Based upon our previous works (Eur.Phys.J.D 6, 319(1999); Chin.Phys.Lett. 18, 236(2001)), we develop a classical approach to calculate the high-order harmonic generation of the laser driven atoms and molecules. The Coulomb singularities in the system have been removed by a regularization procedure. Action-angle variables have been used to generate the initial microcanonical distribution which satisfies the inversion symmetry of the system. The numerical simulation show, within a proper laser intensity, a harmonic plateau with only odd harmonics appears. At higher intensities, the spectra become noisier because of the existence of chaos. With further increase in laser intensity, ionization takes place, and the high-order harmonics disappear. Thus chaos introduces noise in the spectra, and ionization suppresses the harmonic generation, with the onset of the ionization follows the onset of chaos.
By using perturbation theory we derive an expression for the electrical field of a Gaussian laser pulse propagating in a gas medium. This expression is used as a trial solution in a variational method to get quasianalytical solutions for the width, intensity and self-focusing distance of ultrashort pulse. The approximation gives an improved agreement with results of numerical simulations for a broad range of values of the input power of the pulse than previous analytical results available in the literature.
We present theoretical results on the high-harmonic generation (HHG) in bulk diamond induced by intense laser pulse of wavelength 800 nm and duration 15 fs. For laser intensity in the range $1 \le I \le 50 $ TW/cm$^2$ above bandgap harmonics are generated after the pulse peak. We find that the intensity of individual harmonics increases non-linearly with the peak laser intensity, following a non-perturbative trend. For moderate intensity the HHG spectrum exhibits a primary plateau with noisy odd order harmonic structure and a cutoff. For increased laser intensity a secondary plateau emerges wi…
In present paper we develop an analytic theory for the harmonic generation of symmetric diatomic molecular ions beyond two-level model, emphasizing the influence of charge-resonance (CR) states those are strongly coupled to electromagnetic fields for large internuclear distance. With taking into account the continuum states that is ignored in the two-level model and become important for intense laser case, our model is capable to produce spectrum for the whole range of harmonic orders consisting of a molecular plateau due to the CR transition and an atomic-like plateau for a long-wavelength ex…
We study theoretically the dipole radiation of a hydrogen atom driven by an intense sub-cycle pulse. The time-dependent Schrödinger equation for the system is solved by ab initio calculation to obtain the dipole response. Remarkably, a narrowband emission lasting longer than the driving pulse appears at a frequency just above the ionization threshold. An additional calculation using the strong field approximation also recovers this emission, which suggests that it corresponds to the oscillation of nearly-bound electrons that behave similarly to Rydberg electrons. The predicted phenomenon is un…
We present calculation of photoexcitation and high-harmonic generation in bulk diamond induced by intense near-infrared laser pulse of photon energy 1.55 eV, time duration of 15 fs and peak field strength $F=$ 0.4 V/Å. Depending on the laser polarization direction, the pulsed irradiation creates electron-hole pairs and transient density fluctuations in a localized region of the crystal momentum space. As a consequence energetic inter- and intra-band harmonics are generated with alternating phase during each half-cycle of the driving pulse. The corresponding inter- and intra-band currents are i…
We present theoretical studies of high-order harmonic generation (HHG) in rare gases driven by plasmonic field enhancement. This kind of fields appears when plasmonic nanostructures are illuminated by an intense few-cycle laser and have a particular spatial dependency, depending on the geometrical shape of the nanostructure. We demonstrate that the strong nonhomogeneous character of the laser enhanced field plays an important role in the HHG process and significantly extends the harmonic cutoff. Our models are based on numerical solution of the time dependent Schroedinger equation (TDSE) and s…
We apply the time-dependent R-matrix method to investigate harmonic generation from Ne(+) at a wavelength of 390 nm and intensities up to 10(15) Wcm(-2). The 1s(2)2s(2)2p(4) (3)P(e), (1)D(e), and (1)S(e) states of Ne(2+) are included as residual-ion states to assess the influence of interference between photoionization channels associated with these thresholds. The harmonic spectrum is well approximated by calculations in which only the (3)P(e) and (1)D(e) thresholds are taken into account, but no satisfactory spectrum is obtained when a single threshold is taken into account. Within the harmo…
At the core of attosecond science lies the ability to generate laser pulses of sub-femtosecond duration. In tabletop devices the process relies on high-harmonic generation, where a major challenge is to obtain high yields and high cutoff energies required for the generation of attosecond pulses. We develop a computational method that can simultaneously resolve these issues by optimizing the driving pulses using quantum optimal control theory. Our target functional, an integral over the harmonic yield over a desired energy range, leads to a remarkable cutoff extension and yield enhancement for …
We investigate the multi-electron dynamics in high-order harmonic generation (HHG) from N2 molecules. Clear spectral minima are observed in the cutoff region at all three mid-infrared wavelengths (i.e., 1300, 1400 and 1500 nm) chosen in our experiment. It is found that the positions of the spectral minima do not depend on the alignment angles of molecules. In addition, the spectral minima shift almost linearly with the increasing laser intensity at all three wavelengths, which provides a strong evidence on the dynamic multi-channel interference origin of these minima. The advantages of observa…
We experimentally investigate the generation of above-threshold harmonics completely from argon atoms on an excited state using mid-infrared femtosecond laser pulses. The highly nonlinear dependences of the observed signal on the pulse energy and polarization of the driver laser pulses indicate its non-perturbative characteristic.
We study the behavior of reduced models for the propagation of intense laser pulses in atomic gases. The models we consider incorporate ionization, blueshifting, and other nonlinear propagation effects in an ab initio manner, by explicitly taking into account the microscopic electron dynamics. Numerical simulations of the propagation of ultrashort linearly-polarized and elliptically-polarized laser pulses over experimentally-relevant propagation distances are presented. We compare the behavior of models where the electrons are treated classically with those where they are treated quantum-mecha…
A generalization of non-perturbative QED model for high harmonic generation is developed for the multi-mode optical field case. By introducing classical-field-dressed quantized Volkov states analytically, a formula to calculate HHG for hydrogen-like atom in ultrashort intense laser pulse is obtained, which has a simple intuitive interpretation. The dressed state QED model indicates a new perspective to understand HHG, for example, the presence of the weak even-order harmonic photons, which has been verified by both theoretical analysis and numerical computation. Long wavelength approximation a…
High-order harmonic generation is investigated for H$_2^+$ and D$_2^+$ with and without Born-Oppenheimer approximation by numerical solution of full dimensional electronic time-dependent Schrödinger equation under 4-cycle intense laser pulses of 800 nm wavelength and $I$=4, 5, 7, 10 $\times 10^{14}$ W$/$cm$^2$ intensities. For most harmonic orders, the intensity obtained for D$_2^+$ is higher than that for H$_2^+$, and the yield difference increases as the harmonic order increases. Only at some low harmonic orders, H$_2^+$ generates more intense harmonics compared to D$_2^+$. The results show …
We present the generation of high order harmonics in crystalline silicon subjected to intense near-infrared 30fs laser pulse. The harmonic spectrum extends from the near infrared to the extreme ultraviolet spectral region. Depending on the pulsed laser intensity, we distinguish two regimes of harmonic generation: (i) perturbative regime: electron-hole pairs born during each half-cycle of the laser pulse via multiphoton and tunnel transitions are accelerated in the laser electric field and gain kinetic energy; the electron-hole pairs then recombine in the ground state by emitting a single high-…
The coherent radiation spectrum of two-level polar molecules with UV transition is studied at the multiphoton resonant excitation by a moderately strong laser field. The spectrum corresponding to harmonic generation and low-frequency radiation is investigated both analytically and numerically. Specifically, a mechanism for generation of intense smoothly tunable terahertz radiation by two-level molecular configurations (with dynamic Stark shifts) possessing permanent dipole moments, is considered.
Quantum-mechanical investigation is presented to study single attosecond pulse generation by gating high-order harmonic emission from H$_2^+$ molecule in intense laser pulses with time-dependent ellipticity. The high-order harmonic generation from H$_2^+$ molecule in superposition of a left and a right-hand circularly polarized Gaussian pulse is studied and the effect of time duration and carrier-envelope phase of laser field on single attosecond pulse generation is investigated. Using laser field formed by combination of a left and a right-hand elliptically polarized Gaussian pulse, the effec…
We present theoretical calculations for polarization and ellipticity of high-order harmonics from aligned N$_2$, CO$_2$, and O$_2$ molecules generated by linearly polarized lasers. Within the rescattering model, the two polarization amplitudes of the harmonics are determined by the photo-recombination amplitudes for photons emitted parallel and perpendicular to the direction of the {\em same} returning electron wave packet. Our results show clear species-dependent polarization states, in excellent agreement with experiments. We further note that the measured polarization ellipse of the harmoni…
One key parameter in the high-order harmonic generation (HHG) phenomenon is the exact frequency of the generated harmonic field. Its deviation from perfect harmonics of the laser frequency can be explained considering (i) the single-atom laser-matter interaction and (ii) the spectral changes of the driving laser. In this work, we perform an experimental and theoretical study of the causes that generate spectral changes in the HHG radiation. We measured the driving laser spectral shift after high harmonic generation in long medium using a correction factor to take into account the multiple poss…
This paper introduces Bohmian mechanics (BM) into the intense laser-atom physics to study high-order harmonic generation. In BM, the trajectories of atomic electrons in intense laser field can be obtained with the Bohm-Newton equation. The power spectrum with the trajectory of an atomic electron is calculated, which is found to be irregular. Next, the power spectrum associated with an atom ensemble from BM is considered, where the power spectrum becomes regular and consistent with that from quantum mechanics. Finally, the reason of the generation of the irregular spectrum is discussed.
Intense extreme-ultraviolet (XUV) pulses enable the investigation of XUV-induced nonlinear processes and are a prerequisite for the development of attosecond pump - attosecond probe experiments. While highly nonlinear processes in the XUV range have been studied at free-electron lasers (FELs), high-harmonic generation (HHG) has allowed the investigation of low-order nonlinear processes. Here we suggest a concept to optimize the HHG intensity, which surprisingly requires a scaling of the experimental parameters that differs substantially from optimizing the HHG pulse energy. As a result, we are…
Contributions of the pre-ionized H$_2$ (PI-H$_2$) and ionized H$_2^+$ subsystems of the two-electron H$_2$ system to its high-order harmonic generation in 8-cycle $\sin^{2}$-like ultrafast intense laser pulses are calculated and analyzed based on the solution of the time-dependent Schrödinger equation (TDSE) for the one-dimensional two-electronic H$_2$ system with fixed nuclei. The laser pulses have $λ =\ 390\ \&\ 532$ nm wavelengths and $I=1\times 10^{14}$, 5$\times 10^{14}$, 1$\times 10^{15}$ \&\ 5$\times 10^{15}$ Wcm$^{-2}$ intensities. It is found that at the two lower intensities, the PI-…
We show that high-order harmonics generated from molecules by intense laser pulses can be expressed as the product of a returning electron wave packet and the photo-recombination cross section (PRCS) where the electron wave packet can be obtained from simple strong-field approximation (SFA) or from a companion atomic target. Using these wave packets but replacing the PRCS obtained from SFA or from the atomic target by the accurate PRCS from molecules, the resulting HHG spectra are shown to agree well with the benchmark results from direct numerical solution of the time-dependent Schrödinger eq…
We present experimental results showing the appearance of a near-continuum in the high-order harmonic generation (HHG) spectra of atomic and molecular species as the driving laser intensity of an infrared pulse increases. Detailed macroscopic simulations reveal that these near-continuum spectra are capable of producing IAPs in the far field if a proper spatial filter is applied. Further, our simulations show that the near-continuum spectra and the IAPs are a product of strong temporal and spatial reshaping (blue shift and defocusing) of the driving field. This offers a possibility of producing…
We report on the comparative experimental investigation on third and fifth harmonic generation (THG and FHG) in atomic and molecular gases driven by mid-infrared ultrafast laser pulses at a wavelength of ~1500 nm. We observe that the conversion efficiencies of both the THG and FHG processes saturate at similar peak intensities close to ~1.5\times1014 W/cm2 for argon, nitrogen, and air, whose ionization potentials are close to each other. Near the saturation intensity, the ratio of yields of the FHG and THG reaches ~10-1 for all the gases. Our results show that high-order Kerr effects do exist,…
Two different induced effects of a laser falling edge on high-order harmonic generation are resolved by solving numerically full-dimensional electronic time-dependent Schrödinger equation beyond the Born-Oppenheimer approximation. The harmonic spectrum of H$_2^+$ and T$_2^+$ isotopes are compared to see the effects of a 4-cycle falling edge of a 800 nm, 15-cycle trapezoidal laser pulse of $I=$3 $\times 10^{14}$ Wcm$^{-2}$ intensity on harmonic emission spectrum. The harmonic emission at the laser falling part is negligible for H$_2^+$ due to ionization suppression, but considerable for T$_2^+$…
The ongoing development of intense high-harmonic generation (HHG) sources has recently enabled highly nonlinear ionization of atoms by the absorption of at least 10 extreme-ultraviolet (XUV) photons within a single atom [Senfftleben \textit{et al.}, arXiv1911.01375]. Here we investigate the role that reshaping of the fundamental, few-cycle, near-infrared (NIR) driving laser within the 30-cm-long HHG Xe medium plays in the generation of the intense HHG pulses. Using an incident NIR intensity that is higher than what is required for phase-matched HHG, signatures of reshaping are found by measuri…
Dipolar Bose and Fermi gases, which are currently being studied extensively experimentally and theoretically, interact through anisotropic, long-range potentials. Here, we replace the long-range potential by a zero-range pseudo-potential that simplifies the theoretical treatment of two dipolar particles in a harmonic trap. Our zero-range pseudo-potential description reproduces the energy spectrum of two dipoles interacting through a shape-dependent potential under external confinement very well, provided that sufficiently many partial waves are included, and readily leads to a classification s…
The underlying physics behind the molecular harmonic emission in relatively long sin$^2$-like laser pulses is investigated. We numerically solved the full-dimensional electronic time-dependent Schrödinger equation beyond the Born-Oppenheimer approximation for simple molecular ion H$_2^+$. The occurrence and the effect of electron localization, non-adiabatic redshift and spatially asymmetric emission are evaluated to understand better complex patterns appearing in the high-order harmonic generation (HHG) spectrum. Results show that the complex patterns in the HHG spectrum originate mainly from …
Effects of the laser pulse wavelength and intensity on the HHG production from the \textit{ionic} and \textit{homolytic} pre-ionization transient states of the two-electron H$_{2}$ system exposed to ultrashort intense laser pulses are studied by solving time-dependent Schrödinger equation. It is found that for the populated homolytic species in each half cycle of the laser pulse having enough strength, a pair of strong and weak HHG radiations are produced simultaneously. For the populated ionic species divided into two regions, in each half cycle, one of the ionic regions has a strong radiatio…
We report theoretical calculations of high-order harmonic generation (HHG) of Xe with the inclusion of multi-electron effects and macroscopic propagation of the fundamental and harmonic fields in an ionizing medium. By using the time-frequency analysis we show that the reshaping of the fundamental laser field is responsible for the continuum structure in the HHG spectra. We further suggest a method for obtaining an isolated attosecond pulse (IAP) by using a filter centered on axis to select the harmonics in the far field with different divergence. We also discuss the carrier-envelope-phase dep…
High-order harmonic generation (HHG) in gases leads to short-pulse extreme ultraviolet (XUV) radiation useful in a number of applications, for example, attosecond science and nanoscale imaging. However, this process depends on many parameters and there is still no consensus on how to choose the target geometry to optimize the source efficiency. Here, we review the physics of HHG with emphasis on the macroscopic aspects of the nonlinear interaction. We analyze the influence of medium length, pressure, position of the medium and intensity of the driving laser on the HHG conversion efficiency (CE…
It is known that the dynamics of two (Coulomb-interacting) nonrelativistic electrons confined by a parabolic potential and driven by a classical, intense laser field (in dipole approximation) is exactly soluble. We calculate the time-dependent population of the harmonic oscillator states and the energy absorbed from the laser. It turns out that the key entity on which all observables sensitively depends is the modulus square of the Fourier-transformed vector potential of the laser field, evaluated at the harmonic oscillator frequency. The system is transparent to laser field configurations for…
High harmonic generation (HHG) is a manifestation of the strongly nonlinear response of matter to intense laser fields and has, as the basis for coherent XUV sources a variety of applications. Recently, HHG from atoms in a phase and polarization structured laser was demonstrated and interpreted based on the transverse electric field component of the driving pulse. Here we point out that as dictated by Maxwell equations, such fields have a longitudinal component which in general has a fundamental influence on the charge dynamics. For instance, its interplay with the transversal field component …
Density-gradient effect in high-harmonic generation in gases
ELI ALPS, The Extreme Light Infrastructure ERIC（ELI ALPS，极轻基础设施 ERIC）；Institute of Physics, University of Szeged（塞格德大学物理研究所）；Department of Optics and Quantum Electronics, University of Szeged（塞格德大学光学与量子电子学系）
Excitation of the isomeric nuclear state 229m Th in the process of thorium atom irradiation by two-color femtosecond pulse of Ti: Sa laser at the fundamental wavelength and second harmonic is analyzed. It is shown that the rate of isomeric state excitation can be enhanced significantly with respect to other nucleus excitation processes in laser plasma or by an external coherent source at the resonance wavelength. This enhancement is due to the process of nonlinear laser nuclear excitation based on the following. First, the atomic current associated with the motion of valence electrons in stron…
A second plateau in the harmonic spectra of laser-driven two-electron atoms is observed both in the numerical solution of a low-dimensional model helium atom and using an extended strong field approximation. It is shown that the harmonics well beyond the usual cut-off are due to the simultaneous recombination of the two electrons, which were emitted during different, previous half-cycles. The new cut-off is explained in terms of classical trajectories. Classical predictions and the time-frequency analysis of the ab initio quantum results are in excellent agreement. The mechanism corresponds to…
Interplay of the channel-closing and bound-bound transition resonances in multiphoton ionization and harmonic generation in intense laser pulses
A.V. Gaponov-Grekhov Institute of Applied Physics of the Russian Academy of Sciences（俄罗斯科学院阿·瓦·加波诺夫-格雷霍夫应用物理研究所）；P.N. Lebedev Physical Institute of the Russian Academy of Sciences（俄罗斯科学院列别捷夫物理研究所）；N.I. Lobachevsky State University of Nizhny Novgorod（下诺夫哥罗德洛巴切夫斯基国立大学）
High-intensity laser pulses covering the ultraviolet to terahertz spectral regions are nowadays routinely generated in a large number of laboratories. In contrast, intense extreme-ultraviolet (XUV) pulses have only been demonstrated using a small number of sources including free-electron laser facilities [1-3] and long high-harmonic generation (HHG) beamlines [4-9]. Here we demonstrate a concept for a compact intense XUV source based on HHG that is focused to an intensity of $2 \times 10^{14}$ W/cm$^2$, with a potential increase up to $10^{17}$ W/cm$^2$ in the future. Our approach uses tight f…
We report on a compact and spectrally intense extreme-ultraviolet (XUV) source, which is based on high-harmonic generation (HHG) driven by 395 nm pulses. In order to minimize the XUV virtual source size and to maximize the XUV flux, HHG is performed several Rayleigh lengths away from the driving laser focal plane in a high-density gas jet. As a result, a high focused XUV intensity of $5 \times 10^{13}$ W/cm$^2$ is achieved, using a beamline with a length of only two meters and a modest driving laser pulse energy of 3 mJ. The high XUV intensity is demonstrated by performing a nonlinear ionizati…
For some time, the theoretical result for the transition temperature of a dilute three-dimensional Bose gas in an arbitrarily wide harmonic trap has been known to first order in the interaction strength. We extend that result to second order. The first-order result for a gas trapped in a harmonic potential can be computed in mean field theory (in contrast to the first order result for a uniform gas, which cannot). We show that, at second order, perturbation theory suffices for relating the transition temperature to the chemical potential at the transition, but the chemical potential is non-per…
The development of schemes for coherent nonlinear time-domain spectroscopy in the extreme-ultraviolet regime (XUV) has so far been impeded by experimental difficulties that arise at these short wavelengths. In this work we present a novel experimental approach, which facilitates the timing control and phase cycling of XUV pulse sequences produced by harmonic generation in rare gases. The method is demonstrated for the generation and high spectral resolution characterization of narrow-bandwidth harmonics ($\approx14\,$eV) in argon and krypton. Our technique simultaneously provides high phase st…
We present an implementation of the multiconfiguration time-dependent Hartree-Fock method based on the adaptive finite element method for molecules under intense laser pulses. For efficient simulations, orbital functions are propagated by a stable propagator using the short iterative Arnoldi scheme and our implementation is parallelized for distributed memory computing. This is demonstrated by simulating high-harmonic generation from a water molecule and achieves a simulation of multielectron dynamics with overwhelmingly less computational time, compared to our previous work.
We investigate dynamics of atomic and molecular systems exposed to intense, shaped chaotic fields and a weak femtosecond laser pulse theoretically. As a prototype example, the photoionization of a hydrogen atom is considered in detail. The net photoionization undergoes an optimal enhancement when a broadband chaotic field is added to the weak laser pulse. The enhanced ionization is analyzed using time-resolved wavepacket evolution and the population dynamics of the atomic levels. We elucidate the enhancement produced by spectrally-shaped chaotic fields of two different classes, one with a tuna…
We study the properties of a spin-polarized Fermi gas in a harmonic trap, using the semiclassical (Thomas-Fermi) approximation. Universal forms for the spatial and momentum distributions are calculated, and the results compared with the corresponding properties of a dilute Bose gas.
