Polarized Laser Pulses Research Articles

Phototransformation of achiral metasurfaces into handedness-selectable transient chiral media

Chirality is a geometric property describing the lack of mirror symmetry. This unique feature enables photonic spin-selectivity in light-matter interaction, which is of great significance in stereochemistry, drug development, quantum optics, and optical polarization control. The versatile control of optical geometry renders optical metamaterials as an effective platform for engineered chiral properties at prescribed spectral regimes. Unfortunately, geometry-imposed restrictions only allow one circular polarization state of photons to effectively interact with chiral meta-structures. This limitation motivates the idea of discovering alternative techniques for dynamically reconfiguring the chiroptical responses of metamaterials in a fast and facile manner. Here, we demonstrate an approach that enables optical, sub-picosecond conversion of achiral meta-structures to transient chiral media in the visible regime with desired handedness upon the inhomogeneous generation of plasmonic hot electrons. As a proof of concept, we utilize linearly polarized laser pulse to demonstrate near-complete conversion of spin sensitivity in an achiral meta-platform-a functionality yet achieved in a non-mechanical fashion. Owing to the generation, diffusion, and relaxation dynamics of hot electrons, the demonstrated technique for all-optical creation of chirality is inherently fast, opening new avenues for ultrafast spectro-temporal construction of chiral platforms with on-demand spin-selectivity.

Quasi-monoenergetic heavy ion acceleration driven by sub-100 PW linearly polarized laser pulses in the radiation-dominated QED regime

Heavy ion acceleration from an ultrathin foil target irradiated by a p-polarized and spatially Gaussian laser pulse at intensity of 1023 W/cm2 is studied by using two-dimensional particle-in-cell simulations. We find that, in the extremely intense laser fields, the radiation reaction force from bright γ-rays radiated by radially oscillating electrons is large enough to match the Coulomb explosive force of foil electrons. The undesirable transverse expansion of the foil from the electron heating and inhomogeneous radial profile of the laser intensity is effectively suppressed. The foil maintains relatively good opacity in its central region stabilizing localized acceleration of heavy ions. With a laser of intensity 3.4 × 1023 W/cm2, duration of 33 fs, and power of 96 PW, a dense monoenergetic Au79+ ion bunch with a peak energy of ∼160 GeV can be obtained in the radiation-dominated QED regime. Such a high-quality heavy ion beam is useful for investigating nuclear matter equation of state and quantum chromodynamic phase transition in intermediate-energy heavy ion collisions.

Ultrafast Chiral Precession of Spin and Orbital Angular Momentum Induced by Circularly Polarized Laser Pulse in Elementary Ferromagnets.

Despite spin (SAM) and orbital (OAM) angular momentum dynamics being well-studied in demagnetization processes, their components receive less focus. Here, we utilize real-time time-dependent density functional theory (rt-TDDFT) to unveil significant x and y components of SAM and OAM induced by circularly left (σ+) and right (σ-) polarized laser pulses in ferromagnetic Fe, Co, and Ni. Our results show that the magnitude of the OAM is an order of magnitude larger than that of the SAM, highlighting a stronger optical response from the orbital degrees of freedom of electrons. Intriguingly, σ+ and σ- pulses induce chirality in the precession of SAM and OAM, respectively, with clear associations with laser frequency and duration. Finally, we demonstrate the time scale of the OAM and SAM precession occurs even earlier than that of the demagnetization process and the OISTR effect. Our results provide detailed insight into the dynamics of SAM and OAM during and shortly after a polarized laser pulse.

Simulations of the correlated momentum distributions for nonsequential double ionization of neon in elliptically polarized laser fields

We use the improved quantitative rescattering (QRS) model to simulate the experimentally measured correlated two-electron momentum distributions (CMDs) for nonsequential double ionization (NSDI) of Ne exposed to intense elliptically polarized laser pulses with a central wavelength of 788 nm at a peak intensity of 5 ×1014 W cm−2 for the ellipticities ranging from 0 to 0.25 (Kang et al 2018 Phys. Rev. A 97 063403). Only the CMDs for recollision direct ionization are calculated and the contribution from recollision excitation with subsequent ionization is ignored. With the assumption that recollisions occur after the zero crossing of the electric field along the major polarization, the QRS model successfully reproduces the experimentally observed asymmetry pattern of electron pairs in the CMDs for NSDI of Ne under elliptical polarization. By reducing the peak intensity claimed in experiment by about 30%, good agreement is achieved between the present results and the experimental measurements.

Investigation of deterministic and cumulative nature in helicity-dependent optical switching of ferrimagnetic Gd–Fe–Co films

The precise control of magnetization using circularly polarized laser pulses in perpendicularly magnetized films is a key approach to develop storage media. Although deterministic helicity-dependent magnetization switching (HDMS) in a single-pulse excitation has been observed in ferrimagnetic Gd–Fe–Co alloys, ferromagnetic [Co/Pt]N multilayers require cumulative effects of multiple pulses to achieve HDMS. In this study, we systematically investigated the single-shot and cumulative nature of HDMS using ferrimagnetic Gd–Fe–Co films with varying compositions and multilayer structures, in terms of angular momentum compensation, thermal diffusion, mobility of domain walls, and the size of the magneto-optical effect. These results provide insights for the realization of single-shot HDMS in various magnetic systems, such as ferromagnetic alloys.

Laser-Induced Electron Diffraction in Chiral Molecules

Strong laser pulses enable probing molecules with their own electrons. The oscillating electric field tears electrons off a molecule, accelerates them, and drives them back toward their parent ion within a few femtoseconds. The electrons are then diffracted by the molecular potential, encoding its structure and dynamics with angstrom and attosecond resolutions. Using elliptically polarized laser pulses, we show that laser-induced electron diffraction is sensitive to the chirality of the target. The field selectively ionizes molecules of a given orientation and drives the electrons along different sets of trajectories, leading them to recollide from different directions. Depending on the handedness of the molecule, the electrons are preferentially diffracted forward or backward along the light propagation axis. This asymmetry, reaching several percent, can be reversed for electrons recolliding from two ends of the molecule. The chiral sensitivity of laser-induced electron diffraction opens a new path to resolve ultrafast chiral dynamics. Published by the American Physical Society 2024

Control of Frustrated Nonsequential Double Ionization Channels With the Carrier-Envelope Phase of Elliptically Polarized Laser Pulses

Abstract Using a classical approach, we theoretically investigate the frustrated double ionization (FDI) of Ar atoms under elliptically polarized (EP) laser fields. The FDI yield is calculated as a function of laser intensity with different carrier-envelope phases (CEPs), and, similar to the carrier-envelope phase (CEP) dependence of nonsequential double ionization (NSDI), several knee-shaped structures appear. Moreover, both recollision and direct ionization trajectories are observed in FDI events for the “knee” structure regime. The footprints of which channel leads to FDI are encoded in the photoelectron momentum distributions. FDI events related to recollision excitation with subsequent ionization channels and recollision impact ionization channels can be controlled by CEP in EP laser fields.

Intense mid-infrared laser pulse generated via flying-mirror red-shifting in near-critical-density plasmas

Abstract Relativistic femtosecond mid-infrared pulses can be generated efficiently by laser interaction with near-critical-density plasmas. It is found theoretically and numerically that the radiation pressure of a circularly polarized laser pulse first compresses the plasma electrons to form a dense flying mirror with a relativistic high speed. The pulse reflected by the mirror is red-shifted to the mid-infrared range. Full three-dimensional simulations demonstrate that the central wavelength of the mid-infrared pulse is tunable from 3 $\rm{\mu m}$ to 14 $\rm{\mu m}$ and the laser energy conversion efficiency can reach as high as 13%. With a 0.5-10 PW incident laser pulse, the generated mid-infrared pulse reaches a peak power of 10-180 TW, which could be interesting for various applications in ultrafast and high-field sciences.

From chiral laser pulses to femto- and attosecond electronic chirality flips in achiral molecules

Chirality is an important topic in biology, chemistry and physics. Here we show that ultrashort circularly polarized laser pulses, which are chiral, can be fired on achiral oriented molecules to induce chirality in their electronic densities, with chirality flips within femtoseconds or even attoseconds. Our results, obtained by quantum dynamics simulations, use the fact that laser pulses can break electronic symmetry while conserving nuclear symmetry. Here two laser pulses generate a superposition of three electronic eigenstates. This breaks all symmetry elements of the electronic density, making it chiral except at the periodic rare events of the chirality flips. As possible applications, we propose the combination of the electronic chirality flips with Chiral Induced Spin Selectivity.

Dephasing Dynamics Accessed by High Harmonic Generation: Determination of Electron-Hole Decoherence of Dirac Fermions.

We reveal the critical effect of ultrashort dephasing on the polarization of high harmonic generation in Dirac fermions. As the elliptically polarized laser pulse falls in or slightly beyond the multiphoton regime, the elliptically polarized high harmonic generation is produced and exhibits a characteristic polarimetry of the polarization ellipse, which is found to depend on the decoherence time T2. T2 could then be determined to be a few femtoseconds directly from the experimentally observed polarimetry of high harmonics. This shows a sharp contrast with the semimetal regime of higher pump intensity, where the polarimetry is irrelevant to T2. An access to the dephasing dynamics would extend the prospect of high harmonic generation into the metrology of a femtosecond dynamic process in the coherent quantum control.

Vortex γ photon generation via spin-to-orbital angular momentum transfer in nonlinear Compton scattering

Vortex γ photons with intrinsic orbital angular momenta possess a wealth of applications in various fields—e.g., strong-laser physics, nuclear physics, particle physics, and astrophysics—yet their generation remains unsettled. In this work, we investigate the generation of vortex γ photons via nonlinear Compton scattering of ultrarelativistic electrons in a circularly polarized laser pulse. We develop a quantum electrodynamics scattering theory that explicitly addresses the multiphoton absorption and the angular momentum transfer mechanism. In pulsed laser fields, we unveil the vortex phase structure of the scattering matrix element, discuss how the vortex phase could be transferred to the radiated photon, and derive the radiation rate of the vortex γ photon. We numerically examine the energy spectra and beam characteristics of the radiation, while also investigating the influence of finite laser pulses on the angular momentum and energy distribution of the emitted vortex γ photons. Published by the American Physical Society 2024

Electron vortex generations in photoionization of hydrogen atoms by circularly-polarized chirped attosecond pulses

By numerically solving the time-dependent Schrödinger equation and employing the analytical perturbative model, we investigated the chirp-induced electron vortex in the photoionization of hydrogen atoms by a pair of counter-rotating circularly polarized chirped attosecond extremely ultraviolet pulses. We demonstrated that single-photon ionization of hydrogen atoms generates photoelectron momentum distributions (PMDs) with distinct helical vortex structures either with or without a time delay between two counter-rotating circularly polarized laser pulses. These structures are highly sensitive to both the time delay between the pulses and their chirp parameters. Our analytical model reveals that the splitting of vortex spirals is caused by the sign changing of the chirp-induced frequency-dependent time delay. We showed that to obtain the counterpart of the PMD under a pair of counter-rotating circularly polarized chirped pulses, both chirp parameters and ordering of pulses need to be reversed.

Conversion efficiency by circularly polarized laser pulse with two different spin states in magnetized quantum plasma

Conversion efficiency by circularly polarized laser pulse with two different spin states in magnetized quantum plasma

Ultrafast magnetic field induced by anisotropy in carbon nanotubes irradiated by intense laser fields

We report an unexpected result of the anisotropy of the nonlinear optical response of carbon nanotubes, inherent to their chirality. Using a model based on the resolution of the semiconductor Bloch equations, we theoretically demonstrate that, upon irradiation with an intense linearly polarized laser pulse along the axial direction, chiral nanotubes exhibit an oscillating azimuthal current that is absent in achiral species. This current induces a magnetic field parallel to the axis of the nanotube that radiates like a loop antenna.

Modulation of High-Order Harmonic Generation from a Monolayer ZnO by Co-rotating Two-Color Circularly Polarized Laser Fields

By numerically solving the two-dimensional semiconductor Bloch equation, we study the high-order harmonic emission of a monolayer ZnO under the driving of co-rotating two-color circularly polarized laser pulses. By changing the relative phase between the fundamental frequency field and the second one, it is found that the harmonic intensity in the platform region can be significantly modulated. In the higher order, the harmonic intensity can be increased by about one order of magnitude. Through time-frequency analysis, it is demonstrated that the emission trajectory of monolayer ZnO can be controlled by the relative phase, and the harmonic enhancement is caused by the second quantum trajectory with the higher emission probability. In addition, near-circularly polarized harmonics can be generated in the co-rotating two-color circularly polarized fields. With the change of the relative phase, the harmonics in the platform region can be altered from left-handed near-circularly polarization to right-handed one. Our results can obtain high-intensity harmonic radiation with an adjustable ellipticity, which provides an opportunity for syntheses of circularly polarized attosecond pulses.

Highly Collimated Monochromatic X-rays Generated by Collision of High-Energy Electrons with Tightly Focused Linearly Polarized Laser Pulse

This article delves into the generation and modulation process of X-rays as high-energy photon sources. Using the principles of classical electrodynamics, this study enables nonrelativistic short pulse lasers to collide with high-energy electrons while the collision center is away from the focal point. This scattering method may produce X-rays with good collimation and monochromaticity, and it progressively approaches inverse Thomson scattering. We studied and analyzed the effects of different electron characteristics and laser parameter settings on the high-energy angular distribution and spectrum of X-rays, especially the setting of the collision center and initial electron velocity, as well as the setting of laser intensity and pulse width. Linear polarized laser pulses with relativistic intensity can generate discrete supercontinuum X-rays with spectral distortion. In addition, the relationships between electronic and laser properties and radiation energy were also studied. Our research can provide valuable insights for manipulating collimated or distorted, monochromatic, or tunable X-rays, as well as understanding their properties.

Effect of wiggler magnetic field on wakefield excitation and electron energy gain in laser wakefield acceleration

Abstract Laser wakefield acceleration is a frequently utilised research methodology for enhancing the energy levels of lighter charged particles, specifically electrons, to relativistic magnitudes. In this investigation, we utilised a linear polarised Gaussian-like laser pulse that propagated along the z-axis through cold collisionless underdense plasma in weakly nonlinear regime. An external planer magnetic wiggler field is applied along the y-axis. The influence of various critical parameters, such as amplitude and propagation constant of wiggler magnetic field, amplitude of laser electric field and laser pulse length on the wakefield and electron energy gain has been studied. A wiggler-assisted laser wakefield accelerator, the electron energy and wakefield evolution can be tuned by the wiggler magnetic field strength. The numerical findings demonstrate that by varying the strength of wiggler magnetic field and laser electric field, the amplitude of the wakefield is affected significantly. Furthermore, the equality of the order of pulse length and plasma wavelength is essential to obtain energy efficient acceleration mechanism. By employing specific parameters, a maximum energy increase of 2.26 GeV is achieved. This research will aid in the development of an energy-efficient electron acceleration technology by choosing suitable laser and plasma parameters.

Light-Shaping of Valley States.

The established paradigm to create valley states, excitations at local band extrema ("valleys"), is through selective occupation of specific valleys via circularly polarized laser pulses. Here we show a second way exists to create valley states, not by valley population imbalance but by "light-shaping" in momentum space, i.e. controlling the shape of the distribution of excited charge at each valley. While noncontrasting in valley charge, such valley states are instead characterized by a valley current, identically zero at one valley and finite and large at the other. We demonstrate that these (i) are robust to quantum decoherence, (ii) allow lossless toggling of the valley state with successive femtosecond laser pulses, and (iii) permit valley contrasting excitation both with and without a gap. Our findings open a route to robust ultrafast and switchable valleytronics in a wide scope of 2d materials, bringing closer the promise of valley-based electronics.

Tunable Tesla-Scale Magnetic Attosecond Pulses through Ring-Current Gating.

Coherent control over electron dynamics in atoms and molecules using high-intensity circularly polarized laser pulses gives rise to current loops, resulting in the emission of magnetic fields. We propose, and demonstrate with ab initio calculations, "current-gating" schemes to generate direct or alternating-current magnetic pulses in the infrared spectral region, with highly tunable waveform and frequency, and showing femtosecond-to-attosecond pulse duration. In optimal conditions, the magnetic pulse can be highly isolated from the driving laser and exhibits a high flux density (∼1 T at a few hundred nanometers from the source, with a pulse duration of 787 attoseconds) for application in forefront experiments of ultrafast spectroscopy. Our work paves the way toward the generation of attosecond magnetic fields to probe ultrafast magnetization, chiral responses, and spin dynamics.

Single Shot Generation of High‐Aspect‐Ratio Nano‐Rods from Sapphire by Ultrafast First Order Bessel Beam

AbstractEngineering the polarization and spatial phase of ultrafast laser pulses represents a compelling strategy for enhancing control over laser–matter interaction and enabling rapid and innovative nano‐fabrication processes. Here, the single‐shot, ultrafast laser fabrication of high‐aspect‐ratio, vertically standing nano‐pillars with a diameter of nm and height up to 15 µm on the surface of sapphire, is reported. To achieve this, the distinctive properties of diffraction‐free, first‐order Bessel beams endowed with either radial or azimuthal polarization distributions, are harnessed under tight focusing conditions. The highly intense laser–matter interaction in this configuration generates a tubular‐shaped, high‐pressure field beneath the material surface, leading to the rapid expulsion of material across the surface. Three distinct regimes for the pillar generation are identified in addition to a mechanism based on the Rayleigh‐Plateau theory that explains the distinct morphological regimes observed. The findings not only shed light on the underlying physical mechanisms of intense excitation of transparent dielectrics but also offer exciting prospects for the rapid fabrication of positive nano‐structures and material compression across various fields of application.