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https://www.readbyqxmd.com/read/28636679/towards-the-analysis-of-attosecond-dynamics-in-complex-systems
#1
C-Z Gao, P M Dinh, P-G Reinhard, E Suraud
We study from a theoretical perspective the ionization of molecules and clusters induced by irradiation of a combined two-color laser field consisting of a train of attosecond XUV pulses in the presence of an IR field. We use time-dependent density-functional theory (TDDFT) in real time and real space as a theoretical tool. The calculated results are compared to experimental data when available. We also compare TDDFT with results obtained using a time-dependent Schrödinger equation (TDSE), which is well suited to simple systems while TDDFT allows dealing with more complex molecules and clusters...
June 21, 2017: Physical Chemistry Chemical Physics: PCCP
https://www.readbyqxmd.com/read/28631783/ultrafast-charge-dynamics-in-glycine-induced-by-attosecond-pulses
#2
David Ayuso, Alicia Palacios, Piero Decleva, Fernando Martín
The combination of attosecond pump-probe techniques with mass spectrometry methods has recently led to the first experimental demonstration of ultrafast charge dynamics in a biomolecule, the amino acid phenylalanine [Calegari et al., Science, 2014, 346, 336]. Using an extension of the static-exchange density functional theory (DFT) method, the observed dynamics was explained as resulting from the coherent superposition of ionic states produced by the broadband attosecond pulse. Here, we have used the static-exchange DFT method to investigate charge migration induced by attosecond pulses in the glycine molecule...
June 20, 2017: Physical Chemistry Chemical Physics: PCCP
https://www.readbyqxmd.com/read/28630331/distinguishing-attosecond-electron-electron-scattering-and-screening-in-transition-metals
#3
Cong Chen, Zhensheng Tao, Adra Carr, Piotr Matyba, Tibor Szilvási, Sebastian Emmerich, Martin Piecuch, Mark Keller, Dmitriy Zusin, Steffen Eich, Markus Rollinger, Wenjing You, Stefan Mathias, Uwe Thumm, Manos Mavrikakis, Martin Aeschlimann, Peter M Oppeneer, Henry Kapteyn, Margaret Murnane
Electron-electron interactions are the fastest processes in materials, occurring on femtosecond to attosecond timescales, depending on the electronic band structure of the material and the excitation energy. Such interactions can play a dominant role in light-induced processes such as nano-enhanced plasmonics and catalysis, light harvesting, or phase transitions. However, to date it has not been possible to experimentally distinguish fundamental electron interactions such as scattering and screening. Here, we use sequences of attosecond pulses to directly measure electron-electron interactions in different bands of different materials with both simple and complex Fermi surfaces...
June 19, 2017: Proceedings of the National Academy of Sciences of the United States of America
https://www.readbyqxmd.com/read/28619939/coherent-imaging-of-an-attosecond-electron-wave-packet
#4
D M Villeneuve, Paul Hockett, M J J Vrakking, Hiromichi Niikura
Electrons detached from atoms or molecules by photoionization carry information about the quantum state from which they originate, as well as the continuum states into which they are released. Generally, the photoelectron momentum distribution is composed of a coherent sum of angular momentum components, each with an amplitude and phase. Here we show, by using photoionization of neon, that a train of attosecond pulses synchronized with an infrared laser field can be used to disentangle these angular momentum components...
June 16, 2017: Science
https://www.readbyqxmd.com/read/28618496/plasma-high-order-harmonic-generation-from-ultraintense-laser-pulses
#5
Suo Tang, Naveen Kumar, Christoph H Keitel
Plasma high-order-harmonic generation from an extremely intense short-pulse laser is explored by including the effects of ion motion, electron-ion collisions, and radiation reaction force in the plasma dynamics. The laser radiation pressure induces plasma ion motion through the hole-boring effect, resulting in frequency shifting and widening of the harmonic spectra. The classical radiation reaction force slightly mitigates the frequency broadening caused by the ion motion. Based on the results and physical considerations, parameter maps highlighting the optimum regions for generating a single intense attosecond pulse and coherent XUV radiation are presented...
May 2017: Physical Review. E
https://www.readbyqxmd.com/read/28597901/a-perspective-for-investigating-photo-induced-molecular-dynamics-from-within-with-femtosecond-free-electron-lasers
#6
Nora Berrah
Photo-induced molecular dynamics can now be investigated using free electron lasers (FELs) whose attributes are unprecedented brightness, few femtosecond pulses duration and in the near future few hundreds of attosecond pulse duration. These relatively new tools are utilized to investigate photon-induced physical and chemical processes by ionizing inner-shell electrons and thus unlocking molecular dynamics from within.
June 9, 2017: Physical Chemistry Chemical Physics: PCCP
https://www.readbyqxmd.com/read/28572835/symmetry-controlled-time-structure-of-high-harmonic-carrier-fields-from-a-solid
#7
F Langer, M Hohenleutner, U Huttner, S W Koch, M Kira, R Huber
High-harmonic (HH) generation in crystalline solids1-6 marks an exciting development, with potential applications in high-efficiency attosecond sources7, all-optical bandstructure reconstruction8,9, and quasiparticle collisions10,11. Although the spectral1-4 and temporal shape5 of the HH intensity has been described microscopically1-6,12, the properties of the underlying HH carrier wave have remained elusive. Here we analyse the train of HH waveforms generated in a crystalline solid by consecutive half cycles of the same driving pulse...
April 2017: Nature Photonics
https://www.readbyqxmd.com/read/28555640/attosecond-interferometry-with-self-amplified-spontaneous-emission-of-a-free-electron-laser
#8
Sergey Usenko, Andreas Przystawik, Markus Alexander Jakob, Leslie Lamberto Lazzarino, Günter Brenner, Sven Toleikis, Christian Haunhorst, Detlef Kip, Tim Laarmann
Light-phase-sensitive techniques, such as coherent multidimensional spectroscopy, are well-established in a broad spectral range, already spanning from radio-frequencies in nuclear magnetic resonance spectroscopy to visible and ultraviolet wavelengths in nonlinear optics with table-top lasers. In these cases, the ability to tailor the phases of electromagnetic waves with high precision is essential. Here we achieve phase control of extreme-ultraviolet pulses from a free-electron laser (FEL) on the attosecond timescale in a Michelson-type all-reflective interferometric autocorrelator...
May 30, 2017: Nature Communications
https://www.readbyqxmd.com/read/28524203/time-resolved-photoelectron-spectroscopy-of-ir-driven-electron-dynamics-in-a-charge-transfer-model-system
#9
Mirjam Falge, Friedrich Georg Fröbel, Volker Engel, Stefanie Gräfe
If the adiabatic approximation is valid, electrons smoothly adapt to molecular geometry changes. In contrast, as a characteristic of diabatic dynamics, the electron density does not follow the nuclear motion. Recently, we have shown that the asymmetry in time-resolved photoelectron spectra serves as a tool to distinguish between these dynamics [Falge et al., J. Phys. Chem. Lett., 2012, 3, 2617]. Here, we investigate the influence of an additional, moderately intense infrared (IR) laser field, as often applied in attosecond time-resolved experiments, on such asymmetries...
May 19, 2017: Physical Chemistry Chemical Physics: PCCP
https://www.readbyqxmd.com/read/28488433/attosecond-electron-dynamics-in-molecules
#10
Mauro Nisoli, Piero Decleva, Francesca Calegari, Alicia Palacios, Fernando Martín
Advances in attosecond science have led to a wealth of important discoveries in atomic, molecular, and solid-state physics and are progressively directing their footsteps toward problems of chemical interest. Relevant technical achievements in the generation and application of extreme-ultraviolet subfemtosecond pulses, the introduction of experimental techniques able to follow in time the electron dynamics in quantum systems, and the development of sophisticated theoretical methods for the interpretation of the outcomes of such experiments have raised a continuous growing interest in attosecond phenomena, as demonstrated by the vast literature on the subject...
May 10, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28468499/attosecond-dynamics-of-molecular-electronic-ring-currents
#11
Kai-Jun Yuan, Chuan-Cun Shu, Daoyi Dong, André D Bandrauk
Ultrafast charge migration is of fundamental importance to photoinduced chemical reactions. However, exploring such a quantum dynamical process requires demanding spatial and temporal resolutions. We show how electronic coherence dynamics induced in molecules by a circularly polarized UV pulse can be tracked by using a time-delayed circularly polarized attosecond X-ray pulse. The X-ray probe spectra retrieve an image at different time delays, encoding instantaneous pump-induced circular charge migration information on an attosecond time scale...
May 5, 2017: Journal of Physical Chemistry Letters
https://www.readbyqxmd.com/read/28463649/extending-quantum-chemistry-of-bound-states-to-electronic-resonances
#12
Thomas-C Jagau, Ksenia B Bravaya, Anna I Krylov
Electronic resonances are metastable states with finite lifetime embedded in the ionization or detachment continuum. They are ubiquitous in chemistry, physics, and biology. Resonances play a central role in processes as diverse as DNA radiolysis, plasmonic catalysis, and attosecond spectroscopy. This review describes novel equation-of-motion coupled-cluster (EOM-CC) methods designed to treat resonances and bound states on an equal footing. Built on complex-variable techniques such as complex scaling and complex absorbing potentials that allow resonances to be associated with a single eigenstate of the molecular Hamiltonian rather than several continuum eigenstates, these methods extend electronic-structure tools developed for bound states to electronic resonances...
May 5, 2017: Annual Review of Physical Chemistry
https://www.readbyqxmd.com/read/28454168/laser-waveform-control-of-extreme-ultraviolet-high-harmonics-from-solids
#13
Yong Sing You, Mengxi Wu, Yanchun Yin, Andrew Chew, Xiaoming Ren, Shima Gholam-Mirzaei, Dana A Browne, Michael Chini, Zenghu Chang, Kenneth J Schafer, Mette B Gaarde, Shambhu Ghimire
Solid-state high-harmonic sources offer the possibility of compact, high-repetition-rate attosecond light emitters. However, the time structure of high harmonics must be characterized at the sub-cycle level. We use strong two-cycle laser pulses to directly control the time-dependent nonlinear current in single-crystal MgO, leading to the generation of extreme ultraviolet harmonics. We find that harmonics are delayed with respect to each other, yielding an atto-chirp, the value of which depends on the laser field strength...
May 1, 2017: Optics Letters
https://www.readbyqxmd.com/read/28430519/energy-resolved-ultrashort-delays-of-photoelectron-emission-clocked-by-orthogonal-two-color-laser-fields
#14
Xiaochun Gong, Cheng Lin, Feng He, Qiying Song, Kang Lin, Qinying Ji, Wenbin Zhang, Junyang Ma, Peifen Lu, Yunquan Liu, Heping Zeng, Weifeng Yang, Jian Wu
A phase-controlled orthogonal two-color (OTC) femtosecond laser pulse is employed to probe the time delay of photoelectron emission in the strong-field ionization of atoms. The OTC field spatiotemporally steers the emission dynamics of the photoelectrons and meanwhile allows us to unambiguously distinguish the main and sideband peaks of the above-threshold ionization spectrum. The relative phase shift between the main and sideband peaks, retrieved from the phase-of-phase of the photoelectron spectrum as a function of the laser phase, gradually decreases with increasing electron energy, and becomes zero for the fast electron which is mainly produced by the rescattering process...
April 7, 2017: Physical Review Letters
https://www.readbyqxmd.com/read/28388142/theory-of-attosecond-delays-in-molecular-photoionization
#15
Denitsa Baykusheva, Hans Jakob Wörner
We present a theoretical formalism for the calculation of attosecond delays in molecular photoionization. It is shown how delays relevant to one-photon-ionization, also known as Eisenbud-Wigner-Smith delays, can be obtained from the complex dipole matrix elements provided by molecular quantum scattering theory. These results are used to derive formulae for the delays measured by two-photon attosecond interferometry based on an attosecond pulse train and a dressing femtosecond infrared pulse. These effective delays are first expressed in the molecular frame where maximal information about the molecular photoionization dynamics is available...
March 28, 2017: Journal of Chemical Physics
https://www.readbyqxmd.com/read/28380932/self-corrected-chip-based-dual-comb-spectrometer
#16
Nicolas Bourbeau Hébert, Jérôme Genest, Jean-Daniel Deschênes, Hugo Bergeron, George Y Chen, Champak Khurmi, David G Lancaster
We present a dual-comb spectrometer based on two passively mode-locked waveguide lasers integrated in a single Er-doped ZBLAN chip. This original design yields two free-running frequency combs having a high level of mutual stability. We developed in parallel a self-correction algorithm that compensates residual relative fluctuations and yields mode-resolved spectra without the help of any reference laser or control system. Fluctuations are extracted directly from the interferograms using the concept of ambiguity function, which leads to a significant simplification of the instrument that will greatly ease its widespread adoption and commercial deployment...
April 3, 2017: Optics Express
https://www.readbyqxmd.com/read/28380889/attosecond-chirp-effect-on-the-transient-absorption-spectrum-of-laser-dressed-helium-atom
#17
Haiwen Zhao, Candong Liu, Yinghui Zheng, Zhinan Zeng, Ruxin Li
We theoretically investigate the attosecond transient absorption spectrum of helium atom in the presence of an infrared-dressed laser pulse upon scanning their relative delay, with the particular emphasis on the chirp effect of the attosecond pulse. By numerically solving the fully three-dimensional time-dependent Schrödinger equation, we identify the attoscecond chirp can induce the temporal shift of the absorption spectrogram along the delay axis. Additionally, it is found that the extent of the temporal shift is dependent on both the position of the absorption line and the infrared pulse wavelength, which is well confirmed and reproduced by a three-level model...
April 3, 2017: Optics Express
https://www.readbyqxmd.com/read/28380874/high-energy-few-cycle-yb-doped-fiber-amplifier-source-based-on-a-single-nonlinear-compression-stage
#18
L Lavenu, M Natile, F Guichard, Y Zaouter, M Hanna, E Mottay, P Georges
A simple, compact, and efficient few-cycle laser source at a central wavelength of 1 µm is presented. The system is based on a high-energy femtosecond ytterbium-doped fiber amplifier delivering 130 fs, 250 µJ pulses at 200 kHz, corresponding to 1.5 GW of peak power and an average power of 50 W. The unprecedented short pulse duration at the output of this system is obtained by use of spectral intensity and phase shaping, allowing for both gain narrowing mitigation and the compensation of the nonlinear accumulated spectral phase...
April 3, 2017: Optics Express
https://www.readbyqxmd.com/read/28362766/selective-suppression-of-high-order-harmonics-within-phase-matched-spectral-regions
#19
Gavriel Lerner, Tzvi Diskin, Ofer Neufeld, Ofer Kfir, Oren Cohen
Phase matching in high-harmonic generation leads to enhancement of multiple harmonics. It is sometimes desired to control the spectral structure within the phase-matched spectral region. We propose a scheme for selective suppression of high-order harmonics within the phase-matched spectral region while weakly influencing the other harmonics. The method is based on addition of phase-mismatched segments within a phase-matched medium. We demonstrate the method numerically in two examples. First, we show that one phase-mismatched segment can significantly suppress harmonic orders 9, 15, and 21...
April 1, 2017: Optics Letters
https://www.readbyqxmd.com/read/28306283/limits-of-strong-field-rescattering-in-the-relativistic-regime
#20
M Klaiber, K Z Hatsagortsyan, J Wu, S S Luo, P Grugan, B C Walker
Recollision for a laser driven atomic system is investigated in the relativistic regime via a strong field quantum description and Monte Carlo semiclassical approach. We find the relativistic recollision energy cutoff is independent of the ponderomotive potential U_{p}, in contrast to the well-known 3.2U_{p} scaling. The relativistic recollision energy cutoff is determined by the ionization potential of the atomic system and achievable with non-negligible recollision flux before entering a "rescattering free" interaction...
March 3, 2017: Physical Review Letters
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