arXiv subjects

Harry A. Atwater

Publications and source records attributed to Harry A. Atwater.

At least 55 records · Page 3Linked to original sources

arXiv2017

Van der Waals Materials for Atomically-Thin Photovoltaics: Promise and Outlook

Two-dimensional (2D) semiconductors provide a unique opportunity for optoelectronics due to their layered atomic structure, electronic and optical properties. To date, a majority of the application-oriented research in this field has been focused on field-effect electronics as well as photodetectors and light emitting diodes. Here we present a perspective on the use of 2D semiconductors for photovoltaic applications. We discuss photonic device designs that enable light trapping in nanometer-thickness absorber layers, and we also outline schemes for efficient carrier transport and collection. We further provide theoretical estimates of efficiency indicating that 2D semiconductors can indeed be competitive with and complementary to conventional photovoltaics, based on favorable energy bandgap, absorption, external radiative efficiency, along with recent experimental demonstrations. Photonic and electronic design of 2D semiconductor photovoltaics represents a new direction for realizing ultrathin, efficient solar cells with applications ranging from conventional power generation to portable and ultralight solar power.

physics.optics↗

arXiv2017

Extremely broadband ultralight thermally emissive metasurfaces

We report the design, fabrication and characterization of ultralight highly emissive metaphotonic structures with record-low mass/area that emit thermal radiation efficiently over a broad spectral (2 to 35 microns) and angular (0-60 degrees) range. The structures comprise one to three pairs of alternating nanometer-scale metallic and dielectric layers, and have measured effective 300 K hemispherical emissivities of 0.7 to 0.9. To our knowledge, these structures, which are all subwavelength in thickness are the lightest reported metasurfaces with comparable infrared emissivity. The superior optical properties, together with their mechanical flexibility, low outgassing, and low areal mass, suggest that these metasurfaces are candidates for thermal management in applications demanding of ultralight flexible structures, including aerospace applications, ultralight photovoltaics, lightweight flexible electronics, and textiles for thermal insulation.

physics.app-ph↗

arXiv2017

Electrical Control of Linear Dichroism in Black Phosphorus from the Visible to Mid-Infrared

The incorporation of electrically tunable materials into photonic structures such as waveguides and metasurfaces enables dynamic control of light propagation by an applied potential. While many materials have been shown to exhibit electrically tunable permittivity and dispersion, including transparent conducting oxides (TCOs) and III-V semiconductors and quantum wells, these materials are all optically isotropic in the propagation plane. In this work, we report the first known example of electrically tunable linear dichroism, observed here in few-layer black phosphorus (BP), which is a promising candidate for multi-functional, broadband, tunable photonic elements. We measure active modulation of the linear dichroism from the mid-infrared to visible frequency range, which is driven by anisotropic quantum-confined Stark and Burstein-Moss effects, and field-induced forbidden-to-allowed optical transitions. Moreover, we observe high BP absorption modulation strengths, approaching unity for certain thicknesses and photon energies.

cond-mat.mes-hall↗

arXiv2017

Purcell Enhancement of Parametric Luminescence: Bright and Broadband Nonlinear Light Emission in Metamaterials

Single-photon and correlated two-photon sources are important elements for optical information systems. Nonlinear downconversion light sources are robust and stable emitters of single photons and entangled photon pairs. However, the rate of downconverted light emission, dictated by the properties of low-symmetry nonlinear crystals, is typically very small, leading to significant constrains in device design and integration. In this paper, we show that the principles for spontaneous emission control (i.e. Purcell effect) of isolated emitters in nanoscale structures, such as metamaterials, can be generalized to describe the enhancement of nonlinear light generation processes such as parametric down conversion. We develop a novel theoretical framework for quantum nonlinear emission in a general anisotropic, dispersive and lossy media. We further find that spontaneous parametric downconversion in media with hyperbolic dispersion is broadband and phase-mismatch-free. We predict a 1000-fold enhancement of the downconverted emission rate with up to 105 photon pairs per second in experimentally realistic nanostructures. Our theoretical formalism and approach to Purcell enhancement of nonlinear optical processes, provides a framework for description of quantum nonlinear optical phenomena in complex nanophotonic structures.

physics.optics↗

arXiv2017

Micro-optical Tandem Luminescent Solar Concentrators

Traditional concentrating photovoltaic (CPV) systems utilize multijunction cells to minimize thermalization losses, but cannot efficiently capture diffuse sunlight, which contributes to a high levelized cost of energy (LCOE) and limits their use to geographical regions with high direct sunlight insolation. Luminescent solar concentrators (LSCs) harness light generated by luminophores embedded in a light-trapping waveguide to concentrate light onto smaller cells. LSCs can absorb both direct and diffuse sunlight, and thus can operate as flat plate receivers at a fixed tilt and with a conventional module form factor. However, current LSCs experience significant power loss through parasitic luminophore absorption and incomplete light trapping by the optical waveguide. Here we introduce a tandem LSC device architecture that overcomes both of these limitations, consisting of a PLMA polymer layer with embedded CdSe/CdS quantum dot (QD) luminophores and InGaP micro-cells, which serve as a high bandgap absorber on top of a conventional Si photovoltaic. We experimentally synthesize CdSe/CdS QDs with exceptionally high quantum-yield (99%) and ultra-narrowband emission optimally matched to fabricated III-V InGaP micro-cells. Using a Monte Carlo ray-tracing model, we show the radiative limit power conversion efficiency for a module with these components to be 30.8% diffuse sunlight conditions. These results indicate that a tandem LSC-on-Si architecture could significantly improve upon the efficiency of a conventional Si photovoltaic module with simple and straightforward alterations of the module lamination steps of a Si photovoltaic manufacturing process, with promise for widespread module deployment across diverse geographical regions and energy markets.

physics.app-ph↗

arXiv2017

Limits to the Optical Response of Graphene and 2D Materials

2D materials provide a platform for strong light--matter interactions, creating wide-ranging design opportunities via new-material discoveries and new methods for geometrical structuring. We derive general upper bounds to the strength of such light--matter interactions, given only the optical conductivity of the material, including spatial nonlocality, and otherwise independent of shape and configuration. Our material figure of merit shows that highly doped graphene is an optimal material at infrared frequencies, whereas single-atomic-layer silver is optimal in the visible. For quantities ranging from absorption and scattering to near-field spontaneous-emission enhancements and radiative heat transfer, we consider canonical geometrical structures and show that in certain cases the bounds can be approached, while in others there may be significant opportunity for design improvement. The bounds can encourage systematic improvements in the design of ultrathin broadband absorbers, 2D antennas, and near-field energy harvesters.

physics.optics↗

arXiv2017

High Photovoltaic Quantum Efficiency in Ultrathin van der Waals Heterostructures

We report experimental measurements for ultrathin (< 15 nm) van der Waals heterostructures exhibiting external quantum efficiencies exceeding 50%, and show that these structures can achieve experimental absorbance > 90%. By coupling electromagnetic simulations and experimental measurements, we show that pn WSe2/MoS2 heterojunctions with vertical carrier collection can have internal photocarrier collection efficiencies exceeding 70%.

cond-mat.mes-hall↗

arXiv2017

Monolithic Photoelectrochemical Device for 19% Direct Water Splitting

Recent rapid progress in efficiencies for solar water splitting by photoelectrochemical devices has enhanced its prospects to enable storable renewable energy. Efficient solar fuel generators all use tandem photoelectrode structures, and advanced integrated devices incorporate corrosion protection layers as well as heterogeneous catalysts. Realization of near thermodynamic limiting performance requires tailoring the energy band structure of the photoelectrode and also the optical and electronic properties of the surface layers exposed to the electrolyte. Here, we report a monolithic device architecture that exhibits reduced surface reflectivity in conjunction with metallic Rh nanoparticle catalyst layers that minimize parasitic light absorption. Additionally, the anatase TiO2 protection layer on the photocathode creates a favorable internal band alignment for hydrogen evolution. An initial solar-to-hydrogen efficiency of 19.3 % is obtained in acidic electrolyte and an efficiency of 18.5 % is achieved at neutral pH condition (under simulated sunlight).

cond-mat.mtrl-sci↗

arXiv2017

Atomic-scale Structural and Chemical Characterization of Hexagonal Boron Nitride Layers Synthesized at the Wafer-Scale with Monolayer Thickness Control

Hexagonal boron nitride (h-BN) is a promising two-dimensional insulator with a large band gap and low density of charged impurities that is isostructural and isoelectronic with graphene. Here we report the chemical and atomic-scale structure of CVD-grown wafer-scale (~25 cm2) h-BN sheets ranging in thickness from 1-20 monolayers. Atomic-scale images of h-BN on Au and graphene/Au substrates obtained by scanning tunneling microscopy (STM) reveal high h-BN crystalline quality in monolayer samples. Further characterization of 1-20 monolayer samples indicates uniform thickness for wafer-scale areas; this thickness control is a result of precise control of the precursor flow rate, deposition temperature and pressure. Raman and infrared spectroscopy indicate the presence of B-N bonds and reveal a linear dependence of thickness with growth time. X-ray photoelectron spectroscopy (XPS) shows the film stoichiometry, and the B/N atom ratio in our films is 1 + 0.6% across the range of thicknesses. Electrical current transport in metal/insulator/metal (Au/h-BN/Au) heterostructures indicates that our CVD-grown h-BN films can act as excellent tunnel barriers with a high hard-breakdown field strength. Our results suggest that large-area h-BN films are structurally, chemically and electronically uniform over the wafer scale, opening the door to pervasive application as a dielectric in layered nanoelectronic and nanophotonic heterostructures.

physics.app-ph↗

arXiv2017

Optical Magnetism in Planar Metamaterial Heterostructures

Harnessing artificial optical magnetism requires rather complex two- and three-dimensional structures, examples include split-ring and fishnet metamaterials and nanoparticles with non-trivial magnetic properties. By contrast, dielectric properties can be tailored even in planar and pattern-free, one-dimensional (1D) arrangements, for example metal/dielectric multilayer metamaterials. These systems are extensively investigated due to their hyperbolic and plasmonic response, which, however, is considered to be limited to TM polarization, based on the general consensus that they do not possess interesting magnetic properties. In this work, we tackle these two seemingly unrelated issues simultaneously, by proposing conceptually and demonstrating experimentally a mechanism for artificial magnetism in planar, 1D metamaterials. We show experimentally that the magnetic response of metal/high-index dielectric hyperbolic metamaterials can be anisotropic, leading to frequency regimes of magnetic hyperbolic dispersion. We investigate the implications of our results for TE polarization and show that such systems can support TE interface-bound states, analogous to their TM counterparts, surface plasmon polaritons. Our results simplify the structural complexity for tailoring artificial magnetism in lithography-free systems and generalize the concept of plasmonic and hyperbolic properties to encompass both TE and TM polarizations at optical frequencies.

physics.optics↗

arXiv2017

Electronically Tunable Perfect Absorption in Graphene

Graphene nanostructures that support surface plasmons have been utilized to create a variety of dynamically tunable light modulators, motivated by theoretical predictions of the potential for unity absorption in resonantly-excited monolayer graphene sheets. Until now, the generally low efficiencies of tunable resonant graphene absorbers have been limited by the mismatch between free-space photons and graphene plasmons. Here, we develop nanophotonic structures that overcome this mismatch and demonstrate electronically tunable perfect absorption achieved with patterned graphenes covering less than 10% of the surface. Experimental measurements reveal 96.9% absorption in the graphene plasmonic nanostructure at 1,389 cm$^{-1}$, with an on/off modulation efficiency of 95.9% in reflection. An analytic effective surface admittance model elucidates the origin of perfect absorption, which is design for critical coupling between free-space modes and the graphene plasmonic nanostructures.

physics.optics↗

arXiv2017

Three-dimensional nanoimprint lithography using two-photon lithography master samples

We demonstrate three-dimensional (3-D) nanoimprint lithography using master samples initially structured by two-photon lithography. Complex geometries like micro prisms, micro parabolic concentrators, micro lenses and other micrometer sized objects with nanoscale features are three-dimensionally fabricated using two-photon lithography. Stamps made out of polydimethylsiloxane are then cast using the two-photon lithographically structured samples as master samples. Hereby, expensive serial nano 3-D printing is transformed into scalable parallel 3-D nanoimprint lithography. Furthermore, the transition from two-photon lithography to imprint lithography increases the freedom in substrate and ink choice significantly. We demonstrate printing on textured surfaces as well as residue-free printing with silver ink using capillary action.

cond-mat.mes-hall↗

arXiv2017

Experimental Demonstration of >230° Phase Modulation in Gate-Tunable Graphene-Gold Reconfigurable Mid-Infrared Metasurfaces

Metasurfaces offer significant potential to control far-field light propagation through the engineering of amplitude, polarization, and phase at an interface. We report here phase modulation of an electronically reconfigurable metasurface and demonstrate its utility for mid-infrared beam steering. Using a gate-tunable graphene-gold resonator geometry, we demonstrate highly tunable reflected phase at multiple wavelengths and show up to 237° phase modulation range at an operating wavelength of 8.50 μm. We observe a smooth monotonic modulation of phase with applied voltage from 0° to 206° at a wavelength of 8.70 μm. Based on these experimental data, we demonstrate with antenna array calculations an average beam steering efficiency of 50% for reflected light for angles up to 30°, relative to an ideal metasurface, confirming the suitability of this geometry for reconfigurable mid-infrared beam steering devices.

cond-mat.mes-hall↗

arXiv2017

Field Effect Optoelectronic Modulation of Quantum-Confined Carriers in Black Phosphorus

We report measurements of the infrared optical response of thin black phosphorus under field-effect modulation. We interpret the observed spectral changes as a combination of an ambipolar Burstein-Moss (BM) shift of the absorption edge due to band-filling under gate control, and a quantum confined Franz-Keldysh (QCFK) effect, phenomena which have been proposed theoretically to occur for black phosphorus under an applied electric field. Distinct optical responses are observed depending on the flake thickness and starting carrier concentration. Transmission extinction modulation amplitudes of more than two percent are observed, suggesting the potential for use of black phosphorus as an active material in mid-infrared optoelectronic modulator applications.

cond-mat.mes-hall↗

arXiv2016

Experimental and ab initio ultrafast carrier dynamics in plasmonic nanoparticles

Ultrafast pump-probe measurements of plasmonic nanostructures probe the non-equilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations of carrier dynamics and optical response, free of any fitting parameters. We account for detailed electronic-structure effects in the density of states, excited carrier distributions, electron-phonon coupling, and dielectric functions which allow us to avoid effective electron temperature approximations. Using this calculation method, we obtain excellent quantitative agreement with spectral and temporal features in transient-absorption measurements. In both our experiments and calculations, we identify the two major contributions of the initial response with distinct signatures: short-lived highly non-thermal excited carriers and longer-lived thermalizing carriers.

physics.optics↗

arXiv2016

Gate-Variable Mid-Infrared Optical Transitions in a $(Bi_{1-x}Sb_x)_2Te_3$ Topological Insulator

We report mid-infrared spectroscopy measurements of an electrostatically gated topological insulator, in which we observe several percent modulation of transmittance and reflectance of (Bi1-xSbx)2Te3 films as gating shifts the Fermi level. Infrared transmittance measurements of gated (Bi1-xSbx)2Te3 films were enabled by use of an epitaxial lift-off method for large-area transfer of topological insulator films from infrared-absorbing SrTiO3 growth substrates to thermal oxidized silicon substrates. We combine these optical experiments with transport measurements and angle-resolved photoemission spectroscopy to identify the observed spectral modulation as a gate-driven transfer of spectral weight between both bulk and topological surface channels and interband and intraband channels. We develop a model for the complex permittivity of gated (Bi1-xSbx)2Te3, and find a good match to our experimental data. These results open the path for layered topological insulator materials as a new candidate for tunable infrared optics and highlight the possibility of switching topological optoelectronic phenomena between bulk and spin-polarized surface regimes.

cond-mat.mes-hall↗

arXiv2016

Near Unity Absorption in Van der Waals Semiconductors for Ultrathin Optoelectronics

We demonstrate near unity, broadband absorbing optoelectronic devices using sub-15 nm thick transition metal dichalcogenides (TMDCs) of molybdenum and tungsten as van der Waals semiconductor active layers. Specifically, we report that near-unity light absorption is possible in extremely thin (< 15 nm) Van der Waals semiconductor structures by coupling to strongly damped optical modes of semiconductor/metal heterostructures. We further fabricate Schottky junction devices using these highly absorbing heterostructures and characterize their optoelectronic performance. Our work addresses one of the key criteria to enable TMDCs as potential candidates to achieve high optoelectronic efficiency.

cond-mat.mtrl-sci↗

arXiv2016

Ab initio phonon coupling and optical response of hot electrons in plasmonic metals

Ultrafast laser measurements probe the non-equilibrium dynamics of excited electrons in metals with increasing temporal resolution. Electronic structure calculations can provide a detailed microscopic understanding of hot electron dynamics, but a parameter-free description of pump-probe measurements has not yet been possible, despite intensive research, because of the phenomenological treatment of electron-phonon interactions. We present ab initio predictions of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We find substantial differences from free-electron and semi-empirical estimates, especially in noble metals above transient electron temperatures of 2000 K, because of the previously-neglected strong dependence of electron-phonon matrix elements on electron energy. We also present first-principles calculations of the electron-temperature dependent dielectric response of hot electrons in plasmonic metals, including direct interband and phonon-assisted intraband transitions, facilitating complete theoretical predictions of the time-resolved optical probe signatures in ultrafast laser experiments.

physics.comp-ph↗