Single Molecular Devices by Atomic Manipulation

Projektinformationen

MolDAM

ID Finanzhilfevereinbarung: 951519

DOI

10.3030/951519

EK-Unterschriftsdatum 22 Januar 2021

Startdatum 1 Oktober 2021

Enddatum 30 September 2027

Finanziert unter

• EXCELLENT SCIENCE - European Research Council (ERC)

Gesamtkosten

€ 9 068 885,00

EU-Beitrag

€ 9 068 885,00

Koordiniert durch

IBM RESEARCH GMBH
Switzerland

Periodic Reporting for period 2 - MolDAM (Single Molecular Devices by Atomic Manipulation)

Berichtszeitraum: 2023-04-01 bis 2024-09-30

Zusammenfassung vom Kontext und den Gesamtzielen des Projekts

Breakthroughs in on-surface chemistry and characterization techniques have recently enabled the creation of novel molecules and the direct imaging of reaction intermediates at the single molecule level. Here, by employing the novel concepts of charge manipulation within molecules and coherent control of reactions by lightwave scanning tunnelling microscopy, we will bring the control and resolution of chemical reactions to an unparalleled level. We will combine our expertise in solution synthesis of dedicated organic molecules, on-surface chemistry, atom manipulation and single-molecule characterization with ultimate resolution in space and time. The combination of on-surface chemistry with charge-state control, possible by working on insulating supports, will unlock a plethora of novel charge-driven reaction pathways far from equilibrium. Employing ultrafast pulses, we aim to resolve chemical reactions with unprecedented resolution in the space and time domain unravelling the mechanisms of relevant molecular transformations. We will discover and characterize novel on-surface reactions, elusive molecules, new allotropes of carbon, intermediates and transition states and fabricate artificial molecular machines and complex molecular networks with engineered topologically protected band structures.

Arbeit, die ab Beginn des Projekts bis zum Ende des durch den Bericht erfassten Berichtszeitraums geleistet wurde, und die wichtigsten bis dahin erzielten Ergebnisse

We demonstrated selectivity in single-molecule reactions by tip-induced redox chemistry, in a collaboration of all three groups, published in Science 377, 298–301 (2022). We obtained reversible and selective bond formation and dissociation promoted by tip-induced reduction-oxidation reactions on a surface. Molecular rearrangements leading to different constitutional isomers are selected by the polarity and magnitude of applied voltage pulses from the tip of a combined scanning tunnelling and atomic force microscope (STM/AFM). Characterization of voltage dependence of the reactions and determination of reaction rates show selectivity in constitutional isomerization reactions and provide insight into the underlying mechanisms. We found that the energy landscape of the isomers in different charge states is important to rationalize the selectivity. Tip-induced selective single-molecule reactions increase our understanding of redox chemistry and could lead to novel molecular machines. The control over the reactions and their reversibility explored in this system, also provide a promising step towards systems that would be suitable for resolving with atomic resolution chemical reactions in time.

Fortschritte, die über den aktuellen Stand der Technik hinausgehen und voraussichtliche potenzielle Auswirkungen (einschließlich der bis dato erzielten sozioökonomischen Auswirkungen und weiter gefassten gesellschaftlichen Auswirkungen des Projekts)

Charge control within molecular devices on insulating supports will allow us to study electron transfer, carrier generation and recombination, redox-reactions and electroluminescence at the molecular level. Novel molecular machines will be directed by controlling single-electron charges within the device. Logic functions based on single-electron transfer will be implemented in molecular networks. Controlling and investigating these atomically defined devices on their intrinsic length and time scales will advance our fundamental understanding of the molecular world with impact on fields as diverse as chemical synthesis, light harvesting, molecular machinery and computing. In the process we expect to introduce novel synthetic procedures in the field of on-surface chemistry and single molecule reactions, as well as designing new graphene nanostructures with improved properties.

Selectivity in single-molecule reactionsby tip-induced redox chemistry. Science 377, 298 (2022)