Optoelectronic device simulations
Over the past 30 years, the world has witnessed the rapid development of optoelectronic devices based on III-V compound semiconductors. Past effort has mainly been directed to the theoretical understanding of, and the technology development for, these devices in applications in telecommunication networks and compact disk (CD) data storage. With the growing deployment of such devices in new fields such as illumination, display, fiber sensor, fiber gyro, optical coherent tomography, etc., research on optoelectronic devices, especially on those light emitting components, continues to expand with the pursuit of many experimental explorations on new materials such as group-III nitride alloys and II-VI compounds and novel structures such as quantum wires, dots, and nanostructures.
As the manufacturing technology becomes mature and standardized and few uncertainties are left, design and simulation become the major issue in the performance enhancement of existing devices and in the development of new devices. Recent progress in numerical techniques as well as computing hardware has provided a powerful platform that makes sophisticated computer-aided design, modeling, and simulation possible. So far, the development of optoelectronic devices seems to replicate the history of electronic devices: from discrete to integrated, from technology intensive to design intensive, from trial-and-error experiments to computer-aided simulation and optimization.
Advanced optoelectronic devices are built on compound semiconductor material systems with complicated geometrical structures; they are also operated under varying conditions. For this reason, we can find hardly any easy, intuitive, and analytical solutions to the first-principle-based governing equations that accurately describe the closely coupled physical processes inside such devices. Although solutions are relatively easy to obtain from the equations derived from the phenomenological model, assumptions have to be made in such a model, which often ignores some important effects and fails to achieve quantitative agreement between theoretically predicted and practically measured results.
Therefore, obtaining the solution directly from the physics-based governing equations through numerical techniques seems to be a promising approach to bridge the gap as mentioned above, as not only a qualitative, but also a quantitative matching between the theory and experiment is achievable.
Publications
Tracking Electron Dynamics of Single Molecules in Scanning Tunneling Microscopy Junctions with Laser Pulses
On the basis of real-time simulations, we devise a method to extend the capability of scanning tunneling microscopy (STM) to track the electronic dynamics of molecules on a material’s surface with the ultrafast temporal resolution of laser pulses. The intrinsic mechanism of visualization of electronic dynamics by measuring tunneling charge is attributed to the interference between the electronic oscillations stimulated by pump and probe pulses. The charge-transfer rate from molecule to the surrounding environment can be estimated with the decay time of electronic dynamics, which can also be detected by measuring the tunneling charge across the STM junction. Moreover, it is found that the tunneling charge can be varied precisely by changing the carrier-envelope phase (CEP) of the pulses, and this phase-dependence of tunnelling diminishes as the duration of incident laser pulses increases. The proposed scheme provides an alternative means for visualization of electron dynamics of single molecules by measuring tunnelling charges.
Electric Field Tunable Ultrafast Interlayer Charge Transfer in Graphene/WS2 Heterostructure
Van der Waals heterostructures composed of two-dimensional materials offer an unprecedented control over their properties and have attracted tremendous research interest in various optoelectronic applications. Here, we study the photoinduced charge transfer in graphene/WS2 heterostructure by time-dependent density functional theory molecular dynamics. Our results show that holes transfer from graphene to WS2 two times faster than electrons, and the occurrence of interlayer charge transfer is found correlated with vibrational modes of graphene and WS2. It is further demonstrated that the carrier dynamics can be efficiently modulated by external electric fields. Detailed analysis confirms that the carrier transfer rate at heterointerface is governed by the coupling between donor and acceptor states, which is the result of the competition between interlayer and intralayer relaxation processes. Our study provides insights into the understanding of ultrafast interlayer charge transfer processes in heterostructures and broadens their future applications in photovoltaic devices.
Controlling the emission frequency of graphene nanoribbon emitters based on spatially excited topological boundary states
Graphene nanoribbons (GNRs) with atomically precise heterojunction interfaces are exploited as nanoscale light emitting devices with modulable emission frequencies. By connecting GNRs with different widths and lengths, topological boundary states can be formed and manipulated. Using first-principles-based atomistic simulations, we studied the luminescence properties of a STM GNR junction and explored the applications of these topological states as nanoscale light sources. Taking advantage of the ultrahigh resolution of the STM tip, direct injection of high energy carriers at selected boundary states can be achieved. In this way, the emission color can be controlled by precisely changing the tip position. The GNR heterojunction can therefore represent a robust and controllable light-emitting device that takes a step forward towards the fabrication of nanoscale graphene-based optoelectronic devices.
Tunable Photoresponse by Gate Modulation in Bilayer Graphene Nanoribbon Devices
Control of absorption and photocurrent conversion is of practical importance for the design of photoelectric devices. In this paper, using simulations, we demonstrate that the photoresponse of a bilayer graphene nanoribbon (GNR) device can be controlled by gate voltage modulation. A vertical gate field shifts the potential on the top and bottom layers in opposite directions, resulting in a continuous change of band gap with applied gate voltage. This field simultaneously facilitates separation of photoexcited electron–hole pairs and gives rise to a photocurrent in a selected photon energy range. The photoresponse of a bilayer GNR device can thus be tuned by adjusting the applied gate voltage. In addition, the light frequency range can be changed by using nanoribbons of different widths. These findings provide a basis for the design of adjustable optoelectronic devices using two-dimensional materials.
Multiscale Study of Plasmonic Scattering and Light Trapping Effect in Silicon Nanowire Array Solar Cells
Nanometallic structures that support surface plasmons provide new ways to confine light at deep-subwavelength scales. The effect of light scattering in nanowire array solar cells is studied by a multiscale approach combining classical electromagnetic (EM) and quantum mechanical simulations. A photovoltaic device is constructed by integrating a silicon nanowire array with a plasmonic silver nanosphere. The light scatterings by plasmonic element and nanowire array are obtained via classical EM simulations, while current–voltage characteristics and optical properties of the nanowire cells are evaluated quantum mechanically. We found that the power conversion efficiency (PCE) of photovoltaic device is substantially improved due to the local field enhancement of the plasmonic effect and light trapping by the nanowire array. In addition, we showed that there exists an optimal nanowire number density in terms of optical confinement and solar cell PCE.
Quantum mechanical modeling the emission pattern and polarization of nanoscale light emitting diodes
Understanding of the electroluminescence (EL) mechanism in optoelectronic devices is imperative for further optimization of their efficiency and effectiveness. Here, a quantum mechanical approach is formulated for modeling the EL processes in nanoscale light emitting diodes (LED). Based on non-equilibrium Green’s function quantum transport equations, interactions with the electromagnetic vacuum environment are included to describe electrically driven light emission in the devices. The presented framework is illustrated by numerical simulations of a silicon nanowire LED device. EL spectra of the nanowire device under different bias voltages are obtained and, more importantly, the radiation pattern and polarization of optical emission can be determined using the current approach. This work is an important step forward towards atomistic quantum mechanical modeling of the electrically induced optical response in nanoscale systems.
Bandgap engineering of GaN nanowires
Bandgap engineering has been a powerful technique for manipulating the electronic and optical properties of semiconductors. In this work, a systematic investigation of the electronic properties of [0001] GaN nanowires was carried out using the density functional based tight-binding method (DFTB). We studied the effects of geometric structure and uniaxial strain on the electronic properties of GaN nanowires with diameters ranging from 0.8 to 10 nm. Our results show that the band gap of GaN nanowires depends linearly on both the surface to volume ratio (S/V) and tensile strain. The band gap of GaN nanowires increases linearly with S/V, while it decreases linearly with increasing tensile strain. These linear relationships provide an effect way in designing GaN nanowires for their applications in novel nano-devices
Fundamental limitations to plasmonic hot-carrier solar cells
Detailed balance between photon-absorption and energy loss constrains the efficiency of conventional solar cells to the Shockley-Queisser limit. However, if solar illumination can be absorbed over a wide spectrum by plasmonic structures, and the generated hot-carriers can be collected before relaxation, the efficiency of solar cells may be greatly improved. In this work, we explore the opportunities and limitations for making plasmonic solar cells, here considering a design for hot-carrier solar cells in which a conventional semiconductor heterojunction is attached to a plasmonic medium such as arrays of gold nanoparticles. The underlying mechanisms and fundamental limitations of this cell are studied using a nonequilibrium Green’s function method, and the numerical results indicate that this cell can significantly improve the absorption of solar radiation without reducing open-circuit voltage, as photons can be absorbed to produce mobile carriers in the semiconductor as long as they have energy larger than the Schottky barrier rather than above the bandgap. However, a significant fraction of the hot-carriers have energies below the Schottky barrier, which makes the cell suffer low internal quantum efficiency. Moreover, quantum efficiency is also limited by hot-carrier relaxation and metal–semiconductor coupling. The connection of these results to recent experiments is described, showing why plasmonic solar cells can have less than 1% efficiency.
Toward rational design of catalysts supported on a topological insulator substrate
Exotic and robust metallic surface states of topological insulators (TIs) have been expected to provide a promising platform for novel surface chemistry and catalysis. However, it is still not fully known how TIs affect the activity of catalysts. In this work, we study the effects of topological surface states (TSSs) on the activity of transition metal clusters (Au, Ag, Cu, Pt, and Pd), which are supported on a TI Bi2Se3 substrate. It was found the adsorption energy of oxygen on the supported catalysts can be always enhanced due to the TSSs. However, it does not necessarily mean an increase of the activity in catalytic oxidation reaction. Rather, the enhanced adsorption behavior in the presence of TSSs exhibits dual effects, determined by the intrinsic reactivity of these catalysts with oxygen. For the Au case, the activity of catalytic oxidation can be improved because the TSSs can enhance the dissociation rate of dioxygen. In contrast, a negative effect is found for the Pt and Pd clusters since the TSSs will suppress the desorption process of reaction products. We also found that the effect of TSSs on the activity of hydrogen evolution reaction (HER) is quite similar (i.e., the metals with original weak reactivity can gain a positive effect from TSSs). The present work can pave a way for more rational design and selection of catalysts when using TIs as substrates.
Quantum-mechanical prediction of nanoscale photovoltaics
Previous simulations of photovoltaic devices are based on classical models, which neglect the atomistic details and quantum-mechanical effects besides the dependence on many empirical parameters. Here, within the nonequilibrium Green’s function formalism, we present a quantum-mechanical study of the performance of inorganic nanowire-based photovoltaic devices. On the basis of density-functional tight-binding theory, the method allows simulation of current–voltage characteristics and optical properties of photovoltaic devices without relying on empirical parameters. Numerical studies of silicon nanowire-based devices of realistic sizes with 10 000 atoms are performed, and the results indicate that atomistic details and nonequilibrium conditions have a clear impact on the photoresponse of the devices.