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Olga Smirnova

Publications and source records attributed to Olga Smirnova.

At least 37 records · Page 2Linked to original sources
arXiv2023

Opportunities for Gas-Phase Science at Short-Wavelength Free-Electron Lasers with Undulator-Based Polarization Control

Free-electron lasers (FELs) are the world's most brilliant light sources with rapidly evolving technological capabilities in terms of ultrabright and ultrashort pulses over a large range of accessible photon energies. Their revolutionary and innovative developments have opened new fields of science regarding nonlinear light-matter interaction, the investigation of ultrafast processes from specific observer sites, and approaches to imaging matter with atomic resolution. A core aspect of FEL science is the study of isolated and prototypical systems in the gas phase with the possibility of addressing well-defined electronic transitions or particular atomic sites in molecules. Notably for polarization-controlled short-wavelength FELs, the gas phase offers new avenues for investigations of nonlinear and ultrafast phenomena in spin orientated systems, for decoding the function of the chiral building blocks of life as well as steering reactions and particle emission dynamics in otherwise inaccessible ways. This roadmap comprises descriptions of technological capabilities of facilities worldwide, innovative diagnostics and instrumentation, as well as recent scientific highlights, novel methodology and mathematical modeling. The experimental and theoretical landscape of using polarization controllable FELs for dichroic light-matter interaction in the gas phase will be discussed and comprehensively outlined to stimulate and strengthen global collaborative efforts of all disciplines.

physics.atom-ph↗
arXiv2023

Control of Spin Polarization through Recollisions

Using only linearly polarized light, we study the possibility of generating spin-polarized photoelectrons from xenon atoms. No net spin polarization is possible, since the xenon ground state is spin-less, but when the photoelectron are measured in coincidence with the residual ion, spin polarization emerges. Furthermore, we show that ultrafast dynamics of the recolliding photoelectrons contribute to an apparent flipping of the spin of the photoelectron, a process that has been completely neglected so far in all analyses of recollision-based processes. We link this phenomenon to the ``spin--orbit clock'' of the remaining ion. These effects arise already in dipole approximation.

physics.atom-ph↗
arXiv2023

Observation of light driven band structure via multi-band high harmonic spectroscopy

Intense light-matter interactions have revolutionized our ability to probe and manipulate quantum systems at sub-femtosecond time scales, opening routes to all-optical control of electronic currents in solids at petahertz rates. Such control typically requires electric field amplitudes $\sim V/Å$, when the voltage drop across a lattice site becomes comparable to the characteristic band gap energies. In this regime, intense light-matter interaction induces significant modifications of electronic and optical properties, dramatically modifying the crystal band structure. Yet, identifying and characterizing such modifications remains an outstanding problem. As the oscillating electric field changes within the driving field's cycle, does the band-structure follow, and how can it be defined? Here we address this fundamental question, proposing all-optical spectroscopy to probe laser-induced closing of the band-gap between adjacent conduction bands. Our work reveals the link between nonlinear light matter interactions in strongly driven crystals and the sub-cycle modifications in their effective band structure.

physics.optics↗
arXiv2023

Role of Spin-Orbit Coupling in High-order Harmonic Generation Revealed by Super-Cycle Rydberg Trajectories

High-harmonic generation is typically thought of as a sub-laser-cycle process, with the electron's excursion in the continuum lasting a fraction of the optical cycle. However, it was recently suggested that long-lived Rydberg states can play a particularly important role in atoms driven by the combination of the counter-rotating circularly polarized fundamental light field and its second harmonic. Here we report direct experimental evidence of long and stable Rydberg trajectories contributing to high-harmonic generation. We confirm their effect on the harmonic emission via Time-Dependent Schr{ö}dinger Equation simulations and track their dynamics inside the laser pulse using the spin-orbit evolution in the ionic core, utilizing the spin-orbit Larmor clock. Our observations contrast sharply with the general view that long-lived Rydberg orbits should generate negligible contribution to the macroscopic far-field high harmonic response of the medium. Indeed, we show how and why radiation from such states can lead to well collimated macroscopic signal in the far field.

physics.atom-ph↗
arXiv2023

Enantiosensitive exceptional points

We show that the position of the exceptional points (EPs) in the parameter space of a chiral molecule coupled to the photoionization continuum by a three-color field is enantiosensitive. Using a minimal model of a three-level system driven by a three-color field to form a cyclic loop transition, we investigate the enantiosensitivity of the EPs with respect to the system parameters and exploit the asymmetric switch mechanism associated with the encirclement of an EP in parameter space in an enantio-selective way. Our work paves the way for future applications of enantiosensitive EPs in chiral systems.

quant-ph↗
arXiv2023

Ultrafast control over chiral sum-frequency generation

We introduce an ultrafast all-optical approach for efficient chiral recognition which relies on the interference between two low-order nonlinear processes which are ubiquitous in nonlinear optics: sum-frequency generation and third-harmonic generation. In contrast to traditional sum-frequency generation, our approach encodes the medium's handedness in the intensity of the emitted harmonic signal, rather than in its phase, and it enables full control over the enantiosensitive response. We show how, by sculpting the sub-optical-cycle oscillations of the driving laser field, we can force one molecular enantiomer to emit bright light while its mirror twin remains dark, thus reaching the ultimate efficiency limit of chiral sensitivity via low-order nonlinear light-matter interactions. Our work paves the way for ultrafast and highly efficient imaging and control of the chiral electronic clouds of chiral molecules using lasers with moderate intensities, in all states of matter: from gases to liquids to solids, with molecular specificity and on ultrafast timescales.

physics.optics↗
arXiv2023

Valleytronics in bulk MoS$_2$ by optical control of parity and time symmetries

The valley degree of freedom of electrons in materials promises routes toward energy-efficient information storage with enticing prospects towards quantum information processing. Current challenges in utilizing valley polarization are symmetry conditions that require monolayer structures or specific material engineering, non-resonant optical control to avoid energy dissipation, and the ability to switch valley polarization at optical speed. We demonstrate all-optical and non-resonant control over valley polarization using bulk MoS$_2$, a centrosymmetric material with zero Berry curvature at the valleys. Our universal method utilizes spin-angular momentum-shaped tri-foil optical control pulses to switch the material's electronic topology to induce valley polarization by transiently breaking time and space inversion symmetry through a simple phase rotation. The dependence of the generation of the second harmonic of an optical probe pulse on the phase rotation directly demonstrates the efficacy of valley polarization. It shows that direct optical control over the valley degree of freedom is not limited to monolayer structures. Instead, it is possible for systems with an arbitrary number of layers and bulk materials. Universal and non-resonant valley control at optical speeds unlocks the possibility of engineering efficient, multi-material valleytronic devices operating on quantum coherent timescales.

cond-mat.mtrl-sci↗
arXiv2022

Imprinting chirality on atoms using synthetic chiral light fields

Atoms are usually thought of as achiral objects. However, one can construct superpositions of atomic states that are chiral [1]. Here we show how to excite such superpositions with tailored light fields both in the weak-field and strong-field regimes, using realistic laser parameters. First, we use time-dependent Schrodinger equation (TDSE) simulations to demonstrate the creation of a time-dependent bound chiral wavepacket in sodium atoms. Second, we show how the time-dependent handedness of this wavepacket can be probed by photoelectron circular dichroism, in spite of the central symmetry of the core potential. Third, we use TDSE simulations to show how chirality can be directly imprinted on a photoelectron wavepacket created by strong-field ionization and introduce an unambigous chiral measure that allows us to characterize its handedness.

physics.atom-ph↗
arXiv2022

Highly spin-polarized multi-GeV electron beams generated by single-species plasma photocathodes

High-gradient and high-efficiency acceleration in plasma-based accelerators has been demonstrated, showing its potential as the building block for a future collider operating at the energy frontier of particle physics. However, generating and accelerating the required spin-polarized beams in such a collider using plasma-based accelerators has been a long-standing challenge. Here we show that the passage of a highly relativistic, high-current electron beam through a single-species (ytterbium) vapor excites a nonlinear plasma wake by primarily ionizing the two outer 6s electrons. Further photoionization of the resultant Yb2+ ions by a circularly polarized laser injects the 4f14 electrons into this wake generating a highly spin-polarized beam. Combining time-dependent Schrodinger equation simulations with particle-in-cell simulations, we show that a sub-femtosecond, high-current (4 kA) electron beam with up to 56% net spin polarization can be generated and accelerated to 15 GeV in just 41 cm. This relatively simple scheme solves the perplexing problem of producing spin-polarized relativistic electrons in plasma-based accelerators.

physics.plasm-ph↗
arXiv2022

Ultrafast chirality: the road to efficient chiral measurements

Today we are witnessing the electric-dipole revolution in chiral measurements. Here we reflect on its lessons and outcomes, such as the perspective on chiral measurements using the complementary principles of "chiral reagent" and "chiral observer", the hierarchy of scalar, vectorial and tensorial observables, the new properties of the chiro-optical response in the ultrafast and non-linear domains, and the geometrical magnetism associated with the chiral response in photoionization. The electric-dipole revolution is a landmark event. It has opened routes to extremely efficient enantio-discrimination with a family of new methods. These methods are governed by the same principles but work in vastly different regimes -- from microwaves to optical light; they address all molecular degrees of freedom -- electronic, vibrational and rotational, and use flexible detection schemes, i.e. detecting photons or electrons, making them applicable to different chiral phases, from gases to liquids to amorphous solids. The electric-dipole revolution has also enabled enantio-sensitive manipulation of chiral molecules with light. This manipulation includes exciting and controlling ultrafast helical currents in vibronic states of chiral molecules, enantio-sensitive control of populations in electronic, vibronic and rotational molecular states, and opens the way to efficient enantio-separation and enantio-sensitive trapping of chiral molecules. The word "perspective" has two meanings: "outlook" and "point of view". In this perspective article, we have tried to cover both meanings.

physics.optics↗
arXiv2021

In Situ Generation of High-Energy Spin-Polarized Electrons in a Beam-Driven Plasma Wakefield Accelerator

In situ generation of a high-energy, high-current, spin-polarized electron beam is an outstanding scientific challenge to the development of plasma-based accelerators for high-energy colliders. In this Letter we show how such a spin-polarized relativistic beam can be produced by ionization injection of electrons of certain atoms with a circularly polarized laser field into a beam-driven plasma wakefield accelerator, providing a much desired one-step solution to this challenge. Using time-dependent Schrödinger equation (TDSE) simulations, we show the propensity rule of spin-dependent ionization of xenon atoms can be reversed in the strong-field multi-photon regime compared with the non-adiabatic tunneling regime, leading to high total spin-polarization. Furthermore, three-dimensional particle-in-cell (PIC) simulations are incorporated with TDSE simulations, providing start-to-end simulations of spin-dependent strong-field ionization of xenon atoms and subsequent trapping, acceleration, and preservation of electron spin-polarization in lithium plasma. We show the generation of a high-current (0.8 kA), ultra-low-normalized-emittance (~37 nm), and high-energy (2.7 GeV) electron beam within just 11 cm distance, with up to ~31% net spin polarization. Higher current, energy, and net spin-polarization beams are possible by optimizing this concept, thus solving a long-standing problem facing the development of plasma accelerators.

physics.plasm-ph↗
arXiv2021

Geometric fields and new enantio-sensitive observables in photoionization of chiral molecules

Chiral molecules are instrumental for molecular recognition in living organisms. Distinguishing between two opposite enantiomers, the mirror twins of the same chiral molecule, is both vital and challenging. Photoelectron circular dichroism (PECD), an extremely sensitive probe of molecular chirality via photoionization, outperforms standard optical methods by many orders of magnitude. Here we show that the physical origin of PECD in chiral molecules is linked to the concept of geometric magnetism, which enables a broad class of phenomena in solids including the anomalous electron velocity, the Hall effect, and related topological phenomena. We uncover the geometric field in molecular photoionization, which leads to a new class of enantio-sensitive observables emerging due to ultrafast excitation of chiral electronic or vibronic currents prior to ionization. Next, we introduce the first member of this new class: enantio-sensitive orientation of chiral molecules via photoionization. This effect opens new routes to both enantio-separation and imaging of chiral dynamics on ultrafast time scales. Our work suggests that geometric fields in photoionization provide the bridge between the two geometrical properties, chirality and topology.

physics.chem-ph↗
arXiv2021

Propensity rules for photoelectron circular dichroism in strong field ionization of chiral molecules

Chiral molecules ionized by circularly polarized fields produce a photoelectron current orthogonal to the polarization plane. This current has opposite directions for opposite enantiomers and provides an extremely sensitive probe of molecular handedness. Recently, such photoelectron currents have been measured in the strong-field ionization regime, where they may serve as an ultrafast probe of molecular chirality. Here we provide a mechanism for the emergence of such strong-field photoelectron currents in terms of two propensity rules that link the properties of the initial electronic chiral state to the direction of the photoelectron current.

physics.atom-ph↗
arXiv2021

Giant chiro-optical response in high harmonic generation

High harmonic generation (HHG) records the ultrafast electronic response of matter to light, encoding key properties of the interrogated quantum system, such as chirality. The first implementation of chiral HHG [Cireasa et al. Nat. Phys. 11, 654 (2015)] relied on the weak electronic response of a medium of randomly oriented chiral molecules to the magnetic component of an elliptically polarized wave, yielding relatively weak chiro-optical signals. Here we show that elliptically polarized light can drive a strong chiral response in chiral molecules via purely electric-dipole interactions -- the magnetic component of the wave does not participate at all. This giant chiro-optical response, which remains hidden in standard HHG experiments, can be mapped into the macroscopic far-field signal using a non-collinear configuration, creating new opportunities for bringing the electric-dipole "revolution" to HHG.

physics.optics↗
arXiv2021

Enantiosensitive steering of free-induction decay

Chiral discrimination, a problem of vital importance, has recently become an emerging frontier in ultrafast physics, with remarkable progress achieved in multiphoton and strong-field regimes. Rydberg excitations, unavoidable in the strong-field regime and intentional for few-photon processes, arise in all these approaches. Here we show how to harness this ubiquitous feature by introducing a new phenomenon, enantiosensitive free-induction decay, steered by a tricolour chiral field at a gentle intensity, structured in space and time. We demonstrate theoretically that an excited chiral molecule accumulates an enantiosensitive phase due to perturbative interactions with the tricolour chiral field, resulting in a spatial phase gradient steering the free-induction decay in opposite directions for opposite enantiomers. Our work introduces a general, extremely sensitive, all-optical, enantiosensitive detection technique which avoids strong fields and takes full advantage of recent advances in structuring light.

physics.optics↗
arXiv2020

Ultrafast optical rotation for extremely sensitive enantio-discrimination

Sculpting sub-cycle temporal structures of optical waveforms allows one to image and even control electronic clouds in atoms, molecules and solids. Here we show how the transverse spin component arising upon spatial confinement of such optical waveforms enables extremely efficient chiral recognition and control of ultrafast chiral dynamics. When an intense few-cycle, linearly polarized laser pulse is tightly focused into a medium of randomly oriented chiral molecules, the medium generates light which is elliptically polarized, with opposite helicities and opposite rotations of the polarization ellipse in media of opposite handedness. In contrast to conventional optical activity of chiral media, this new nonlinear optical activity is driven by purely electric-dipole interactions and leads to giant enantio-sensitivity in the near VIS-UV domain, where optical instrumentation is readily available. Adding a polarizer turns rotation of the polarization ellipse into highly enantio-sensitive intensity of the nonlinear-optical response. Sub-cycle optical control of the incident light wave enables full control over the enantio-sensitive response. The proposed all-optical method not only enables extremely efficient chiral discrimination, but also ultrafast imaging and control of chiral dynamics with commercially available optical technology.

physics.optics↗
arXiv2020

On the molecular information revealed by photoelectron angular distributions of isotropic samples

We propose an alternative approach to the description and analysis of photoelectron angular distributions (PADs) resulting from isotropic samples in the case of few-photon absorption via electric fields of arbitrary polarization. As we demonstrate for the one- and two-photon cases, this approach reveals the molecular frame information encoded in the $b_{l,m}$ expansion coefficients of the PAD in a particularly clear way. Our approach does not rely on explicit partial wave expansions of the scattering wave function and the expressions we obtain are therefore interpreted in terms of the vector field structure of the photoionization dipole $\vec{D}(\vec{k})$ as a function of the photoelectron momentum $\vec{k}$. This provides very compact expressions that reveal how molecular rotational invariants couple to the setup (electric field polarization and detectors) rotational invariants. We rely heavily on this approach in a companion paper on tensorial chiral setups. Here we apply this approach to one-photon ionization and find that while $b_{0,0}$ depends only on the magnitude of $\vec{D}(\vec{k})$, $b_{1,0}$ (non-zero for chiral molecules) is sensitive only to the components of $\vec{D}(\vec{k})$ perpendicular to $\vec{k}$ encoded in the propensity field $\vec{B}(\vec{k})\equiv i\vec{D}^{*}(\vec{k})\times\vec{D}(\vec{k})$, and $b_{2,0}$ is sensitive only to the the component of $\vec{D}(\vec{k})$ along $\vec{k}$. We also analyze the resonantly enhanced two-photon case where we show that $b_{0,0}$ and $b_{1,0}$ can be written in terms of an effectively stretched $\vec{D}(\vec{k})$, and that $b_{1,0}$ and $b_{3,0}$ reveal structural information of the field $\vec{B}(\vec{k})$ encoded in three of its vector spherical harmonic expansion coefficients.

physics.atom-ph↗