Attosecond dynamical Franz-Keldysh effect in polycrystalline diamond

Lucchini, Matteo; Sato, Shunsuke A.; Ludwig, André; Herrmann, J.; Volkov, Mikhail; Kasmi, Lamia; Shinohara, Yuji; Yabana, Kazuhiro; Gallmann, L.; Keller, U.

doi:10.1126/science.aag1268

Cited by 255 publications

(234 citation statements)

References 43 publications

Supporting

Mentioning

219

Contrasting

Order By: Relevance

“…This technique provides rich information about the interplay between the laser field and the Coulombic potential on the excited electron dynamics. Its background-free nature enables us to use a large range of gas pressures and to reveal the influence of collisions in the relaxation process.Transient Absorption Spectroscopy (TAS) in the extreme ultraviolet (XUV) range is a powerful technique for ultrafast dynamical studies, from the gas phase [1][2][3] to the solid state [4,5]. The recent progress of attosecond science has made the extension of TAS to the attosecond regime (ATAS) a reality.…”

mentioning

confidence: 99%

See 1 more Smart Citation

Phase-resolved two-dimensional spectroscopy of electronic wave packets by laser-induced XUV free induction decay

et al. 2017

View full text Add to dashboard Cite

We present a novel time-and phase-resolved, background-free scheme to study the extreme ultraviolet dipole emission of a bound electronic wavepacket, without the use of any extreme ultraviolet exciting pulse. Using multiphoton transitions, we populate a superposition of quantum states which coherently emit extreme ultraviolet radiation through free induction decay. This emission is probed and controlled, both in amplitude and phase, by a time-delayed infrared femtosecond pulse. We directly measure the laser-induced dephasing of the emission by using a simple heterodyne detection scheme based on two-source interferometry. This technique provides rich information about the interplay between the laser field and the Coulombic potential on the excited electron dynamics. Its background-free nature enables us to use a large range of gas pressures and to reveal the influence of collisions in the relaxation process.Transient Absorption Spectroscopy (TAS) in the extreme ultraviolet (XUV) range is a powerful technique for ultrafast dynamical studies, from the gas phase [1][2][3] to the solid state [4,5]. The recent progress of attosecond science has made the extension of TAS to the attosecond regime (ATAS) a reality. In the past few years, different configurations of ATAS experiments have emerged. In the first and most intuitive scheme, the XUV attosecond pulses probe a sample that has been pre-excited by an infrared (IR) pump laser pulse. This scheme was for instance used to follow the ultrafast coherent hole dynamics initiated in strong-field ionized krypton [1]. In the second arrangement, the XUV and IR pulses are temporally overlapped. The XUV absorption thus probes the IR-dressed atomic or molecular states, allowing the observation of light-induced states [6,7] as well as sub-cycle AC-Stark-shifts [8]. Finally, in what turned out to be the most widely used scheme, the XUV pulse comes first and serves as a pump, exciting a broadband superposition of quantum states through single-photon absorption. The wavepacket relaxes by coherently emitting XUV radiation (called XUV Free Induction Decay, XFID) that interferes with the incident light. A delayed IR laser field is used to follow or control the relaxation dynamics, such that these experiments can be seen as Transient Reshaping of the Absorption spectrum of the XUV light (TRAX) [9,10].In TRAX experiments, the delayed IR laser pulse has three main effects on the XFID emission ( Fig. 1) : (i) Damping of the emission by ionization of the excited states. This effect induces a lowering and a spectral broadening of the absorption features [2]. (ii) Field coupling of different electronic states, leading to population transfers. The resulting amplitude reshaping of the electronic wavepacket can be detected through temporal beatings in the absorption signal, as demonstrated in atoms [9,10] and molecules [11,12]. (iii) Phase shift induced by the Stark-shift of the excited states. This laser-induced phase was shown to enable full control over the absorption lineshapes, from Lorentz ...

show abstract

mentioning

confidence: 99%

“…Transient Absorption Spectroscopy (TAS) in the extreme ultraviolet (XUV) range is a powerful technique for ultrafast dynamical studies, from the gas phase [1][2][3] to the solid state [4,5]. The recent progress of attosecond science has made the extension of TAS to the attosecond regime (ATAS) a reality.…”

mentioning

confidence: 99%

Phase-resolved two-dimensional spectroscopy of electronic wave packets by laser-induced XUV free induction decay

et al. 2017

View full text Add to dashboard Cite

show abstract

“…This method has already been successfully applied to the description of strong-field phenomena in atoms [38,39] and solids [40][41][42][43]. Being interested in the microscopic origin of HHG in solids, we have neglected macroscopic propagation effects in our quantum-mechanical simulations, thus making a sudden approximation, and we consider only the intrinsic bulk contribution.…”

mentioning

confidence: 99%

Impact of the Electronic Band Structure in High-Harmonic Generation Spectra of Solids

et al. 2017

View full text Add to dashboard Cite

An accurate analytic model describing the microscopic mechanism of high-harmonic generation (HHG) in solids is derived. Extensive first-principles simulations within a time-dependent density-functional framework corroborate the conclusions of the model. Our results reveal that (i) the emitted HHG spectra are highly anisotropic and laser-polarization dependent even for cubic crystals; (ii) the harmonic emission is enhanced by the inhomogeneity of the electron-nuclei potential; the yield is increased for heavier atoms; and (iii) the cutoff photon energy is driver-wavelength independent. Moreover, we show that it is possible to predict the laser polarization for optimal HHG in bulk crystals solely from the knowledge of their electronic band structure. Our results pave the way to better control and optimize HHG in solids by engineering their band structure. DOI: 10.1103/PhysRevLett.118.087403 Atoms and molecules interacting with strong laser pulses emit high-order harmonics of the fundamental driving laser field. The high-harmonic generation (HHG) in gases is routinely used nowadays to produce isolated attosecond pulses [1][2][3][4] and coherent radiation ranging from the visible to soft x rays [5]. Because of a higher electronic density, solids are one promising route towards compact, brighter HHG sources. The recent observation of nonperturbative HHG in solids without damage [6][7][8][9][10], extending even beyond the atomic limit [10], has opened the door to the observation and control of attosecond electron dynamics in solids [8,9,11], all-optical band-structure reconstruction [12], and solid-state sources of isolated extreme-ultraviolet pulses [9,11]. However, in contrast to HHG from gases, the microscopic mechanism underlying HHG from solids is still controversially debated in the attoscience community, in some cases casting doubts on the validity of the proposed microscopic model and resulting in confusion about the correct interpretation of experimental data. Various competing simplified models have been proposed but they often are based on strong approximations and a priori assumptions, often stating that there is a strong similarity with the processes underlying atomic-gas HHG emission. However, it is clear that many-body effects due to the crystalline structure of solids and the fermionic nature of interaction electrons play a decisive role that fundamentally distinguishes the solid from the gas case. It is the scope of the present work to unravel within an ab initio approach what the impact is of the underlying electronic band structure of the solids in the observed HHG emission.The process of HHG from gases is by now well understood in terms of the three-step model [13][14][15] in which electrons are first promoted from the ground state of the atom (or molecule) to the continuum, then accelerated by the electric field, and finally recombine with the parent ion. With this simple, intuitive model most of the observed effects are well described, in particular, the dependence of the harmonic cutoff energ...

show abstract

“…By using this phenomenon, we can produce an ultra-fast modulator of light or an ultra-fast optical switch. Recently, the Tr-DFKE has been observed by Lucchini et al [26] in thin film polycrystalline diamond on an attosecond time scale. Similar effects have also been reported for the excitonic state in GaAs quantum well [27].…”

Section: Introductionmentioning

confidence: 97%

“…With regards to the experiment, the effects of the propagation of pump and probe lasers is also important in material. For higher frequency region, Tr-DFKE in polycrystalline diamond was reported [26]. Far above the band gap, diamond has low transmission and includes the interaction between some conduction bands.…”

Section: Introductionmentioning

confidence: 99%

Multi-Scale Simulation for Transient Absorption Spectroscopy under Intense Few-Cycle Pulse Laser

Otobe

2016

Photonics

View full text Add to dashboard Cite

Numerical pump-probe simulations for the sub-cycle transient spectroscopy of thin film diamond under intense few cycle pulse laser field is reported. The electron dynamics is calculated by the time-dependent Kohn-Sham equation. Simultaneously, the propagation of electromagnetic field is calculated by the Maxwell equation. Our result shows that the modulation of the reflectivity, transmission, and absorption around the optical gap do not coincide with the field amplitude of the pump laser. The phase shift of the modulation with respect to the pump field depends on the pump intensity and probe frequency. The modulation of the reflectivity is sensitive to the choice of the exchange-correlation potential, and dynamical effect of the mean-field in meta-GGA potential.

show abstract

Attosecond dynamical Franz-Keldysh effect in polycrystalline diamond

Cited by 255 publications

References 43 publications

Phase-resolved two-dimensional spectroscopy of electronic wave packets by laser-induced XUV free induction decay

Phase-resolved two-dimensional spectroscopy of electronic wave packets by laser-induced XUV free induction decay

Impact of the Electronic Band Structure in High-Harmonic Generation Spectra of Solids

Multi-Scale Simulation for Transient Absorption Spectroscopy under Intense Few-Cycle Pulse Laser

Contact Info

Product

Resources

About