Time-dependent ab initio approaches for high-harmonic generation spectroscopy

Author(s):  
Emanuele Coccia ◽  
Eleonora Luppi

Abstract High-harmonic generation (HHG) is a nonlinear physical process used for the production of ultrashort pulses in XUV region, which are then used for investigating ultrafast phenomena in time-resolved spectroscopies. Moreover, HHG signal itself encodes information on electronic structure and dynamics of the target, possibly coupled to nuclear degrees of freedom. Investigating HHG signal leads to HHG spectroscopy, which is applied to atoms, molecules, solids and recently also to liquids. Analysing the number of generated harmonics, their intensity and shape gives a detailed insight of, e.g., ionisation and recombination channels occurring in the strong-field dynamics. A number of valuable theoretical models has been developed over the years to explain and interpret HHG features, with the three-step model being the most known one. Originally, these models neglect the complexity of the propagating electronic , by only using an approximated formulation of ground and continuum states. Many effects unravelled by HHG spectroscopy are instead due to electron correlation effects, quantum interference, and Rydberg-state contributions, which are all properly captured by an ab initio electronic-structure approach. In this Review we have collected recent advances in modelling HHG by means of ab initio time-dependent approaches relying on the propagation of the time-dependent Schr\"odinger equation (or derived equations) in presence of a very intense electromagnetic field. We limit ourselves to gas-phase atomic and molecular targets, and to solids. We focus on the various levels of theory for describing the electronic structure of the target, coupled with strong-field dynamics and ionisation approaches, and on the basis used to represent electronic states. Selected applications and perspectives for future developments are also given.

2018 ◽  
Vol 20 (12) ◽  
pp. 8311-8325 ◽  
Author(s):  
M. Ruberti ◽  
P. Decleva ◽  
V. Averbukh

Electron-correlation effects on the multi-channel dynamics underlying strong-field HHG response of CO2 molecule were demonstrated by ab initio ADC study.


2020 ◽  
Author(s):  
Emanuele Coccia ◽  
Eleonora Luppi ◽  
Carlo Federico Pauletti

<p>This study arises from the attempt to answer the following question: how different descriptions of electronic exchange and correlation affect the high-harmonic generation (HHG) spectroscopy of H2, N2 and CO2 molecules? We compare HHG spectra for H2, N2 and CO2 with different ab initio electronic structures methods: real-time time-dependent configuration interaction (RT-TDCIS) and real-time time-dependent density functional theory (RT-TDDFT) using truncated basis sets composed of correlated wave functions expanded on Gaussian basis sets. In the framework of RT-TDDFT, we employ PBE and LC-ωPBE functionals. We study HHG spectroscopy by disentangling the effect of electronic exchange and correlation. We first analyse the electronic exchange alone and in the case of RT-TDDFT with LC-ωPBE, we use ω = 0.3 and ω = 0.4 to tune the percentage of long-range Hartree-Fock exchange and of short-range exchange PBE. Then, we added the correlation as described by PBE functional. All the methods give very similar HHG spectra and they seem not to be particularly sensitive to the different description of exchange and correlation or to the correct asymptotic behaviour of the Coulomb potential. Despite this general trend, some differences are found in the region connecting the cutoff and the background. Here, the harmonics can be resolved with different accuracy depending on the theoretical schemes used. We believe that the investigation of the molecular continuum and its coupling with strong fields merits further theoretical investigations in the next future. </p>


1996 ◽  
Vol 77 (9) ◽  
pp. 1743-1746 ◽  
Author(s):  
Ivan P. Christov ◽  
J. Zhou ◽  
J. Peatross ◽  
A. Rundquist ◽  
M. M. Murnane ◽  
...  

Symmetry ◽  
2018 ◽  
Vol 10 (8) ◽  
pp. 313 ◽  
Author(s):  
Hidemasa Yamane ◽  
Satoshi Tanaka

We studied the high-harmonic generation (HHG) of a two-level-system (TLS) driven by an intense monochromatic phase-locked laser based on complex spectral analysis with the Floquet method. In contrast with phenomenological approaches, this analysis deals with the whole process as a coherent quantum process based on microscopic dynamics. We have obtained the time-frequency resolved spectrum of spontaneous HHG single-photon emission from an excited TLS driven by a laser field. Characteristic spectral features of the HHG, such as the plateau and cutoff, are reproduced by the present model. Because the emitted high-harmonic photon is represented as a superposition of different frequencies, the Fano profile appears in the long-time spectrum as a result of the quantum interference of the emitted photon. We reveal that the condition of the quantum interference depends on the initial phase of the driving laser field. We have also clarified that the change in spectral features from the short-time regime to the long-time regime is attributed to the interference between the interference from the Floquet resonance states and the dressed radiation field.


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