Mode-Selective Vibrational Control of Polaron Dynamics in Hybrid 2D Perovskites and Devices

The European Commission aims to achieve climate neutrality by 2050, with a key pillar of this ambition being the deployment of efficient and affordable renewable energy. The rapid progress in developing low-cost perovskite solar cells has created exciting opportunities to achieve this target. Their enhanced performance arises from unique optoelectronic features, including long carrier diffusion lengths, suppressed recombination, defect tolerance, and efficient charge transport. Building on this success, quantum-confined hybrid 2D perovskites (H2DPs) present additional prospects, where structural deformations and vibrational interactions play a crucial role in controlling polaron formation, carrier localization, and electronic dynamics, thereby governing material and device behavior. Yet, most current investigations focus primarily on passive correlations across compositional series, while only a limited number of studies directly probe molecular-scale motions and their influence on charge dynamics in perovskite devices under operating conditions. The MSCA project MOVHOP will reveal the impact of specific vibrational modes on polaron formation, photoconductivity, and device photocurrent. To achieve this, I will develop and apply UV/visible pump–IR push–THz probe (PPTHz) and pump–push–photocurrent (PPPc) techniques. This hybrid approach will provide insights spanning from structural dynamics to device performance, establishing structure–function relationships and design principles to maximize efficiency. My expertise in THz spectroscopy and perovskite photophysics, combined with the host group’s proficiency in multipulse and vibrational–electronic spectroscopies, ensures the successful implementation of this project. This MSCA program will not only advance the field toward sustainable energy solutions but also strengthen my research skills, career development, and professional network, ultimately supporting the establishment of my independent research group.