Extreme ultraviolet (EUV) high-harmonic radiation emerging from laser-driven atoms, molecules or plasmas underlies powerful attosecond spectroscopy techniques and provides insight into fundamental structural and dynamic properties of matter. The advancement of these spectroscopy techniques to study strong-field electron dynamics in condensed matter calls for the generation and manipulation of EUV radiation in bulk solids, but this capability has remained beyond the reach of optical sciences. Recent experiments and theoretical predictions paved the way to strong-field physics in solids by demonstrating the generation and optical control of deep ultraviolet radiation in bulk semiconductors, driven by femtosecond mid-infrared fields or the coherent up-conversion of terahertz fields to multi-octave spectra in the mid-infrared and optical frequencies. Here we demonstrate that thin films of SiO2 exposed to intense, few-cycle to sub-cycle pulses give rise to wideband coherent EUV radiation extending in energy to about 40 electronvolts. Our study indicates the association of the emitted EUV radiation with intraband currents of multi-petahertz frequency, induced in the lowest conduction band of SiO2. To demonstrate the applicability of high-harmonic spectroscopy to solids, we exploit the EUV spectra to gain access to fine details of the energy dispersion profile of the conduction band that are as yet inaccessible by photoemission spectroscopy in wide-bandgap dielectrics. In addition, we use the EUV spectra to trace the attosecond control of the intraband electron motion induced by synthesized optical transients. Our work advances lightwave electronics in condensed matter into the realm of multi-petahertz frequencies and their attosecond control, and marks the advent of solid-state EUV photonics.

Manipulation of electron dynamics calls for electromagnetic forces that can be confined to and controlled over sub-femtosecond time intervals. Tailored transients of light fields can provide these forces. We report on the generation of subcycle field transients spanning the infrared, visible, and ultraviolet frequency regimes with a 1.5-octave three-channel optical field synthesizer and their attosecond sampling. To demonstrate applicability, we field-ionized krypton atoms within a single wave crest and launched a valence-shell electron wavepacket with a well-defined initial phase. Half-cycle field excitation and attosecond probing revealed fine details of atomic-scale electron motion, such as the instantaneous rate of tunneling, the initial charge distribution of a valence-shell wavepacket, the attosecond dynamic shift (instantaneous ac Stark shift) of its energy levels, and its few-femtosecond coherent oscillations.

The time it takes a bound electron to respond to the electromagnetic force of light sets a fundamental speed limit on the dynamic control of matter and electromagnetic signal processing. Time-integrated measurements of the nonlinear refractive index of matter indicate that the nonlinear response of bound electrons to optical fields is not instantaneous; however, a complete spectral characterization of the nonlinear susceptibility tensors--which is essential to deduce the temporal response of a medium to arbitrary driving forces using spectral measurements--has not yet been achieved. With the establishment of attosecond chronoscopy, the impulsive response of positive-energy electrons to electromagnetic fields has been explored through ionization of atoms and solids by an extreme-ultraviolet attosecond pulse or by strong near-infrared fields. However, none of the attosecond studies carried out so far have provided direct access to the nonlinear response of bound electrons. Here we demonstrate that intense optical attosecond pulses synthesized in the visible and nearby spectral ranges allow sub-femtosecond control and metrology of bound-electron dynamics. Vacuum ultraviolet spectra emanating from krypton atoms, exposed to intense waveform-controlled optical attosecond pulses, reveal a finite nonlinear response time of bound electrons of up to 115 attoseconds, which is sensitive to and controllable by the super-octave optical field. Our study could enable new spectroscopies of bound electrons in atomic, molecular or lattice potentials of solids, as well as light-based electronics operating on sub-femtosecond timescales and at petahertz rates.

Ultrafast studies using liquid cells Advances in microscopy techniques aim to make it possible to study materials under more realistic conditions, such as in liquid cells, or to use fast probes to capture dynamics. Fu et al. combined liquid cell transmission electron microscopy with ultrafast pump-probe spectroscopy to perform time-resolved studies of nanoscale objects (see the Perspective by Baum). They successfully captured the change in rotational dynamics of coupled gold nanoparticles and also observed the dynamics as two particles fused together in a liquid environment. Science , this issue p. 494 ; see also p. 458

Ultimate control over light entails the capability of crafting its field waveform. Here, we detail the technological advances that have recently permitted the synthesis of light transients confinable to less than a single oscillation of its carrier wave and the precise attosecond tailoring of their fields. Our work opens the door to light field based control of electrons on the atomic, molecular, and mesoscopic scales.

Ultrafast Electron Microscopy (UEM) has been demonstrated to be an effective table-top technique for imaging the temporally-evolving dynamics of matter with subparticle spatial resolution on the time scale of atomic motion. However, imaging the faster motion of electron dynamics in real time has remained beyond reach. Here, we demonstrate more than an order of magnitude (16 times) enhancement in the typical temporal resolution of UEM by generating isolated ~ 30 fs electron pulses, accelerated at 200 keV, via the optical-gating approach, with sufficient intensity for efficiently probing the electronic dynamics of matter. Moreover, we investigate the feasibility of attosecond optical gating to generate isolated subfemtosecond electron pulses, attaining the desired temporal resolution in electron microscopy for establishing the "Attomicroscopy" to allow the imaging of electron motion in the act.

Attosecond science capitalizes on the extreme nonlinearity of strong fields, driven by few-cycle pulses, to attain attosecond temporal resolution and give access to the electron motion dynamics of matter in real-time. Here, we measured the electronic delay response of the dielectric system triggered by a strong field of few-cycle pulses to be in the order of 425 ± 98 as. Moreover, we exploited the electronic response following the strong driver field to demonstrate all-optical light field metrology with attosecond resolution. This field sampling methodology provides a direct connection between the driver field and the induced ultrafast dynamics in matter. Also, we demonstrate the quantum electron motion control in dielectric using synthesized light waveforms. This on-demand electron motion control realizes the long-anticipated ultrafast optical switches and quantum electronics. This advancement promises to increase the limiting speed of data processing and information encoding to rates that exceed 1 petabit/s, opening a new realm of information technology. Main text:Advancements in attosecond pulse generation and spectroscopic measurements by high harmonic generation in gases and solids opened a new window to study the electronic response driven by strong fields in real-time [1][2][3][4][5][6][7][8][9][10][11] . The strong-field-induced electron dynamics and the related phase transition to a semimetal-like state of dielectric systems have been studied theoretically [12][13][14][15] and experimentally by XUV attosecond spectroscopy [16][17][18][19] . Accordingly, the strong-field interaction induces a current in the dielectric nanocircuit as

Ultrafast electron microscopy (UEM) is a pivotal tool for imaging of nanoscale structural dynamics with subparticle resolution on the time scale of atomic motion. Photon-induced near-field electron microscopy (PINEM), a key UEM technique, involves the detection of electrons that have gained energy from a femtosecond optical pulse via photon-electron coupling on nanostructures. PINEM has been applied in various fields of study, from materials science to biological imaging, exploiting the unique spatial, energy, and temporal characteristics of the PINEM electrons gained by interaction with a "single" light pulse. The further potential of photon-gated PINEM electrons in probing ultrafast dynamics of matter and the optical gating of electrons by invoking a "second" optical pulse has previously been proposed and examined theoretically in our group.Here, we experimentally demonstrate this photon-gating technique, and, through diffraction, visualize the phase transition dynamics in vanadium dioxide nanoparticles. With optical gating of PINEM electrons, imaging temporal resolution was improved by a factor of 3 or better, being limited only by the optical pulse widths. This work enables the combination of the high spatial resolution of electron microscopy and the ultrafast temporal response of the optical pulses, which provides a promising approach to attain the resolution of few femtoseconds and attoseconds in UEM.photon-induced near-field electron microscopy | attosecond electron microscopy | optical-gated electron pulse | time-resolved PINEM | photon-electron gating I n ultrafast electron microscopy (UEM) (1-3), electrons generated by photoemission at the cathode of a transmission electron microscope are accelerated down the microscope column to probe the dynamic evolution of a specimen initiated by an ultrafast light pulse. The use of femtosecond lasers to generate the electron probe and excite the specimen has made it possible to achieve temporal resolution on the femtosecond time scale, as determined by the cross-correlation of the optical and electron pulses. One important method in the UEM repertoire is photon-induced near-field electron microscopy (PINEM) (4, 5), in which the dynamic response detected by the electron probe is the pump-induced charge density redistribution in nanoscale specimens (6).Photon-electron coupling is the basic building block of PINEM, which takes place in the presence of nanostructures when the energy-momentum conservation condition is satisfied (4, 5). This coupling leads to inelastic gain/loss of photon quanta by electrons in the electron packet, which can be resolved in the electron energy spectrum (5,7,8). This spectrum consists of discrete peaks, spectrally separated by multiples of the photon energy (nZω), on the higher and lower energy sides of the zero loss peak (ZLP) (4) (Fig. 1). The development of PINEM enables the visualization of the spatiotemporal dielectric response of nanostructures (9), visualization of plasmonic fields (4, 5) and their spatial interferences (10), imag...