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Misha Ivanov

Publications and source records attributed to Misha Ivanov.

At least 19 recordsLinked to original sources

Valley polarization driven by two-color circular fields from a strong-field tunneling 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 $ω+Nω$ 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 $ω+2ω$ and co-rotating $ω+4ω$ fields.

physics.optics↗

Physical Mechanisms of Light-Induced Molecular Fragmentation in the Long-Wavelength Regime

Strong near-infrared (NIR) laser fields ionize polyatomic molecules through tunneling and multiphoton processes, while subsequent molecular fragmentation can be driven by electron rescattering and field-induced nonadiabatic excitation of the molecular ion. How these competing mechanisms deposit energy into molecular ions and determine fragmentation branching remains unresolved. By combining wavelength- and ellipticity-dependent intensity-difference mass spectrometry of methanol with time-dependent Schrödinger equation (TDSE) and semiclassical Monte Carlo simulations, we demonstrate that, in the tunneling-to-intermediate regime ($γ\lesssim 1$), molecular fragmentation is governed by the interplay of electron recollision and field-driven nonadiabatic excitation, revealing competing physical mechanisms relevant to polyatomic molecules more broadly. Ellipticity-dependent measurements demonstrate that these mechanisms can be experimentally distinguished for individual cationic fragments. Channels requiring high internal energies exhibit the strong ellipticity-dependent suppression characteristic of rescattering-driven processes, while lower-energy channels are comparatively less sensitive. Although small-fragment yields decrease substantially with increasing wavelength, their relative distributions remain largely unchanged, indicating that the underlying fragmentation pathways are preserved and that the suppression primarily reflects reduced probabilities of electron recollision and nonadiabatic excitations at longer wavelengths.

physics.chem-ph↗

Generation of Stable Peak-Power Similaritons through Gain-Managed Nonlinearity

Fiber lasers and amplifiers offer attractive alternatives to conventional solid-state systems. However, generation of high-energy ultrashort laser pulses in fibers faces challenges due to the complex interplay of multiple nonlinear effects arising due to pulse confinement within a small fiber core and also limitations imposed by the gain bandwidth of the available active fibers. The discovery of self-similar amplification and gain-managed nonlinear amplification (GMNA) pulse propagation regimes in fibers with normal dispersion suggests that these challenges can be turned into an advantage. Here we show that pulses generated in the GMNA regime are, in fact, the realization of the idealized similariton-type pulses in realistic fibers with limited gain bandwidth. Our analytical and numerical results show how one should shape the fiber gain as a function of propagation length to achieve constant peak power similariton-like pulses with steadily increasing energy, the pulse bandwidth exceeding the gain bandwidth, and the nearly linear frequency chirp allowing for efficient pulse compression to its Fourier limit. Absent Raman nonlinearities, these pulses can reach $μ$J level energies in standard single-mode fibers, representing a tenfold increase in pulse energy compared to the best currently available nonlinear amplifiers. Our results have significant implications for the fundamental understanding of nonlinear wave dynamics and for the advancement of fiber laser technology, supporting the reliable generation of high-energy pulses for practical use in areas such as micromachining, metrology, and bioimaging.

physics.optics↗

Photonic architectures for synthetic chiral light-driven chiral sensing

Molecular chirality gives rise to left- and right-handed enantiomers whose balance underpins biochemical function. Deviations from this enantiomeric excess are promising biomarkers of disease. Despite its importance, rapid and sensitive detection of enantiomeric excess in trace amounts of small chiral molecules remains an outstanding challenge. Synthetic chiral light introduces new opportunities for chiroptical spectroscopy, with the potential to enhance light-matter interactions by several orders of magnitude. Here we propose a new class of photonic architectures for synthetic chiral light, in which photonic structures generate, guide and optimize chiral light-matter interactions. As a first realization, we show that hollow dielectric waveguides support phase-matched propagation of multicolor fields enabling coherent accumulation of the enantio-sensitive nonlinear response over centimeter-scale distances. By combining microscopic quantum-response simulations with Maxwell's equations, we predict that incident pulse energies of around 1 uJ produce hundreds of picojoules of third-harmonic emission from only picomole quantities of carvone gas at 50 mbar over just 2 cm of propagation, with enantio-sensitive contrast approaching 5%. Phase-resolved Fourier analysis isolates a background-free chiral signal exhibiting the maximum possible dichroism of 200%. Beyond efficient chiral sensing, photonic architectures for synthetic chiral light establish a scalable platform for integrated nonlinear chiral spectroscopy, molecular fingerprinting based on ultrafast electron dynamics, and topologically robust chiroptical observables.

physics.optics↗

Phase-sensitive avalanche quantum sensing of sub-shot-noise fields

Avalanche-based detection of small perturbations is commonplace in precision measurement devices from Geiger counters to single-photon avalanche detectors. Here, we expand this principle to sensing of light waves below the quantum shot noise limit, demonstrating numerically how atomic clouds trapped in photonic cavities can exhibit non-perturbative sensitivity to changes in the cavity field when the cavity mode is tuned to a parity-prohibited transition. We find that, when pumped by a continuous-wave laser, the atomic cloud creates emissions which amplify the initially sub-shot-noise fluctuation by two orders of magnitude. Crucially, this amplification is broadly tunable with respect to frequency and independent of atomic energy structure. Even more strikingly, our amplification mechanism preserves the phase imparted on the atoms by the original ultra-weak light wave, marking a qualitative improvement over conventional protocols. Our finding has implications for both quantum state characterization and detection of weak classical signals.

quant-ph↗

Reconstructing Molecular-Ion Quantum States with Two-Color Strong-Field Scattering

Strong-field ionization of molecules can prepare coherent superpositions of ionic states whose amplitudes and relative phases govern the ensuing ultrafast dynamics, but accessing this information experimentally remains a challenge. Here we introduce two-color strong-field scattering, in which a strong mid-infrared field ionizes the molecule and launches an electron, while a weak second harmonic field resonantly couples vibronic states of the parent ion during the electron's continuum excursion, thereby introducing structural changes on the sub-laser-cycle timescale. Scanning the relative phase between the two colors controls the ionic evolution and maps it onto phase-dependent sub-angstrom bond-length changes retrieved from the rescattering signal. Using the example of N$_2$, we apply the two-color setup to probe the coherence between different ionization channels and to reconstruct the initial ionic superposition. Our results establish two-color strong-field scattering as a powerful structural approach to characterize the complex amplitudes of ion quantum wavepackets.

physics.atom-ph↗

Strong-field electro-optic sampling of light

We report the experimental realization of electro-optic sampling of light utilizing strong-field light-matter interaction. We show that in contrast to the perturbative regime where the non-linear signal (eg. sum-frequency generation) is localized at the narrowband spectrum that must match the local oscillator, the strong-field regime relies on the generation of a supercontinuum that automatically fulfills the overlaps with a local oscillator providing extremely broadband detection bandwidth. We develop a semi-classical model, benchmark it against the experiments with carrier-envelope-phase (CEP) stable sub-3 femtosecond pulses of octave-spanning bandwidth, and further validate it by a first-principle time-dependent density functional (TDDFT) theory. Our work establishes a simple electro-optic approach for investigating broadband high-frequency dynamics of matter on sub-cycle timescales with attosecond precision.

physics.optics↗

Semiconductor Wannier equations: a real-time, real-space approach to the nonlinear optical response in crystals (ATATA)

We develop the semiconductor Wannier equations (SWEs), a real-time, real-space formulation of ultrafast light-matter dynamics in crystals, by deriving the equations of motion for the electronic reduced density matrix in a localized Wannier basis. Working in real space removes the structure-gauge ambiguities that hinder reciprocal-space semiconductor Bloch equations. Electron--electron interactions are included at the time-dependent Hartree plus static screened-exchange (TD-HSEX) level. Decoherence is modeled with three complementary channels: pure dephasing, population relaxation, and distance-dependent real-space dephasing; providing physically grounded damping for strong-field phenomena such as high-harmonic generation. Conceptually, the SWEs bridge real-space semiclassical intuition with many-body solid-state optics, offering a numerically robust and gauge-clean alternative to reciprocal-space approaches for nonlinear optical response and attosecond spectroscopy in solids.

physics.optics↗

Quantum Optics of harmonic generation in the strongly driven Jaynes-Cummings-type system

We adapt the Jaynes-Cummings model to study the interface of cavity quantum electrodynamics with strong field and attosecond physics. We show how multi-photon resonances in the Jaynes- Cummings system driven by a strong low-frequency classical light field lead to the generation of highly non-classical, quantum-correlated harmonics of the classical driver. Our treatment assumes no approximations, apart from the typical Jaynes-Cummings model assumption of only a few discrete quantum modes of light. The paper is dedicated to Joseph Henry Eberly, whose remarkable research has left indelible mark on both strong field physics and quantum optics.

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↗

Extreme Ultrafast Dynamics of the Refractive Index in Transparent Conductive Oxides: Theory and Experiment

Recent experiments in transparent conductive oxides (TCOs) have revealed light-induced order-unity variations in the refractive index occurring at extreme time scales, as short as a few-femtoseconds. These experimental observations remain unexplained, especially the ultrafast 10-20 femtoseconds relaxation of the index change, that cannot be explained by known phonon-mediated relaxation processes. Here, we present a simplified model followed by comprehensive simulations describing the phenomena, relying on the microscopic dynamics of electrons in TCOs under powerful ultrafast laser pulses. With this physical model, we predict and experimentally observe the unexplored regime of intraband modulation of electrons in the conduction band, leading to ultrafast oscillations of the refractive index. The observation of the oscillations validates the theory as a predictive tool, utilizing it to design experiments targeting novel effects that hinge on extreme alterations of optical properties of materials, such as photonic time-crystals and a plethora of novel extreme ultrafast phenomena.

physics.optics↗

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 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↗

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↗

Coherent control of chirality in Weyl semimetals

Weyl fermions in inversion-symmetric Weyl semimetals occur in pairs of opposite chirality, leading to symmetric optical responses under circularly-polarised light and a vanishing net photocurrent. Here, we show that tailored two-colour light fields break this symmetry and enable selective excitation of individual Weyl nodes. The interference between a circularly-polarised $ω$ field and a phase-locked linearly-polarised $2ω$ field generates a chirality-dependent redistribution of carriers in momentum space, resulting in a nonzero controllable photocurrent. We demonstrate that both the magnitude and sign of the photocurrent can be tuned via the relative phase and field strength of the two colours, and identify an optimal regime in which chiral selectivity is maximised. Our results establish a general route to optically-controlled chiral charge dynamics in Weyl semimetals using polarisation-structured light.

cond-mat.mes-hall↗

Sub-cycle field-driven dynamical Berry phase in solids

In quantum mechanics, a wavepacket acquires a geometric phase, known as the Berry phase, as it evolves along a closed trajectory in parameter space. In condensed matter systems, the Berry phase underlies a broad range of phenomena, including the anomalous Hall effect, orbital magnetism, and electric polarization. However, in centrosymmetric materials possessing time-reversal (TR) symmetry, its manifestation is suppressed and effectively vanishes. When a system is driven by a strong terahertz (THz) field, it can be coherently driven far from equilibrium, transiently reshaping its symmetry on sub-picosecond timescales. This capability opens new avenues for quantum control with potential applications in information processing and sensing. Here, we experimentally demonstrate that a strong THz field can transiently break inversion symmetry in MgO, inducing a dynamical complex Berry phase, thereby manipulating the topological properties of the material. Applying high-harmonic generation (HHG) spectroscopy, we directly resolve the Berry phase, accessing both its real and imaginary components. The first is associated with coherent intraband dynamics while the second with quantum tunneling through a potential barrier. This observation enables the reconstruction of the time-dependent evolution of the Berry phase within the cycle of the THz field. The coherent manipulation of solids with strong fields, combined with attosecond-resolved HHG spectroscopy, represents a fundamental step toward unveiling and controlling geometric quantum phenomena in condensed matter systems.

cond-mat.mtrl-sci↗

Spontaneous symmetry breaking in nonlinear superradiance

Creation and manipulation of non-classical states of light is rapidly becoming the focus of modern attosecond science. Here, we demonstrate numerically how interaction with such states can trigger the emergence of a many-body system with spontaneously broken symmetry by considering a modification of the well-known problem of superradiance encountered already by Dicke. Similarly to him, we investigate photon emission by ensembles of indistinguishable atoms. In contrast to him, however, we leverage symmetry-based selection rules to suppress emission of single photons by single atoms. A steady state is therefore only reached following a spontaneous transition into a collective symmetry-broken state of atoms and photonic modes. This transition permanently locks the atomic dipoles to the quantum field experienced by the system at a particular instant, transforming the entire setup into a potent quantum sensor reproducing the phase of the recorded quantum fluctuation.

quant-ph↗

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↗