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Strong Hot Carrier Effects Observed in a Single Nanowire Heterostructure

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 Added by Leigh Smith
 Publication date 2018
  fields Physics
and research's language is English




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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.

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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.
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.
84 - N. Johnson , C. Emary , S. Ryu 2017
Using a recently-developed time-of-flight measurement technique with 1 ps time resolution and electron-energy spectroscopy, we developed a method to measure the longitudinal-optical-phonon emission rate of hot electrons travelling along a depleted edge of a quantum Hall bar. A comparison of the experimental results to a single-particle model implies that the main scattering mechanism involves a two-step process via intra-Landau-level transition. We show this scattering can be suppressed by controlling the edge potential profile, and a scattering length > 1 mm can be achieved, allowing the use of this system for scalable single-electron device applications.
Compared to traditional pn-junction photovoltaics, hot carrier solar cells offer potentially higher efficiency by extracting work from the kinetic energy of photogenerated hot carriers before they cool to the lattice temperature. Hot carrier solar cells have been demonstrated in high-bandgap ferroelectric insulators and GaAs/AlGaAs heterostructures, but so far not in low-bandgap materials, where the potential efficiency gain is highest. Recently, a high open-circuit voltage was demonstrated in an illuminated wurtzite InAs nanowire with a low bandgap of 0.39 eV, and was interpreted in terms of a photothermoelectric effect. Here, we point out that this device is a hot carrier solar cell and discuss its performance in those terms. In the demonstrated devices, InP heterostructures are used as energy filters in order to thermoelectrically harvest the energy of hot electrons photogenerated in InAs absorber segments. The obtained photovoltage depends on the heterostructure design of the energy filter and is therefore tunable. By using a high-resistance, thermionic barrier an open-circuit voltage is obtained that is in excess of the Shockley-Queisser limit. These results provide generalizable insight into how to realize high voltage hot carrier solar cells in low-bandgap materials, and therefore are a step towards the demonstration of higher efficiency hot carrier solar cells.
We numerically study the interaction of a terahertz pulse with monolayer graphene. We observe that the electron momentum density is affected by the carrier-envelope phase (CEP) of the single- to few-cycle terahertz laser pulse that induces the electron dynamics. In particular, we see strong asymmetric electron momentum distributions for non-zero values of the CEP. We explain the origin of the asymmetry within the adiabatic-impulse model by finding conditions to reach minimal adiabatic gap between the valence band and the conduction band. We discuss how these conditions and the interference pattern, emanating from successive non-adiabatic transitions at this minimal gap, affect the electron momentum density and how they are modified by the CEP. This opens the door to control fundamental time-dependent electron dynamics in the tunneling regime in Dirac materials. Also, this control suggests a way to measure the CEP of a terahertz laser pulse when it interacts with condensed matter systems.
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