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Nanoscale manipulation and characterization of individual molecules is necessary to understand the intricacies of molecular structure, which governs phenomena such as reaction mechanisms, catalysis, local effective temperatures, surface interactions, and charge transport. Here we utilize Raman enhancement between two nanostructured electrodes in combination with direct charge transport measurements to allow for simultaneous characterization of the electrical, optical, and mechanical properties of a single molecule. This multi‐dimensional information yields repeatable, self‐consistent, verification of single‐molecule resolution, and allows for detailed analysis of structural and configurational changes of the molecule in situ. These experimental results are supported by a machine‐learning based statistical analysis of the spectral information and calculations to provide insight into the correlation between structural changes in a single‐molecule and its charge‐transport properties.

 

Systems that are capable of robustly reproducing single‐molecule junctions are an essential prerequisite for enabling the wide‐spread testing of molecular electronic properties, the eventual application of molecular electronic devices, and the development of single‐molecule based electrical and optical diagnostics. Here, a new approach is proposed for achieving a reliable single‐molecule break junction system by using a microelectromechanical system device on a chip. It is demonstrated that the platform can (i) provide subnanometer mechanical resolution over a wide temperature range (≈77–300 K), (ii) provide mechanical stability on par with scanning tunneling microscopy and mechanically controllable break junction systems, and (iii) operate in a variety of environmental conditions. Given these fundamental device performance properties, the electrical characteristics of two standard molecules (hexane‐dithiol and biphenyl‐dithiol) at the single‐molecule level, and their stability in the junction at both room and cryogenic temperatures (≈77 K) are studied. One of the possible distinctive applications of the system is demonstrated, i.e., observing real‐time Raman scattering in a single‐molecule junction. This approach may pave a way to achieving high‐throughput electrical characterization of single‐molecule devices and provide a reliable platform for the convenient characterization and practical application of single‐molecule electronic systems in the future.

 

Quantum interference effects in single-molecule devices can significantly enhance the thermoelectric properties of these devices. However, single-molecule systems have limited utility for power conversion. In this work, we study the effects of destructive quantum interference in molecular junctions on the thermoelectric properties of hybrid, 2-dimensional molecule–nanoparticle monolayers. We study two isomers of benzenedithiol molecules, with either a para or meta configuration for the thiol groups, as molecular interlinkers between gold nanoparticles in the structure. The asymmetrical structure in the meta configuration significantly improves the Seebeck coefficient and power factor over the para configuration. These results suggest that thermoelectric performance of engineered, nanostructured material can be enhanced by harnessing quantum interference effects in the substituent components. 

Abstract Background The all-electronic Single Molecule Break Junction (SMBJ) method is an emerging alternative to traditional polymerase chain reaction (PCR) techniques for genetic sequencing and identification. Existing work indicates that the current spectra recorded from SMBJ experimentations contain unique signatures to identify known sequences from a dataset. However, the spectra are typically extremely noisy due to the stochastic and complex interactions between the substrate, sample, environment, and the measuring system, necessitating hundreds or thousands of experimentations to obtain reliable and accurate results. Results This article presents a DNA sequence identification system based on the current spectra of ten short strand sequences, including a pair that differs by a single mismatch. By employing a gradient boosted tree classifier model trained on conductance histograms, we demonstrate that extremely high accuracy, ranging from approximately 96 % for molecules differing by a single mismatch to 99.5 % otherwise, is possible. Further, such accuracy metrics are achievable in near real-time with just twenty or thirty SMBJ measurements instead of hundreds or thousands. We also demonstrate that a tandem classifier architecture, where the first stage is a multiclass classifier and the second stage is a binary classifier, can be employed to boost the single mismatched pair’s identification accuracy to 99.5 %. Conclusions A monolithic classifier, or more generally, a multistage classifier with model specific parameters that depend on experimental current spectra can be used to successfully identify DNA strands.