Search NASA⌕ Search

Engineering topics

You, Yong Sing

Publications and source records attributed to You, Yong Sing.

Attosecond synchronization of extreme ultraviolet high harmonics from crystals

The interaction of strong near-infrared (NIR) laser pulses with wide-bandgap dielectrics produces high harmonics in the extreme ultraviolet (XUV) wavelength range. These observations have opened up the possibility of attosecond metrology in solids, which would benefit from a precise measurement of the emission times of individual harmonics with respect to the NIR laser field. In this work, we show that, when high-harmonics are detected from the input surface of a magnesium oxide crystal, a bichromatic probing of the XUV emission shows a clear synchronization largely consistent with a semiclassical model of electron–hole recollisions in bulk solids. On the other hand, the bichromatic spectrogram of harmonics originating from the exit surface of the 200 μm-thick crystal is strongly modified, indicating the influence of laser field distortions during propagation. Our tracking of sub-cycle electron and hole re-collisions at XUV energies is relevant to the development of solid-state sources of attosecond pulses.

74 ATOMIC AND MOLECULAR PHYSICS↗

Crystal orientation-dependent polarization state of high-order harmonics

We analyze the crystal orientation-dependent polarization state of extreme ultraviolet (XUV) high-order harmonics from bulk magnesium oxide crystals subjected to intense linearly polarized laser fields. We find that only along high-symmetry directions in crystals high-order harmonics follow the polarization direction of the laser field. In general, the polarization direction of high-order harmonics deviates from that of the laser field, and the deviation amplitude depends on the crystal orientation, harmonic order and the strength of the laser field. We use a real-space electron trajectory model to understand the crystal orientation-dependent polarization state of XUV harmonics. The polarization analysis allows us to track the motion of strong-field-driven electron in conduction bands in two dimensions. These results have implications in all-optical probing of atomic-scale structure in real-space, electronic band-structure in momentum space, and in the possibility of generating attosecond pulses with time-dependent polarization in a compact setup.

36 MATERIALS SCIENCE↗

Interferometry of dipole phase in high harmonics from solids

Understanding the temporal profiles of high harmonics is essential for their applications in attosecond science. Microscopically, the dipole phase plays an important role in determining the high-harmonic emission phase. In gas-phase high-harmonic generation, the tunnel-ionized electron spends much of its travel time in the continuum—far from the parent ion, where it accumulates the dipole phase. Therefore, the atomic dipole phase is largely independent of the target atom. In solid-state high-harmonic generation, since the driven electron experiences a periodic potential during the entire travel time, the dipole phase may depend on the electronic structures of source materials. Here, we employ an interferometric method to characterize high harmonics from magnesium oxide and quartz crystals. We measure material-dependent intensity-induced high-harmonic phase delays that we attribute to the intensity-induced changes in the dipole phase originating from the interband polarization. The material-dependent dipole phase can provide a robust platform for high-harmonic spectroscopy of solids.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Probing periodic potential of crystals via strong-field re-scattering

Strong-field ionization and re-scattering phenomena have been used to image angstrom-scale structures of isolated molecules in the gas phase. These methods typically make use of the anisotropic response of the participating molecular orbital. Recently, an anisotropic strong-field response has also been observed in high-order harmonic generation (HHG) from bulk crystals. In a (100) cut magnesium oxide crystal, extreme ultraviolet high-harmonics are found to depend strongly on the crystal structure and inter-atomic bonding. Here, we extend these measurements to other two important crystal orientations: (111) and (110). We find that HHG from these orientations is also strongly anisotropic. The underlying dynamics is understood using a real-space picture, where high-harmonics are produced via coherent collision of strong-field driven electrons from the atomic sites, including from the nearest neighbor atoms. We find that harmonic efficiency is enhanced when semi-classical electron trajectories connect to the concentrated valence charge distribution regions around the atomic cores. Similarly, the efficiency is suppressed when the trajectories miss the atomic cores. Furthermore, these results further support the real-space picture of HHG with implications for retrieving the periodic potential of the crystal, if not the wavefunctions in three-dimensions.

74 ATOMIC AND MOLECULAR PHYSICS↗

High-harmonic generation in amorphous solids

High-harmonic generation in isolated atoms and molecules has been widely utilized in extreme ultraviolet photonics and attosecond pulse metrology. Recently, high-harmonic generation has been observed in solids, which could lead to important applications such as all-optical methods to image valance charge density and reconstruct electronic band structures, as well as compact extreme ultraviolet light sources. So far these studies are confined to crystalline solids; therefore, decoupling the respective roles of long-range periodicity and high density has been challenging. Here we report the observation of high-harmonic generation from amorphous fused silica. We also decouple the role of long-range periodicity by comparing harmonics generated from fused silica and crystalline quartz, which contain the same atomic constituents but differ in long-range periodicity. These results advance current understanding of the strong-field processes leading to high-harmonic generation in solids with implications for the development of robust and compact extreme ultraviolet light sources.

36 MATERIALS SCIENCE↗

Anisotropic high-harmonic generation in bulk crystals

The microscopic valence electron density determines the optical, electronic, structural and thermal properties of materials. However, current techniques for measuring this electron charge density are limited: for example, scanning tunnelling microscopy is confined to investigations at the surface, and electron diffraction requires very thin samples to avoid multiple scattering. Therefore, an optical method is desirable for measuring the valence charge density of bulk materials. Since the discovery of high-harmonic generation (HHG) in solids, there has been growing interest in using HHG to probe the electronic structure of solids. Here, using single-crystal MgO, we demonstrate that high-harmonic generation in solids is sensitive to interatomic bonding. We find that harmonic efficiency is enhanced (diminished) for semi-classical electron trajectories that connect (avoid) neighbouring atomic sites in the crystal. Finally, these results indicate the possibility of using materials’ own electrons for retrieving the interatomic potential and thus the valence electron density, and perhaps even wavefunctions, in an all-optical setting.

36 MATERIALS SCIENCE↗

High-harmonic generation from an atomically thin semiconductor [Observation of high harmonics from an atomically thin semiconductor]

High-harmonic generation (HHG) in bulk solids permits the exploration of materials in a new regime of strong fields and attosecond timescales. The generation process has been discussed in the context of strongly driven electron dynamics in single-particle bands. Two-dimensional materials exhibit distinctive electronic properties compared to the bulk that could significantly modify the HHG process, including different symmetries, access to individual valleys and enhanced many-body interactions. Here we demonstrate non-perturbative HHG from a monolayer MoS 2 crystal, with even and odd harmonics extending to the 13th order. The even orders are predominantly polarized perpendicular to the pump and are compatible with the anomalous transverse intraband current arising from the material’s Berry curvature, while the weak parallel component suggests the importance of interband transitions. The odd harmonics exhibit a significant enhancement in efficiency per layer compared to the bulk, which is attributed to correlation effects. In conclusion, the combination of strong many-body Coulomb interactions and widely tunable electronic properties in two-dimensional materials offers a new platform for attosecond physics.

36 MATERIALS SCIENCE↗