Ultrabroadband infrared nanospectroscopic imaging.

Characterizing and ultimately controlling the heterogeneity underlying biomolecular functions, quantum behavior of complex matter, photonic materials, or catalysis requires large-scale spectroscopic imaging with simultaneous specificity to structure, phase, and chemical composition at nanometer spatial resolution. However, as with any ultrahigh spatial resolution microscopy technique, the associated demand for an increase in both spatial and spectral bandwidth often leads to a decrease in desired sensitivity. We overcome this limitation in infrared vibrational scattering-scanning probe near-field optical microscopy using synchrotron midinfrared radiation. Tip-enhanced localized light-matter interaction is induced by low-noise, broadband, and spatially coherent synchrotron light of high spectral irradiance, and the near-field signal is sensitively detected using heterodyne interferometric amplification. We achieve sub-40-nm spatially resolved, molecular, and phonon vibrational spectroscopic imaging, with rapid spectral acquisition, spanning the full midinfrared (700-5,000 cm(-1)) with few cm(-1) spectral resolution. We demonstrate the performance of synchrotron infrared nanospectroscopy on semiconductor, biomineral, and protein nanostructures, providing vibrational chemical imaging with subzeptomole sensitivity.

Phase resolved near-field mode imaging for the design of frequency-selective surfaces.

Frequency-selective surfaces (FSS) are a class of metasurfaces with engineered reflectance, absorbance, and transmittance behavior. We study an array of metallic crossed dipole FSS elements in the infrared using interferometric scattering-type scanning near-field optical microscopy (s-SNOM). We resolve the dependence of the near-field phase on the dimensions of the elements and compare with numerical models. The combined phase and amplitude information of the underlying near-field mode distribution compared to conventional far-field absorption spectroscopy greatly improves the targeted design of frequency-selective surfaces.

Light on the Tip of a Needle: Plasmonic Nanofocusing for Spectroscopy on the Nanoscale.

The efficiency of plasmonic nanostructures as optical antennas to concentrate optical fields to the nanoscale has been limited by intrinsically short dephasing times and small absorption cross sections. We discuss a new optical antenna concept based on surface plasmon polariton (SPP) nanofocusing on conical noble metal tips to achieve efficient far- to near-field transformation of light from the micro- to the nanoscale. The spatial separation of the launching of propagating SPPs from their subsequent apex confinement with high energy concentration enables background-free near-field imaging, tip-enhanced Raman scattering, and nonlinear nanospectroscopy. The broad bandwidth and spectral tunability of the nanofocusing mechanism in combination with frequency domain pulse shaping uniquely allow for the spatial confinement of ultrashort laser pulses and few-femtosecond spatiotemporal optical control on the nanoscale. This technique not only extends powerful nonlinear and ultrafast spectroscopies to the nanoscale but can also generate fields of sufficient intensity for electron emission and higher harmonic generation.

Femtosecond nanofocusing with full optical waveform control.

The simultaneous nanometer spatial confinement and femtosecond temporal control of an optical excitation has been a long-standing challenge in optics. Previous approaches using surface plasmon polariton (SPP) resonant nanostructures or SPP waveguides have suffered from, for example, mode mismatch, or possible dependence on the phase of the driving laser field to achieve spatial localization. Here we take advantage of the intrinsic phase- and amplitude-independent nanofocusing ability of a conical noble metal tip with weak wavelength dependence over a broad bandwidth to achieve a 10 nm spatially and few-femtosecond temporally confined excitation. In combination with spectral pulse shaping and feedback on the second-harmonic response of the tip apex, we demonstrate deterministic arbitrary optical waveform control. In addition, the high efficiency of the nanofocusing tip provided by the continuous micro- to nanoscale mode transformation opens the door for spectroscopy of elementary optical excitations in matter on their natural length and time scales and enables applications from ultrafast nano-opto-electronics to single molecule quantum coherent control.

Near-field measurement of infrared coplanar strip transmission line attenuation and propagation constants.

Impedance matched and low loss transmission lines are essential for optimal energy delivery through an integrated optical or plasmonic nanocircuit. A novel method for the measurement of the attenuation and propagation constants of an antenna-coupled coplanar strip (CPS) transmission line is demonstrated at 28.3 THz using scattering-type scanning near-field optical microscopy. Reflection of the propagating optical wave upon an open-circuit or short-circuit load at the terminal of the CPS provides a standing voltage wave, which is mapped through the associated surface-normal E(z) electric near-field component at the metal-air interface. By fitting the analytical standing wave expression to the near-field data, the transmission line properties are determined. Full-wave models and measured results are presented and are in excellent agreement.

Near-field localization in plasmonic superfocusing: a nanoemitter on a tip.

Focusing light to subwavelength dimensions has been a long-standing desire in optics but has remained challenging, even with new strategies based on near-field effects, polaritons, and metamaterials. The adiabatic propagation of surface plasmon polaritons (SPP) on a conical taper as proposed theoretically has recently emerged as particularly promising to obtain a nanoconfined light source at the tip. Employing grating-coupling of SPPs onto gold tips, we demonstrate plasmonic nanofocusing into a localized excitation of approximately 20 nm in size and investigate its near- and far-field behavior. For cone angles of approximately 10-20 degrees , the breakdown of the adiabatic propagation conditions is found to be localized at or near the apex region with approximately 10 nm radius. Despite an asymmetric side-on SPP excitation, the apex far-field emission with axial polarization characteristics representing a radially symmetric SPP mode in the nanofocus confirms that the conical tip acts as an effective mode filter with only the fundamental radially symmetric TM mode (m = 0) propagating to the apex. We demonstrate the use of these tips as a source for nearly background-free scattering-type scanning near-field optical microscopy (s-SNOM).

Determination of electric-field, magnetic-field, and electric-current distributions of infrared optical antennas: a near-field optical vector network analyzer.

In addition to the electric field E(r), the associated magnetic field H(r) and current density J(r) characterize any electromagnetic device, providing insight into antenna coupling and mutual impedance. We demonstrate the optical analogue of the radio frequency vector network analyzer implemented in interferometric homodyne scattering-type scanning near-field optical microscopy for obtaining E(r), H(r), and J(r). The approach is generally applicable and demonstrated for the case of a linear coupled-dipole antenna in the midinfrared spectral region. The determination of the underlying 3D vector electric near-field distribution E(r) with nanometer spatial resolution and full phase and amplitude information is enabled by the design of probe tips with selectivity with respect to E(∥) and E(⊥) fabricated by focused ion-beam milling and nano-chemical-vapor-deposition methods.

Mid-IR plasmonics: near-field imaging of coherent plasmon modes of silver nanowires.

Chemically synthesized metallic nanostructures can exhibit a strong local optical field enhancement associated with their high degree of crystallinity and well-defined geometry-dependent surface plasmon resonances. The extension of the plasmon modes into the mid-IR spectral range (3-30 microm) is shown for micrometer-sized nanowires with high aspect ratios available in the form of pentagonally twinned Ag crystallites as grown by polyol synthesis. Using scattering-scanning near-field optical microscopy, the associated IR plasmon modes are identified, and their underlying spatial distribution and enhancement of the optical polarization density is measured via phase, amplitude, and polarization resolved optical vector-field mapping. The transition from dipolar to multipolar resonances is observed and described by modeling the Ag wires using a modified cylindrical waveguide theory. For 10.6 microm excitation, dipole antenna resonances are observed at a resonant length of L = lambda(eff)/2 with lambda(eff) approximately 10.6 microm/(1.8 +/- 0.5) approximately 6 +/- 2 microm. This effective wavelength scaling is the result of electronic damping, despite the high aspect ratios of the wires of order 1:10 to 1:200. With the optical cycle period tau(IR) being comparable to the Drude relaxation time of tau approximately 40 fs the mid-IR defines the low-energy limit of the coherent plasmon regime (tau(IR) less, similar tau) at the transition to purely geometric antenna resonances (tau(IR) > tau).

Near-field imaging of optical antenna modes in the mid-infrared.

Optical antennas can enhance the coupling between free-space propagating light and the localized excitation of nanoscopic light emitters or receivers, thus forming the basis of many nanophotonic applications. Their functionality relies on an understanding of the relationship between the geometric parameters and the resulting near-field antenna modes. Using scattering-type scanning near-field optical microscopy (s-SNOM) with interferometric homodyne detection, we investigate the resonances of linear Au wire antennas designed for the mid-IR by probing specific vector near-field components. A simple effective wavelength scaling is observed for single wires with lambda(eff) = lambda /(2.0+/- 0.2), specific to the geometric and material parameters used. The disruption of the coherent current oscillation by introducing a gap gives rise to an effective multipolar mode for the two near-field coupled segments. Using antenna theory and numerical electrodynamics simulations two distinct coupling regimes are considered that scale with gap width or reactive near-field decay length, respectively. The results emphasize the distinct antenna behavior at optical frequencies compared to impedance matched radio frequency (RF) antennas and provide experimental confirmation of theoretically predicted scaling laws at optical frequencies.