Searcharxiv⌕ Search

arXiv subjects

Misha Ivanov

Publications and source records attributed to Misha Ivanov.

At least 73 records · Page 4Linked to original sources

Control of helicity of high-harmonic radiation using bichromatic circularly polarized laser fields

High-harmonic generation in two-colour ($ω-2ω$) counter-rotating circularly polarised laser fields opens the path to generate isolated attosecond pulses and attosecond pulse trains with controlled ellipticity. The generated harmonics have alternating helicity, and the ellipticity of the generated attosecond pulse depends sensitively on the relative intensities of two adjacent, counter-rotating harmonic lines. For the $s$-type ground state, such as in Helium, the successive harmonics have nearly equal amplitude, yielding isolated attosecond pulses and attosecond pulse trains with linear polarisation, rotated by 120$^{\circ}$ from pulse to pulse. In this work, we suggest a solution to overcome the limitation associated with the $s$-type ground state. It is based on modifying the three propensity rules associated with the three steps of the harmonic generation process: ionisation, propagation, and recombination. We control the first step by seeding high harmonic generation with XUV light tuned well below the ionisation threshold, which generates virtual excitations with the angular momentum co-rotating with the $ω$-field. We control the propagation step by increasing the intensity of the $ω$-field relative to the $2ω$-field, further enhancing the chance of the $ω$-field being absorbed versus the $2ω$-field, thus favouring the emission co-rotating with the seed and the $ω-$field. We demonstrate our proposed control scheme using Helium atom as a target and solving time-dependent Schr{ö}dinger equation in two and three-dimensions.

physics.optics↗

Electron correlations and pre-collision in the re-collision picture of high harmonic generation

We discuss the seminal three-step model and the recollision picture in the context of high harmonic generation in molecules. In particular, we stress the importance of multi-electron correlation during the first and the third of the three steps of the process: (1) the strong field ionization and (3) the recombination. We point out how accurate account for multi-electron correlations during the third, recombination, step allows one to gauge the importance of pre-collision: the term coined by J. H. Eberly to describe unusual pathways during the first, ionization, step.

physics.atom-ph↗

Control of attosecond light polarization in two-color bi-circular fields

We develop theoretically and confirm both numerically and experimentally a comprehensive analytical model which describes the propensity rules in the emission of circularly polarized high harmonics by systems driven by two-color counter-rotating fields, a fundamental and its second harmonic. We identify and confirm the three propensity rules responsible for the contrast between the 3N+1 and 3N+2 harmonic lines in the HHG spectra of noble gas atoms. We demonstrate how these rules depend on the laser parameters and how they can be used in the experiment to shape the polarization properties of the emitted attosecond pulses.

physics.atom-ph↗

Ultrafast Preparation and Detection of Ring Currents in Single Atoms

Quantum particles can penetrate potential barriers by tunneling (1). If that barrier is rotating, the tunneling process is modified (2,3). This is typical for electrons in atoms, molecules or solids exposed to strong circularly polarized laser pulses (4,5). Here we measure how the transmission probability through a rotating tunnel depends on the sign of the magnetic quantum number m of the electron and thus on the initial sense of rotation of its quantum phase. We further show that the electron keeps part of that rotary motion on its way through the tunnel by measuring m-dependent modification of the electron emission pattern. These findings are relevant for attosecond metrology as well as for interpretation of strong field electron emission from atoms and molecules (6-13) and directly demonstrates the creation of ring currents in bound states of ions with attosecond precision. In solids, this could open a way to inducing and controlling ring-current related topological phenomena (14).

physics.atom-ph↗

Time-resolved high harmonic spectroscopy of dynamical symmetry breaking in bi-circular laser fields

The bi-circular scheme for high harmonic generation, which combines two counter-rotating circular fields with frequency ratio 2:1, has recently permitted to generate high harmonics with essentially circular polarization, opening the way for ultrafast chiral studies. This scheme produces harmonic lines at 3N + 1 and 3N + 2 multiples of the fundamental driving frequency, while the 3N lines are forbidden owing to the three-fold symmetry of the field. It is generally established that the routinely observed signals at these forbidden harmonic lines come from a slight ellipticity in the driving fields, which breaks the three-fold symmetry. We find that this is neither the only nor it is the dominant mechanism responsible. The forbidden lines can be observed even for perfectly circular, long driving pulses. We show that they encode rich information on the sub-cycle electronic dynamics that occur during the generation process. By varying the time delay and relative intensity between the two drivers, we demonstrate that when the second harmonic either precedes or is more intense than the fundamental field, the dynamical symmetry of the system is broken by electrons trapped in Rydberg orbits (i.e., Freeman resonances), and that the forbidden harmonic lines are a witness of this.

physics.optics↗

Electron spin polarization in strong-field ionization of Xenon atoms

As a fundamental property of the electron, the spin plays a decisive role in the electronic structure of matter from solids to molecules and atoms, e.g. causing magnetism. Yet, despite its importance, the spin dynamics of electrons released during the interaction of atoms with strong ultrashort laser pulses has remained unexplored. Here we report on the experimental detection of electron spin polarization by strong-field ionization of Xenon atoms and support our results by theoretical analysis. We found up to 30% spin polarization changing its sign with electron energy. This work opens the new dimension of spin to strong-field physics. It paves the way to production of subfemtosecond spin polarized electron pulses with applications ranging from probing magnetic properties of matter at ultrafast time scales to testing chiral molecular systems with subfemtosecond temporal and sub-Ångström spatial resolution.

physics.atom-ph↗

Attosecond control of spin polarization in electron-ion recollision driven by intense tailored fields

We show that electrons recolliding with the ionic core upon tunnel ionization of noble gas atoms driven by a strong circularly polarized laser field in combination with a counter-rotating second harmonic are spin polarized and that their degree of polarization depends strongly on the recollision time. Spin polarization arises as a consequence of (1) entanglement between the recolliding electron and the ion, and (2) sensitivity of ionization to the sense of electron rotation in the initial state. We demonstrate that one can engineer the degree of spin polarization as a function of time by tuning the relative intensities of the counter-rotating fields, opening the door for attosecond control of spin-resolved dynamics.

physics.atom-ph↗

Interference stabilization of autoionizing states in molecular $N_2$ studied by time- and angular-resolved photoelectron spectroscopy

An autoionizing resonance in molecular N$_2$ is excited by an ultrashort XUV pulse and probed by a subsequent weak IR pulse, which ionizes the contributing Rydberg states. Time- and angular-resolved photoelectron spectra recorded with a velocity map imaging spectrometer reveal two electronic contributions with different angular distributions. One of them has an exponential decay rate of $20\pm5$ fs, while the other one is shorter than 10 fs. This observation is interpreted as a manifestation of interference stabilization involving the two overlapping discrete Rydberg states. A formalism of interference stabilization for molecular ionization is developed and applied to describe the autoionizing resonance. The results of calculations reveal, that the effect of the interference stabilization is facilitated by rotationally-induced couplings of electronic states with different symmetry.

physics.atom-ph↗

High harmonic interferometry of the Lorentz force in strong mid-infrared laser fields

The interaction of intense mid-infrared laser fields with atoms and molecules leads to a range of new opportunities, from the production of bright, coherent radiation in the soft x-ray range to imaging molecular structures and dynamics with attosecond temporal and sub-angstrom spatial resolution. However, all these effects, which rely on laser-driven recollision of an electron removed by the strong laser field and the parent ion, suffer from the rapidly increasing role of the magnetic field component of the driving pulse: the associated Lorentz force pushes the electrons off course in their excursion and suppresses all recollision-based processes, including high harmonic generation, elastic and inelastic scattering. Here we show how the use of two non-collinear beams with opposite circular polarizations produces a forwards ellipticity which can be used to monitor, control, and cancel the effect of the Lorentz force. This arrangement can thus be used to re-enable recollision-based phenomena in regimes beyond the long-wavelength breakdown of the dipole approximation, and it can be used to observe this breakdown in high-harmonic generation using currently-available light sources.

physics.atom-ph↗

XUV lasing during strong-field assisted transient absorption in molecules

Using ab-initio non-Born-Oppenheimer simulations, we demonstrate amplification of XUV radiation in a high-harmonic generation type process using the example of the hydrogen molecular ion. A small fraction of the molecules is pumped to a dissociative Rydberg state from which IR-assisted XUV amplification is observed. We show that starting at sufficiently high IR driving field intensities the ground state molecules become quasi-transparent for XUV radiation, while due to stabilization gain from Rydberg states is maintained, thus leading to lasing from strongly driven Rydberg states. Further increase of the IR intensity even leads to gain by initially unexcited molecules, which are quickly excited by the driving IR pulse.

physics.atom-ph↗

Spin-Orbit Larmor Clock for Ionisation Times in One-Photon and Strong-Field Regimes

Photoionisation is a process where absorption of one or several photons liberates an electron and creates a hole in a quantum system, such as an atom or a molecule. Is it faster to remove an electron using one or many photons, and how to define this time? Here we introduce a clock that allows us to define ionisation time for both one-photon and many-photon ionisation regimes. The clock uses the interaction of the electron or hole spin with the magnetic field created by their orbital motion, known as the spin-orbit interaction. The angle of spin precession in the magnetic field records time. We use the combination of analytical theory and ab-initio calculations to show how ionisation delay depends on the number of absorbed photons, how it appears in the experiment and what electron dynamics it signifies. In particular, we apply our method to calculate the derived time delays in tunnelling regime of strong-field ionisation.

quant-ph↗

Quantum theory of an electromagnetic observer: classically behaving macroscopic systems and emergence of classical world in quantum electrodynamics

Quantum electrodynamics under conditions of distinguishability of interacting matter entities, and of controlled actions and back-actions between them, is considered. Such "mesoscopic quantum electrodynamics" is shown to share its dynamical structure with the classical stochastic electrodynamics. In formal terms, we demonstrate that all general relations of the mesoscopic quantum electrodynamics may be recast in a form lacking Planck's constant. Mesoscopic quantum electrodynamics is therefore subject to "doing quantum electrodynamics while thinking classically," allowing one to substitute essentally classical considerations for quantum ones without any loss in generality. Implications of these results for the quantum measurement theory are discussed.

quant-ph↗

Slalom in complex time: emergence of low-energy structures in tunnel ionization via complex time contours

The ionization of atoms by strong, low-frequency fields can generally be described well by assuming that the photoelectron is, after the ionization step, completely at the mercy of the laser field. However, certain phenomena, like the recent discovery of low-energy structures in the long-wavelength regime, require the inclusion of the Coulomb interaction with the ion once the electron is in the continuum. We explore the first-principles inclusion of this interaction, known as analytical R-matrix theory, and its consequences on the corresponding quantum orbits. We show that the trajectory must have an imaginary component, and that this causes branch cuts in the complex time plane when the real trajectory revisits the neighbourhood of the ionic core. We provide a framework for consistently navigating these branch cuts based on closest-approach times, which satisfy the equation $\mathbf{r}(t) \cdot \mathbf{v}(t) = 0$ in the complex plane. We explore the geometry of these roots and describe the geometrical structures underlying the emergence of LES in both the classical and quantum domains.

quant-ph↗

Attosecond time delay in valence photoionization and photorecombination of argon: a TDLDA study

We determine and analyze the quantum phases and time delays in photoionization and photorecombination of valence 3p and 3s electrons of argon using the Kohn-Sham local density functional approach. The time-dependent local density approximation (TDLDA) is used to account for the electron correlation. Resulting attosecond Wigner-Smith time delays show excellent agreements with two recent independent experiments on argon that measured the relative 3s-3p time delay in photoionization [Physical Review Letters {\bf 106}, 143002 (2011)] and the delay in 3p photorecombination [Physical Review Letters {\bf 112}, 153002 (2014)]

physics.atom-ph↗

Interpreting Attoclock Measurements of Tunnelling Times

Resolving in time the dynamics of light absorption by atoms and molecules, and the electronic rearrangement this induces, is among the most challenging goals of attosecond spectroscopy. The attoclock is an elegant approach to this problem, which encodes ionization times in the strong-field regime. However, the accurate reconstruction of these times from experimental data presents a formidable theoretical challenge. Here, we solve this problem by combining analytical theory with ab-initio numerical simulations. We apply our theory to numerical attoclock experiments on the hydrogen atom to extract ionization time delays and analyse their nature. Strong field ionization is often viewed as optical tunnelling through the barrier created by the field and the core potential. We show that, in the hydrogen atom, optical tunnelling is instantaneous. By calibrating the attoclock using the hydrogen atom, our method opens the way to identify possible delays associated with multielectron dynamics during strong-field ionization.

physics.atom-ph↗

Spin conservation in high-order-harmonic generation using bicircular fields

We present an alternative theoretical model for a recent experiment [A.Fleischer et al., Nature Photon. 8, 543 (2014)] which used bichromatic, counter-rotating high intensity laser pulses to probe the conservation of spin angular momentum in high harmonic generation. We separate elliptical polarizations into independent circular fields with definite angular momentum, instead of using the expectation value of spin for each photon in the conservation equation, and we find good agreement with the experimental results. In our description the generation of each individual harmonic conserves spin angular momentum, in contrast to the model proposed by Fleischer et al. Our model also correctly describes analogous processes in standard perturbative optics.

physics.atom-ph↗

Momentum transfers in correlation-assisted tunnelling

We consider correlation-assisted tunnel ionization of a small molecule by an intense low-frequency laser pulse. In this mechanism, the departing electron excites the state of the ion via a Coulomb interaction. We show that the angular distribution for this process has significant qualitative differences compared to direct tunnelling of an electron from a deeper orbital. These differences could be used to distinguish the two contributions, and give rise to interference effects when the contributions are comparable. The saddle-point approximation is also shown to require special attention in this geometric analysis.

physics.atom-ph↗

X-ray imaging of chemically active valence electrons during a pericyclic reaction

Time-resolved imaging of chemically active valence electron densities is a long sought goal, as these electrons dictate the course of chemical reactions. However, x-ray scattering is always dominated by the core and inert valence electrons, making time-resolved x-ray imaging of chemically active valence electron densities extremely challenging. To image such electron densities, we demonstrate an effective and robust method, which emphasizes the information encoded in weakly scattered photons. The degenerate Cope rearrangement of semibullvalene, a pericyclic reaction, is used as an example to visually illustrate our approach. Our work also provides experimental access to the long-standing problem of synchronous versus asynchronous bond formation and breaking during pericyclic reactions.

physics.chem-ph↗