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Instruments / Technical Area	Publication Details	Published
I07-Surface & interface diffraction	Electron spin as fingerprint for charge generation and transport in doped organic semiconductors Alberto Privitera , Ross Warren , Giacomo Londi , Pascal Kaienburg , Junjie Liu , Andreas Sperlich , Andreas E. Lauritzen , Oliver Thimm , Arzhang Ardavan , David Beljonne , Moritz Riede Journal Of Materials Chemistry C 210 DOI: 10.1039/D0TC06097F Diamond Proposal Number(s): [20426] Open Access Show Abstract ▼ Abstract: We use the electron spin as a probe to gain insight into the mechanism of molecular doping in a p-doped zinc phthalocyanine host across a broad range of temperatures (80–280 K) and doping concentrations (0–5 wt% of F6-TCNNQ). Electron paramagnetic resonance (EPR) spectroscopy discloses the presence of two main paramagnetic species distinguished by two different g-tensors, which are assigned based on density functional theory calculations to the formation of a positive polaron on the host and a radical anion on the dopant. Close inspection of the EPR spectra shows that radical anions on the dopants couple in an antiferromagnetic manner at device-relevant doping concentrations, thereby suggesting the presence of dopant clustering, and that positive polarons on the molecular host move by polaron hopping with an activation energy of 5 meV. This activation energy is substantially smaller than that inferred from electrical conductivity measurements (∼233 meV), as the latter also includes a (major) contribution from charge-transfer state dissociation. It emerges from this study that probing the electron spin can provide rich information on the nature and dynamics of charge carriers generated upon doping molecular semiconductors, which could serve as a basis for the design of the next generation of dopant and host materials.	Feb 2021
I19-Small Molecule Single Crystal Diffraction	Making hybrid [n]-rotaxanes as supramolecular arrays of molecular electron spin qubits Antonio Fernandez , Jesus Ferrando Soria , Eufemio Moreno Pineda , Floriana Tuna , Iñigo J. Vitorica-Yrezabal , Christiane Knappke , Jakub Ujma , Chris Muryn , Grigore A. Timco , Perdita E. Barran , Arzhang Ardavan , Richard E. P. Winpenny Nature Communications 7 DOI: 10.1038/ncomms10240 Open Access Show Abstract ▼ Abstract: Quantum information processing (QIP) would require that the individual units involved—qubits—communicate to other qubits while retaining their identity. In many ways this resembles the way supramolecular chemistry brings together individual molecules into interlocked structures, where the assembly has one identity but where the individual components are still recognizable. Here a fully modular supramolecular strategy has been to link hybrid organic–inorganic [2]- and [3]-rotaxanes into still larger [4]-, [5]- and [7]-rotaxanes. The ring components are heterometallic octanuclear [Cr7NiF8(O2CtBu)16]– coordination cages and the thread components template the formation of the ring about the organic axle, and are further functionalized to act as a ligand, which leads to large supramolecular arrays of these heterometallic rings. As the rings have been proposed as qubits for QIP, the strategy provides a possible route towards scalable molecular electron spin devices for QIP. Double electron–electron resonance experiments demonstrate inter-qubit interactions suitable for mediating two-qubit quantum logic gates.	Jan 2016
I10-Beamline for Advanced Dichroism - scattering	Probing the local electronic structure in metal halide perovskites through cobalt substitution Amir A. Haghighirad , Matthew T. Klug , L. B. Duffy , Junjie Liu , Arzhang Ardavan , Gerrit Van Der Laan , Thorsten Hesjedal , Henry J. Snaith Small Methods 642 DOI: 10.1002/smtd.202300095 Diamond Proposal Number(s): [16141] Open Access Show Abstract ▼ Abstract: Owing to the unique chemical and electronic properties arising from 3d-electrons, substitution with transition metal ions is one of the key routes for engineering new functionalities into materials. While this approach has been used extensively in complex metal oxide perovskites, metal halide perovskites have largely resisted facile isovalent substitution. In this work, it is demonstrated that the substitution of Co2+ into the lattice of methylammonium lead triiodide imparts magnetic behavior to the material while maintaining photovoltaic performance at low concentrations. In addition to comprehensively characterizing its magnetic properties, the Co2+ ions themselves are utilized as probes to sense the local electronic environment of Pb in the perovskite, thereby revealing the nature of their incorporation into the material. A comprehensive understanding of the effect of transition metal incorporation is provided, thereby opening the substitution gateway for developing novel functional perovskite materials and devices for future technologies.	Mar 2023

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