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Artificial Relativistic Molecules (2002.00603v1)

Published 3 Feb 2020 in cond-mat.mtrl-sci

Abstract: We fabricate artificial molecules composed of heavy atom lead on a van der Waals crystal. Pb atoms templated on a honeycomb charge-order superstructure of IrTe2 form clusters ranging from dimers to heptamers including benzene-shaped ring hexamers. Tunneling spectroscopy and electronic structure calculations reveal the formation of unusual relativistic molecular orbitals within the clusters. The spin-orbit coupling is essential both in forming such Dirac electronic states and stabilizing the artificial molecules by reducing the adatom-substrate interaction. Lead atoms are found to be ideally suited for a maximized relativistic effect. This work initiates the use of novel two dimensional orderings to guide the fabrication of artificial molecules of unprecedented properties.

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Summary

  • The paper demonstrates that Pb clusters on IrTe2 form artificial molecules with uniquely split relativistic orbitals due to strong spin-orbit coupling.
  • It employs scanning tunneling spectroscopy and electronic structure calculations to detail the behavior of Pb 6p states in various cluster configurations.
  • The findings imply that controlling Pb atom distances on vdW crystals can enable exotic quantum states for advanced material and nanotechnology applications.

Exploration of Artificial Relativistic Molecules through Lead Atom Clusters on Van der Waals Crystals

Introduction

The fabrication and investigation of artificial molecules composed of lead (Pb) atoms situated on van der Waals crystal substrates have offered a fascinating glimpse into the formation of unusual molecular orbitals that are relativistic in nature. By strategically positioning Pb atoms on a honeycomb charge-order superstructure of IrTe2, this paper has successfully created a series of molecular clusters whose properties are modulated through strong relativistic effects, primarily due to spin-orbit coupling (SOC). These clusters range from dimers to heptamers, including configurations resembling benzene-like hexagonal rings.

Key Findings and Methodological Approach

Charge Order Superstructure Hosting Pb Clusters

The paper’s pivotal achievement lies in templating Pb atoms on an IrTe2 substrate, leading to the spontaneous assembly of Pb clusters varying in size and form. The most striking configurations are those resembling benzene rings, achieved through the manipulation of interatomic Pb-Pb distances dictated by the substrate. This is complemented by scanning tunneling spectroscopy (STS) and electronic structure calculations which meticulously detail the formation of relativistic molecular orbitals.

Relativistic Molecular Orbitals in Pb Clusters

Through STS, distinct electronic energy levels associated with Pb 6p valence electrons were identified, confirming the partial ionization of Pb adatoms and the shifting of 6p states to higher energy levels — a phenomenon particularly modified by SOC. This leads to the molecular orbital splits into bonding and antibonding states suggesting a direct overlap of relativistic p orbitals of Pb atoms at an exceptionally large interatomic distance.

Mechanism of Pb Atom Interaction

Crucially, the attractive interaction between Pb atoms is attributed exclusively to SOC. The optimal 2a0 distance, enforced by the substrate, facilitates the formation of Pb dimers and larger clusters. This underlying mechanism is unveiled through sophisticated spin-orbit coupling calculations, demonstrating Pb’s uniquely strong relativistic effects which notably influence the templating process on vdW crystals.

Theoretical and Practical Implications

This research not only advances our understanding of relativistic effects in artificial molecules but also opens avenues for fabricating molecules with novel properties. The formation of Dirac molecular orbitals at significantly large Pb-Pb distances distinguishes these artificial molecules from their natural counterparts, offering insights into the quantum mechanical interactions at play in heavy atom clusters.

The practical implications extend to the development of new materials and nanostructures with customized electronic, magnetic, and optical characteristics. The application of such relativistic molecules could revolutionize areas from quantum computing to nanoelectronics, where control over electronic properties at the atomic scale is pivotal.

Future Perspectives

Looking forward, the fabrication techniques and theoretical insights gleaned from this paper provide a robust framework for further exploration into 2D superstructures and the varied potential of vdW heterostructures. The interplay between relativistic SOC effects and substrate-induced modifications beckons a broader investigation into the stabilization mechanisms of artificial molecules and their quantum mechanical behaviors.

Moreover, the potential to leverage these findings in designing materials with exotic quantum states opens promising research trajectories. Exploring magnetic atoms on similar substrates could unveil new interfacial phenomena and quantum states of matter, setting the stage for groundbreaking advancements in material science and nanotechnology.

In essence, this exploration into artificial relativistic molecules marks a significant stride in our quest to harness the quantum mechanical properties of heavy atoms, paving the way for innovations in material science and beyond.

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