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Register a new userReversible electron-hole separation in a hot carrier solar cell
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Hot-carrier solar cells are envisioned to utilize energy filtering to extract power from photogenerated electron-hole pairs before they thermalize with the lattice, and thus potentially offer higher power conversion efficiency compared to conventional, single absorber solar cells. The efficiency of hot-carrier solar cells can be expected to strongly depend on the details of the energy filtering process, a relationship which to date has not been satisfactorily explored. Here, we establish the conditions under which electron-hole separation in hot-carrier solar cells can occur reversibly, that is, at maximum energy conversion efficiency. We thus focus our analysis on the internal operation of the hot-carrier solar cell itself, and in this work do not consider the photon-mediated coupling to the sun. After deriving an expression for the voltage of a hot-carrier solar cell valid under conditions of both reversible and irreversible electrical operation, we identify separate contributions to the voltage from the thermoelectric effect and the photovoltaic effect. We find that, under specific conditions, the energy conversion efficiency of a hot-carrier solar cell can exceed the Carnot limit set by the intra-device temperature gradient alone, due to the additional contribution of the quasi-Fermi level splitting in the absorber. We also establish that the open-circuit voltage of a hot-carrier solar cell is not limited by the band gap of the absorber, due to the additional thermoelectric contribution to the voltage. Additionally, we find that a hot-carrier solar cell can be operated in reverse as a thermally driven solid-state light emitter. Our results help explore the fundamental limitations of hot-carrier solar cells, and provide a first step towards providing experimentalists with a guide to the optimal configuration of devices.
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Extraction of charge carriers from a hot carrier solar cell using energy selective contacts, and the impact on limiting power conversion efficiency is analyzed. It is shown that assuming isentropic conversion of carrier heat into voltage implies zero power output at all operating points. Under conditions of power output, lower voltages than in the isentropic case are obtained due to the irreversible entropy increase associated with carrier flow. This lowers the limiting power conversion efficiency of a hot carrier solar cell.
The separation of hot carriers in semiconductors is of interest for applications such as thermovoltaic photodetection and third-generation photovoltaics. Semiconductor nanowires offer several potential advantages for effective hot-carrier separation such as: a high degree of control and flexibility in heterostructure-based band engineering, increased hot-carrier temperatures compared to bulk, and a geometry well suited for local control of light absorption. Indeed, InAs nanowires with a short InP energy barrier have been observed to produce electric power under global illumination, with an open-circuit voltage exceeding the Shockley-Queisser limit. To understand this behaviour in more detail, it is necessary to maintain control over the precise location of electron-hole pair-generation in the nanowire. In this work we perform electron-beam induced current measurements with high spatial resolution, and demonstrate the role of the InP barrier in extracting energetic electrons. We interprete the results in terms of hot-carrier separation, and extract estimates of the hot carrier mean free path.
A consistent explanation of the formation of a ring-shaped pattern of exciton luminescence in GaAs/AlGaAs double quantum wells is suggested. The pattern consists of two concentric rings around the laser excitation spot. It is shown that the luminescence rings appear due to the in-layer transport of hot charge carriers at high photoexcitation intensity. Interestingly, one of two causes of this transport might involve self-organized criticality (SOC) that would be the first case of the SOC observation in semiconductor physics. We test this cause in a many-body numerical model by performing extensive molecular dynamics simulations. The results show good agreement with experiments. Moreover, the simulations have enabled us to identify the particular kinetic processes underlying the formation of each of these two luminescence rings.
We use Transient Rayleigh Scattering to study the thermalization of hot photoexcited carriers in single GaAsSb/InP nanowire heterostructures. By comparing the energy loss rate in single bare GaAsSb nanowires which do not show substantial hot carrier effects with the core-shell nanowires, we show that the presence of an InP shell substantially suppresses the LO phonon emission rate at low temperatures leading to strong hot carrier effects.
We investigate hot carrier propagation across graphene using an electrical nonlocal injection/detection method. The device consists of a monolayer graphene flake contacted by multiple metal leads. Using two remote leads for electrical heating, we generate a carrier temperature gradient that results in a measurable thermoelectric voltage VNL across the remaining (detector) leads. Due to the nonlocal character of the measurement, VNL is exclusively due to the Seebeck effect. Remarkably, a departure from the ordinary relationship between Joule power P and VNL, VNL ~ P, becomes readily apparent at low temperatures, representing a fingerprint of hot-carrier dominated thermoelectricity. By studying VNL as a function of bias, we directly determine the carrier temperature and the characteristic cooling length for hot-carrier propagation, which are key parameters for a variety of new applications that rely on hot-carrier transport.
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