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Engineering the energetics of perovskite photovoltaic devices through thedeliberate introduction of dipoles to control the built-in potential of thedevices offers the opportunity to enhance their performance without the need tomodify the active layer itself. In this work, we demonstrate how theincorporation of molecular dipoles into the bathocuproine (BCP) hole-blockinglayer of inverted perovskite solar cells improves the device open-circuitvoltage (VOC) and consequently, its performance. We explore a series of fourthiaazulenic derivatives that exhibit increasing dipole moments and demonstratethat these molecules can be introduced into the solution-processed BCP layer toeffectively increase the built-in potential within the device, without alteringany of the other device layers. As a result the VOC of the devices is enhancedby up to 130 mV with larger dipoles resulting in higher VOCs. To investigatethe limitations of this approach, we employ numerical device simulations thatdemonstrate that the highest dipole derivatives used in this work eliminate alllimitations on the VOC stemming from the built-in potential of the device.

Enhancing the Open-Circuit Voltage of Perovskite Solar Cells by Embedding Molecular Dipoles within their Hole-Blocking Layer