keyword
https://read.qxmd.com/read/38536928/bond-length-dependence-of-attosecond-ionization-delays-in-o-2-arising-from-electron-correlation-to-a-shape-resonance
#1
JOURNAL ARTICLE
Daniel Hammerland, Thomas Berglitsch, Pengju Zhang, Tran Trung Luu, Kiyoshi Ueda, Robert R Lucchese, Hans Jakob Wörner
We experimentally and theoretically demonstrate that electron correlation can cause the bond-length sensitivity of a shape resonance to induce an unexpected vibrational state-dependent ionization delay in a nonresonant channel. This discovery was enabled by a high-resolution attosecond-interferometry experiment based on a 400-nm driving and dressing wavelength. The short-wavelength driver results in a 6.2-electron volt separation between harmonics, markedly reducing the spectral overlap in the measured interferogram...
March 29, 2024: Science Advances
https://read.qxmd.com/read/38530933/simulating-attochemistry-which-dynamics-method-to-use
#2
JOURNAL ARTICLE
Thierry Tran, Anthony Ferté, Morgane Vacher
Attochemistry aims to exploit the properties of coherent electronic wavepackets excited via attosecond pulses to control the formation of photoproducts. Such molecular processes can, in principle, be simulated with various nonadiabatic dynamics methods, yet the impact of the approximations underlying the methods is rarely assessed. The performances of widely used mixed quantum-classical approaches, Tully surface hopping, and classical Ehrenfest methods are evaluated against the high-accuracy DD-vMCG quantum dynamics...
March 26, 2024: Journal of Physical Chemistry Letters
https://read.qxmd.com/read/38530705/far-field-petahertz-sampling-of-plasmonic-fields
#3
JOURNAL ARTICLE
Kai-Fu Wong, Weiwei Li, Zilong Wang, Vincent Wanie, Erik Månsson, Dominik Hoeing, Johannes Blöchl, Thomas Nubbemeyer, Abdallah Azzeer, Andrea Trabattoni, Holger Lange, Francesca Calegari, Matthias F Kling
The response of metal nanostructures to optical excitation leads to localized surface plasmon (LSP) generation with nanoscale field confinement driving applications in, for example, quantum optics and nanophotonics. Field sampling in the terahertz domain has had a tremendous impact on the ability to trace such collective excitations. Here, we extend such capabilities and introduce direct sampling of LSPs in a more relevant petahertz domain. The method allows to measure the LSP field in arbitrary nanostructures with subcycle precision...
March 26, 2024: Nano Letters
https://read.qxmd.com/read/38530393/nonadiabatic-charge-transfer-within-photoexcited-nickel-porphyrins
#4
JOURNAL ARTICLE
Maria A Naumova, Gheorghe Paveliuc, Mykola Biednov, Katharina Kubicek, Aleksandr Kalinko, Jie Meng, Mingli Liang, Ahibur Rahaman, Mohamed Abdellah, Stefano Checchia, Frederico Alves Lima, Peter Zalden, Wojciech Gawelda, Christian Bressler, Huifang Geng, Weihua Lin, Yan Liu, Qian Zhao, Qinying Pan, Marufa Akter, Qingyu Kong, Marius Retegan, David J Gosztola, Mátyás Pápai, Dmitry Khakhulin, Max Lawson Daku, Kaibo Zheng, Sophie E Canton
Metalloporphyrins with open d-shell ions can drive biochemical energy cycles. However, their utilization in photoconversion is hampered by rapid deactivation. Mapping the relaxation pathways is essential for elaborating strategies that can favorably alter the charge dynamics through chemical design and photoexcitation conditions. Here, we combine transient optical absorption spectroscopy and transient X-ray emission spectroscopy with femtosecond resolution to probe directly the coupled electronic and spin dynamics within a photoexcited nickel porphyrin in solution...
March 26, 2024: Journal of Physical Chemistry Letters
https://read.qxmd.com/read/38523743/angular-dispersion-of-free-electron-light-coupling-in-an-optical-fiber-integrated-metagrating
#5
JOURNAL ARTICLE
Matthias Liebtrau, Albert Polman
Free electrons can couple to optical material excitations on nanometer-length and attosecond-time scales, opening-up unique opportunities for both the generation of radiation and the manipulation of the electron wave function. Here, we exploit the Smith-Purcell effect to experimentally study the coherent coupling of free electrons and light in a circular metallo-dielectric metagrating that is fabricated onto the input facet of a multimode optical fiber. Using hyperspectral angle-resolved (HSAR) far-field imaging inside a scanning electron microscope, we probe the angular dispersion of Smith-Purcell radiation (SPR) that is simultaneously generated in free space and inside the fiber by an electron beam that grazes the metagrating at a nanoscale distance...
March 20, 2024: ACS Photonics
https://read.qxmd.com/read/38491712/spectral-modulation-of-high-order-harmonics-in-relativistic-laser-solid-interaction
#6
JOURNAL ARTICLE
B Y Li, F Liu, M Chen, X H Yuan, Z M Sheng, J Zhang
Spectral modulation of high-order harmonics generated in relativistic laser-solid interaction is investigated. Numerical simulations show that the modulation depends on surface plasma density profile, resulting in spectral envelope modulation and regular and irregular harmonic splitting. The mathematical and physical connections between the spectral modulation of high-order harmonics and the temporal modification of attosecond pulse train are explained. Based on these understandings, we propose a possible method to produce isolated attosecond pulses by tailoring surface the plasma profile...
February 2024: Physical Review. E
https://read.qxmd.com/read/38489453/interference-induced-generation-of-a-chirp-free-short-isolated-attosecond-pulse-in-the-water-window-region-with-multicolor-laser-fields
#7
JOURNAL ARTICLE
Jin-Xu Du, Guo-Li Wang, Xuan-Hong Gao, Xiao-Yong Li, Zhi-Hong Jiao, Song-Feng Zhao, Xiao-Xin Zhou
Compensating for the intrinsic attosecond chirp (atto-chirp) of wideband high-order harmonics in the water window region is a significant challenge, in order to obtain isolated attosecond pulses (IAPs) with a width of tens of attoseconds (as). Here, we propose to realize the generation of IAP with duration as short as 20 as, central energy of 365 eV, and bandwidth exceeding 150 eV from chirp-free high harmonics generated by a four-color driving laser, without the necessity for atto-chirp compensation with natural materials...
March 15, 2024: Optics Letters
https://read.qxmd.com/read/38444565/high-harmonic-spectroscopy-of-impulsively-aligned-1-3-cyclohexadiene-signatures-of-attosecond-charge-migration
#8
JOURNAL ARTICLE
Andres Tehlar, Jakob T Casanova, Andrey Dnestryan, Frank Jensen, Lars Bojer Madsen, Oleg I Tolstikhin, Hans Jakob Wörner
High-harmonic spectroscopy is an all-optical technique with inherent attosecond temporal resolution that has been successfully employed to reconstruct charge migration, electron-tunneling dynamics, and conical-intersection dynamics. Here, we demonstrate the extension of two key components of high-harmonic spectroscopy, i.e., impulsive alignment and measurements with multiple driving wavelengths to 1,3-cyclohexadiene and benzene. In the case of 1,3-cyclohexadiene, we find that the temporal sequence of maximal and minimal emitted high-harmonic intensities as a function of the delay between the alignment and probe pulses inverts between 25 and 30 eV and again between 35 and 40 eV when an 800-nm driver is used, but no inversions are observed with a 1420-nm driver...
January 2024: Structural Dynamics (Melville, N.Y.)
https://read.qxmd.com/read/38439240/furion-modeling-of-fel-pulses-propagation-in-dispersive-soft-x-ray-beamline-systems
#9
JOURNAL ARTICLE
Ye Zhu, Chuan Yang, Kai Hu, Chen Wu, Junyao Luo, Zhou Hao, Zhenjiang Xing, Qinming Li, Zhongmin Xu, Weiqing Zhang
Modern X-ray free-electron lasers (XFELs) can generate pulses with durations ranging from femtoseconds to attoseconds. The numerical evaluation of ultra-short XFEL pulses through beamline systems is a critical process of beamline system design. However, the bandwidth of such ultra-short XFEL pulses is often non-negligible, and the propagation cannot be simply approximated using the central wavelength, especially in dispersive beamline systems. We developed a numerical model which is called Fourier optics based Ultrashort x-Ray pulse propagatION tool (FURION)...
February 12, 2024: Optics Express
https://read.qxmd.com/read/38437291/design-and-simulation-of-an-extreme-ultraviolet-metalens-based-on-the-pancharatnam-berry-phase
#10
JOURNAL ARTICLE
Xu Mao, Gang Yu, Yongmei Zhao, Bo Wei, Zhaofeng Li, Fuhua Yang, Xiaodong Wang
Extreme ultraviolet (EUV) radiation plays a key role in the fields of material science, attosecond metrology, and lithography. However, the reflective optical components typically used in EUV systems contribute to their bulky size, weight, and increased costs for fabrication. In this paper, we theoretically investigate transmissive metalens designs capable of focusing the EUV light based on the Pancharatnam-Berry phase. The designed metalens is composed of nanoscale elliptical holes, which can guide and manipulate EUV light due to the higher refractive index of the vacuum holes compared to that of the surrounding material...
March 1, 2024: Applied Optics
https://read.qxmd.com/read/38394372/anisotropy-parameters-for-two-color-photoionization-phases-in-randomly-oriented-molecules-theory-and-experiment-in-methane-and-deuteromethane
#11
JOURNAL ARTICLE
Dominik Ertel, David Busto, Ioannis Makos, Marvin Schmoll, Jakub Benda, Francesca Bragheri, Roberto Osellame, Eva Lindroth, Serguei Patchkovskii, Zdeněk Mašín, Giuseppe Sansone
We present combined theoretical and experimental work investigating the angle-resolved phases of the photoionization process driven by a two-color field consisting of an attosecond pulse train and an infrared pulse in an ensemble of randomly oriented molecules. We derive a general form for the two-color photoelectron (and time-delay) angular distribution valid also in the case of chiral molecules and when relative polarizations of the photons contributing to the attosecond photoelectron interferometer differ...
February 23, 2024: Journal of Physical Chemistry. A
https://read.qxmd.com/read/38381830/compact-realization-of-all-attosecond-pump-probe-spectroscopy
#12
JOURNAL ARTICLE
Martin Kretschmar, Evaldas Svirplys, Mikhail Volkov, Tobias Witting, Tamás Nagy, Marc J J Vrakking, Bernd Schütte
The ability to perform attosecond-pump attosecond-probe spectroscopy (APAPS) is a longstanding goal in ultrafast science. While first pioneering experiments demonstrated the feasibility of APAPS, the low repetition rates (10 to 120 Hz) and the large footprints of existing setups have so far hindered the widespread exploitation of APAPS. Here, we demonstrate two-color APAPS using a commercial laser system at 1 kHz, straightforward post-compression in a hollow-core fiber, and a compact high-harmonic generation (HHG) setup...
February 23, 2024: Science Advances
https://read.qxmd.com/read/38373145/high-order-harmonic-generation-in-solids-the-role-of-intraband-transitions-in-extreme-nonlinear-optics
#13
REVIEW
Hideki Hirori, Shunsuke A Sato, Yoshihiko Kanemitsu
High-order harmonic generation (HHG) in gases is frequently used nowadays to produce attosecond pulses and coherent radiation in the visible-to-soft X-ray spectral range. HHG in solids is a natural extension of the idea of HHG in gases, and its first observation about ten years ago opened the door to investigations on attosecond electron dynamics in solids and the development of solid-state attosecond light sources. The common process in both types of HHG is nonlinear photocarrier generation, and thus, transitions between different bands (interband transitions) are always important for HHG...
February 19, 2024: Journal of Physical Chemistry Letters
https://read.qxmd.com/read/38366970/tracking-molecular-fragmentation-in-electron-ionization-mass-spectrometry-with-ultrafast-time-resolution
#14
JOURNAL ARTICLE
Marcos Dantus
ConspectusMass spectrometry is a powerful analytical method capable of identifying compounds given a minute amount of material. The fragmentation pattern that results following molecular activation serves as a fingerprint that can be matched to a database compound for identification. Over the past half century, studies have addressed and, in many cases, named the chemical reactions that lead to some of the principal fragment ions. Theories have been developed to predict the observed fragmentation patterns, many of which assume that energy redistributes prior to dissociation...
February 17, 2024: Accounts of Chemical Research
https://read.qxmd.com/read/38364263/tracking-electron-motion-within-and-outside-of-floquet-bands-from-attosecond-pulse-trains-in-time-resolved-arpes
#15
JOURNAL ARTICLE
Ofer Neufeld, Hannes Huebener, Umberto De Giovannini, Angel Rubio
Floquet engineering has recently emerged as a technique for controlling material properties with light. Floquet phases can be probed with time- and angle-resolved photoelectron spectroscopy (Tr-ARPES), providing direct access to the laser-dressed electronic bands. Applications of Tr-ARPES to date focused on observing the Floquet-Bloch bands themselves, and their build-up and dephasing on sub-laser-cycle timescales. However, momentum and energy resolved sub-laser-cycle dynamics between Floquet bands have not been analyzed...
February 16, 2024: Journal of Physics. Condensed Matter: An Institute of Physics Journal
https://read.qxmd.com/read/38359104/attosecond-pump-attosecond-probe-x-ray-spectroscopy-of-liquid-water
#16
JOURNAL ARTICLE
Shuai Li, Lixin Lu, Swarnendu Bhattacharyya, Carolyn Pearce, Kai Li, Emily T Nienhuis, Gilles Doumy, R D Schaller, S Moeller, M-F Lin, G Dakovski, D J Hoffman, D Garratt, Kirk A Larsen, J D Koralek, C Y Hampton, D Cesar, Joseph Duris, Z Zhang, Nicholas Sudar, James P Cryan, A Marinelli, Xiaosong Li, Ludger Inhester, Robin Santra, Linda Young
Attosecond-pump/attosecond-probe experiments have long been sought as the most straightforward method to observe electron dynamics in real time. Although numerous successes have been achieved with overlapped near infrared femtosecond and extreme ultraviolet attosecond pulses combined with theory, true attosecond-pump/attosecond-probe experiments have been limited. We used a synchronized attosecond x-ray pulse pair from an x-ray free electron laser to study the electronic response to valence ionization in liquid water via all x-ray attosecond transient absorption spectroscopy (AX-ATAS)...
February 15, 2024: Science
https://read.qxmd.com/read/38349969/raman-spectroscopy-of-conical-intersections-using-entangled-photons
#17
JOURNAL ARTICLE
Deependra Jadoun, Zhedong Zhang, Markus Kowalewski
Ultrafast Raman spectroscopy with attosecond pulses in the extreme ultraviolet and X-ray regime has been proposed theoretically for tracking the non-adiabatic dynamics of molecules in great detail. The large bandwidth of these pulses, which span several electronvolts within a couple of femtoseconds, provides a unique tool for tracking non-adiabatic phenomena. However, spectroscopy with classical light is limited by the time-bandwidth product of the probe laser pulse. In this work, we theoretically investigate an ultrafast Raman spectroscopy scheme that utilizes pairs of entangled photons...
February 13, 2024: Journal of Physical Chemistry Letters
https://read.qxmd.com/read/38335335/generation-of-ultrabrilliant-polarized-attosecond-electron-bunches-via-dual-wake-injection
#18
JOURNAL ARTICLE
Ting Sun, Qian Zhao, Feng Wan, Yousef I Salamin, Jian-Xing Li
Laser wakefield acceleration is paving the way for the next generation of electron accelerators, for their own sake and as radiation sources. A controllable dual-wake injection scheme is put forward here to generate an ultrashort triplet electron bunch with high brightness and high polarization, employing a radially polarized laser as a driver. We find that the dual wakes can be driven by both transverse and longitudinal components of the laser field in the quasiblowout regime, sustaining the laser-modulated wakefield which facilitates the subcycle and transversely split injection of the triplet bunch...
January 26, 2024: Physical Review Letters
https://read.qxmd.com/read/38324399/tracing-photoinduced-hydrogen-migration-in-alcohol-dications-from-time-resolved-molecular-frame-photoelectron-angular-distributions
#19
JOURNAL ARTICLE
T Kuraoka, S Goto, M Kanno, S Díaz-Tendero, J Reino-González, F Trinter, A Pier, L Sommerlad, N Melzer, O D McGinnis, J Kruse, T Wenzel, T Jahnke, H Xue, N Kishimoto, K Yoshikawa, Y Tamura, F Ota, K Hatada, K Ueda, F Martín
The recent implementation of attosecond and few-femtosecond X-ray pump/X-ray probe schemes in large-scale free-electron laser facilities has opened the way to visualize fast nuclear dynamics in molecules with unprecedented temporal and spatial resolution. Here, we present the results of theoretical calculations showing how polarization-averaged molecular-frame photoelectron angular distributions (PA-MFPADs) can be used to visualize the dynamics of hydrogen migration in methanol, ethanol, propanol, and isopropyl alcohol dications generated by X-ray irradiation of the corresponding neutral species...
February 7, 2024: Journal of Physical Chemistry. A
https://read.qxmd.com/read/38300104/unveiling-out-of-loop-attosecond-timing-jitter-precision-in-ti-sapphire-mode-locked-lasers-with-an-optical-heterodyne-technique
#20
JOURNAL ARTICLE
Haitao Wu, Hao Xu, Jianye Zhao
The out-of-loop timing jitter exhibited in free-running Ti:sapphire mode-locked lasers with attosecond resolution is demonstrated using an optical heterodyne technique. To assess the feasibility of the experiment and discrimination signal properties, numerical simulations were conducted for Ti:sapphire mode-locked lasers. For accurately characterizing the genuine phase noise exhibited by Ti:sapphire mode-locked lasers, out-of-loop measurements were conducted, and a straightforward yet improved optical heterodyne setup was employed, allowing simultaneous low-bandwidth locking and out-of-loop timing jitter measurements with two Ti:sapphire mode-locked lasers...
February 1, 2024: Optics Letters
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