The identification of molecules that combine long spin coherence times and efficient spin-optical interfaces, ideally at room temperature, is pivotal towards the development of molecular quantum techn...

Dysprosium-based single-molecule magnets (SMMs) exhibit large magnetic anisotropy and coercive fields, offering the potential to support information storage at the molecular level. Owing to the molecu...

Phonons induce fast dephasing in magnetic molecules.

ConspectusThe growing field of coordination supramolecular chemistry constitutes a fruitful avenue for accessing a variety of multifunctional materials with a range of applications. Their versatility is enhanced if they have the ability to encapsulate guest molecules, opening opportunities for host/guest synergies. One of the most paradigmatic categories of such assemblies is coordination supramolecular helicates, which exhibit a central cavity for the potential allocation of small species, provided that their symmetry and volumes are compatible. The presence of noncovalent interactions (NCIs) between host and guest strongly contributes to the thermodynamic stability of these edifices, sometimes giving rise to a template effect. All those features are exploited for the case of triple-stranded helicates, which are predictably obtained from reactions of metal ions that adopt an octahedral coordination geometry with ligands made of two chelating moieties sufficiently separated by a spacer. The properties of the cavity of the helicate can be tuned by adjusting the central spacer of the ligand, which in turn, may incorporate functionalities facilitating NCIs with potential guests, such as hydrogen bonds. In this manner, a collection of pyrazolylpyridine (or -quinoline) ligands (L) has given rise to a large family of (G@[M2L3])n+ species (where G represents various guests), in which the encapsulated entities are firmly held in place by [N–H···G] hydrogen bonds. These assemblies can thus be employed for the selective recognition of anions or small coordination complexes, capitalizing on the specific architecture of the ligand strands. Furthermore, they have opened a plethora of possibilities for the investigation of synergic multifunctionality. The host can be made to exhibit molecular switching behavior (for example, spin-crossover, SCO, if M = FeII) or single-ion magnet (SIM) behavior (if M = CoII) while the guest has been exploited to tune these properties or to incorporate new ones. More recently, anionic coordination complexes such as these from the series [M(ox)3]3– (“ox” being the oxalate anion and M = Fe, Cr, Al, Ru) have been efficiently trapped inside the metallo-helices. This has unveiled unprecedented phenomena resulting from encapsulation, such as the first manifestation of SIM behavior for CrIII or the enhancement of the quantum coherence of a molecular qubit when acting as the guest. This family has been expanded with the inclusion of the anilate analogues of oxalates, opening unlimited options for multiproperty explorations (such as photophysical, redox chemistry, radical generation, etc.). More recently, within this group of systems, the guest has been employed as a template to selectively assemble specific combinations of two different ligands in the form of G@[M2LxL′(3–x)]m+ heteroleptic helicates, thus leading to a further opportunity of function tunability and enhancement. In this Account, we survey this and other related types of host/guest assemblies and place them in the general context of triple-stranded supramolecular helicates while assessing their impact in fields like molecular magnetism, quantum technologies, or anion recognition.

The study of spin decoherence is often performed by assuming that spin-phonon interactions lead to relaxation at high temperatures, and spin-spin dipolar interactions instead contribute to pure dephas...

Chiral helicene-based metal complexes have emerged as an extremely promising class of multifunctional molecules for a wide range of applications. Despite significant progress in the synthesis of helic...

The loss of information about the relative phase between two quantum states, known as decoherence, strongly limits resolution in electron paramagnetic spectrosc

Applications are invited for a University Assistant Professor to work in the area of theoretical chemistry, broadly defined, to be taken up in October 2026 (or earlier, by agreement). The successful a...

Ligands are key to passivate the surface of CsPbBr3 nanocrystals, but not all are equally effective. Beyond the insulating nature of alkyl chains, the interaction between a ligand's anchoring group a...

Dysprosium-based single-molecule magnets (SMMs) exhibit large values of magnetic anisotropy and large coercive fields, offering the potential to support magnetic information storage at the molecular l...

The design of coordination compounds with target properties often requires years of continuous feedback loop between theory, simulations, and experiments. In the case of magnetic molecules, this conve...

Spin-phonon interaction is known to drive magnetic relaxation in solid-state systems, but little evidence is available on how it affects coherence time. Here we extend fourth-order quantum master equa...

This study presents the first-ever investigation of spin-phonon coupling mechanisms in fullerene-based single-molecule magnets (SMMs) using ab initio CASSCF combined with DFT calculations. While lanth...

Optical methods stand out as one of the most promising approaches to initialize and read-out spin states in molecules. Herein we critically review ear…

The nature of electronic excited states has a deep impact on the dynamics of molecular spins, but remains poorly understood and characterized. Here we carry out a thorough multiconfigurational investi...

The loss of information about the relative phase between two quantum states, known as decoherence, strongly limits resolution in electron paramagnetic spectroscopy and hampers the use of molecules for...

The design of coordination compounds with target properties often requires years of continuous feedback loop between theory, simulations and experiments. In the case of magnetic molecules, this conven...

Magnetic relaxation in coordination compounds is largely dominated by the interaction of the spin with phonons. Although a comprehensive understanding of spin-phonon relaxation has been achieved for m...