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We investigate the physics-based design of colloidal quantum dot (CQD) solar cells using self-consistent computational modeling. The significance of band alignment engineering and optimized carrier mobility is quantitatively explored as a function of subbandgap defect density (Nt) in the bulk CQD. For Nt &#x2264; 1015 cm-3, band alignment engineering near the interface of CQD and the metal contact could significantly improve open-circuit voltage by suppressing the forward-bias dark current. This effect could enhance cell efficiency up to ~37% for thinner (&lt;;1 &#x03BC;m) CQD layers. For the thicker (&gt;1 &#x03BC;m) CQD layer, the effect of band engineering is diminished, as the forward-bias dark current becomes diffusion limited and less dependent on the interfacial band offsets. An optimal carrier mobility in CQD lies in the range ~10-2-100 cm2/V&#x00B7;s and shows variation as a function of CQD layer thickness and the interfacial band offset. For Nt &#x2248; 1014cm-3, an optimally designed cell could provide ~20% efficiency under AM1.5G solar spectrum without employing advanced structural optimizations such as the nanostructured electrodes. These physical insights contribute to a better understanding of the quantum dot solar cell design that is needed for improving the efficiency for this emerging low-cost solar cell technology.

Role of Carrier Mobility and Band Alignment Engineering on the Efficiency of Colloidal Quantum Dot Solar Cells