Many applications of the extreme ultraviolet (XUV) radiation obtained by high-order harmonic generation (HHG) in gases require a small focus area in order to enable attosecond pulses to reach a high intensity. Here, high-order harmonics generated in Ar with a multiterawatt laser system in a loose focusing geometry are focused to a few micrometers using two toroidal mirrors in a Wolter configuration with a high demagnification factor. Using a knife-edge measurement technique, we determine the position and size of the XUV foci as a function of harmonic order. We show that the focus properties vary with harmonic order and the generation conditions. Simulations, based on a classical description of the harmonic dipole phase and assuming that the individual harmonics can be described as Gaussian beams, reproduce the experimental behavior. We discuss how the generation geometry affects the intensity and duration of the focused attosecond pulses.

Maria Hoflund

Jasper Peschel

Marius Plach

Hugo Dacasa

K&#x00E9;vin Veyrinas

Eric Constant

Peter Smorenburg

Hampus Wikmark

Sylvain Maclot

Chen Guo

Cord Arnold

Anne L'Huillier

Per Eng-Johnsson

Focusing Properties of High-Order Harmonics

We present a systematic study of the crystal-orientation dependence of high-harmonic generation in monolayer transition-metal dichalcogenides, WS2 and MoSe2, subjected to intense linearly polarized midinfrared laser fields. The measured spectra consist of both odd- and even-order harmonics, with a high-energy cutoff extending beyond the 15th order for a laser-field strength around &#x007E;1&#x2009;V/nm. In WS2, we find that the polarization direction of the odd-order harmonics smoothly follows that of the laser field irrespective of the crystal orientation, whereas the direction of the even-order harmonics is fixed by the crystal mirror planes. Furthermore, the polarization of the even-order harmonics shows a flip in the course of crystal rotation when the laser field lies between two of the crystal mirror planes. By numerically solving the semiconductor Bloch equations for a gapped-graphene model, we qualitatively reproduce these experimental features and find the polarization flipping to be associated with a significant contribution from interband polarization. In contrast, high-harmonic signals from MoSe2 exhibit deviations from the laser-field following of odd-order harmonics and crystal-mirror-plane following of even-order harmonics. We attribute these differences to the competing roles of the intraband and interband contributions, including the deflection of the electron-hole trajectories by nonparabolic crystal bands.

Yuki Kobayashi

Christian Heide

Hamed Koochaki Kelardeh

Amalya Johnson

Fang Liu

Tony F. Heinz

David A. Reis

Shambhu Ghimire

Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides

Since the first isolated attosecond pulse was demonstrated through high-order harmonics generation (HHG) in 2001, researchers&#x2019; interest in the ultrashort time region has expanded. However, one realizes a limitation for related research such as attosecond spectroscopy. The bottleneck is concluded to be the lack of a high-peak-power isolated attosecond pulse source. Therefore, currently, generating an intense attosecond pulse would be one of the highest priority goals. In this paper, we review our recent work of a TW-class parallel three-channel waveform synthesizer for generating a gigawatt-scale soft-X-ray isolated attosecond pulse (IAP) using HHG. By employing several stabilization methods, we have achieved a stable 50&#x2009;mJ three-channel optical-waveform synthesizer with a peak power at the multi-TW level. This optical-waveform synthesizer is capable of creating a stable intense optical field for generating an intense continuum harmonic beam thanks to the successful stabilization of all the parameters. Furthermore, the precision control of shot-to-shot reproducible synthesized waveforms is achieved. Through the HHG process employing a loose-focusing geometry, an intense shot-to-shot stable supercontinuum (50&#x2013;70&#x2009;eV) is generated in an argon gas cell. This continuum spectrum supports an IAP with a transform-limited duration of 170&#x2009;as and a submicrojoule pulse energy, which allows the generation of a GW-scale IAP. Another supercontinuum in the soft-X-ray region with higher photon energy of approximately 100&#x2013;130&#x2009;eV is also generated in neon gas from the synthesizer. The transform-limited pulse duration is 106&#x2009;as. Thus, the enhancement of HHG output through optimized waveform synthesis is experimentally proved.

Bing Xue

Yuuki Tamaru

Yuxi Fu

Hua Yuan

Pengfei Lan

Oliver D. M&#x00FC;cke

Akira Suda

Katsumi Midorikawa

Eiji J. Takahashi

A Custom-Tailored Multi-TW Optical Electric Field for Gigawatt Soft-X-Ray Isolated Attosecond Pulses

Terahertz- (THz-) based electron manipulation has recently been shown to hold tremendous promise as a technology for manipulating and driving the next generation of compact ultrafast electron sources. Here, we demonstrate an ultrafast electron diffractometer with THz-driven pulse compression. The electron bunches from a conventional DC gun are compressed by a factor of 10 and reach a duration of &#x007E;180&#x2009;fs (FWHM) with 10,000 electrons/pulse at a 1&#x2009;kHz repetition rate. The resulting ultrafast electron source is used in a proof-of-principle experiment to probe the photoinduced dynamics of single-crystal silicon. The THz-compressed electron beams produce high-quality diffraction patterns and enable the observation of the ultrafast structural dynamics with improved time resolution. These results validate the maturity of THz-driven ultrafast electron sources for use in precision applications.

Dongfang Zhang

Tobias Kroh

Felix Ritzkowsky

Timm Rohwer

Moein Fakhari

Huseyin Cankaya

Anne-Laure Calendron

Nicholas H. Matlis

Franz X. K&#x00E4;rtner

THz-Enhanced DC Ultrafast Electron Diffractometer

Understanding the evolution of molecular electronic structures is the key to explore and control photochemical reactions and photobiological processes. Subjected to strong laser fields, electronic holes are formed upon ionization and evolve in the attosecond timescale. It is crucial to probe the electronic dynamics in real time with attosecond-temporal and atomic-spatial precision. Here, we present molecular attosecond interferometry that enables the in situ manipulation of holes in carbon dioxide molecules via the interferometry of the phase-locked electrons (propagating in opposite directions) of a laser-triggered rotational wave packet. The joint measurement on high-harmonic and terahertz spectroscopy (HATS) provides a unique tool for understanding electron dynamics from picoseconds to attoseconds. The optimum phases of two-color pulses for controlling the electron wave packet are precisely determined owing to the robust reference provided with the terahertz pulse generation. It is noteworthy that the contribution of HOMO-1 and HOMO-2 increases reflecting the deformation of the hole as the harmonic order increases. Our method can be applied to study hole dynamics of complex molecules and electron correlations during the strong-field process. The threefold control through molecular alignment, laser polarization, and the two-color pulse phase delay allows the precise manipulation of the transient hole paving the way for new advances in attochemistry.

Yindong Huang

Jing Zhao

Zheng Shu

Yalei Zhu

Jinlei Liu

Wenpu Dong

Xiaowei Wang

Zhihui L&#x00FC;

Dongwen Zhang

Jianmin Yuan

Jing Chen

Zengxiu Zhao

Ultrafast Hole Deformation Revealed by Molecular Attosecond Interferometry

Matters are generally classified within four states: solid, liquid, gas, and plasma. Three of the four states of matter (solid, gas, and plasma) have been used for THz wave generation with short laser pulse excitation for decades, including the recent vigorous development of THz photonics in gases (air plasma). However, the demonstration of THz generation from liquids was conspicuously absent. It is well known that water, the most common liquid, is a strong absorber in the far infrared range. Therefore, liquid water has historically been sworn off as a source for THz radiation. Recently, broadband THz wave generation from a flowing liquid target has been experimentally demonstrated through laser-induced microplasma. The liquid target as the THz source presents unique properties. Specifically, liquids have the comparable material density to that of solids, meaning that laser pulses over a certain area will interact with three orders more molecules than an equivalent cross-section of gases. In contrast with solid targets, the fluidity of liquid allows every laser pulse to interact with a fresh area on the target, meaning that material damage or degradation is not an issue with the high-repetition rate intense laser pulses. These make liquids very promising candidates for the investigation of high-energy-density plasma, as well as the possibility of being the next generation of THz sources.

Yiwen E

Liangliang Zhang

Anton Tcypkin

Sergey Kozlov

Cunlin Zhang

X.-C. Zhang

Broadband THz Sources from Gases to Liquids

Qihuang Gong

Wei Zhao

Ultrafast Science to Capture Ultrafast Motions

About this journal

The Open Access journal Ultrafast Science, published in association with&nbsp;Xi’an Institute of Optics and Precision Mechanics, is a&nbsp;platform for cutting-edge and emerging topics in ultrafast science with broad interest from scientific communities.

Journal profile

Meet the editorial board

Ultrafast Science's editorial board is led by Qihuang Gong (Peking University)&nbsp;and Wei Zhao (Xi'an Institute of Optics and Precision Mechanics, CAS),&nbsp;and is comprised of experts who have made significant and well recognized contributions to the field of ultrafast science.

Editorial board

More special issue details

Ultrafast Science is now accepting submissions for its first special issue:

<a href="https://spj.sciencemag.org/ultrafast-science-special-issues/attosecond/">Attosecond Science and Technology</a>