Concept: Pauli exclusion principle
The interaction between the inner atoms/cluster and the outer fullerene cage is the source of various novel properties of endohedral metallofullerenes. Herein, we introduce an adatom-type spin polarization defect on the surface of a typical endohedral stable U(2)@C(60) to predict the associated structure and electronic properties of U(2)@C(61) based on the density functional theory method. We found that defect induces obvious changes in the electronic structure of this metallofullerene. More interestingly, the ground state of U(2)@C(61) is nonet spin in contrast to the septet of U(2)@C(60). Electronic structure analysis shows that the inner U atoms and the C ad-atom on the surface of the cage contribute together to this spin state, which is brought about by a ferromagnetic coupling between the spin of the unpaired electrons of the U atoms and the C ad-atom. This discovery may provide a possible approach to adapt the electronic structure properties of endohedral metallofullerenes.
Substitutional donor atoms in silicon are promising qubits for quantum computation with extremely long relaxation and dephasing times demonstrated. One of the critical challenges of scaling these systems is determining inter-donor distances to achieve controllable wavefunction overlap while at the same time performing high fidelity spin readout on each qubit. Here we achieve such a device by means of scanning tunnelling microscopy lithography. We measure anti-correlated spin states between two donor-based spin qubits in silicon separated by 16 ± 1 nm. By utilising an asymmetric system with two phosphorus donors at one qubit site and one on the other (2P-1P), we demonstrate that the exchange interaction can be turned on and off via electrical control of two in-plane phosphorus doped detuning gates. We determine the tunnel coupling between the 2P-1P system to be 200 MHz and provide a roadmap for the observation of two-electron coherent exchange oscillations.
Spin selectivity in a ferromagnet results from a difference in the density of up- and down-spin electrons at the Fermi energy as a consequence of which the scattering rates depend on the spin orientation of the electrons. This property is utilized in spintronics to control the flow of electrons by ferromagnets in a ferromagnet (F1)/normal metal (N)/ferromagnet (F2) spin valve, where F1 acts as the polarizer and F2 the analyser. The feasibility of superconducting spintronics depends on the spin sensitivity of ferromagnets to the spin of the equal spin-triplet Cooper pairs, which arise in superconductor (S)-ferromagnet (F) heterostructures with magnetic inhomogeneity at the S-F interface. Here we report a critical temperature dependence on magnetic configuration in current-in-plane F-S-F spin valves with a holmium spin mixer at the S-F interface providing evidence of a spin selectivity of the ferromagnets to the spin of the triplet Cooper pairs.
The origin of the anomeric effect has remained an open question. After Mo demonstrated that hyperconjugation is not responsible for the anomeric effect [Y. Mo, Nature Chem., 2010, 2, 666.], electrostatic interactions and Pauli repulsions have been at the center of this debate. In this work, the total energies of the most stable rotamers of the equatorial and axial anomers of fluoro, hydroxyl, cyano and amino groups in cyclohexane and 2-substituted tetrahydropyran rings are decomposed into their fundamental kinetic, electrostatic and exchange components. In this partitioning scheme, the differences in the total energies among the most stable rotamers of each anomer correlate very well with the differences in the exchange components, revealing that the anomeric effect has no electrostatic origin. Indeed, the anomeric effect is dominated by the exchange energy. This proposal for the origin of the anomeric effect brings new insights that, once incorporated, may improve qualitative chemical models. Implications of this new proposal for the origin of the anomeric effect on geometric parameters and solvation are also discussed.
Recently, much effort has been devoted to improve the efficiency of organic photovoltaic solar cells based on blends of donors and acceptors molecules in bulk heterojunction architecture. One of the major losses in organic photovoltaic devices has been recombination of polaron pairs at the donor-acceptor domain interfaces. Here, we present a novel method to suppress polaron pair recombination at the donor-acceptor domain interfaces and thus improve the organic photovoltaic solar cell efficiency, by doping the device active layer with spin ½ radical galvinoxyl. At an optimal doping level of 3 wt%, the efficiency of a standard poly(3-hexylthiophene)/1-(3-(methoxycarbonyl)propyl)-1-1-phenyl)(6,6)C(61) solar cell improves by 18%. A spin-flip mechanism is proposed and supported by magneto-photocurrent measurements, as well as by density functional theory calculations in which polaron pair recombination rate is suppressed by resonant exchange interaction between the spin ½ radicals and charged acceptors, which convert the polaron pair spin state from singlet to triplet.
The integration of ferromagnetic Mn5Ge3 with the Ge matrix is promising for spin injection in a silicon-compatible geometry. In this paper, we report the preparation of magnetic Mn5Ge3 nanocrystals embedded inside the Ge matrix by Mn ion implantation at elevated temperature. By X-ray diffraction and transmission electron microscopy, we observe crystalline Mn5Ge3 with variable size depending on the Mn ion fluence. The electronic structure of Mn in Mn5Ge3 nanocrystals is a 3d6 configuration, which is the same as that in bulk Mn5Ge3. A large positive magnetoresistance has been observed at low temperatures. It can be explained by the conductivity inhomogeneity in the magnetic/semiconductor hybrid system.
The single phase Pb0.8Co0.2TiO3 thin films were synthesized on a Pt/Ti/SiO2/Si substrate by the sol-gel route. The present films exhibited homogeneous microstructure with low porosity. O 1s X-ray photoelectron spectroscopy (XPS) was used to detect the amount of oxygen vacancies. The ferroelectric measurements showed that the ferroelectricity deteriorates with the increase in the number of oxygen vacancies. X-ray absorption spectroscopy (XAS) and XPS were used to study the electronic structure. The results indicated that the decreased ferroelectricity might be ascribed to the weakened hybridization between O 2p and Pb 6s and Ti 3d orbitals. The ferromagnetic behaviors were also observed in the thin films and saturated magnetization raised monotonously with the oxygen vacancy rising due to the enhanced F-center exchange interaction. Magnetoelectric coupling of the films weakened with oxygen vacancy increase.
Spin qubits based on interacting spins in double quantum dots have been demonstrated successfully. Readout of the qubit state involves a conversion of spin to charge information, which is universally achieved by taking advantage of a spin blockade phenomenon resulting from Pauli’s exclusion principle. The archetypal spin blockade transport signature in double quantum dots takes the form of a rectified current. At present, more complex spin qubit circuits including triple quantum dots are being developed. Here we show, both experimentally and theoretically, that in a linear triple quantum dot circuit the spin blockade becomes bipolar with current strongly suppressed in both bias directions and also that a new quantum coherent mechanism becomes relevant. In this mechanism, charge is transferred non-intuitively via coherent states from one end of the linear triple dot circuit to the other, without involving the centre site. Our results have implications for future complex nanospintronic circuits.
The Bethe-Slater (BS) curve describes the relation between the exchange coupling and interatomic distance. Based on a simple argument of orbital overlaps, it successfully predicts the transition from antiferromagnetism to ferromagnetism, when traversing the 3d series. In a previous article [Phys. Rev. Lett. 116, 217202 (2016)] we reported that the dominant nearestneighbour (NN) interaction for 3d metals in the bcc structure indeed follows the BS curve, but the trends through the series showed a richer underlying physics than was initially assumed. The orbital decomposition of the inter-site exchange couplings revealed that various orbitals contribute to the exchange interactions in a highly non-trivial and sometimes competitive way. In this communication we perform a deeper analysis by comparing 3d metals in the bcc and fcc structures. We find that there is no coupling between the E g orbitals of one atom and T 2g orbitals of its NNs, for both cubic phases. We demonstrate that these couplings are forbidden by symmetry and formulate a general rule allowing to predict when a similar situation is going to happen. In γ-Fe, as in α-Fe, we find a strong competition in the symmetry-resolved orbital contributions and analyse the differences between the high-spin and low-spin solutions.
Epitaxial attachment of quantum dots into ordered superlattices enables the synthesis of quasi-two-dimensional materials that theoretically exhibit features such as Dirac cones and topological states, and have major potential for unprecedented optoelectronic devices. Initial studies found that disorder in these structures causes localization of electrons within a few lattice constants, and highlight the critical need for precise structural characterization and systematic assessment of the effects of disorder on transport. Here we fabricated superlattices with the quantum dots registered to within a single atomic bond length (limited by the polydispersity of the quantum dot building blocks), but missing a fraction (20%) of the epitaxial connections. Calculations of the electronic structure including the measured disorder account for the electron localization inferred from transport measurements. The calculations also show that improvement of the epitaxial connections will lead to completely delocalized electrons and may enable the observation of the remarkable properties predicted for these materials.