Time and space waveform optimization to extend the harmonic cutoff and to produce the water window single attosecond pulse

Based on the three-step theory of high-order harmonic generation, the harmonic cutoff is very sensitive to the few-cycle laser waveform in both time and space regions. Therefore, in this paper, we propose the method to control the harmonic cutoff and to produce the water window attosecond pulse through the optimization of time and space waveform. It is found that, in the time region, by properly choosing the delay and phase of the few-cycle two-color pulse, not only the harmonic intensity is enhanced, but also the quantum path of the harmonic emission can be controlled. Further, with the introduction of the 3rd pulse (i.e., the infrared pulse or the unipolar pulse), the harmonic cutoff from the single harmonic emission peak can be extended, showing a water window harmonic plateau. In the space region, by using the positive spatial inhomogeneous effect, the harmonic cutoff from the basic two-color waveform can also be extended, which leads to a water window spectral continuum. Finally, by Fourier transformation of harmonics during the water window region, the ultrashort single 29 as pulses can be obtained.

Chirp form selection to produce intense and broad harmonic spectra and attosecond pulses in the presence of single and superposition initial states

The chirp form selection for producing intense and broad high-order harmonic spectra has been investigated when the initial state is chosen to be the single or superposition states. It is found that, for the case of a single ground initial state, the down-chirp is much better for extending the harmonic cutoff with the stronger emission intensity. Moreover, the multi-color combined field is beneficial to produce the larger harmonic cutoff and higher harmonic intensity. After the control of laser waveform, the combination of 3-color down-chirps with a proper UV pulse is the best condition to obtain the intense X-ray spectral continuum and the isolated attosecond pulse. For the case of superposition initial state, both the up-chirp and down-chirp are beneficial to generate the high-intensity spectral regions. However, with the combination of multi-color field, only the harmonic cutoff can be further extended, and the harmonic intensity presents almost no changes for the superposition initial state case. Finally, by properly choosing the 3-color up-chirps or 3-color down-chirps combined pulses, the stronger intensity harmonic spectra covering the X-ray region can be obtained, which can produce the isolated pulses of 37 as.

Pushing and pulling on OH- and H3O+ with electric fields across water’s surface

We use second harmonic generation (SHG) spectroscopy, molecular dynamics simulation, and theoretical modeling to study the response of the neat liquid water-air interface to changes in the potential of an external electrode positioned above the liquid. We observe a parabolic dependence of second harmonic intensity on applied potential. This dependence is reminiscent of bulk-phase electric field induced second harmonic (EFISH) but more complicated because it combines the second-order response of the topmost water layer and the potential dependent response of the interfacial electrical double-layer. Based on the literature values for these contributions, we derive a physical interpretation of our measurements that reveals new insight into the response of the neat water interface to external electric fields. Specifically, we find that the net dipolar orientation of water molecules within the double-layer is primarily responsive to the internal fields generated by the excess surface concentrations of OH- and H3O+ that arise to screen the external potential. Notably, this interpretation implies that the orientational response of water dipoles at the interface can actually oppose the direction of the external field, a subtle effect that is not captured by traditional models.

Generation of elliptical isolated attosecond pulse from oriented $\textrm{H}_{2}^{+}$ in a linearly polarized laser field

We investigate the ellipticity of the high-order harmonic generation from the oriented $\textrm{H}_{2}^{+}$ exposed to a linearly polarized laser field by numerically solving the two dimensional time-dependent Schr$\ddot{\textrm{o}}$dinger equation (2D TDSE). Numerical simulations show that the harmonic ellipticity is remarkably sensitive to the alignment angle. The harmonic spectrum is highly elliptically polarized at a specific alignment angle $\theta = 30^\circ $, which is insensitive to the variation of the laser parameters. The position of the harmonic intensity minima indicates the high ellipticity, which can be attributed to the two-center interference effect. The high ellipticity can be explained by the phase difference of the harmonics. The results that we obtain facilitates the synthesis of a highly elliptical isolated attosecond pulses with duration down to 65 as, which can be served as a powerful tool to explore the ultrafast dynamics of molecules and study chiral light-matter interaction.

Giant Second Harmonic Generation Enhancement by Ag Nanoparticles Compactly Distributed on Hexagonal Arrangements

The association of plasmonic nanostructures with nonlinear dielectric systems has been shown to provide useful platforms for boosting frequency conversion processes at metal-dielectric interfaces. Here, we report on an efficient route for engineering light–matter interaction processes in hybrid plasmonic-χ(2) dielectric systems to enhance second harmonic generation (SHG) processes confined in small spatial regions. By means of ferroelectric lithography, we have fabricated scalable micrometric arrangements of interacting silver nanoparticles compactly distributed on hexagonal regions. The fabricated polygonal microstructures support both localized and extended plasmonic modes, providing large spatial regions of field enhancement at the optical frequencies involved in the SHG process. We experimentally demonstrate that the resonant excitation of the plasmonic modes supported by the Ag nanoparticle-filled hexagons in the near infrared region produces an extraordinary 104-fold enhancement of the blue second harmonic intensity generated in the surface of a LiNbO3 crystal. The results open new perspectives for the design of efficient hybrid plasmonic frequency converters in miniaturized devices.

Harmonic Extraction in Graphene: Monte Carlo Analysis of the Substrate Influence

Graphene on different substrates, such as SiO2, h-BN and Al2O3, has been subjected to oscillatory electric fields to analyse the response of the carriers in order to explore the generation of terahertz radiation by means of high-order harmonic extraction. The properties of the ensemble Monte Carlo simulator employed for such study have allowed us to evaluate the high-order harmonic intensity and the spectral density of velocity fluctuations under different amplitudes of the periodic electric field, proving that strong field conditions are preferable for the established goal. Furthermore, by comparison of both harmonic intensity and noise level, the threshold bandwidth for harmonic extraction has been determined. The results have shown that graphene on h-BN presents the best featuring of the cases under analysis and that in comparison to III–V semiconductors, it is a very good option for high-order harmonic extraction under AC electric fields with large amplitudes.

Second harmonic generation in glass-based metasurfaces using tailored surface lattice resonances

Dielectric metasurfaces have shown prominent applications in nonlinear optics due to strong field enhancement and low dissipation losses at the nanoscale. Chalcogenide glasses are one of the promising materials for the observation of nonlinear effects thanks to their high intrinsic nonlinearities. Here, we demonstrate, experimentally and theoretically, that significant second harmonic generation (SHG) can be obtained within amorphous Selenium (Se)-based chalcogenide metasurfaces by exploiting the coupling between lattice and particle resonances. We further show that the high-quality factor resonance at the origin of the SHG can be tuned over a wide wavelength range using a simple and versatile fabrication approach. The measured second harmonic intensity is orders of magnitude higher than that from a dewetted Se film consisting of random Se nanoparticles. The achieved conversion efficiency in the resonance region is of the order of 10−6 which is comparable with direct bandgap materials and at least two orders of magnitude higher than that of conventional plasmonics- and Si-based structures. Fabricated via a simple and scalable technique, these all-dielectric architectures are ideal candidates for the design of flat nonlinear optical components on flexible substrates.

Nonlinear chirp combination effect on the improvement of high harmonic spectra and attosecond pulses

The effect of nonlinear chirp combination on the enhancement of harmonic cutoff and harmonic intensity has been investigated by using a two-color chirped pulse. It is found that with the combination of 2-order chirp form, the strongest intensity enhancement of harmonic spectrum can be found. While, with the combination of 2-order and 3-order chirp forms, the largest cutoff extension of the harmonic spectrum can be obtained. Finally, by properly using the harmonic spectra driven by the above two kinds of combined pulses, the single attosecond pulses (SAPs) of 43 as and 33 as can be generated.

Pushing and Pulling on OH-and H3O+ with Electric Fields Across Water’s Surface

<p>We use second harmonic generation spectroscopy, molecular dynamics simulation, and theoretical modeling to study the response of the neat liquid water-air interface to changes in the potential of an external electrode positioned above the liquid. We observe a parabolic dependence of second harmonic intensity on applied potential, indicating that water’s net interfacial dipole responds linearly. We also observe a minimum intensity when the potential is tuned to a specific positive value. Interpreting this minimum based on the macroscopic electrostatic potential profile yields misleading physical conclusions because it neglects the internal bias exerted on molecular orientations by the excess surface concentrations of OH^- or H₃O⁺. We thus find that water’s net interfacial dipole orientation is primarily responsive to the effects of these ionic species rather than the external electric field. </p>

Pushing and Pulling on OH-and H3O+ with Electric Fields Across Water’s Surface

<p>We use second harmonic generation spectroscopy, molecular dynamics simulation, and theoretical modeling to study the response of the neat liquid water-air interface to changes in the potential of an external electrode positioned above the liquid. We observe a parabolic dependence of second harmonic intensity on applied potential, indicating that water’s net interfacial dipole responds linearly. We also observe a minimum intensity when the potential is tuned to a specific positive value. Interpreting this minimum based on the macroscopic electrostatic potential profile yields misleading physical conclusions because it neglects the internal bias exerted on molecular orientations by the excess surface concentrations of OH^- or H₃O⁺. We thus find that water’s net interfacial dipole orientation is primarily responsive to the effects of these ionic species rather than the external electric field. </p>