Matias Urdampilleta

Supramolecular spin valves

Magnetic molecules are potential building blocks for the design of spintronic devices. Moreover, molecular materials enable the combination of bottom-up processing techniques, for example with conventional top-down nanofabrication. The development of solid-state spintronic devices based on the giant magnetoresistance, tunnel magnetoresistance and spin-valve effects has revolutionized magnetic memory applications. Recently, a significant improvement of the spin-relaxation time has been observed in organic semiconductor tunnel junctions, single non-magnetic molecules coupled to magnetic electrodes have shown giant magnetoresistance and hybrid devices exploiting the quantum tunnelling properties of single-molecule magnets have been proposed. Herein, we present an original spin-valve device in which a non-magnetic molecular quantum dot, made of a single-walled carbon nanotube contacted with non-magnetic electrodes, is laterally coupled through supramolecular interactions to TbPc(2) single-molecule magnets (Pc=phthalocyanine). Their localized magnetic moments lead to a magnetic field dependence of the electrical transport through the single-walled carbon nanotube, resulting in magnetoresistance ratios up to 300% at temperatures less than 1 K. We thus demonstrate the functionality of a supramolecular spin valve without magnetic leads. Our results open up prospects of new spintronic devices with quantum properties.

Surface-Enhanced Raman Signal for Terbium Single-Molecule Magnets Grafted on Graphene

We report the preparation and characterization of monolayer graphene decorated with functionalized single-molecule magnets (SMMs). The grafting ligands provide a homogeneous and selective deposition on graphene. The grafting is characterized by combined Raman microspectroscopy, atomic force microscopy (AFM), and electron transport measurements. We observe a surface-enhanced Raman signal that allowed us to study the grafting down to the limit of a few isolated molecules. The weak interaction through charge transfer is in agreement with ab initio DFT calculations. Our results indicate that both molecules and graphene are essentially intact and the interaction is driven by van der Waals forces.

Molecular quantum spintronics: supramolecular spin valves based on single-molecule magnets and carbon nanotubes

We built new hybrid devices consisting of chemical vapor deposition (CVD) grown carbon nanotube (CNT) transistors, decorated with TbPc2 (Pc = phthalocyanine) rare-earth based single-molecule magnets (SMMs). The drafting was achieved by tailoring supramolecular π-π interactions between CNTs and SMMs. The magnetoresistance hysteresis loop measurements revealed steep steps, which we can relate to the magnetization reversal of individual SMMs. Indeed, we established that the electronic transport properties of these devices depend strongly on the relative magnetization orientations of the grafted SMMs. The SMMs are playing the role of localized spin polarizer and analyzer on the CNT electronic conducting channel. As a result, we measured magneto-resistance ratios up to several hundred percent. We used this spin valve effect to confirm the strong uniaxial anisotropy and the superparamagnetic blocking temperature (TB ~ 1 K) of isolated TbPc2 SMMs. For the first time, the strength of exchange interaction between the different SMMs of the molecular spin valve geometry could be determined. Our results introduce a new design for operable molecular spintronic devices using the quantum effects of individual SMMs.

Magnetic interaction between a radical spin and a single-molecule magnet in a molecular spin-valve.

Molecular spintronics using single molecule magnets (SMMs) is a fast growing field of nanoscience that proposes to manipulate the magnetic and quantum information stored in these molecules. Herein we report evidence of a strong magnetic coupling between a metallic ion and a radical spin in one of the most extensively studied SMMs: the bis(phtalocyaninato)terbium(III) complex (TbPc2). For that we use an original multiterminal device comprising a carbon nanotube laterally coupled to the SMMs. The current through the device, sensitive to magnetic interactions, is used to probe the magnetization of a single Tb ion. Combining this electronic read-out with the transverse field technique has allowed us to measure the interaction between the terbium ion, its nuclear spin, and a single electron located on the phtalocyanine ligands. We show that the coupling between the Tb and this radical is strong enough to give extra resonances in the hysteresis loop that are not observed in the anionic form of the complex. The experimental results are then modeled by diagonalization of a three-spins Hamiltonian. This strong coupling offers perspectives for implementing nuclear and electron spin resonance techniques to perform basic quantum operations in TbPc2.

Single-Chain Magnets and Related Systems

In this chapter, the static and dynamic magnetic properties of single-chain magnets and related systems are reviewed. We will particularly focus on the so-called Ising limit for which the magnetic anisotropy energy is much larger than the energy of the intrachain exchange interactions. The simple regular chain of ferromagnetically coupled spins will be first described. Static properties will be summarized to introduce the dominant role of domain walls at low temperature. The slow relaxation of the magnetization will be then discussed using a stochastic description. The deduced dynamic critical behavior will be analyzed in detail to explain the observed magnet behavior. In particular, the effect of applying a magnetic field, often ignored in the literature, will be discussed. Then, more complicated structures including chains of antiferromagnetically coupled magnetic sites will be discussed. Finally, the importance of interchain couplings will be introduced to discriminate between a “real” single-chain magnet and a sample presenting both a magnet-type property and a three-dimensional antiferromagnetic ordered state at low temperature.

Landau-Zener tunneling of a single Tb 3+ magnetic moment allowing the electronic read-out of a nuclear spin

A multi-terminal device based on a carbon nanotube quantum dot was used at very low tem- perature to probe a single electronic and nuclear spin embedded in a bis-phthalocyanine Terbium (III) complex (TbPc2). A spin-valve signature with large conductance jumps was found when two molecules were strongly coupled to the nanotube. The application of a transverse field separated the magnetic signal of both molecules and enabled single-shot read-out of the Terbium nuclear spin. The Landau-Zener (LZ) quantum tunneling probability was studied as a function of field sweep rate, establishing a good agreement with the LZ equation and yielding the tunnel splitting \Delta. It was found that ? increased linearly as a function of the transverse field. These studies are an essential prerequisite for the coherent manipulation of a single nuclear spin in TbPc2.

Charge Dynamics and Spin Blockade in a Hybrid Double Quantum Dot in Silicon

Electron spin qubits in silicon, whether in quantum dots or in donor atoms, have long been considered attractive qubits for the implementation of a quantum computer because of silicon’s “semiconductor vacuum” character and its compatibility with the microelectronics industry. While donor electron spins in silicon provide extremely long coherence times and access to the nuclear spin via the hyperfine interaction, quantum dots have the complementary advantages of fast electrical operations, tunability, and scalability. Here, we present an approach to a novel hybrid double quantum dot by coupling a donor to a lithographically patterned artificial atom. Using gate-based rf reflectometry, we probe the charge stability of this double quantum-dot system and the variation of quantum capacitance at the interdot charge transition. Using microwave spectroscopy, we find a tunnel coupling of 2.7 GHz and characterize the charge dynamics, which reveals a charge T2 of 200 ps and a relaxation time T1 of 100 ns. Additionally, we demonstrate a spin blockade at the inderdot transition, opening up the possibility to operate this coupled system as a singlet-triplet qubit or to transfer a coherent spin state between the quantum dot and the donor electron and nucleus.

Hyperfine Stark effect of shallow donors in silicon

This research was funded by the joint EPSRC (EP/I035536) / NSF (DMR-1107606) Materials World Network grant (BWL, GP, JJLM, SAL), EPSRC grant EP/K025562/1 (BWL and JJLM), the European Research Council under the European Communitys Seventh Framework Programme (FP7/2007-2013) / ERC Grant Agreement No. 279781 (JJLM), partly by the NSF MRSEC grant DMR-0819860 (SAL), the Department of Energy, Office of Basic Energy Sciences grant DE-SC0002140 (RNB). BWL and JJLM thank the Royal Society for a University Research Fellowship.

Conditional control of donor nuclear spins in silicon using Stark shifts

Electric fields can be used to tune donor spins in silicon using the Stark shift, whereby the donor electron wave function is displaced by an electric field, modifying the hyperfine coupling between the electron spin and the donor nuclear spin. We present a technique based on dynamic decoupling of the electron spin to accurately determine the Stark shift, and illustrate this using antimony donors in isotopically purified silicon-28. We then demonstrate two different methods to use a dc electric field combined with an applied resonant radio-frequency (rf) field to conditionally control donor nuclear spins. The first method combines an electric-field induced conditional phase gate with standard rf pulses, and the second one simply detunes the spins off resonance. Finally, we consider different strategies to reduce the effect of electric field inhomogeneities and obtain above 90% process fidelities.

Magnetic tetrastability in a spin chain

Bistability in magnetism is extensively used, in particular for information storage. Here an alternative approach using tetrastable magnetic domains in one-dimensional (1D) spin systems is presented. Using numerical and analytical calculations, we show that a spin chain with a canting angle of π/4 possesses four energy-equivalent states. We discuss the static properties of this canted 1D system such as the profile and the energy of the domain walls as they govern the dynamics of themagnetization. The realization of this π/4 canted spin chain could enable the encoding of the information on four bits, which is a potential alternative toward the increase of storage density.