The use of water as a solvent to facilitate supramolecular self-assembly and polymerization is well-documented; however, it is rare that water acts as a monomer that undergoes polymerization. We repor...

The use of water as a solvent to facilitate supramolecular self-assembly and polymerization is well-documented; however, it is rare that water acts as a monomer that undergoes polymerization. We repor...

L’objet élémentaire de mémoire d’ordinateur, appelé bit, peut présenter deux états : 0 ou 1.

Molecular approaches in quantum information science are highly promising, but the synthesis and scale-up of suitable covalently linked moieties represent major challenges. Here it is demonstrated that...

Molecular approaches in quantum information science are highly promising, but the synthesis and scale-up of suitable covalently linked moieties represent major challenges. Here it is demonstrated that...

Molecular approaches in quantum information science are highly promising, but the synthesis and scale-up of suitable covalently linked moieties represent major challenges. Here it is demonstrated that...

Light-driven spin hyperpolarization of organic molecules is a crucial technique for spin-based applications such as quantum information science (QIS) and dynamic nuclear polarization (DNP). Synthetic chemistry provides the design of spins with atomic precision and enables the scale-up of individual spins to hierarchical structures. The high designability and extended pore structure of metal–organic frameworks (MOFs) can control interactions between spins and guest molecules. However, the effective design of polarizing radical electron spins by photoexcitation in MOFs has been unexplored. Here, we show that it is possible to effectively hyperpolarize radical electron spins by harvesting mobile excitons in MOFs. As a proof of concept, we introduce 4-carboxy TEMPO molecules as electron spins into MOF-525, which contains an array of porphyrin chromophores, and demonstrate that this light-harvesting MOF system generates a spin-polarized excited quartet state and doublet ground state even by doping a small amount of electron spins. The current material design leads to the creation of highly spin-polarized nanospaces that can be used for quantum sensing and DNP by efficiently generating high-spin polarization in MOFs doped with small amounts of electron spins to prevent spin relaxation.

For several decades, molecular motor directionality has been rationalized in terms of the free energy of molecular conformations visited before and after the motor takes a step, a so-called power stroke mechanism with analogues in macroscopic engines. Despite theoretical and experimental demonstrations of its flaws, the power stroke language is quite ingrained, and some communities still value power stroke intuition. By building a catalysis-driven motor into simulated numerical experiments, we here systematically report on how directionality responds when the motor is modified accordingly to power stroke intuition. We confirm that the power stroke mechanism generally does not predict motor directionality. Nevertheless, the simulations illustrate that the relative stability of molecular conformations should be included as a potential design element to adjust the motor directional bias. Though power strokes are formally unimportant for determining directionality, we show that practical attempts to alter a power stroke have side effects that can in fact alter the bias. The change in the bias can align with what power stroke intuition would have suggested, offering a potential explanation for why the flawed power stroke mechanism can retain apparent utility when engineering specific systems.

The interaction between unpaired electrons determines the magnetic properties of molecular materials and consequently their applicability. In particular, for ap