Alexander Haußmann

Nanoscale and macroscopic electrical ac transport along conductive domain walls in lithium niobate single crystals

The electrical impedance properties of UV-illuminated (λ = 310 nm) charged, conductive domain walls (CDWs) in 5 mol% magnesium-doped lithium niobate (LNO) single crystals are investigated on the nm-length scale using nanoimpedance microscopy (NIM) as well as by comparing the macroscopically measured complex impedance response between multi- and single-domain LNO samples. Similar to the case of dc conductivity, a higher conductivity of domain walls (DWs) compared to the bulk insulating matrix was observed. The contrast between DWs and bulk is most pronounced at lower frequencies (f 200 Hz) due to the large bulk capacitance at higher frequencies. Moreover, the simultaneous application of both an ac and dc bias results in an increased real part of the ac DW current. Also, equivalent circuits accurately describing both the domain and CDW contributions were developed; as a result we are able to analyze and quantify the complex dielectric conductive behavior of both bulk and CDWs in LNO within the framework of the mixed conduction model. Hopping of excited charge carriers along the CDWs was identified as the dominant charge transport process.

Photographic evidence for the third-order rainbow

The first likely photographic observation of the tertiary rainbow caused by sunlight in the open air is reported and analyzed. Whereas primary and secondary rainbows are rather common and easily seen phenomena in atmospheric optics, the tertiary rainbow appears in the sunward side of the sky and is thus largely masked by forward scattered light. Up to now, only a few visual reports and no reliable photographs of the tertiary rainbow are known. Evidence of a third-order rainbow has been obtained by using image processing techniques on a digital photograph that contains no obvious indication of such a rainbow. To rule out any misinterpretation of artifacts, we carefully calibrated the image in order to compare the observed bows angular position and dispersion with those predicted by theory.

Multiphoton photoluminescence contrast in switched Mg:LiNbO3 and Mg:LiTaO3 single crystals

We observed a multiphoton luminescence contrast between virgin and single-switched domains in Mg-doped LiNbO3 (LNO) and LiTaO3 (LTO) single crystals with different doping levels of 0–7 mol. % and 0–8 mol. %, respectively. A luminescence contrast in the range of 3% was measured between as-grown and electrically inverted domain areas in Mg:LNO samples, while the contrast reaches values of up to 30% for the Mg:LTO case. Under annealing, an exponential decay of the domain contrast was observed. The activation energy of about 1 eV being determined for the decay allowed a comparison with reported activation energies of associated defects, clearly illustrating a strong connection between thermal contrast decay and the H+ and Li+-ion mobility. Finally, performing similar experiments on oxidized samples undoubtedly demonstrated that the origin of the reported luminescence contrast is strongly connected with lithium ions.

Multiphoton-induced luminescence contrast between antiparallel ferroelectric domains in Mg-doped LiNbO3

We report on differentiating antiparallel ferroelectric domains in congruent Mg-doped LiNbO3 (Mg:LNO) single crystals through a multiphoton photoluminescence technique. Sample illumination with femtosecond laser pulses at λ = 790 nm results in a broad multiphoton emission spectrum revealing a domain contrast of >3% between virgin and inverted domains. The contrast decreases via annealing and shows an exponential decay in the temperature range from 80 to 150 °C. Our findings give clear ground of a thermally induced structural change by surpassing a specific activation energy. Hence, the reported contrast dynamics must be closely connected to the thermal activation of charged defects, which dramatically alters the internal bias field of these defects. This explanation is also supported when using single crystal LNO of different Mg doping levels showing much lower multiphoton effects for a < 5% Mg concentration. Based on this effect of multiphoton luminescence, it becomes easy to microscopically monitor and ...

Enhancing the Domain Wall Conductivity in Lithium Niobate Single Crystals

Domain walls (DWs) in ferroelectric/ferroic materials have been a central research focus for the last 50 years; DWs bear a multitude of extraordinary physical parameters within a unit-cell-sized lateral confinement. Especially, one outstanding feature has recently attracted a lot of attention for room-temperature applications, which is the potential to use DWs as two-dimensional (2D) conducting channels that completely penetrate bulk compounds. Domain wall currents in lithium niobate (LNO) so far lie in the lower pA regime. In this work, we report on an easy-to-use and reliable protocol that allows enhancing domain wall conductivity (DWC) in single-crystalline LNO (sc-LNO) by 3 to 4 orders of magnitude. sc-LNO thus has become one of the most prospective candidates to engineer DWC applications, notably for domain wall transport both with and without photoexcitation. DWs were investigated here for several days to weeks, both before and after DWC enhancement. 2D local-scale inspections were carried out using adequate local-probe techniques, i.e., piezoresponse force microscopy and conductive atomic force microscopy, while Cerenkov second-harmonic generation was applied for mapping the DW constitution in three-dimensional space across the full LNO single crystal. The comparison between these nano- and microscale inspections allows us to unambiguously correlate the DW inclination angle α close to the sample surface to the measured domain wall current distribution. Moreover, ohmic or diode-like electronic transport characteristics along such DWs can be readily interpreted when analyzing the DW inclination profile.

Observation, analysis, and reconstruction of a twinned rainbow

A photograph of a twinned rainbow, obtained on 11 May, 2012, in Dresden, Germany, is precisely calibrated with respect to lens projection and camera orientation. Since the twinning was only located in a part of the picture, it was possible to read out the red-green-blue intensity data from both a twinned and nontwinned position of the rainbow. These data were fitted with modeled spectra for polydisperse drop distributions, which were calculated with a Debye series algorithm and shifted in the scattering angle to account for the nonspherical shape of natural raindrops. The shift data were acquired from raytracing through realistic raindrop shapes modeled by two conjoined half-spheroids of different oblateness. Effective drop size distributions along the line of sight are derived from the fit for the two sampling positions and used to generate a true-color simulation of the original photograph. By this, the optical determination of physical rainfall properties is demonstrated.

SHG simulations of plasmonic nanoparticles using curved elements

We demonstrate that simulating plasmonic nanostructures by means of curved elements (CEs) significantly increases the accuracy and computation speed not only in the linear but also in the nonlinear regime. We implemented CEs within the discontinuous Galerkin (DG) method and, as an example of a nonlinear effect, investigated second-harmonic generation (SHG) at a silver nanoparticle. The second-harmonic response of the material is simulated by an extended Lorentz model (ELM). In the linear regime the CEs are ≈ 9 times faster than ordinary elements for the same accuracy, provide a much better convergence and show fewer unphysical field artifacts. For DG-SHG calculations CEs are almost indispensable to obtain physically reasonable results at all. Additionally, their boundary approximation has to be of the same order as their polynomial degree to achieve artifact-free field distributions. In return, the use of such CEs with the DG method pays off more than evidently, since the additional computation time is only 1%.

Advanced analysis of domain walls in Mg doped LiNbO 3 crystals with high resolution OCT

The structure of domain walls (DW) in ferroelectric media is of great interest as this material is used for frequency doublers and other applications. We show that the structure of the DWs can nicely be visualized by high resolution optical coherence tomography (OCT). While the high group refractive index of lithium niobate allows a resolution much better than 1 µm, the large dispersion can blur the image and has to be compensated. Therefore, we developed an adaptive dispersion compensation algorithm based on maximizing the intensity of the DWs. By measuring a group of DWs, the mean period of the DWs could be measured with an accuracy of less than 10 nm differentiating samples with only 30 nm distinct periods. By analyzing the peak position, amplitude and phase shift within a DW, we were able to determine steps in the DW of only 50 nm. Furthermore, the inclined course of the DWs in a fan-shaped frequency doubler could be displayed. Therefore, we conclude that OCT is able to provide valuable information about the structure of domain walls in periodically poled lithium niobate (PPLN).

Bottom-Up Assembly of Molecular Nanostructures by Means of Ferroelectric Lithography

Here, we report on the photochemical deposition of Rhodamine 6G (Rh6G) and Alexa647 molecules from aqueous and methanolic solution along 180° ferroelectric (FE) domain walls (DWs) of z-cut lithium niobate (LNO) single crystals. Molecules and FE domains were investigated by means of dynamic-mode AFM, piezoresponse force microscopy (PFM), and confocal scanning fluorescence microscopy. A high deposition affinity for 180° DWs on the LNO surface is observed, leading to the formation of molecular nanowires. Additionally, a more complex deposition pattern for Rh6G adsorbed to the domain areas of freshly poled samples was equally observed, being associated with the DW dynamics. These results are explained by considering contributions from screening-charge-dependent photochemistry as confined to the DWs, UV-induced DW motion, and transient electrostatic fields arising from the metastable defect distribution shortly after poling. Hence, tuning these effects offers the possibility for accurately controlling the complex bottom-up assembly of functional molecular nanostructures through domain-structured ferroelectric templates.

Nano Lithography Based on Domain Patterning of Ferroelectrics

We report on both the assembly of noble-metal nanowires by means of the nanotechnological and large-scale integrable approach of ferroelectric lithography and their performance testing upon electrical transport. Our results on \(\mathrm{ LiNbO}_3\) single crystal templates show that the deposition of different elemental metals from ionic solutions by photochemical reduction is confined to the ferroelectric 180\(^\circ \) domain walls. Current-voltage-characteristics recorded from such nanowires of typically \((30\ldots 300)\,\)µm in length revealed an ohmic behavior that even improved with time. Additionally, we also examined the local topographic and potentiostatic properties of such wires using dynamic scanning force microscopy (SFM) in combination with Kelvin probe force microscopy (KPFM).