Publication date: 1st July 2014
In 2013, Zhong et al. demonstrated that a panchromatic type II core-shell CdTe/CdSe device is capable to absorb light in the NIR leading to photocurrents of up to 19 mA/cm2. With a Voc of 0.61 V and a fill factor of 0.57, this device is to date the most performing sensitized quantum dot solar cell (QDSSC) with a 6.76% power conversion efficiency (PCE). Despite this important result, this PCE, however, still lags behind perovskite solar cells, which until now holds a record of 15.4%. Unlike perovskites, quantum dots present a higher tunability of the band gap, which can favor the absorption of a larger fraction of the solar emission spectrum, and therefore the generation of larger photocurrents, potentially leading to higher cell efficiencies.
In this work, we investigated the possibility to deduce the performances of a QDSSC using first principle calculations, in particular with Density Functional Theory (DFT). We designed a computational protocol that allows calculating with good accuracy the absorption spectra, the IPCE, the photocurrent and, finally, the efficiency of a QD-based solar architecture. Unlike other approaches, we rely minimally on experimental parameters, rendering this protocol very robust. After successfully benchmarking this model on known QDSSC, we decided to design new panchromatic core-shell structures that might be good candidates to achieve higher efficiencies. We found out that in the same experimental conditions found for the CdTe/CdSe device, the CdTe/HgSe core-shell architecture could deliver photocurrents higher than 25 mA/cm2, and provide efficiencies greater than 9%. In addition, this newly designed protocol permits to analyze in-silico the effect of other elements present in QDSSC, like, for example, type of ions, ligands, size of the QD, to estimate the outcome they might have on the spectroscopic properties of these materials and, therefore, their efficiencies.
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