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Two-step photon upconversion solar cells (TPU-SCs) based on III–V semiconductors can achieve enhanced sub-bandgap photon absorption because of intraband transitions at the heterointerface. From a technological aspect, the question arose whether similar intraband transitions can be realized by using perovskite/III–V semiconductor heterointerfaces. In this article, we demonstrate a TPU-SC based on a CsPbBr3/GaAs heterointerface. Such a solar cell can ideally achieve an energy conversion efficiency of 48.5% under 1-sun illumination. This is 2.1% higher than the theoretical efficiency of an Al0.3Ga0.7As/GaAs-based TPU-SC. Experimental results of the CsPbBr3/GaAs-based TPU-SC show that both the short-circuit current JSC and the open-circuit voltage VOC increase with additional illumination of sub-bandgap photons. We analyze the excitation power dependence of JSC for different excitation conditions to discuss the mechanisms behind the enhancement. In addition, the observed voltage-boost clarifies that the JSC enhancement is caused by an adiabatic optical process at the CsPbBr3/GaAs heterointerface, where sub-bandgap photons efficiently pump the electrons accumulated at the heterointerface to the conduction band of CsPbBr3. Besides the exceptional optoelectronic properties of CsPbBr3 and GaAs, the availability of a CsPbBr3/GaAs heterointerface for two-step photon upconversion paves the way for the development of high-efficiency perovskite/III–V semiconductor-based single-junction solar cells. [ABSTRACT FROM AUTHOR]

Photon upconversion (PU) is a process where an electron is excited from the valence band to the conduction band of a wide-gap semiconductor by the sequential absorption of two or more photons via real states. For example, two-step PU can generate additional photocurrent in the so-called intermediate-band solar cells. In this work, we consider two- and three-step processes; we study multi-step PU in a quantum dot (QD)-based single-junction solar cell with a double-heterointerface structure. The solar cell consists of three different absorber layers: Al0.7Ga0.3As, Al0.3Ga0.7As, and GaAs, which form two heterointerfaces. Just beneath each heterointerface, an InAs/GaAs QD layer was inserted. After band-to-band excitation, electrons accumulate at each heterointerface, and then, below-bandgap photons excite a certain fraction of these electrons above the barrier energy. The photoluminescence spectra of the InAs QDs reveal slightly different QD size distributions at the two heterointerfaces. We show that the external quantum efficiency is improved by additional irradiation with below-bandgap infrared photons, which suggests a multi-step PU process that involves the two heterointerfaces. The dependence of the photocurrent on the infrared excitation power density only shows a superlinear behavior when the GaAs layer is excited but the Al0.3Ga0.7As layer is not. These data demonstrate a multi-step PU process that consists of one intraband transition at each of the two heterointerfaces and one interband transition in GaAs. [ABSTRACT FROM AUTHOR]