Simulation of nanostructure-based and ultra-thin film solar cell devices beyond the classical picture

In this paper, an optoelectronic device simulation framework valid for arbitrary spatial variation of electronic potentials and optical modes, and for transport regimes ranging from ballistic to diffusive, is used to study non-local photon absorption, photocurrent generation and carrier extraction in ultra-thin film and nanostructure-based solar cell devices at the radiative limit. Among the effects that are revealed by the microscopic approach and which are inaccessible to macroscopic models is the impact of structure, doping or bias induced nanoscale potential variations on the local photogeneration rate and the photocarrier transport regime.Comment: 15 pages, 10 figure

Quantum-kinetic theory of steady-state photocurrent generation in thin films: Coherent versus incoherent coupling

The generation of photocurrents due to coupling of electrons to both classical and quantized electromagnetic fields in thin semiconductor films is described within the framework of the nonequilibrium Green's function formalism. For the coherent coupling to classical fields corresponding to single field operator averages, an effective two-time intraband self-energy is derived from a band decoupling procedure. The evaluation of coherent photogeneration is performed self-consistently with the propagation of the fields by using for the latter a transfer matrix formalism with an extinction coefficient derived from the electronic Green's functions. For the "incoherent" coupling to fluctuations of the quantized fields, which need to be considered for the inclusion of spontaneous emission, the first self-consistent Born self-energy is used, with full spatial resolution in the photon Green's functions. These are obtained from the numerical solution of Dyson and Keldysh equations including a nonlocal photon self-energy based on the same interband polarization function as used for the coherent case. A comparison of the spectral and integral photocurrent generation pattern reveals a close agreement between coherent and incoherent coupling for the case of an ultrathin, selectively contacted absorber layer at short circuit conditions.Comment: 11 pages, 7 figures, published versio

Nonequilibrium Green's function theory of coherent excitonic effects in the photocurrent response of semiconductor nanostructures

Excitonic contributions to absorption and photocurrent generation in semiconductor nanostructures are described theoretically and simulated numerically using steady-state non-equilibrium Green's function theory. In a first approach, the coherent interband polarization including Coulomb corrections is determined from a Bethe-Salpeter-type equation for the equal time interband single-particle charge carrier Green's function. The effects of excitonic absorption on photocurrent generation are considered on the same level of approximation via the derivation of the corresponding corrections to the electron-photon self-energy.Comment: 8 pages, 4 figure

Quantum-kinetic perspective on photovoltaic device operation in nanostructure-based solar cells

The implementation of a wide range of novel concepts for next-generation high-efficiency solar cells is based on nanostructures with configuration-tunable optoelectronic properties. On the other hand, effective nano-optical light-trapping concepts enable the use of ultra-thin absorber architectures. In both cases, the local density of electronic and optical states deviates strongly from that in a homogeneous bulk material. At the same time, non-local and coherent phenomena like tunneling or ballistic transport become increasingly relevant. As a consequence, the semi-classical, diffusive bulk picture conventionally assumed may no longer be appropriate to describe the physical processes of generation, transport, and recombination governing the photovoltaic operation of such devices. In this review, we provide a quantum-kinetic perspective on photovoltaic device operation that reaches beyond the limits of the standard simulation models for bulk solar cells. Deviations from bulk physics are assessed in ultra-thin film and nanostructure-based solar cell architectures by comparing the predictions of the semi-classical models for key physical quantities such as absorption coefficients, emission spectra, generation and recombination rates as well as potentials, densities and currents with the corresponding properties as given by a more fundamental description based on non-equilibrium quantum statistical mechanics. This advanced approach, while paving the way to a comprehensive quantum theory of photovoltaics, bridges simulations at microscopic material and macroscopic device levels by providing the charge carrier dynamics at the mesoscale.Comment: 22 pages, 8 figures; review article based on an invited talk at the MRS Spring Meeting 2017 in Phoeni

Spectral properties of photogenerated carriers in quantum well solar cells

The use of low-dimensional structures such as quantum wells, wires or dots in the absorbing regions of solar cells strongly affects the spectral response of the latter, the spectral properties being drastically modified by quantum confinement effects. Due to the microscopic nature of these effects, a microscopic theory of absorption and transport is required for their quantification. Such a theory can be developed in the framework of the non-equilibrium Green's function approach to semiconductor quantum transport and quantum optics. In this paper, the theory is used to numerically investigate the density of states, non-equilibrium occupation and corresponding excess concentration of both electrons and holes in single quantum well structures embedded in the intrinsic region of a p-i-n semiconductor diode, under illumination with monochromatic light of different energies. Escape of carriers from the quantum well is considered via the inspection of the spectral photocurrent at a given excitation energy. The investigation shows that escape from deep levels may be inefficient even at room temperature.Comment: 11 pages, 6 figure

Theoretical investigation of direct and phonon-assisted tunneling currents in InAlGaAs-InGaAs bulk and quantum well interband tunnel junctions for multi-junction solar cells

Direct and phonon-assisted tunneling currents in InAlGaAs-InGaAs bulk and double quantum well interband tunnel heterojunctions are simulated rigorously using the non-equilibrium Green's function formalism for coherent and dissipative quantum transport in combination with a simple two-band tight-binding model for the electronic structure. A realistic band profile and associated built-in electrostatic field is obtained via self-consistent coupling of the transport formalism to Poisson's equation. The model reproduces experimentally observed features in the current-voltage characteristics of the device, such as the structure appearing in the negative differential resistance regime due to quantization of emitter states. Local maps of density of states and current spectrum reveal the impact of quasi-bound states, electric fields and electron-phonon scattering on the interband tunneling current. In this way, resonances appearing in the current through the double quantum well structure in the negative differential resistance regime can be related to the alignment of subbands in the coupled quantum wells.Comment: 4 pages, 5 figure

Simulation of nanostructure-based high-efficiency solar cells: challenges, existing approaches and future directions

Many advanced concepts for high-efficiency photovoltaic devices exploit the peculiar optoelectronic properties of semiconductor nanostructures such as quantum wells, wires and dots. While the optics of such devices is only modestly affected due to the small size of the structures, the optical transitions and electronic transport can strongly deviate from the simple bulk picture known from conventional solar cell devices. This review article discusses the challenges for an adequate theoretical description of the photovoltaic device operation arising from the introduction of nanostructure absorber and/or conductor components and gives an overview of existing device simulation approaches.Comment: Invited paper, accepted for publication in IEEE Journal of Selected Topics in Quantum Electronic

Microscopic theory of absorption and emission in nanostructured solar cells: Beyond the generalized Planck formula

Absorption and emission in inorganic bipolar solar cells based on low dimensional structures exhibiting the effects of quantum confinement is investigated in the framework of a comprehensive microscopic theory of the optical and electronic degrees of freedom of the photovoltaic system. In a quantum-statistical treatment based on non-equilibrium Green's functions, the optical transition rates are related to the conservation of electronic currents, providing a quantum version of the balance equations describing the operation of a photovoltaic device. The generalized Planck law used for the determination of emission from an excited semiconductor in quasi-equilibrium is replaced by an expression of extended validity, where no assumptions on the distribution of electrons and photons are made. The theory is illustrated by the numerical simulation of single quantum well diodes at the radiative limit.Comment: 6 pages, 5 figures, extended LaTeX version of the EUPVSEC09 proceedings articl

Impact of nanostructure configuration on the photovoltaic performance of quantum dot arrays

In this work, a mesoscopic model based on the non-equilibrium Green's function formalism for a tight-binding-like effective Hamiltonian is used to investigate a selectively contacted quantum dot array designed for operation as a single junction quantum dot solar cell. By establishing a direct relation between nanostructure configuration and optoelectronic properties, the investigation reveals the influence of inter-dot and dot-contact coupling strengths on the rates of charge carrier photogeneration, radiative recombination, and extraction at contacts, and consequently on the ultimate performance of photovoltaic devices with finite quantum dot arrays as the active medium. For long carrier lifetimes, the dominant configuration effects originate in the dependence of the joint density of states on the inter-dot coupling in terms of band width and effective band gap. In the low carrier lifetime regime, where recombination competes with carrier extraction, the extraction efficiency shows a critical dependence on the dot-contact coupling.Comment: 11 pages, 15 figures; extensively revised and substantially extended versio