Péter Makk

Regular atomic narrowing of Ni, Fe, and v nanowires resolved by two-dimensional correlation analysis

We present a novel statistical method for the study of stable atomic configurations in breaking nanowires based on the 2D cross-correlation analysis of conductance versus electrode separation traces. Applying this method, we can clearly resolve the typical evolutions of the conductance staircase in some transition metal nanojunctions (Ni, Fe, V) up to high conductance values. In these metals our analysis demonstrates a very well ordered atomic narrowing of the nanowire, indicating a very regular, stepwise decrease of the number of atoms in the minimal cross section of the junction, in contrast to the majority of the metals. All these features are hidden in traditional conductance histograms.

Huge negative differential conductance in Au- H2 molecular nanojunctions

Experimental results showing huge negative differential conductance in gold-hydrogen molecular nanojunctions are presented. The results are analyzed in terms of two-level system (TLS) models: It is shown that a simple TLS model cannot produce peaklike structures in the differential conductance curves, whereas an asymmetrically coupled TLS model gives perfect fit to the data. Our analysis implies that the excitation of a bound molecule to a large number of energetically similar loosely bound states is responsible for the peaklike structures. Recent experimental studies showing related features are discussed within the framework of our model.

Pulling platinum atomic chains by carbon monoxide molecules

The interaction of carbon monoxide molecules with atomic-scale platinum nanojunctions is investigated by low temperature mechanically controllable break junction experiments. Combining plateau length analysis, two-dimensional conductance-displacement histograms and conditional correlation analysis a comprehensive microscopic picture is proposed about the formation and evolution of Pt-CO-Pt single-molecule configurations. Our analysis implies that before pure Pt monoatomic chains are formed a CO molecule infiltrates the junction, first in a configuration that is perpendicular to the contact axis. This molecular junction is strong enough to pull a monoatomic platinum chain with the molecule being incorporated in the chain. Along the chain formation the molecule can either stay in the perpendicular configuration, or rotate to a parallel configuration. The evolution of the single-molecule configurations along the junction displacement shows quantitative agreement with theoretical predictions, justifying the interpretation in terms of perpendicular and parallel molecular alignment. Our analysis demonstrates that the combination of two-dimensional conductance-displacement histograms with conditional correlation analysis is a useful tool to analyze separately fundamentally different types of junction trajectories in single molecule break junction experiments.

Temporal correlations and structural memory effects in break junction measurements

We review data analysis techniques that can be used to study temporal correlations among conductance traces in break junction measurements. We show that temporal histograms are a simple but efficient tool to check the temporal homogeneity of the conductance traces, or to follow spontaneous or triggered temporal variations, like structural modifications in trained contacts, or the emergence of single-molecule signatures after molecule dosing. To statistically analyze the presence and the decay time of temporal correlations, we introduce shifted correlation plots. Finally, we demonstrate that correlations between opening and subsequent closing traces may indicate structural memory effects in atomic-sized metallic and molecular junctions. Applying these methods on measured and simulated gold metallic contacts as a test system, we show that the surface diffusion induced flattening of the broken junctions helps to produce statistically independent conductance traces at room temperature, whereas at low temperature repeating tendencies are observed as long as the contacts are not closed to sufficiently high conductance setpoints. Applying opening-closing correlation analysis on Pt-CO-Pt single-molecule junctions, we demonstrate pronounced contact memory effects and recovery of the molecule for junctions breaking before atomic chains are formed. However, if chains are pulled the random relaxation of the chain and molecule after rupture prevents opening-closing correlations.

Alternative types of molecule-decorated atomic chains in Au–CO–Au single-molecule junctions

Summary We investigate the formation and evolution of Au–CO single-molecule break junctions. The conductance histogram exhibits two distinct molecular configurations, which are further investigated by a combined statistical analysis. According to conditional histogram and correlation analysis these molecular configurations show strong anticorrelations with each other and with pure Au monoatomic junctions and atomic chains. We identify molecular precursor configurations with somewhat higher conductance, which are formed prior to single-molecule junctions. According to detailed length analysis two distinct types of molecule-affected chain-formation processes are observed, and we compare these results to former theoretical calculations considering bridge- and atop-type molecular configurations where the latter has reduced conductance due to destructive Fano interference.

Interaction of hydrogen with metallic nanojunctions

We study the behavior of hydrogen molecules between atomic-sized metallic electrodes using the mechanically controllable break junction technique. We focus on the interaction H2 with monoatomic gold chains demonstrating the possibility of a hydrogen molecule being incorporated in the chain. We also show that niobium is strongly reactive with hydrogen, which enables molecular transport studies between superconducting electrodes. This opens the possibility for a full characterization of the transmission properties of molecular junctions with superconducting subgap structure measurements.