High Harmonic Emission Research Articles

Dominant role of charge ordering on high harmonic generation in Pr0.6Ca0.4MnO3

High harmonic generation (HHG) is a typical high-order nonlinear optical phenomenon and can be used to probe electronic structures of solids. Here, we investigate the temperature dependence of HHG from Pr0.6Ca0.4MnO3 in the range of 7–294 K, including the charge ordering (CO) transition and magnetic transition temperatures. The high harmonic (HH) intensity remains almost constant in the high-temperature charge-disordered phase. However, as the temperature is lowered, it starts to increase near the CO transition temperature where an optical gap related to the CO appears. The anomalous gap energy dependence resembles the one recently reported in a Mott insulator. We attribute the suppression of the HH intensity at high temperatures to the destructive interference among HH emissions from thermally activated multiple charge configurations. Our results suggest that HHG is a promising tool for probing the fluctuation of local order in strongly correlated systems. Published by the American Physical Society 2024

High harmonic Mach–Zehnder interferometer for probing sub-laser-cycle electron dynamics in solids

High harmonic emissions from crystalline solids contain rich information on the dynamics of electrons driven by intense infrared laser fields and have been intensively studied owing to their potential use as a probe of microscopic electronic structures. In particular, the ability to measure the temporal response of high harmonics may allow us to investigate electron dynamics directly. Here, we demonstrate a Mach–Zehnder high harmonic interferometer, where high harmonics are generated in each path of a Mach–Zehnder interferometer and an interferogram of them is captured. The high harmonic interferometer allows us to detect high harmonic signals with higher sensitivity than conventional high harmonic intensity measurements, and achieve a relative time resolution between the target and reference high harmonics of less than 150 attoseconds, which is sufficient to track sub-cycle dynamics of electrons in solids. Using high harmonic interferometry, we succeeded in capturing the real time dynamics of Floquet states in WSe2, whose indirect signature has so far been caught only by time-averaged measurements. Our simple technique could enable to access attosecond electron dynamics in solids.

Lightwave-controlled relativistic plasma mirrors.

We report on attosecond-scale control of high-harmonic and fast electron emission from plasma mirrors driven by relativistic-intensity near-single-cycle light waves at a kHz repetition rate. By controlling the waveform of the intense light transient, we reproducibly form a sub-cycle temporal intensity gate at the plasma mirror surface, leading to the observation of extreme ultraviolet spectral continua, characteristic of isolated attosecond pulse (IAP) generation. We also observe the correlated emission of a waveform-dependent relativistic electron beam, paving the way toward fully lightwave-controlled dynamics of relativistic plasma mirrors.

Controlling the bandwidth of high harmonic emission peaks with the spectral polarization of the driver.

We demonstrate a high harmonic-generation scheme that offers control over the bandwidth of the spectral peaks. The scheme uses a vectorial two-color driver with close central frequencies, generated by spectrally splitting a linearly polarized input femtosecond-duration laser pulse and subsequently recombining the two halves after their polarizations are made cross-elliptical and counter-rotating. This results in the generation of new emission channels that coalesce into broad odd-integer HHG peaks, the bandwidth of each being proportional to the frequency difference between the two colors, to the harmonic order and inversely proportional to the driver fields' ellipticities. Peak broadening to the extent that a supercontinuum is formed is also demonstrated. This source will find use in HHG applications benefiting from high-flux broadband extreme ultraviolet radiation, such as attosecond transient absorption spectroscopy.

High-harmonic Plasma Emission Induced by Electron Beams in Weakly Magnetized Plasmas

Electromagnetic radiation at higher harmonics of the plasma frequency (ω ∼ n ω pe, n > 2) has been occasionally observed in type II and type III solar radio bursts, yet the underlying mechanism remains undetermined. Here we present two-dimensional fully kinetic electromagnetic particle-in-cell simulations with high spectral resolution to investigate the beam-driven plasma emission process in weakly magnetized plasmas of typical coronal conditions. We focused on the generation mechanisms of high-harmonic emission. We found that a larger beam velocity (u d ) favors the generation of the higher-harmonic emission. The emissions grow later for higher harmonics and decrease in intensity by ∼2 orders of magnitude for each jump of the harmonic number. The second and third harmonic (H2 and H3) emissions get closer in intensity with larger u d . We also show that (1) the H3 emission is mainly generated via the coalescence of the H2 emission with the Langmuir waves, i.e., H2 + L → H3, wherein the coalescence with the forward-propagating beam-Langmuir wave leads to the forward-propagating H3, and coalescence with the backward-propagating Langmuir wave leads to the backward-propagating H3; and (2) the H4 emission mainly arises from the coalescence of the H3 emission with the forward- (backward-)propagating Langmuir wave, in terms of H3 + L → H4.

Research of electric vehicle battery packs and charging stations based on an active three-phase rectifier

Problem. The proliferation of electric vehicles has underscored the need for the development of energy-efficient charging stations and systems. These systems must deliver high efficiency, maintain a power factor close to unity, adhere to electromagnetic compatibility standards, emit low levels of higher harmonics, and enable fast charging capabilities. Current electric vehicle charging devices encounter issues such as significant power losses, high harmonic emissions to the power grid, and challenges in implementing fast charging modes. Consequently, enhancing the energy efficiency of charging stations – by reducing power losses, minimizing harmonic emissions, ensuring a high power factor, and supporting modes for regulated current and voltage sources for fast charging – is a pressing concern. Goal. The aim of this work is to perform a comparative analysis of different types of batteries for electric vehicles, exemplified by TESLA cars, presenting comparative characteristics of lithium-ion, lithium-iron-phosphate, and lithium-titanate batteries. Methodology. The study showcases an evaluation of battery units for electric vehicles and outlines a comparative assessment of lithium-ion, lithium-iron-phosphate, and lithium-titanate batteries. The research focuses on enhancing the energy efficiency of electric vehicle charging station systems through the use of active rectifiers, with modes for active power factor correction and optimal configuration. Results. An examination of the quality of converters for electric vehicle charging stations was conducted, proposing schemes for a three-phase active voltage source rectifier and an active current source rectifier. Power circuitry and space-vector switching states for power transistors are introduced. Analysis concludes that an active current rectifier may be a more promising topology. Originality. A model of a charging station based on an active current source rectifier was developed using Matlab/Simulink. Transient processes of the converter's operation and the charging of a 60 kWh battery pack were examined. It was found that the active rectifier facilitates regulation of the battery charging current, achieves a power factor close to unity, and maintains a low level of higher harmonic emissions with a harmonic distortion factor of 2.52%. Practical value. The advancement of electric vehicles necessitates the ongoing development and enhancement of the energy indicators for electric vehicle batteries and the converters of charging stations, especially those that enable fast charging. Active progress is being made in each of these areas.

Orbital perspective on high-harmonic generation from solids

High-harmonic generation in solids allows probing and controlling electron dynamics in crystals on few femtosecond timescales, paving the way to lightwave electronics. In the spatial domain, recent advances in the real-space interpretation of high-harmonic emission in solids allows imaging the field-free, static, potential of the valence electrons with picometer resolution. The combination of such extreme spatial and temporal resolutions to measure and control strong-field dynamics in solids at the atomic scale is poised to unlock a new frontier of lightwave electronics. Here, we report a strong intensity-dependent anisotropy in the high-harmonic generation from ReS2 that we attribute to angle-dependent interference of currents from the different atoms in the unit cell. Furthermore, we demonstrate how the laser parameters control the relative contribution of these atoms to the high-harmonic emission. Our findings provide an unprecedented atomic perspective on strong-field dynamics in crystals, revealing key factors to consider in the route towards developing efficient harmonic emitters.

Higher-Order Harmonics in Hexagonal Graphene Quantum Dots

We have considered the high-order harmonic generation in plane graphene quantum dots of hexagonal shape by the independent quasiparticle approximation-tight binding model. We have investigated how such a nonlinear effect is affected by a strong optical wave field, quantum dot typical band gap and lateral size, and dephasing processes. The equation of motion for the density matrix is solved by performing the time integration with the eight-order Runge–Kutta algorithm. If the optical wave frequency is much less than the quantum dot intrinsic band gap, the main aspects of multiphoton high harmonic emission in quantum dots are revealed. In such case dependence of the cutoff photon energy on the strength of the optical pump wave is almost linear. But when the wave frequency is comparable to the bandgap of the quantum dot, the cutoff photon energy shows saturation behavior with an increase in the wave field strength.

Valley-Selective High Harmonic Generation and Polarization Induced by an Orthogonal Two-Color Laser Field

The valley pseudospin properties of electrons in two-dimensional hexagonal materials result in many fascinating physical phenomena, which opens up the new field of valleytronics. The valley-contrasting physics aims at distinguishing the valley degree of freedom based on valley-dependent effects. Here, we theoretically demonstrate that both of the valley-selective high harmonic generation and valley-selective electronic excitation can be achieved by using an orthogonal two-color (OTC) laser field in gapped graphene. It is shown that the asymmetry degrees of harmonic yields in the plateaus, cutoff energies of generated harmonics and electron populations from two different valleys can be precisely controlled by the relative phase of the OTC laser field. Thus, the selectivity of the dominant valley for the harmonic radiation and electronic polarization can be switched by adjusting the relative phase of the OTC laser field. Our work offers an all-optical route to produce the valley-resolved high harmonic emissions and manipulate the ultrafast valley polarization on a femtosecond timescale in condensed matter.

Disorder-induced effects in high-harmonic generation process in fullerene molecules

The objective of this article is to investigate the profound nonlinear optical response exhibited by inversion symmetric fullerene molecules under the influence of different types of disorders described by the Anderson model. Our aim is to elucidate the localization effects on the spectra of high harmonic generation in such molecules. We show that the disorder-induced effects are imprinted onto molecules’ high-harmonic spectrum. Specifically, we observe a presence of strong even-order harmonic signals already for relatively small disorders. The odd-order harmonics intrinsic for disorder-free systems are generally robust to minor disorders. Both diagonal and off-diagonal disorders lift the degeneracy of states, opening up new channels for interband transitions, leading to the enhancement of the high-harmonic emission. The second harmonic signal has a special behavior depending on the disorder strength. Specifically in the case of diagonal disorder, the second harmonic intensity exhibits a quadratic scaling with the disorder strength, which enables the usage of the harmonic spectrum as a tool in measuring the type and the strength of a disorder.

Noncollinear antiferromagnetic textures driven high-harmonic generation from magnetic dynamics in the absence of spin-orbit coupling

We demonstrate the generation of high order harmonics in carrier pumping from precessing ferromagnetic or antiferromagnetic orders, excited via magnetic resonance, in the presence of topological antiferromagnetic textures. This results in an enhancement of the carrier dynamics by orders of magnitude, enabling for an emission deep in the THz frequency range. Interestingly, the generation process occurs in an intrinsic manner, and is solely governed by the interplay between the s-d exchange coupling underlying the noncollinear antiferromagnetic order and the dynamical s-d exchange constant of the magnetic drive. Therefore, the relativistic spin–orbit interaction is not required for the emergence of high harmonics in the pumped currents. Accordingly, the noncollinear topological antiferromagnetic order is presented as an alternative to spin–orbit interaction for the purpose of harnessing high harmonic emission in carrier pumping. Furthermore, we demonstrate the emergence of high harmonics from random magnetic impurities. This suggests the universality of the magnetically induced high harmonic emission in the presence of real and/or momentum space noncollinear textures. Our proposal initiates a tantalizing prospect for the utilization of topological textures in the context of the highly active domains of ultrafast spintronics and THz emission.

High-harmonic generation from artificially stacked 2D crystals

Abstract We report a coherent layer-by-layer build-up of high-order harmonic generation (HHG) in artificially stacked transition metal dichalcogenides (TMDC) crystals in their various stacking configurations. In the experiments, millimeter-sized single crystalline monolayers are synthesized using the gold foil-exfoliation method, followed by artificially stacking on a transparent substrate. High-order harmonics up to the 19th order are generated by the interaction with a mid-infrared (MIR) driving laser. We find that the generation is sensitive to both the number of layers and their relative orientation. For AAAA stacking configuration, both odd- and even-orders exhibit a quadratic increase in intensity as a function of the number of layers, which is a signature of constructive interference of high-harmonic emission from successive layers. Particularly, we observe some deviations from this scaling at photon energies above the bandgap, which is explained by self-absorption effects. For AB and ABAB stacking, even-order harmonics remain below the detection level, consistent with the presence of inversion symmetry. Our study confirms our capability of producing nonperturbative high-order harmonics from stacked layered materials subjected to intense MIR fields without damaging samples. Our results have implications for optimizing solid-state HHG sources at the nanoscale and developing high-harmonics as an ultrafast probe of artificially stacked layered materials. Because the HHG process is a strong-field driven process, it has the potential to probe high-momentum and energy states in the bandstructure combined with atomic-scale sensitivity in real space, making it an attractive probe of novel material structures such as the Moiré pattern.

Real-Time Observation of Electron-Hole Coherence Induced by Strong-Field Ionization

We introduce and demonstrate a new approach to measure the electron-hole dynamics and coherence induced by strong-field ionization using hole-assisted high-harmonic spectroscopy. The coherent driving of the infrared and XUV pulses correlates the dynamics of the core-hole and the valence-hole by coupling multiple continua, which leads to the otherwise forbidden absorption and emission of high harmonics. An analytical model is developed based on the strong-field approximation by taking into account the essential multielectron configurations. The emission spectra from the core-valence transition and the core-hole recombination are found to modulate strongly as functions of the time delay between the two pulses, suggesting that the coherent electron wave packets in multiple continua can be utilized to temporally resolve the core-valence transition in attoseconds.

Deep learning and high harmonic generation

Using machine learning, we explore the utility of various deep neural networks when applied to high harmonic generation scenarios. First, we train the neural networks to predict the time-dependent dipoles and spectra of high harmonic emission from reduced-dimensionality models of di- and triatomic systems based on sets of randomly generated parameters (laser pulse intensity, internuclear distance, and molecular orientation). These networks, once trained, are useful tools to rapidly simulate the high harmonic spectra of our systems. Similarly, we have trained the neural networks to solve the inverse problem—to determine the molecular parameters based on high harmonic spectra or dipole acceleration data. The latter types of networks could then be used as spectroscopic tools to invert high harmonic spectra in order to recover the underlying physical parameters of a system. Next, we demonstrate that transfer learning can be applied to our networks to expand the range of applicability of the networks with only a small number of new test cases added to our training sets. Finally, we demonstrate neural networks that can be used to classify molecules by type: di- or triatomic, symmetric or asymmetric. With outlooks toward training with experimental data, these neural network topologies offer a novel set of spectroscopic tools that could be incorporated into high harmonic generation experiments.

Spin-orbit coupling induced ultrahigh-harmonic generation from magnetic dynamics

The recent boost in data transfer rates puts a daring strain on information technology. Sustaining such a growth rate requires the development of sources, detectors and systems working in the so-called TeraHertz (THz) gap covering the frequency window from 0.1 to 10 THz (1 THz = 10$^{12}$~Hz). This gap represents a challenge for conventional electronic devices due to carrier transit delays ($\sim$1-10ps), as well as for photonic devices due to thermal fluctuations (300K$\sim$6THz). Nonetheless, designing efficient, room-temperature THz sources would constitute a key enabler to applications spanning from high-resolution imaging to extreme wide band wireless communication. Whereas high-harmonic generation in solid is usually limited to less than ten harmonics, broadband THz emission has been demonstrated using laser-induced superdiffusive spin currents in magnetic bilayers composed of a ferromagnet deposited on top of a noble metal. While promising, this technique presents the major disadvantage of necessitating optical pumping and hence lacks scalability. Here, we demonstrate that extremely high harmonic emission can be achieved by exploiting conventional spin pumping, without the need of optical excitation. We show that when the spin-orbit coupling strength is close to the s-d exchange energy, a strongly non linear regime resulting from resonant spin flip scattering occurs leading to the generation of a thousand of harmonics at realistic antiferromagnetic precession frequencies, thereby enhancing both spin and charge dynamics by two orders of magnitude, and allowing for an emission at frequencies above 300 THz.

Intense Laser Pulse Interaction With Graphene and Graphene Ribbons.

In this work we investigate quantum mechanically the interaction of an intense ultrashort laser pulse with the graphene monolayer as well as with the armchair graphene ribbons of different widths. We consider a tight binding (TB) Hamiltonian of the monolayer graphene and give two rules for deriving the dispersion relations of the armchair graphene ribbons of any width, N, from the TB eigenvalues of the monolayer. The band structure of the monolayer and the armchair ribbons of different widths are discussed with illustrations. The time-dependent wavefunctions of the systems and the expectation values of interest are determined by solving the coupled equations of the band amplitudes “exactly” (numerically). First, simulations are made for the population excitation in the conduction band (CB) from the valence band (BV), the VB-CB interband correlation (or “coherence”), the intraband, the interband and the total currents in the monolayer graphene. The graphene currents are compared with the corresponding currents induced in an armchair ribbon (width, N = 3). The change from the 2D monolayer to the 1D ribbon shows a remarkable transition of the dominance of the intraband current that leads to a near steady total current in the monolayer, to a dominance of the interband current in the ribbon that induces an oscillatory current in the ribbon beyond the pulse duration. The difference observed might be a combined effect of the “confinement” in one dimention and a finite band-gap minimum in the case of the ribbon. However, this transition should be further investigated for better clarity. A brief comparison of the radiation spectra emitted from the monolayer and from the ribbon is also made. They show a grossly similar structure and a relative insensitivity with respect to the detailed structure of the targets chosen. This might be due to the dominance of virtual continuum-continuum transitions, to and from the bands states, that lie behind the fundamental quantum process of high harmonic emissions. Lastly, the dependence of the charge currents, induced in a ribbon of unit width (N = 1), on the carrier-envelope-phase (CEP) of the incident laser pulse is investigated. It is seen that the shape of the main part of the current produced in the ribbon can be fully reversed by changing the CEP of the ultrashort laser pulse from 0 to π. More generally, it is suggested that the pulse shape of the charge carriers in the ribbon could be designed by similarly tailoring the form of the vector potential of the incident laser pulse.

Bright High-Harmonic Generation through Coherent Synchrotron Emission Based on the Polarization Gating Scheme

Relativistic surface high harmonics, combined with the use of polarization gating, present a promising route towards intense single attosecond pulses. However, they impose stringent requirements on ultra-high laser contrast and are restricted by large intensity losses in real experiments. Here, we numerically demonstrate that by setting an optimal time delay in the polarization gating scheme, the intensity of the generated single attosecond pulses can become approximately 100 times stronger than that with nonoptimal time delay in the coherent synchrotron emission process. When a petawatt-class driving laser irradiates a solid target, an ultra-dense electron nanobunch and a strong space-charge sheath develop, and the accumulated electrostatic energy is only released in half of the laser cycle when this electron nanobunch moves backward. This process results in the emission of intense high harmonics. Our study provides a reliable method for developing bright attosecond extreme ultraviolet pulses.

Multi-beam vortex generation induced by the non-linear optical anisotropy of graphene

We analyse the high harmonic emission from single-layer graphene driven by infrared vector beams. We demonstrate that graphene’s anisotropy offers a privileged scenario to explore non-trivial light spin-orbit couplings, which substantially extends the possibilities for the generation of high-harmonic structured beams currently studied in atomic and molecular targets. In our case, graphene’s crystal symmetry introduces a spin-dependent diffraction pattern that, coupled with the fundamental conservation of the driver’s topological phase, leads to the splitting of the harmonic field in a multi-beam structure, composed of spatially diverging vortices. Our work demonstrates that anisotropic targets are extraordinary tools to sculpt complex structured short-wavelength beams.

Influence of driving-laser wavelength on emission of high-order harmonic wave generated by atoms irradiated by ultrashort laser pulse

With the numerical solution of the time-dependent Schrodinger equation, we theoretically investigate the high-order harmonic emissions generated by the atoms irradiated by the ultrashort lasers with different wavelengths but the same pondermotive energy. As the driving-laser wavelength increases, the intensity of the high-harmonic emission decreases. Comparing with the harmonic spectra of atoms driven by a 1000-nm-wavelength laser pulse, a new peak structure appears in the spectra of atoms driven by a 5000-nm-wavelength laser wavelength. It is shown by the time-frequency analysis of the harmonic emission, the time-dependent evolution of the electron density, and the time-dependent population analysis of the eigenstate, that the physical mechanism behind the new peak appearing in the harmonic spectra is the interference between the harmonic emission generated by the electrons ionized out of the excited atoms returning to the parent ions and the harmonic emissions resulting from the ground state ionization.

Attosecond Delays of High-Harmonic Emissions from Hydrogen Isotopes Measured by XUV Interferometer

High-harmonic spectroscopy can access structural and dynamical information on molecular systems encoded in the amplitude and phase of high-harmonic generation (HHG) signals. However, measurement of the harmonic phase is a daunting task. Here, we present a precise measurement of HHG phase difference between two isotopes of molecular hydrogen using the advanced extreme-ultraviolet (XUV) Gouy phase interferometer. The measured phase difference is about 200 mrad, corresponding to ~3 attoseconds ( 1 as = 10 − 18 s ) time delay which is nearly independent of harmonic order. The measurements agree very well with numerical calculations of a four-dimensional time-dependent Schödinger equation. Numerical simulations also reveal the effects of molecular orientation and intramolecular two-center interference on the measured phase difference. This technique opens a new avenue for measuring the phase of harmonic emission for different atoms and molecules. Together with isomeric or isotopic comparisons, it also enables the observation of subtle effects of molecular structures and nuclear motion on electron dynamics in strong laser fields.