Alessandro Lunghi

Multifunctional Guest-Hosting Triple-Stranded Helicates: From Anion Recognition to Quantum Information Applications 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.

Our recent accounts on Triple-stranded supramolecular helicates enable host–guest synergy, tunable spin-crossover, single-ion magnetism, anion recognition, and quantum coherence advances. Cheers to All 😇😊 @labmoldesign-ub.bsky.social @hymat-inma.bsky.social
pubs.acs.org/doi/10.1021/...

On the challenge of simulating dipolar contributions to spin relaxation with generalized cluster correlation expansion methods 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...

New preprint out:

On the challenge of simulating dipolar contributions to spin relaxation with generalized cluster correlation expansion methods

arxiv.org/abs/2602.14613

Come join me in Ireland @ucddublin.bsky.social @ucdchemistry.bsky.social! Help us understand the messiness of cross-talk in metal-ion batteries!

#BattChat #NewPI #sustainability #electrochem

Come join our team at Trinity College Dublin's @tcddublin.bsky.social School of Physics, where we are hiring two new Assistant Professors, one in Physics (experimental) and one in Astrophysics.

See www.tcd.ie/hr/vacancies/ and www.tcd.ie/physics/

Please share! #physics #academicjobs #physicsjobs

Until we are able to fairly assess the quality of our own work without the need of surrogates like journals' prestige, we won't be able to fix the way peer recognition and faculty hiring/promotion is managed and we remain stuck in this loop.

I think a big change in mentality by researchers and faculty would also be needed to stop all this. I have often the feeling that we are incapable of judging the merit of literature if it doesn't come with a rubber stamp of an IF or similar.

I guess having funders to directly pay the society to support their publishing branch would in the end be the same as giving money to researchers to pay APCs but with the advantage of having a much bigger negotiating power, is that what you are suggesting?

Very interesting, what's your take on non-profit publishers charging APCs for OA? Is that justified?

Chiral Dysprosium-[7]Helicene Macrocycles Showing Record Single-Molecule Magnet Properties in the Lanthanide–Helicene Family 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...

A beautiful slow-relaxing chiral Dy SMM by Zhu, Tang and collaborators, with simulations by L. Mariano. Congrats!

@erc.europa.eu

pubs.acs.org/doi/10.1021/...

I knew you'd say that 😆

Now we want to know the answer

Spin decoherence in molecular crystals: Nuclear vs electronic spin baths The loss of information about the relative phase between two quantum states, known as decoherence, strongly limits resolution in electron paramagnetic spectrosc

What really drives electron spin decoherence in molecular crystals at low-T? Nuclear or Electron spins?

Turns out you have do magnetically dilute your samples quite a bit if you want to really remove electron-electron dipolar interactions...

pubs.aip.org/aip/jcp/arti...

So happy this piece is finally out! A tremendous collaborative effort of colleagues and friends from 8 institutions all over Europe. Thank you! doi.org/10.1038/s414...
Photochemistry and photophysics in a single crystal @jagiellonskiuni.bsky.social @cleracr.bsky.social @natcomms.nature.com

This Friday is #EuropeanResearchersNight ⚗️🧪Come visit us and other research groups @TCD_Chemistry
in @tcdTBSI @TCD_Chemistry @tcddublin.bsky.social . Everyone is welcome 📢! Great science and fun people 👨‍🔬👩‍🔬😀#porphyrins #chlorophyll #cubane #BODIPY #PDT #bicyclopentane @researchireland.ie

#chemjobs #compchem

Assistant Professorship in Theoretical Chemistry at University of Cambridge

www.ch.cam.ac.uk/job/52637

Optimizing Carrier Balance in CsPbBr3 Nanocrystal LEDs: The Role of Alkyl Ligands and Polar Electron Transport Layers 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...

Happy to share my latest collaborative work from @mpip-mainz.mpg.de
Optimizing Carrier Balance in CsPbBr3 Nanocrystal LEDs: The Role of Alkyl Ligands and Polar Electron Transport Layers - Advanced Optical Materials - Wiley Online Library advanced.onlinelibrary.wiley.com/doi/10.1002/...

🤤

Supramolecular Interactions Modulate Raman Relaxation in D5h Symmetric Dy(III) Single-Molecule Magnets Opening the Magnetic Hysteresis up to 50 K 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...

A preprint from a collaborazion with Qian-Cheng Luo from the group of Yan-Zhen Zheng:

"Supramolecular Interactions Modulate Raman Relaxation in D5h Symmetric Dy(III) Single-Molecule Magnets Opening the Magnetic Hysteresis up to 50 K"

chemrxiv.org/engage/chemr...

Generating New Coordination Compounds via Multireference Simulations, Genetic Algorithms, and Machine Learning: The Case of Co(II) and Dy(III) Molecular Magnets 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...

The work of Lion, Zahra and Lorenzo

Generating New Coordination Compounds via Multireference Simulations, Genetic Algorithms, and Machine Learning: The Case of Co(II) and Dy(III) Molecular Magnets

Now out in JACS Au 🔥🔥

@erc.europa.eu

pubs.acs.org/doi/10.1021/...

A Multireference Picture of Electronic Excited States in Vanadyl and Copper Tetraphenyl Porphyrin Molecular Qubits

Now published in JPC A

Excellent job by @arups.bsky.social 👏👏

@erc.europa.eu and MSCA

pubs.acs.org/doi/10.1021/...

Fourth-order quantum master equations reveal that spin-phonon decoherence undercuts long magnetization relaxation times in single-molecule magnets 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...

New preprint out:

"Fourth-order quantum master equations reveal that spin-phonon decoherence undercuts long magnetization relaxation times in single-molecule magnets"

arxiv.org/abs/2507.20716

@erc.europa.eu

Mariano teaching us how to compute vibronic coupling

Loosely quoting a synthetic coordination chemist friend of mine: Same ingredients, tools and recipe in the hands of a michelene star chef or a random person will lead to very different results

The Mechanism of Spin-Phonon Relaxation in Endohedral Metallofullerene Single Molecule Magnets

Just made it into @chemicalscience.rsc.org

A work in collab with Rajaraman's group at IITB

@erc.europa.eu

pubs.rsc.org/en/Content/A...

Optical control of spin states in magnetic molecules 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…

Optical control of spin states in magnetic molecules:

A few thoughts on a rapidly evolving and very promising research topic from myself and Matteo Atzori

www.sciencedirect.com/science/arti...

Great taste of Irish food, beer and music at @ecmols2025.bsky.social dinner at #merryploughboypub

Here we go with our first speaker in the final session of day2 with Prof. Elke Scheer from University of Konstanz #ECMOLS2025

The second day of #ECMolS2025 concluded with the final session, featuring a compelling talk by Prof. Pascal Gehring from Université catholique de Louvain

Third speaker from the 2nd session on Day2 is delivered by Prof. Mathias O. Senge from @tcddublin @TCD_Chemistry #ECMolS2025

Our first speaker (tutorial speaker) for the morning session on Day2 is Prof. Fernando Luis from the University of Zaragoza #ecmols2025