Domain-engineered ferroelectric BiFeO$_3$ thin films for efficient bias-free THz emission

Abstract

Ultrashort light pulses can drive transient photocurrents in solids, the basis of modern terahertz (THz) emitters. Ferroelectrics have recently emerged in this context as sources that require neither the bias voltage of photoconductive antennas nor the magnetic field of spintronic emitters, yet the ultrafast photocurrent generating the emission has remained debated. Here, we resolve this question in epitaxial BiFeO$_3$ thin films with engineered ferroelectric domain configurations, from single-domain to periodic stripe patterns. The stripe-domain film emits a THz field four times stronger than the single-domain configurations, reaching about half the output of a metallic spintronic reference emitter while remaining unsaturated at our highest excitation fluences. Resolving the emitted THz field in amplitude and phase as a function of the pump light polarization and the crystal orientation, we separate the coexisting photocurrents by their symmetry. This identifies the ultrafast screening of the ferroelectric polarization by photocarriers as the dominant emission mechanism in the in-plane-polarized films, enhanced in multidomain films by the strong built-in fields at the domain walls, while an out-of-plane polarization favors the bulk photovoltaic current. Our results establish the ferroelectric domain configuration as a design parameter setting both the strength and the microscopic origin of light-driven THz emission.