The use of molecular spin state as a quantum of information for storage, sensing and computing has generated considerable interest in the context of next-generation data storage and communication devices 1, 2 , opening avenues for developing multifunctional molecular spintronics 3 . Such ideas have been researched extensively, using singlemolecule magnets 4, 5 and molecules with a metal ion 6 or nitrogen vacancy 7 as localized spin-carrying centres for storage and for realizing logic operations 8 . However, the electronic coupling between the spin centres of these molecules is rather weak, which makes construction of quantum memory registers a challenging task 9 . In this regard, delocalized carbon-based radical species with unpaired spin, such as phenalenyl 10 , have shown promise. These phenalenyl moieties, which can be regarded as graphene fragments, are formed by the fusion of three benzene rings and belong to the class of open-shell systems. The spin structure of these molecules responds to external stimuli 11, 12 (such as light, and electric and magnetic fields), which provides novel schemes for performing spin memory and logic operations. Here we construct a molecular device using such molecules as templates to engineer interfacial spin transfer resulting from hybridization and magnetic exchange interaction with the surface of a ferromagnet; the device shows an unexpected interfacial magnetoresistance of more than 20 per cent near room temperature. Moreover, we successfully demonstrate the formation of a nanoscale magnetic molecule with a well-defined magnetic hysteresis on ferromagnetic surfaces. Owing to strong magnetic coupling with the ferromagnet, such independent switching of an adsorbed magnetic molecule has been unsuccessful with single-molecule magnets 13 . Our findings suggest the use of chemically amenable phenalenyl-based molecules as a viable and scalable platform for building molecular-scale quantum spin memory and processors for technological development.The diversity and flexibility of molecular synthesis has given researchers ample freedom to design functional molecules for spintronics. These include molecular magnets 14 , spinfilter molecules 15 , spin-crossover molecules 16 , molecular batteries 17 , molecular conductors 10 , molecular switches 12 , and spacer layers for organic spin valves 18 and magnetic tunnel junctions 19,20 . Using such synthetic techniques, we have designed a neutral planar phenalenyl-based molecule, zinc methyl phenalenyl (ZMP, C 14 H 10 O 2 Zn; see Fig. 1a and Methods), that has no net spin. When these molecules are grown on a ferromagnetic surface, interface spin transfer causes a hybridized organometallic supramolecular magnetic layer to develop, which shows a large magnetic anisotropy and spin-filter properties 21 . This interface layer creates a spin-dependent resistance and gives rise to an interface magnetoresistance (IMR) effect.
This article reports the reduction of [{2,6-iPr2C6H3NC(CH3)}2C6H3SnCl] (1) with potassium graphite to afford a new distannyne [{2,6-iPr2C6H3NC(CH3)}2C6H3Sn]2 (2) with a Sn–Sn bond. The most striking phenomenon of 2 is the presence of two differently coordinated Sn atoms (one is three-coordinated, the other is four-coordinated). The Sn–Sn bond length in 2 is 2.8981(9) Å, which is very close to that of a Sn–Sn single bond (2.97–3.06 Å). To elucidate the nature of the Sn–Sn bond, DFT calculation is carried out that shows there is no multiple bond character in 2. Furthermore, the reaction of 2 with white P4 affords the tetraphosphabicylobutane derivative 3. This is the first example of gentle activation of white phosphorus by a compound with low valent Sn atoms. Note that, unlike 2, in 3 both Sn atoms are four-coordinated.
We have previously shown that the self-assembly of dibenzosuberone-based bis-monodentate pyridyl ligands L(1) with Pd(II) cations leads to the quantitative formation of interpenetrated coordination cages [BF4@Pd4L(1)8]. The BF4(-) anion inside the central cavity serves as a template, causing the outer two pockets to show a tremendous affinity for allosteric binding of two small chloride anions. Here we show that derivatization of the ligand backbone with a bulky aryl substituent allows us to control the dimerization and hence the guest-binding ability of the cage by the choice of the templating anion. Steric constraints imposed by L(2) prevent the large BF4(-) anion from serving as a template for the formation of interpenetrated double cages. Instead, a single isomer of the monomeric cage [Pd2L(2)4] is formed. Addition of the small anionic template Cl(-) permits dimerization, yielding the interpenetrated double cage [Cl@Pd4L(2)8], whose enlarged outer pockets show a preference for the binding of large anions such as ReO4(-).
An acyclic P4 chain supported by a silicon‐substituted amidinato ligand was formed from the reaction of PhC(NtBu)2SiN(TMS)2 with P4 (TMS=Me3Si). This is the first example of an acyclic SiP chain that contains 6π electrons. When the benzamidinato moiety was replaced with Cp* (Cp*=Me5C5), an unusual silicon–phosphorus cage surprisingly formed (see scheme).
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