Subcritical switching dynamics and humidity effects in nanoscale studies of domain growth in ferroelectric thin films

Ferroelectric domain switching in c-axis-oriented epitaxial Pb(Zr$_{0.2}$Ti$_{0.8}$)O$_3$ thin films was studied using biased scanning probe microscopy tips. While linear and logarithmic dependence of domain size on tip bias and writing time, respectively, are well known, we report an additional linear dependence on relative humidity in the 28-65% range. We map out the switched domain size as a function of both the tip bias and the applied pulse time and describe a growth-limited regime for very short pulses and a nucleation-limited regime for very low tip bias. Using "interrupted-switching" measurements, we probe the nucleation regime with subcritical pulses and identify a surprisingly long relaxation time on the order of 100 ms, which we relate to ionic redistribution both on the surface and within the thin film itself.Comment: 11 pages, 4 figure

Understanding polarization vs. charge dynamics effects in ferroelectric-carbon nanotube devices

To optimize the performance of multifunctional carbon nanotube-ferroelectric devices, it is necessary to understand both the polarization and charge dynamics effects on their transconductance. Directly comparing ferroelectric Pb(Zr0.2Ti0.8)O3 and dielectric SrTiO3 field effect transistors, we show that the two effects strongly compete, with transient charge dynamics initially masking up to 40% of the ferroelectric field effect. For applications, it is therefore crucial to maximize the quality of the ferroelectric film and the interface with the carbon nanotube to take full advantage of the switchable polarization.Comment: 5 pages, 4 figure

Nanoscale studies of domain wall motion in epitaxial ferroelectric thin films

Atomic force microscopy was used to investigate ferroelectric switching and nanoscale domain dynamics in epitaxial PbZr0.2Ti0.8O3 thin films. Measurements of the writing time dependence of domain size reveal a two-step process in which nucleation is followed by radial domain growth. During this growth, the domain wall velocity exhibits a v ~ exp[-(1/E)^mu] dependence on the electric field, characteristic of a creep process. The domain wall motion was analyzed both in the context of stochastic nucleation in a periodic potential as well as the canonical creep motion of an elastic manifold in a disorder potential. The dimensionality of the films suggests that disorder is at the origin of the observed domain wall creep. To investigate the effects of changing the disorder in the films, defects were introduced during crystal growth (a-axis inclusions) or by heavy ion irradiation, producing films with planar and columnar defects, respectively. The presence of these defects was found to significantly decrease the creep exponent mu, from 0.62 - 0.69 to 0.38 - 0.5 in the irradiated films and 0.19 - 0.31 in the films containing a-axis inclusions.Comment: 13 pages, 15 figures, to be published in J. App. Phys. special issue on ferroelectric

Identification of a strong contamination source for graphene in vacuum systems

To minimize parasitic doping effects caused by uncontrolled material adsorption, graphene is often investigated under vacuum. Here we report an entirely unexpected phenomenon occurring in vacuum systems, namely strong n-doping of graphene due to chemical species generated by common ion high-vacuum gauges. The effect --reversible upon exposing graphene to air-- is significant, as doping rates can largely exceed 10^{12} cm^{-2}/hour, depending on pressure and the relative position of the gauge and the graphene device. It is important to be aware of the phenomenon, as its basic manifestation can be mistakenly interpreted as vacuum-induced desorption of p-dopants.Comment: 10 pages, 4 figure

Nanoscale domain engineering in SrRuO3_3 thin films

We investigate nanoscale domain engineering via epitaxial coupling in a set of SrRuO$_3$/PbTiO$_3$/SrRuO$_3$ heterostructures epitaxially grown on (110)$_o$-oriented DyScO$_3$ substrates. The SrRuO$_3$ layer thickness is kept at 55 unit cells, whereas the PbTiO$_3$ layer is grown to thicknesses of 23, 45 and 90 unit cells. Through a combination of atomic force microscopy, x-ray diffraction and high resolution scanning transmission electron microscopy studies, we find that above a certain critical thickness of the ferroelectric layer, the large structural distortions associated with the ferroelastic domains propagate through the top SrRuO$_3$ layer, locally modifying the orientation of the orthorhombic SrRuO$_3$ and creating a modulated structure that extends beyond the ferroelectric layer boundaries.Comment: 19 pages, 6 figures, supplementary materials. arXiv admin note: text overlap with arXiv:2304.0694

Full control of polarization in ferroelectric thin films using growth temperature to modulate defects

P.P. and C.W. acknowledge partial support by Swiss National Science Foundation Division II grant 200021_178782. L.R.D. acknowledges support from the US National Science Foundation under grant DMR‐1708615. L.W.M. acknowledges support from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under Contract No. DE‐AC02‐05‐CH11231 (Materials Project program KC23MP) for the growth and study of defect structures in ferroic materials. A.B.N. gratefully acknowledges support from the Engineering and Physics Sciences Research Council (EPSRC) through grants EP/R023751/1 and EP/L017008/1.Deterministic control of the intrinsic polarization state of ferroelectric thin films is essential for device applications. Independently of the well-established role of electrostatic boundary conditions and epitaxial strain, the importance of growth temperature as a tool to stabilize a target polarization state during thin film growth is shown here. Full control of the intrinsic polarization orientation of PbTiO3 thin films is demonstrated-from monodomain up, through polydomain, to monodomain down as imaged by piezoresponse force microscopy-using changes in the film growth temperature. X-ray diffraction and scanning transmission electron microscopy reveal a variation of c-axis related to out-of-plane strain gradients. These measurements, supported by Ginzburg-Landau-Devonshire free energy calculations and Rutherford backscattering spectroscopy, point to a defect mediated polarization gradient initiated by a temperature dependent effective built-in field during growth, allowing polarization control not only under specific growth conditions, but ex-situ, for subsequent processing and device applications.Publisher PDFPeer reviewe

Switchable tribology of ferroelectrics

Switchable tribological properties of ferroelectrics offer an alternative route to visualize and control ferroelectric domains. Here, we observe the switchable friction and wear behavior of ferroelectrics using a nanoscale scanning probe—down domains have lower friction coefficients and show slower wear rates than up domains and can be used as smart masks. This asymmetry is enabled by flexoelectrically coupled polarization in the up and down domains under a sufficiently high contact force. Moreover, we determine that this polarization-sensitive tribological asymmetry is widely applicable across various ferroelectrics with different chemical compositions and crystalline symmetry. Finally, using this switchable tribology and multi-pass patterning with a domain-based dynamic smart mask, we demonstrate three-dimensional nanostructuring exploiting the asymmetric wear rates of up and down domains, which can, furthermore, be scaled up to technologically relevant (mm–cm) size. These findings demonstrate that ferroelectrics are electrically tunable tribological materials at the nanoscale for versatile applications.Peer ReviewedPostprint (published version

Observation of flat Γ\Gamma moir\'e bands in twisted bilayer WSe2_2

The recent observation of correlated phases in transition metal dichalcogenide moir\'e systems at integer and fractional filling promises new insight into metal-insulator transitions and the unusual states of matter that can emerge near such transitions. Here, we combine real- and momentum-space mapping techniques to study moir\'e superlattice effects in 57.4$^{\circ}$ twisted WSe$_2$ (tWSe$_2$). Our data reveal a split-off flat band that derives from the monolayer $\Gamma$ states. Using advanced data analysis, we directly quantify the moir\'e potential from our data. We further demonstrate that the global valence band maximum in tWSe$_2$ is close in energy to this flat band but derives from the monolayer K-states which show weaker superlattice effects. These results constrain theoretical models and open the perspective that $\Gamma$-valley flat bands might be involved in the correlated physics of twisted WSe$_2$