Dennis F. Gardner

Self-Alignment of Plasmonic Gold Nanorods in Reconfigurable Anisotropic Fluids for Tunable Bulk Metamaterial Applications

We demonstrate the bulk self-alignment of dispersed gold nanorods imposed by the intrinsic cylindrical micelle self-assembly in nematic and hexagonal liquid crystalline phases of anisotropic fluids. External magnetic field and shearing allow for alignment and realignment of the liquid crystal matrix with the ensuing long-range orientational order of well-dispersed plasmonic nanorods. This results in a switchable polarization-sensitive plasmon resonance exhibiting stark differences from that of the same nanorods in isotropic fluids. The device-scale bulk nanoparticle alignment may enable optical metamaterial mass production and control of properties arising from combining the switchable nanoscale structure of anisotropic fluids with the surface plasmon resonance properties of the plasmonic nanorods.

Tabletop nanometer extreme ultraviolet imaging in an extended reflection mode using coherent Fresnel ptychography

We demonstrate the first (to our knowledge) general purpose full-field reflection-mode extreme ultraviolet (EUV) microscope based on coherent diffractive imaging. This microscope is capable of nanoscale amplitude and phase imaging of extended surfaces at an arbitrary angle of incidence in a noncontact, nondestructive manner. We use coherent light at 29.5 nm from high-harmonic upconversion to illuminate a surface, directly recording the scatter as the surface is scanned. Ptychographic reconstruction is then combined with tilted plane correction to obtain an image with amplitude and phase information. The image quality and detail from this diffraction-limited tabletop EUV microscope compares favorably with both scanning electron microscope and atomic force microscope images. The result is a general and completely extensible imaging technique that can provide a comprehensive and definitive characterization of how light at any wavelength scatters from a surface, with imminent feasibility of elemental imaging with

Towards Reconfigurable Optical Metamaterials: Colloidal Nanoparticle Self-Assembly and Self-Alignment in Liquid Crystals

We explore the nanoscale colloidal self-assembly and self-alignment in liquid crystals. We use model particles with controlled shapes and sizes, including quantum dots and rods and metal nanoparticles in the form of spheres, rods, and polygonal platelets. To study these composites on the scales ranging from nanometers to millimeters and to motivate their use in metamaterial fabrication, we utilize optical microscopies, freeze-fracture transmission electron microscopy, and cryogenic transmission electron microscopy. We discuss the long-range alignment and assembly of anisotropic nanoparticles imposed by the orientational elasticity of liquid crystals, showing that these composites provide a powerful platform for self-assembly of metamaterials.

High numerical aperture reflection mode coherent diffraction microscopy using off-axis apertured illumination.

We extend coherent diffraction imaging (CDI) to a high numerical aperture reflection mode geometry for the first time. We derive a coordinate transform that allows us to rewrite the recorded far-field scatter pattern from a tilted object as a uniformly spaced Fourier transform. Using this approach, FFTs in standard iterative phase retrieval algorithms can be used to significantly speed up the image reconstruction times. Moreover, we avoid the isolated sample requirement by imaging a pinhole onto the specimen, in a technique termed apertured illumination CDI. By combining the new coordinate transformation with apertured illumination CDI, we demonstrate rapid high numerical aperture imaging of samples illuminated by visible laser light. Finally, we demonstrate future promise for this technique by using high harmonic beams for high numerical aperture reflection mode imaging.

High contrast 3D imaging of surfaces near the wavelength limit using tabletop EUV ptychography.

Scanning electron microscopy and atomic force microscopy are well-established techniques for imaging surfaces with nanometer resolution. Here we demonstrate a complementary and powerful approach based on tabletop extreme-ultraviolet ptychography that enables quantitative full field imaging with higher contrast than other techniques, and with compositional and topographical information. Using a high numerical aperture reflection-mode microscope illuminated by a tabletop 30 nm high harmonic source, we retrieve high quality, high contrast, full field images with 40 nm by 80 nm lateral resolution (≈1.3 λ), with a total exposure time of less than 1 min. Finally, quantitative phase information enables surface profilometry with ultra-high, 6 Å axial resolution. In the future, this work will enable dynamic imaging of functioning nanosystems with unprecedented combined spatial (<10 nm) and temporal (<10 fs) resolution, in thick opaque samples, with elemental, chemical and magnetic sensitivity.

Full field tabletop EUV coherent diffractive imaging in a transmission geometry.

We demonstrate the first general tabletop EUV coherent microscope that can image extended, non-isolated, non-periodic, objects. By implementing keyhole coherent diffractive imaging with curved mirrors and a tabletop high harmonic source, we achieve improved efficiency of the imaging system as well as more uniform illumination at the sample, when compared with what is possible using Fresnel zone plates. Moreover, we show that the unscattered light from a semi-transparent sample can be used as a holographic reference wave, allowing quantitative information about the thickness of the sample to be extracted from the retrieved image. Finally, we show that excellent tabletop image fidelity is achieved by comparing the retrieved images with scanning electron and atomic force microscopy images, and show superior capabilities in some cases.

Quantitative Chemically Specific Coherent Diffractive Imaging of Reactions at Buried Interfaces with Few Nanometer Precision

We demonstrate quantitative, chemically specific imaging of buried nanostructures, including oxidation and diffusion reactions at buried interfaces, using nondestructive tabletop extreme ultraviolet (EUV) coherent diffractive imaging (CDI). Copper nanostructures inlaid in SiO2 are coated with 100 nm of aluminum, which is opaque to visible light and thick enough that neither visible microscopy nor atomic force microscopy can image the buried interface. Short wavelength high harmonic beams can penetrate the aluminum layer, yielding high-contrast images of the buried structures. Quantitative analysis shows that the reflected EUV light is extremely sensitive to the formation of multiple oxide layers, as well as interdiffusion of materials occurring at the metal-metal and metal-insulator boundaries deep within the nanostructure with few nanometers precision.

Ptychographic hyperspectral spectromicroscopy with an extreme ultraviolet high harmonic comb

We report a proof-of-principle demonstration of a new scheme of spectromicroscopy in the extreme ultraviolet (EUV) spectral range, where the spectral response of the sample at different wavelengths is imaged simultaneously. This scheme is enabled by combining ptychographic information multiplexing (PIM) with a tabletop EUV source based on high harmonic generation, where four spectrally narrow harmonics near 30 nm form a spectral comb structure. Extending PIM from previously demonstrated visible wavelengths to the EUV/X-ray wavelengths promises much higher spatial resolution and a more powerful spectral contrast mechanism, making PIM an attractive spectromicroscopy method in both microscopy and spectroscopy aspects. In addition to spectromicroscopy, this method images the multicolor EUV beam in situ, making this a powerful beam characterization technique. In contrast to other methods, the techniques described here use no hardware to separate wavelengths, leading to efficient use of the EUV radiation.

Spatial, spectral, and polarization multiplexed ptychography.

We introduce a novel coherent diffraction imaging technique based on ptychography that enables simultaneous full-field imaging of multiple, spatially separate, sample locations. This technique only requires that diffracted light from spatially separated sample sites be mutually incoherent at the detector, which can be achieved using multiple probes that are separated either by wavelength or by orthogonal polarization states. This approach enables spatially resolved polarization spectroscopy from a single ptychography scan, as well as allowing a larger field of view to be imaged without loss in spatial resolution. Further, we compare the numerical efficiency of the multi-mode ptychography algorithm with a single mode algorithm.

A generalization for optimized phase retrieval algorithms

In this work, we demonstrate an improved method for iterative phase retrieval with application to coherent diffractive imaging. By introducing additional operations inside the support term of existing iterated projection algorithms, we demonstrate improved convergence speed, higher success rate and, in some cases, improved reconstruction quality. New algorithms take a particularly simple form with the introduction of a generalized projection-based reflector. Numerical simulations verify that these new algorithms surpass the current standards without adding complexity to the reconstruction process. Thus the introduction of this new class of algorithms offers a new array of methods for efficiently deconvolving intricate data.