Nikolay Golubev

Nikolay Golubev
The University of Arizona | UA · Department of Physics

PhD

About

37
Publications
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636
Citations

Publications

Publications (37)
Article
Full-text available
Advances in attosecond spectroscopy have enabled tracing and controlling the electron motion dynamics in matter, although they have yielded insufficient information about the electron dynamic in the space domain. Hence, ultrafast electron and x-ray imaging tools have been developed to image the ultrafast dynamics of matter in real time and space. T...
Preprint
Full-text available
In the last decade, advancements in attosecond spectroscopy have allowed us to study electron motion dynamics in condensed matter. The access to these electron dynamics and, consequently, its control by an ultrafast light field paves the way for establishing ultrafast optoelectronics. Here, we report the generation of light-induced quantum tunnelli...
Preprint
Full-text available
Visualizing the electron dynamics in four dimensions of space and time is crucial to the understanding of several ubiquitous processes in nature. Hence, ultrafast X-ray and electron imaging tools have been developed to probe the dynamics of matter by means of the time-resolved diffraction imaging (TRDI). In this work, we report an extension of the...
Preprint
Full-text available
The electron motion in atoms and molecules is at the heart of all phenomena in nature that occur outside the nucleus. Recently, ultrafast electron and X-ray imaging tools have been developed to image the ultrafast dynamics of matter in real time and space. The cutting-edge temporal resolution of these imaging tools is on the order of a few tens to...
Article
Full-text available
Under certain conditions, the ionization of a molecule may create a superposition of electronic states, leading to ultrafast electron dynamics. If controlled, this motion could be used in attochemistry applications, but it has been shown that the decoherence induced by the nuclear motion typically happens in just a few femtoseconds. We recently dev...
Preprint
Under certain conditions, the ionization of a molecule may create a superposition of electronic states, leading to ultrafast electron dynamics. If controlled, this motion could be used in attochemistry applications, but it has been shown that the decoherence induced by the nuclear motion typically happens in just a few femtoseconds. We recently dev...
Article
Full-text available
Attosecond charge migration is a periodic evolution of the charge density at specific sites of a molecule on a timescale defined by the energy intervals between the electronic states involved. Here we report the observation of charge migration in neutral silane (SiH4) in 690 as, its decoherence within 15 fs and its revival after 40–50 fs, using X-r...
Article
Full-text available
Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of fundamental physics behind the electron-nuclear interactions and dynamics, accurate numerical simulations of light-indu...
Preprint
Full-text available
Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of fundamental physics behind the electron-nuclear interactions and dynamics, accurate numerical simulations of light-indu...
Article
Full-text available
Using a combination of high-level ab initio electronic structure methods with efficient on-the-fly semiclassical evaluation of nuclear dynamics, we performed a massive scan of small polyatomic molecules searching for a long-lasting oscillatory dynamics of the electron density triggered by the outer-valence ionization. We observed that in most of th...
Preprint
Full-text available
Using a combination of high-level ab initio electronic structure methods with efficient on-the-fly semiclassical evaluation of nuclear dynamics, we performed a massive scan of small polyatomic molecules searching for a long lasting oscillatory dynamics of the electron density triggered by the outer-valence ionization. We observed that in most of th...
Preprint
Full-text available
Attosecond charge migration is a periodic evolution of the charge density of a molecule on a time scale defined by the energy intervals between the electronic states involved. Here, we report the observation of charge migration in neutral silane (SiH$_4$) in 690~as, its decoherence within 15~fs, and its revival after 40-50~fs using X-ray attosecond...
Article
Full-text available
Tracing ultrafast processes induced by interaction of light with matter is often very challenging. In molecular systems, the initially created electronic coherence becomes damped by the slow nuclear rearrangement on a femtosecond timescale which makes real-time observations of electron dynamics in molecules particularly difficult. In this work, we...
Conference Paper
The attosecond quantum beat of an electronic state superposition was captured in SiH 4 using soft-X-Ray attosecond transient-absorption spectroscopy. Its decoher-ence and revival, induced by non-adiabatic vibrational dynamics, were reproduced using MCTDH calculations.
Preprint
Full-text available
Tracing ultrafast processes induced by interaction of light with matter is often very challenging. In molecular systems, the initially created electronic coherence becomes damped by the slow nuclear rearrangement on a femtosecond timescale which makes real-time observations of electron dynamics in molecules particularly difficult. In this work, we...
Article
Full-text available
Irradiation of a molecular system by an intense laser field can trigger dynamics of both electronic and nuclear subsystems. The lighter electrons usually move on much faster, attosecond timescale but the slow nuclear rearrangement damps ultrafast electronic oscillations, leading to the decoherence of the electronic dynamics within a few femtosecond...
Conference Paper
Soft-X-ray attosecond transient absorption spectroscopy has been performed on silane (SiH 4 ), capturing dephasing and revival of Rydberg-valence electronic wavepackets with periods of 1.32-1.39 fs. The experimental results are confirmed with fully quantum dynamics simulations.
Preprint
Full-text available
Irradiation of a molecular system by an intense laser field can trigger dynamics of both electronic and nuclear subsystems. Being much lighter than the nuclei, the electrons usually move on much faster time scale that is reflected in the attosecond dynamics of the electron density along a molecular chain. Due to a strong correlation between electro...
Preprint
The hitherto unexplored two-photon doubly-excited states [Ne$^{*}$($2p^{-1}3s$)]$_{2}$ were experimentally identified using the seeded, fully coherent, intense extreme ultraviolet free-electron laser FERMI. These states undergo ultrafast interatomic Coulombic decay (ICD) which predominantly produces singly-ionized dimers. In order to obtain the rat...
Article
Ionization of molecules very often populates several cationic states launching pure electron dynamics that appear as ultrafast migration of the hole charge throughout the system. A crucial question in the emerging field of attochemistry is whether these pure electronic coherences last long enough to allow for their efficient observation and eventua...
Article
Clusters and nanoparticles have been widely investigated to determine how plasmonic near fields influence the strong-field induced energetic electron emission from finite systems. We focus on the contrary, i.e., the slow electrons, and discuss a hitherto unidentified low-energy structure (LES) in the photoemission spectra of rare gas clusters in in...
Article
Full-text available
X-ray free-electron lasers (XFELs) made available a new regime of x-ray intensities, revolutionizing the ultrafast structure determination and laying the foundations of the novel field of nonlinear x-ray optics. Although earlier studies revealed nanoplasma formation when an XFEL pulse interacts with any nanometer-scale matter, the formation process...
Thesis
Full-text available
In recent years, the rapid development of attosecond pulse techniques opened the door for studying and eventually controlling electronic dynamics. Due to strong coupling between the electronic and nuclear motion, control over the pure electronic step offers the extremely interesting possibility to steer the succeeding chemical reactivity by predete...
Article
Full-text available
Observing the crucial first few femtoseconds of photochemical reactions requires tools typically not available in the femtochemistry toolkit. Such dynamics are now within reach with the instruments provided by attosecond science. Here, we apply experimental and theoretical methods to assess the ultrafast nonadiabatic vibronic processes in a prototy...
Article
The hitherto unexplored two-photon doubly excited states [Ne∗(2p-13s)]2 were experimentally identified using the seeded, fully coherent, intense extreme ultraviolet free-electron laser FERMI. These states undergo ultrafast interatomic Coulombic decay (ICD), which predominantly produces singly ionized dimers. In order to obtain the rate of ICD, the...
Article
Using direct search algorithms for solving the quantum optimization problem, we demonstrate on model systems that with specifically tailored Gaussian-form laser pulses one can achieve a very good control over the dynamics in complicated quantum systems. We show that by manipulating a very limited number of laser-pulse parameters, one is able to con...
Article
Full-text available
In high-intensity laser light, matter can be ionized by direct multiphoton absorption even at photon energies below the ionization threshold. However on tuning the laser to the lowest resonant transition, the system becomes multiply excited, and more efficient, indirect ionization pathways become operative. These mechanisms are known as interatomic...
Conference Paper
A surprisingly dominant contribution of slow electrons is observed following NIR strong-field ionization of clusters. This is consistent with highly efficient intra-Rydberg correlated electronic decay processes, from which the emission of low-energy electrons is expected.
Conference Paper
Full-text available
Due to electronic many-body effects, the ionization of a molecule can trigger ultrafast electron dynamics appearing as a migration of the created hole charge throughout the system. Here we propose a scheme for control of the charge migration dynamics with a single ultrashort laser pulse. We demonstrate by fully ab initio calculations on a molecule...
Article
Due to electronic many-body effects, the ionization of a molecule can trigger ultrafast electron dynamics appearing as a migration of the created hole charge throughout the system. Here we propose a scheme for control of the charge migration dynamics with a single ultrashort laser pulse. We demonstrate by fully ab initio calculations on a molecule...
Article
We present a simple approach allowing to obtain analytical expressions for laser pulses that can drive a two-level system in an arbitrarily chosen way. The proposed scheme relates every desired population-evolution path to a single resonant laser pulse. It allows to drive the system from any initial superposition of the two states to a final state...
Article
Full-text available
The treatment of dispersion interactions is ubiquitous but computationally demanding for seamless ab initio approaches. A highly popular and simple remedy consists in correcting for the missing interactions a posteriori by adding an attractive energy term summed over all atom pairs to standard density functional approximations. These corrections we...
Article
Formation of the SiP radical through radiative association of Si((3)P) and P((4)S) atoms is studied using classical and quantum dynamics. Rate coefficients for formation in the two lowest doublet states and the two lowest quartet states are calculated for T = 10-20 000 K. Breit-Wigner theory is used to properly account for contribution from quantum...

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