Lanthanide-based logic: a venture for the future of molecular computing

Zanella, Sofia; Hernández-Rodríguez, M.A.; Ferreira, Rute A. S.; Brites, Carlos D. S.

doi:10.1039/d3cc01827j

Cited by 7 publications

(1 citation statement)

References 87 publications

(126 reference statements)

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“…Triketone cyclophanes, the redox partners of the corresponding trialcohols, have smaller cavities so that 1 and 2 are not accommodated except when perching modes are enabled through hydrophobic contacts. Since cyclophanes 3 and 5 distinguish between popular Ru(II) complexes 1 and 2 , despite their similarities, such selectivity will be exploitable in sensors and logic gates − with “lumophore–spacer–receptor” motifs, as well as in myriad other application areas of 1 . Since our previous effort did not include the excellent selectivity seen here, the analogy of our cyclophane-(bipyridine) 3 Ru(II) system with signaling proteins and allosteric enzymes could not be made until now.…”

Section: Discussionmentioning

confidence: 99%

Remarkably Selective Binding, Behavior Modification, and Switchable Release of (Bipyridine)₃Ru(II) vis-à-vis (Phenanthroline)₃Ru(II) by Trimeric Cyclophanes in Water

Lin

Yao

et al. 2023

JACS Au

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A recurring dream of molecular recognition is to create receptors that distinguish between closely related targets with sufficient accuracy, especially in water. The more useful the targets, the more valuable the dream becomes. We now present multianionic trimeric cyclophane receptors with a remarkable ability to bind the iconic (bipyridine) 3 Ru(II) (with its huge range of applications) while rejecting the nearly equally iconic (phenanthroline) 3 Ru(II). These receptors not only selectively capture (bipyridine) 3 Ru(II) but also can be redox-switched to release the guest. 1D-and 2D(ROESY)-NMR spectroscopy, luminescence spectroscopy, and molecular modeling enabled this discovery. This outcome allows the control of these applications, e.g., as a photocatalyst or as a luminescent sensor, by selectively hiding or exposing (bipyridine) 3 Ru(II). Overall, a 3D nanometric object is selected, picked-up, and dropped-off by a discrete molecular host. The multianionic receptors protect excited states of these metal complexes from phenolate quenchers so that the initial step in photocatalytic phenolate oxidation is retarded by nearly 2 orders of magnitude. This work opens the way for (bipyridine) 3 Ru(II) to be manipulated in the presence of other functional nano-objects so that many of its applications can be commanded and controlled. We have a cyclophane-based toolkit that can emulate some aspects of proteins that selectively participate in cell signaling and metabolic pathways by changing shape upon environmental commands being received at a location remote from the active site.

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Section: Discussionmentioning

confidence: 99%

Remarkably Selective Binding, Behavior Modification, and Switchable Release of (Bipyridine)₃Ru(II) vis-à-vis (Phenanthroline)₃Ru(II) by Trimeric Cyclophanes in Water

Lin

Yao

et al. 2023

JACS Au

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Designing Next‐Generation Molecular Logic Circuits: Photonic Concatenation in Upconverting Nanocrystals

Zanella,

Hernández‐Rodríguez,

et al. 2023

Advanced Optical Materials

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Computers and computing systems are getting an increasingly essential role in society, as revealed by the current emergence of Artificial Intelligence. The further increase in computer systems and digitalization of society will certainly demand innovative computing systems with higher processing speeds at low energetic and capital costs. Remarkable developments in the last five years have been reported for quantum computing; nevertheless, photonic and molecular computing has also been evolving with the potential of reaching the maximum possible miniaturization by using molecules as building blocks for basilar logic systems. One of the main challenges for molecular logic is the logical connection between molecular elements, called concatenation. Until now, concatenation of molecular logic gates has been exclusively reported using chemical species, with obvious practical limitations. In this work, the first photonic concatenation of a NAND with an AND molecular logic gate is presented. The logic system is implemented on nanoplatforms of Yb3+/Er3+ core@shell Sr2YF7 nanocrystals that are used to define combinatory logic gates and temperature‐reconfigurable logic systems. The results show that upconverting nanocrystals are promising platforms for the development of solid‐state molecular logic devices. These devices can reproduce the logical operations that are currently implemented in electronic devices.

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Purely Optical, Reversible, Read‐Write‐Erase Cycling Using Photoswitchable Beads in Micropatterned Arrays

Zhang,

Dharpure,

Philipp

et al. 2024

Advanced Optical Materials

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Using surface‐templated electrophoretic deposition, arrays of polymer beads (photonic units) incorporating photo‐switchable DAE molecules are created, which can be reversibly and individually switched between high and low emission states by direct photo‐excitation, without any energy or electron transfer processes within the molecular system. The micropatterned array of these photonic units is spectroscopically characterized in detail and optimized with respect to both signal contrast and cross‐talk. The optimum optical parameters including laser intensity, wavelength and duration of irradiation are elucidated and ideal conditions for creating reversible on/off cycles in a micropatterned array are determined. 500 such cycles are demonstrated with no obvious on/off contrast attenuation. The ability to process binary information is demonstrated by selectively writing information to the given photonic unit, reading the resultant emissive signal pattern and finally erasing the information again, which in turn demonstrates the possibility of continuous recording. This basic study paves the way for building complex circuits using spatially well‐arranged photonic units.

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Lanthanide-based logic: a venture for the future of molecular computing

Abstract: Managing the continuous and fast-growing volume of information, the progress on the Internet-of-Things, evolution from digitalization to networking, are huge technological chores. Si-based integrated chips face increasing demands as they...

Cited by 7 publications

References 87 publications

Remarkably Selective Binding, Behavior Modification, and Switchable Release of (Bipyridine)₃Ru(II) vis-à-vis (Phenanthroline)₃Ru(II) by Trimeric Cyclophanes in Water

Remarkably Selective Binding, Behavior Modification, and Switchable Release of (Bipyridine)₃Ru(II) vis-à-vis (Phenanthroline)₃Ru(II) by Trimeric Cyclophanes in Water

Designing Next‐Generation Molecular Logic Circuits: Photonic Concatenation in Upconverting Nanocrystals

Purely Optical, Reversible, Read‐Write‐Erase Cycling Using Photoswitchable Beads in Micropatterned Arrays

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Lanthanide-based logic: a venture for the future of molecular computing

Abstract: Managing the continuous and fast-growing volume of information, the progress on the Internet-of-Things, evolution from digitalization to networking, are huge technological chores. Si-based integrated chips face increasing demands as they...

Cited by 7 publications

References 87 publications

Remarkably Selective Binding, Behavior Modification, and Switchable Release of (Bipyridine)3Ru(II) vis-à-vis (Phenanthroline)3Ru(II) by Trimeric Cyclophanes in Water

Remarkably Selective Binding, Behavior Modification, and Switchable Release of (Bipyridine)3Ru(II) vis-à-vis (Phenanthroline)3Ru(II) by Trimeric Cyclophanes in Water

Designing Next‐Generation Molecular Logic Circuits: Photonic Concatenation in Upconverting Nanocrystals

Purely Optical, Reversible, Read‐Write‐Erase Cycling Using Photoswitchable Beads in Micropatterned Arrays

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Product

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Remarkably Selective Binding, Behavior Modification, and Switchable Release of (Bipyridine)₃Ru(II) vis-à-vis (Phenanthroline)₃Ru(II) by Trimeric Cyclophanes in Water

Remarkably Selective Binding, Behavior Modification, and Switchable Release of (Bipyridine)₃Ru(II) vis-à-vis (Phenanthroline)₃Ru(II) by Trimeric Cyclophanes in Water