Two-color Field Research Articles

Dynamical channel coupling in strong-field ionization of CO2

We present a theoretical study employing the time-dependent density functional theory (TDDFT) to explore the effects of angle-resolved channel coupling in strong field ionization of carbon dioxide (CO2) molecules. Our results reveal significant angular sensitivity of both the channel-resolved ionization probabilities and the effects of laser-induced channel couplings. By applying a linearly polarized two-color field scheme, we demonstrate the ability to significantly modify the strength of the laser-induced coupling, evidenced by the changes in the population distributions among the ionic states induced by the strong-field ionization. Importantly, the two-color field optimally modulates the coupling strength at the alignment angle where ionization of the highest occupied molecular orbital (HOMO) electrons is most efficient. This optimization is attributed to the reduction of the electron shielding effect. Our research provides valuable insights into the coherent manipulation of electron distribution within the cation, paving the way for the precise control of ultrafast electron dynamics during strong-field ionization processes.

Scheme for generation of spatiotemporal optical vortex attosecond pulse trains

The realization of spatiotemporal vortex structure of various physical fields with transverse orbital angular momentum (OAM) has attracted much attention and is expected to expand the research scope and open new opportunities in their respective fields. Here we present theoretically the first, to the best of our knowledge, study on the generation of attosecond pulse trains featuring a spatiotemporal optical vortex (STOV) structure by a two-color femtosecond light field, with each color carrying transverse OAM. Through careful optimization of relative phase and intensity ratio, we validate the efficient upconversion of the infrared pulse into its tens of order harmonics, showing that each harmonic preserves a corresponding intact topological charge. This unique characteristic enables the synthesis of an extreme ultraviolet attosecond pulse train with transverse OAM. In addition, we reveal that ionization depletion plays an outsize role therein. Our studies pave the way for the generation and utilization of light fields with STOV in the attosecond regime.

Deciphering the role of three-color synthesized laser pulse parameters in N2 ionization and attosecond pulse shaping

Photoionization of atoms or molecules is a fundamental process in strong-field physics, essential for generating high-order harmonics and producing attosecond pulses. Here, we investigate how a three-color laser field, consisting of wavelengths at 800 nm and its second and third harmonics, photoionizes N2 molecules and evaluates its effect on the properties of attosecond pulses. It has been discovered that by altering the relative phase, these harmonics periodically influence molecular ionization, increasing the discreteness and strength of the attosecond pulse trains. Three-color field driving dramatically raises the pulse peak while decreasing the width of the strongest peak pulse, whereas two-color field driving just slightly enhances the pulse intensity and duration. Furthermore, the effectiveness of harmonic production is significantly increased by varying the laser intensity ratios. Even though the efficiency and pulse intensity of the three-color field are limited by conversion efficiency, attosecond pulses with higher intensities can be produced with proper parameter tuning at lower ionization rates. These findings offer a significant foundation for precisely controlling attosecond pulse generation. Ocis codes320.7110; 320.7120.

Efficient Control of Electron Localization and Probability Modulation with Synthesized Two-Color Intense Laser Pulses.

A coupled electron-nuclear dynamical study at attosecond time scale is performed on the HD+ and H2+ molecular ions under the influence of synthesized intense two-color electric fields. We have employed ω - 2ω and also, ω - 3ω two-color fields in the infrared/mid-infrared regime to study the different fragmentation processes originating from the interference of n - (n + i) (i = 1, 2) photon absorption pathways. The branching ratios corresponding to different photofragments are controlled by tuning the relative phase as well as intensity of the two-color pulses, while the effect of the initial nuclear wave function is also studied by taking an individual vibrational eigenstate or a coherent superposition of several eigenstates of HD+ and H2+. By comprehensive analysis, the efficacy of the two different types of synthesized two-color pulses (ω - 2ω and ω - 3ω) are analyzed with respect to one-color intense pulses in terms of controlling the probability modulation and electron localization asymmetry and compared with previous theoretical calculations and experimental findings. Through the detailed investigation, we have addressed which one is the major controlling knob to have better electron localization as well as probability modulation.

Photoelectron angular distributions for photoionization of argon by two-color fields

Photoelectron angular distributions for photoionization of argon by two-color fields

Interference of harmonics emitted by different tunneling momentum channels in laser fields

Abstract By numerically solving the semiconductor Bloch equation (SBEs), we theoretically study the high-harmonic generation of ZnO crystals driven by one-color and two-color intense laser pulses. The results show the enhancement of harmonics and the cut-off remains the same in the two-color field, which can be explained by the recollision trajectories and electron excitation from multi-channels. Based on the quantum path analysis, we investigate contribution of different ranges of the crystal momentum k of ZnO to the harmonic yield, and find that in two-color laser fields, the intensity of the harmonic yield of different ranges from the crystal momentum makes a big difference and the harmonic intensity is depressed from all k channels, which is related to the interferences between harmonics from symmetric k channels.

Steering the energy sharing of electrons in nonsequential double ionization with orthogonally polarized two-color field

Abstract Using the semiclassical ensemble model, the dependence of relative amplitude for the recollision dynamics in nonsequential double ionization (NSDI) of neon atom driven by the orthogonally polarized two-color field (OTC) laser field is theoretically studied. And the dynamics in two typical collision pathways, recollision-impact-ionization (RII) and recollision-excitation with subsequent ionization (RESI), is systematically explored. Our results reveal that the V-shaped structure in the correlated momentum distribution is mainly caused by the RII mechanism when the relative amplitude of the OTC laser field is zero, and the first ionized electrons will quickly skim through the nucleus and share few energy with the second electron. As the relative amplitude increases, the V-shaped structure gradually disappears and electrons are concentrated on the diagonal in the electron correlation spectrum, indicating that the energy sharing after electrons collision is symmetric for OTC laser fields with large relative amplitudes. Our studies show that changing the relative amplitude of the OTC laser field can efficiently control the electron–electron collisions and energy exchange efficiency in the NSDI process.

Ultrafast photoinduced C-H bond formation from two small inorganic molecules

The formation of carbon-hydrogen (C-H) bonds via the reaction of small inorganic molecules is of great significance for understanding the fundamental transition from inorganic to organic matter, and thus the origin of life. Yet, the detailed mechanism of the C-H bond formation, particularly the time scale and molecular-level control of the dynamics, remain elusive. Here, we investigate the light-induced bimolecular reaction starting from a van der Waals molecular dimer composed of two small inorganic molecules, H2 and CO. Employing reaction microscopy driven by a tailored two-color light field, we identify the pathways leading to C-H photobonding thereby producing HCO+ ions, and achieve coherent control over the reaction dynamics. Using a femtosecond pump-probe scheme, we capture the ultrafast formation time, i.e., 198 ± 16 femtoseconds. The real-time visualization and coherent control of the dynamics contribute to a deeper understanding of the most fundamental bimolecular reactions responsible for C–H bond formation, thus contributing to elucidate the emergence of organic components in the universe.

Vortex harmonic generation in indium tin oxide thin film irradiated by a two-color field.

When a two-color Laguerre-Gaussian laser beam propagates through an indium tin oxide (ITO) material, the spatial distributions of odd- and even-order vortex harmonics carrying orbital angular momentum (OAM) are studied. The origin of vortex harmonics can be directly clarified by investigating their dependence on the incident laser field amplitude and frequency. In addition, it is shown that the spectral intensities of vortex harmonics are sensitive to the epsilon-near-zero nonlinear enhancing effects and the thickness of ITO materials. Thus the vortex harmonics can be conveniently tunable, which provides a wider potential application in optical communications based on high-order OAM coherent vortex beams.

Anisotropy Parameters for Two-Color Photoionization Phases in Randomly Oriented Molecules: Theory and Experiment in Methane and Deuteromethane.

We present combined theoretical and experimental work investigating the angle-resolved phases of the photoionization process driven by a two-color field consisting of an attosecond pulse train and an infrared pulse in an ensemble of randomly oriented molecules. We derive a general form for the two-color photoelectron (and time-delay) angular distribution valid also in the case of chiral molecules and when relative polarizations of the photons contributing to the attosecond photoelectron interferometer differ. We show a comparison between the experimental data and theoretical predictions in an ensemble of methane and deuteromethane molecules, discussing the effect of nuclear dynamics on the photoionization phases. Finally, we demonstrate that the oscillating component and the phase of the two-color signal can be fitted by using complex asymmetry parameters, in perfect analogy to the atomic case.

The Coulomb effect in nonsequential double ionization by counter-rotating two-color elliptical polarization fields.

Using a three-dimensional classical ensemble model, nonsequential double ionization (NSDI) of Ar atoms by counter-rotating two-color elliptical polarization (TCEP) fields is investigated. The major axes of the two elliptical fields are aligned in different directions. The relative alignment of the two elliptical fields strongly affects the waveform of the combined electric field and the ultrafast dynamics of NSDI in TCEP fields. Numerical results show that the correlated electron momentum distributions in the x direction evolve from a V-shaped structure near the axis to a distribution concentrated on the diagonal with the angle between the two elliptical major axes increasing. The asymmetry of the energy sharing between the two electrons during recollision results in the V-shaped structure in the correlated momentum spectrum. Back analysis indicates that the recollision times of a part of the trajectories move from the peak to the valley of the combined electric field with the angle between the two elliptical major axes increasing. Therefore, for the case of a larger angle between the two elliptical major axes, the electrons experience a longer time to escape away from the vicinity of the parent ion and thus the stronger Coulomb effect from the parent ion makes the momentum difference between two electrons small, which results in a distribution concentrated on the diagonal. This provides an effective avenue to control the electron ultrafast dynamics in NSDI.

Ideal two-color field ratio for holographic angular streaking of electrons

Ideal two-color field ratio for holographic angular streaking of electrons

Controlling polarization of high-order harmonics generated in the mixed gases with orthogonal two-color laser fields

The generation of highly elliptically polarized high-order harmonics (EPHHs) is indispensable for investigating chirality-sensitive light-matter interactions. Recently, high-order harmonic generation (HHG) with controllable ellipticity and helicity has attracted considerable attention. In this work, we theoretically demonstrate the possibility of generating broadband EPHHs with the same helicity from mixed gases in orthogonal two-color fields. There is a specific relative phase between the HHG from different gas components of the mixture. In addition, manipulation of the phase difference can be achieved by controlling the alignment angle of the molecule in mixed gases. It enables us to selectively enhance one helicity component of the high-order harmonics in a wide spectral range. This scheme paves a way for possibly generating elliptically polarized attosecond pulses.

Steering photoassociation of cold 85Rb atoms by two-color slowly-turned-on and rapidly-turned-off laser pulses

Photoassociation (PA) of 85Rb atoms from the ground state to the excited and states by two-color laser pulses at 100 is investigated by using quantum wavepacket method. Two pulses with detunings δ 1 and δ 2 varying from −1.0 to 1. cm−1 are taken into account. The specific case is generalized to the condition of arbitrary combination of δ 1 and δ 2 for both the Gaussian-pulse field and the slowly-turned-on and rapidly-turned-off (STRT) field. It is found that the introduce of the detunings in the two pluses can enhance the asymmetry of the time profile and broaden the linewidth of the laser field. The two factors can further enhance the PA probability for both resonant and nonresonant regions. Compared to the Gaussian field, the STRT field which is even more asymmetric in time profile and more broaden in linewidth can significantly enhance the PA probability, with the nonresonant transition dominating the PA process. It can be expected that once the two detunings are both positive, which is a relatively loose restriction for coherent control, a considerable PA probability can be obtained in a two-color STRT field.

Influence of nuclear dynamics on molecular attosecond photoelectron interferometry.

In extreme ultraviolet spectroscopy, the photoionization process occurring in a molecule due to the absorption of a single photon can trigger an ultrafast nuclear motion in the cation. Taking advantage of attosecond photoelectron interferometry, where the absorption of the extreme ultraviolet photon is accompanied by the exchange of an additional infrared quantum of light, one can investigate the influence of nuclear dynamics by monitoring the characteristics of the photoelectron spectra generated by the two-color field. Here, we show that attosecond photoelectron interferometry is sensitive to the nuclear response by measuring the two-color photoionization spectra in a mixture of methane (CH4) and deuteromethane (CD4). The effect of the different nuclear evolution in the two isotopologues manifests itself in the modification of the amplitude and contrast of the oscillations of the photoelectron peaks. Our work indicates that nuclear dynamics can affect the coherence properties of the electronic wave packet emitted by photoionization on a time scale as short as a few femtoseconds.

Strong polarization-controlled terahertz generation by bi-elliptical polarized laser fields

Terahertz generation from atoms driven by two color linearly polarized (LP) and circularly polarized (CP) laser fields have been well investigated. In this work, based on the photocurrent model, we investigate theoretically the intensity and polarization characteristics of terahertz waves radiated by the bi-elliptical polarized two-color laser fields with orthogonal or parallel major axes. We show that polarization-controlled, including circularly polarized terahertz waves with sufficient intensity comparable to that of co-rotating CP or parallel LP laser field, can be generated by using a longer-wavelength few-cycle bi-elliptical field. Our simulations also show that THz energy and ellipticity can be dramatically improved with dual-color elliptical field with tiny or large ellipticity, compared with that with two-color orthogonal LP field and counter-rotating CP laser field, respectively. Bi-elliptical polarized laser field provides a huge parameter space allowing for far-reaching control of THz emission.

Enhancement of valley-selective excitation by a linearly polarized two-color laser pulse

Here, we propose valley-selective excitations via a two-color $(\ensuremath{\omega}+2\ensuremath{\omega})$ laser field, made by superimposing two linearly polarized pulses at frequencies $\ensuremath{\omega}$ and $2\ensuremath{\omega}$. We have studied the intensity ratio between a few-cycle pulse of an $\ensuremath{\omega}$ and $2\ensuremath{\omega}$ laser, and its enhancement factor by employing time-dependent first-principles calculations. The valley polarization depends on the carrier-envelope phases (CEPs) of the pulses and the intensity ratio ${I}_{\ensuremath{\omega}}/{I}_{2\ensuremath{\omega}}$. We found that a two-color field enhances valley polarization by as much as 1.2 times larger than a single-color pulse. Maximum valley asymmetry is achieved for an intensity ratio ${I}_{\ensuremath{\omega}}/{I}_{2\ensuremath{\omega}}$ of 36 with a relative CEP of $\ensuremath{\pi}$. In our previous work, we found that the asymmetric vector potential induces valley polarization [A. Hashmi et al., Phys. Rev. B 105, 115403 (2022)]. In this paper, we find that the asymmetry of the electric field modulates the valley polarization. Our two-color scheme offers another path toward the optical control of valley pseudospins.

High-Order Above-Threshold Ionization Using a Bi-Elliptic Orthogonal Two-Color Laser Field with Optimal Field Parameters

In the present paper, we study the high-order above-threshold ionization of noble-gas atoms using a bi-elliptic orthogonal two-color (BEOTC) field. We give an overview of the SFA theory and calculate the differential ionization rate for various values of the laser field parameters. We show that the ionization rate strongly depends on the ellipticity and the relative phase between two field components. Using numerical optimization, we find the values of ellipticity and relative phase that maximize the ionization rate at energies close to the cutoff energy. To explain the obtained results, we present, to the best of our knowledge, for the first time the quantum-orbit analysis in the BEOTC field. We find and classify the saddle-point (SP) solutions and study their contributions to the total ionization rate. We analyze quantum orbits and corresponding velocities to explain the contribution of relevant SP solutions.

Controlling multiple returnings in non-sequential double ionization with orthogonal two-color laser pulses

With the three-dimensional semi-classical ensemble model, we studied the non-sequential double ionization by orthogonal two-color laser pulses. Our calculations show that the proportion of events experiencing multiple returnings, the sum of the final energies of two electrons, and the ion momentum distribution depend on the relative phase of the two-color fields, exhibiting oscillatory behavior with a period of π. Back analysis of these trajectories reveals that we can control the recollision energy of the electron by changing the relative phase of the two-color laser pulse. As a consequence, the trajectories of multiple-returning ions change with the relative phase, resulting in relative-phase-dependent ion momentum distributions. The result shows that the momentum distribution of the ions in the trajectories of multiple returnings is clearly wider than that for the case of single returning. For the multiple-returning events, the binary recollision leads to a smaller scattering angle of the first electron.

Coulomb potential determining terahertz polarization in a two-color laser field.

The orientation and ellipticity of terahertz (THz) polarization generated by a two-color strong field not only casts light on underlying mechanisms of laser-matter interaction, but also plays an important role for various applications. We develop the Coulomb-corrected classical trajectory Monte Carlo (CTMC) method to well reproduce the joint measurements, that the THz polarization generated by the linearly polarized 800 nm and circularly polarized 400 nm fields is independent on two-color phase delay. The trajectory analysis shows that the Coulomb potential twists the THz polarization by deflecting the orientation of asymptotic momentum of electron trajectories. Further, the CTMC calculations predict that, the two-color mid-infrared field can effectively accelerate the electron rapidly away from the parent core to relieve the disturbance of Coulomb potential, and simultaneously create large transverse acceleration of trajectories, leading to the circularly polarized THz radiation.