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Directly contrasting ultrafast excited-state dynamics in the gas and liquid phases is crucial to understanding the influence of complex environments. Previous studies have often relied on different spectroscopic observables, rendering direct comparisons challenging. Here, we apply extreme-ultraviolet time-resolved photoelectron spectroscopy to both gaseous and liquid cis-stilbene, revealing the coupled electronic and nuclear dynamics that underlie its isomerization. Our measurements track the excited-state wave packets from excitation along the complete reaction path to the final products. We observe coherent excited-state vibrational dynamics in both phases of matter that persist to the final products, enabling the characterization of the branching space of the S-1-S-0 conical intersection. We observe a systematic lengthening of the relaxation timescales in the liquid phase and a red shift of the measured excited-state frequencies that is most pronounced for the complex reaction coordinate. These results characterize in detail the influence of the liquid environment on both electronic and structural dynamics during a complete photochemical transformation. ISSN:1755-4349 ISSN:1755-4330

Circularly polarized sources of radiation play a vital role in photoelectron circular dichroism and magnetic circular dichroism experiments. While circularly polarized radiation can be routinely generated in the visible domain of the electromagnetic spectrum due to the availability of laser sources and optics in this range, generation of circularly polarized radiation in the extreme ultraviolet (XUV) domain is challenging and, using table-top sources it is currently limited to high harmonic generation from gases using bi-circular, complicated two-source and/or interferometry arrangement. In this work, being fueled by recent development of high harmonic generation and spectroscopy of solids, we demonstrate the generation of circularly polarized extreme ultraviolet light using interaction of intense circularly polarized drivers. The simplicity of our experimental setup enables rapid application of circularly polarized XUV light in circular dichroism experiments.

We report the first observation of intermolecular Coulombic decay (ICD) in liquid water following inner-valence ionization. By combining a monochromatized tabletop high-harmonic source with a liquid microjet, we record electron-electron coincidence spectra at two photon energies that identify the ICD electrons, together with the photoelectrons originating from the 2a1 inner-valence band of liquid water. Our results confirm the importance of ICD as a source of low-energy electrons in bulk liquid water and provide quantitative results for modeling the velocity distribution of the slow electrons that are thought to dominate radiation damage in aqueous environments., Physical Review Letters, 128 (13), ISSN:0031-9007, ISSN:1079-7114

Extreme ultraviolet high-harmonic generation (HHG) from bulk liquids has only recently been demonstrated (T.T. Luu, Z. Yin et al, Nat. Comm. 9, 3724, (2018)). This has opened new prospects for the development of bright high-harmonic sources and the development of liquid-phase high-harmonic spectroscopy (HHS). Here, we report on the first observation of HHG in liquids driven by few-cycle (~7 fs) pulses. We observe the emission of a broad quasi-continuum in the extreme ultraviolet, which is strongly modulated on a photon-energy scale much finer than the central photon energy of the driver. We show that these modulations arise from an etalon effect inside the flat microjet, which we use to perform an in-operando measurement of the flat-jet's thickness. The possibility to directly characterize flat microjets during HHG will greatly support their optimization for light-source applications and facilitate the development of liquid-phase HHS., JPhys Photonics, 2 (4), ISSN:2515-7647

Intermolecular Coulombic decay has been observed in liquid water for the first time. This was achieved using monochromatized high-harmonic radiation coupled to a liquid microjet and an electron-electron coincidence spectrometer.

Measuring time-resolved photoelectron spectra of liquids, and achieving photon energies to probe electronic ground states is challenging. We present gas- and liquid-phase XUV-TRPES of cis-stilbene, providing new insight into this prototype of molecular photoisomerisation dynamics.

Berry phase and Berry curvature have become ubiquitous concepts in physics, relevant to a variety of phenomena, such as polarization, various Hall effects, etc. Studies of these phenomena call for characterization of Berry phase or curvature which is largely limited to theory, and a few measurements in optical lattices. In this work, we report polarimetry of high-harmonic emission from solids and exploit this novel capability to directly retrieve the Berry curvature of α-quartz. We show that the two manifestations of broken inversion symmetry in solids lead to perpendicular or parallel polarization of even harmonics with respect to the driving field. Using semiclassical transport theory, we retrieve the Berry curvature from spectra measured in perpendicular polarization, the results being supported by ab initio calculation. Our work demonstrates an approach for the direct measurement of Berry curvature in solids, which could serve as a benchmark for theoretical studies., Nature Communications, 9 (1), ISSN:2041-1723

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.

Physical Review A, 98 (4), ISSN:1094-1622, ISSN:0556-2791, ISSN:1050-2947

We used attosecond streaking to probe the temporal structure of isolated attosecond EUV pulses generated in a bulk solid (here, SiO2 nanofilms) using a single-cycle optical driver. The fine details of the dynamic response of the system encoded in the chirp of the emerging attosecond pulse enabled the establishment of a firm link between the emission of EUV radiation and the intraband electric currents induced by the field-driven, coherent, nonlinear scattering of charge carriers in the bulk of SiO2. EUV emission from SiO2 has been shown to be phase coherent (field reproducible) and immune to minor phase fluctuation of the driving laser pulses.

Attosecond Pulse Trains (APT) generated by high-harmonic generation (HHG) of high-intensity near-infrared (IR) laser pulses have proven valuable for studying the electronic dynamics of atomic and molecular species. However, the high intensities required for high-photon-energy, high-flux HHG usually limit the class of adequate laser systems to repetition rates below 10 kHz. Here, APT's generated from the 100 kHz, 160 W, 40 fs laser system (HR-1) currently under commissioning at the extreme light infrastructure attosecond light pulse source (ELI-ALPS) are reconstructed using the reconstruction of attosecond beating by interference of two-photon Transitions (RABBIT) technique. These experiments constitute the first attosecond time-resolved photoelectron spectroscopy measurements with attosecond pulses performed at 100 kHz repetition rate and one of the first experiments performed at ELI-ALPS in the framework of projects commissioning its newly installed technologies. These RABBIT measurements were taken with an additional IR field temporally locked to the extreme-ultraviolet APT, resulting in an atypical ω beating. We show that the phase of the 2ω beating recorded under these conditions is strictly identical to that observed in standard RABBIT measurements within second-order perturbation theory. This work highlights an experimental simplification for future experiments based on attosecond interferometry (or RABBIT), which is particularly useful when lasers with high average powers are used., Journal of Physics B: Atomic, Molecular and Optical Physics, 52 (23), ISSN:1361-6455, ISSN:0368-3508, ISSN:0953-4075, ISSN:0022-3700

Physical Review B, 94 (11), ISSN:1098-0121, ISSN:0163-1829, ISSN:1550-235X, ISSN:0556-2805, ISSN:2469-9969, ISSN:1095-3795, ISSN:2469-9950

We report on design, production and implementation of a highly dispersive broadband dielectric multilayer mirror covering near ultraviolet range from 290 nm to 350 nm. The described mirrors, having 92% spectrally averaged reflectance in the ultraviolet range and ∼ 85 fs of group delay difference, that allow compression to ∼ 7 fs, provide a strong foundation for generation of few-fs pulses in the near ultraviolet.

Investigations using single-cycle intense optical fields to drive electron motion in bulk silicon dioxide show that the light-induced electric currents extend in frequency up to about 8 petahertz. The speed of electronics, and hence of computing, is limited by the frequencies of the electric currents that are used. Light fields can induce and manipulate electric currents at vastly higher frequencies than are achievable in conventional devices, and Eleftherios Goulielmakis and colleagues now extend this approach to reach an even faster regime. They use single-cycle intense optical fields to drive electron motion in the bulk of silicon dioxide and show that the light-induced intraband electric currents extend in frequency up to about eight petahertz. This demonstration of real-time access to the dynamic nonlinear conductivity of silicon dioxide, with the ability to directly probe and control the intraband currents on attosecond timescales, establishes intense light fields as a platform for multi-petahertz coherent electronics and points to new opportunities for fundamental studies of electron dynamics in condensed matter. The frequency of electric currents associated with charge carriers moving in the electronic bands of solids determines the speed limit of electronics and thereby that of information and signal processing1. The use of light fields to drive electrons promises access to vastly higher frequencies than conventionally used, as electric currents can be induced and manipulated on timescales faster than that of the quantum dephasing of charge carriers in solids2. This forms the basis of terahertz (1012 hertz) electronics in artificial superlattices2, and has enabled light-based switches3,4,5 and sampling of currents extending in frequency up to a few hundred terahertz. Here we demonstrate the extension of electronic metrology to the multi-petahertz (1015 hertz) frequency range. We use single-cycle intense optical fields (about one volt per angstrom) to drive electron motion in the bulk of silicon dioxide, and then probe its dynamics by using attosecond (10−18 seconds) streaking6,7 to map the time structure of emerging isolated attosecond extreme ultraviolet transients and their optical driver. The data establish a firm link between the emission of the extreme ultraviolet radiation and the light-induced intraband, phase-coherent electric currents that extend in frequency up to about eight petahertz, and enable access to the dynamic nonlinear conductivity of silicon dioxide. Direct probing, confinement and control of the waveform of intraband currents inside solids on attosecond timescales establish a method of realizing multi-petahertz coherent electronics. We expect this technique to enable new ways of exploring the interplay between electron dynamics and the structure of condensed matter on the atomic scale.

Here we demonstrate the first intense optical attosecond pulses synthesized in the visible and nearby spectral ranges and their use for revealing the nonlinear response time of bound electrons of Kr atoms.

We analyzed frequency-domain characteristics of a femtosecond laser whose carrier-envelope phase (CEP) was stabilized by the direct locking method (DLM). To evaluate the CEP-stabilized laser with zero carrier-envelope-offset frequency (f ceo), as imposed by DLM, a self-referencing f-to-2f interferometer with a shifted frequency comb by an acousto-optic modulator was employed in an out-of-loop. The measurement of the square root of triangle variance confirmed that DLM is a phase-locking method. The tight locking was verified from a narrow bandwidth of f ceo, measured using the out-of-loop interferometer, and from a small frequency jitter measured with a frequency counter referenced to a Rb-clock. The femtosecond laser with CEP stabilized by DLM is, thus, well suited for applications in the frequency domain as well as in the time domain.

A comprehensive real-time spectral phase interferometry for direct electric field reconstruction (SPIDER) apparatus for characterizing femtosecond laser pulses is demonstrated. The SPIDER provides the temporal profiles of femtosecond laser pulses, reconstructed at the speed of 3.5 Hz, with parameters of the spectral phase such as group delay dispersion and third-order dispersion. The apparatus is applied successfully to optimize the spectral dispersion of a kHz femtosecond Ti:Sapphire laser by adjusting a grating compressor in real time.

Coherent extreme ultraviolet (EUV) radiation using high-harmonic generation (HHG) in α–quartz is demonstrated from 10 to 200 kHz, using 50 fs laser pulses at the center wavelength of 1030 nm. The EUV radiation extends beyond 25 eV in the nondamaging regime. The number of photons generated in a single harmonic order at 15.6 eV is measured to be ≈(3.5±2.5)×1010 per second which, to the best of our knowledge, is a first and record value reported to date using EUV HHG from solids. This Letter demonstrates one of the first all-solid-state EUV sources based on industrial-grade fiber lasers, enabling the possibility of bringing reliable EUV sources to the mass market.

We have observed and studied a nonlinear response of dispersive dielectric multilayer mirrors (DM). It was found that the structure of the mirror itself causes strong enhancement of the electric field inside the multilayer stack consequently triggering strong two-photon absorption (2PA). We have developed a mathematical model, that allows estimation of the coefficient of the 2PA, β, subsequent prediction and to some extent tuning of the strength of the nonlinear response of any multilayer coating.

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.

We characterize the Auger decay of core-shell excitations in Krypton atoms in an all-photonic fashion, using a novel attosecond EUV pump - attosecond optical probe scheme. An intuitive model, where the optical field acts as a temporal amplitude and phase gate on the EUV excited dipole, is used to retrieve the Auger core-hole decay time.

We demonstrate synthesis of superoctave, intense, subcycle transients of light and their application to attosecond control of matter.

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.

Electron dynamics in atoms [1] molecules and condensed matter are typically clocked in tens to thousands of attoseconds. Real-time control of these dynamics requires the exertion of electric or magnetic fields controllable in strength and in direction on that time scale. Such precisely controlled fields can become available via waveform synthesis of continuous (to warrant isolated structures in the time domain) light spectra that span over more than an optical octave.

The long-term carrier-envelope phase (CEP) coherence of a femtosecond laser with same pulse-to-pulse CEP value, obtained using the direct locking method, is demonstrated by employing a quasi-common-path interferometer (QPI). For the evaluation of the CEP stability, the phase noise properties of a femtosecond laser with the CEP stabilized using a QPI are compared with those obtained using a Mach-Zehnder f-2f interferometer, for which the phase power spectral density and the Allan deviation were calculated from the beat signals of the interferometers. With the improved CEP stability, the long-term CEP coherent signal with an accumulated phase noise well below 1 radian can be maintained for more than 56 hours, i.e., the CEP coherence is preserved without a phase cycle slip for more than 1.6 × 10(13) pulses at a repetition rate of 80 MHz. The relative stability is also estimated to be approximately 1.4 × 10(-22) at a central wavelength of 790 nm.

Within the last two decades dispersive dielectric multilayer mirrors (DMs), also known as chirped mirrors (CMs), have played a significant role in the progress of ultrafast science. Their ability to manipulate the phase of a light pulse has advanced the synthesis of intense femtosecond optical pulses followed by remarkable progress in the disciplines of nonlinear optics. Meanwhile, the performance of the mirrors themselves has been strictly limited to the linear regime, as essential mirror characteristics such as reflectance, transmittance, and dispersion are evaluated with only intensity-independent values of refractive indices and extinction coefficients taken into the design formalism. Here, we report, to the best of our knowledge, the first observation of a strong nonlinear response of the DMs. We have found that the DM’s multilayer stack causes very significant enhancement of the internal electric field that becomes sufficient to enable third-order nonlinearity. Remarkably, in our particular case, the response is solely emerging in the form of nonlinear absorbance. By modifying the multilayer structure of the mirror, we gained control over observed nonlinearity and were able to predict and to some extent to tune the magnitude of the response, without perturbing the dispersive properties of the DMs. This demonstration not only expands the functionality of DMs into the nonlinear domain, but also marks a new approach to the development of multilayer coatings for applications in ultrafast science.

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.