Investigation of the Photocatalytic Hydrogen Production of Semiconductor Nanocrystal-Based Hydrogels

Destabilization of a ligand-stabilized semiconductor nanocrystal solution with an oxidizing agent can lead to a macroscopic highly porous self-supporting nanocrystal network entitled hydrogel, with good accessibility to the surface. The previously reported charge carrier delocalization beyond a single nanocrystal building block in such gels can extend the charge carrier mobility and make a photocatalytic reaction more probable. The synthesis of ligand-stabilized nanocrystals with specific physicochemical properties is possible, thanks to the advances in colloid chemistry made in the last decades. Combining the properties of these nanocrystals with the advantages of nanocrystal-based hydrogels will lead to novel materials with optimized photocatalytic properties. This work demonstrates that CdSe quantum dots, CdS nanorods, and CdSe/CdS dot-in-rod-shaped nanorods as nanocrystal-based hydrogels can exhibit a much higher hydrogen production rate compared to their ligand-stabilized nanocrystal solutions. The gel synthesis through controlled destabilization by ligand oxidation preserves the high surface-to-volume ratio, ensures the accessible surface area even in hole-trapping solutions and facilitates photocatalytic hydrogen production without a co-catalyst. Especially with such self-supporting networks of nanocrystals, the problem of colloidal (in)stability in photocatalysis is circumvented. X-ray photoelectron spectroscopy and photoelectrochemical measurements reveal the advantageous properties of the 3D networks for application in photocatalytic hydrogen production

Publications of the Jet Propulsion Laboratory, January through December 1974

Formalized technical reporting is described and indexed, which resulted from scientific and engineering work performed, or managed, by the Jet Propulsion Laboratory. The five classes of publications included are technical reports, technical memorandums, articles from the bimonthly Deep Space Network Progress Report, special publications, and articles published in the open literature. The publications are indexed by author, subject, and publication type and number

Shape Evolution of Nanostructures by Thermal and Ion Beam Processing: Modeling & Atomistic Simulations

Single-crystalline nanostructures often exhibit gradients of surface (and/or interface) curvature that emerge from fabrication and growth processes or from thermal fluctuations. Thus, the system-inherent capillary force can initiate morphological transformations during further processing steps or during operation at elevated temperature. Therefore and because of the ongoing miniaturization of functional structures which causes a general rise in surface-to-volume ratios, solid-state capillary phenomena will become increasingly important: On the one hand diffusion-mediated capillary processes can be of practical use in view of non-conventional nanostructure fabrication methods based on self-organization mechanisms, on the other hand they can destroy the integrity of nanostructures which can go along with the failure of functionality. Additionally, capillarity-induced shape transformations are effected and can thereby be controlled by applied fields and forces (guided or driven evolution). With these prospects and challenges at hand, formation and shape transformation of single-crystalline nanostructures due to the system-inherent capillary force in combination with external fields or forces are investigated in the frame of this dissertation by means of atomistic computer simulations. For the exploration (search, description, and prediction) of reaction pathways of nanostructure shape transformations, kinetic Monte Carlo (KMC) simulations are the method of choice. Since the employed KMC code is founded on a cellular automaton principle, the spatio-temporal development of lattice-based N-particle systems (N up to several million) can be followed for time spans of several orders of magnitude, while considering local phenomena due to atomic-scale effects like diffusion, nucleation, dissociation, or ballistic displacements. In this work, the main emphasis is put on nanostructures which have a cylindrical geometry, for example, nanowires (NWs), nanorods, nanotubes etc

Metal Oxide Nanomaterials

This is a timely collection of recent diverse work on metal oxide nanomaterials, connecting their fundamental aspects and application perspectives in a concise fashion to give a broad view of the current status of this fascinating field. This book presents eight original research articles and two comprehensive reviews to highlight the recent development and understanding of different types of metal oxide nanoparticles and their use for applications in luminescence, photocatalysis, water–oil separation, optoelectronics, gas sensors, energy-saving smart windows, etc. It presents just the tip of the iceberg of the broad, dynamic, and active fundamental research and applications in the developing field of metal oxide nanomaterials by collecting a few examples of the latest advancements

Rigorous direct and inverse design of photonic-plasmonic nanostructures

Designing photonic-plasmonic nanostructures with desirable electromagnetic properties is a central problem in modern photonics engineering. As limited by available materials, engineering geometry of optical materials at both element and array levels becomes the key to solve this problem. In this thesis, I present my work on the development of novel methods and design strategies for photonic-plasmonic structures and metamaterials, including novel Green’s matrix-based spectral methods for predicting the optical properties of large-scale nanostructures of arbitrary geometry. From engineering elements to arrays, I begin my thesis addressing toroidal electrodynamics as an emerging approach to enhance light absorption in designed nanodisks by geometrically creating anapole configurations using high-index dielectric materials. This work demonstrates enhanced absorption rates driven by multipolar decomposition of current distributions involving toroidal multipole moments for the first time. I also present my work on designing helical nano-antennas using the rigorous Surface Integral Equations method. The helical nano-antennas feature unprecedented beam-forming and polarization tunability controlled by their geometrical parameters, and can be understood from the array perspective. In these projects, optimization of optical performances are translated into systematic study of identifiable geometric parameters. However, while array-geometry engineering presents multiple advantages, including physical intuition, versatility in design, and ease of fabrication, there is currently no rigorous and efficient solution for designing complex resonances in large-scale systems from an available set of geometrical parameters. In order to achieve this important goal, I developed an efficient numerical code based on the Green’s matrix method for modeling scattering by arbitrary arrays of coupled electric and magnetic dipoles, and show its relevance to the design of light localization and scattering resonances in deterministic aperiodic geometries. I will show how universal properties driven by the aperiodic geometries of the scattering arrays can be obtained by studying the spectral statistics of the corresponding Green’s matrices and how this approach leads to novel metamaterials for the visible and near-infrared spectral ranges. Within the thesis, I also present my collaborative works as examples of direct and inverse designs of nanostructures for photonics applications, including plasmonic sensing, optical antennas, and radiation shaping

Annual Report 2009 - Institute of Ion Beam Physics and Materials Research

The Institute of Ion Beam Physics and Materials Research (IIM) is one of the six institutes of the Forschungszentrum Dresden-Rossendorf (FZD), and contributes the largest part to its Research Program \"Advanced Materials\", mainly in the fields of semiconductor physics and materials research using ion beams. The institute operates a national and international Ion Beam Center, which, in addition to its own scientific activities, makes available fast ion technologies to universities, other research institutes, and industry. Parts of its activities are also dedicated to exploit the infrared/THz free-electron laser at the 40 MeV superconducting electron accelerator ELBE for condensed matter research. For both facilities the institute holds EU grants for funding access of external users

Recent Advances in Linear and Nonlinear Optics

Sight is the dominant sense of mankind to apprehend the world at the earth scale and beyond the frontiers of the infinite, from the nanometer to the incommensurable. Primarily based on sunlight and natural and artificial light sources, optics has been the major companion of spectroscopy since scientific observation began. The invention of the laser in the early sixties has boosted optical spectroscopy through the intrinsic or specific symmetry electronic properties of materials at the multiscale (birefringence, nonlinear and photonic crystals), revealed by the ability to monitor light polarization inside or on the surface of designed objects. This Special Issue of Symmetry features articles and reviews that are of tremendous interest to scientists who study linear and nonlinear optics, all oriented around the common axis of symmetry. Contributions transverse the entire breadth of this field, including those concerning polarization and anisotropy within colloids of chromophores and metal/semiconducting nanoparticles probed by UV-visible and fluorescence spectroscopies; microscopic structures of liquid–liquid, liquid–gas, and liquid–solid interfaces; surface- and symmetry-specific optical techniques and simulations, including second-harmonic and sum-frequency generations, and surface-enhanced and coherent anti-Stokes Raman spectroscopies; orientation and chirality of bio-molecular interfaces; symmetry breaking in photochemistry; symmetric multipolar molecules; reversible electronic energy transfer within supramolecular systems; plasmonics; and light polarization effects in materials