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 equation, for the case of H$_2^+$ in laser fields. The result illustrates that these powerful theoretical tools can be used for obtaining high-order harmonic spectra from molecules. More importantly, the results imply that the PRCS extracted from laser-induced HHG spectra can be used for time-resolved dynamic chemical imaging of transient molecules with temporal resolutions down to a few femtoseconds.
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.
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…
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 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…
We present a two-timescale Floquet method that allows one to apply the Kramers-Henneberger approach to short pulses and arbitrary laser frequencies. An efficient numerical procedure to propagate the Floquet Hamiltonian is provided that relies on the Toeplitz matrix formalism and Fast Fourier Transformations. It enables efficient time propagation with large Floquet expansions, while still taking advantage of the cycle-averaged Kramers-Henneberger basis. Three illustrative cases of ionization with different photon energies are analyzed, where the envelope of a short and intense pulse is crucial …
Experiments with cold molecules usually begin with a molecular source. We describe the construction and characteristics of a cryogenic buffer gas source of CaF molecules. The source emits pulses with a typical duration of 240 $μ$s, a mean speed of about 150 m/s, and a flux of $5\times 10^{10}$ molecules per steradian per pulse in a single rotational state.
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…
A simple model for sequential multiphoton ionization by ultra-intense x-rays is presented. The derived scaling of the ion yield with pulse energy quantitatively reproduces the experimental data, which shows that the ion yield increases according to the "power law" behavior typical of multiphoton ionization, followed by saturation at high pulse energies. The calculated average time interval between ionizations for producing ions at a certain charge state is found to be proportional to the pulse duration and independent of all other x-ray pulse parameters. This agrees with previous studies where…
This paper concerns the theory of non-recollisional ionization or detachment of atoms or ions by intense few-cycle pulses. It is shown that in certain conditions of pulse duration, peak intensity and carrier-envelope phase, the ionization probability integrated over ejection angle varies almost periodically with energy, with a period roughly equal to the photon energy for slow enough outgoing electrons. This modulation is found both in calculations based on the strong field approximation (SFA) and in ab initio time-dependent calculations. It is explained as resulting from the interference betw…
Ionization by relativistically intense laser pulses of finite duration is considered in the framework of strong-field quantum electrodynamics. Our main focus is on the formation of ionization supercontinua. More specifically, when studying the energy distributions of photoelectrons ionized by circularly polarized pulses, we observe the appearance of broad structures lacking the interference patterns. These supercontinua extend over hundreds of driving photon energies, thus corresponding to high-order nonlinear processes. The corresponding polar-angle distributions show asymmetries which are at…
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…
The photoionization of a helium atom by short intense laser pulses is studied theoretically in the vicinity of the $2s2p\,^1P$ doubly-excited state with the intention to investigate the impact of the intensity and duration of the exciting pulse on the dynamics of the autoionization process. For that purpose, we solve numerically the corresponding time-dependent Schrödinger equation by applying the time-dependent restricted-active-space configuration-interaction method (TD-RASCI). The present numerical results clearly demonstrate that the Fano-interferences can be controlled by a single high-fr…
We examine correlated electron and doubly charged ion momentum spectra from strong field double ionization of Neon employing intense elliptically polarized laser pulses. An ellipticity-dependent asymmetry of correlated electron and ion momentum distributions has been observed. Using a 3D semiclassical model, we demonstrate that our observations reflect the sub-cycle dynamics of the recollision process. Our work reveals a general physical picture for recollision-impact double ionization with elliptical polarization, and demonstrates the possibility of ultrafast control of the recollision dynami…
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…
We present a theoretical study of the ionization dynamics of a hydrogen atom exposed to attosecond laser pulses in the extreme ultra violet region at very high intensities. The pulses are such that the electron is expected to reach relativistic velocities, thus necessitating a fully relativistic treatment. We solve the time dependent Dirac equation and compare its predictions with those of the corresponding non-relativistic Schr{ö}dinger equation. We find that as the electron is expected to reach about 20% of the speed of light, relativistic corrections introduces a finite yet small decrease i…
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 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 study in detail the strong-field QED process of non-linear Compton scattering in short intense plane wave laser pulses of circular polarization. Our main focus is placed on how the spectrum of the back-scattered laser light depends on the shape and duration of the initial short intense pulse. Although this pulse shape dependence is very complicated and highly non-linear, and has never been addressed explicitly, our analysis reveals that all the dependence on the laser pulse shape is contained in a class of three-parameter master integrals. Here we present completely analytical expressions f…
We study the breakup of $\text{H}_2^+$ exposed to super-intense, femtosecond laser pulses with frequencies greater than that corresponding to the ionization potential. By solving the time-dependent Schrödinger equation in an extensive field parameter range, it is revealed that highly nonresonant dissociation channels can dominate over ionization. By considering field-dressed Born-Oppenheimer potential energy curves in the reference frame following a free electron in the field, we propose a simple physical model that characterizes this dissociation mechanism. The model is used to predict contro…
Ionization of hydrogen-like ions by intense, circularly polarized laser pulses is analyzed under the scope of the relativistic strong-field approximation. We show that, for specific parameters of the laser field, the energy spectra of photoelectrons present a broad region without interference (supercontinuum) which can be controlled by modifying the laser field intensity. The physical interpretation of the process is developed according to the Keldysh theory, emphasizing the importance of the complex-time saddle point contributions to the total probability of photoionization. The corresponding…
The generation of electron vortex states in ionization by intense and short laser pulses is analyzed under the scope of the lowest-order Born approximation. For near infrared laser fields and nonrelativistic intensities of the order of $10^{16}$~W/cm$^2$, we show that one has to modify the nonrelativistic treatment of ionization by accounting for recoil and mass relativistic corrections. By using the corrected quasi-relativistic theory, the requirements for the observation of electron vortex states with non-negligible probability and large topological charge are determined.
Double photoelectron emission from He atoms by intense laser pulses with a wave length of $394.5\,nm$ is computed for intensities $3.5 - 9.2\times 10^{14}W/cm^2$. Joint momentum distributions confirm the characteristics seen in classical trajectory calculations. The pronounced transition from back-to-back to side-by-side emission with increasing intensity, the $He^{++}/He^+$ ratios, and a modulation of joint energy spectra agree well with a recent experiment [Henrichs et al., PRA 98, 43405 (2018)], if one admits an increase of experimental intensities by a factor $\sim 2$. We find that Freeman…
A unitary model describing the electronic transitions in an atom subject to a strong high frequency laser pulse is proposed. The model fully accounts for the initial state coupling with the continuum spectrum. Continuum-continuum as well as discrete-discrete transitions are neglected. The model leads to a single integro-differential equation for the initial state amplitude. Exact numerical and approximate closed semi-analytical solutions of this equation are obtained. A comparison of present results with full time dependent Schrödinger equation solution for Hydrogen atoms subject to a laser pu…
Strong-field approximation for Coulomb explosion of H_2^+ by short intense laser pulses
提出了一个简单的量子力学模型来描述H $_2^+$在短脉冲强红外激光作用下的库仑爆炸。该模型是基于长度规范版本的分子强场近似，是有效的脉冲短于50 fs的电离前的解离过程是可以忽略不计的。并与最近的质子能谱实验结果作了比较[I]。Ben-Itzhak等人，物理修订版信函95，073002（2005），B. D. Esry等人，物理修订版信函97，013003（2006）]。尽管峰值能量略低于观测值，但模型的预测再现了光谱的轮廓。为了比较，我们还提出了两种不同的隧道模型，这个过程中得到的结果。
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 study the Compton scattering of x-rays off electrons that are driven by a relativistically intense short optical laser pulse. The frequency spectrum of the laser-assisted Compton radiation shows a broad plateau in the vicinity of the laser-free Compton line due to a nonlinear mixing between x-ray and laser photons. Special emphasis is placed on how the shape of the short assisting laser pulse affects the spectrum of the scattered x-rays. In particular, we observe sharp peak structures in the plateau region, whose number and locations are highly sensitive to the laser pulse shape. These stru…
Modern laser systems are able to generate short and intense laser pulses ionizing matter in the poorly explored barrier-suppression regime. Field ionization in this regime is studied analytically and numerically. For analytical studies, both the classical and the quantum approaches are used. Two approximations to solve the time-dependent Schrödinger equation are proposed: the free electron approximation, in which the atomic potential is neglected, and the motionless approximation, in which only the external field term is considered. In the motionless approximation, the ionization rate in extre…
Classically allowed transport is shown to compete with quantum tunneling during the ionization of atoms by ultrashort and intense laser pulses, despite Keldysh parameters smaller than unity. This is done by comparing exact probability densities with the ones obtained from purely classical propagation using the Truncated Wigner Approximation. Not only is classical transport capable of moving trajectories away from the core, but it can also furnish ionization probabilities of the same order as the quantum ones for intensities currently employed in experiments. Our results have implications rangi…
