Current Induced Spin-Polarization in Chiral Molecules.

The inverse spin-galvanic effect or current-induced spin-polarization is mainly associated with interfaces between different layers in semiconducting heterostructures, surfaces of metals, and bulk semiconducting materials. Here, we theoretically predict that the inverse spin-galvanic effect should also be present in chiral molecules, as a result of the chiral induced spin selectivity effect. As proof-of-principle, we calculate the nonequilibrium properties of a model system that previously has been successfully used to explain a multitude of aspects related to the chiral induced spin selectivity effect. Here we show that current driven spin-polarization in a chiral molecule gives rise to a magnetic moment that is sensitive to external magnet field. The chiral molecule then behaves like a soft ferromagnet. This, in turn, suggests that magnetic permeability measurement in otherwise nonmagnetic systems may be used noninvasively to detect the presence of spin-polarized currents.

Temperature activated chiral induced spin selectivity.

Recent experiments performed on chiral molecules, comprising transition metal or rare earth elements, indicate temperature reinforced chiral induced spin selectivity. In these compounds, spin selectivity is suppressed in the low temperature regime but grows by one to several orders of magnitude as the temperature is increased to room temperature. By relating temperature to nuclear motion, it is proposed that nuclear displacements acting on the local spin moments, through indirect exchange interactions, generate an anisotropic magnetic environment that is enhanced with temperature. The induced local anisotropy field serves as the origin of a strongly increased spin selectivity at elevated temperature.

Emergent Magnetism as a Cooperative Effect of Interactions and Reservoir.

Closed shell molecular structures are under normal conditions time-reversal invariant. Experimental evidence points, however, toward that this invariance may be locally violated when the structure is in contact with a particle reservoir. The mechanisms behind such local symmetry breaking are not clear by any means. By considering a minimal model for a closed shell structure, here we propose that the symmetry breaking may result from a combination of internal and/or external interactions. It is shown that a magnetic moment of a localized electron level can be generated and maintained under the influence of such a combination. The theoretical results should cast new light on the mechanisms that may form magnetic properties in molecular compounds.

Vibrationally Induced Magnetism in Supramolecular Aggregates.

Magnetic phenomena in chemistry and condensed matter physics are considered to be associated with low temperatures. That a magnetic state or order is stable below a critical temperature as well as becoming stronger the lower the temperature is a nearly unquestioned paradigm. It is, therefore, surprising that recent experimental observations made on supramolecular aggregates suggest that, for instance, the magnetic coercivity may increase with an increasing temperature and the chiral-induced spin selectivity effect may be enhanced. Here, a mechanism for vibrationally stabilized magnetism is proposed, and a theoretical model is introduced with which the qualitative aspects of the recent experimental findings can be explained. It is argued that anharmonic vibrations, which become increasingly occupied with an increasing temperature, enable nuclear vibrations to both stabilize and sustain magnetic states. The theoretical proposal, hence, pertains to structures without inversion and/or reflection symmetries, for instance, chiral molecules and crystals.

Holes in the tundra: Invasive earthworms alter soil structure and moisture in tundra soils.

Human introductions have resulted in earthworms establishing in the Arctic, species known to cause cascading ecosystem change. However, few quantitative outdoor experiments have been performed that describe how these soil modifying earthworms are reshaping structures in tundra soils. In this study, we used three-dimensional (3-D) X-ray images of soil cores (approximately 10 cm diameter, 20 cm height, N = 48) to assess how earthworms (Aporrectodea sp. and Lumbricus sp.) affect soil structure and macropore networks in an outdoor mesocosm experiment that lasted four summers. Effects were assessed in both shrub-dominated (heath) and herb-dominated (meadow) tundra. Earthworms almost doubled the macroporosity in meadow soils and tripled macroporosity in heath. Interestingly, the fractal dimension of macropores decreased in response to earthworm burrowing in both systems, indicating that the presence of earthworms reduced the geometric complexity in comparison to other pore-generating processes active in the tundra. Observed effects on soil structure occurred along with a dramatically reduced soil moisture content, which was observed the first winter after earthworm introduction in the meadow. Our findings suggest that predictions of future changes in vegetation and soil carbon pools in the Arctic should include major impacts on soil properties that earthworms induce.

Charge and Spin Dynamics and Enantioselectivity in Chiral Molecules.

Charge and spin dynamics are addressed in chiral molecules immediately after their instantaneous coupling to an external metallic reservoir. This work describes how a spin polarization is induced in the chiral structure as a response to the charge dynamics. The dynamics indicate that chiral induced spin selectivity is an excited state phenomenon that in the transient regime can be partly captured using a simplistic single-particle description but in the stationary limit definitively shows that electron correlations, e.g., electron-vibration interactions, crucially contribute to sustain an intrinsic spin anisotropy that can lead to a nonvanishing spin selectivity. The dynamics, moreover, provide insight into enantiomer separation, due to different acquired spin polarizations.

Monolayer CrCl_{3} as an Ideal Test Bed for the Universality Classes of 2D Magnetism.

The monolayer halides CrX_{3} (X=Cl, Br, I) attract significant attention for realizing 2D magnets with genuine long-range order (LRO), challenging the Mermin-Wagner theorem. Here, we show that monolayer CrCl_{3} has the unique benefit of exhibiting tunable magnetic anisotropy upon applying a compressive strain. This opens the possibility to use CrCl_{3} for producing and studying both ferromagnetic and antiferromagnetic 2D Ising-type LRO as well as the Berezinskii-Kosterlitz-Thouless (BKT) regime of 2D magnetism with quasi-LRO. Using state-of-the-art density functional theory, we explain how realistic compressive strain could be used to tune the monolayer's magnetic properties so that it could exhibit any of these phases. Building on large-scale quantum Monte Carlo simulations, we compute the phase diagram of strained CrCl_{3}, as well as the magnon spectrum with spin-wave theory. Our results highlight the eminent suitability of monolayer CrCl_{3} to achieve very high BKT transition temperatures, around 50 K, due to their singular dependence on the weak easy-plane anisotropy of the material.

Remote Mesoscopic Signatures of Induced Magnetic Texture in Graphene.

Mesoscopic conductance fluctuations are a ubiquitous signature of phase-coherent transport in small conductors, exhibiting universal character independent of system details. In this Letter, however, we demonstrate a pronounced breakdown of this universality, due to the interplay of local and remote phenomena in transport. Our experiments are performed in a graphene-based interaction-detection geometry, in which an artificial magnetic texture is induced in the graphene layer by covering a portion of it with a micromagnet. When probing conduction at some distance from this region, the strong influence of remote factors is manifested through the appearance of giant conductance fluctuations, with amplitude much larger than e^{2}/h. This violation of one of the fundamental tenets of mesoscopic physics dramatically demonstrates how local considerations can be overwhelmed by remote signatures in phase-coherent conductors.

First-principles Dzyaloshinskii-Moriya interaction in a non-collinear framework.

We have derived an expression of the Dzyaloshinskii-Moriya interaction (DMI), where all the three components of the DMI vector can be calculated independently, for a general, non-collinear magnetic configuration. The formalism is implemented in a real space-linear muffin-tin orbital-atomic sphere approximation (RS-LMTO-ASA) method. We have chosen the Cr triangular trimer on Au(111) and Mn triangular trimers on Ag(111) and Au(111) surfaces as numerical examples. The results show that the DMI (module and direction) is drastically different between collinear and non-collinear states. Based on the relation between the spin and charge currents flowing in the system and their coupling to the non-collinear magnetic configuration of the triangular trimer, we demonstrate that the DMI interaction can be significant, even in the absence of spin-orbit coupling. This is shown to emanate from the non-collinear magnetic structure, that can induce significant spin and charge currents even with spin-orbit coupling is ignored.

Universal scaling of weak localization in graphene due to bias-induced dispersion decoherence.

The differential conductance of graphene is shown to exhibit a zero-bias anomaly at low temperatures, arising from a suppression of the quantum corrections due to weak localization and electron interactions. A simple rescaling of these data, free of any adjustable parameters, shows that this anomaly exhibits a universal, temperature- (T) independent form. According to this, the differential conductance is approximately constant at small voltages (V < kBT/e), while at larger voltages it increases logarithmically with the applied bias. For theoretical insight into the origins of this behaviour, which is inconsistent with electron heating, we formulate a model for weak-localization in the presence of nonequilibrium transport. According to this model, the applied voltage causes unavoidable dispersion decoherence, which arises as diffusing electron partial waves, with a spread of energies defined by the value of the applied voltage, gradually decohere with one another as they diffuse through the system. The decoherence yields a universal scaling of the conductance as a function of eV/kBT, with a logarithmic variation for eV/kBT > 1, variations in accordance with the results of experiment. Our theoretical description of nonequilibrium transport in the presence of this source of decoherence exhibits strong similarities with the results of experiment, including the aforementioned rescaling of the conductance and its logarithmic variation as a function of the applied voltage.

Chirality-Induced Spin Selectivity: The Role of Electron Correlations.

Chirality-induced spin selectivity, discovered about two decades ago in helical molecules, is a nonequilibrium effect that emerges from the interplay between geometrical helicity and spin-orbit interactions. Several model Hamiltonians building on this interplay have been proposed, and while these can yield spin-polarized transport properties that agree with experimental observations, they simultaneously depend on unrealistic values of the spin-orbit interaction parameters. It is likely, however, that a common deficit originates from the fact that all these models are uncorrelated or single-electron theories. Therefore, chirality-induced spin selectivity is here addressed using a many-body approach, which allows for nonequilibrium conditions and a systematic treatment of the correlated state. The intrinsic molecular spin polarization increases by 2 orders of magnitude, or more, compared to the corresponding result in the uncorrelated model. In addition, the electronic structure responds to varying external magnetic conditions which, therefore, enables comparisons of the currents provided for different spin polarizations in one or both of the leads between which the molecule is mounted. Using experimentally feasible parameters and room temperature, the obtained normalized difference between such currents may be as large as 5-10% for short molecular chains, clearly suggesting the vital importance of including electron correlations when searching for explanations of the phenomenon.

Spin-Resolved Spectroscopy of the Yu-Shiba-Rusinov States of Individual Atoms.

A magnetic atom in a superconducting host induces so-called Yu-Shiba-Rusinov (YSR) bound states inside the superconducting energy gap. By combining spin-resolved scanning tunneling spectroscopy with simulations we demonstrate that the pair of peaks associated with the YSR states of an individual Fe atom coupled to an oxygen-reconstructed Ta surface gets spin polarized in an external magnetic field. As theoretically predicted, the electron and hole parts of the YSR states have opposite signs of spin polarizations which keep their spin character when crossing the Fermi level through the quantum phase transition. The simulation of a YSR state right at the Fermi level reveals zero spin polarization which can be used to distinguish such states from Majorana zero modes in chains of YSR atoms.

Evaluating the Sources of Graphene's Resistivity Using Differential Conductance.

We explore the contributions to the electrical resistance of monolayer and bilayer graphene, revealing transitions between different regimes of charge carrier scattering. In monolayer graphene at low densities, a nonmonotonic variation of the resistance is observed as a function of temperature. Such behaviour is consistent with the influence of scattering from screened Coulomb impurities. At higher densities, the resistance instead varies in a manner consistent with the influence of scattering from acoustic and optical phonons. The crossover from phonon-, to charged-impurity, limited conduction occurs once the concentration of gate-induced carriers is reduced below that of the residual carriers. In bilayer graphene, the resistance exhibits a monotonic decrease with increasing temperature for all densities, with the importance of short-range impurity scattering resulting in a "universal" density-independent (scaled) conductivity at high densities. At lower densities, the conductivity deviates from this universal curve, pointing to the importance of thermal activation of carriers out of charge puddles. These various assignments, in both systems, are made possible by an approach of "differential-conductance mapping", which allows us to suppress quantum corrections to reveal the underlying mechanisms governing the resistivity.

Electron Paramagnetic Resonance of Single Magnetic Moment on a Surface.

We address electron spin resonance of single magnetic moments in a tunnel junction using time-dependent electric fields and spin-polarized current. We show that the tunneling current directly depends on the local magnetic moment and that the frequency of the external electric field mixes with the characteristic Larmor frequency of the local spin. The importance of the spin-polarized current induced anisotropy fields acting on the local spin moment is, moreover, demonstrated. Our proposed model thus explains the absence of an electron spin resonance for a half integer spin, in contrast with the strong signal observed for an integer spin.

Voltage-Induced Switching Dynamics of a Coupled Spin Pair in a Molecular Junction.

Molecular spintronics is made possible by the coupling between electronic configuration and magnetic polarization of the molecules. For control and application of the individual molecular states, it is necessary to both read and write their spin states. Conventionally, this is achieved by means of external magnetic fields or ferromagnetic contacts, which may change the intentional spin state and may present additional challenges when downsizing devices. Here, we predict that coupling magnetic molecules together opens up possibilities for all electrical control of both the molecular spin states as well as the current flow through the system. By tuning between the regimes of ferromagnetic and antiferromagnetic exchange interaction, the current can be at least an order of magnitude enhanced or reduced. The effect is susceptible to the tunnel coupling and molecular level alignment that can be used to achieve current rectification.

Tuning the Fano resonance with an intruder continuum.

Through a combination of experiment and theory we establish the possibility of achieving strong tuning of Fano resonances (FRs), by allowing their usual two-path geometry to interfere with an additional, "intruder", continuum. As the coupling strength to this intruder is varied, we predict strong modulations of the resonance line shape that, in principle at least, may exceed the amplitude of the original FR itself. For a proof-of-concept demonstration of this phenomenon, we construct a nanoscale interferometer from nonlocally coupled quantum point contacts and utilize the unique features of their density of states to realize the intruder. External control of the intruder coupling is enabled by means of an applied magnetic field, in the presence of which we demonstrate the predicted distortions of the FR. This general scheme for resonant control should be broadly applicable to a variety of wave-based systems, opening up the possibility of new applications in areas such as chemical and biological sensing and secure communications.

Identification of vibrational signatures from short chains of interlinked molecule-nanoparticle junctions obtained by inelastic electron tunnelling spectroscopy.

Short chains containing a series of metal-molecule-nanoparticle nanojunctions are a nano-material system with the potential to give electrical signatures close to those from single molecule experiments while enabling us to build portable devices on a chip. Inelastic electron tunnelling spectroscopy (IETS) measurements provide one of the most characteristic electrical signals of single and few molecules. In interlinked molecule-nanoparticle (NP) chains containing typically 5-7 molecules in a chain, the spectrum is expected to be a superposition of the vibrational signatures of individual molecules. We have established a stable and reproducible molecule-AuNP multi-junction by placing a few 1,8-octanedithiol (ODT) molecules onto a versatile and portable nanoparticle-nanoelectrode platform and measured for the first time vibrational molecular signatures at complex and coupled few-molecule-NP junctions. From quantum transport calculations, we model the IETS spectra and identify vibrational modes as well as the number of molecules contributing to the electron transport in the measured spectra.

Detection and cloaking of molecular objects in coherent nanostructures using inelastic electron tunneling spectroscopy.

We address quantum invisibility in the context of electronics in nanoscale quantum structures. We make use of the freedom of design that quantum corrals provide and show that quantum mechanical objects can be hidden inside the corral, with respect to inelastic electron scattering spectroscopy in combination with scanning tunneling microscopy, and we propose a design strategy. A simple illustration of the invisibility is given in terms of an elliptic quantum corral containing a molecule, with a local vibrational mode, at one of the foci. Our work has implications to quantum information technology and presents new tools for nonlocal quantum detection and distinguishing between different molecules.

Spin inelastic electron tunneling spectroscopy on local spin adsorbed on surface.

The recent experimental conductance measurements taken on magnetic impurities on metallic surfaces, using scanning tunneling microscopy technique and suggesting occurrence of inelastic scattering processes, are theoretically addressed. We argue that the observed conductance signatures are caused by transitions between the spin states that have opened due to, for example, exchange coupling between the local spins and the tunneling electrons, and are directly interpretable in terms of inelastic transitions energies. Feasible measurements using spin-polarized scanning tunneling microscopy that would enable new information about the excitation spectrum of the local spins are discussed.

Evolving properties of two-dimensional materials: from graphene to graphite.

We have studied theoretically, using density functional theory, several material properties when going from one C layer in graphene to two and three graphene layers and on to graphite. The properties we have focused on are the elastic constants, electronic structure (energy bands and density of states), and the dielectric properties. For any of the properties we have investigated the modification due to an increase in the number of graphene layers is within a few per cent. Our results are in agreement with the analysis presented recently by Kopelevich and Esquinazi (unpublished).