The combined effect of mechanical strain and electric field cycling on the ferroelectric performance of P(VDF-TrFE) thin films on flexible substrates and underlying mechanisms

In this manuscript, we study the combined effect of mechanical strain and electric field cycling on the ferroelectric properties and polarization fatigue of P(VDF-TrFE) based flexible thin film capacitors from the perspective of flexible memory applications. The devices show nearly 80% retention of ferroelectric polarization after 30 000 bending cycles at mechanical strains of up to ca. 0.8%, mimicking a typical number of bending cycles a product is expected to go through. On the other hand, electric field cycling of the unstrained as well as mechanically strained devices results in over 50% drop in the ferroelectric polarization of the capacitors within 105 bipolar switching cycles. We find that 20% reduction in the polarization upon mechanical cycling is due to the formation of cracks in P(VDF-TrFE) thin films whilst ca. 50% polarization reduction during purely electrical or mechano-electrical fatigue is concomitant with the development of bubbles in the top electrode of the devices which eventually coalesce to give rise to bursting and eventual delamination of the electrode. A detailed investigation into the electrical fatigue mechanisms shows that the fatigue is primarily driven by the degradation of the P(VDF-TrFE) thin films due to HF elimination triggered by a high enough electric field, also manifested by reduced crystallinity and a reduced number of total dipoles of P(VDF-TrFE) films. The results clearly suggest that polarization reduction upon electric field cycling i.e. electrical fatigue is a greater bottleneck in the use of flexible memory devices than the mechanical cycling.