Searcharxiv⌕ Search

arXiv subjects

Joaquín Fernández-Rossier

Publications and source records attributed to Joaquín Fernández-Rossier.

At least 19 recordsLinked to original sources

Landau quantization of $C_3$ high-fold fermions in honeycomb lattices

We present the theory of the Landau levels of $C_3$ high-fold fermions in honeycomb lattices. These fermions arise as a generalization of the tight-binding model in a honeycomb lattice with one orbital per site, known to describe graphene, to a family of models with several orbitals per site transforming according to representations of $C_3$, relevant for triangulene two-dimensional crystals. The models are defined by the number of orbitals $n_a$ and $n_b$ at the $a$ and $b$ sites of the unit cell. They feature energy bands that combine flat bands and Dirac cones, that are isomorphic to those of graphene, the Lieb, $p_{xy}$ honeycomb, and the Kagome tight-binding models. Combining tight-binding and $k\cdot p$ methods, here we compute the Landau levels of the $(1,1)$, $(1,2)$, $(2,2)$ and $(3,3)$ models, we compare them to those of the reference models, and we explore the similarities and differences with the Landau levels in graphene. Our findings reveal that the nature of $C_3$ high-fold fermions combine Dirac-type Landau quantization, originating from the linear crossings and associated relativistic band dispersion, with anomalous Landau quantization rooted in the quantum geometry of the singular flat bands.

cond-mat.mes-hall↗

Two topological phases in exchange alternating spin-1 nanographene chains

Magnetic nanographenes are emerging as versatile building blocks for artificial spin lattices, enabling the exploration of flagship one-dimensional quantum-magnetism models with unprecedented control. The spin-1 Heisenberg model, including bilinear and biquadratic exchange, was first realized using [3]-triangulenes, revealing the Haldane phase. More recently, Clar's goblets enabled the spin-1/2 Heisenberg model with exchange alternation, uncovering additional topological phases. Here we show that spin-1 nanographenes can be used to explore bond-alternating chains both in the Haldane phase and beyond it, in a dimerized phase with emergent edge spin-1. We use density matrix renormalization group (DMRG) to analyze how biquadratic exchange, which is known to be large in spin-1 nanographenes, determines the phase transition boundary. Combining multiconfigurational and first-principles calculations, we identify two realistic candidates to realize these two different phases: the recently synthesized extended Clar's goblet and a passivated [4]-triangulene. We demonstrate how to distinguish these phases experimentally using inelastic electron tunneling spectroscopy, paving the way for their observation.

cond-mat.mes-hall↗

Ultra-long-range spin coupling in graphene revealed by atomically resolved spin excitations

Magnetic interactions between localized spins-1/2 play a central role in quantum magnetism, spin-based quantum computing, and quantum simulation. The range and strength of these interactions are key figures of merit. Here, we probe exchange interactions in pairs and trimers of spins-1/2 introduced by chemisorption of individual hydrogen atoms on graphene. Using scanning tunneling microscopy and inelastic electron tunneling spectroscopy, supported by large-scale mean-field Hubbard calculations, we demonstrate 3 meV exchange couplings at separations beyond 10 nm, surpassing all prior systems. The couplings can be ferro- or antiferromagnetic depending on the relative sublattice arrangement. Real-space mapping of spin excitation amplitudes enables characterization with atomic-resolution. Through atomic manipulation we extend this control to spin trimers, revealing collective spin excitations when pairwise exchange couplings are comparable.

cond-mat.mes-hall↗

Electrically tunable quantum interference of atomic spins on surfaces

Controlling quantum interference near avoided energy-level crossings is crucial for fast and reliable coherent manipulation in quantum information processing. However, achieving tunable quantum interference in atomically-precise engineered structures remains challenging. Here, we demonstrate electrical control of quantum interference using atomic spins on an insulating film in a scanning tunneling microscope. Using bias voltages applied across the tunnel junction, we modulate the atomically-confined magnetic interaction between the probe tip and surface atoms with a strong electric field, and drive the spin state rapidly through the energy-level anticrossing. This all-electrical manipulation allows us to achieve Landau-Zener-Stückelberg-Majorana (LZSM) interferometry on both single spins and pairs of interacting spins. The LZSM pattern exhibits multiphoton resonances, and its asymmetry suggests that the spin dynamics is influenced by spin-transfer torque of tunneling electrons. Multi-level LZSM spectra measured on coupled spins with tunable interactions show distinct interference patterns depending on their many-body energy landscapes. These results open new avenues for all-electrical quantum manipulation in spin-based quantum processors in the strongly driven regime.

cond-mat.mes-hall↗

Non-resonant electric quantum control of individual on-surface spins

Quantum control techniques play an important role in manipulating and harnessing the properties of different quantum systems, including isolated atoms. Here, we propose to achieve quantum control over a single on-surface atomic spin using Landau-Zener-Stückelberg-Majorana (LZSM) interferometry implemented with Scanning Tunneling Microscopy (STM). Specifically, we model how the application of time-dependent, non-resonant AC electric fields across the STM tip-surface gap makes it possible to achieve precise quantum state manipulation in an isolated Fe atom on a MgO/Ag(100) surface. We propose a protocol to combine Landau Zener tunneling with LZSM interferometry that permits one to measure the quantum spin tunneling of an individual Fe atom. The proposed experiments can be implemented with ESR-STM instrumentation, opening a new venue in the research of on-surface single spin control.

quant-ph↗

Gapless spin excitations in nanographene-based antiferromagnetic spin-1/2 Heisenberg chains

Haldane's seminal work established two fundamentally different types of excitation spectra for antiferromagnetic Heisenberg quantum spin chains: gapped excitations in integer-spin chains and gapless excitations in half-integer-spin chains. In finite-length half-integer spin chains, quantization, however, induces a gap in the excitation spectrum, with the upper bound given by the Lieb-Schulz-Mattis (LSM) theorem. Here, we investigate the length-dependent excitations in spin-1/2 Heisenberg chains obtained by covalently linking olympicenes--Olympic rings shaped nanographenes carrying spin-1/2--into one-dimensional chains. The large exchange interaction (J~38 mV) between olympicenes and the negligible magnetic anisotropy in these nanographenes make them an ideal platform for studying quantum spin excitations, which we directly measure using inelastic electron tunneling spectroscopy. We observe a power-law decay of the lowest excitation energy with increasing chain length L, remaining below the LSM boundary. In a long chain with L = 50, a nearly V-shaped excitation continuum is observed, reinforcing the system's gapless nature in the thermodynamic limit. Finally, we visualize the standing wave of a single spinon confined in odd-numbered chains using low-bias current maps. Our results provide compelling evidence for the realization of a one-dimensional analog of a gapless spin liquid.

cond-mat.mtrl-sci↗

Building spin-1/2 antiferromagnetic Heisenberg chains with diaza-nanographenes

Understanding and engineering the coupling of spins in nanomaterials is of central importance for designing novel devices. Graphene nanostructures with π-magnetism offer a chemically tunable platform to explore quantum magnetic interactions. However, realizing spin chains bearing controlled odd-even effects with suitable nanographene systems is challenging. Here, we demonstrate the successful on-surface synthesis of spin-1/2 antiferromagnetic Heisenberg chains with parity-dependent magnetization based on antiaromatic diaza-hexa-peri-hexabenzocoronene (diaza-HBC) units. Using distinct synthetic strategies, two types of spin chains with different terminals were synthesized, both exhibiting a robust odd-even effect on the spin coupling along the chain. Combined investigations using scanning tunneling microscopy, non-contact atomic force microscopy, density functional theory calculations, and quantum spin models confirmed the structures of the diaza-HBC chains and revealed their magnetic properties, which has an S = 1/2 spin per unit through electron donation from the diaza-HBC core to the Au(111) substrate. Gapped excitations were observed in even-numbered chains, while enhanced Kondo resonance emerged in odd-numbered units of odd-numbered chains due to the redistribution of the unpaired spin along the chain. Our findings provide an effective strategy to construct nanographene spin chains and unveil the odd-even effect in their magnetic properties, offering potential applications in nanoscale spintronics.

cond-mat.mtrl-sci↗

Tunable topological phases in nanographene-based spin-1/2 alternating-exchange Heisenberg chains

Unlocking the potential of topological order within many-body spin systems has long been a central pursuit in the realm of quantum materials. Despite extensive efforts, the quest for a versatile platform enabling site-selective spin manipulation, essential for tuning and probing diverse topological phases, has persisted. Here, we utilize on-surface synthesis to construct spin-1/2 alternating-exchange Heisenberg (AH) chains[1] with antiferromagnetic couplings $J_1$ and $J_2$ by covalently linking Clar's goblets -- nanographenes each hosting two antiferromagnetically-coupled unpaired electrons[2]. Utilizing scanning tunneling microscopy, we exert atomic-scale control over the spin chain lengths, parities and exchange-coupling terminations, and probe their magnetic response by means of inelastic tunneling spectroscopy. Our investigation confirms the gapped nature of bulk excitations in the chains, known as triplons[3]. Besides, the triplon dispersion relation is successfully extracted from the spatial variation of tunneling spectral amplitudes. Furthermore, depending on the parity and termination of chains, we observe varying numbers of in-gap $S=1/2$ edge spins, enabling the determination of the degeneracy of distinct topological ground states in the thermodynamic limit-either 1, 2, or 4. By monitoring interactions between these edge spins, we identify the exponential decay of spin correlations. Our experimental findings, corroborated by theoretical calculations, present a phase-controlled many-body platform, opening promising avenues toward the development of spin-based quantum devices.

cond-mat.mtrl-sci↗

From Heisenberg to Hubbard: An initial state for the shallow quantum simulation of correlated electrons

The widespread use of the noninteracting ground state as the initial state for the digital quantum simulation of the Fermi-Hubbard model is largely due to the scarcity of alternative easy-to-prepare approximations to the exact ground state in the literature. Exploiting the fact that the spin-$\frac{1}{2}$ Heisenberg model is the effective low-energy theory of the Fermi-Hubbard model at half-filling in the strongly interacting limit, here we propose a three-step deterministic quantum routine to prepare an educated guess of the ground state of the Fermi-Hubbard model through a shallow circuit suitable for near-term quantum hardware. First, the ground state of the Heisenberg model is initialized via a hybrid variational method using an ansatz that explores only the correct symmetry subspace. Second, a general method is devised to convert a multi-spin-$\frac{1}{2}$ wave function into its fermionic version. Third, taking inspiration from the Baeriswyl ansatz, a constant-depth single-parameter layer that adds doublon-holon pairs is applied to this fermionic state. Numerical simulations on chains and ladders with up to 12 sites confirm the improvement over the noninteracting ground state of the overlap with the exact ground state for the intermediate values of the interaction strength at which quantum simulation is bound to be most relevant.

cond-mat.str-el↗

Optimizing tip-surface interactions in ESR-STM experiments

Electron-spin resonance carried out with scanning tunneling microscopes (ESR-STM) is a recently developed experimental technique that is attracting enormous interest on account of its potential to carry out single-spin on-surface resonance with subatomic resolution. Here we carry out a theoretical study of the role of tip-adatom interactions and provide guidelines for choosing the experimental parameters in order to optimize spin resonance measurements. We consider the case of the Fe adatom on a MgO surface and its interaction with the spin-polarized STM tip. We address three problems: first, how to optimize the tip-sample distance to cancel the effective magnetic field created by the tip on the surface spin, in order to carry out proper magnetic field sensing. Second, how to reduce the voltage dependence of the surface-spin resonant frequency, in order to minimize tip-induced decoherence due to voltage noise. Third, we propose an experimental protocol to infer the detuning angle between the applied field and the tip magnetization, which plays a crucial role in the modeling of the experimental results.

cond-mat.mes-hall↗

Theory of intermolecular exchange in coupled spin-1/2 nanographenes

Open-shell nanographenes can be covalently bonded and still preserve their local moments, forming interacting spins lattices. In the case of benzenoid nanographenes, the Ovchinnikov-Lieb rules anticipate the spin of the ground state of the superstructure, and thereby the sign of the intermolecular exchange. Here we address the underlying microscopic mechanisms for intermolecular exchange in this type of system. We find that, in general, three different mechanisms contribute. First, Hund's ferromagnetic exchange that promotes ferromagnetic interactions of electrons in overlapping orbitals. Second, superexchange driven by intermolecular hybridization, identical to Anderson kinetic exchange, which is a decreasing function of the Hubbard-$U$ energy scale, and is always antiferromagnetic. Third, a Coulomb-driven superexchange, that increases as a function of $U$, and involves virtual excitation of excited molecular orbitals that are extended over the entire structure. We find that Coulomb-driven superexchange can be either ferro or antiferromagnetic, accounting for Ovchinnikov-Lieb rules. We compute these exchange energies for the case of coupled $S=1/2$ phenalenyl triangulenes, using multi-configurational methods both with Hubbard and extended Hubbard models, thereby addressing the influence of long-range Coulomb interactions on the exchange interactions.

cond-mat.mes-hall↗

Renormalization of spin excitations and Kondo effect in open shell nanographenes

We study spin excitations and Kondo effect in open-shell nanographenes, motivated by recent scanning tunneling inelastic spectroscopy experiments. Specifically, we consider three systems, the triangulene, the extended triangulene with rocket shape, both with an $S=1$ ground state, and a triangulene dimer with $S=0$ on account of intermolecular exchange. We focus on the consequences of hybridization of the nanographene zero-modes with a conducting substrate on the $dI/dV$ lineshapes associated with spin excitations. The partially filled nanographene zero-modes coupled to the conduction electrons in the substrate constitute multi-orbital Anderson impurity models that we solve in the one-crossing approximation which treats the coupling to the substrate to infinite order. We find that the coupling to the substrate leads to (i) renormalization of the spin flip excitation energies of the bare molecule, (ii) broadening of the spectral features and (iii) the emergence of zero bias Kondo peaks for the $S=1$ ground states. The calculated substrate induced shift of the spin excitation energies is found to be significantly larger than their broadening, which implies that this effect has to be considered when comparing experimental results and theory.

cond-mat.mes-hall↗

Gutzwiller wave function on a digital quantum computer

The determination of the ground state of quantum many-body systems via digital quantum computers rests upon the initialization of a sufficiently educated guess. This requirement becomes more stringent the greater the system. Preparing physically-motivated ansätze on quantum hardware is therefore important to achieve quantum advantage in the simulation of correlated electrons. In this spirit, we introduce the Gutzwiller Wave Function (GWF) within the context of the digital quantum simulation of the Fermi-Hubbard model. We present a quantum routine to initialize the GWF that comprises two parts. In the first, the noninteracting state associated with the $U = 0$ limit of the model is prepared. In the second, the non-unitary Gutzwiller projection that selectively removes states with doubly-occupied sites from the wave function is performed by adding to every lattice site an ancilla qubit, the measurement of which in the $|0\rangle$ state confirms the projection was made. Due to its non-deterministic nature, we estimate the success rate of the algorithm in generating the GWF as a function of the lattice size and the interaction strength $U/t$. The scaling of the quantum circuit metrics and its integration in general quantum simulation algorithms are also discussed.

quant-ph↗

Probing local moments in nanographenes with electron tunneling spectroscopy

The emergence of local moments in graphene zigzag edges, grain boundaries, vacancies and sp3 defects has been widely studied theoretically. However, conclusive experimental evidence is scarce. Recent progress in on-surface synthesis has made it possible to create nanographenes, such as triangulenes, with local moments in their ground states, and to probe them using scanning tunnelling microscope (STM) spectroscopy. Here we review the application of the theory of sequential and cotunneling transport to relate the dI/dV spectra with the spin properties of nanographenes probed by STM. This approach permits us to connect the dI/dV with the many-body energies and wavefunctions of the graphene nanostructures. We apply this method describing the electronic states of the nanographenes by means of exact diagonalization of the Hubbard model within a restricted Active Space. This permits us to provide a proper quantum description of the emergence of local moments in graphene and its interplay with transport. We discuss the results of this theory in the case of diradical nanographenes, such as triangulene, rectangular ribbons and the Clar goblet, that have been recently studied experimentally by means of STM spectroscopy. This approach permits us to calculate both the dI/dV spectra, that yields excitation energies, as well as the atomically resolved conductivity maps, that provide information on the wavefunctions of the collective spin modes.

cond-mat.mes-hall↗

Single spin resonance driven by electric modulation of the g factor anisotropy

We address the problem of electronic and nuclear spin resonance of an individual atom on a surface driven by a scanning tunnelling microscope. Several mechanisms have been proposed so far, some of them based on the modulation of exchange and crystal field associated to a piezoelectric displacement of the adatom driven by the RF tip electric field. Here we consider a new mechanism, where the piezoelectric displacement modulates the g factor anisotropy, leading both to electronic and nuclear spin flip transitions. We discuss thoroughly the cases of Ti-H (S = 1/2) and Fe (S = 2) on MgO, relevant for recent experiments. We model the system using two approaches. First, an analytical model that includes crystal field, spin orbit coupling and hyperfine interactions. Second, we carry out density functional based calculations. We find that the modulation of the anisotropy of the g tensor due to the piezoelectric displacement of the atom is an additional mechanism for STM based single spin resonance, that would be effective in S = 1/2 adatoms with large spin orbit coupling. In the case of Ti-H on MgO, we predict a modulation spin resonance frequency driven by the DC electric field of the tip.

cond-mat.mes-hall↗

Exchange rules for diradical π-conjugated hydrocarbons

A variety of planar π-conjugated hydrocarbons such as heptauthrene, Clar's goblet and, recently synthesized, triangulene have two electrons occupying two degenerate molecular orbitals. The resulting spin of the interacting ground state is often correctly anticipated as S = 1, extending the application of Hund's rules to these systems, but this is not correct in some instances. Here we provide a set of rules to correctly predict the existence of zero mode states, as well as the spin multiplicity of both the ground state and the low-lying excited states, together with their open- or closed-shell nature. This is accomplished using a combination of analytical arguments and configuration interaction calculations with a Hubbard model, both backed by quantum chemistry methods with a larger Gaussian basis set. Our results go beyond the well established Lieb's theorem and Ovchinnikov's rule, as we address the multiplicity and the open-/closed-shell nature of both ground and excited states.

cond-mat.mes-hall↗

Tuning the exchange bias on a single atom from 1 mT to 10 T

Shrinking spintronic devices to the nanoscale ultimately requires localized control of individual atomic magnetic moments. At these length scales, the exchange interaction plays important roles, such as in the stabilization of spin-quantization axes, the production of spin frustration, and creation of magnetic ordering. Here, we demonstrate the precise control of the exchange bias experienced by a single atom on a surface, covering an energy range of four orders of magnitude. The exchange interaction is continuously tunable from milli-eV to micro-eV by adjusting the separation between a spin-1/2 atom on a surface and the magnetic tip of a scanning tunneling microscope (STM). We seamlessly combine inelastic electron tunneling spectroscopy (IETS) and electron spin resonance (ESR) to map out the different energy scales. This control of exchange bias over a wide span of energies provides versatile control of spin states, with applications ranging from precise tuning of quantum state properties, to strong exchange bias for local spin doping. In addition we show that a time-varying exchange interaction generates a localized AC magnetic field that resonantly drives the surface spin. The static and dynamic control of the exchange interaction at the atomic-scale provides a new tool to tune the quantum states of coupled-spin systems.

cond-mat.mes-hall↗

Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling

Magnetic insulators are a key resource for next-generation spintronic and topological devices. The family of layered metal halides promises ultrathin insulating multiferroics, spin liquids, and ferromagnets, but new characterization methods are required to unlock their potential. Here, we report tunneling through the layered magnetic insulator CrI3 as a function of temperature and applied magnetic field. We electrically detect the magnetic ground state and inter-layer coupling and observe a field-induced metamagnetic transition. The metamagnetic transition results in magnetoresistances of 95%, 300%, and 550% for bilayer, trilayer, and tetralayer CrI3 barriers, respectively. We further measure inelastic tunneling spectra for our junctions, unveiling a rich spectrum of collective magnetic excitations (magnons) in CrI3. Our results establish vertical tunneling as a versatile probe of magnetism in atomically thin insulators.

cond-mat.mes-hall↗