Using the Hubbard model we study how the process of high-order harmonic generation (HHG) is modified by beyond mean-field electron-electron correlation for both finite and bulk systems. A finite-size enhancement of the HHG signal is found and attributed to electrons backscattering off the lattice edges. Additionally, with increasing strength of the electron-electron correlation an enhancement of the high-frequency regime of the HHG spectrum is found. This is attributed to the on-site Coulomb repulsion between electrons giving rise to a localized quiver motion of the electrons. The finite-lattice enhancement dominates the HHG spectra from a few harmonic orders until a threshold from which the correlational enhancement dominates. This threshold is determined by the degree of correlation and decreases into the low-frequency regime for increasing electron-electron correlation. This infers that as the Mott insulator limit of high electron-electron correlation is approached, the finite-size effect on the electron dynamics becomes negligible.
We study high-order harmonic generation (HHG) driven by seeded plasmonic-enhanced fields. On one hand, plasmonic-enhanced fields have shown a great potential to extend the HHG cutoff, an instrumental pre-requisite for the generation of attosecond pulses. On another hand, the use of XUV seeds appears to have a considerable potential to improve the HHG conversion efficiency, which is typically modest when a unique fundamental laser pulse is employed. By mixing these two sources, we show it is possible to, simultaneously, boost the HHG cutoff and to increase the harmonic photon flux. The combinat…
A three step model for high harmonic generation from impurities in solids is developed. The process is found to be similar to high harmonic generation in atomic and molecular gases with the main difference coming from the non-parabolic nature of the bands. This opens a new avenue for strong field atomic and molecular physics in the condensed matter phase. As a first application, our conceptual study demonstrates the feasibility of tomographic measurement of impurity orbitals.
We show that two-color high-harmonic spectroscopy can reveal finite-size and edge-state-induced dynamic electron correlation effects in a generic nanostructured band-gap material. Compared to the response of a bulk sample, we demonstrate a significant correlation-induced increase in the efficiency of the generated signal over a wide range of frequencies by harnessing the power of these ultrafast many-electron dynamics.
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…
Theoretical studies of high-harmonic generation: Effects of symmetry, degeneracy and orientation
利用量子力学三步模型对四个多原子分子的高次谐波产生进行了数值计算。乙烯（C $_2$ H $_4$）用作其中轨道对称性直接影响谐波产率的实例。我们处理的情况下，甲烷（CH $_4$），以解决高谐波产生与简并轨道的分子。为此，我们说明了如何单轨道的贡献显示在总的高谐波信号。这个例子说明了从单个简并轨道相干地增加振幅贡献的重要性。最后，我们研究了丙烷（C $_3$ H $_8$）和丁烷（C $_4$ H $_{10}$）的高次谐波产生。这两个分子，被扩展和远离球形的结构，产生谐波与非平凡的取向依赖性。特别是，丙烷可以定向，使非常高的频率谐波被分解，因此该分子包含产生紫外阿秒脉冲的前景。
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 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.
The generation of the below threshold harmonics (BTHs) under different driving laser intensities is investigated. The linearly shifting of photon energy and resonantly enhancement of photon yield of the harmonics from 23rd (H23) to 27th (H27) are found by changing the laser intensity around 18.6 TW/cm2. It is identified that this driving laser intensity dependence is due to the transient ac Stark-shifted resonance between the first excited state and the ground state. With this transient ac Stark, the linearly shifting of the photon energy can be interpreted very well by considering the sub-cyc…
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 investigate the role of excited states in High-order Harmonic Generation by studying the spectral, spatial and temporal characteristics of the radiation produced near the ionization threshold of argon by few-cycle laser pulses. We show that the population of excited states can lead either to direct XUV emission through Free Induction Decay or to the generation of high-order harmonics through ionization from these states and recombination to the ground state. By using the attosecond lighthouse technique, we demonstrate that the high-harmonic emission from excited states is temporally delayed…
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…
We report a study of high harmonic generation from noble gas clusters of xenon atoms in a gas jet. Harmonic spectra were investigated as a function of backing pressure, showing spectral shifts due to the nanoplasma electrons in the clusters. At certain value of laser intensity this process may oppose the effect of the well-known ionization-induced blueshift. In addition, these cluster-induced harmonic redshifts may give the possibility to estimate cluster density and cluster size in the laser-gas jet interaction range.
We report the generation of five phase-locked harmonics, f_1: 2403 nm, f_2: 1201 nm, f_3: 801 nm, f_4: 600 nm, and f_5: 480 nm with an exact frequency ratio of 1 : 2 : 3 : 4 : 5 by implementing a divide-by-three optical-frequency divider in the high harmonic generation process. All five harmonics are generated coaxially with high phase coherence in time and space, which are applicable for various practical uses.
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 demonstrate the capability of ab-initio time-dependent R-matrix theory to obtain accurate harmonic generation spectra of noble-gas atoms at Near-IR wavelengths between 1200 and 1800 nm and peak intensities up to 1.8 X 10(14) W/cm(2) . To accommodate the excursion length of the ejected electron, we use an angular-momentum expansion up to Lmax = 279. The harmonic spectra show evidence of atomic structure through the presence of a Cooper minimum in harmonic generation for Kr, and of multielectron interaction through the giant resonance for Xe. The theoretical spectra agree well with those obta…
We present a complete theory of bicircular high-order-harmonic emission from N-fold rotationally symmetric molecules. Using a rotating frame of reference we predict the complete structure of the high-order-harmonic spectra for arbitrary driving frequency ratios and show how molecular symmetries can be directly identified from the harmonic signal. Our findings reveal that a characteristic fingerprint of rotational molecular symmetries can be universally observed in the ultrafast response of molecules to strong bicircular fields.
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…
High-harmonic generation by a laser-driven solid slab is simulated using time-dependent density functional theory. Multiple harmonic plateaus up to very high harmonic orders are observed already at surprisingly low field strengths. The full all-electron harmonic spectra are, in general, very different from those of any individual Kohn-Sham orbital. Freezing the Kohn-Sham potential instead is found to be a good approximation for the laser intensities and harmonic orders considered. The origins of the plateau cutoffs are explained in terms of band gaps that can be reached by Kohn-Sham electrons …
We observe the generation of high harmonics in the plane perpendicular to the driving laser polarization and show that these are driven by the spin-orbit interaction. Using R-Matrix with time-dependence theory, we demonstrate that for certain initial states either circularly- or linearly- polarized harmonics arise via well-known selection rules between atomic states controlled by the spin-orbit interaction. Finally, we elucidate the connection between the observed harmonics and the phase of the intial state.
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.
