Owen D. Miller

Strong Internal and External Luminescence as Solar Cells Approach the Shockley–Queisser Limit

Absorbed sunlight in a solar cell produces electrons and holes. However, at the open-circuit condition, the carriers have no place to go. They build up in density, and ideally, they emit external luminescence that exactly balances the incoming sunlight. Any additional nonradiative recombination impairs the carrier density buildup, limiting the open-circuit voltage. At open circuit, efficient external luminescence is an indicator of low internal optical losses. Thus, efficient external luminescence is, counterintuitively, a necessity for approaching the Shockley–Queisser (SQ) efficiency limit. A great solar cell also needs to be a great light-emitting diode. Owing to the narrow escape cone for light, efficient external emission requires repeated attempts and demands an internal luminescence efficiency 90%.

Light Trapping Textures Designed by Electromagnetic Optimization for Subwavelength Thick Solar Cells

Light trapping in solar cells allows for increased current and voltage, as well as reduced materials cost. It is known that in geometrical optics, a maximum 4 n2 absorption enhancement factor can be achieved by randomly texturing the surface of the solar cell, where n is the material refractive index. This ray-optics absorption enhancement (AE) limit only holds when the thickness of the solar cell is much greater than the optical wavelength. In subwavelength thin films, the fundamental questions remain unanswered: 1) what is the subwavelength AE limit and 2) what surface texture realizes this optimal AE? We turn to computational electromagnetic optimization in order to design nanoscale textures for light trapping in subwavelength thin films. For high-index thin films, in the weakly absorbing limit, our optimized surface textures yield an angle- and frequency-averaged enhancement factor ~39. They perform roughly 30% better than randomly textured structures, but they fall short of the ray optics enhancement limit of 4 n2 ~ 50.

Fundamental Limits to Extinction by Metallic Nanoparticles

O. D. Miller, C. W. Hsu, 3 M. T. H. Reid, W. Qiu, B. G. DeLacy, J. D. Joannopoulos, M. Soljačić, and S. G. Johnson Department of Mathematics, Massachusetts Institute of Technology, Cambridge, MA 02139 Department of Physics, Massachusetts Institute of Technology, Cambridge, MA 02139 Department of Physics, Harvard University, Cambridge, MA 02138 U.S. Army Edgewood Chemical Biological Center, Research and Technology Directorate, Aberdeen Proving Ground, MD 21010

Effectiveness of Thin Films in Lieu of Hyperbolic Metamaterials in the Near Field

We show that the near-field functionality of hyperbolic metamaterials (HMM), typically proposed for increasing the photonic local density of states (LDOS), can be achieved with thin metal films. Although HMMs have an infinite density of internally propagating plane-wave states, the external coupling to nearby emitters is severely restricted. We show analytically that properly designed thin films, of thicknesses comparable to the metal size of a hyperbolic metamaterial, yield an LDOS as high as (if not higher than) that of HMMs. We illustrate these ideas by performing exact numerical computations of the LDOS of multilayer HMMs, along with their application to the problem of maximizing near-field heat transfer, to show that single-layer thin films are suitable replacements in both cases.

Shape-Independent Limits to Near-Field Radiative Heat Transfer

We derive shape-independent limits to the spectral radiative heat transfer rate between two closely spaced bodies, generalizing the concept of a blackbody to the case of near-field energy transfer. Through conservation of energy and reciprocity, we show that each body of susceptibility χ can emit and absorb radiation at enhanced rates bounded by |χ|(2)/Im χ, optimally mediated by near-field photon transfer proportional to 1/d(2) across a separation distance d. Dipole-dipole and dipole-plate structures approach restricted versions of the limit, but common large-area structures do not exhibit the material enhancement factor and thus fall short of the general limit. By contrast, we find that particle arrays interacting in an idealized Born approximation (i.e., neglecting multiple scattering) exhibit both enhancement factors, suggesting the possibility of orders-of-magnitude improvement beyond previous designs and the potential for radiative heat transfer to be comparable to conductive heat transfer through air at room temperature, and significantly greater at higher temperatures.

The opto-electronic physics that broke the efficiency limit in solar cells

The internal physics of a solar cell changes as it approaches the fundamental Shockley-Queisser limit. Photonic considerations overtake electronic ones, as an intense internal and external luminescence requires careful photon management. Counter-intuitively, maximizing light extraction increases voltage and therefore efficiency. Until 2010 the one-sun, single-junction efficiency record was set by a GaAs solar cell with an efficiency of 26.4% and an open-circuit voltage VOC= 1.03 V. Alta Devices recently improved the record with a GaAs cell that achieved 28.8% efficiency and VOC=1.12V, demonstrating the importance of photon management. Even with the best materials, the highest efficiencies cannot be achieved unless the solar cell is also designed to also be a good light emitting diode (LED). The physics of light extraction will be necessary in the next generation of high-efficiency solar cells.

General theory of spontaneous emission near exceptional points

We present a general theory of spontaneous emission at exceptional points (EPs)-exotic degeneracies in non-Hermitian systems. Our theory extends beyond spontaneous emission to any light-matter interaction described by the local density of states (e.g., absorption, thermal emission, and nonlinear frequency conversion). Whereas traditional spontaneous-emission theories imply infinite enhancement factors at EPs, we derive finite bounds on the enhancement, proving maximum enhancement of 4 in passive systems with second-order EPs and significantly larger enhancements (exceeding 400×) in gain-aided and higher-order EP systems. In contrast to non-degenerate resonances, which are typically associated with Lorentzian emission curves in systems with low losses, EPs are associated with non-Lorentzian lineshapes, leading to enhancements that scale nonlinearly with the resonance quality factor. Our theory can be applied to dispersive media, with proper normalization of the resonant modes.

Low-Loss Plasmonic Dielectric Nanoresonators

Material losses in metals are a central bottleneck in plasmonics for many applications. Here we propose and theoretically demonstrate that metal losses can be successfully mitigated with dielectric particles on metallic films, giving rise to hybrid dielectric-metal resonances. In the far field, they yield strong and efficient scattering, beyond even the theoretical limits of all-metal and all-dielectric structures. In the near field, they offer high Purcell factor (>5000), high quantum efficiency (>90%), and highly directional emission at visible and infrared wavelengths. Their quality factors can be readily tailored from plasmonic-like (∼10) to dielectric-like (∼103), with wide control over the individual resonant coupling to photon, plasmon, and dissipative channels. Compared with conventional plasmonic nanostructures, such resonances show robustness against detrimental nonlocal effects and provide higher field enhancement at extreme nanoscopic sizes and spacings. These hybrid resonances equip plasmonics with high efficiency, which has been the predominant goal since the fields inception.

Layer-by-layer self-assembly of plexcitonic nanoparticles

Colloidal suspensions of multilayer nanoparticles composed of a silver core, a polyelectrolyte spacer layer (inner shell), and a J-aggregate cyanine dye outer shell have been prepared for the first time. Absorption properties of the colloid were measured in the visible region. This multilayer architecture served as a framework for examining the coupling of the localized surface plasmon resonance exhibited by the silver core with the molecular exciton exhibited by the J-aggregate outer shell. The polyelectrolyte spacer layer promotes the formation of an excitonic J-aggregate while serving as a means of controlling the plasmon-exciton (i.e. plexciton) coupling strength through changing the distance between the core and the shell. An analytical expression based on Mie Theory and the Transfer Matrix Method was obtained for describing the optical response of these multilayered nanostructures. Computational and experimental results indicate that the absorption wavelength of the J-aggregate form of the dye is dependent on both the distance of the dye layer from the silver core and the degree of dye aggregation.

Rectification by charging: Contact-induced current asymmetry in molecular conductors

We outline the qualitatively different physics behind charging-induced current asymmetries in molecular conductors operating in the weakly interacting self-consistent field (SCF) and the strongly interacting Coulomb blockade (CB) regimes. The SCF conductance asymmetry originates in the asymmetric shifts of the closed-shell molecular conducting levels, driven by unequal mean-field potentials for positive and negative biases. A very different current asymmetry arises for CB due to the unequal number of open-shell excitation channels at opposite bias voltages. The CB regime, dominated by single charge effects, typically requires a computationally demanding many-electron or Fock-space description to do justice to its complex excitation spectrum. However, our analysis of molecular CB measurements reveals that many novel signatures can be explained using a simpler orthodox model that involves an incoherent sum of Fock-space excitations and hence treats the molecule as a metallic dot. This also reduces the complexity of the Fock-space description by including charge configurations alone, somewhat underscoring the richness of its electronic structure while retaining the essential single charge nature of the transport process. The inclusion of electronic structure with well-resolved Fock space excitations is, however, crucial in some notable examples.