arXiv subjects

Angel Rubio

Publications and source records attributed to Angel Rubio.

At least 199 records · Page 11Linked to original sources

arXiv2022

A New Era of Quantum Materials Mastery and Quantum Simulators In and Out of Equilibrium

We provide a perspective on the burgeoning field of controlling quantum materials at will and its potential for quantum simulations in and out equilibrium. After briefly outlining a selection of key recent advances in controlling materials using novel high fluence lasers as well as in innovative approaches for novel quantum materials synthesis (especially in the field of twisted two-dimensional solids), we provide a vision for the future of the field. By merging state of the art developments we believe it is possible to enter a new era of quantum materials mastery, in which exotic and for the most part evasive collective as well as topological phenomena can be controlled in a versatile manner. This could unlock functionalities of unprecedented capabilities, which in turn can enable many novel quantum technologies in the future.

cond-mat.str-el↗

arXiv2022

A perspective on ab initio modeling of polaritonic chemistry: The role of non-equilibrium effects and quantum collectivity

This perspective provides a brief introduction into the theoretical complexity of polaritonic chemistry, which emerges from the hybrid nature of strongly coupled light-matter states. To tackle this complexity, the importance of ab initio methods is highlighted. Based on those, novel ideas and research avenues are developed with respect to quantum collectivity, as well as for resonance phenomena immanent in reaction rates under vibrational strong coupling. Indeed, fundamental theoretical questions arise about the mesoscopic scale of quantum-collectively coupled molecules, when considering the depolarization shift in the interpretation of experimental data. Furthermore, to rationalise recent findings based on quantum electrodynamical density-functional theory (QEDFT), a simple, but computationally efficient, Langevin framework is proposed, based on well-established methods from molecular dynamics. It suggests the emergence of cavity induced non-equilibrium nuclear dynamics, where thermal (stochastic) resonance phenomena could emerge in the absence of external periodic driving. Overall, we believe the latest ab initio results indeed suggest a paradigmatic shift for ground-state chemical reactions under vibrational strong coupling, from the collective quantum interpretation towards a more local, (semi)-classically and non-equilibrium dominated perspective. Finally, various extensions towards a refined description of cavity-modified chemistry are introduced in the context of QEDFT and future directions of the field are sketched.

physics.chem-ph↗

arXiv2022

Wavefunction Embedding for Molecular Polaritons

Polaritonic chemistry relies on the strong light-matter interaction phenomena for altering the chemical reaction rates inside optical cavities. To explain and to understand these processes, the development of reliable theoretical models is essential. While computationally efficient quantum electrodynamics self-consistent field (QED-SCF) methods, such as quantum electrodynamics density functional theory (QEDFT) needs accurate functionals, quantum electrodynamics coupled cluster (QED-CC) methods provide a systematic increase in accuracy but at much greater cost. To overcome this computational bottleneck, herein we introduce and develop the QED-CC-in-QED-SCF projection-based embedding method that inherits all the favorable properties from the two worlds, computational efficiency and accuracy. The performance of the embedding method is assessed by studying some prototypical but relevant reactions, such as methyl transfer reaction, proton transfer reaction, as well as protonation reaction in a complex environment. The results obtained with the new embedding method are in excellent agreement with more expensive QED-CC results. The analysis performed on these reactions indicate that the strong light-matter interaction is very local in nature and that only a small region should be treated at the QED-CC level for capturing important effects due to cavity. This work sets the stage for future developments of polaritonic quantum chemistry methods and it will serve as a guideline for development of other polaritonic embedding models.

physics.chem-ph↗

arXiv2022

New Class of Landau Levels and Hall Phases in a 2D Electron Gas Subject to an Inhomogeneous Magnetic Field: An Analytic Solution

An analytic closed form solution is derived for the bound states of electrons subject to a static, inhomogeneous ($1/r$-decaying) magnetic field, including the Zeeman interaction. The solution provides access to many-body properties of a two-dimensional, non-interacting, electron gas in the thermodynamic limit. Radially distorted Landau levels can be identified as well as magnetic field induced density and current oscillations close to the magnetic impurity. These radially localised oscillations depend strongly on the coupling of the spin to the magnetic field, which give rise to non-trivial spin currents. Moreover, the Zeeman interaction introduces a lowest flat band for $E_F=0^+$ assuming a spin $g_s$-factor of two. Surprisingly, in this case the charge and current densities can be computed analytically in the thermodynamic limit. Numerical calculations show that the total magnetic response of the electron gas remains diamagnetic (similar to Landau levels) independent of the Fermi energy. However, the contribution of certain, infinitely degenerate energy levels may become paramagnetic. Furthermore, numerical computations of the Hall conductivity reveal asymptotic properties of the electron gas, which are driven by the anisotropy of the vector potential instead of the magnetic field, i.e. become independent of spin. Eventually, the distorted Landau levels give rise to different Hall conductivity phases, which are characterized by sharp sign flips at specific Fermi energies. Overall, our work merges "impurity" with Landau-level physics, which provides novel physical insights, not only locally, but also in the asymptotic limit. This paves the way for a large number of future theoretical as well as experimental investigations.

cond-mat.mes-hall↗

arXiv2022

Ab-initio cluster approach for high-harmonic generation in liquids

High harmonic generation (HHG) takes place in all phases of matter. In gaseous atomic and molecular media, it has been extensively studied and is very well-understood. In solids research is ongoing, but a consensus is forming for the dominant microscopic HHG mechanisms. In liquids on the other hand, no established theory yet exit and approaches developed for gases and solids are generally inapplicable, hindering our current understanding. We develop here a powerful and reliable ab-initio cluster-based approach for describing the nonlinear interactions between isotropic bulk liquids and intense laser pulses. The scheme is based on time-dependent density functional theory and utilizes several approximations that make it feasible yet accurate in realistic systems. We demonstrate our approach with HHG calculations in water, ammonia, and methane liquids, and compare the characteristic response of polar and non-polar liquids. We identify unique features in the HHG spectra of liquid methane that could be utilized for ultrafast spectroscopy of its chemical and physical properties: (i) a structural minima at 15-17eV, and (ii) a well-like shape in the perturbative region that is reminiscent of a shape resonance. Our results pave the way to accessible calculations of HHG in liquids and illustrate the unique nonlinear nature of liquid systems.

physics.chem-ph↗

arXiv2022

Probing phonon dynamics with multi-dimensional high harmonic carrier envelope phase spectroscopy

We explore pump-probe high harmonic generation (HHG) from monolayer hexagonal-Boron-Nitride, where a terahertz pump excites coherent optical phonons that are subsequently probed by an intense infrared pulse that drives HHG. We find, through state-of-the-art ab-initio calculations, that the structure of the emission spectrum is attenuated by the presence of coherent phonons, and is no longer comprised of discrete harmonic orders, but rather of a continuous emission in the plateau region. The HHG yield strongly oscillates as a function of the pump-probe delay, corresponding to ultrafast changes in the lattice such as bond compression or stretching. We further show that in the regime where the excited phonon period and the pulse duration are of the same order of magnitude, the HHG process becomes sensitive to the carrier-envelope-phase (CEP) of the driving field, even though the pulse duration is so long that no such sensitivity is observed in the absence of coherent phonons. The degree of CEP sensitivity vs. pump-probe delay is shown to be a highly selective measure for instantaneous structural changes in the lattice, providing a new approach for ultrafast multi-dimensional HHG-spectroscopy. Remarkably, the obtained temporal resolution for phonon dynamics is ~1 femtosecond, which is much shorter than the probe pulse duration because of the inherent sub-cycle contrast mechanism. Our work paves the way towards novel routes of probing phonons and ultrafast material structural changes and provides a mechanism for controlling the high harmonic response.

cond-mat.mtrl-sci↗

arXiv2022

Floquet engineering the band structure of materials with optimal control theory

We demonstrate that the electronic structure of a material can be deformed into Floquet pseudo-bands with arbitrarily tailored shapes. We achieve this goal with a novel combination of quantum optimal control theory and Floquet engineering. The power and versatility of this framework is demonstrated here by utilizing the independent-electron tight-binding description of the $π$ electronic system of graphene. We show several prototype examples focusing on the region around the K (Dirac) point of the Brillouin zone: creation of a gap with opposing flat valence and conduction bands, creation of a gap with opposing concave symmetric valence and conduction bands -- which would correspond to a material with an effective negative electron-hole mass --, or closure of the gap when departing from a modified graphene model with a non-zero field-free gap. We employ time periodic drives with several frequency components and polarizations, in contrast to the usual monochromatic fields, and use control theory to find the amplitudes of each component that optimize the shape of the bands as desired. In addition, we use quantum control methods to find realistic switch-on pulses that bring the material into the predefined stationary Floquet band structure, i.e. into a state in which the desired Floquet modes of the target bands are fully occupied, so that they should remain stroboscopically stationary, with long lifetimes, when the weak periodic drives are started. Finally, we note that although we have focused on solid state materials, the technique that we propose could be equally used for the Floquet engineering of ultracold atoms in optical lattices, and to other non-equilibrium dynamical and correlated systems.

cond-mat.mes-hall↗

arXiv2022

Common microscopic origin of the phase transitions in Ta$_2$NiS$_5$ and the excitonic insulator candidate Ta$_2$NiSe$_5$

The structural phase transition in Ta$_2$NiSe$_5$ has been envisioned as driven by the formation of an excitonic insulating phase. However, the role of structural and electronic instabilities on crystal symmetry breaking has yet to be disentangled. Meanwhile, the phase transition in its complementary material Ta$_2$NiS$_5$ does not show any experimental hints of an excitonic insulating phase. We present a microscopic investigation of the electronic and phononic effects involved in the structural phase transition in Ta$_2$NiSe$_5$ and Ta$_2$NiS$_5$ using extensive first-principles calculations. In both materials the crystal symmetries are broken by phonon instabilities, which in turn lead to changes in the electronic bandstructure also observed in experiment. A total energy landscape analysis shows no tendency towards a purely electronic instability and we find that a sizeable lattice distortion is needed to open a bandgap. We conclude that an excitonic instability is not needed to explain the phase transition in both Ta$_2$NiSe$_5$ and Ta$_2$NiS$_5$.

cond-mat.mtrl-sci↗

arXiv2022

Moiré Engineering of Spin-Orbit Coupling in Twisted Platinum Diselenide

We study the electronic structure and correlated phases of twisted bilayers of platinum diselenide using large-scale ab initio simulations combined with the functional renormalization group. PtSe$_2$ is a group-X transition metal dichalcogenide, which hosts emergent flat bands at small twist angles in the twisted bilayer. Remarkably, we find that moiré engineering can be used to tune the strength of Rashba spin-orbit interactions, altering the electronic behavior in a novel manner. We reveal that an effective triangular lattice with a twist-controlled ratio between kinetic and spin-orbit coupling scales can be realized. Even dominant spin-orbit coupling can be accessed in this way and we discuss consequences for the interaction driven phase diagram, which features pronounced exotic superconducting and entangled spin-charge density waves.

cond-mat.str-el↗

arXiv2022

Frequency-dependent Sternheimer linear-response formalism for strongly coupled light-matter systems

The rapid progress in quantum-optical experiments especially in the field of cavity quantum electrodynamics and nanoplasmonics, allows to substantially modify and control chemical and physical properties of atoms, molecules and solids by strongly coupling to the quantized field. Alongside such experimental advances has been the recent development of ab-initio approaches such as quantum electrodynamical density-functional theory (QEDFT) that is capable of describing these strongly coupled systems from first-principles. To investigate response properties of relatively large systems coupled to a wide range of photon modes, ab-initio methods that scale well with system size become relevant. In light of this, we extend the linear-response Sternheimer approach within the framework of QEDFT to efficiently compute excited-state properties of strongly coupled light-matter systems. Using this method, we capture features of strong light-matter coupling both in the dispersion and absorption properties of a molecular system strongly coupled to the modes of a cavity. We exemplify the efficiency of the Sternheimer approach by coupling the matter system to the continuum of an electromagnetic field. We observe changes in the spectral features of the coupled system as Lorentzian line shapes turn into Fano resonances when the molecule interacts strongly with the continuum of modes. This work provides an alternative approach for computing efficiently excited-state properties of large molecular systems interacting with the quantized electromagnetic field.

physics.chem-ph↗

arXiv2022

Spin-orbit induced equilibrium spin currents in materials

The existence of spin-currents in absence of any driving external fields is commonly considered an exotic phenomenon appearing only in quantum materials, such as topological insulators. We demonstrate instead that equilibrium spin currents are a rather general property of materials with non negligible spin-orbit coupling (SOC). Equilibrium spin currents can be present at the surfaces of a slab. Yet, we also propose the existence of global equilibrium spin currents, which are net bulk spin-currents along specific crystallographic directions of materials. Equilibrium spin currents are allowed by symmetry in a very broad class of systems having gyrotropic point groups. The physics behind equilibrium spin currents is uncovered by making an analogy between electronic systems with SOC and non-Abelian gauge theories. The electron spin can be seen as the analogous of the color degree of freedom and equilibrium spin currents can then be identified with diamagnetic color currents appearing as the response to an effective non-Abelian magnetic field generated by SOC. Equilibrium spin currents are not associated with spin transport and accumulation, but they should nonetheless be carefully taken into account when computing transport spin currents. We provide quantitative estimates of equilibrium spin currents for several systems, specifically metallic surfaces presenting Rashba-like surface states, nitride semiconducting nanostructures and bulk materials, such as the prototypical gyrotropic medium tellurium. In doing so, we also point out the limitations of model approaches showing that first-principles calculations are needed to obtain reliable predictions. We therefore use Density Functional Theory computing the so-called bond currents, which represent a powerful tool to understand the relation between equilibrium currents, electronic structure and crystal point group.

cond-mat.mes-hall↗

arXiv2021

First-principles modelling for time-resolved ARPES under different pump-probe conditions

First-principles methods for time-resolved angular resolved photoelectron spectroscopy play a pivotal role in providing interpretation and microscopic understanding of the complex experimental data and in exploring novel observables or observation conditions that may be achieved in future experiments. Here we describe an efficient, reliable and scalable first-principles method for tr-ARPES based on time-dependent density functional theory including propagation and surface effects usually discarded in the widely used many-body techniques based on computing the non-equilibrium spectral function and discuss its application to a variety of pump-probe conditions. We identify four conditions, depending on the length of the probe relative to the excitation in the materials on the one hand and on the overlap between pump and probe on the other hand. Within this paradigm different examples of observables of time-resolved ARPES are discussed in view of the newly developed and highly accurate time-resolved experimental spectroscopies.

cond-mat.mtrl-sci↗

arXiv2021

Magnon frequency renormalization by the electronic geometrical spin torque in itinerant magnets

We investigate non-adiabatic effects on the magnon frequency in an interacting system of localized spins and itinerant electrons. Including the lowest order corrections to the adiabatic dynamics in an analytically solvable model, applicable to simple ferromagnets like Fe, Co and Ni, we find that the magnon frequency is renormalized by a geometrical torque arising from the electronic spin Berry curvature. Comparison to exact numerical simulations reveals that our analytical solution captures essential low-energy features, and provides a mechanism for the magnon frequency hardening observed in recent first principles calculations for Fe, provided the geometrical torque is taken into account.

cond-mat.mtrl-sci↗

arXiv2021

Cavity-Modulated Proton Transfer Reactions

Proton transfer is ubiquitous in many fundamental chemical and biological processes, and the ability to modulate and control the proton transfer rate would have a major impact on numerous quantum technological advances. One possibility to modulate the reaction rate of proton transfer processes is given by exploiting the strong light-matter coupling of chemical systems inside optical or nanoplasmonic cavities. In this work, we investigate the proton transfer reactions in the prototype malonaldehyde and Z-3-amino-propenal (aminopropenal) molecules using different quantum electrodynamics methods, in particular quantum electrodynamics coupled cluster theory (QED-CC) and quantum electrodynamical density functional theory (QEDFT). Depending on the cavity mode polarization direction, we show that the optical cavity can increase the reaction energy barrier by 10--20$\%$ or decrease the reaction barrier by $\sim$5$\%$. By using first principles methods, this work establishes strong light-matter coupling as a viable and practical route to alter and catalyze proton transfer reactions.

physics.chem-ph↗

arXiv2021

Nonlinear electric conductivity and THz-induced charge transport in graphene

Based on the quantum master equation approach, the nonlinear electric conductivity of graphene is investigated under static electric fields for various chemical potential shifts. The simulation results show that, as the field strength increases, the effective conductivity is firstly suppressed, reflecting the depletion of effective carriers due to the large displacement in the Brillouin zone caused by the strong field. Then, as the field strength exceeds $1$~MV/m, the effective conductivity increases, overcoming the carrier depletion via the Landau--Zener tunneling process. Based on the nonlinear behavior of the conductivity, the charge transport induced by few-cycle THz pulses is studied to elucidate the ultrafast control of electric current in matter.

cond-mat.mes-hall↗

arXiv2021

Attosecond correlated electron dynamics at C$_{60}$ giant plasmon resonance

Fullerenes have unique physical and chemical properties that are associated with their delocalized conjugated electronic structure. Among them, there is a giant ultra-broadband - and therefore ultrafast - plasmon resonance, which for C$_{60}$ is in the extreme-ultraviolet energy range. While this peculiar resonance has attracted considerable interest for the potential downscaling of nanoplasmonic applications such as sensing, drug delivery and photocatalysis at the atomic level, its electronic character has remained elusive. The ultrafast decay time of this collective excitation demands attosecond techniques for real-time access to the photoinduced dynamics. Here, we uncover the role of electron correlations in the giant plasmon resonance of C$_{60}$ by employing attosecond photoemission chronoscopy. We find a characteristic photoemission delay of up to 200 attoseconds pertaining to the plasmon that is purely induced by coherent large-scale correlations. This result provides novel insight into the quantum nature of plasmonic resonances, and sets a benchmark for advancing nanoplasmonic applications.

physics.atom-ph↗

arXiv2021

Local Sensing of Correlated Electrons in Dual-moiré Heterostructures using Dipolar Excitons

Moiré heterostructures are rapidly emerging as a tunable platform to study correlated electronic phenomena. Discovery of exotic quantum phases in moiré systems requires novel probes of charge and spin order. Unlike detection schemes which average over several moiré cells, local sensors can provide richer information with greater sensitivity. We study a WSe$_2$/MoSe$_2$/WSe$_2$ heterotrilayer which hosts excitons and electrons in distinct moiré lattices, and show that localized dipolar excitons are sensitive proximity charge sensors, uncovering numerous correlated electronic states at fractional fillings of the multi-orbital moiré lattice. In addition, the emission polarization can reveal the local electronic spin configuration at different fillings. Our results establish dipolar excitons as promising candidates to study emergent quantum matter and quantum magnetism in moiré crystals with higher spatial resolution.

cond-mat.mes-hall↗

arXiv2021

Nanometer-scale lateral p-n junctions in graphene/$α$-RuCl$_3$ heterostructures

The ability to create high-quality lateral p-n junctions at nanometer length scales is essential for the next generation of two-dimensional (2D) electronic and plasmonic devices. Using a charge-transfer heterostructure consisting of graphene on $α$-RuCl$_3$, we conduct a proof-of-concept study demonstrating the existence of intrinsic nanoscale lateral p-n junctions in the vicinity of graphene nanobubbles. Our multi-pronged experimental approach incorporates scanning tunneling microscopy (STM) and spectroscopy (STS) and scattering-type scanning near-field optical microscopy ($\textit{s}$-SNOM) in order to simultaneously probe both the electronic and optical responses of nanobubble p-n junctions. Our STM and STS results reveal that p-n junctions with a band offset of more than 0.6 eV can be achieved over lateral length scale of less than 3 nm, giving rise to a staggering effective in-plane field in excess of 10$^8$ V/m. Concurrent $\textit{s}$-SNOM measurements confirm the utility of these nano-junctions in plasmonically-active media, and validate the use of a point-scatterer formalism for modeling surface plasmon polaritons (SPPs). Model $\textit{ab initio}$ density functional theory (DFT) calculations corroborate our experimental data and reveal a combination of sub-angstrom and few-angstrom decay processes dictating the dependence of charge transfer on layer separation. Our study provides experimental and conceptual foundations for the use of charge-transfer interfaces such as graphene/$α$-RuCl$_3$ to generate p-n nano-junctions.

cond-mat.mes-hall↗