Junjie Liu

Quantum Interference in Graphene Nanoconstrictions

We report quantum interference effects in the electrical conductance of chemical vapor deposited graphene nanoconstrictions fabricated using feedback controlled electroburning. The observed multimode Fabry-Pérot interferences can be attributed to reflections at potential steps inside the channel. Sharp antiresonance features with a Fano line shape are observed. Theoretical modeling reveals that these Fano resonances are due to localized states inside the constriction, which couple to the delocalized states that also give rise to the Fabry-Pérot interference patterns. This study provides new insight into the interplay between two fundamental forms of quantum interference in graphene nanoconstrictions.

Quantum spin coherence in halogen-modified Cr7Ni molecular nanomagnets

Among the factors determining the quantum coherence of the spin in molecular magnets are the presence and the nature of nuclear spins in the molecule. We have explored modifying the nuclear-spin environment in Cr7Ni-based molecular nanomagnets by replacing hydrogen atoms with deuterium or the halogen atoms, fluorine or chlorine. We find that the spin coherence, studied at low temperatures by pulsed electron-spin resonance, is modified by a range of factors, including nuclear spin and magnetic moment, changes in dynamics owing to nuclear mass, and molecular morphology changes.

Three-terminal graphene single-electron transistor fabricated using feedback-controlled electroburning

We report room-temperature Coulomb blockade in a single layer graphene three-terminal single-electron transistor fabricated using feedback-controlled electroburning. The small separation between the side gate electrode and the graphene quantum dot results in a gate coupling up to 3 times larger compared to the value found for the back gate electrode. This allows for an effective tuning between the conductive and Coulomb blocked state using a small side gate voltage of about 1 V. The technique can potentially be used in the future to fabricate all-graphene based room temperature single-electron transistors or three terminal single molecule transistors with enhanced gate coupling.

Antiferromagnetism in a Family of S = 1 Square Lattice Coordination Polymers NiX2(pyz)2 (X = Cl, Br, I, NCS; pyz = Pyrazine)

The crystal structures of NiX2(pyz)2 (X = Cl (1), Br (2), I (3), and NCS (4)) were determined by synchrotron X-ray powder diffraction. All four compounds consist of two-dimensional (2D) square arrays self-assembled from octahedral NiN4X2 units that are bridged by pyz ligands. The 2D layered motifs displayed by 1-4 are relevant to bifluoride-bridged [Ni(HF2)(pyz)2]EF6 (E = P, Sb), which also possess the same 2D layers. In contrast, terminal X ligands occupy axial positions in 1-4 and cause a staggered packing of adjacent layers. Long-range antiferromagnetic (AFM) order occurs below 1.5 (Cl), 1.9 (Br and NCS), and 2.5 K (I) as determined by heat capacity and muon-spin relaxation. The single-ion anisotropy and g factor of 2, 3, and 4 were measured by electron-spin resonance with no evidence for zero-field splitting (ZFS) being observed. The magnetism of 1-4 spans the spectrum from quasi-two-dimensional (2D) to three-dimensional (3D) antiferromagnetism. Nearly identical results and thermodynamic features were obtained for 2 and 4 as shown by pulsed-field magnetization, magnetic susceptibility, as well as their Néel temperatures. Magnetization curves for 2 and 4 calculated by quantum Monte Carlo simulation also show excellent agreement with the pulsed-field data. Compound 3 is characterized as a 3D AFM with the interlayer interaction (J⊥) being slightly stronger than the intralayer interaction along Ni-pyz-Ni segments (J(pyz)) within the two-dimensional [Ni(pyz)2](2+) square planes. Regardless of X, J(pyz) is similar for the four compounds and is roughly 1 K.

Endohedral Metallofullerene as Molecular High Spin Qubit: Diverse Rabi Cycles in Gd2@C79N

An anisotropic high-spin qubit with long coherence time could scale the quantum system up. It has been proposed that Grovers algorithm can be implemented in such systems. Dimetallic aza[80]fullerenes M2@C79N (M = Y or Gd) possess an unpaired electron located between two metal ions, offering an opportunity to manipulate spin(s) protected in the cage for quantum information processing. Herein, we report the crystallographic determination of Gd2@C79N for the first time. This molecular magnet with a collective high-spin ground state (S = 15/2) generated by strong magnetic coupling (JGd-Rad = 350 ± 20 cm-1) has been unambiguously validated by magnetic susceptibility experiments. Gd2@C79N has quantum coherence and diverse Rabi cycles, allowing arbitrary superposition state manipulation between each adjacent level. The phase memory time reaches 5 μs at 5 K by dynamic decoupling. This molecule fulfills the requirements of Grovers searching algorithm proposed by Leuenberger and Loss.

Magnetic ground state of the two isostructual polymeric quantum magnets [Cu(HF2)(pyrazine)2]SbF6 and [Co(HF2)(pyrazine)2]SbF6 investigated with neutron powder diffraction

The magnetic ground state of two isostructural coordination polymers (i) the quasi two- dimensional S = 1/2 square-lattice antiferromagnet [Cu(HF2 )(pyrazine)2 ]SbF6 ; and (ii) a re- lated compound [Co(HF2)(pyrazine)2]SbF6, were examined with neutron powder diffraction measurements. We find the ordered moments of the Heisenberg S = 1/2 Cu(II) ions in [Cu(HF2)(pyrazine)2]SbF6 are 0.6(1)μb, whilst the ordered moments for the Co(II) ions in [Co(HF2)(pyrazine)2]SbF6 are 3.02(6)μb. For Cu(II), this reduced moment indicates the presence of quantum fluctuations below the ordering temperature. We show from heat capacity and electron spin resonance measurements, that due to the crystal electric field splitting of the S = 3/2 Co(II) ions in [Co(HF2)(pyrazine)2]SbF6, this isostructual polymer also behaves as an effective spin-half magnet at low temperatures. The Co moments in [Co(HF2)(pyrazine)2]SbF6 show strong easy-axis anisotropy, neutron diffraction data which do not support the presence of quantum fluctuations in the ground state and heat capacity data which are consistent with 2D or close to 3D spatial exchange anisotropy.

Implications of bond disorder in a S = 1 kagome lattice

Strong hydrogen bonds such as F···H···F offer new strategies to fabricate molecular architectures exhibiting novel structures and properties. Along these lines and, to potentially realize hydrogen-bond mediated superexchange interactions in a frustrated material, we synthesized [H2F]2[Ni3F6(Fpy)12][SbF6]2 (Fpy = 3-fluoropyridine). It was found that positionally-disordered H2F+ ions link neutral NiF2(Fpy)4 moieties into a kagome lattice with perfect 3-fold rotational symmetry. Detailed magnetic investigations combined with density-functional theory (DFT) revealed weak antiferromagnetic interactions (J ~ 0.4 K) and a large positive-D of 8.3 K with ms = 0 lying below ms = ±1. The observed weak magnetic coupling is attributed to bond-disorder of the H2F+ ions which leads to disrupted Ni-F···H-F-H···F-Ni exchange pathways. Despite this result, we argue that networks such as this may be a way forward in designing tunable materials with varying degrees of frustration.

Correction to “Endohedral Metallofullerene as Molecular High Spin Qubit: Diverse Rabi Cycles in Gd2@C79N”

Page 1125. Near the end of the section on “Energy Spectrum” and in the caption of Figure 2a, the parameters of spin Hamiltonian were reported incorrectly. The parameters should be B2 0 = 0.32(2) GHz, B2 2 = 0.14(1) GHz, B4 0 = −6(3) × 10−5 GHz, and giso = 1.99. The ZFS strain should be StrB20 = 0.02 GHz and StrB22 = 0.045 GHz. The main conclusions associated with these parameters are unaffected by these changes. Addition/Correction