Flexible multiferroic heterostructures are promising to unveil technological developments in wearable magnetic field sensing, nonvolatile memory, soft robotics, and portable energy harvesters. Here, we report an enhanced and a zero-biased magnetoelectric (ME) effect in flexible, cost-effective, and room temperature sensitive Ni/FSMA/PMN-PT magnetization-graded ME heterostructure. Flexible Ni foil with −q (piezomagnetic coefficient) and the ferromagnetic shape memory alloy (FSMA; Ni-Mn-In) layer with +q offers the desired q-grading. The temperature-dependent dielectric behavior shows an anomaly in the martensite transformation regime of the FSMA layer. The Ni/FSMA/PMN-PT ME heterostructure exhibits noteworthy ME output of ∼3.7 V/cm Oe, significantly higher than Ni/PMN-PT (∼1 V/cm Oe). The q-grading-induced bending moment impedes the asymmetry-related flexural strain and strengthens the ME interaction. The zero-bias ME output of ∼0.4 V/cm Oe is ascribed to the interaction between q-grading-induced transverse magnetization and AC magnetic field. Ni/Ni-Mn-In/PMN-PT ME heterostructure displays excellent magnetic field sensing parameters: correlation coefficient, sensitivity, inaccuracy, and hysteresis of 0.99916, ∼0.74 mV/Oe, 1.5% full-scale output (FSO), and 1.8% FSO, respectively. The reversible and repeatable nonvolatile switching of the ME coefficient obtained with positive and negative electric fields is useful for next-generation memory devices. The flexible ME heterostructure shows no degradation in performance up to 1500 bending cycles. Such Ni/FSMA/PMN-PT based ME heterostructures are propitious for multifunctional flexible magnetic field sensors and nonvolatile memory applications.
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