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Olga Smirnova

Publications and source records attributed to Olga Smirnova.

At least 19 recordsLinked to original sources

Valley polarization driven by two-color circular fields: a rotating frame and strong-field perspective

Valley polarization in hexagonal materials driven by the form of the lightwave and its orientation relative to the lattice, rather than solely by the helicity of the driver, has recently been demonstrated both theoretically and experimentally. This has extended valley control to the non-resonant, sub-cycle regime and to inversion-symmetric materials. One interpretation of this field-orientation-dependent valley polarization is that the laser-dressed, cycle-averaged band structure obtained from a Floquet-type approach is modified so as to lift the degeneracy between the valleys. Here, we derive a complementary explanation based on strong-field tunneling dynamics. We show that the effective valley gap at the dominant injection times depends on the orientation of the field relative to the lattice through the trigonal-warping term of the low-energy dispersion. We derive general expressions for co- and counter-rotating $\omega+N\omega$ fields and show that the leading orientation-dependent contribution survives the cycle average only for field configurations compatible with the threefold lattice symmetry, most notably counter-rotating $\omega+2\omega$ and co-rotating $\omega+4\omega$ fields. As a complementary weak-field result, we show that, for counter-rotating bicircular fields, the one-photon valley selection rules can be represented as valley-dependent energy detunings in a rotating frame where both colors acquire the same frequency.

physics.optics

Roadmap on Attosecond Science

Twenty-five years have passed since the first experimental demonstration of attosecond pulses, marking the advent of our ability to resolve and control electron motion in real time. What began as a technological breakthrough - generating the shortest flashes ever produced - has evolved into a powerful approach for probing and steering electronic dynamics in atoms, molecules, and solids. This roadmap, authored by leading experts in the field, surveys the recent rapid progress in the generation and characterization of attosecond pulses, emerging attosecond measurement and control techniques, and their expanding range of applications. It reviews current and future developments in attosecond light sources, including novel laser technologies, waveform synthesizers, new schemes for high-order harmonic generation, attosecond pulse generation at free-electron lasers, and structured light. Advances in attosecond measurement methodologies are also discussed, encompassing all-attosecond pump-probe spectroscopy, attosecond four-wave mixing, attosecond microscopy, spectroscopy with light transients, and attosecond interferometry. Furthermore, the roadmap addresses applications of attosecond spectroscopy to reveal electron dynamics in molecules and condensed matter systems from both theoretical and experimental perspectives, and highlights emerging directions at the interface with quantum optics and quantum entanglement. Overall, this work aims to serve as a comprehensive resource for navigating the evolving landscape of attosecond science.

physics.optics

Geometric mechanisms enabling spin- and enantio-sensitive observables in one photon ionization of chiral molecules

We examine spin-resolved photoionization of randomly oriented chiral molecules via circularly polarized light, and revisit earlier predictions of Cherepkov (J. Phys. B: Atom. Mol. Phys. 16, 1543, 1983). We will show that the dynamical origin of spin- and enantio-sensitive observables arise from two intrinsic mechanisms that are quantified by two pseudovectors stemming from the geometric properties of the photoionization dipoles in spin space and in real space, and an extrinsic mechanism which is a directional bias introduced by the well-defined direction of light polarization. These mechanisms arise solely from electric dipole interactions. Consequently, this means that the ten independent parameters that was earlier predicted by Cherepkov to fully describe spin-resolved photoionization of chiral molecules can be reduced as moments of these three pseudovectors. We also find that the molecular pseudoscalars describing the spin- and enantio-sensitive components of the yield can be described by the flux of these pseudovectors through the energy shell, which changes sign upon switching enantiomers. Our results provide compact expressions for these observables which provide an intuitive picture on what determines the strength of these spin- and enantio-sensitive observables. The approach can be readily generalized to photoexcitation, multiphoton processes, and arbitrary field polarizations. Regardless of the specific driving conditions, the resulting spin- and enantio-sensitive observables are still controlled by the same three pseudovectors, underscoring their universal role as the primary generators of chirality-induced spin asymmetries, emphasizing their fundamental geometric origin and the universality of the mechanism identified here.

physics.atom-ph

Spin-current correlations in photoionization of chiral molecules

Chirality-induced spin selectivity (CISS) refers to phenomena where molecular chirality governs spin polarization. While symmetry simply requires chiral molecules to support spin-vector correlations, we show that CISS is fundamentally a conditioned measurement of these correlations. We illustrate this principle for spin-resolved one-photon ionization of a randomly oriented ensemble of chiral molecules. We introduce and quantify the phenomenon of enantio-sensitive locking of the photoelectron current to its spin, thereby providing a complete description of spin-conditioned photoelectron currents in one-photon ionization.

quant-ph

Enantiosensitive molecular compass

Chirality describes the asymmetry between an object and its mirror image and underlies diverse functionalities across molecular, mesoscopic and bulk matter. A particularly intriguing example is chirality-induced spin selectivity (CISS), where chiral structures generate enantio-sensitive spin polarization. Despite extensive research, its microscopic origin and unexpectedly large magnitude remain unresolved. Here, we isolate the intrinsic coupling between chirality and spin by considering spin-resolved photoionization of randomly oriented chiral molecules under isotropic illumination. We show that electric-dipole photoionization in the presence of spin-orbit coupling generates intrinsic correlations between molecular orientation and photoelectron spin that survive complete isotropic averaging. We identify these spin-orientation correlations as the microscopic origin of CISS in photoionization and reveal their complementary manifestation: selecting the photoelectron spin orients the residual molecular ensemble, realizing spin-orientation locking, whereas selecting molecular orientation produces CISS. Both effects are governed by the same correlation strength, set by the magnitude of a molecular-frame photoionization Bloch vector that defines an enantio-sensitive molecular compass. An analogous compass emerges in photoexcitation. Our results establish spin - orientation correlations as a fundamental ingredient of chiral spin photodynamics and provide a microscopic framework for understanding and exploiting spin selectivity in chiral matter.

cond-mat.mes-hall

Geometry of chiral temporal structures II: The formalism

We develop a mathematical formalism underlying the emergence of enantio-sensitive molecular orientation due to photoionization or photoexitation of chiral molecules. We consider geometric quantities such as the Berry connection and Berry curvature in light-driven chiral electronic states in the space of complex light polarization vectors. The parametric dependence of the light-driven electronic wavefunction on such vectors emerges due to various possible mutual orientations between the laser field and a chiral molecule. Using the tools of differential geometry we show how the enantio-sensitive observables emerge from the geometry of the molecular response in such spaces.

quant-ph

In Search Of Lost Tunneling Time

The measurement of tunneling times in strong-field ionization has been the topic of much controversy in recent years, with the attoclock and Larmor clock being two of the main contenders for correctly reproducing these times. By expressing the attoclock as the weak value of temporal delay, we extend its meaning beyond the traditional setup. This allows us to calculate the attoclock time for a static one-dimensional tunneling model consisting of a binding delta potential and a constant electric field. We apply the Steinberg weak-value interpretation of the Larmor clock. Using this definition, we obtain the position-resolved time density during tunnel ionization, yielding a non-zero Larmor tunneling time. Our model allows us to derive the analogue of the position-resolved attoclock tunneling time. While non-zero at the tunnel exit, it vanishes at the detector, far away from the atom. Formally, this means that the attoclock does not measure the "local" Larmor time, but instead a "non-local" time closely related to the phase time.

quant-ph

Enantiosensitive exceptional points in open chiral systems

Exceptional points (EPs) are remarkable spectral degeneracies in a non-Hermitian system's parameter space, where both eigenvalues and eigenstates coalesce. Here, we show that in non-Hermitian molecular chiral systems the position of EPs in the parameter space is enantiomer-specific. First, we show that encircling the EP of one enantiomer drives robust topological population transfer in the chiral molecule while its mirror twin remains unaffected, offering a new route for selective chiral control. Second, we reveal how resonant excitation of EPs in chiral molecules can amplify weak chiral effects, offering an alternative approach to the enhancement of chiral interactions. Third, we demonstrate that a twisted chiral fiber immersed in a liquid solution of chiral molecules exhibits topologically different behavior depending on the solution's enantiomeric excess, offering a new approach to the detection of molecular chirality. Our results combine high enantiosensitivity with topological robustness in chiral discrimination and control, paving the way for new approaches in the exploration of non-Hermitian and chiral phenomena.

quant-ph

Geometry of chiral temporal structures I: Physical effects

In non-relativistic physics, the concepts of geometry and topology are usually applied to characterize spatial structures or structures in momentum space. We introduce the concept of temporal geometry, which encompasses the geometric and topological properties of temporal shapes, i.e. trajectories traced by the tip of a time-dependent vector in vector space. We apply it to vectors describing ultrafast electron currents or induced polarization in chiral molecules. The central concepts of temporal geometry - Berry curvature and Berry connection - emerge as ubiquitous features of photoexcited, non-equilibrium, chiral electron dynamics. We demonstrate that the Berry curvature and Berry connection (i) rely on the polarization properties of light pulses, (ii) can be introduced for multiphoton processes, and (iii) control enantio-sensitive geometric observables via non-equilibrium electronic dynamics excited by tailored laser fields. Our findings may open a way to ultrafast, topologically non-trivial, and enantio-sensitive chemical dynamics.

quant-ph

Revealing the Berry phase under the tunneling barrier

In quantum mechanics, a quantum wavepacket may acquire a geometrical phase as it evolves along a cyclic trajectory in parameter space. In condensed matter systems, the Berry phase plays a crucial role in fundamental phenomena such as the Hall effect, orbital magnetism, and polarization. Resolving the quantum nature of these processes commonly requires sensitive quantum techniques, as tunneling, being the dominant mechanism in STM microscopy and tunneling transport devices. In this study, we integrate these two phenomena - geometrical phases and tunneling - and observe a complex-valued Berry phase via strong field light matter interactions in condensed matter systems. By manipulating the tunneling barrier, with attoseconds precision, we measure the imaginary Berry phase accumulated as the electron tunnels during a fraction of the optical cycle. Our work opens new theoretical and experimental directions in geometrical phases physics and their realization in condensed matter systems, expanding solid state strong field light metrology to study topological quantum phenomena.

cond-mat.mes-hall

Ultrafast TACOS -- Terahertz-Assisted Chiro-Optical Spectroscopy

We bring together the advantages of terahertz (THz) and optical spectroscopies to introduce TACOS (Terahertz-Assisted Chiro-Optical Spectroscopy), a novel approach for ultrafast and highly efficient imaging of molecular chirality and control over chiral electronic dynamics. We show how, using a THz pulse, we can induce a transient electronic orientation in a medium of randomly oriented chiral molecules that breaks the isotropy of the molecular sample. This symmetry breaking twists the nonlinear response of the medium to an ultrashort linearly polarised optical pulse in a highly enantiosensitive manner. As a result, the medium emits elliptically polarised light at new optical frequencies that records the molecular handedness via purely electric-dipole interactions. The long wavelength and period of the THz pulse enable both spatial coherence across the sample and a substantial degree of electronic orientation over the duration of the ultrashort optical pulse. TACOS does not require optical carrier-envelope phase stability or working in vacuum, and it creates exciting avenues for ultrafast and highly efficient chiral sensing and manipulation.

physics.optics

Bidirectional cascaded superfluorescent lasing in air enabled by resonant third harmonic photon exchange from nitrogen to argon

Cavity-free lasing in atmospheric air has stimulated intense research towards fundamental understanding of underlying physical mechanisms. In this Letter, we identify a new mechanism -- third harmonic photon mediated resonant energy transfer pathway leading to population inversion in argon via initial three-photon excitation of nitrogen molecules irradiated by intense 261 nm pulses -- that enables bidirectional two-color cascaded lasing in atmospheric air. By making pump-probe measurements, we conclusively show that such cascaded lasing results from superfluorescence (SF) rather than amplified spontaneous emission (ASE). Such cascaded lasing with the capability of producing bidirectional multicolor coherent pulses opens additional possibilities for remote sensing applications.

physics.optics

Capturing electron-driven chiral dynamics in UV-excited molecules

Molecular chirality is a key design property for many technologies including bioresponsive imaging, circularly polarized light detection and emission, molecular motors and switches. Imaging and manipulating the primary steps of transient chirality is therefore central for controlling numerous physical, chemical and biological properties that arise from chiral molecules in response to external stimuli. So far, the manifestation of electron-driven chiral dynamics in neutral molecules has not been demonstrated at their intrinsic timescale. Here, we use time-resolved photoelectron circular dichroism (TR-PECD) with an unprecedented instrument response function of 2.9 fs to image the dynamics of coherent electronic motion activated by prompt UV-excitation in neutral chiral molecules, disclosing its impact on the molecular chiral response. We find that electronic beatings between Rydberg states lead to periodic modulations of the chiroptical response on the few-femtosecond timescale, showing a sign inversion in less than 10 fs. Calculations including both the molecular UV-excitation and subsequent photoionization confirm this interpretation and provide further evidence that the combination of the resulting photoinduced chiral current with a circularly polarized probe pulse realizes an enantio-selective filter of molecular orientations upon photoionization, opening up a route towards enantio-selective charge-directed reactivity.

physics.chem-ph

Generation of massively entangled bright states of light during harmonic generation in resonant media

At the fundamental level, full description of light-matter interaction requires quantum treatment of both matter and light. However, for standard light sources generating intense laser pulses carrying quadrillions of photons in a coherent state, the classical description of light during intense laser-matter interaction has been expected to be adequate. Here we show how nonlinear optical response of matter can be controlled to generate dramatic deviations from this standard picture, including generation of several squeezed and entangled harmonics of the incident laser light. In particular, such non-trivial quantum states of harmonics are generated as soon as one of the harmonics induces a transition between different laser-dressed states of the material system. Such transitions generate an entangled light-matter wavefunction, which can generate quantum states of harmonics even in the absence of a quantum driving field or material correlations. In turn, entanglement of the material system with a single harmonic generates and controls entanglement between different harmonics. Hence, nonlinear media that are near-resonant with at least one of the harmonics appear to be quite attractive for controlled generation of massively entangled quantum states of light. Our analysis opens remarkable opportunities at the interface of attosecond physics and quantum optics, with implications for quantum information science.

quant-ph

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

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

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

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