The photothermoelectric (PTE) effect uses nonuniform absorption of light to produce a voltage via the Seebeck effect and is of interest for optical sensing and solar-to-electric energy conversion. However, the utility of PTE devices reported to date has been limited by the need to use a tightly focused laser spot to achieve the required, nonuniform illumination and by their dependence upon the Seebeck coefficients of the constituent materials, which exhibit limited tunability and, generally, low values. Here, we use InAs/InP heterostructure nanowires to overcome these limitations: first, we use naturally occurring absorption "hot spots" at wave mode maxima within the nanowire to achieve sharp boundaries between heated and unheated subwavelength regions of high and low absorption, allowing us to use global illumination; second, we employ carrier energy-filtering heterostructures to achieve a high Seebeck coefficient that is tunable by heterostructure design. Using these methods, we demonstrate PTE voltages of hundreds of millivolts at room temperature from a globally illuminated nanowire device. Furthermore, we find PTE currents and voltages that change polarity as a function of the wavelength of illumination due to spatial shifting of subwavelength absorption hot spots. These results indicate the feasibility of designing new types of PTE-based photodetectors, photothermoelectrics, and hot-carrier solar cells using nanowires.
Nanowires bring new possibilities to the field of hot-carrier photovoltaics by providing flexibility in combining materials for band engineering and using nanophotonic effects to control light absorption. Previously, an open-circuit voltage beyond the Shockley–Queisser limit was demonstrated in hot-carrier devices based on InAs–InP–InAs nanowire heterostructures. However, in these first experiments, the location of light absorption, and therefore the precise mechanism of hot-carrier extraction, was uncontrolled. In this Letter, we combine plasmonic nanoantennas with InAs–InP–InAs nanowire devices to enhance light absorption within a subwavelength region near an InP energy barrier that serves as an energy filter. From photon-energy- and irradiance-dependent photocurrent and photovoltage measurements, we find that photocurrent generation is dominated by internal photoemission of nonthermalized hot electrons when the photoexcited electron energy is above the barrier and by photothermionic emission when the energy is below the barrier. We estimate that an internal quantum efficiency up to 0.5–1.2% is achieved. Insights from this study provide guidelines to improve internal quantum efficiencies based on nanowire heterostructures.
Semiconductor nanowires have great potential for realizing broadband photodetectors monolithically integrated with silicon. However, the spectral range of such detectors has so far been limited to selected regions in the ultraviolet, visible, and near-infrared regions. Here, we report on the first intersubband nanowire heterostructure array photodetectors exhibiting a spectrally resolved photoresponse from the visible to long-wavelength infrared. In particular, the infrared response from 3 to 20 μm is enabled by intersubband transitions in low-bandgap InAsP quantum discs synthesized axially within InP nanowires. The intriguing optical characteristics, including unexpected sensitivity to normal incident radiation, are explained by excitation of the longitudinal component of optical modes in the photonic crystal formed by the nanostructured portion of the detectors. Our results provide a generalizable insight into how broadband nanowire photodetectors may be designed and how engineered nanowire heterostructures open up new, fascinating opportunities for optoelectronics.
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 hotcarrier 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 intradevice 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 solidstate 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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