Comparative study of photo-induced electronic transport along ferroelectric domain walls in lithium niobate single crystals

Abstract

Ferroelectric domain wall conductivity (DWC) is an intriguing functional property, that can be controlled through external stimuli such as electric and mechanical fields. Optical-field control, as a non-invasive flexible handle, has rarely been applied so far, but significantly expands the possibility for both tuning and probing DWC. On the one hand, as known from Second-Harmonic, Raman, and CARS micro-spectroscopy, the optical in-and-out approach delivers parameters on the DW distribution, the DW inclination, and probes the DW vibrational modes; on the other hand, photons might be applied also to directly generate charge carriers within the DW, hence acting as a functional and spectrally tunable probe to deduce the integral or local absorption properties and bandgaps of conductive DWs. Here, we report on such an optoelectronic approach by investigating the photo-induced DWC (PI-DWC) in DWs of the model system lithium niobate, a material that is well known for hosting conductive DWs. We compare three different crystals containing different numbers of domain walls: (A) none, (B) one, and (C) many conductive DWs. All samples are inspected for their current-voltage (I-V) behavior (i) in darkness, and (ii) for different illumination wavelengths swept from 500 nm down to 310 nm. All samples show their maximum PI-DWC at 310 nm, i.e., at the optical bandgap of lithium niobate; moreover, sample (C) reaches PI-DWCs of several $\mu$A. Interestingly, a noticeable PI-DWC is also observed for sub-bandgap illumination, i.e., wavelengths as high as 500 nm, hinting towards the existence and decisive role of electronic in-gap states that contribute to the electronic transport along DWs. Finally, conductive atomic force microscopy (c-AFM) investigations under illumination proved that the PI-DWC is confined to the DW area, and does not originate from photo-induced bulk conductivity.