Chemical Synthesis at Surfaces with Atomic Precision: Taming Complexity and Perfection

Wang, Can; Chi, Lifeng; Ciesielski, Artur; Samorı́, Paolo

doi:10.1002/anie.201906645

Cited by 18 publications

(16 citation statements)

References 145 publications

(224 reference statements)

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“…Moreover, it is reported that chemical reactions can occur in the molecule junctions. [7][8][9][10][11][12][13] Thus, single-molecule junction is an ideal platform to obtain the real-time information of chemical reactions. For example, Guo integrated a single molecule Pd catalyst into GMG-SMJ and achieved the real-time and full description of Suzuki-Miyaura cross-coupling reaction.…”

Section: Introductionmentioning

confidence: 99%

In Situ Monitoring of Transmetallation in Electric Potential-Promoted Oxidative Coupling in a Single-Molecule Junction

et al. 2023

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To monitor and investigate chemical reaction in real-time and in situ is a long-standing and challenging goal in chemistry. Herein, an electric potential-promoted oxidative coupling reaction of organoboron compounds without the addition of base is reported, and the transmetallation process involved is monitored in real-time and in situ with STMBJ technique. We found the electric potential applied determined the transmetallation. At low bias voltage, the first-step transmetallation process occurred and afforded Au-C bonded aryl gold intermediates. The electronic properties of organoboron compounds have a strong influence on transmetallation process, and electron-rich compounds facilitate this transformation. At high bias voltage, the second-step transmetallation process took place, and the corresponding intermediate ( highly reactive diaryl metal complex) was detected with the assistant of Pd (OAc) 2 . Our work demonstrates the applications of STMBJ on in situ monitoring and catalyzing of chemical reactions, and provides a new methodology to fabricate singlemolecule devices.

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Section: Introductionmentioning

confidence: 99%

In Situ Monitoring of Transmetallation in Electric Potential-Promoted Oxidative Coupling in a Single-Molecule Junction

et al. 2023

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“…Milestones include on‐surface‐created polymers, [2] graphene nanoribbons, [3] a plethora of novel molecules and a wealth of one‐ and two‐dimensional nanostructures with intriguing properties [4, 5] . By contrast, the on‐surface covalent coupling by atom manipulation is still in its infancy, and only a few successful examples have been reported so far [6–9] …”

Section: Methodsmentioning

confidence: 99%

Intramolecular Coupling of Terminal Alkynes by Atom Manipulation

et al. 2020

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Glaser-like coupling of terminal alkynes by thermal activation is extensively used in on-surface chemistry. Here we demonstrate an intramolecular version of this reaction performed by atom manipulation. We used voltage pulses from the tip to trigger a Glaser-like coupling between terminal alkyne carbons within a custom-synthesized precursor molecule adsorbed on bilayer NaCl on Cu(111). Different conformations of the precursor molecule and the product were characterized by molecular structure elucidation with atomic force microscopy and orbital density mapping with scanning tunneling microscopy, accompanied by density functional theory calculations. We revealed partially dehydrogenated intermediates, providing insight into the reaction pathway. Scheme 1. a) Intermolecular Glaser-like coupling. b) Intramolecular Glaser-like coupling. c) Synthesis of compound 1.

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“…Solid-state materials, however, form a variety of complex, geometrical structures that are typically not balanced, hypercubic lattices [22,23,24,25]. Moreover, techniques such as scanning tunnelling microscopy and chemical synthesis mean that experimentalists now have an enormous degree of control over the lattice structure of the correlated materials they can synthesise [26,27,28,29,30,31,32,33]. Moire superlattices -stacked sheets of Van der Waals heterostructures -are such materials [34,35,36,37].…”

Section: Introductionmentioning

confidence: 99%

Lieb's Theorem and Maximum Entropy Condensates

Tindall

Schlawin

Sentef

et al. 2021

Quantum

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Coherent driving has established itself as a powerful tool for guiding a many-body quantum system into a desirable, coherent non-equilibrium state. A thermodynamically large system will, however, almost always saturate to a featureless infinite temperature state under continuous driving and so the optical manipulation of many-body systems is considered feasible only if a transient, prethermal regime exists, where heating is suppressed. Here we show that, counterintuitively, in a broad class of lattices Floquet heating can actually be an advantageous effect. Specifically, we prove that the maximum entropy steady states which form upon driving the ground state of the Hubbard model on unbalanced bi-partite lattices possess uniform off-diagonal long-range order which remains finite even in the thermodynamic limit. This creation of a `hot' condensate can occur on any driven unbalanced lattice and provides an understanding of how heating can, at the macroscopic level, expose and alter the order in a quantum system. We discuss implications for recent experiments observing emergent superconductivity in photoexcited materials.

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Chemical Synthesis at Surfaces with Atomic Precision: Taming Complexity and Perfection

Cited by 18 publications

References 145 publications

In Situ Monitoring of Transmetallation in Electric Potential-Promoted Oxidative Coupling in a Single-Molecule Junction

In Situ Monitoring of Transmetallation in Electric Potential-Promoted Oxidative Coupling in a Single-Molecule Junction

Intramolecular Coupling of Terminal Alkynes by Atom Manipulation

Lieb's Theorem and Maximum Entropy Condensates

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