We report theoretical investigations of the tomographic procedure suggested by Itatani {\it et al.} [Nature, {\bf 432} 867 (2004)] for reconstructing highest occupied molecular orbitals (HOMO) using high-order harmonic generation (HHG). Using the limited range of harmonics from the plateau region, we found that under the most favorable assumptions, it is still very difficult to obtain accurate HOMO wavefunction, but the symmetry of the HOMO and the internuclear separation between the atoms can be accurately extracted, especially when lasers of longer wavelengths are used to generate the HHG. We also considered the possible removal or relaxation of the approximations used in the tomographic method in actual applications. We suggest that for chemical imaging, in the future it is better to use an iterative method to locate the positions of atoms in the molecule such that the resulting HHG best fits the macroscopic HHG data, rather than by the tomographic method.
We present a theoretical analysis of high-order harmonic generation from ion-atom collisions in the presence of linearly polarized intense laser pulses. Photons with frequencies significantly higher than in standard atomic high-harmonic generation are emitted. These harmonics are due to two different mechanisms: (i) collisional electron capture and subsequent laser-driven transfer of an electron between projectile and target atom; (ii) reflection of a laser-driven electron from the projectile leading to recombination at the parent atom.
We investigate the process of circularly polarized high harmonic generation in molecules using a bicircular laser field. In this context, we show that molecules offer a very robust framework for the production of circularly polarized harmonics, provided their symmetry is compatible with that of the laser field. Using a discrete time-dependent symmetry analysis, we show how all the features (harmonic order and polarization) of spectra can be explained and predicted. The symmetry analysis is generic and can easily be applied to other target and/or field configurations.
We theoretically investigate correlated electron dynamics in high-harmonic generation (HHG), using all-electron \emph{ab initio} simulations for three-dimensional real alkali-metal atoms. The resulting harmonic spectra exhibit a plateau extended beyond the usual cutoff and a prominent resonance peak above the plateau. These remarkable features arise from the cation response dramatically enhanced by laser-induced electron recollision, which is a key process of attosecond science. This demonstrates that high-harmonic spectroscopy provides new possibilities to explore dynamical electron correlati…
We present studies of high-order harmonic generation (HHG) at laser intensities well above saturation. We use driving laser pulses which present a particular electron dynamics in the turn-on stage. Our results predict an increasing on the harmonic yield, after an initial dropping, when the laser intensity is increased. This fact contradicts the general belief of a progressive degradation of the harmonic emission at ultrahigh intensities. We have identified a particular set of trajectories which emerges in the turn-on stage of these singular laser pulses, responsible of the unexpected growth on…
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…
When a laser pulse impinges on a molecule which is invariant under certain symmetry operations selection rules for harmonic generation (HG) arise. In other words: symmetry controls which channels are open for the deposition and emission of laser energy---with the possible application of filtering or amplification. We review the derivation of HG selection rules and study numerically the interaction of laser pulses with an effectively one-dimensional ring-shaped model molecule. The harmonic yields obtained from that model and their dependence on laser frequency and intensity are discussed. In a …
We investigate the polarization properties of high harmonics generated with the bichromatic counterrotating circularly polarized (BCCP) laser fields by numerically solving time-dependent Schrödinger equation (TDSE). It is found that, the helicity of the elliptically polarized harmonic emission is reversed at particular harmonic orders. Based on the time-frequency analysis and the classical three-step model, the correspondence between the positions of helicity reversions and the classical trajectories of continuum electrons is established. It is shown that, the electrons ionized at one lobe of …
New approach to study the spontaneous emission of the atomic system in the presence of the high-intensity laser field is used to study the process of harmonic generation. The analysis is based on the consideration of quantum system interaction with quantized field modes beeing in vacuum state, while the intense laser field is considered classically beyond the perturbation theory. The numerical analysis of the emission from the single one-electron one dimensional atom irradiated by the femtosecond laser pulse of Ti-Sa laser is discussed. It is demonstrated that not only odd but also even harmon…
By analyzing ``exact'' theoretical results from solving the time-dependent Schrödinger equation of atoms in few-cycle laser pulses, we established the general conclusion that differential elastic scattering and photo-recombination cross sections of the target ion with {\em free} electrons can be extracted accurately from laser-generated high-energy electron momentum spectra and high-order harmonic spectra, respectively. Since both electron scattering and photoionization (the inverse of photo-recombination) are the conventional means for interrogating the structure of atoms and molecules, this …
We generate high-order harmonics at high pulse repetition rates using a turnkey laser. High-order harmonics at 400 kHz are observed when argon is used as target gas. In neon we achieve generation of photons with energies exceeding 90 eV ($\sim$13 nm) at 20 kHz. We measure a photon flux of 4.4$\cdot10^{10}$ photons per second per harmonic in argon at 100 kHz. Many experiments employing high-order harmonics would benefit from higher repetition rates, and the user-friendly operation opens up for applications of coherent extreme ultra-violet pulses in new research areas.
We study the influence of the pulse duration on high harmonic generation (HHG) with exploring a wide laser-parameter region theoretically. Previous studies have showed that for high laser intensities near to the saturation ionization intensity, the HHG inversion efficiency is higher for shorter pulses since the ground-state depletion is weaker in the latter. Surprisingly, our simulations show this high efficiency also appears even for a moderate laser intensity at which the ionization is not strong. A classical effect relating to shorter travel distances of the rescattering electron in shorter…
We study high-order harmonic generation (HHG) from aligned molecules in strong elliptically polarized laser fields numerically and analytically. Our simulations show that the spectra and polarization of HHG depend strongly on the molecular alignment and the laser ellipticity. In particular, for small laser ellipticity, large ellipticity of harmonics with high intensity is observed for parallel alignment, with forming a striking ellipticity hump around the threshold. We show that the interplay of the molecular structure and two-dimensional electron motion plays an important role here. This phen…
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 becom…
The selection rules of high harmonic generation (HHG) are investigated using three-dimensional time-dependent density functional theory (TDDFT). From the harmonic spectra obtained with various real molecules and different forms of laser fields, several factors that contribute to selection rules are revealed. Extending the targets to stereoscopic molecules, it is shown that the allowed harmonics are dependent on the symmetries of the projections of molecules. For laser fields, the symmetries contributing to the selection rules are discussed according to Lissajous figures and their dynamical dir…
High-harmonic generation from hydrogenlike muonic atoms exposed to ultraintense high-frequency laser fields is calculated. Systems of low nuclear charge number Z are considered where a nonrelativistic description applies. By comparing the radiative response for different isotopes we demonstrate characteristic signatures of the finite nuclear mass and size in the harmonic spectra. In particular, for Z>1, an effective muon charge appears in the Schrödinger equation for the relative particle motion, which influences the position of the harmonic cutoff. Cutoff energies in the MeV domain can be ach…
The generation of harmonics by atoms interacting with two circularly polarized and frequency related laser fields is addressed through ab initio numerical simulations. A detailed charaterization of a few specific harmonics is given. In particular, the two different cases where the total energy absorbed through photons is far-off or close to the energy gap between different atomic states are investigated. It is found that the conversion efficiency in the harmonic generation is strongly dependent on the inner atomic structure and in certain specific cases it can be significantly enhanced within …
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…
We investigate the harmonic response of neon atoms to mid-IR laser fields (2000-3000nm) using a single-active electron (SAE) model and the fully ab initio all-electron R-Matrix with Time-dependence (RMT) method. The laser peak intensity and wavelength are varied to find suitable parameters for high-harmonic imaging in the water window. Comparison of the SAE and RMT results shows qualitative agreement between them as well as parameters such as the cutoff frequency predicted by the classical three-step model. However, there are significant differences in the details, particularly in the predicte…
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 study the temporal and spatial dynamics of the large amplitude and frequency modulation that can be induced in an intense, few cycle laser pulse as it propagates through a rapidly ionizing gas. Our calculations include both single atom and macroscopic interactions between the non-linear medium and the laser field. We analyze the harmonic generation by such pulses and show that it is spatially separated from the ionization dynamics which produce a large dynamical blue shift of the laser pulse. This means that small changes in the initial laser focusing conditions can lead to large difference…
The generation of harmonics by atoms or ions in a two-color, coplanar field configuration with commensurate frequencies is investigated through both, an analytical calculation based on the Lewenstein model and the numerical ab initio solution of the time-dependent Schroedinger equation of a two-dimensional model ion. Through the analytical model, selection rules for the harmonic orders in this field configuration, a generalized cut-off for the harmonic spectra, and an integral expression for the harmonic dipole strength is provided. The numerical results are employed to test the predictions of…
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 investigate the high harmonic generation (HHG) from solids by simulating the dynamics of a single active electron in periodic potentials. The corresponding time-dependent Schrödinger equations (TDSE) are solved numerically by using B-spline basis sets in coordinate space. The energy band structure and wave vectors can be directly retrived from the eigenfunctions. The harmonic spectra obtained agree well with the results simulated by TDSE in $k$ space using Bloch states and show a two-plateau structure. Both of the cutoff energies of the two plateaus in the harmonic spectrum scale linearly w…
The present work reports on the generation of short-pulse coherent extreme ultraviolet radiation of controlled polarization. The proposed strategy is based on high-order harmonics generated in pre-aligned molecules. Field-free molecular alignment produced by a short linearly-polarized infrared laser pulse is used to break the isotropy of a gas medium. Driving the aligned molecules by a circularly-polarized infrared pulse allows to transfer the anisotropy of the medium to the polarization of the generated harmonic light. The ellipticity of the latter is controlled by adjusting the angular distr…
We analytically describe the strong-field light-electron interaction using a quantized coherent laser state with arbitrary photon number. We obtain a light-electron wave function which is a closed-form solution of the time-dependent Schrodinger equation (TDSE). This wave function provides information about the quantum optical features of the interaction not accessible by semi-classical theories. With this approach we can reveal the quantum optical properties of high harmonic generation (HHG) process in gases by measuring the photon statistics of the transmitted infrared (IR) laser radiation. T…
A theoretical model is developed describing high-order harmonic generation (HHG) from a gas of multiply-charged ions driven by a laser field of relativistic intensity. Macroscopic propagation of harmonics is investigated in a relativistic HHG setup where the relativistic drift is suppressed by means of x-ray field assistance of the driving laser field. The possibility of phase-matched emission of the harmonics is shown. The laser field geometry is optimized to maximize the HHG yield with the corresponding phase-matching schemes. Crucial issues determining the macroscopic HHG yield are discusse…
We develop a numerical scheme to investigate the high-order harmonic generation (HHG) in intense laser-matter interactions. Tracing the time evolution of every electronic laser-field-free state, we "observe" the HHG in a time-integrated quantum transition picture. Our full-quantum simulations reveal that continuum electrons with a broad energy distribution contribute equally to one harmonic and the excited state also plays an important role in the molecular HHG. These results imply a laser-intensity-dependent picture of intramolecular interference in the HHG.
We present Floquet calculations of high harmonic generation (HHG) for the lowest two electronic states of the $\mbox{H}_2^+$ ion by strong continuous-wave laser fields. We solve the non-Hermitian matrix problem to get accurate solutions to the periodic time-dependent Schrödinger equation (TDSE) by applying a pseudospectral representation combined with a complex absorbing potential method. This represents an alternative approach to direct TDSE solutions to obtain the harmonic spectra for the ion. We compare our HHG rates for the lower and upper states of $\mbox{H}^{+}_{2}$, which correspond to …
We discuss harmonic generation in the case of laser field-dressed Hamiltonians that are invariant under so-called dynamical symmetry operations. Examples for such systems are molecules which exhibit a discrete rotational symmetry of order N (e.g. benzene with N=6) interacting with a circularly polarized laser field and single atoms in a bichromatic field, with the two lasers having circular polarizations. Within a general group theory approach we study the harmonics one obtains from the interaction of a laser pulse and a circular molecule. When the system is in a pure field-dressed state the k…
The interaction of intense mid-infrared laser fields with atoms and molecules leads to a range of new opportunities, from the production of bright, coherent radiation in the soft x-ray range to imaging molecular structures and dynamics with attosecond temporal and sub-angstrom spatial resolution. However, all these effects, which rely on laser-driven recollision of an electron removed by the strong laser field and the parent ion, suffer from the rapidly increasing role of the magnetic field component of the driving pulse: the associated Lorentz force pushes the electrons off course in their ex…
In recent publications, it has been shown that high-order harmonic generation can be manipulated by employing a time-delayed attosecond pulse train superposed to a strong, near-infrared laser field. It is an open question, however, which is the most adequate way to approximate the attosecond pulse train in a semi-analytic framework. Employing the Strong-Field Approximation and saddle-point methods, we make a detailed assessment of the spectra obtained by modeling the attosecond pulse train by either a monochromatic wave or a Dirac-Delta comb. These are the two extreme limits of a real train, w…
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 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-…
We present single-molecule and macroscopic calculations showing that laser-induced Stark shifts contribute significantly to the phase of high-order harmonics from polar molecules. This is important for orbital tomography, where phases of field-free dipole matrix elements are needed in order to reconstruct molecular orbitals. We derive an analytical expression that allows the first-order Stark phase to be subtracted from experimental measurements.
The strong-field approximation for high-harmonic generation in near-infrared and infrared laser pulses is formulated in the accelerated Kramers-Henneberger frame. The accompanying physical picture is discussed and the nature of the leading-order term is contrasted with that of the three-step model following the strong-field-approximation formulation in the length or velocity gauges. The theory is illustrated by high-harmonic generation spectra for atomic hydrogen.
We studied the high-harmonic generation by the interaction of sub-cycle laser pulses with the He atom. The sub-cycle pulses are modeled using the complex source vector beam model, which is an exact solution to Maxwell's equations and accurately models the sub-cycle field profiles. We observed that the harmonic cutoff could be extended with the variation of the sub-cycle pulse duration, mainly because of the inherent blueshift associated with shorter pulses. The scaling laws for the harmonic yield and harmonic cutoff energy with pulse duration and fundamental driver wavelengths are also deduced…
Present photoionization experiments cannot measure molecular frame photoelectron angular distributions (MFPAD) from the outermost valence electrons of molecules. We show that details of the MFPAD can be retrieved with high-order harmonics generated by infrared lasers from aligned molecules. Using accurately calculated photoionization transition dipole moments for fixed-in-space molecules, we show that the dependence of the magnitude and phase of the high-order harmonics on the alignment angle of the molecules observed in recent experiments can be quantitatively reproduced. This result provides…
We illustrate an iterative method for retrieving the internuclear separations of N$_2$, O$_2$ and CO$_2$ molecules using the high-order harmonics generated from these molecules by intense infrared laser pulses. We show that accurate results can be retrieved with a small set of harmonics and with one or few alignment angles of the molecules. For linear molecules the internuclear separations can also be retrieved from harmonics generated using isotropically distributed molecules. By extracting the transition dipole moment from the high-order harmonic spectra, we further demonstrated that it is p…
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…
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…
It is demonstrated by single-atom simulations that X-ray signals in the 3.4 to 4 keV region from an 8 micron laser driven high harmonic generation can be increased by more than two orders of magnitude when a single-cycle pulse centered at 800 nm is added. The ionization probability of a helium atom by the two-pulse field is set to 4.56x10^-5, which is needed for balancing the index of refraction of free electrons with that of neutral helium atoms to achieve phase matching.
We present numerical simulations of high-order harmonic generation in helium using a temporally synthesised and spatially non-homogeneous strong laser field. The combination of temporal and spatial laser field synthesis results in a dramatic cut-off extension far beyond the usual semiclassical limit. Our predictions are based on the convergence of three complementary approaches: resolution of the three dimensional Time Dependent Schrödinger Equation, time-frequency analysis of the resulting dipole moment and classical trajectories extraction. Employing a combination of temporally and spatially…
High-harmonic generation from muonic atoms exposed to intense laser fields is considered. Our particular interest lies in effects arising from the finite nuclear mass and size. We numerically perform a fully quantum mechanical treatment of the muon-nucleus dynamics by employing modified soft-core and hard-core potentials. It is shown that the position of the high-energy cutoff of the harmonic spectrum depends on the nuclear mass, while the height of the spectral plateau is sensitive to the nuclear radius. We also demonstrate that $γ$-ray harmonics can be generated from muonic atoms in ultrastr…
We theoretically study high-order harmonic generation (HHG) from solid-phase systems in spatially inhomogeneous strong laser fields originated by resonant plasmons within a metallic nanostructure. The intensity of the second plateau in HHG may be enhanced by two-three orders and be comparable with the intensity of the first plateau. This is due to bigger transition probabilities to higher conduction bands. It provides us a practical way to increase the yields of HHG with laser intensity below the damage threshold. It presents a promising way to triple the range of HHG spectra in experimental m…
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$_2^+$…
We investigate the electron quantum path interference effects during high harmonic generation in atomic gas medium driven by ultrashort chirped laser pulses. To achieve that, we identify and vary the different experimentally relevant control parameters of such a driving laser pulse influencing the high harmonic spectra. Specifically, the impact of the pulse duration, peak intensity and instantaneous frequency is studied in a self-consistent manner based on Lewenstein formalism. Simulations involving macroscopic propagation effects are also considered. The study aims to reveal the microscopic b…
We report on the investigation on harmonic-seeded remote laser emissions at 391 nm wavelength from strong-field ionized nitrogen molecules in three different gas mixtures, i.e., N2-Ar, N2-Xe and N2-Ne. We observed a decrease in the remote laser intensity in the N2-Xe mixture because of the decreased clamped intensity in the filament; whereas in the N2-Ne mixture, the remote laser intensity slightly increases because of the increased clamped intensity within the filament. Remarkably, although the clamped intensity in the filament remains nearly unchanged in the N2-Ar mixture because of the simi…
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.
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…
High-order harmonic generation (HHG) by hydrogenlike atoms/ions in the uniform periodic electric field, formed by the two linearly polarized counterpropagating laser beams of relativistic intensities, is studied. The relativistic quantum theory of HHG in such fields, at which the impeding factor of relativistic magnetic drift of a strong wave can be eliminated, is presented arising from the Dirac equation. Specifically, a scheme of HHG in underdense plasma with the copropagating ultraintense laser and fast ion beams is proposed.
High-order harmonic generation (HHG) is investigated for H$_2^+$ and its isotopomers under seven- and ten-cycle trapezoidal laser pulses at 800 nm wavelength and $I$=4$\times 10^{14}$ W$/$cm$^2$ intensity. We solved numerically full-dimensional electronic time-dependent Schrödinger equation with and without the Born-Oppenheimer approximation. We show that the HHG at the falling edge of a trapezoidal laser pulse can result in redshift and complexity on the total HHG spectrum which can be removed by considering different laser pulse duration and nuclear motion not possible for sin$^2$ and Gaussi…
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 explore the significance of laser-induced correlation effects for high-order harmonic generation (HHG) in a linear chain model of a generic band gap material for both single-IR-pulse and VUV-pump--IR-probe HHG schemes. We examine various pump-pulse excitations, and catagorize signatures of laser-induced correlation effects into two classes related to edge-state and bulk-like effects. The relative importance of the edge-state effects decrease with increasing system-size, while the bulk-like effects remain. We identify regimes where these effects may alter the harmonic yield by an order of ma…
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 study the effect of gas pressure on the generation of high-order harmonics where harmonics due to individual atoms are calculated using the recently developed quantitative rescattering theory, and the propagation of the laser and harmonics in the medium is calculated by solving the Maxwell's wave equation. We illustrate that the simulated spectra are very sensitive to the laser focusing conditions at high laser intensity and high pressure since the fundamental laser field is severely reshaped during the propagation. By comparing the simulated results with several experiments we show that th…
We present a method to distinguish the high harmonics generated in individual half-cycle of the driving laser pulse by mixing a weak ultraviolet pulse, enabling one to observe the cutoff of each half-cycle harmonic. We show that the detail information of the driving laser pulse, including the laser intensity, pulse duration and carrier-envelope phase, can be {\it in situ} retrieved from the harmonic spectrogram. In addition, our results show that this method also distinguishes the half-cycle high harmonics for a pulse longer than 10 fs, suggesting a potential to extend the CEP measurement to t…
The generation of high harmonics in laser-irradiated light homonuclear diatomics (H2+, N2 and O2) compared to that in atomic counterparts (of nearly identical binding energy) is studied within the velocity gauge version of conventional strong-field approximation. The applied strong-field approach (we alternatively developed earlier to incorporate rescattering effects beyond the conventional saddle-point approximation) is currently extended to molecular case by means of supplement the standard linear combination of atomic orbitals} and molecular orbitals method. The associated model proved to a…
