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Register a new userEnhanced energy storage density by reversible domain switching in acceptor doped ferroelectrics
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Typical ferroelectrics possess a large spontaneous polarization Ps but simultaneously a large remnant polarization Pr as well, resulting in an inferior energy storage density.A mechanism that can reduce the Pr while maintain the Ps is demanded to enhance the energy storage property of ferroelectrics.In the present study, it is shown that after acceptor doping and aging treatment, the domain switching in ferroelectrics becomes reversible, giving rise to a pinched double hysteresis loop. The pinched loop with a large Ps and a small Pr thus results in an enhanced energy storage density. The physics behind is a defect induced internal field that provides a restoring force for the domains to switch back.The idea is demonstrated through a time-dependent Ginzburg-Landau simulation as well as experimental measurements in BaTiO$_3$ based single crystal and ceramics. The mechanism is general and can be applied to various ferroelectrics, especially the environment-friendly ones.
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Evolution of a stripe array of polarization domains triggered by the oxygen vacancy migration in an acceptor doped ferroelectric is investigated in a self-consistent manner. A comprehensive model based on the Landau-Ginzburg-Devonshire approach includes semiconductor features due to the presence of electrons and holes, and effects of electrostriction and flexoelectricity especially significant near the free surface and domain walls. A domain array spontaneously formed in the absence of an external field is shown to undergo a reconstruction in the course of the gradual oxygen vacancy migration driven by the depolarization fields. The charge defect accumulation near the free ferroelectric surface causes a series of phenomena: (i) symmetry breaking between the positive and negative c-domains, (ii) appearance of an effective dipole layer at the free surface followed by the formation of a surface electrostatic potential, (iii) tilting and recharging of the domain walls, especially pronounced at higher acceptor concentrations. An internal bias field determined by the gain in the free energy of the structure exhibits dependences of its amplitude on time and dopant concentration well comparable with available experimental results on aging in BaTiO3.
Searching for performant multiferroic materials attracts general research interests in energy science as they have been increasingly exploited as the conversion media among thermal, electric, magnetic and mechanical energies by using their temperature-dependent ferroic properties. Here we report a material development strategy that guides us to discover a reversible phase-transforming ferroelectric material exhibiting enduring energy harvesting from small temperature differences. The material satisfies the crystallographic compatibility condition between polar and nonpolar phases, which shows only 2.5C thermal hysteresis and high figure of merit. It stably generates 15uA electricity in consecutive thermodynamic cycles in absence of any bias fields. We demonstrate our device to consistently generate 6uA/cm2 current density near 100C over 540 complete phase transformation cycles without any electric and functional degradation. The energy conversion device can light up a LED directly without attaching an external power source. This promising material candidate brings the low-grade waste heat harvesting closer to a practical realization, e.g. small temperature fluctuations around the water boiling point can be considered as a clean energy source.
Consecutive stochastic 90{deg} polarization switching events, clearly resolved in recent experiments, are described by a new nucleation and growth multi-step model. It extends the classical Kolmogorov-Avrami-Ishibashi approach and includes possible consecutive 90{deg}- and parallel 180{deg}-switching events. The model predicts the results of simultaneous time-resolved macroscopic measurements of polarization and strain, performed on a tetragonal Pb(Zr,Ti)O3 ceramic in a wide range of electric fields over a time domain of five orders of the magnitude. It allows the determination of the fractions of individual switching processes, their characteristic switching times, activation fields, and respective Avrami indices.
Early work by the author with Prof. Ishibashi [Scott et al., J. Appl. Phys. 64, 787 (1988)] showed that switching kinetics in ferroelectrics satisfy a constraint on current transients compatible with d = 2.5 dimensionality. At that time with no direct observations of the domains, it was not possible to conclude whether this was a true Hausdorff dimension or a numerical artefact caused by an approximation in the theory (which ignored the dependence of domain wall velocity upon domain diameter). Recent data suggest that the switching dimensionality is truly fractal with d = 2.5. The critical exponent beta characterizing the order parameter P(T) can be written as a continuous function of dimension d as beta(d)= [ u(d)/2] [d+eta(d)-2], which is exact within hyperscaling; here u and eta are the exponents characterizing the pair correlation function G(r,T) and the structure factor S(q,T). For d=2.5 the estimate is that beta is approximately 1/4.
Doping is a widely used method to tune physical properties of ferroelectric perovskites. Since doping can induce charges due to the substitution of certain elements, charge effects shall be considered in doped samples. To understand how charges can affect the system, we incorporate the dipole-charge interaction into our simulations, where the pinched hysteresis loops can well be reproduced. Two charge compensation models are proposed and numerically investigated to understand how lanthanum doping affect BaTiO$_{3}$s ferroelectric phase transition temperature and hysteresis loop. The consequences of the two charge compensation models are compared and discussed.
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