Search NASA⌕ Search
Home/Archive/DOE OSTI

DOE OSTI · 2587681

Ultrafast high-harmonic spectroscopy of solids

Heide, Christian·Kobayashi, Yuki·Haque, Sheikh Rubaiat Ul·Ghimire, Shambhu
View original source ↗Read source document ↗Export metadata ↓

Abstract

High-harmonic spectroscopy, an ultrafast all-optical technique initially conceptualized in atomic and molecular systems, has now emerged as a powerful platform for studying the structure and dynamics of condensed matter. Unlike that in the gas phase, solid-state high-harmonic generation relies on the fundamental response from high atomic density and periodicity, leading to interband transitions and coherent driving of electrons and holes in their respective bands. These mechanisms make high-harmonic spectroscopy particularly sensitive to the electronic band structure, topological properties and many-body correlations in condensed media. An advantage of high-harmonic spectroscopy over other spectroscopic methods is its ability to probe ultrafast phenomena, capturing femto- to attosecond dynamics of multi-band and strongly correlated electron interactions in solids. Furthermore, in this Review, we discuss the latest experimental and theoretical advances in ultrafast high-harmonic spectroscopy of solids and provide perspectives for future research in this field.

Explore related subjects

High-harmonic generationOptical spectroscopyQuantum fluids and solidsTopological matter

Keep this discovery

Explore connections, maps & timelines

BibTeXRIS

Heide, Christian, Kobayashi, Yuki, Haque, Sheikh Rubaiat Ul, Ghimire, Shambhu. 2024-10-10. Ultrafast high-harmonic spectroscopy of solids. https://doi.org/10.1038/s41567-024-02640-8

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related reports

DOE OSTI2026

Efficiency-optimized relativistic plasma harmonics for extreme fields

Bright harmonic radiation from relativistically oscillating laser plasmas offers a direct route for generating extreme electromagnetic fields. Theory predicts that under optimized conditions, the plasma medium can support strong spatiotemporal compression of laser energy in a coherent harmonic focus (CHF), delivering intensity boosts many orders of magnitude greater than the incident driving laser pulse. Although diffraction-limited performance (spatial compression) and attosecond phase locking (temporal compression) have been demonstrated experimentally, efficient coupling of relativistically intense laser pulse energy into the emitted harmonic cone has not been realized so far. Here we demonstrate that this highly nonlinear interaction can be tailored to deliver the maximum conversion efficiencies predicted from simulations. By fine-tuning the temporal profile of the driving laser on sub-picosecond (<10 −12 s) timescales, energies >9 mJ between the 12th and 47th harmonics are observed. These results are in agreement with the theoretically expected efficiency dependence on harmonic order, verifying that optimal conditions have been achieved in the generation process. This is the important final element required to achieve the expected intensity boosts from a CHF in experiments. Although obtaining spatiotemporal compression and optimal efficiency simultaneously remains challenging, the path to realizing extreme optical field strengths approaching the critical field of quantum electrodynamics (the Schwinger limit at >10 16 V cm −1 or >10 29 W cm −2 ) is now open, permitting all-optical studies of the quantum vacuum and new frontiers for intense attosecond science.

High-harmonic generation↗
DOE OSTI2025

Extreme-ultraviolet spatiotemporal vortices via high harmonic generation

Spatiotemporal optical vortices (STOVs) are space–time structured light pulses with a unique topology that couples spatial and temporal domains and carry transverse orbital angular momentum (OAM). Up to now, their generation has been limited to the visible and infrared regions of the spectrum. During the last decade, it was shown that through the process of high-order harmonic generation, it is possible to upconvert spatial optical vortices that carry longitudinal OAM from the near-infrared into the extreme-ultraviolet (EUV), thereby producing vortices with distinct femtosecond and attosecond structure. In this work, we demonstrate theoretically and experimentally the generation of EUV spatiotemporal and spatiospectral vortices using near-infrared STOV driving laser pulses. Here, we use analytical expressions for focused STOVs to perform macroscopic calculations of high-order harmonic generation that are directly compared to the experimental results. As STOV beams are not eigenmodes of propagation, we characterize the highly charged EUV STOVs in both the near and far fields to show that they represent conjugated spatiotemporal and spatiospectral vortex pairs. Our work provides high-frequency light beams topologically coupled at the nanometre/attosecond scales domains with transverse OAM that could be suitable to explore electronic dynamics in magnetic materials, chiral media and nanostructures.

High-harmonic generation↗
DOE OSTI2020

Towards isolated attosecond electron bunches using ultrashort-pulse laser-solid interactions

We investigate MeV-level attosecond electron bunches from ultrashort-pulse laser-solid interactions through similarities between experimental and simulated electron energy spectra. We show measurements of the bunch duration and temporal structure from particle-in-cell simulations. The experimental observation of such bunches favors specular reflection direction when focusing the laser pulse onto a subwavelength boundary of thick overdense plasmas at grazing incidence. Particle-in-cell simulation further reveals that the attosecond duration is a result of ultra-thin (~tenth of a micron) gaps of zero electromagnetic energy density in the modulated reflected radiation, while the bunching (locally peaked electron concentration) comes from the highly-directional electron angular distribution acquired by the electrons in a grazing incidence setup. To isolate a single electron bunch, we perform simulations using 1-cycle laser pulses and analyze the effect of carrier-envelop phase with particle tracking. The duration of the electron bunch can be further decreased by increasing the laser intensity and the focal spot size, while its direction can be changed by tuning the preplasma density gradient.

High-harmonic generation↗