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https://www.readbyqxmd.com/read/28524203/time-resolved-photoelectron-spectroscopy-of-ir-driven-electron-dynamics-in-a-charge-transfer-model-system
#1
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
#2
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
#3
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
#4
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
#5
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
#6
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
#7
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
#8
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
#9
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
#10
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
#11
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
#12
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
https://www.readbyqxmd.com/read/28295094/excess-carrier-envelope-phase-noise-generation-in-saturable-absorbers
#13
Nils Raabe, Tianli Feng, Mark Mero, Haochen Tian, Youjian Song, Wolfgang Hänsel, Ronald Holzwarth, Alexander Sell, Armin Zach, Günter Steinmeyer
Attosecond spectroscopy and precision frequency metrology depend on the stabilization of the carrier-envelope phase (CEP) of mode-locked lasers. Unfortunately, the phase of only a few types of lasers can be stabilized to jitters in the few-hundred millirad range. In a comparative experimental study, we analyze a femtosecond Ti:sapphire laser and three mode-locked fiber lasers. We numerically demodulate recorded time series of the free-running carrier-envelope beat note. Our analysis indicates a correlation between amplitude and frequency fluctuations at low Fourier frequencies for essentially all lasers investigated...
March 15, 2017: Optics Letters
https://www.readbyqxmd.com/read/28295083/ellipticity-tunable-attosecond-xuv-pulse-generation-with-a-rotating-bichromatic-circularly-polarized-laser-field
#14
Xiaofan Zhang, Xiaosong Zhu, Xi Liu, Dian Wang, Qingbin Zhang, Pengfei Lan, Peixiang Lu
We propose and theoretically demonstrate a method to generate attosecond XUV pulses with tunable ellipticity from aligned molecules irradiated by a bichromatic counterrotating circularly polarized (BCCP) driving laser field. By rotating the BCCP field, the attoseond XUV pulse varies from being left elliptically polarized to right elliptically polarized. The rotation of the BCCP field can be easily achieved by adjusting the relative phases between the two circularly polarized components. This scheme will benefit a broad range of applications, including the exploration of chiral-sensitive properties of the light-matter interaction and time-resolved imaging of magnetic structures...
March 15, 2017: Optics Letters
https://www.readbyqxmd.com/read/28295061/harmonic-generation-in-solids-with-direct-fiber-laser-pumping
#15
Kevin F Lee, Xiaoyan Ding, T J Hammond, M E Fermann, G Vampa, P B Corkum
High harmonic generation in solids presents the possibility for bringing attosecond techniques to semiconductors and a simple source for frequency comb spectroscopy in the vacuum ultraviolet. We generate up to the seventh harmonic of a Tm fiber laser by focusing in silicon or zinc oxide. The harmonics are strong and stable, with no indication of material damage. Calculations show the potential for generating nineteenth harmonic photons at 12 eV photons of energy.
March 15, 2017: Optics Letters
https://www.readbyqxmd.com/read/28282194/electron-dynamics-upon-ionization-of-polyatomic-molecules-coupling-to-quantum-nuclear-motion-and-decoherence
#16
Morgane Vacher, Michael J Bearpark, Michael A Robb, João Pedro Malhado
Knowledge about the electronic motion in molecules is essential for our understanding of chemical reactions and biological processes. The advent of attosecond techniques opens up the possibility to induce electronic motion, observe it in real time, and potentially steer it. A fundamental question remains the factors influencing electronic decoherence and the role played by nuclear motion in this process. Here, we simulate the dynamics upon ionization of the polyatomic molecules paraxylene and modified bismethylene-adamantane, with a quantum mechanical treatment of both electron and nuclear dynamics using the direct dynamics variational multiconfigurational Gaussian method...
February 24, 2017: Physical Review Letters
https://www.readbyqxmd.com/read/28281655/extreme-ultraviolet-fractional-orbital-angular-momentum-beams-from-high-harmonic-generation
#17
Alex Turpin, Laura Rego, Antonio Picón, Julio San Román, Carlos Hernández-García
We investigate theoretically the generation of extreme-ultraviolet (EUV) beams carrying fractional orbital angular momentum. To this end, we drive high-order harmonic generation with infrared conical refraction (CR) beams. We show that the high-order harmonic beams emitted in the EUV/soft x-ray regime preserve the characteristic signatures of the driving beam, namely ringlike transverse intensity profile and CR-like polarization distribution. As a result, through orbital and spin angular momentum conservation, harmonic beams are emitted with fractional orbital angular momentum, and they can be synthesized into structured attosecond helical beams -or "structured attosecond light springs"- with rotating linear polarization along the azimuth...
March 10, 2017: Scientific Reports
https://www.readbyqxmd.com/read/28241577/gouy-phase-shift-for-annular-beam-profiles-in-attosecond-experiments
#18
F Schlaepfer, A Ludwig, M Lucchini, L Kasmi, M Volkov, L Gallmann, U Keller
Attosecond pump-probe measurements are typically performed by combining attosecond pulses with more intense femtosecond, phase-locked infrared (IR) pulses because of the low average photon flux of attosecond light sources based on high-harmonic generation (HHG). Furthermore, the strong absorption of materials at the extreme ultraviolet (XUV) wavelengths of the attosecond pulses typically prevents the use of transmissive optics. As a result, pump and probe beams are typically recombined geometrically with a center-hole mirror that reflects the larger IR beam and transmits the smaller XUV, which leads to an annular beam profile of the IR...
February 20, 2017: Optics Express
https://www.readbyqxmd.com/read/28241522/high-dynamic-range-arrival-time-control-for-flexible-accurate-and-precise-parametric-sub-cycle-waveform-synthesis
#19
Roland E Mainz, Giulio Maria Rossi, Giovanni Cirmi, Yudong Yang, Oliver D Mücke, Franz X Kärtner
We introduce a simple all-inline variation of a balanced optical cross-correlator (BOC) that allows to measure the arrival time difference (ATD), over the full Nyquist bandwidth, with increased common-mode rejection and long-term stability. An FPGA-based signal processing unit allows for real-time signal normalization and enables locking to any setpoint with an unprecedented accuracy of 0.07 % within an increased ATD range of more than 400 fs, resulting in attosecond resolution locking. The setup precision is verified with an out-of-loop measurement to be less than 80 as residual jitter paving the way for highly demanding applications such as parametric waveform synthesizers...
February 20, 2017: Optics Express
https://www.readbyqxmd.com/read/28240892/potential-energy-surfaces-of-core-hole-and-shake-up-states-for-dissociative-ionization-studies
#20
Inés Corral, Jesús González-Vázquez, Fernando Martín
The theoretical description of core-hole and core-hole excited (shake-up) states resulting from the interaction of a molecule with X-ray free-electron lasers, attosecond pulses, and synchrotron radiation is a challenging task, as these states lie in the ionization continuum and, therefore, are subject to variational collapse. Although much effort has been devoted in the past to describe core-hole states in the Franck-Condon (FC) region, very few attempts, even less for shake-up states, have been reported near the dissociation threshold, where multistate degeneracy introduces additional complications...
March 15, 2017: Journal of Chemical Theory and Computation
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