Quasi-Phase-Matching in Chiral Materials

The second-order nonlinear optical coefficients associated with chirality differ in sign for the two mirror-image forms (enantiomers) of a chiral material. Structures comprised of alternating stacks of the enantiomers can therefore be used for quasi-phase-matched frequency conversion, as we demonstrate here by second-harmonic generation from Langmuir-Blodgett films of a helicenebisquinone. Such structures could lead to new types of frequency converters in which both the second-order nonlinear response and quasi-phase-matching arise from the chirality of a material rather than its polar order. PACS numbers: 42.65.Ky, 42.70.Nq, 78.66.Q

Media 1: Particle plasmon resonances in L-shaped gold nanoparticles

Originally published in Optics Express on 02 August 2010 (oe-18-16-16601

Media 2: Nonlinear optical activity effects in complex anisotropic three-dimensional media

Originally published in Optical Materials Express on 01 January 2015 (ome-5-1-11

Efficient hybrid-mode excitation in plasmonic nanoantennas by tightly focused higher-order vector beams

Efficient optical excitation of hybridized plasmon modes in nanoantennas is vital to achieve many promising functionalities, but it can be challenging due to a field-profile mismatch between the incident light and the hybrid mode. We present a general approach for efficient hybrid-mode excitation by focusing the incident light field in the basis of cylindrically polarized vector beams of various higher-order spiral phases. Such basis vector beams are described in the higher-order polarization states and Stokes parameters (both defined locally in polar coordinates), and visualized correspondingly on the higher-order Poincar\'e spheres. The focal field is formulated exclusively in cylindrical coordinates as a series sum of all focused beams of the associated high-order paraxial beams. Our focal field decomposition enables an analysis of hybrid-mode excitation via higher-order vector beams, and thus yields a straightforward design of effective mode-matching field profile in the tightly focused region

Microscopic Determination of Second-Order Nonlinear Optical Susceptibility Tensors

We demonstrate a microscopy technique that extracts tensorial information about the second-order nonlinear optical susceptibility and hyperpolarizability of molecular materials. Our technique is based on polarization-dependent second-harmonic generation and a genetic algorithm, using which the best possible match with the measured data, and the possible susceptibility tensor components are found. In contrast to existing techniques, which access only the magnitude of the nonlinear response, our technique also provides information about the phase of the tensor components, which is associated with molecular resonances. After verifying the technique using simulated model structures with well-known symmetries, we demonstrate its capabilities using model surface samples consisting of single purple membrane (PM) fragments of bacteriorhodopsin (bR) chromoproteins. Since the supramolecular structures of PM, bR, and photoactive retinal molecules are known, complex-valued tensorial information on the molecular hyperpolarizabilities can also be extracted. Our technique opens new possibilities for obtaining detailed structural information on biomolecular samples with microscopic resolution

Collective Effects in Second-Harmonic Generation from Plasmonic Oligomers

We investigate collective effects in plasmonic oligomers of different symmetries using second-harmonic generation (SHG) microscopy with cylindrical vector beams (CVBs). The oligomers consist of gold nanorods that have a longitudinal plasmon resonance close to the fundamental wavelength that is used for SHG excitation and whose long axes are arranged locally such that they follow the distribution of the transverse component of the electric field of radially or azimuthally polarized CVBs in the focal plane. We observe that SHG from such rotationally symmetric oligomers is strongly modified by the interplay between the polarization properties of the CVB and interparticle coupling. We find that the oligomers with radially oriented nanorods exhibit small coupling effects. In contrast, we find that the oligomers with azimuthally oriented nanorods exhibit large coupling effects that lead to silencing of SHG from the whole structure. Our experimental results are in very good agreement with numerical calculations based on the boundary element method. The work describes a new route for studying coupling effects in complex arrangements of nano-objects and thereby for tailoring the efficiency of nonlinear optical effects in such structures

Second-Harmonic Generation Imaging of Metal Nano-Objects with Cylindrical Vector Beams

We introduce an imaging technique based on second-harmonic generation with cylindrical vector beams that is extremely sensitive to three-dimensional orientation and nanoscale morphology of metal nano-objects. Our experiments and second-harmonic field calculations based on frequency-domain boundary element method are in very good agreement. The technique provides contrast for structural features that cannot be resolved by linear techniques or conventional states of polarization and shows great potential for simple and cost-effective far-field optical imaging in plasmonics

Second-Harmonic Generation from Metal Nanoparticles: Resonance Enhancement versus Particle Geometry

We demonstrate that optical second-harmonic generation (SHG) from arrays of noncentrosymmetric gold nanoparticles depends essentially on particle geometry. We prepare nanoparticles with different geometrical shapes (L and T) but similar wavelengths for the polarization-dependent plasmon resonances. In contrast to recent interpretations emphasizing resonances at the fundamental frequency, the T shape leads to stronger SHG when only one, instead of both, polarization component of the fundamental field is resonant. This is explained by the character of plasmon oscillations supported by the two shapes. Our numerical simulations for both linear and second-order responses display unprecedented agreement with measurements

Metamaterials with Tailored Nonlinear Optical Response

We demonstrate that the second-order nonlinear optical response of noncentrosymmetric metal nanoparticles (metamolecules) can be efficiently controlled by their mutual ordering in an array. Two samples with minor change in ordering have nonlinear responses differing by a factor of up to 50. The results arise from polarization-dependent plasmonic resonances modified by long-range coupling associated with metamolecular ordering. The approach opens new ways for tailoring the nonlinear responses of metamaterials and their tensorial properties

Local Field Asymmetry Drives Second-Harmonic Generation in Noncentrosymmetric Nanodimers

We demonstrate that second-harmonic generation (SHG) from arrays of noncentrosymmetric T-shaped gold nanodimers with a nanogap arises from asymmetry in the local fundamental field distribution and is not related strictly to nanogap size. Calculations show that the local field contains orthogonal polarization components not present in the exciting field, which yield the dominant SHG response. The strongest SHG responses occur through the local surface susceptibility of the particles for a fundamental field distributed asymmetrically at the particle perimeters. Weak responses result from more symmetric distributions despite high field enhancement in the nanogap. Nearly constant field enhancement persists for relatively large nanogap sizes