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| Open AccessRaman time-delay in attosecond transient absorption of strong-field created krypton vacancy
The advent of isolated attosecond XUV pulse sources marks a new era in attosecond science, pivotal for the investigation of core electron dynamics. Here the authors discover that the coherent Raman coupling between the cation states leads to extra timedelay between different transition channels by applying the attosecond transient absorption spectroscopy on the investigation of complex dynamics of strong field ionization of Krypton.
- Li Wang
- , Guangru Bai
- & Zengxiu Zhao
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Article
| Open AccessFrom chiral laser pulses to femto- and attosecond electronic chirality flips in achiral molecules
Chirality is a unique property of certain molecules. Here the authors discuss method to induce and flip electronic chirality in oriented NaK molecules using circularly polarized laser pulses.
- Yunjiao Chen
- , Dietrich Haase
- & Yonggang Yang
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Article
| Open AccessSpatiotemporal imaging and shaping of electron wave functions using novel attoclock interferometry
Electrons detached from atoms by photoionization carry valuable information about light-atom interactions. Here, authors propose a novel attoclock interferometry to spatiotemporally shape and image the electron wave function, from which the quantum nature of strong-field ionization is identified.
- Peipei Ge
- , Yankun Dou
- & Yunquan Liu
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Article
| Open AccessCarrier-envelope phase on-chip scanner and control of laser beams
Measurement and control of the carrier-envelope phase (CEP) is essential for applications of few-cycle laser beams. The authors present a compact on-chip, ambient-air, CEP scanning probe and show a 3D map of spatial changes of CEP and demonstrate CEP control in the focal volume with a spatial light modulator.
- Václav Hanus
- , Beatrix Fehér
- & Péter Dombi
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Article
| Open AccessAttosecond delays between dissociative and non-dissociative ionization of polyatomic molecules
The role of nuclear motion on photoionization delays is an interesting open question. Here the authors study photoionization delays in dissociative and non-dissociative ionization of a polyatomic molecule and explore the effect of isotopic substitution.
- Xiaochun Gong
- , Étienne Plésiat
- & Hans Jakob Wörner
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Article
| Open AccessHigh-order harmonic generation from a thin film crystal perturbed by a quasi-static terahertz field
Here the authors establish a biochromatic method for ultrafast probe and control of the strong field high harmonic generation process in solid by combining strong mid-infrared and weak terahertz fields.
- Sha Li
- , Yaguo Tang
- & Louis F. DiMauro
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Article
| Open AccessAttosecond dynamics of multi-channel single photon ionization
Understanding of photoionization dynamics, one of the fastest processes in nature, requires the characterization of all underlying ionization channels. Here the authors use an interferometry technique based on attosecond pulses to measure the phase and amplitude of the individual angular momentum channels in the photoionization of neon.
- Jasper Peschel
- , David Busto
- & Per Eng-Johnsson
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Article
| Open AccessAtomic partial wave meter by attosecond coincidence metrology
Understanding the photoelectron emission time after the interaction of photon with atoms and molecules is of fundamental interest. Here the authors examine the role of partial waves to the photoionization phase shift of atoms using an attosecond clock and electron-ion coincidence spectroscopy.
- Wenyu Jiang
- , Gregory S. J. Armstrong
- & Jian Wu
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Article
| Open AccessEntanglement of orbital angular momentum in non-sequential double ionization
In strong field ionization, entanglement between an electron and an ion has been discussed previously. Here the authors explore orbital angular momentum entanglement between the electrons released in non-sequential double ionization.
- Andrew S. Maxwell
- , Lars Bojer Madsen
- & Maciej Lewenstein
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Article
| Open AccessFilming movies of attosecond charge migration in single molecules with high harmonic spectroscopy
Seeing molecules in action under the influence of very short pulses is interesting. Here the authors demonstrate charge migration dynamics in molecules by using high harmonic spectroscopy and machine learning algorithm.
- Lixin He
- , Siqi Sun
- & C. D. Lin
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Article
| Open AccessUltraviolet supercontinuum generation driven by ionic coherence in a strong laser field
Supercontinuum generation can be utilized for light source development. Here the authors demonstrate ultraviolet supercontinuum generation from ions due to strong field ionization and multiphoton resonance effect.
- Hongbin Lei
- , Jinping Yao
- & Zengxiu Zhao
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Article
| Open AccessInfluence of shape resonances on the angular dependence of molecular photoionization delays
It is an interesting topic to find the time it takes for an electron to escape an atom or a molecule after photoionization. Here the authors measure the angular dependence of photoionization time delay in the molecular frame and discuss the role of shape resonances.
- F. Holzmeier
- , J. Joseph
- & R. R. Lucchese
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Article
| Open AccessStrong-field coherent control of isolated attosecond pulse generation
Attosecond pulse generation needs improvements both in terms of tunability and photon flux for next level attosecond experiments. Here the authors show how to control the HHG emission and its spectral-temporal characteristics by driving the IAP generation with synthesized sub-cycle optical pulses.
- Yudong Yang
- , Roland E. Mainz
- & Franz X. Kärtner
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Article
| Open AccessObservation of laser-assisted electron scattering in superfluid helium
Laser-assisted electron scattering (LAES) is a commonly observed strong field process in gas phase systems. Here the authors use helium droplets with core atoms and molecules to observe increased electron energy due to multiple LAES events within the droplets.
- Leonhard Treiber
- , Bernhard Thaler
- & Markus Koch
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Article
| Open AccessEnantio-sensitive unidirectional light bending
Developing new methods for structuring light’s chirality in space would be advantageous for various next-generation applications. Here, the authors report enantio-sensitive unidirectional light bending by interacting light with isotropic chiral media.
- David Ayuso
- , Andres F. Ordonez
- & Olga Smirnova
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Article
| Open AccessAttosecond intra-valence band dynamics and resonant-photoemission delays in W(110)
Accessing intraband dynamics is challenging due to simultaneous requirements on energy, momentum and time resolution. Here, the authors measure intraband delays between sp- and d-band electronic states in the valence band photoemission from W(110) using intracavity generated attosecond pulse trains.
- S. Heinrich
- , T. Saule
- & U. Kleineberg
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Article
| Open AccessAngular dependence of the Wigner time delay upon tunnel ionization of H2
Light-matter interaction leading to photoelectron emission via the photoelectric effect illustrates the quantum nature of light. Here, the authors report the dependence of the photoelectron’s Wigner time delay on the photoelectron’s emission direction relative to the molecular axis of hydrogen in strong field tunnel-ionization.
- D. Trabert
- , S. Brennecke
- & S. Eckart
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Article
| Open AccessLight phase detection with on-chip petahertz electronic networks
On-chip optical-field emission devices may be useful for fast electronics and signal processing. Here the authors show a compact on-chip light phase detector capable of monitoring photocurrents oscillating at optical frequencies using electrically connected arrays of plasmonic bow-tie nanoantennae.
- Yujia Yang
- , Marco Turchetti
- & Phillip D. Keathley
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Perspective
| Open AccessAttosecond science based on high harmonic generation from gases and solids
Different methods are demonstrated in recent years to produce attosecond pulses. Here, the authors discuss recent development and future prospects of the generation of such pulses from gases and solids and their potential applications in spectroscopy and ultrafast dynamics in atoms, molecules and other complex systems.
- Jie Li
- , Jian Lu
- & Zenghu Chang
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Article
| Open AccessProbing multiphoton light-induced molecular potentials
Conical intersections, a hallmark of polyatomic molecules, can be induced with light, leading to new reaction pathways. Here, the authors show that intense fields can create complex, beyond-conical intersections even in diatomics, resulting in an unexpected angular distribution of fragment ions.
- M. Kübel
- , M. Spanner
- & A. Staudte
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Article
| Open AccessTracking attosecond electronic coherences using phase-manipulated extreme ultraviolet pulses
Light pulses with controllable parameters are desired for studying the fundamental properties of matter. Here the authors generate and use phase-manipulated and highly time-stable XUV pulse pairs to probe the coherent evolution and dephasing of XUV electronic coherences in helium and argon.
- Andreas Wituschek
- , Lukas Bruder
- & Frank Stienkemeier
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Article
| Open AccessIntense attosecond pulses carrying orbital angular momentum using laser plasma interactions
Vortices in light fields are of growing importance in the XUV and X-ray ranges. Here the authors show by simulations that high harmonics and attosecond pulses, generated while irradiating a deformed thin foil with circularly-polarized Gaussian laser pulses, carry a well-defined orbital angular momentum.
- J. W. Wang
- , M. Zepf
- & S. G. Rykovanov
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Article
| Open AccessSub-cycle time resolution of multi-photon momentum transfer in strong-field ionization
Understanding momentum transfer in light–matter interaction is intriguing. Here the authors study momentum transfer from photons to electrons and observe a time delay in the linear momentum transfer during strong-field ionization of xenon atoms using time-resolved measurements with velocity map imaging.
- Benjamin Willenberg
- , Jochen Maurer
- & Ursula Keller
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Article
| Open AccessSymmetry of molecular Rydberg states revealed by XUV transient absorption spectroscopy
Transient absorption spectroscopy is used to identify the structural characteristics of the atoms and molecules. Here the authors used extreme ultraviolet transient absorption spectroscopy to identify the Rydberg state symmetry of aligned molecules.
- Peng Peng
- , Claude Marceau
- & D. M. Villeneuve
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Article
| Open AccessCoherent control in the extreme ultraviolet and attosecond regime by synchrotron radiation
Synchrotron light sources have wide range of tunable parameters like frequency, intensity. Here the authors demonstrate quantum control of Rydberg states of helium using delay controlled XUV wavepackets generated from synchrotron radiation.
- Y. Hikosaka
- , T. Kaneyasu
- & M. Katoh
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Article
| Open AccessDisentangling conical intersection and coherent molecular dynamics in methyl bromide with attosecond transient absorption spectroscopy
Excited-state molecular dynamics may be too complex to be resolved by femtosecond spectroscopic studies. Here the authors resolve the competing pathways in the excited state dynamics of methyl bromide by attosecond transient absorption spectroscopy, from excitation to fragmentation.
- Henry Timmers
- , Xiaolei Zhu
- & Stephen R. Leone
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Article
| Open AccessNonlinear XUV signal generation probed by transient grating spectroscopy with attosecond pulses
Ultrafast dynamics following light-matter interaction are governed by nonlinear processes. Here the authors show that initial nonlinear signal time-evolution is a consequence of phase grating accumulation using transient grating measurements with attosecond and near-infrared pulses.
- Ashley P. Fidler
- , Seth J. Camp
- & Stephen R. Leone
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Article
| Open AccessSpatiotemporal imaging of valence electron motion
Light absorption in matter often induces ultrafast electron dynamics within the system. Here, the authors record a femtosecond movie of the electron density of an argon ion as it oscillates in a quantum beat of two fine-structure states.
- M. Kübel
- , Z. Dube
- & A. Staudte
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Article
| Open AccessElectron correlation driven non-adiabatic relaxation in molecules excited by an ultrashort extreme ultraviolet pulse
The many-body quantum nature of molecules determines their static and dynamic properties, but remains the main obstacle in their accurate description. Here, the authors employ ultrafast spectroscopic methods to explore the dynamics of highly excited organic molecules, revealing many-body effects and hints of coherent vibronic dynamics which persist despite their molecular complexity.
- A. Marciniak
- , V. Despré
- & F. Lépine
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Article
| Open AccessEvidence of depolarization and ellipticity of high harmonics driven by ultrashort bichromatic circularly polarized fields
Polarization parameters of the high harmonics driven by bichromatic circularly polarized pulses are usually assumed near perfect. Here the authors use polarimetry measurement to show that depolarization and ellipticity can arise from symmetry breaking in the ionization of a medium by the ultrashort driving fields.
- Lou Barreau
- , Kévin Veyrinas
- & Pascal Salières
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Article
| Open AccessConical-intersection dynamics and ground-state chemistry probed by extreme-ultraviolet time-resolved photoelectron spectroscopy
Recent progress in extreme-ultraviolet table-top light sources is enabling advances in ultrafast molecular dynamics. Here the authors demonstrate time-resolved photoelectron spectroscopy with such a source, observing how a molecular wave packet crosses a conical intersection, performs large-amplitude motion and eventually dissociates.
- A. von Conta
- , A. Tehlar
- & H. J. Wörner
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Article
| Open AccessAttosecond coherent control of free-electron wave functions using semi-infinite light fields
Manipulation of the electron–photon coupling is crucial for quantum circuits and exploration of electronic motions and nuclear phenomena. Here the authors discuss a scheme to coherently control the electron wave function from attosecond to zeptosecond timescales by using semi-infinite light fields.
- G. M. Vanacore
- , I. Madan
- & F. Carbone
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Article
| Open AccessQuantum simulation of ultrafast dynamics using trapped ultracold atoms
There is a close theoretical correspondence between the ultrafast dynamics of bound electrons and the slow dynamics of trapped ultracold atoms. Here the authors exploit this mapping to experimentally simulate ultrafast phenomena with a large temporal magnification factor.
- Ruwan Senaratne
- , Shankari V. Rajagopal
- & David M. Weld
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Article
| Open AccessMulti-petahertz electron interference in Cr:Al2O3 solid-state material
Signal processing in electronic devices is in the THz regime. Here the authors measure NIR lightwave-field-induced multiple dipole oscillations in Cr:Al2O3 in the time domain reaching PHz scale by using an isolated attosecond pulse and this method shows potential for higher speed signal processing.
- Hiroki Mashiko
- , Yuta Chisuga
- & Hideki Gotoh
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Article
| Open AccessAnisotropic photoemission time delays close to a Fano resonance
Ionization time delays are of interest in understanding the photoionization mechanism in atoms and molecules in ultra-short time scales. Here the authors investigate the angular dependence of photoionization time delays in the presence of an autoionizing resonance in argon atom using RABBITT technique.
- Claudio Cirelli
- , Carlos Marante
- & Ursula Keller
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Article
| Open AccessAttosecond recorder of the polarization state of light
Attosecond pulses are useful in exploring processes involving ultrafast electron motion in atomic and molecular systems. Here the authors discuss a method to characterize the complex time-varying polarization state of broadband attosecond pulses by using asymmetry in photoelectron spectra.
- Álvaro Jiménez-Galán
- , Gopal Dixit
- & Misha Ivanov
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Article
| Open AccessUltrafast quantum control of ionization dynamics in krypton
Photoionization of atoms and molecules is a complex process and requires sensitive probes to explore the ultrafast dynamics. Here the authors combine transient absorption and photo-ion spectroscopy methods to explore and control the attosecond pulse initiated excitation, ionization and Auger decay in Kr atoms.
- Konrad Hütten
- , Michael Mittermair
- & Birgitta Bernhardt
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Article
| Open AccessSelf-probing spectroscopy of XUV photo-ionization dynamics in atoms subjected to a strong-field environment
Single photon ionization—one of the most fundamental light matter interactions—can be significantly altered in a strong-field environment. Here the authors demonstrate a self-probing spectroscopy technique, resolving the evolution of the interaction in helium atoms with attosecond precision.
- Doron Azoury
- , Michael Krüger
- & Nirit Dudovich
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Article
| Open AccessAnisotropic attosecond charge carrier dynamics and layer decoupling in quasi-2D layered SnS2
Owing to their layered nature, transition metal dichalcogenides possess an anisotropic electronic structure whose impact on carrier dynamics is not fully known. Here, the authors use X-ray spectroscopy to unveil the electronic coupling and attosecond dynamics in SnS2, a prototypical van der Waals layered crystal.
- Calley N. Eads
- , Dmytro Bandak
- & Oliver L. A. Monti
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Article
| Open AccessNanoplasmonic electron acceleration by attosecond-controlled forward rescattering in silver clusters
Accelerating electrons to high energy and controlling their properties on ultrafast timescales is challenging. Here the authors show controlled acceleration of electron bunches using forward scattering in the resonantly enhanced polarization field of silver clusters driven by a phase-tuned two-color laser field.
- Johannes Passig
- , Sergey Zherebtsov
- & Thomas Fennel
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Article
| Open AccessFew-femtosecond passage of conical intersections in the benzene cation
Attosecond science is beginning to provide the tools to study the previously unattainable crucial first few femtoseconds of photochemical reactions. Here, the authors investigate extremely rapid population transfer via conical intersections in the excited benzene cation, both by experiment and computation.
- M. C. E. Galbraith
- , S. Scheit
- & J. Mikosch
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Article
| Open AccessHigh-order harmonic generation from the dressed autoionizing states
High-energy photons in XUV range and attosecond pulses are generated from infrared laser pulses through high harmonic generation in gases and solids. Here, the authors demonstrate the microscopic origin of resonant harmonic generation involving the autoionizing states of Sn in plasma plumes.
- M. A. Fareed
- , V. V. Strelkov
- & T. Ozaki
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Article
| Open AccessDynamics of valence-shell electrons and nuclei probed by strong-field holography and rescattering
Capturing ultrafast molecular dynamics is difficult as the process involves coupled and very fast motions of electrons and nuclei. Here the authors study non-adiabatic dynamics in the NO molecule using strong-field photoelectron holography to shed light on the valence-shell electron dynamics.
- Samuel G. Walt
- , Niraghatam Bhargava Ram
- & Hans Jakob Wörner
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Article
| Open AccessOptical gating and streaking of free electrons with sub-optical cycle precision
Pulsed electron beams with ultrafast duration are desirable to study atomic processes occurring over the natural time scales of electronic motion. Here the authors demonstrate the generation of electron pulses down to attosecond time scales by using optical gating and streaking method.
- M. Kozák
- , J. McNeur
- & P. Hommelhoff
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Article
| Open AccessSub-10-fs control of dissociation pathways in the hydrogen molecular ion with a few-pulse attosecond pulse train
Attosecond laser pulses allow to explore the ultrafast atomic or molecular processes occurring in chemical reactions. Here the authors utilize a sequence of two XUV pump-probe pulses to control the dissociation dynamics of the hydrogen molecular ion.
- Yasuo Nabekawa
- , Yusuke Furukawa
- & Katsumi Midorikawa
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Article
| Open AccessSynthesis and characterization of attosecond light vortices in the extreme ultraviolet
Twisted light beams have found several applications in the infrared and visible regime, but reaching the extreme ultraviolet has been difficult due to lack of sources. Here the authors report generation of helically shaped extreme ultraviolet trains of attosecond pulses via high harmonic generation.
- R. Géneaux
- , A. Camper
- & T. Ruchon
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Article
| Open AccessAttosecond nanoscale near-field sampling
Photoemission from nanometre-scale structures offer a route toward ultrafast light-field-driven electronic nanocircuits. Here, the authors use attosecond streaking spectroscopy for nanoscale characterization of near-fields in the vicinity of tapered gold nanowires.
- B. Förg
- , J. Schötz
- & M. F. Kling
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Article
| Open Access0.5-keV Soft X-ray attosecond continua
Attosecond soft X-ray pulses hold promise for probing electronic dynamics in real time, but it is challenging to achieve element sensitivity while maintaining temporal resolution. Teichmann et al. report the cover of carbon, nitrogen and oxygen absorption edges with an isolated pulse supporting 13 as duration.
- S. M. Teichmann
- , F. Silva
- & J. Biegert
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Article
| Open AccessSpectral phase measurement of a Fano resonance using tunable attosecond pulses
Resonant absorption of light in atoms can lead to autoionization, whose probability exhibits a Fano intensity profile. Here, the authors use attosecond pulses and weak infrared radiation to study the phase variation of the photoionization amplitude across an autoionization resonance in argon.
- M. Kotur
- , D. Guénot
- & A. L’Huillier