Henri J. Lezec

Diffracted evanescent wave model for enhanced and suppressed optical transmission through subwavelength hole arrays

Transmission enhancements of order 1000 have been reported for subwavelength hole arrays in metal films and attributed to surface plasmon (SP) resonance. We show that the properly normalized enhancement factor is consistently less than 7, and that similar enhancements occur in nonmetallic systems that do not support SPs. We present a new model in which the transmission is modulated not by coupling to SPs but by interference of diffracted evanescent waves generated by subwavelength features at the surface, leading to transmission suppression as well as enhancement. This mechanism accounts for the salient optical properties of subwavelength apertures surrounded by periodic surface corrugations.

All-angle negative refraction and active flat lensing of ultraviolet light

Decades ago, Veselago predicted that a material with simultaneously negative electric and magnetic polarization responses would yield a ‘left-handed’ medium in which light propagates with opposite phase and energy velocities—a condition described by a negative refractive index. He proposed that a flat slab of left-handed material possessing an isotropic refractive index of −1 could act like an imaging lens in free space. Left-handed materials do not occur naturally, and it has only recently become possible to achieve a left-handed response using metamaterials, that is, electromagnetic structures engineered on subwavelength scales to elicit tailored polarization responses. So far, left-handed responses have typically been implemented using resonant metamaterials composed of periodic arrays of unit cells containing inductive–capacitive resonators and conductive wires. Negative refractive indices that are isotropic in two or three dimensions at microwave frequencies have been achieved in resonant metamaterials with centimetre-scale features. Scaling the left-handed response to higher frequencies, such as infrared or visible, has been done by shrinking critical dimensions to submicrometre scales by means of top-down nanofabrication. This miniaturization has, however, so far been achieved at the cost of reduced unit-cell symmetry, yielding a refractive index that is negative along only one axis. Moreover, lithographic scaling limits have so far precluded the fabrication of resonant metamaterials with left-handed responses at frequencies beyond the visible. Here we report the experimental implementation of a bulk metamaterial with a left-handed response to ultraviolet light. The structure, based on stacked plasmonic waveguides, yields an omnidirectional left-handed response for transverse magnetic polarization characterized by a negative refractive index. By engineering the structure to have a refractive index close to −1 over a broad angular range, we achieve Veselago flat lensing, in free space, of arbitrarily shaped, two-dimensional objects beyond the near field. We further demonstrate active, all-optical modulation of the image transferred by the flat lens.

Electrooptic Modulation in Thin Film Barium Titanate Plasmonic Interferometers

We demonstrate control of the surface plasmon polariton wavevector in an active metal-dielectric plasmonic interferometer by utilizing electrooptic barium titanate as the dielectric layer. Arrays of subwavelength interferometers were fabricated from pairs of parallel slits milled in silver on barium titanate thin films. Plasmon-mediated transmission of incident light through the subwavelength slits is modulated by an external voltage applied across the barium titanate thin film. Transmitted light modulation is ascribed to two effects, electrically induced domain switching and electrooptic modulation of the barium titanate index.

Universal optical transmission features in periodic and quasiperiodic hole arrays

We investigate the influence of array order in the optical transmission properties of subwavelength hole arrays, by comparing the experimental spectral transmittance of periodic and quasiperiodic hole arrays as a function of frequency. We find that periodicity and long-range order are not necessary requirements for obtaining enhanced and suppressed optical transmission, provided short-range order is maintained. Transmission maxima and minima are shown to result, respectively, from constructive and destructive interference at each hole, between the light incident upon and exiting from a given hole, and surface plasmon polaritons (SPPs) arriving from individual neighboring holes. These SPPs are launched along both illuminated and exit surfaces, by diffraction of the incident and emerging light at the neighboring individual subwavelength holes. By characterizing the optical transmission of a pair of subwavelength holes as a function of hole-hole distance, we demonstrate that a subwavelength hole can launch SPPs with an efficiency up to 35%, and with an experimentally determined launch phase phi = pi /2, for both input-side and exit-side SPPs. This characteristic phase has a crucial influence on the shape of the transmission spectra, determining transmission minima in periodic arrays at those frequencies where grating coupling arguments would instead predict maxima.

Quantitative determination of optical transmission through subwavelength slit arrays in Ag films: Role of surface wave interference and local coupling between adjacent slits

Measurement of the transmitted intensity from a coherent monomode light source through a series of subwavelength slit arrays in Ag films, with varying array pitch and number of slits, demonstrate enhancement (suppression) by as much as a factor of 6 (9) when normalized to that of an isolated slit. Pronounced minima in the transmitted intensity were observed at array pitches corresponding to λSPP, 2 λSPP and 3λSPP where λSPP is the wavelength of the surface plasmon polariton (SPP). Increasing the number of slits to more than four does not increase appreciably the per-slit transmission intensity. These results are consistent with a model for interference between SPPs and the incident wave that fits well the measured transmitted intensity profile.

Loss mechanisms of surface plasmon polaritons on gold probed by cathodoluminescence imaging spectroscopy

We use cathodoluminescence imaging spectroscopy to excite surface plasmon polaritons and measure their decay length on single crystal and polycrystalline gold surfaces. The surface plasmon polaritons are excited on the gold surface by a nanoscale focused electron beam and are coupled into free space radiation by gratings fabricated into the surface. By scanning the electron beam on a line perpendicular to the gratings, the propagation length is determined. Data for single-crystal gold are in agreement with calculations based on dielectric constants. For polycrystalline films, grain boundary scattering is identified as additional loss mechanism, with a scattering coefficient SG=0.2%.

Direct imaging of propagation and damping of near-resonance surface plasmon polaritons using cathodoluminescence spectroscopy

Cathodoluminescence imaging spectroscopy is used to determine the propagation distance of surface plasmon polaritons near the surface plasmon resonance on both silver and gold films. Surface plasmon polaritons are generated by a focused (diameter of 5nm) electron beam spot in the metal and coupled out through a grating. By gradually varying the distance between the excitation spot and the grating the damping is probed. Propagation lengths as small as several hundred nanometers are probed, and an increase in propagation length is observed if the wavelength is increased above resonance. The measured data are compared with the calculated propagation lengths taking into account both absorption in the film and leakage radiation, and it is found that other loss mechanisms appear to be significant as well.

Surface plasmon polariton modes in a single-crystal Au nanoresonator fabricated using focused-ion-beam milling

We use focused-ion-beam milling of a single-crystal Au surface to fabricate a 590-nm-long linear ridge that acts as a surface plasmon nanoresonator. Cathodoluminescence imaging spectroscopy is then used to excite and image surface plasmons on the ridge. Principal component analysis reveals distinct plasmonic modes, which proves confinement of surface plasmon oscillations to the ridge. Boundary-element-method calculations confirm that a linear ridge is able to support highly localized surface plasmon modes (mode diameter <100 nm). The results demonstrate that focused-ion-beam milling can be used in rapid prototyping of nanoscale single-crystal plasmonic components.

High-contrast and fast electrochromic switching enabled by plasmonics

With vibrant colours and simple, room-temperature processing methods, electrochromic polymers have attracted attention as active materials for flexible, low-power-consuming devices. However, slow switching speeds in devices realized to date, as well as the complexity of having to combine several distinct polymers to achieve a full-colour gamut, have limited electrochromic materials to niche applications. Here we achieve fast, high-contrast electrochromic switching by significantly enhancing the interaction of light—propagating as deep-subwavelength-confined surface plasmon polaritons through arrays of metallic nanoslits, with an electrochromic polymer—present as an ultra-thin coating on the slit sidewalls. The switchable configuration retains the short temporal charge-diffusion characteristics of thin electrochromic films, while maintaining the high optical contrast associated with thicker electrochromic coatings. We further demonstrate that by controlling the pitch of the nanoslit arrays, it is possible to achieve a full-colour response with high contrast and fast switching speeds, while relying on just one electrochromic polymer.

Nanoscale Imaging of Photocurrent and Efficiency in CdTe Solar Cells

The local collection characteristics of grain interiors and grain boundaries in thin-film CdTe polycrystalline solar cells are investigated using scanning photocurrent microscopy. The carriers are locally generated by light injected through a small aperture (50-300 nm) of a near-field scanning optical microscope in an illumination mode. Possible influence of rough surface topography on light coupling is examined and eliminated by sculpting smooth wedges on the granular CdTe surface. By varying the wavelength of light, nanoscale spatial variations in external quantum efficiency are mapped. We find that the grain boundaries (GBs) are better current collectors than the grain interiors (GIs). The increased collection efficiency is caused by two distinct effects associated with the material composition of GBs. First, GBs are charged, and the corresponding built-in field facilitates the separation and the extraction of the photogenerated carriers. Second, the GB regions generate more photocurrent at long wavelength corresponding to the band edge, which can be caused by a smaller local band gap. Resolving carrier collection with nanoscale resolution in solar cell materials is crucial for optimizing the polycrystalline device performance through appropriate thermal processing and passivation of defects and surfaces.