Ellipticity Dependence Research Articles

Dependence of high-harmonic generation in twisted bilayer graphene on laser pulse ellipticity

The ellipticity of a laser pulse offers a control knob to tune the efficiency and polarization of emitted higher-order harmonics. In this paper, we systematically investigate the ellipticity dependence of high-harmonic generation in various bilayer graphene systems, such as AA-stacked, AB-stacked, and twisted bilayer graphene. We demonstrate how the underlying symmetries and electronic band structures of different bilayer systems distinctly contribute to the characteristics of ellipticity dependence, such as elliptical enhancement and elliptical dichroism. Additionally, we showcase a unique applicability of high-harmonic spectroscopy as a tool for identifying stacking faults in bilayer graphene systems. Our findings offer valuable insights into the nonlinear optical interactions of twisted bilayer graphene with different twist angles. Published by the American Physical Society 2024

Effect of light ellipticity and polarization angle on the transient dynamics of the ground-state Hanle effect

We report theoretical investigations on the transient dynamics of the ground-state Hanle effect in the Voigt geometry, where a time-varying scanning magnetic field B (t) is applied perpendicular to the light propagation direction. Transient Hanle signals are calculated for different light polarizations using a theoretical model based on the density matrix approach. First, we study the ellipticity dependence of transient Hanle signals in two configurations in which the major axis of the light polarization ellipse () is aligned either perpendicular or parallel to the field B . For B , elliptical polarization of the light produces oscillations of frequencies 2ΩL(t) and ΩL(t) simultaneously, where ΩL(t) is the Larmor frequency of the corresponding field B (t). On the other hand, in the case of || B , only ΩL(t) oscillation is observed using elliptically polarized light. Second, we vary the tilt angle between the polarization vector of a linearly polarized light and the orientation of the field B and study its effect on the transient response of Hanle signals. Both the amplitude and the decay rate of the oscillations show a strong dependence on the light ellipticity and tilt angle of the polarization vector. In addition, the influence of the magnetic field sweep rate on the transient signals is demonstrated for given values of light ellipticity and polarization angle.

Effects of initial electronic state on elliptically polarized attosecond pulses

We investigate the ellipticity dependence of the high-order harmonic generation from molecular hydrogen ions with different initial states ( and ). The ellipticity of the harmonics can be tuned and is more sensitive to the alignment angle with the ground state. The position of the maximum ellipticity shifts with the increase of the alignment angles, which can be illustrated by the two-center interference model and molecular orbital symmetry. The underlying physical mechanisms of the ellipticity can be demonstrated by the phase difference and amplitude difference of the x and y components of the harmonics. In addition, with specific carrier envelope phase of the laser fields, the elliptically polarized attosecond pulse with high intensity and large ellipticity ɛ = 0.77 is synthesized from the first excited state, which can be used as the bright elliptically polarized EUV light source.

Roles of laser ellipticity in attoclocks

We study ionization of atoms in strong elliptically polarized laser fields numerically and analytically. We focus on the effects of laser ellipticity on the offset angle in the photoelectron momentum distribution. This angle is considered to encode the time information of tunneling ionization in attoclock experiments. The calculated offset angle increases with the decrease of ellipticity, but the momentum along the major axis of laser polarization related to this angle changes slowly, in agreement with experiments. With a Coulomb-included strong-field model, the scaling laws for the ellipticity dependence of this angle and relevant momentum components are obtained, and the ellipticity dependence of Coulomb-induced ionization time lag encoded in this angle is also addressed.

The ellipticity dependence of Rydberg state excitation of noble gas atoms subject to strong laser fields

In this work, we theoretically investigate the ellipticity dependence of the Rydberg state excitation (RSE) and ionization of noble gas atoms subject to strong laser fields at a series of intensities and wavelengthes by a semiclassical model, where the nonadiabtic effect is considered or ignored. Our results demonstrate that, if the nonadiabatic effect has been ignored, the ratio between RSE and ionization yields exhibits an anomalous maximum at a nonzero ellipticity. On the other hand, if the nonadiabatic effect has been considered, this anomalous behavior disappears. The analysis indicates that the absence of this anomalous behavior can be attributed to the nonadiabatic corrections of instantaneous ionization rate and the initial photoelectron momentum distribution at the tunnel exit.

Ellipticity dependence of anticorrelation in the nonsequential double ionization of Ar.

Within the framework of the improved quantitative rescattering (QRS) model, we simulate the correlated two-electron momentum distributions (CMDs) for nonsequential double ionization (NSDI) of Ar by elliptically polarized laser pulses with a wavelength of 788 nm at an intensity of 0.7 × 1014 W/cm2 for the ellipticities ranging from 0 to 0.3. Only the CMDs for recollision excitation with subsequent ionization (RESI) are calculated and the contribution from recollision direct ionization is neglected. According to the QRS model, the CMD for RESI can be factorized as a product of the parallel momentum distribution (PMD) for the first released electron after recollision and the PMD for the second electron ionized from an excited state of the parent ion. The PMD for the first electron is obtained from the laser-free differential cross sections for electron impact excitation of Ar+ calculated using state-of-the-art many-electron R-matrix theory while that for the second electron is evaluated by solving the time-dependent Schrödinger equation. The results show that the CMDs for all the ellipticities considered here exhibit distinct anticorrelated back-to-back emission of the electrons along the major polarization direction, and the anticorrelation is more pronounced with increasing ellipticity. It is found that anticorrelation is attributed to the pattern of the PMD for the second electron ionized from the excited state that, in turn, is caused by the delayed recollision time with respect to the instant of the external field crossing. Our work shows that both the ionization potential of the excited parent ion and the laser intensity play important roles in the process.

Wavelength- and ellipticity-dependent photoelectron spectra from multiphoton ionization of atoms

We theoretically study the photoelectron momentum distributions from multiphoton ionization of a model lithium atom over a range of laser wavelengths from 500 nm to 700 nm by numerically solving the time-dependent Schrödinger equation. The photoelectron momentum distributions display many ring-like patterns for the three-photon ionization, which vary dramatically with the change of the laser wavelength. We show that the wavelength-dependent photoelectron energy spectrum can be used to effectively identify the resonant and nonresonant ionization pathways. We also find an abnormal ellipticity dependence of the electron yield for the (2+1) resonance-enhanced ionization via the 4d intermediate state, which is relevant to the two-photon excitation probability from the ground state to the 4d state.

Orientation dependence of even-order harmonics generation in biased bilayer graphene

We theoretically study the orientation dependence of even-order harmonics in biased bilayer graphene (BLG) by numerically solving the semiconductor Bloch equations in the velocity gauge. It is shown that the yield of even-order harmonics has a perfect periodicity of ${60}^{\ensuremath{\circ}}$ with the rotation of the crystal orientation. The even-harmonic intensity reaches the maximum when the laser field is polarized along with the nearest-neighbor atom. By investigating the crystal orientation dependence for the parallel and perpendicular components of even harmonics, it is found that the Berry curvature plays an insignificant role in the even-harmonic generation of biased BLG. Further analysis reveals that the asymmetric electron density between in-plane adjacent atoms caused by polarization is responsible for the generation of even harmonics in biased BLG. Additionally, we study the ellipticity dependence of even harmonics in biased BLG when the elliptical principal axis of the laser pulse is along with the in-plane nearest-neighbor atoms. As expected, the yield of even harmonics decreases with the ellipticity. Our findings give access to understanding deeply the mechanism of the orientation dependence of even harmonics in biased BLG.

High-order harmonic generation in an x-ray range from laser-induced multivalent ions of noble gas

Tabletop coherent x-ray sources extending to multi-keV or higher photon energies have versatile applications, including in 4D imaging and semiconductor detectors. However, these sources can be realized only via high-order harmonic generation (HHG) with an ∼ 10 µ m laser interacting with neutral atoms. As shown in previous work by Popmintchev et al. [Science 350, 1225 (2015)10.1126/science.aac9755SCIEAS0036-8075], multiply ionized plasmas can efficiently produce hundred-eV harmonics with an ultraviolet laser. Here, we experimentally investigate multi-keV x-ray sources up to ∼ 5.2 k e V , the highest photon energy generated via HHG to date, to our knowledge, using a 1.45-µm driving laser that interacts with multivalent ions. Both the angular distribution and the ellipticity dependence of the signal are strong evidence of the HHG mechanism.

Ellipticity dependence of high-order harmonic generation in disordered semiconductors

We analyze the ellipticity dependence of high order harmonic generation (HHG) in disordered semiconductors. We show that a disordered crystal can radiated HHG spectra containing only odd harmonics of the laser frequency for all values of the ellipticity of the laser. Furthermore, we show that the HHG yield of our disordered models decreases monotonically with increasing laser ellipticity as observed in recent experiments. I particular, our numerical calculations, based on a coarse grained model, reproduce many of the qualitative features of the experimental HHG spectra of ZnO and GaAs.

Orientation and ellipticity dependence of high-order harmonic generation in nanowires

It has been predicted that high-order harmonic generation (HHG) in nanowires has the potential to scale up photon energy and harmonic yield. However, studies on HHG in nanowires are still theoretical and no relevant experimental results have been reported as yet. Our experimental observation of the high-order harmonic in cadmium sulfide nanowires (CdS NWs) excited by a mid-infrared laser is, to our knowledge, the first of such study, and it verifies some of the theoretical results. Our experimental results show that the observed harmonics are strongest when a pump laser is parallel to the nanowires. Therefore, the theoretical prediction that harmonics are strongest under the nanowires parallel to the laser field is confirmed experimentally, and this can be used to determine the orientation of the nanowire. In addition, harmonics are sensitive to the variation of pump light ellipticities. This orientation dependence opens new opportunities to access the ultrafast and strong-field physics of nanowires.

Semiclassical analysis of ellipticity dependence of harmonic yield in graphene

We theoretically investigate the ellipticity dependence of high-order harmonic generation in graphene driven by the midinfrared laser field. The ellipticity dependence of the harmonic yield in the experiment [N. Yoshikawa, T. Tamaya, and K. Tanaka, Science 356, 736 (2017)] is reproduced perfectly by solving the semiconductor Bloch equations in the Houston basis under the tight-binding approximation. Based on the semiclassical recollision model, it is found that the recollision distance of the electron-hole pair excited from the zone $0.5{\ensuremath{\omega}}_{0}\ensuremath{\leqslant}\mathrm{\ensuremath{\Delta}}E\ensuremath{\leqslant}2.5{\ensuremath{\omega}}_{0}$ instead of the Dirac points can reach a minimum value at finite ellipticity, which enhances the harmonic yield. In addition, the ellipticity dependence of harmonics can be controlled by varying the chemical potential of graphene. When the chemical potential is decreased to $\ensuremath{-}1.52\phantom{\rule{0.16em}{0ex}}\mathrm{eV}$, the ellipticity dependence of harmonics can transit into the normal behavior. This work uncovers the microscopic mechanism of the ellipticity dependence of the harmonics in graphene and constructs a clear physical picture to understand the unique ellipticity-dependent behaviors in graphene.

Relativistic photoionization with elliptically polarized laser fields in the ultraviolet region

We study relativistic effects in photoionization of a hydrogen atom exposed to an intense laser pulse of general ellipticity. The frequency of the laser pulse resides in the ultraviolet region. To this end, the semirelativistic approach introduced in Kjellsson Lindblom et al. [T. Kjellsson Lindblom, M. F\o{}rre, E. Lindroth, and S. Selst\o{}, Phys. Rev. Lett. 121, 253202 (2018)] is applied. We present in some detail how this approximation is derived from the Dirac equation for elliptically polarized light within the so-called long-wavelength approximation. The validity of the semirelativistic approach is confirmed by direct comparison with the solution of the Dirac equation. It is found that the total ionization yield depends very weakly on ellipticity in the case of ionization from the isotropic ground state. With the excited initial state $n=2$, $\ensuremath{\ell}={m}_{\ensuremath{\ell}}=1$; however, pronounced ellipticity dependence is seen---in particular at the stabilization peak. Albeit small, relativistic corrections to the ionization probabilities are found. The correction is found to be largest for linear polarization. While relativistic effects tend to reduce the total ionization probability for most intensities considered, we also report a slight relativistic enhancement at comparatively modest field strengths.

Orbital effects in strong-field Rydberg state excitation of N2, Ar, O2 and Xe

Rather than being freed to the continuum, the strong-field tunneled electrons can make a trajectory driven by the remaining laser fields and have certain probability to be captured by the high lying Rydberg states of the parent atoms or molecules. To explore the effect of molecular orbital on Rydberg state excitation, the ellipticity dependence of Rydberg state yields of N2 and O2 molecules are experimentally investigated using cold target recoil ion momentum spectroscopy and are compared with their counterpart atoms Ar and Xe with comparable ionization potentials. We found the generation probability of the neutral Rydberg fragment O2* was orders of magnitude higher than that of Xe* due to the butterfly-shaped highest occupied molecular orbital of O2. Meanwhile, our experimental and simulation results reveal that it is the initial momentum distribution (determined by the detailed characteristics of orbitals) that finally leads to the tendency that the Rydberg state yield of O2 (Ar) decreased slower than that obtained for Xe (N2) when the ellipticity of the excitation laser field is increased.

Anomalous ellipticity dependence of the generation of near-threshold harmonics in noble gases

We measured the ellipticity dependence of the harmonic yield of He, Ne, Ar, Kr, and Xe. It is found that the harmonic yield in general decreases monotonically with increasing laser ellipticity but anomalous dependence does occur for each atom for some harmonic orders. We found that the degree of anomaly is weakest in helium but is stronger for the heavier atoms. The anomaly also depends on laser intensity. To explain these features, we developed a quantum trajectory Monte Carlo (QTMC) model based on the quantum path integral theory to study high-order harmonic generation (HHG). The model includes the effect of Coulomb potential from the target ion, thus it is capable of calculating near-threshold harmonics quantitatively. This model reveals that the presence of Coulomb potential would generate orbiting trajectories which are responsible for the anomalous ellipticity dependence near the threshold.

Comparison study on atomic and molecular ellipticity dependence of high-order harmonic generation

We systematically investigate ellipticity dependence of high-order harmonic generation of Ar and ${\mathrm{N}}_{2}$ in intense elliptically polarized laser fields. The experimental normalized ratios of low-order harmonic intensity to high-order harmonic intensity increase with ellipticity for both Ar and ${\mathrm{N}}_{2}$, and quantitatively depend on targets and trajectory paths. The experimental results are well reproduced by a nonadiabatic semiclassical simulation and explained by trajectory-based analysis. In addition, the influence of nuclear distance on the ratios is theoretically investigated. Our work reveals that the difference between atoms and molecules can be attributed to the influence of different ionic potentials, which depends on the molecular structure (internuclear distance) and alignment, on the evolution of the photoelectron.

High-harmonic generation from monolayer and bilayer graphene

High-harmonic generation (HHG) in solids is an emerging method to probe ultrafast electron dynamics in solids at attosecond timescale. In this work, we study HHG from monolayer and bilayer graphene. Bilayer graphenes with AA and AB stacking are considered in this work. It is found that the monolayer and bilayer graphenes exhibit significantly different harmonic spectra. The difference in the spectra is attributed to the interlayer coupling between the two layers. Also, the intraband and interband contributions to the total harmonic spectrum play a significant role. Moreover, interesting polarization and ellipticity dependence are noticed in total harmonic spectrum for monolayer and bilayer graphene.

Polarization Dependent Excitation and High Harmonic Generation from Intense Mid-IR Laser Pulses in ZnO.

The generation of high order harmonics from femtosecond mid-IR laser pulses in ZnO has shown great potential to reveal new insight into the ultrafast electron dynamics on a few femtosecond timescale. In this work we report on the experimental investigation of photoluminescence and high-order harmonic generation (HHG) in a ZnO single crystal and polycrystalline thin film irradiated with intense femtosecond mid-IR laser pulses. The ellipticity dependence of the HHG process is experimentally studied up to the 17th harmonic order for various driving laser wavelengths in the spectral range 3–4 µm. Interband Zener tunneling is found to exhibit a significant excitation efficiency drop for circularly polarized strong-field pump pulses. For higher harmonics with energies larger than the bandgap, the measured ellipticity dependence can be quantitatively described by numerical simulations based on the density matrix equations. The ellipticity dependence of the below and above ZnO band gap harmonics as a function of the laser wavelength provides an efficient method for distinguishing the dominant HHG mechanism for different harmonic orders.

Ellipticity dependence of excitation and ionization of argon atoms by short-pulse infrared radiation

When atoms or molecules are exposed to strong short-pulse infrared radiation, ionization as well as "frustrated tunneling ionization" (FTI) can occur, in which a portion of the almost ionized electrons recombine into the initial ground or an excited bound state. We analyze the ellipticity dependence of the relative signals that are predicted in a single-active electron approximation (SAE), the validity of which is checked against a parameter-free multi-electron \hbox{$R$-matrix} (close-coupling) with time dependence approach. We find good agreement between the results from both models, thereby providing confidence in the SAE model potential to treat the process of interest. Comparison of the relative excitation probabilities found in our numerical calculations with the predictions of Landsman {\it et al.}\ (New Journal of Physics {\bf 15} (2013) 013001) and Zhao {\it et al.}\ (Optics Express {\bf 27} (2019) 21689) reveals good agreement with the former for short pulses. For longer pulses, the ellipticity dependence becomes wider than that obtained from the Landsman {\it et al.} formula, but we do not obtain the increase compared to linearly polarized radiation predicted by Zhao {\it et al.}

Ellipticity dependence of the third-order nonlinear optical response of graphene irradiated by two-color lights

We theoretically investigate the third-order optical response of graphene irradiated by two-color lights, paying special attention to the quantum interference. Our studies reveal that the interplay between harmonic generation and four-wave mixing leads to unusual nonlinear optical properties with nontrivial ellipticity dependence. It is shown that, unlike the case of monochromatic light with frequency ω0 (where the intensity of the third order response (I(3ω0)) decreases monotonically with the ellipticity and becomes zero for circularly polarized light), I(3ω0) may increase monotonically with the ellipticity, or be nearly independent on the ellipticity. In particular, under suitable condition, there exists an optimal nonzero ellipticity for the highest I(3ω0). Moreover, circularly polarized third-order optical response can be generated. We have found effective methods of modulating the nonlinear optical processes, which may have various applications in optical devices based on two dimensional materials.