Carl Hägglund

Electromagnetic coupling of light into a silicon solar cell by nanodisk plasmons

Photocurrents of silicon pn junctions patterned with arrays of elliptical Au nanodisks were experimentally and theoretically investigated near the particle plasmon resonance wavelengths, for varying light polarizations and angles of incidence. At plasmon resonance wavelengths, overall backscattering and dissipation were strongly enhanced compared to an unpatterned junction, resulting in lower photocurrents. In contrast, enhanced photocurrents were observed for wavelengths slightly off resonance. Measurements and finite element calculations show that the photocurrent changes occur via plasmon-induced far field effects, rather than by near field enhancement close to the particles. The far field effects are strongly dependent on the particle proximity and coupling to the Si substrate.

Enhanced charge carrier generation in dye sensitized solar cells by nanoparticle plasmons

An interesting possibility to improve the conversion and cost efficiencies of photovoltaic solar cells is to exploit the large optical cross sections of localized (nanoparticle) surface plasmon resonances (LSPRs). We have investigated this prospect for dye sensitized solar cells. Photoconductivity measurements were performed on flat TiO2 films, sensitized by a combination of dye molecules and arrays of nanofabricated elliptical gold disks. An enhanced dye charge carrier generation rate was found and shown to derive from the LSPR contribution by means of the polarization dependent resonance frequency in the anisotropic, aligned gold disks.

Enhanced nanoplasmonic optical sensors with reduced substrate effect.

We present a straightforward method to double the refractive index sensitivity of surface-supported nanoplasmonic optical sensors by lifting the metal nanoparticles above the substrate by a dielectric nanopillar. The role of the pillar is to substantially decrease the spatial overlap between the substrate and the enhanced fields generated at plasmon resonance. Data presented for nanodisks and nanoellipsoids supported by pillars of varying heights are found to be in excellent agreement with electrodynamics simulations. The described concepts apply to multitude of plasmonic nanostructures, fabricated by top-down or bottom-up techniques, and are likely to further facilitate the development of novel nanooptical sensors for biomedicine and diagnostics.

Plasmonic Near-Field Absorbers for Ultrathin Solar Cells

If the active layer of efficient solar cells could be made 100 times thinner than in todays thin film devices, their economic competitiveness would greatly benefit. However, conventional solar cell materials do not have the optical capability to allow for such thickness reductions without a substantial loss of light absorption. To address this challenge, the use of plasmon resonances in metal nanostructures to trap light and create charge carriers in a nearby semiconductor material is an interesting opportunity. In this Perspective, recent progress with regards to ultrathin (∼10 nm) plasmonic nanocomposites is reviewed. Their optimal internal geometry for plasmon near-field induced absorption is discussed, and a zero thickness effective medium representation is used to optimize stacks including an Al back reflector for photovoltaics. This shows that high conversion efficiencies (>20%) are possible even when taking surface scattering effects and thin passivating layers inserted between the metal and semiconductor into account.

Maximized Optical Absorption in Ultrathin Films and Its Application to Plasmon-Based Two-Dimensional Photovoltaics

For ultrathin films of a given material, light absorption is proportional to the film thickness. However, if the optical constants of the film are chosen in an optimal way, light absorption can be high even for extremely thin films and optical path length. We derive the optimal conditions and show how the maximized absorptance depends on film thickness. It is then shown that the optimal situation can be emulated by tuning of the geometric parameters in feasible nanocomposites combining plasmonic materials with semiconductors. Useful design criteria and estimates for the spatial absorption-distribution over the composite materials are provided. On the basis of efficient exchange of oscillator strength between the plasmonic and semiconductor constituents, a high quantum yield for semiconductor absorption can be achieved. The results are far-reaching with particularly promising opportunities for plasmonic solar cells.

Self-assembly based plasmonic arrays tuned by atomic layer deposition for extreme visible light absorption.

Achieving complete absorption of visible light with a minimal amount of material is highly desirable for many applications, including solar energy conversion to fuel and electricity, where benefits in conversion efficiency and economy can be obtained. On a fundamental level, it is of great interest to explore whether the ultimate limits in light absorption per unit volume can be achieved by capitalizing on the advances in metamaterial science and nanosynthesis. Here, we combine block copolymer lithography and atomic layer deposition to tune the effective optical properties of a plasmonic array at the atomic scale. Critical coupling to the resulting nanocomposite layer is accomplished through guidance by a simple analytical model and measurements by spectroscopic ellipsometry. Thereby, a maximized absorption of light exceeding 99% is accomplished, of which up to about 93% occurs in a volume-equivalent thickness of gold of only 1.6 nm. This corresponds to a record effective absorption coefficient of 1.7 × 10(7) cm(-1) in the visible region, far exceeding those of solid metals, graphene, dye monolayers, and thin film solar cell materials. It is more than a factor of 2 higher than that previously obtained using a critically coupled dye J-aggregate, with a peak width exceeding the latter by 1 order of magnitude. These results thereby substantially push the limits for light harvesting in ultrathin, nanoengineered systems.

Nanoparticle Plasmonics for 2D-Photovoltaics: Mechanisms, Optimization, and Limits

Plasmonic nanostructures placed within or near photovoltaic (PV) layers are of high current interest for improving thin film solar cells. We demonstrate, by electrodynamics calculations, the feasibility of a new class of essentially two dimensional (2D) solar cells based on the very large optical cross sections of plasmonic nanoparticles. Conditions for inducing absorption in extremely thin PV layers via plasmon near-fields, are optimized in 2D-arrays of (i) core-shell particles, and (ii) plasmonic particles on planar layers. At the plasmon resonance, a pronounced optimum is found for the extinction coefficient of the PV material. We also characterize the influence of the dielectric environment, PV layer thickness and nanoparticle shape, size and spatial distribution. The response of the system is close to that of a 2D effective medium layer, and subject to a 50% absorption limit when the dielectric environment around the 2D layer is symmetric. In this case, a plasmon induced absorption of about 40% is demonstrated in PV layers as thin as 10 nm, using silver nanoparticle arrays of only 1 nm effective thickness. In an asymmetric environment, the useful absorption may be increased significantly for the same layer thicknesses. These new types of essentially 2D solar cells are concluded to have a large potential for reducing solar electricity costs.

Tin oxide atomic layer deposition from tetrakis(dimethylamino)tin and water

Due to the abundance and usefulness of tin oxide for applications such as transparent conductors, sensors, and catalysts, it is desirable to establish high quality atomic layer deposition (ALD) of this material. ALD allows for uniform, conformal coating of complex topographies with ultrathin films and can broaden the applicability of tin oxide to systems such as nanostructured solar cells. The present work examines the ALD of tin oxide by means of the precursor tetrakis(dimethylamino)tin and water as a counter-reactant. Low temperature growth in the range of 30–200 °C on Si(100) and glass substrates is studied. It is found that the growth rate increases with reduced temperature, up to ∼2.0 A/cycle at 30 °C, as compared to 0.70 A/cycle at 150 °C. The ALD process is established to be saturated even at the lowest temperature studied, for which the film contamination levels are below the detection limits of x-ray photoelectron spectroscopy. As-deposited films are smooth (rms roughness of 33 A for a 460 A thic...

Vapor transport deposition and epitaxy of orthorhombic SnS on glass and NaCl substrates

Polycrystalline SnS, Sn2S3, and SnS2 were deposited onto glass substrates by vapor transport deposition, with the stoichiometry controlled by deposition temperature. In addition, epitaxial growth of orthorhombic SnS(010) films on NaCl(100) with thicknesses up to 600 nm was demonstrated. The in-plane [100] directions of SnS and NaCl are oriented approximately 45° apart, and the translational relationship between SnS and NaCl was predicted by density functional theory. The epitaxial SnS is p-type with carrier concentration on the order of 1017 cm−3 and Hall hole mobility of 385 cm2 V−1 s−1 in-plane. It has indirect and direct bandgaps of 1.0 and 2.3 eV, respectively.

Growth characteristics, material properties, and optical properties of zinc oxysulfide films deposited by atomic layer deposition

Zinc oxysulfide—Zn(O,S)—is a wide bandgap semiconductor with tunable electronic and optical properties, making it of potential interest as a buffer layer for thin film photovoltaics. Atomic layer deposition (ALD) of ZnS, ZnO, and Zn(O,S) films from dimethylzinc, H2O, and H2S was performed, and the deposited films were characterized by means of x-ray diffraction, x-ray photoelectron spectroscopy, and spectroscopic ellipsometry. With focus on the investigation of Zn(O,S) film growth characteristics and material properties, the ZnO/(ZnO + ZnS) ALD cycle ratios were systematically varied from 0 (ZnS ALD) to 1 (ZnO ALD). Notably, a strong effect ofthematerial properties on the optical characteristics is confirmed for the ternary films. The Zn(O,S) ALD growth and crystal structure resemble those of ZnS up to a 0.6 cycle ratio, at whichpoint XPS indicates 10% oxygen is incorporated into the film. For higher cycle ratios thefilm structure becomes amorphous, which is confirmed with XRD patterns and also reflected ...