arXiv subjects

Camilo Granados

Publications and source records attributed to Camilo Granados.

11 recordsLinked to original sources

arXiv2026

Carrier-Envelope Phase Control of Orbital Angular Momentum in Solid-State High-Harmonic Generation

High-order harmonic generation (HHG) driven by optical vortices is a powerful route to produce structured light in different spectral regions. The nonlinear process transfers orbital angular momentum (OAM) from the driving field to the emitted harmonics according to the scaling law $l_q = q\times l$, a consequence of the rotational invariance and angular momentum conservation. Here, we show that, in the regime of few-cycle pulses, the topological charge (TC) of the harmonic radiation detected within a finite spectral window is no longer fixed by this scaling law alone, but is governed by the interplay between broken crystal inversion symmetry and carrier-envelope phase (CEP)-sensitive sub-cycle electron dynamics. By driving HHG in a ZnO crystal with few-cycle ($\approx 1.5$ cycles) vortex beams centered at 3.2~$\mu$m, we observed that the measured TC becomes strongly CEP-dependent, switching between adjacent integer values, but only when the inversion symmetry is broken and the harmonic emission is CEP-sensitive. The TC switching vanishes when either condition is removed. Numerical analysis reveals that the TC switching originates from a CEP-controlled redistribution of spectral weight among spectrally overlapping harmonic orders, which changes the dominant OAM channel within the detection window. These results identify the CEP as a degree of freedom for tailoring the topological structure of high-harmonic radiation, pointing toward waveform-controlled structured attosecond light sources.

physics.optics↗

arXiv2026

Field-driven helicity in solid-state high-harmonic generation

The polarization state of light plays a central role in strong-field light--matter interactions and is widely used to probe electronic structure in solids via high-order harmonic generation (HHG). In particular, helicity-resolved HHG has been interpreted as a fingerprint of crystal symmetry and topology. Here, we demonstrate deterministic and continuous control of harmonic helicity in solids using polarization-crafted beams, formed by two orthogonally polarized pulses with a controlled time delay. By tuning this delay, the polarization state of individual harmonics can be driven from linear to circular, independent of the material under investigation. We show that this behavior is robust across systems with distinct symmetry and topology, and originates from the sub-cycle modulation of the light--matter interaction mediated by the dipole coupling. Furthermore, the orthogonal configuration allows to break the dynamical symmetry of the light-matter interaction which is manifested in the generation of otherwise forbidden harmonics under standard selection rules.. These results establish harmonic helicity as a field-controlled observable rather than a direct material fingerprint.

physics.optics↗

arXiv2026

Fluctuation-induced symmetry breaking in high harmonic generation for bicircular quantum light

Symmetries are ubiquitous in physics and play a pivotal role in light-matter interactions, where they determine the selection rules governing allowed atomic transitions and define the associated conserved quantities. For the up-conversion process of high harmonic generation, the symmetries of the driving field determine the allowed frequencies and the polarization properties of the resulting harmonics. As a consequence, it is possible to establish classical selection rules when the process is driven by coherent radiation. In this work, we show that fluctuation-induced symmetry breaking in the driving field leads to the appearance of otherwise forbidden harmonics. This is achieved by considering bicircular quantum light, and demonstrate that the enhanced quantum fluctuations due to squeezing in the driving field break the classical selection rules. To this end, we develop a quantum optical description of the dynamical symmetries in the process of high harmonic generation, revealing corrections to the classical selection rules. Moreover, we show that the new harmonics show squeezing-like signatures in their photon statistics, allowing them to be clearly distinguished from classical thermal fluctuations.

quant-ph↗

arXiv2026

Twisting harmonics: Transfer of orbital angular momentum in solid-state high-harmonic generation

Although solid-state platforms underpin modern electronics, little is known about how intense ultrashort light pulses carrying orbital angular momentum (OAM) interact with solids. This gap persists even though, for more conventional light-matter interactions, the complex underlying electron dynamics can often be confined to a single Brillouin zone and described well within the dipole approximation. Previous studies were restricted to nonlinear, perturbative regimes, largely because the generation of intense ultrashort vortex pulses, particularly in the mid-infrared spectral regime, has remained a long-standing challenge. Consequently, the role of structured light in driving nonlinear, non-perturbative processes in solids, and the associated transfer of angular momentum during these interactions, has not been systematically explored. Here, we investigate solid-state high-harmonic generation (HHG) driven by intense ultrashort structured light using a versatile experimental approach applicable to different materials and geometries. We demonstrate that the OAM of the driving field is coherently transferred to the emitted harmonics. In particular, we show that the OAM is conserved independently of the crystal symmetry, the range of electronic interactions, and the presence of strong spin-orbit coupling. These results establish OAM-resolved HHG as a robust framework for characterizing and controlling angular momentum transfer in solid-state HHG and open new avenues for structured-light-driven quantum technologies and topological materials investigations.

physics.optics↗

arXiv2025

Sculpting ultrafast mid-infrared light for solid-state high harmonic generation

The ability to sculpt light in space, time, and polarization has revolutionized studies of light-matter interaction and enabled breakthroughs in optical communication, imaging, and ultrafast science. Among the many degrees of freedom of light, orbital angular momentum (OAM) further expands these capabilities by unlocking new regimes of control in information encoding, particle trapping and manipulation, and symmetry-driven selection rules. However, exploiting OAM to drive nonlinear, non-perturbative effects in solids remains challenging, especially in the mid-infrared (MIR) spectral regime-a key region for accessing these effects in ambient air, where spatial light modulators do not operate. Here, we circumvent this limitation by generating femtosecond, few-cycle MIR Bessel-Gauss vortex (BGV) and perfect optical vortices (POVs), using a robust, static spatial-shaping strategy. By utilizing these beams to drive nonlinear optical processes such as second-harmonic generation (SHG) and high-harmonic generation (HHG) in various solid-state materials, we show that the resulting harmonic beams faithfully inherit the structural characteristics of the drivers: the constant-intensity ring of the POVs is preserved across harmonic orders, while the BGV harmonic beams retain their intrinsic topological charge-dependent intensity profiles. Furthermore, by verifying the linear OAM up-scaling law, we confirm the conservation of OAM during SHG and HHG in solids. These results establish strong-field HHG in solids as a robust platform for synthesizing ultrafast structured harmonic light with controllable, high-value OAM.

physics.optics↗

arXiv2025

Optical Vortices: Revolutionizing the field of linear and nonlinear optics

Light is the fundamental medium through which we perceive the world around us. In the modern era, light can not only be used in its raw form but can also be used as a versatile tool. Generally, light fields carry energy and momentum (both linear and angular). Due to the transfer of linear momentum from light to matter, the radiation pressure is exerted, whereas, the intrinsic spin angular momentum (SAM) is associated with the polarization states of light. Light fields embedded with optical orbital angular momentum (OAM) -- also known as optical vortices or phase singular beams -- have truly revolutionized the field of optics and extended our basic understanding of the light-matter interaction process across various scales. Optical vortices -- spatially characterized by the presence of twisted phase fronts and a central intensity null -- have found a myriad of applications starting from microparticle trapping and manipulation to microscopy, optical communication, and quantum information science, among others. Here, we revisit some of the fundamental concepts on optical vortices and discuss extensively on how this new dimension of light i.e., the OAM, has been exploited in both linear and nonlinear optical regimes. We discuss the different types of vortex beams, the techniques used to generate and detect their OAM, and their propagation. Particularly, we put a special emphasis on the utilization of vortex beams in nonlinear regimes to explain different optical phenomena such as the second harmonic generation, parametric down-conversion, and high-order harmonic generation. The generation of vortex beams in the UV to XUV regimes, encoded with higher OAM values, could potentially extend their application range to areas such as high-capacity data transmission, stimulated emission depletion microscopy, phase-contrast imaging, and particle trapping in optical tweezers, among others.

physics.optics↗

arXiv2025

High Harmonic Spectroscopy from Lower-Order to Higher-Order Topological Insulators

Over the past decades, high-harmonic spectroscopy (HHS) has emerged as a powerful tool for all-optical probing of topological properties of solids. There are outstanding questions regarding universal nature of the spectral features of harmonics in their relationship to the non-trivial topological properties. Here, we present a systematic theoretical study of HHS in topological materials, including lower-order and higher-order topological insulators (LOTIs and HOTIs), focusing on observables such as helicity, circular dichroism, ellipticity dependence, and channel-resolved intensity yields. Using the Haldane, Kane-Mele, and breathing Kagome lattice models, we theoretically extend all-optical approaches from the LOTI to the HOTI regime by explicitly incorporating contributions from bulk, edge, and it corner states. Depending on the crystalline system, our calculations suggest that these observables can encode topological information through distinct modifications of the HHG spectra in topological phases. In particular, we identify significant enhancements of the harmonic intensity yields, reaching up to two orders of magnitude relative to trivial phases, together with distinct spectral signatures associated with edge and corner contributions revealed through channel-resolved intensity yields. These results show that channel-resolved HHS provides a promising route for probing topological states in both LOTIs and HOTIs.

cond-mat.mtrl-sci↗

arXiv2025

Two-color harmonic spectroscopy of ultrafast Dirac electron dynamics

High-harmonic generation (HHG), the hallmark effect of attosecond science, is a nonperturbative nonlinear process leading to the emission of high-harmonic light from gases and solids. In gases, extreme driving laser pulse intensities can deplete the ground state, suppressing harmonic emission during the trailing edge of the pulse. Here, we report a similar effect, pronounced ultrafast carrier saturation dynamics and harmonic emission suppression during nonperturbative harmonic generation (NPHG) in a gapless Dirac semimetal -- highly oriented pyrolytic graphite (HOPG). Remarkably, HOPG supports NPHG at laser intensities as low as $\sim 10^{10}$ W cm$^{-2}$, facilitated by its vanishing bandgap. Ultrafast carrier saturation strongly modulates the interplay between interband and intraband currents, a key characteristic of NPHG in Dirac materials. Using two-color spectroscopy, we reveal the excitation dynamics of Dirac electron-hole pairs as it affects the emission of harmonics during the presence of the driving laser pulse. The excitation of out-of-equilibrium hot carriers and the concomitant saturation near the Dirac points leads to a marked suppression of interband harmonics and induces measurable temporal shifts. These observations are supported by simulations based on semiconductor Bloch equations. Our finding reveal that field-driven carrier saturation plays a critical role in gapless solid NPHG. We demonstrate the potential of NPHG and HHG as a sensitive, all-optical probe of ultrafast carrier dynamics, offering novel opportunities for ultrafast optoelectronics in Dirac materials.

physics.optics↗

arXiv2023

Above-threshold ionization by polarization-crafted pulses

Coherent light has revolutionized scientific research, spanning biology, chemistry, and physics. To delve into ultrafast phenomena, the development of high-energy, high-tunable light sources is instrumental. Here, the photo-electric effect is a pivotal tool for dissecting electron correlations and system structures. Particularly, above-threshold ionization (ATI), characterized by simultaneous multi-photon absorption, has been widely explored, both theoretical and experimentally. ATI decouples laser field effects from the structural information carried by photo-electrons, particularly when utilizing ultra-short pulses. In this contribution we study ATI driven by polarization-crafted (PC) pulses, which offer precise control over the electron emission directions, through an accurate change of the polarization state. PC pulses enable the manipulation of electron trajectories, opening up new avenues for understanding and harnessing coherent light. Our work explores how structured light could allow a high degree of control of the emitted photo-electrons.

physics.atom-ph↗

arXiv2023

Single photon zeptosecond interferometry

We demonstrate the generation of a train of attosecond XUV pulses that are in a superposition of wavefront states. Such superposition yields a high precision, self-referencing, common path XUV interferometer setup to produce pairs of spatially separated and independently controllable XUV pulses that are locked in phase and time with a temporal jitter of 3.5 zs (zs = zeptoseconds = $10^{-21}$). In our approach, we can independently control the relative phase/delay of the two optical beams with a resolution of 52 zs. Since the jitter is on the order of the Compton time scale, we explore the level of correlation between the non-local photons by comparing different spatial mode superpositions. Further, thanks to the stability of the interferometer we can retrieve the interference pattern through photon counting. Through post-selection of different particle events we can analyze one, two or more photon events. We argue that this zeptosecond level of temporal precision will open the door for new dynamical QED tests at lower intensities while photon counting experiments can also have an impact on the emerging field of quantum light in strong fields. We also discuss the potential impact on other areas, such as time-dependent QED, imaging, measurements of non-locality, and molecular quantum tomography.

physics.optics↗

arXiv2020

The electron affinity of astatine

One of the most important properties influencing the chemical behavior of an element is the energy released with the addition of an extra electron to the neutral atom, referred to as the electron affinity (EA). Among the remaining elements with unknown EA is astatine, the purely radioactive element 85. Astatine is the heaviest naturally occurring halogen and its isotope $^{211}$At is remarkably well suited for targeted radionuclide therapy of cancer. With the At$^-$ anion being involved in many aspects of current astatine labelling protocols, the knowledge of the electron affinity of this element is of prime importance. In addition, the EA can be used to deduce other concepts such as the electronegativity, thereby further improving the understanding of astatine's chemistry. Here, we report the first measurement of the EA for astatine to be 2.41578(7)eV. This result is compared to state-of-the-art relativistic quantum mechanical calculations, which require incorporation of the electron-electron correlation effects on the highest possible level. The developed technique of laser-photodetachment spectroscopy of radioisotopes opens the path for future EA measurements of other radioelements such as polonium, and eventually super-heavy elements, which are produced at a one-atom-at-a-time rate.

physics.atom-ph↗