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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]

The generation of two-photon photocurrent plays an essential role in realizing intermediate-band solar cells (IBSCs) with high conversion efficiencies. This current generation process strongly depends on the photocarrier dynamics in the intermediate levels, which can sometimes give rise to a deficient output current unexpectedly. In this work, we investigated the two-photon photocurrent generation process in InAs quantum dot (QD)-in-well intermediate-band solar cells. The two-photon photocurrent is generated by an interband transition in the structure (for example, in the well or the QD) and a subsequent intraband transition in the QD, and we used two different light sources to separately control these transitions. We found that, in the case of QD interband excitation in a sample with multiple wells, the carrier collection efficiency does not simply increase with the intraband excitation intensity; in the range from about 0.08 to 0.5 W/cm2, the collection efficiency decreases with increasing intraband excitation density. A comparison between samples with different numbers of wells revealed that the repetition of carrier trapping and detrapping during the transport in a multi-well structure can effectively modulate the recombination rate. This modulation induces a reduction of the current yield under certain illumination conditions. We propose a model to explain this phenomenon and verify it by investigating the bias dependence of the two-photon photocurrent from the QD. [ABSTRACT FROM AUTHOR]

A two-step photon upconversion (TPU) solar cell is a single-junction solar cell with a suitably designed heterointerface in the intrinsic layer. At this interface, upconversion can take place by absorbing infrared light, which excites carriers to energies above the heterojunction barrier, and then an electric field extracts these upconverted carriers to the barrier material. In this work, we study this photoabsorption process in a TPU solar cell with a modulation-doped structure. The modulation doping technique enables us to control the electric field at the heterointerface, and we demonstrate that the efficiency of the TPU process strongly depends on the electric field at the heterointerface. While we show that the TPU process induced by infrared light leads to a significant increase in the external quantum efficiency, we also note that this TPU process is an adiabatic process. It is shown that the adiabatic intraband photoexcitation at the heterointerface is able to increase the open-circuit voltage even above the open-circuit voltage that we predict from the diode equation and the actual current increase. We demonstrate obvious voltage boost effects and elucidate the relationship between the current and voltage. [ABSTRACT FROM AUTHOR]

Owing to the additional usage of sub-bandgap photons, the intermediate-band solar cell has been regarded as a promising device design to exceed the conversion limits of conventional photovoltaic devices. An output-voltage preservation is theoretically possible in this kind of device in the case of independent quasi-Fermi levels. This phenomenon manifests experimentally in a voltage recovery induced by supplementary two-step photon absorption processes. Here, we study the excitation-power and temperature dependences of the voltage performance in an intermediate-band solar cell containing InAs quantum dots in Al0.3Ga0.7As/GaAs quantum wells. The two-color photoexcitation method is used to separately control the interband and quantum dot-conduction band transitions. The output voltage is sensitive to the balance between the two excitation densities and the cell temperature. It is found that a strongly asymmetric irradiation can even lead to a voltage decrease. The temperature-dependent data suggest a faster electron–hole annihilation at lower temperatures. We introduce a new characteristic index to qualitatively evaluate the carrier loss in the intermediate band. [ABSTRACT FROM AUTHOR]