Hierarchical Synthesis, Structure, and Photophysical Properties of Gallium‐ and Ruthenium‐Porphyrins with Axially Bonded Azo Ligands

Gao, Yueze; Walter, Vroni; Ferguson, Michael J.; Tykwinski, Rik R.

doi:10.1002/chem.202002030

Cited by 5 publications

(4 citation statements)

References 66 publications

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“…Time-dependent photoswitching is demonstrated in Figures S7−S8 in the Supporting Information. Due to the overlap of the B band of CoPc and the π−π* band of TFAP (which is in accordance with the literature 43,44 ), even at the photostationary state of both V th shifts, a weak absorption at 300−400 nm has been observed. The Q-band turned out to be unaffected by the photoisomerization of TFAP, indicating the absence of electronic coupling between the two chromophores (Figure S8, Supporting Information).…”

Section: Resultssupporting

confidence: 91%

Light-Programmable Logic-in-Memory in 2D Semiconductors Enabled by Supramolecular Functionalization: Photoresponsive Collective Effect of Aligned Molecular Dipoles

et al. 2021

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Nowadays, the unrelenting growth of the digital universe calls for radically novel strategies for data processing and storage. An extremely promising and powerful approach relies on the development of logic-in-memory (LiM) devices through the use of floating gate and ferroelectric technologies to write and erase data in a memory operating as a logic gate driven by electrical bias. In this work, we report an alternative approach to realize the logic-in-memory based on two-dimensional (2D) transition metal dichalcogenides (TMDs) where multiple memorized logic output states have been established via the interfacing with responsive molecular dipoles arranged in supramolecular arrays. The collective dynamic molecular dipole changes of the axial ligand coordinated onto self-assembled metal phthalocyanine nanostructures on the surface of 2D TMD enables large reversible modulation of Fermi level of both n-type molybdenum disulfide (MoS2) and p-type tungsten diselenide (WSe2) field-effect transistors (FETs), to achieve multiple memory states by programming and erasing with ultraviolet (UV) with visible light, respectively. As a result, logic-in-memory devices were built up with our supramolecular layer/2D TMD architecture where the output logic is encoded by the motion of the molecular dipoles. Our strategy relying on the dynamic control of the 2D electronics by harnessing the functions of molecular-dipole-induced memory in a supramolecular hybrid layer represents a versatile way to integrate the functional programmability of molecular science into the next generation nano-electronics.

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Section: Resultssupporting

confidence: 91%

Light-Programmable Logic-in-Memory in 2D Semiconductors Enabled by Supramolecular Functionalization: Photoresponsive Collective Effect of Aligned Molecular Dipoles

et al. 2021

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“…[113] Tykwinski and co-workers incorporated 4,4'-azopyridyl linkers as axial coordinating units in Gaand Ru-metalloporphyrins, 61 (Figure 18). [114] A detailed quantitative analysis was carried out to test the effects of diamagnetic anisotropy (DA) by using 1 H NMR spectroscopic and X-ray crystallographic analyses, which confirmed the previous theoretical predictions about the limit of DA being 2 nm. The transcis photoisomerization of azopyridine-incorporated Ga-porphyrins was ineffective.…”

Section: Porphyrin-based Systemssupporting

confidence: 67%

Section: Porphyrin-based Systemsmentioning

confidence: 99%

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Light‐Switchable Metal Complexes: Introducing Photoresponsive Behaviour Through Azoheteroarenes

et al. 2023

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Azoheteroarenes are emerging classes of photoswitches with versatile scaffolds that offer distinct features such as efficient photoisomerization, tunable stability of the photoswitched states, and bidirectional photoswitching. Moreover, the heteroatoms of such photoswitches exhibit coordination ability to bind to the metal centers. The resulting azoheteroarene‐based metal complexes can be designed and developed to tune various metal‐based properties towards intriguing applications such as in optics, magnetic properties, data storage applications, and catalysis. Despite the diverse utility of azopyridines in such contexts, other azoheteroarenes, particularly the state‐of‐the‐art five‐membered heterocycle‐based photoswitches, remain under‐explored. In this Review, we describe the diverse classes of azoheteroarene‐coordinated metal complexes reported in the literature and survey their photoswitching behaviour and applications. Furthermore, we identify potential azoheteroarene candidates for building photochrome‐coupled metal complexes and supramolecular architectures for maximizing the photo‐tuning of metal‐related properties.

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Laterally π‐Extensed Nitrogen‐Doped Molecular Nanographenes – From Anti‐Kasha Emission to Ping‐Pong Energy Transfer Events

Beneventi,

Schöll,

Platzer

et al. 2024

Advanced Energy Materials

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Nanographenes, which feature at least one dimension smaller than 100 nm, are drawing interdisciplinary attention. Understanding the interplay between structure and properties is, however, still in its infancy. Molecular nanographenes are much better suited to fill this knowledge gap than graphene quantum dots or nanoribbons. Their bottom‐up synthesis allows atomic precision and, thereby, assists in handling structure and connecting it with properties. Herein, the effects of nitrogen‐doping and lateral π‐extension in molecular nanographenes and in their coordination complexes with ruthenium porphyrins are investigated. The presence of just nitrogen resulted in an increase of the fluorescence quantum yield, without, however, affecting the energy levels. Lateral π‐extension of the nanographenes, instead, resulted in a modulation of the excited states energy, which leads to a thermally‐activated dual fluorescence with quantum yields as high as 61%. In the corresponding coordination complexes, lateral π‐extension resulted in a ping‐pong energy transfer cascade, that is, from the nanographene to the metalloporphyrin and back to the nanographene. The results help to directly rationalize properties observed in both graphene quantum dots and nanoribbons. Moreover, they prove that molecular nanographenes are appealing components for solar energy conversion schemes, where the modulation of inter‐component energy transfer is of utmost importance.

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Hierarchical Synthesis, Structure, and Photophysical Properties of Gallium‐ and Ruthenium‐Porphyrins with Axially Bonded Azo Ligands

Cited by 5 publications

References 66 publications

Light-Programmable Logic-in-Memory in 2D Semiconductors Enabled by Supramolecular Functionalization: Photoresponsive Collective Effect of Aligned Molecular Dipoles

Light-Programmable Logic-in-Memory in 2D Semiconductors Enabled by Supramolecular Functionalization: Photoresponsive Collective Effect of Aligned Molecular Dipoles

Light‐Switchable Metal Complexes: Introducing Photoresponsive Behaviour Through Azoheteroarenes

Laterally π‐Extensed Nitrogen‐Doped Molecular Nanographenes – From Anti‐Kasha Emission to Ping‐Pong Energy Transfer Events

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