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Olga Smirnova

Publications and source records attributed to Olga Smirnova.

At least 55 records · Page 3Linked to original sources

Disentangling enantiosensitivity from dichroism using bichromatic fields

We discuss how tensorial observables, available in photoelectron angular distributions resulting from interaction between isotropic chiral samples and cross polarized $ω$-$2ω$ bichromatic fields, allow for chiral discrimination without chiral light and within the electric-dipole approximation. We extend the concept of chiral setup [Phys. Rev. A 98, 063428 (2018)], which explains how chiral discrimination can be achieved in the absence of chiral light, to the case of tensorial observables. We derive selection rules for the enantiosensitivity and dichroism of the $b_{l,m}$ coefficients describing the photoelectron angular distribution valid for both weak and strong fields and for arbitrary $ω$-$2ω$ relative phase. Explicit expressions for simple perturbative cases are given. We find that, besides the dichroic non-enantiosensitive [J. Chem. Phys. 151 074106 (2019)], and dichroic-and-enantiosensitive $b_{l,m}$ coefficients found recently [Phys. Rev. A 99, 063406 (2019)], there are also enantiosensitive non-dichroic $b_{l,m}$ coefficients. These reveal the molecular enantiomer independently of the relative phase between the two colors and are therefore observable even in the absence of stabilization of the $ω$-$2ω$ relative phase.

physics.atom-ph↗

Inducing enantiosensitive permanent multipoles in isotropic samples with two-color fields

We find that two-color fields can induce field-free permanent dipoles in initially isotropic samples of chiral molecules via resonant electronic excitation in a one-$3ω$-photon vs. three-$ω$-photons scheme. These permanent dipoles are enantiosensitive and can be controlled via the relative phase between the two colors. When the two colors are linearly polarized perpendicular to each other, the interference between the two pathways induces excitation sensitive to the molecular handedness and orientation, leading to uniaxial orientation of the excited molecules and to an enantio-sensitive permanent dipole perpendicular to the polarization plane. We also find that although a corresponding one-$2ω$-photon vs. two-$ω$-photons scheme cannot produce enantiosensitive permanent dipoles, it can produce enantiosensitive permanent quadrupoles that are also controllable through the two-color relative phase.

physics.atom-ph↗

Sub-cycle valleytronics: control of valley polarization using few-cycle linearly polarized pulses

So far, selective excitation of a desired valley in the Brillouin zone of a hexagonal two-dimensional material has relied on using circularly polarized fields. We theoretically demonstrate a way to induce, control, and read valley polarization in hexagonal 2D materials on a few-femtosecond timescale using a few-cycle, linearly polarized pulse with controlled carrier-envelope phase. The valley pseudospin is encoded in the helicity of the emitted high harmonics of the driving pulse, allowing one to avoid additional probe pulses and permitting one to induce, manipulate and read the valley pseudospin all-optically, in one step. High circularity of the harmonic emission offers a method to generate highly elliptic attosecond pulses with a linearly polarized driver, in an all-solid-state setup.

physics.optics↗

Polarization of chirality

It has been long recognized that the spatial polarization of the electronic clouds in molecules, and the spatial arrangements of atoms into chiral molecular structures, play crucial roles in physics, chemistry and biology. However, these two fundamental concepts - chirality and polarization - have remained unrelated so far. This work connects them by introducing and exploring the concept of polarization of chirality. We show that, like charge, chirality, or handedness, can be polarized, and that such polarization leads to fundamental consequences, demonstrated here using light. First, we analyze how chirality dipoles and higher-order chirality multipoles manifest in experimental observables. Next, we show how to create chirality-polarized optical fields of alternating handedness in space. Despite being achiral, these racemic space-time light structures interact differently with chiral matter of opposite handedness, and the chirality dipole of light controls and quantifies the strength of the enantio-sensitive response. Using nonlinear interactions, we can make a medium of randomly oriented chiral molecules emit light to the left, or to the right, depending on the molecular handedness and on the chirality dipole of light. The chiral dichroism in emission direction reaches its highest possible value of 200%. Our work opens the field of chirality polarization shaping of light and new opportunities for efficient chiral discrimination and control of chiral and chirality-polarized light and matter on ultrafast time scales.

physics.optics↗

N$_2^+$ Lasing: Gain and Absorption in the Presence of Rotational Coherence

We simulate the pump-probe experiments of lasing in molecular nitrogen ions with particular interest on the effects of rotational wave-packet dynamics. Our computations demonstrate that the coherent preparation of rotational wave packets in N$_2^+$ by an intense short non-resonant pulse results in a modulation of the subsequent emission from $B^2Σ_u^+ \rightarrow X^2Σ_g^+$ transitions induced by a resonant seed pulse. We model the dynamics of such pumping and emission using density matrix theory to describe the N$_2^+$ dynamics and the Maxwell wave equation to model the seed pulse propagation. We show that the gain and absorption of a delayed seed pulse is dependent on the pump-seed delay, that is, the rotational coherences excited by the pump pulse can modulate the gain and absorption of the delayed seed pulse. Further, we demonstrate that the coherent rotational dynamics of the nitrogen ions can cause lasing without electronic inversion.

physics.optics↗

Rotational Quantum Beat Lasing Without Inversion

In standard lasers, light amplification requires population inversion between an upper and a lower state to break the reciprocity between absorption and stimulated emission. However, in a medium prepared in a specific superposition state, quantum interference may fully suppress absorption while leaving stimulated emission intact, opening the possibility of lasing without inversion. Here we show that lasing without inversion arises naturally during propagation of intense femtosecond laser pulses in air. It is triggered by the combination of molecular ionization and molecular alignment, both unavoidable in intense light fields. The effect could enable inversionless amplification of broadband radiation in many molecular gases, opening unusual opportunities for remote sensing.

physics.optics↗

Propensity rules in photoelectron circular dichroism in chiral molecules I: Chiral hydrogen

Photoelectron circular dichroism results from one-photon ionization of chiral molecules by circularly polarized light and manifests itself in forward-backward asymmetry of electron emission in the direction orthogonal to the light polarization plane. What is the physical mechanism underlying asymmetric electron ejection? How "which way" information builds up in a chiral molecule and maps into forward-backward asymmetry? We introduce instances of bound chiral wave functions resulting from stationary superpositions of states in a hydrogen atom and use them to show that the chiral response in one-photon ionization of aligned molecular ensembles originates from two propensity rules: (i) Sensitivity of ionization to the sense of electron rotation in the polarization plane. (ii) Sensitivity of ionization to the direction of charge displacement or stationary current orthogonal to the polarization plane. In the companion paper we show how the ideas presented here are part of a broader picture valid for all chiral molecules and arbitrary degrees of molecular alignment.

physics.atom-ph↗

Propensity rules in photoelectron circular dichroism in chiral molecules II: General picture

Photoelectron circular dichroism results from one-photon ionization of chiral molecules by circularly polarized light and manifests itself in forward-backward asymmetry of electron emission in the direction orthogonal to the light polarization plane. To expose the physical mechanism responsible for asymmetric electron ejection, we first establish a rigorous relation between the responses of unaligned and partially or perfectly aligned molecules. Next, we identify a propensity field, which is responsible for the chiral response in the electric-dipole approximation, i.e. a chiral response without magnetic interactions. We find that this propensity field, up to notations, is equivalent to the Berry curvature in a two-band solid. The propensity field directly encodes optical propensity rules, extending our conclusions regarding the role of propensity rules in defining the sign of forward-backward asymmetry from the specific case of chiral hydrogen to generic chiral systems. Optical propensity rules underlie the chiral response in photoelectron circular dichroism. The enantiosensitive flux of the propensity field through the sphere in momentum space determines the forward-backward asymmetry in unaligned molecules and suggests a geometrical origin of the chiral response. This flux has opposite sign for opposite enantiomers and vanishes for achiral molecules.

physics.atom-ph↗

Locally and globally chiral fields for ultimate control of chiral light matter interaction

Light is one of the most powerful and precise tools allowing us to control, shape and create new phases of matter. In this task, the magnetic component of a light wave has so far played a unique role in defining the wave's helicity, but its influence on the optical response of matter is weak. Chiral molecules offer a typical example where the weakness of magnetic interactions hampers our ability to control the strength of their chiral optical response. It is limited several orders of magnitude below the full potential. Here we introduce freely propagating locally and globally chiral electric fields, which interact with chiral quantum systems extremely efficiently. To demonstrate the degree of control enabled by such fields, we focus on the nonlinear optical response of randomly oriented chiral molecules. We show full control over intensity, polarization and propagation direction of the chiral optical response, enabling its background-free detection. This response can be fully suppressed or enhanced at will depending on the molecular handedness, achieving the ultimate limit in chiral discrimination. Our findings open a way to extremely efficient control of chiral matter and to ultrafast imaging of chiral structure and dynamics in gases, liquids and solids.

physics.optics↗

Multi-Band Petahertz Currents Resolved via High Harmonic Generation Spectroscopy

Strong field driven electric currents in condensed matter systems open new frontiers in petahertz electronics. In this regime new challenges arise as the role of the band structure and the quantum nature of electron-hole dynamics have yet to be resolved. Here we reveal the underlying attosecond dynamics that dictates the temporal evolution of carriers in multi-band solid state systems, via high harmonic generation (HHG) spectroscopy. We demonstrate that when the electron-hole relative velocity approaches zero, enhanced quantum interference leads to the appearance of spectral caustics in the HHG spectrum. Introducing the role of the dynamical joint density of states (JDOS) we identify its direct mapping into the spectrum, exhibiting singularities at the spectral caustics. By probing these singularities, we visualize the structure of multiple unpopulated high conduction bands. Our results open a new path in the control and study of attosecond quasi-particle interactions within the field dressed band structure of crystals.

physics.optics↗

Generalized perspective on chiral measurements without magnetic interactions

We present a unified description of several methods of chiral discrimination based exclusively on electric-dipole interactions. It includes photoelectron circular dichroism (PECD), enantio-sensitive microwave spectroscopy (EMWS), photoexcitation circular dichroism (PXCD), and photoelectron-photoexcitation circular dichroism (PXECD). We show that, in spite of the fact that the physics underlying the appearance of a chiral response is very different in all these methods, the enantio-sensitive and dichroic observable in all cases has a unique form. It is a polar vector given by the product of (i) a molecular pseudoscalar and (ii) a field pseudovector specified by the configuration of the electric fields interacting with the isotropic ensemble of chiral molecules. The molecular pseudoscalar is a rotationally invariant property, which is composed from different molecule-specific vectors and in the simplest case is a triple product of such vectors. The key property that enables the chiral response is the non-coplanarity of the vectors forming such triple product. The key property that enables chiral detection without relying on the chirality of the electromagnetic fields is the vectorial nature of the enantio-sensitive observable. Our compact and general expression for this observable shows what ultimately determines the efficiency of the chiral signal and if, or when, it can reach 100%. We also discuss the differences between the two phenomena, which rely on the bound states, PXCD and EMWS, and the two phenomena using the continuum states, PECD and PXECD. Finally, we extend these methods to arbitrary polarizations of the electric fields used to induce and probe the chiral response.

physics.atom-ph↗

Amplification of intense light fields by nearly free electrons

Light can be used to modify and control properties of media, as in the case of electromagnetically induced transparency or, more recently, for the generation of slow light or bright coherent XUV and X-ray radiation. Particularly unusual states of matter can be created by light fields with strengths comparable to the Coulomb field that binds valence electrons in atoms, leading to nearly-free electrons oscillating in the laser field and yet still loosely bound to the core [1,2]. These are known as Kramers-Henneberger states [3], a specific example of laser-dressed states [2]. Here, we demonstrate that these states arise not only in isolated atoms [4,5], but also in rare gases, at and above atmospheric pressure, where they can act as a gain medium during laser filamentation. Using shaped laser pulses, gain in these states is achieved within just a few cycles of the guided field. The corresponding lasing emission is a signature of population inversion in these states and of their stability against ionization. Our work demonstrates that these unusual states of neutral atoms can be exploited to create a general ultrafast gain mechanism during laser filamentation.

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↗

Strong-field control and enhancement of chiral response in bi-elliptical high-order harmonic generation: an analytical model

The generation of high-order harmonics in a medium of chiral molecules driven by intense bi-elliptical laser fields can lead to strong chiroptical response in a broad range of harmonic numbers and ellipticities [D. Ayuso et al, J. Phys. B 51, 06LT01 (2018)]. Here we present a comprehensive analytical model that can describe the most relevant features arising in the high-order harmonic spectra of chiral molecules driven by strong bi-elliptical fields. Our model recovers the physical picture underlying chiral high-order harmonic generation based on ultrafast chiral hole motion and identifies the rotationally invariant molecular pseudoscalars responsible for chiral dynamics. Using the chiral molecule propylene oxide as an example, we show that one can control and enhance the chiral response in bi-elliptical high-order harmonic generation by tailoring the driving field, in particular by tuning its frequency, intensity and ellipticity, exploiting a suppression mechanism of achiral background based on the linear Stark effect.

physics.optics↗

General theory of photoexcitation induced photoelectron circular dichroism

The photoionization of chiral molecules prepared in a coherent superposition of excited states can give access to the underlying chiral coherent dynamics in a procedure known as photoexcitation induced photoelectron circular dichroism (PXECD). This exclusive dependence on coherence can also be seen in a different part of the angular spectrum, where it is not contingent on the chirality of the molecule, thus allowing extension of PXECD's sensitivity to tracking coherence to non-chiral molecules. Here we present a general theory of PXECD based on angular momentum algebra and derive explicit expressions for all pertinent asymmetry parameters which arise for arbitrary polarisation of pump and probe pulses. The theory is developed in a way that clearly and simply separates chiral and non-chiral contributions to the photoelectron angular distribution, and also demonstrates how PXECD and PECD-type contributions, which may be distinguished by whether pump or ionizing probe enables chiral response, are mixed when arbitrary polarization is used.

physics.atm-clus↗

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↗

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↗