We perform a detailed analysis of high-order harmonic generation in diatomic molecules within the strong-field approximation, with emphasis on quantum-interference effects. Specifically, we investigate how the different types of electron orbits, involving one or two centers, affect the interference patterns in the spectra. We also briefly address the influence of the choice of gauge, and of the initial and final electronic bound states on such patterns. For the length-gauge SFA and undressed bound states, there exist additional terms, which can be interpreted as potential energy shifts. If, on the one hand, such shifts alter the potential barriers through which the electron initially tunnels, and may lead to a questionable physical interpretation of the features encountered, on the other hand they seem to be necessary in order to reproduce the overall maxima and minima in the spectra. Indeed, for dressed electronic bound states in the length gauge, or undressed bound states in the velocity gauge, for which such shifts are absent, there is a breakdown of the interference patterns. In order to avoid such a problem, we provide an alternative pathway for the electron to reach the continuum, by means of an additional attosecond-pulse train. A comparison of the purely monochromatic case with the situation for which the attosecond pulses are present suggests that the patterns are due to the interference between the electron orbits which finish at different centers, regardless of whether one or two centers are involved.
In the present paper, we investigate the high-order harmonic generation (HHG) from diatomic molecules with large internuclear distance using a strong field approximation (SFA) model. We find that the hump and dip structure emerges in the plateau region of the harmonic spectrum, and the location of this striking structure is sensitive to the laser intensity. Our model analysis reveals that two-center interference as well as the interference between different recombination electron trajectories are responsible for the unusual enhanced or suppressed harmonic yield at a certain order, and these in…
The generation of high-order harmonics in diatomic molecules is investigated within the framework of the strong-field approximation. We show that the conventional saddle-point approximation is not suitable for large internuclear distances. An adapted saddle-point method that takes into account the molecular structure is presented. We analyze the predictions for the harmonic-generation spectra in both the velocity and the length gauge. At large internuclear separations, we compare the resulting cutoffs with the predictions of the simple-man's model. Good agreement is obtained only by using the …
We calculate angle-resolved above-threshold ionization spectra for diatomic molecules in linearly polarized laser fields, employing the strong-field approximation. The interference structure resulting from the individual contributions of the different scattering scenarios is discussed in detail, with respect to the dependence on the internuclear distance and molecular orientation. We show that, in general, the contributions from the processes in which the electron is freed at one center and rescatters off the other obscure the interference maxima and minima obtained from single-center processe…
We present a theoretical model of high-harmonic generation from diatomic molecules. The theory includes effects of alignment as well as nuclear motion and is used to predict results for N$_2$, O$_2$, H$_2$ and D$_2$. The results show that the alignment dependence of high-harmonics is governed by the symmetry of the highest occupied molecular orbital and that the inclusion of the nuclear motion in the theoretical description generally reduces the intensity of the harmonic radiation. We compare our model with experimental results on N$_2$ and O$_2$, and obtain very good agreement.
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 address the influence of the orbital symmetry and of the molecular alignment with respect to the laser-field polarization on laser-induced nonsequential double ionization of diatomic molecules, in the length and velocity gauges. We work within the strong-field approximation and assume that the second electron is dislodged by electron-impact ionization, and also consider the classical limit of this model. We show that the electron-momentum distributions exhibit interference maxima and minima due to the electron emission at spatially separated centers. The interference patterns survive the in…
We investigate high-order harmonic spectra from aligned diatomic molecules in intense driving fields whose components have orthogonal polarizations. We focus on how the driving-field ellipticity influences structural interference patterns in a macroscopic medium. In a previous publication [Phys. Rev. A 88, 023404 (2013)] we have shown that the non-vanishing ellipticity introduces an effective dynamic shift in the angle for which the two-center interference maxima and minima occur, with regard to the existing condition for linearly polarized fields. In this work we show through simulation that …
We analyze the influence of different recombination scenarios, involving one or two centers, on high-order harmonic generation (HHG) in diatomic molecules, for different values of the internuclear separation. We work within the strong-field approximation, and employ modified saddle-point equations, in which the structure of the molecule is incorporated. We find that the two-center interference patterns, attributed to high-order harmonic emission at spatially separated centers, are formed by the quantum interference of the orbits starting at a center $C_{j}$ and finishing at a different center …
We analyze the imprint of nodal planes in high-order harmonic spectra from aligned diatomic molecules in intense laser fields whose components exhibit orthogonal polarizations. We show that the typical suppression in the spectra associated to nodal planes is distorted, and that this distortion can be employed to map the electron's angle of return to its parent ion. This investigation is performed semi-analytically at the single-molecule response and single-active orbital level, using the strong-field approximation and the steepest descent method. We show that the velocity form of the dipole op…
The single ionization of noble gas atoms by the combined action of XUV attopulses and an infrared laser field is theoretically investigated by means of a non-perturbative model that under certain approximations gives closed-form expressions for the angular distributions of photoelectrons. Interestingly, our model allow us to interpret the angular distributions as two-center interferences where the separation between the centers is governed by the infrared laser field. Angular distributions are compared to the available experimental data showing a good agreement. Finally, we deduce the conditio…
The generation of high harmonics (HHG) in atomic systems by the highly non-linear response to an intense laser field is a prominent pathway to the synthesis of ever shorter laser pulses at increasingly higher photon energies. Extensions of this process to molecules add to the complexity but also offers novel opportunities as multi-center effects and the coupling to nuclear degrees of freedom can influence HHG. In this work we theoretically explore the impact of coherent vibronic excitations of diatomic molecules on the HHG spectrum within the framework of time-dependent density functional theo…
We investigate the influence of intense, elliptically polarized driving fields on high-order harmonic spectra from aligned diatomic molecules. We derive a generalized two-center interference condition for elliptically polarized fields, which accounts for s-p mixing and the orbital symmetry, within the strong-field and the single-active electron approximation. We show that the non-vanishing ellipticity introduces an effective dynamic shift in the angle for which the two-center interference maxima and minima occur, with regard to the existing condition for linearly polarized fields. This shift d…
Electron quantum path interferences in strongly laser-driven aligned molecules and their dependence on the molecular alignment is an essential open problem in strong-field molecular physics. Here, we demonstrate an approach which provides direct access to the observation of these interference processes. The approach is based on the combination of the time-gated-ion-microscopy technique with a pump-probe arrangement used to align the molecules and generate high-order harmonics. By spatially resolving the interference pattern produced by the spatiotemporal overlap of the harmonics emitted by the…
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…
We address the influence of the molecular orbital geometry and of the molecular alignment with respect to the laser-field polarization on laser-induced nonsequential double ionization of diatomic molecules for different molecular species, namely $\mathrm{N}_2$ and $\mathrm{Li}_2$. We focus on the recollision excitation with subsequent tunneling ionization (RESI) mechanism, in which the first electron, upon return, promotes the second electron to an excited state, from where it subsequently tunnels. We show that the electron-momentum distributions exhibit interference maxima and minima due to t…
We investigate laser-induced nonsequential double ionization from aligned diatomic molecules, using the strong-field approximation in its length and velocity gauge formulations. Throughout, we consider that the first electron dislodges the second by electron-impact ionization. Employing modified saddle-point equations, we single out the contributions of different scattering scenarios to the maxima and minima observed in the differential electron momentum distributions. We show that the quantum interference between the electron orbits starting and ending at a specific center $C_{j}$%, and those…
The direct above-threshold ionization (ATI) of diatomic molecules in linearly-polarized infrared and extreme ultraviolet (IR+XUV) laser fields is investigated by the frequency-domain theory based on the nonperturbative quantum electrodynamics. The destructive interference fringes on the angle-resolved ATI spectra, which are closely related to the molecular structure, can be well fitted by a simple predictive formula for any alignment of the molecular axis. By comparing the direct ATI spectra for monochromatic and two-color laser fields, we found that the XUV laser field can both raise the ioni…
Diatomic molecules (e.g., O$_2$) in intense laser field exhibit a peculiar suppressed ionization behavior compared to their companion atoms. Several physical models have been proposed to account for this suppression while no consensus has been achieved. In this letter, we aim to clarify the underlying mechanisms behind this molecular ionization suppression. Experimental data recorded at midinfrared laser wavelength and its comparison with that at near-infrared wavelength revealed a peculiar wavelength and intensity dependence of the suppressed ionization of O$_2$ with respect to its companion …
The elastic scattering of twisted electrons by diatomic molecules is studied within the framework of the non-relativistic first Born approximation. In this process, the coherent interaction of incident electrons with two molecular centers may cause interference patterns in the angular distributions of outgoing particles. We investigate how this Young-type interference is influenced by the complex internal structure of twisted beams. In particular, we show that the corkscrew-like phase front and the inhomogeneous intensity profile of the incident beam can strongly modify the angular distributio…
We investigate theoretically the dissociative ionization of a H2+ molecule using two ultrashort laser (pump-probe) pulses. The pump pulse prepares a dissociating nuclear wave packet on an ungerade surface of H2+. Next, an UV (or XUV) probe pulse ionizes this dissociating state at large (R = 20 - 100 bohr) internuclear distance. We calculate the momenta distributions of protons and photoelectrons which show a (two-slit-like) interference structure. A general, simple interference formula is obtained which depends on the electron and protons momenta, as well as on the pump-probe delay on the puls…
For a molecule, the two-center interference and the molecular scattering phase of the electron are important for almost all the processes that may occur in a laser field. In this study, we investigate their effects in the transfer of linear photon momentum to the ionized electron by absorbing a single photon. The time-dependent Schrödinger equation of H$_2^+$ is numerically solved in {the multipolar} gauge in which the electric quadrupole term and the magnetic dipole term are explicitly expressed. This allows us to separate the contributions of the two terms in the momentum transfer. For diffe…
We present an implementation of a time-dependent multiconfiguration self-consistent-field (TD-MCSCF) method [R. Anzaki et al., Phys. Chem. Chem. Phys. 19, 22008 (2017)] with the full configuration interaction expansion for coupled electron-nuclear dynamics in diatomic molecules subject to a strong laser field. In this method, the total wave function is expressed as a superposition of different configurations constructed from time-dependent electronic Slater determinants and time-dependent orthonormal nuclear basis functions. The primitive basis functions of nuclei and electrons are strictly in…
We consider harmonics generation and wave-mixing by two-color multi photon resonant excitation of three-level atoms/molecules in strong laser fields. The coherent part of the spectra corresponding to multicolor harmonics generation is investigated. The obtained analytical results on the basis of generalized rotating wave approximation are in a good agreement with numerical calculations. The results applied to the hydrogen atom and homonuclear diatomic molecular ion show that one can achieve efficient generation of moderately high multicolor harmonics via multiphoton resonant excitation by appr…
In this work we report ab initio calculations for the $H_2^+$ molecule interacting with ultrashort intense laser pulses. We analyse several observables that can, in principle, be available experimentally, in order to get a deeper understanding of the strong field molecular dynamics. In particular, we will focus our attention to the interplay between electronic and nuclear dynamics and how the two motions are correlated. We have extended the Resolvent Technique to molecules and we have extracted the correlated energy spectra in different regimes of ionization: from the perturbative regime to th…
Experiments have shown that the internal vibrational state of a molecule can affect the intensity of high harmonic light generated from that molecule. This paper presents a model which explains this modulation in terms of interference between different vibrational states occurring during the high harmonic process. In addition, a semiclassical model of the continuum electron propagation is developed which connects with rigorous treatments of the electron-ion scattering.
We study ionization dynamics of aligned diatomic molecules N$_2$ in strong elliptical laser fields experimentally and theoretically. The alignment dependence of photoelectron momentum distributions (PMDs) of N$_2$ measured in experiments is highlighted with comparing to Ar measured synchronously. Our results show that the PMDs of N$_2$ depend strongly on the alignment of the molecule, relative to the main axis of the laser ellipse. In particular, the most-probable electron-emission angle which is often used in attosecond measurement, differs remarkably when changing the molecular alignment. We…
We investigate the influence of the autoionizing 3s3p(6)nl resonances on the fifth harmonic generated by 200 - 240 nm laser fields interacting with Ar. To determine the influence of a multi-electron response we have developed capability within time dependent R-matrix theory to determine the harmonic spectra generated. The fifth harmonic is affected by interference between the response of a 3s electron and the response of a 3p electron, as demonstrated by the asymmetric profiles in the harmonic yields as functions of wavelength.
We present a theoretical investigation into the two-center interference in aligned H$_2^+$. The influence of the laser field on the recombination step is investigated by comparing laser-induced harmonic generation with harmonic generation from field-free collisions of Gaussian wave packets with the core. We find that for different Gaussian wave packets colliding with the molecule, the interference minimum occurs at the same alignment angle. The same result is obtained for the laser-induced spectrum when only a single electronic trajectory per harmonic contributes. When multiple electronic traj…
By using Bohmian trajectory method, we investigate the dynamic interference in diatomic molecular high-order harmonic generation progress. It is demonstrated that the main characteristics of the molecular harmonic spectrum can be well reproduced by only two Bohmain trajectories which are located respectively at the two ions. This is because these two localized trajectories can receive and store the whole collision information coming from all of the other recollision trajectories. Therefore, the amplitudes and frequencies of these two trajectories represent the intensity and frequency distribut…
We report on calculations of harmonic generation by neon in a mixed (800-nm + time-delayed 400-nm) laser pulse scheme. In contrast with previous studies we employ a short (few-cycle) 400-nm pulse, finding that this affords control of the interference between electron trajectories contributing to the cutoff harmonics. The inclusion of the 400-nm pulse enhances the yield and cutoff energy, both of which exhibit a strong dependence on the time delay between the two pulses. Using a combination of time-dependent R-matrix theory and a classical trajectory model, we assess the mechanisms leading to t…
High-order harmonic generation (HHG) is investigated theoretically in the over-the-barrier ionization (OBI) regime revealing the strong signature of interference between two separately ionized and separately propagating free wave packets of a single electron. The interference leads to the emission of coherent light at a photon energy corresponding to the kinetic-energy difference of the two recolliding electron quantum paths, thus complementary to the well-known classical three-step picture of HHG. As will be shown by time-frequency analysis of the emitted radiation, the process entirely domin…
We investigate how short and long electron trajectory contributions to high harmonic emission and their interferences give access to intra-molecular dynamics. In the case of unaligned molecules, we show experimental evidences that the long trajectory signature is more dependent upon the molecule than the short one, providing a high sensitivity to cation nuclear dynamics within 100's of as to few fs. Using theoretical approaches based on Strong Field Approximation and Time Dependent Schrodinger Equation, we examine how quantum path interferences encode electronic motion whilst molecules are ali…
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 present an experimental technique using orbital angular momentum (OAM) in a fundamental laser field to drive High Harmonic Generation (HHG). The mixing of beams with different OAM allows to generate two laser foci tightly spaced to study the phase and amplitude of HHG produced in diatomic nitrogen. Nitrogen is used as a well studied system to show the quality of OAM based HHG interferometry.
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…
We describe phase-dependent wavelength scaling of high-order harmonic generation efficiency driven by ultra-short laser fields in the mid-infrared. We employ both numerical solution of the time-dependent Schrödinger equation and the Strong Field Approximation to analyze the fine-scale oscillations in the harmonic yield in the context of channel-closing effects. We show, by varying the carrier-envelope phase, that the amplitude of these oscillations depend strongly on the number of returning electron trajectories. Furthermore, the peak positions of the oscillations vary significantly as a funct…
We investigated the high-order harmonic generation (HHG) process of diatomic molecular ion $\mathrm{H}_2^+$ in non-Born-Oppenheimer approximations. The corresponding three-dimensional time-dependent Schrödinger equation is solved with arbitrary alignment angles. It is found that the nuclear motion can lead to spectral modulation of HHG. Redshifts are unique in molecular HHG which decrease with the increase of alignment angles of the molecules and are sensitive to the initial vibrational states. It can be used to extract the ultrafast electron-nuclear dynamics and image molecular structure.
We consider a quantum mechanical model for the high-order harmonic generation in bulk solids. The bandgap is assumed to be considerably larger than the exciting photon energy. Using dipole approximation, the dynamical equations for different initial Bloch states are decoupled in the velocity gauge. Although there is no quantum mechanical interference between the time evolution of different initial states, the complete harmonic radiation results from the interference of fields emitted by all the initial (valence band) states. In particular, this interference is shown to be responsible for the s…
We extend a model of two-center interference to include the superposition of opposite orientations in aligned polar molecules. We show that the position of the minimum in the harmonic spectrum from both aligned and oriented CO depends strongly on the relative recombination strength at different atoms, not just the relative phase. We reinterpret the minimum in aligned CO as an interference between opposite orientations, and obtain good agreement with numerical calculations. Inclusion of the first-order Stark effect shifts the position of the interference minimum in aligned CO even though aligne…
Chemical reactions at ultracold temperatures are expected to be dominated by quantum mechanical effects. Although progress towards ultracold chemistry has been made through atomic photoassociation, Feshbach resonances and bimolecular collisions, these approaches have been limited by imperfect quantum state selectivity. In particular, attaining complete control of the ground or excited continuum quantum states has remained a challenge. Here we achieve this control using photodissociation, an approach that encodes a wealth of information in the angular distribution of outgoing fragments. By phot…
The double-slit interference in single-photon ionization of the diatomic molecular ion $\mathrm{H}_2^+$ is theoretically studied beyond the dipole approximation. Via simulating and comparing the interactions of the prealigned $\mathrm{H}_2^+$ and the hydrogen atom with the xuv pulses propagating in different directions, we illustrate two kinds of effects that are encoded in the interference patterns of the photoelectrons from $\mathrm{H}_2^+$: (i) the photon-momentum transfer and (ii) the finite speed of light. While both effects could modify the maxima of the interference fringes, we show tha…
We investigate the dependence of the intensity of radiation due to high-harmonic generation (HHG) as a function of the wavelength of the fundamental driver field. Superimposed on a smooth power-law dependence observed previously we find surprisingly strong and rapid fluctuations on a fine wavelength scale. We identify the origin of these fluctuations in terms of quantum path interferences with up to five returning orbits significantly contributing.
We theoretically investigate the interference effect of high-order harmonics generated from molecules at different alignment angles. It is shown that the interference of the harmonic emissions from molecules aligned at different angles can significantly modulate the spectra and result in the anomalous harmonic cutoffs observed in a recent experiment [ Nature Phys. 7, 822 (2011) ]. The shift of the spectral minimum position with decreasing the degree of alignment is also explained by the interference effect of the harmonic emissions.
The spectrum of higher harmonics in atoms calculated with a uniformized semiclassical propagator is presented and it is shown that higher harmonic generation is an interference phenomenon which can be described semiclassically. This can be concluded from the good agreement with the quantum spectrum. Moreover, the formation of a plateau in the spectrum is specifically due to the interference of irregular, time delayed, trajectories with regular orbits without a time-delay. This is proven by the absence of the plateau in an artificial semiclassical spectrum generated from a sample of trajectorie…
Explicit algebraic expressions for the expansion of the vibrational matrix elements in series of matrix elements on the wave functions of the ground vibrational state have been obtained for arbitrary sufficiently differentiable functions of the internuclear distance, arbitrary values v and v', and the potential curves whose ladder operators can be constructed. A diagram technique have been developed for it that consists in: 1) the numeration of the matrix elements by points of the 2D diagram with coordinates (l, k), 2) the drawing arrows between points of this diagram corresponding to the acti…
An algebraic model taking into account the influence of the molecular rotation on the wave functions of vibrational-rotational states of the diatomic molecule using the formalism of the ladder operators and an expansion in a small parameter characterizing the vibrational-rotational interaction have been proposed for the potentials whose the creation and annihilation operators can be constructed. Expressions for the expansion of the wave function of the vibrational-rotational states in a set of wave functions of the rotationless vibrational states have been obtained of the second order in the p…
We investigate direct above-threshold ionization in diatomic molecules, with particular emphasis on how quantum interference is altered by a driving field of non-vanishing ellipticity. This interference may be either temporal, i.e., related to ionization events occurring at different times, or spatial, i.e., related to the electron emission at different centers in the molecule. Employing the strong-field approximation and saddle-point methods, we find that, in general, for non-vanishing ellipticity, there will be a blurring of the temporal and spatial interference patterns. The former blurring…
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 experimentally disentangle the contributions of different quantum paths in high-order harmonic generation (HHG) from the spectrally and spatially resolved harmonic spectra. By adjusting the laser intensity and focusing position, we simultaneously observe the spectrum splitting, frequency shift and intensity-dependent modulation of harmonic yields both for the short and long paths. Based on the simulations, we discriminate the physical mechanisms of the intensity-dependent modulation of HHG due to the quantum path interference and macroscopic interference effects. Moreover, it is shown that …
We investigate the contributions from the $3σ_{g}$ and $1π_{u}$ and molecular orbitals in high-order harmonic generation in $N_{2}$, with particular emphasis on quantum-interference effects. We consider both the physical processes in which the electron is freed and returns to the same orbital, and those in which it is ionized off one orbital and recombines with the other. We show that the quantum-interference patterns observed in the high-order harmonic spectra are predominantly determined by the $3σ_{g}$ orbital. This holds both for the situation in which only the $1π_{ux}$ orbital is conside…
We study the signature of two-center interferences in molecular high-order harmonic spectra, with an emphasis on the spectral phase. With the help of both ab initio computations based on the time-dependent Schrödinger equation and the molecular Strong-Field Approximation (SFA) as developed by Chirila et al. [Physical Review A, 73, 023410 (2006)] and Faria [Physical Review A, 76, 043407 (2007)], we observe that the phase behavior is radically different for the short and the long trajectory contributions. By means of Taylor expansions of the molecular SFA, we link this effect to the dynamics of …
High-order harmonic generation (HHG) results from strong-field laser matter interaction and it is one of the main processes that are used to extract electron structural and dynamical information about the atomic or molecular targets with sub-femtosecond temporal resolution. Moreover, it is the workhorse for the generation of attosecond pulses. Here we develop an analytical description of HHG, which extends the well established theoretical strong-field approximation (SFA). Our approach involves two innovative aspects: i) First, using a model non-local, but separable potential, we calculate the …
We present a new theory that the molecular high order harmonic generation in an intense laser field is determined by molecular internal symmetry and momentum distribution of the tunneling-ionized electron. The molecular internal symmetry determines the quantum interference form of the returning electron inside the molecule. The electron momentum distribution determines the relative interference strength of each individual electron de Broglie wave. All individual electron de Broglie wave interferences add together to collectively modulate the molecular high harmonic generation. We specifically …
We investigate the effect on high-order harmonic generation of the distortion of molecular orbitals by the driving laser field. Calculations for high-order harmonic generation including orbital distortion are performed for N2. Our results allow us to suggest that field-distortion is the reason why the two-center interference minimum has never been observed experimentally in N2. We propose experimental parameters which should allow an observation of the two-center interference minimum.
Replacing the canonical pair q and p of the harmonic oscillator (HO) by the locally and symplectically equivalent pair angle phi and action variable I implies a qualitative change of the global topological structure of the associated phase spaces: the pair (q,p) is an element of a topologically trivial plane R^2 whereas the pair (phi,I>0) is an element of a topologically non-trivial, infinitely connected, punctured plane R^2-{0}, which has the group SO(1,2) as its "canonical" group. Due to its infinitely many covering groups the resulting ("symplectic") spectrum of the associated quantum Hamil…
We experimentally observe longer than long trajectory influence in high order harmonic generation (HHG) by varying the peak intensity of the driving laser field through either direct attenuation, or by chirping the laser pulse. Using a theoretical Gaussian beam model to simulate spatial interference resulting from quantum path interference we show that the measured interference patterns cannot be solely explained by the well established short and long trajectories. The structure change is most prominent for the more divergent, off-axis components of the lower plateau harmonic region, affecting…
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.
