Scalable, economical, and stable sequestration of agricultural fixed carbon.

We describe a scalable, economical solution to the carbon dioxide problem. CO2 is captured from the atmosphere by plants, and the harvested vegetation is then buried in an engineered dry biolandfill. Plant biomass can be preserved for hundreds to thousands of years by burial in a dry environment with sufficiently low thermodynamic "Water Activity," which is the relative humidity in equilibrium with the biomass. Maintaining a dry environment within the engineered dry biolandfill is assisted by salt that preserves biomass, which has been known since Biblical times. A "Water Activity" <60%, assisted by salt, will not support life, suppressing anaerobic organisms, thus preserving the biomass for thousands of years. Current agricultural costs, and biolandfill costs, indicate US$60/tonne of sequestered CO2 which corresponds to ~US$0.53 per gallon of gasoline. The technology is scalable owing to the large area of land available for nonfood biomass sources. If biomass production is scaled to the level of a major crop, existing CO2 can be extracted from the atmosphere, and will simultaneously sequester a significant fraction of world CO2 emissions.

Efficient spontaneous emission by metal-dielectric antennas; antenna Purcell factor explained.

The rate of spontaneous emission from an optical emitter can be greatly enhanced using a metallic optical antenna at the penalty of efficiency. In this paper we propose a metal-dielectric antenna that eliminates the tradeoff between spontaneous emission enhancement and radiative efficiency by using nanoscopic dielectric structures at the antenna tips. This tradeoff occurs due to Ohmic loss and is further exacerbated by electron surface collisions. We find that our metal-dielectric antenna can enhance spontaneous emission by a factor 5 × 105 with efficiency = 70%, greatly exceeding the radiative efficiency of a purely metallic antenna with similar enhancement. Moreover, the metal-dielectric antenna design strategy is naturally amenable to short-distance optical communications applications. We go on to discuss the Purcell effect within the context of antenna enhancement. Metallic optical antennas are best analyzed with conventional antenna circuit models, but if the Purcell enhancement were to be employed, we provide the effective mode volume, Veff = (3/4π2)2d2λ(λ/l)5, that would be needed.

Physics successfully implements Lagrange multiplier optimization.

Optimization is a major part of human effort. While being mathematical, optimization is also built into physics. For example, physics has the Principle of Least Action; the Principle of Minimum Power Dissipation, also called Minimum Entropy Generation; and the Variational Principle. Physics also has Physical Annealing, which, of course, preceded computational Simulated Annealing. Physics has the Adiabatic Principle, which, in its quantum form, is called Quantum Annealing. Thus, physical machines can solve the mathematical problem of optimization, including constraints. Binary constraints can be built into the physical optimization. In that case, the machines are digital in the same sense that a flip-flop is digital. A wide variety of machines have had recent success at optimizing the Ising magnetic energy. We demonstrate in this paper that almost all those machines perform optimization according to the Principle of Minimum Power Dissipation as put forth by Onsager. Further, we show that this optimization is in fact equivalent to Lagrange multiplier optimization for constrained problems. We find that the physical gain coefficients that drive those systems actually play the role of the corresponding Lagrange multipliers.

Inverse design optimization for efficient coupling of an electrically injected optical antenna-LED to a single-mode waveguide.

Efficient high-speed nanoscale optical sources are required for low-power next-generation data communication. Here we propose an integrated antenna-LED on a single-mode optical waveguide. By leveraging inverse design optimization, we achieved a waveguide coupling efficiency of 94% and an antenna efficiency of 64%, while maintaining a high average enhancement of 144 - potentially enabling >100GHz direct modulation.

Ultraefficient thermophotovoltaic power conversion by band-edge spectral filtering.

Thermophotovoltaic power conversion utilizes thermal radiation from a local heat source to generate electricity in a photovoltaic cell. It was shown in recent years that the addition of a highly reflective rear mirror to a solar cell maximizes the extraction of luminescence. This, in turn, boosts the voltage, enabling the creation of record-breaking solar efficiency. Now we report that the rear mirror can be used to create thermophotovoltaic systems with unprecedented high thermophotovoltaic efficiency. This mirror reflects low-energy infrared photons back into the heat source, recovering their energy. Therefore, the rear mirror serves a dual function; boosting the voltage and reusing infrared thermal photons. This allows the possibility of a practical >50% efficient thermophotovoltaic system. Based on this reflective rear mirror concept, we report a thermophotovoltaic efficiency of 29.1 ± 0.4% at an emitter temperature of 1,207 °C.

Electrical suppression of all nonradiative recombination pathways in monolayer semiconductors.

Defects in conventional semiconductors substantially lower the photoluminescence (PL) quantum yield (QY), a key metric of optoelectronic performance that directly dictates the maximum device efficiency. Two-dimensional transition-metal dichalcogenides (TMDCs), such as monolayer MoS2, often exhibit low PL QY for as-processed samples, which has typically been attributed to a large native defect density. We show that the PL QY of as-processed MoS2 and WS2 monolayers reaches near-unity when they are made intrinsic through electrostatic doping, without any chemical passivation. Surprisingly, neutral exciton recombination is entirely radiative even in the presence of a high native defect density. This finding enables TMDC monolayers for optoelectronic device applications as the stringent requirement of low defect density is eased.

Fundamental Efficiency Limit of Lead Iodide Perovskite Solar Cells.

Lead halide materials have seen a recent surge of interest from the photovoltaics community following the observation of surprisingly high photovoltaic performance, with optoelectronic properties similar to GaAs. This begs the question: What is the limit for the efficiency of these materials? It has been known that under 1-sun illumination the efficiency limit of crystalline silicon is ∼29%, despite the Shockley-Queisser (SQ) limit for its bandgap being ∼33%: the discrepancy is due to strong Auger recombination. In this article, we show that methyl ammonium lead iodide (MAPbI3) likewise has a larger than expected Auger coefficient. Auger nonradiative recombination decreases the theoretical external luminescence efficiency to ∼95% at open-circuit conditions. The Auger penalty is much reduced at the operating point where the carrier density is less, producing an oddly high fill factor of ∼90.4%. This compensates the Auger penalty and leads to a power conversion efficiency of 30.5%, close to ideal for the MAPbI3 bandgap.

Inverse design of near unity efficiency perfectly vertical grating couplers.

Efficient coupling between integrated optical waveguides and optical fibers is essential to the success of silicon photonics. While many solutions exist, perfectly vertical grating couplers that scatter light out of a waveguide in the direction normal to the waveguide's top surface are an ideal candidate due to their potential to reduce packaging complexity. Designing such couplers with high efficiencies, however, has proven difficult. In this paper, we use inverse electromagnetic design techniques to optimize a high efficiency two-layer perfectly vertical silicon grating coupler. Our base design achieves a chip-to-fiber coupling efficiency of 99.2% (-0.035 dB) at 1550 nm. Using this base design as a starting point, we run subsequent constrained optimizations to realize vertical couplers with coupling efficiencies over 96% and back reflections of less than -40 dB which can be fabricated using 65 nm-resolution lithography. These results demonstrate a new path forward for designing fabrication-tolerant ultra high efficiency grating couplers.

Leveraging continuous material averaging for inverse electromagnetic design.

Inverse electromagnetic design has emerged as a way of efficiently designing active and passive electromagnetic devices. This maturing strategy involves optimizing the shape or topology of a device in order to improve a figure of merit-a process which typically requires that we compute the gradient of a figure of merit which describes device performance, potentially with respect to many design variables. In this paper, we introduce a new strategy based on smoothing abrupt material interfaces which enables us to efficiently compute these gradients with high accuracy irrespective of the resolution of the underlying simulation. This has advantages over previous approaches to shape and topology optimization in nanophotonics which are either prone to gradient errors or place important constraints on the shape of the device. As a demonstration of this new strategy, we optimize a non-adiabatic waveguide taper between a narrow and wide waveguide. This optimization leads to a non-intuitive design with a very low insertion loss of only 0.041 dB at 1550 nm.

Short-channel field-effect transistors with 9-atom and 13-atom wide graphene nanoribbons.

Bottom-up synthesized graphene nanoribbons and graphene nanoribbon heterostructures have promising electronic properties for high-performance field-effect transistors and ultra-low power devices such as tunneling field-effect transistors. However, the short length and wide band gap of these graphene nanoribbons have prevented the fabrication of devices with the desired performance and switching behavior. Here, by fabricating short channel (L ch ~ 20 nm) devices with a thin, high-κ gate dielectric and a 9-atom wide (0.95 nm) armchair graphene nanoribbon as the channel material, we demonstrate field-effect transistors with high on-current (I on > 1 µA at V d = -1 V) and high I on /I off ~ 105 at room temperature. We find that the performance of these devices is limited by tunneling through the Schottky barrier at the contacts and we observe an increase in the transparency of the barrier by increasing the gate field near the contacts. Our results thus demonstrate successful fabrication of high-performance short-channel field-effect transistors with bottom-up synthesized armchair graphene nanoribbons.Graphene nanoribbons show promise for high-performance field-effect transistors, however they often suffer from short lengths and wide band gaps. Here, the authors use a bottom-up synthesis approach to fabricate 9- and 13-atom wide ribbons, enabling short-channel transistors with 105 on-off current ratio.

Measuring the Edge Recombination Velocity of Monolayer Semiconductors.

Understanding edge effects and quantifying their impact on the carrier properties of two-dimensional (2D) semiconductors is an essential step toward utilizing this material for high performance electronic and optoelectronic devices. WS2 monolayers patterned into disks of varying diameters are used to experimentally explore the influence of edges on the material's optical properties. Carrier lifetime measurements show a decrease in the effective lifetime, τeffective, as a function of decreasing diameter, suggesting that the edges are active sites for carrier recombination. Accordingly, we introduce a metric called edge recombination velocity (ERV) to characterize the impact of 2D material edges on nonradiative carrier recombination. The unpassivated WS2 monolayer disks yield an ERV ∼ 4 × 104 cm/s. This work quantifies the nonradiative recombination edge effects in monolayer semiconductors, while simultaneously establishing a practical characterization approach that can be used to experimentally explore edge passivation methods for 2D materials.

Goos-Hänchen Shift and Even-Odd Peak Oscillations in Edge-Reflections of Surface Polaritons in Atomically Thin Crystals.

Two-dimensional surface polaritons (2DSPs), such as graphene plasmons, exhibit various unusual properties, including electrical tunability and strong spatial confinement with high Q-factor, which can enable tunable photonic devices for deep subwavelength light manipulations. Reflection of plasmons at the graphene's edge plays a critical role in the manipulation of 2DSP and enables their direct visualization in near-field infrared microscopy. However, a quantitative understanding of the edge-reflections, including reflection phases and diffraction effects, has remained elusive. Here, we show theoretically and experimentally that edge-reflection of 2DSP exhibits unusual behaviors due to the presence of the evanescent waves, including an anomalous Goos-Hänchen phase shift as in total internal reflections and an unexpected even-odd peak amplitude oscillation from the wave diffraction at the edge. Our theory is not only valid for plasmons in graphene but also for other 2D polaritons, such as phonon polaritons in ultrathin boron nitride flakes and exciton polariton in two-dimensional semiconductors.

Large spontaneous-emission enhancements in metallic nanostructures: towards LEDs faster than lasers.

Recent progress in the design and realization of optical antennas enclosing fluorescent materials has demonstrated large spontaneous-emission enhancements and, simultaneously, high radiation efficiencies. We discuss here that an important objective of such work is to increase spontaneous-emission rates to such a degree that light-emitting diodes (LEDs) can possess modulation speeds exceeding those of typical semiconductor lasers, which are usually in the range ~20-50 GHz. We outline the underlying physics that enable large spontaneous-emission enhancements in metallic nanostructures, and we then discuss recent theoretical and experimentally promising results, where enhancements larger than a factor of ~300 have been reported, with radiation efficiencies exceeding 50%. We provide key comparative advantages of these structures in comparison to conventional dielectric microcavity designs, namely the fact that the enhancement of spontaneous emission can be relatively nonresonant (i.e., broadband) and that the antenna nanostructures can be spectrally and structurally compatible for integration with a wide class of emitters, including organic dyes, diamond nanocrystals and colloidal quantum dots. Finally, we point out that physical insight into the underlying effects can be gained by analyzing these metallic nanostructures in their equivalent-circuit (or nano-antenna) model, showing that all main effects (including the Purcell factor) can adequately be described in that approach.

High Luminescence Efficiency in MoS2 Grown by Chemical Vapor Deposition.

One of the major challenges facing the rapidly growing field of two-dimensional (2D) transition metal dichalcogenides (TMDCs) is the development of growth techniques to enable large-area synthesis of high-quality materials. Chemical vapor deposition (CVD) is one of the leading techniques for the synthesis of TMDCs; however, the quality of the material produced is limited by defects formed during the growth process. A very useful nondestructive technique that can be utilized to probe defects in semiconductors is the room-temperature photoluminescence (PL) quantum yield (QY). It was recently demonstrated that a PL QY near 100% can be obtained in MoS2 and WS2 monolayers prepared by micromechanical exfoliation by treating samples with an organic superacid: bis(trifluoromethane)sulfonimide (TFSI). Here we have performed a thorough exploration of this chemical treatment on CVD-grown MoS2 samples. We find that the as-grown monolayers must be transferred to a secondary substrate, which releases strain, to obtain high QY by TFSI treatment. Furthermore, we find that the sulfur precursor temperature during synthesis of the MoS2 plays a critical role in the effectiveness of the treatment. By satisfying the aforementioned conditions we show that the PL QY of CVD-grown monolayers can be improved from ∼0.1% in the as-grown case to ∼30% after treatment, with enhancement factors ranging from 100 to 1500× depending on the initial monolayer quality. We also found that after TFSI treatment the PL emission from MoS2 films was visible by eye despite the low absorption (5-10%). The discovery of an effective passivation strategy will speed the development of scalable high-performance optoelectronic and electronic devices based on MoS2.

High Photoluminescence Quantum Yield in Band Gap Tunable Bromide Containing Mixed Halide Perovskites.

Hybrid organic-inorganic halide perovskite based semiconductor materials are attractive for use in a wide range of optoelectronic devices because they combine the advantages of suitable optoelectronic attributes and simultaneously low-cost solution processability. Here, we present a two-step low-pressure vapor-assisted solution process to grow high quality homogeneous CH3NH3PbI3-xBrx perovskite films over the full band gap range of 1.6-2.3 eV. Photoluminescence light-in versus light-out characterization techniques are used to provide new insights into the optoelectronic properties of Br-containing hybrid organic-inorganic perovskites as a function of optical carrier injection by employing pump-powers over a 6 orders of magnitude dynamic range. The internal luminescence quantum yield of wide band gap perovskites reaches impressive values up to 30%. This high quantum yield translates into substantial quasi-Fermi level splitting and high "luminescence or optically implied" open-circuit voltage. Most importantly, both attributes, high internal quantum yield and high optically implied open-circuit voltage, are demonstrated over the entire band gap range (1.6 eV ≤ Eg ≤ 2.3 eV). These results establish the versatility of Br-containing perovskite semiconductors for a variety of applications and especially for the use as high-quality top cell in tandem photovoltaic devices in combination with industry dominant Si bottom cells.

Near-unity photoluminescence quantum yield in MoS2.

Two-dimensional (2D) transition metal dichalcogenides have emerged as a promising material system for optoelectronic applications, but their primary figure of merit, the room-temperature photoluminescence quantum yield (QY), is extremely low. The prototypical 2D material molybdenum disulfide (MoS2) is reported to have a maximum QY of 0.6%, which indicates a considerable defect density. Here we report on an air-stable, solution-based chemical treatment by an organic superacid, which uniformly enhances the photoluminescence and minority carrier lifetime of MoS2 monolayers by more than two orders of magnitude. The treatment eliminates defect-mediated nonradiative recombination, thus resulting in a final QY of more than 95%, with a longest-observed lifetime of 10.8 ± 0.6 nanoseconds. Our ability to obtain optoelectronic monolayers with near-perfect properties opens the door for the development of highly efficient light-emitting diodes, lasers, and solar cells based on 2D materials.

Tunneling Nanoelectromechanical Switches Based on Compressible Molecular Thin Films.

Abrupt switching behavior and near-zero leakage current of nanoelectromechanical (NEM) switches are advantageous properties through which NEMs can outperform conventional semiconductor electrical switches. To date, however, typical NEMs structures require high actuation voltages and can prematurely fail through permanent adhesion (defined as stiction) of device components. To overcome these challenges, in the present work we propose a NEM switch, termed a "squitch," which is designed to electromechanically modulate the tunneling current through a nanometer-scale gap defined by an organic molecular film sandwiched between two electrodes. When voltage is applied across the electrodes, the generated electrostatic force compresses the sandwiched molecular layer, thereby reducing the tunneling gap and causing an exponential increase in the current through the device. The presence of the molecular layer avoids direct contact of the electrodes during the switching process. Furthermore, as the layer is compressed, the increasing surface adhesion forces are balanced by the elastic restoring force of the deformed molecules which can promote zero net stiction and recoverable switching. Through numerical analysis, we demonstrate the potential of optimizing squitch design to enable large on-off ratios beyond 6 orders of magnitude with operation in the sub-1 V regime and with nanoseconds switching times. Our preliminary experimental results based on metal-molecule-graphene devices suggest the feasibility of the proposed tunneling switching mechanism. With optimization of device design and material engineering, squitches can give rise to a broad range of low-power electronic applications.

Optical antenna enhanced spontaneous emission.

Atoms and molecules are too small to act as efficient antennas for their own emission wavelengths. By providing an external optical antenna, the balance can be shifted; spontaneous emission could become faster than stimulated emission, which is handicapped by practically achievable pump intensities. In our experiments, InGaAsP nanorods emitting at ∼ 200 THz optical frequency show a spontaneous emission intensity enhancement of 35 × corresponding to a spontaneous emission rate speedup ∼ 115 ×, for antenna gap spacing, d = 40 nm. Classical antenna theory predicts ∼ 2,500 × spontaneous emission speedup at d ∼ 10 nm, proportional to 1/d(2). Unfortunately, at d < 10 nm, antenna efficiency drops below 50%, owing to optical spreading resistance, exacerbated by the anomalous skin effect (electron surface collisions). Quantum dipole oscillations in the emitter excited state produce an optical ac equivalent circuit current, I(o) = qω|x(o)|/d, feeding the antenna-enhanced spontaneous emission, where q|x(o)| is the dipole matrix element. Despite the quantum-mechanical origin of the drive current, antenna theory makes no reference to the Purcell effect nor to local density of states models. Moreover, plasmonic effects are minor at 200 THz, producing only a small shift of antenna resonance frequency.