be tuned through patterning of the ITO NR arrays. In addition, environment dielectric sensing has been demonstrated through the shift of the resonances as a result of index change surrounding the NRs. These initial results suggest potential for further improvement and opportunities to develop a good understanding of infrared plasmonics using ITO and other transparent conducting oxide semiconducting materials.
[Show abstract][Hide abstract] ABSTRACT: Plasmonic nanostructures concentrate optical fields into nanoscale volumes, which is useful for plasmonic nanolasers, surface enhanced Raman spectroscopy and white-light generation. However, the short lifetimes of the emissive plasmons correspond to a rapid depletion of the plasmon energy, preventing further enhancement of local optical fields. Dark (subradiant) plasmons have longer lifetimes, but their resonant wavelengths cannot be tuned over a broad wavelength range without changing the overall geometry of the nanostructures. Also, fabrication of the nanostructures cannot be readily scaled because their complex shapes have subwavelength dimensions. Here, we report a new type of subradiant plasmon with a narrow (∼5 nm) resonant linewidth that can be easily tuned by changing the height of large (>100 nm) gold nanoparticles arranged in a two-dimensional array. At resonance, strong coupling between out-of-plane nanoparticle dipolar moments suppresses radiative decay, trapping light in the plane of the array and strongly localizing optical fields on each nanoparticle. This new mechanism can open up applications for subradiant plasmons because height-controlled nanoparticle arrays can be manufactured over wafer-scale areas on a variety of substrates.
[Show abstract][Hide abstract] ABSTRACT: This paper reports an all-moldable nanofabrication platform that can generate, from a single master, large-area nanoscale patterns with programmable densities, fill factors, and lattice symmetries. Solvent-assisted nanoscale embossing (SANE) could increase the spacing of patterns up to 100% as well as decrease them down to 50% in a single step by stretching or heating a polymer substrate. Also, SANE could reduce critical feature sizes as small as 45% compared to the master by controlled swelling of patterned molds with different solvents. These capabilities were applied to generate plasmonic nanoparticle arrays with continuously variable separations and hence different optical properties on the same substrate.
[Show abstract][Hide abstract] ABSTRACT: This paper describes three-dimensional (3D) nanohole arrays whose high optical transmission is mediated more by localized surface plasmon (LSP) excitations than by surface plasmon polaritons (SPPs). First, LSPs on 3D hole arrays lead to optical transmission an order of magnitude higher than 2D planar hole arrays. Second, LSP-mediated transmission is broadband and more tunable than SPP-enhanced transmission, which is restricted by Bragg coupling. Third, for the first time, two types of surface plasmons can be selectively excited and manipulated on the same plasmonic substrate. This new plasmonic substrate fabricated by high-throughput nanolithography techniques paves the way for cutting-edge optoelectronic and biomedical applications.
[Show abstract][Hide abstract] ABSTRACT: The angle-dependent optical properties of rhombic plasmonic crystals are described. We show that by extending the capabilities of soft interference lithography, subwavelength periodic patterns with arbitrary 2D Bravais lattices can be generated. In addition, we demonstrate that by lowering the plasmonic crystal lattice symmetry, degenerate conditions can be lifted and more plasmon bands can be excited within a fixed wavelength range. Degeneracies were also removed by changing the polar and azimuthal angles of excitation and visualized in dispersion diagrams. Anticrossings between different plasmon bands were observed to depend significantly on the local refractive index and the excitation direction.
[Show abstract][Hide abstract] ABSTRACT: Surface plasmons are responsible for a variety of phenomena, including nanoscale optical focusing, negative refraction, and surface-enhanced Raman scattering. Their characteristic evanescent electromagnetic fields offer opportunities for sub-diffraction imaging, optical cloaking, and label-free molecular sensing. The selection of materials for such applications, however, has been traditionally limited to the noble metals Au and Ag because there has been no side-by-side comparison of other materials. This feature article describes recent progress on manipulating surface plasmons from ultraviolet to near-infrared wavelengths using plasmonic crystals made from 2D nanopyramidal arrays. A library of plasmon resonances is constructed in the form of dispersion diagrams for a series of unconventional and new composite plasmonic materials. These resonances are tuned by controlling both intrinsic factors (unit cell shape, materials type) and extrinsic factors (excitation conditions, dielectric environment). Finally, plasmonic crystals with reduced lattice symmetries are fabricated as another means to tailor resonances for broadband coupling.