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Theoretical description of high-order harmonic generation in solids

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 Added by Alexander Kemper
 Publication date 2012
  fields Physics
and research's language is English




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We consider several aspects of high-order harmonic generation in solids: the effects of elastic and inelastic scattering; varying pulse characteristics; and inclusion of material-specific parameters through a realistic band structure. We reproduce many observed characteristics of high harmonic generation experiments in solids including the formation of only odd harmonics in inversion-symmetric materials, and the nonlinear formation of high harmonics with increasing field. We find that the harmonic spectra are fairly robust against elastic and inelastic scattering. Furthermore, we find that the pulse characteristics play an important role in determining the harmonic spectra.



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By using the Floquet eigenstates, we derive a formula to calculate the high-harmonic components of the electric current (HHC) in the setup where a monochromatic laser field is turned on at some time. On the basis of this formulation, we study the HHC spectrum of electrons on a one-dimensional chain with the staggered potential to study the effect of multiple sites in the unit cell such as the systems with charge density wave (CDW) order. With the help of the solution for the Floquet eigenstates, we analytically show that two plateaus of different origins emerge in the HHC spectrum. The widths of these plateaus are both proportional to the field amplitude, but inversely proportional to the laser frequency and its square, respectively. We also show numerically that multi-step plateaus appear when both the field amplitude and the staggered potential are strong.
We consider noninteracting electrons coupled to laser fields, and study perturbatively the effects of the lattice potential involving disorder on the harmonic components of the electric current, which are sources of high-order harmonic generation (HHG). By using the Floquet-Keldysh Green functions, we show that each harmonic component consists of the coherent and the incoherent parts, which arise respectively from the coherent and the incoherent scatterings by the local ion potentials. As the disorder increases, the coherent part decreases, the incoherent one increases, and the total harmonic component of the current first decreases rapidly and then approaches a nonzero value. Our results highlight the importance of the periodicity of crystals, which builds up the Bloch states extending over the solid. This is markedly different from the traditional HHG in atomic gases, where the positions of individual atoms are irrelevant.
High-order harmonic generation (HHG) in isolated atoms and molecules has been widely utilized in extreme ultraviolet (XUV) photonics and attosecond pulse metrology. Recently, HHG has also been observed in solids, which could lead to important applications such as all-optical methods to image valance charge density and reconstruction of electronic band structures, as well as compact XUV light sources. Previous HHG studies are confined on crystalline solids; therefore decoupling the respective roles of long-range periodicity and high density has been challenging. Here, we report the first observation of HHG from amorphous fused silica. We decouple the role of long-range periodicity by comparing with crystal quartz, which contains same atomic constituents but exhibits long-range periodicity. Our results advance current understanding of strong-field processes leading to high harmonic generation in solids with implications in robust and compact coherent XUV light sources.
We propose a novel picture of high-harmonic generation (HHG) in solids based on the concept of temporally changing band structures. To demonstrate the utility of this picture, we focus on the high-order sideband generation (HSG) caused by strong terahertz (THz) and weak near-infrared (NIR) light in the context of pump-probe spectroscopy. We find that the NIR frequency dependence of the HSG indicates the existence of new energy levels (sub-bands) around the band-gap energy, which have multiple frequencies of THz light. This sub-band picture explains why the HSG intensity becomes a non-monotonic function of the THz light amplitude. The present analysis not only reveals the origin of the plateau structure in HHG spectra, but also provides a connection to other high-field phenomena.
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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.
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