arXiv subjects

Rui E. F. Silva

Publications and source records attributed to Rui E. F. Silva.

At least 19 recordsLinked to original sources

arXiv2026

Semiconductor Wannier equations: a real-time, real-space approach to the nonlinear optical response in crystals (ATATA)

We develop the semiconductor Wannier equations (SWEs), a real-time, real-space formulation of ultrafast light-matter dynamics in crystals, by deriving the equations of motion for the electronic reduced density matrix in a localized Wannier basis. Working in real space removes the structure-gauge ambiguities that hinder reciprocal-space semiconductor Bloch equations. Electron--electron interactions are included at the time-dependent Hartree plus static screened-exchange (TD-HSEX) level. Decoherence is modeled with three complementary channels: pure dephasing, population relaxation, and distance-dependent real-space dephasing; providing physically grounded damping for strong-field phenomena such as high-harmonic generation. Conceptually, the SWEs bridge real-space semiclassical intuition with many-body solid-state optics, offering a numerically robust and gauge-clean alternative to reciprocal-space approaches for nonlinear optical response and attosecond spectroscopy in solids.

physics.optics↗

arXiv2026

Valley polarization driven by two-color circular fields: a rotating frame and strong-field perspective

Valley polarization in hexagonal materials driven by the form of the lightwave and its orientation relative to the lattice, rather than solely by the helicity of the driver, has recently been demonstrated both theoretically and experimentally. This has extended valley control to the non-resonant, sub-cycle regime and to inversion-symmetric materials. One interpretation of this field-orientation-dependent valley polarization is that the laser-dressed, cycle-averaged band structure obtained from a Floquet-type approach is modified so as to lift the degeneracy between the valleys. Here, we derive a complementary explanation based on strong-field tunneling dynamics. We show that the effective valley gap at the dominant injection times depends on the orientation of the field relative to the lattice through the trigonal-warping term of the low-energy dispersion. We derive general expressions for co- and counter-rotating $ω+Nω$ fields and show that the leading orientation-dependent contribution survives the cycle average only for field configurations compatible with the threefold lattice symmetry, most notably counter-rotating $ω+2ω$ and co-rotating $ω+4ω$ fields. As a complementary weak-field result, we show that, for counter-rotating bicircular fields, the one-photon valley selection rules can be represented as valley-dependent energy detunings in a rotating frame where both colors acquire the same frequency.

physics.optics↗

arXiv2026

Programmable high-harmonic emission in solids through photon pathways

Ultrafast all-optical control of light emission is a central goal of extreme nonlinear optics, with implications for compact short-wavelength sources, petahertz optoelectronics, and label-free superresolution microscopy. High-harmonic generation in solids is a particularly attractive platform for this goal because it is highly sensitive to both the driving field and the material response, yet a generally applicable framework for controlling harmonic emission has remained elusive. Here, we demonstrate programmable control of high-harmonic emission in solids and show that it can be quantitatively described within a photon-pathway framework. We find that harmonic emission can be suppressed or enhanced by tuning two experimentally accessible quantities: the effective nonlinear order and the intrinsic emission phase. Across a wide range of semiconductors and dielectrics, this approach unifies parametric and non-parametric modulation, explains distinct delay-dependent spectral responses, and reproduces strong suppression, enhancement, and higher-order pathway revivals. Semiconductor Bloch equation simulations support the model and provide a complementary time-domain picture in which the control field reshapes the interference of sub-cycle emission events. These results establish high-harmonic generation in solids as a programmable emission process and provide a general route towards ultrafast optical switching, compact coherent short-wavelength sources, and label-free attosecond super-resolution microscopy.

physics.optics↗

arXiv2026

Contrasting ultrafast light-driven electron-hole interaction dynamics in monolayer MoS$_2$ and metallic NbSe$_2$

We study strong-field driven ultrafast dynamics and high-harmonic generation (HHG) in monolayer 2H-NbSe$_2$ and compare them with those of monolayer 2H-MoS$_2$ by solving the multiband reduced-density-matrix equations including time-dependent electron-electron interaction effects within the time-dependent Hartree + screened exchange (TD-HSEX). In MoS$_2$, these interactions strongly enhance the harmonic yield and modify the harmonic phases and angular emission patterns, wheras in NbSe$_2$ the yield enhancement is weaker but clear phase and angular changes remain. We trace these differences to the distinct optical resonances and to the different bands involved in the emission in each material. Finally, we show that carrier injection into empty bands of NbSe$_2$ differs qualitatively from interband excitation in MoS$_2$, and is well captured at a qualitative level by a Keldysh tunneling rate with a time-dependent band separation, allowing to control the timing and the region of injection of carriers to empty bands of the metal with the field parameters. Our work provides a framework to interpret ultrafast electron-hole interaction effects in experimental high harmonic generation spectra across semiconducting and metallic systems.

physics.optics↗

arXiv2025

Effects of Zero-Point Motion in the High Harmonic Generation Spectrum of Solids

The interpretation of high-harmonic generation (HHG) in solids typically relies on phenomenological dephasing times far shorter than what is expected from microscopic scattering processes. Here we show that zero-point fluctuations associated with optical phonons naturally suppress long-range electronic coherences and generate clean harmonic spectra without introducing ad-hoc decoherence parameters. Using a 1D semiconductor composed of two distinct sites per unit cell and realistic phonon amplitudes, we demonstrate that random per-site optical-phonon jitter reproduces the spectral sharpening typically attributed to ultrafast $T_2$ dephasing. In contrast, acoustic phonons and local strain, whose distortions are correlated over nanometer scales, produce negligible spectral cleaning. We further show that such long-range site coherence leads to carrier-envelope-phase-dependent effects in the HHG spectrum driven by long pulses, but these effects collapse once optical-phonon-induced decoherence is included. Our results (i) identify optical zero-point motion as a key mechanism governing coherence in solid-state HHG, (ii) demonstrate that it can be qualitatively modeled in periodic solids through site-distance-dependent dephasing, and (iii) suggest that CEP-resolved measurements can probe electronic coherence lengths and atomic fluctuations in crystalline materials.

physics.optics↗

arXiv2025

Unambiguous discrimination of high harmonic generation mechanisms in solids

Using real-space view of high harmonic generation (HHG) in solids, we develop a physically transparent and gauge-invariant approach for distinguishing intraband and interband HHG mechanisms. Our approach relies on resolving the harmonic emission according to the separation between Wannier states involved in radiative transitions. We show that the intra- and inter-band HHG emission exhibit striking qualitative differences in their dependence on this separation and can be clearly distinguished using the Wannier basis.

physics.optics↗

arXiv2025

Attosecond high-harmonic interferometry probes orbital- and band-dependent dipole phase in magnesium oxide

Control over the spatial coherence, wavefront, and focusability of emitted light relies on understanding the intrinsic phase of the emission process, and vice versa, measuring phase can reveal insights about microscopic generation mechanisms. A thorough understanding of the origin of the dipole phase in solid-state high-harmonic generation is currently missing. Here, by employing attosecond interferometry with phase-locked XUV pulses, we directly assess the intensity- and frequency-dependent dipole phases in magnesium oxide (MgO) in solid-state HHG. We also quantify a nonlinear phase shift of the fundamental and disentangle its contribution from the dipole phase. Theoretical models (analytical, two-band, and full-band numerical simulations) support our results. The analytical approach aids future solid-state HHG experiments and simulations, while the full numerical model details orbital- and band-resolved current contributions to the dipole phase. Our research delivers the first combined quantitative measurement and rigorous theoretical description of the harmonic emission phase in solids.

physics.optics↗

arXiv2025

High Harmonic Generation from a Noble Metal

High-harmonic generation (HHG) in solids has typically been explored in transparent dielectrics and semiconductors. Metals have long been dismissed due to their strong reflectivity at infrared wavelengths. Here, we demonstrate HHG from silver - a noble metal - using few-cycle near-infrared laser pulses at near-normal incidence. Our results show that sub-cycle electron dynamics within the material's penetration depth can drive high-order harmonics, challenging the prevailing notion that metals are unsuited for infrared-driven strong-field processes. Despite silver's high reflectivity and large free-electron density, we observe nonperturbative harmonics extending into the extreme ultraviolet (up to 20 eV). Moreover, silver's multi-shot damage threshold proves surprisingly high (30 TW/cm^2) - comparable to large-bandgap dielectrics like magnesium oxide - thereby enabling intense strong-field processes in a metallic environment. Measuring the orientation dependence of the emitted harmonics reveals that the process arises from coherent electron dynamics in the crystal lattice, rather than from a plasma-driven mechanism. Time-dependent density-matrix simulations based on maximally localized Wannier functions show that low-order harmonics predominantly originate from conduction electrons near the Fermi surface (s- and p-type orbitals), whereas higher harmonics rely on bound d-electron excitations. These findings establish metals - long thought unfavorable for HHG - as a promising platform for ultrafast strong-field physics, extending high-harmonic spectroscopy to regimes in which lattice order and plasma formation directly intersect. This work expands the frontier of solid-state HHG to all-metallic attosecond pulse generation and underscores the potential of metals as robust XUV sources for advanced attosecond metrology.

physics.optics↗

arXiv2024

Ultrafast valleytronic logic operations

Information processing currently reaches speeds as high as 800 GHz. However, the underlying transistor technology is quickly approaching its fundamental limits and further progress requires a disruptive approach. One such path is to manipulate quantum properties of solids, such as the valley degree of freedom, with ultrashort controlled lightwaves. Here we employ a sequence of few-optical-cycle visible pulses controlled with attosecond precision to excite and switch the valley pseudospin in a 2D semiconductor. We show that a pair of pulses separated in time with linear orthogonal polarizations can induce a valley-selective population. Additionally, exploiting a four-pump excitation protocol, we perform logic operations such as valley de-excitation and re-excitation at room temperature at rates as high as ~10 THz.

cond-mat.mes-hall↗

arXiv2024

Spatial polarization gating of high-harmonic generation in solids

High-harmonic generation from solids can be utilized as probe of ultrafast dynamics, but thus far only over extended sample areas, since its spatial resolution is diffraction-limited. Here we propose spatial polarization gating, that is using a spatially varying ellipticity of a driving laser pulse to reduce the spatial profile of high-harmonic emission below the diffraction limit and hence increase spatial resolution. We show experimentally and by numerical simulations that our method is generally applicable as suppressing high harmonics in elliptical fields is a common response in all solids. We also briefly explore the possibility of applying this technique to widefield imaging, specifically to nonlinear structured illumination microscopy. Our findings indicate that spatial polarization gating can enable all-optical femto-to-attosecond label-free imaging beyond the Abbe limit.

physics.optics↗

arXiv2024

Revealing the Berry phase under the tunneling barrier

In quantum mechanics, a quantum wavepacket may acquire a geometrical phase as it evolves along a cyclic trajectory in parameter space. In condensed matter systems, the Berry phase plays a crucial role in fundamental phenomena such as the Hall effect, orbital magnetism, and polarization. Resolving the quantum nature of these processes commonly requires sensitive quantum techniques, as tunneling, being the dominant mechanism in STM microscopy and tunneling transport devices. In this study, we integrate these two phenomena - geometrical phases and tunneling - and observe a complex-valued Berry phase via strong field light matter interactions in condensed matter systems. By manipulating the tunneling barrier, with attoseconds precision, we measure the imaginary Berry phase accumulated as the electron tunnels during a fraction of the optical cycle. Our work opens new theoretical and experimental directions in geometrical phases physics and their realization in condensed matter systems, expanding solid state strong field light metrology to study topological quantum phenomena.

cond-mat.mes-hall↗

arXiv2023

Ultrafast dephasing in solid state high harmonic generation: macroscopic origin revealed by real-space dynamics

Using a fully real-space perspective on high harmonic generation (HHG) in solids, we examine the relationship between microscopic response, macroscopic propagation of this response to the far field, and the extremely short dephasing times routinely used in the theoretical simulations of experimentally measured solid-state HHG spectra. We find that far field propagation naturally reduces the contribution to the observed HHG emission from electrons that do not return to the lattice site where they have been injected into the conduction band. We then show that extremely short dephasing times routinely used in microscopic simulations suppress many electron trajectories that contribute to the far-field spectra, leading to significant distortions of the true high harmonic response. We show that a real-space based dephasing mechanism, which preferentially suppresses trajectories which veer too far away from their original lattice site, yield HHG spectra that faithfully retain those trajectories that contribute to the far-field spectra while filtering out those which do not, already at the microscopic level. Our findings emphasize the similarities between atomic and solid-state HHG by highlighting the importance of the intensity-dependent phase of HHG emission and address the longstanding issue regarding the origin of extremely short dephasing times in solid-state HHG.

physics.optics↗

arXiv2023

A Real-Space Perspective on Dephasing in Solid-State High Harmonic Generation

We develop and demonstrate a fully real-space perspective on HHG in crystals. Due to Wannier-Stark localization induced on sub-cycle timescales in the presence of a strong field, real-space descriptions are natural for strongly driven solids. Our approach allows us to address the origin of the extremely short dephasing times, which appear necessary for agreement between experimental HHG measurements and theoretical calculations generally performed in reciprocal space. We develop a physically transparent model of real-space dephasing which relates its rate to the distance between different sites in a laser-driven lattice. Our approach leads to well-structured high harmonic spectra at the microscopic level, reproduces results of macroscopic propagation, and demonstrates that the requirement for ultrafast dephasing times stems from the need for suppressing recombination events with large electron-hole separations during radiative recombination.

physics.optics↗

arXiv2023

Observation of light driven band structure via multi-band high harmonic spectroscopy

Intense light-matter interactions have revolutionized our ability to probe and manipulate quantum systems at sub-femtosecond time scales, opening routes to all-optical control of electronic currents in solids at petahertz rates. Such control typically requires electric field amplitudes $\sim V/Å$, when the voltage drop across a lattice site becomes comparable to the characteristic band gap energies. In this regime, intense light-matter interaction induces significant modifications of electronic and optical properties, dramatically modifying the crystal band structure. Yet, identifying and characterizing such modifications remains an outstanding problem. As the oscillating electric field changes within the driving field's cycle, does the band-structure follow, and how can it be defined? Here we address this fundamental question, proposing all-optical spectroscopy to probe laser-induced closing of the band-gap between adjacent conduction bands. Our work reveals the link between nonlinear light matter interactions in strongly driven crystals and the sub-cycle modifications in their effective band structure.

physics.optics↗

arXiv2023

All-optical valley switch and clock of electronic dephasing

2D materials with broken inversion symmetry posses an extra degree of freedom, the valley pseudospin, that labels in which of the two energy-degenerate crystal momenta, K or K', the conducting carriers are located. It has been shown that shining circularly-polarized light allows to achieve close to $100\%$ of valley polarization, opening the way to valley-based transistors. Yet, switching of the valley polarization is still a key challenge for the practical implementation of such devices due to the short coherence lifetimes. Recent progress in ultrashort laser technology now allows to produce trains of attosecond pulses with controlled phase and polarization between the pulses. Taking advantage of such technology, we introduce a coherent control protocol to turn on, off and switch the valley polarization at faster timescales than electronic and valley decoherence, that is, an ultrafast optical valley switch. We theoretically demonstrate the protocol for hBN and MoS$_2$ monolayers calculated from first principles. Additionally, using two time-delayed linearly-polarized pulses with perpendicular polarization, we show that we can extract the electronic dephasing time $T_2$ from the valley Hall conductivity.

quant-ph↗

arXiv2023

Formation, stability, and highly nonlinear optical response of excitons to intense light fields interacting with two-dimensional materials

Excitons play a key role in the linear optical response of 2D materials. However, their significance in the highly nonlinear optical response to intense mid-infrared light has often been overlooked. Using hBN as a prototypical example, we theoretically demonstrate that excitons play a major role in this process. Specifically, we illustrate their formation and stability in intense low-frequency fields, where field strengths surpass the Coulomb field binding the electron-hole pair in the exciton. Additionally, we establish a parallelism between these results and the already-known physics of Rydberg states using an atomic model. Finally, we propose an experimental setup to test the effect of excitons in the nonlinear optical response

physics.optics↗

arXiv2023

High-Harmonic Generation with a twist: all-optical characterization of magic-angle twisted bilayer graphene

If we stack up two layers of graphene while changing their respective orientation by some twisting angle, we end up with a system that has striking differences when compared to single-layer graphene. For a very specific value of this twist angle, known as magic angle, twisted bilayer graphene displays a unique phase diagram that cannot be found in other systems. Recently, high harmonic generation spectroscopy has been successfully applied to elucidate the electronic properties of quantum materials. The purpose of the present work is to exploit the nonlinear optical response of magic-angle twisted bilayer graphene to unveil its electronic properties. We show that the band structure of magic-angle twisted bilayer graphene is imprinted onto its high-harmonic spectrum. Specifically, we observe a drastic decrease of harmonic signal as we approach the magic angle. Our results show that high harmonic generation can be used as a spectroscopy tool for measuring the twist angle and also the electronic properties of twisted bilayer graphene, paving the way for an all-optical characterization of moiré materials.

cond-mat.mes-hall↗

arXiv2022

A theoretical approach for electron dynamics and ultrafast spectroscopy

In this manuscript we present a theoretical framework and its numerical implementation to simulate the out-of-equilibrium electron dynamics induced by the interaction of ultrashort laser pulses in condensed-matter systems. Our approach is based on evolving in real-time the density matrix of the system in reciprocal space. It considers excitonic and non-perturbative light-matter interactions. We show some relevant examples that illustrate the efficiency and flexibility of the approach to describe realistic ultrafast spectroscopy experiments. Our approach is suitable for modeling the promising and emerging ultrafast studies at the attosecond time scale that aim at capturing the electron dynamics and the dynamical electron-electron correlations via X-ray absorption spectroscopy.

physics.optics↗