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Avner Fleischer

Publications and source records attributed to Avner Fleischer.

17 recordsLinked to original sources

Reducing the Carrier-Envelope-Phase-dependence of High-Harmonic-Generation by Vectorial-Time-Polarization-Gating

A well-known shortcoming of High Harmonic Generation (HHG) is the strong dependence of the broadband HHG spectra (HGS) on the carrier envelope phase (CEP) of the driver. Here we numerically show that compared to the current well-established scalar (linearly polarized) schemes for generating broadband HGS, namely a short driver [Amplitude gating (AG)], Polarization-Gating (PG) or Time-Gating (TG), the vectorial driver of the Vectorial-Time-Polarization-Gating (VTPG) scheme renders the cutoff HGS much less sensitive to the CEP of the driver. The polarization state (helicity) of the emitted radiation is likewise CEP-resilient. Unlike scalar schemes, where the number of recollisions heavily depends on the CEP, in VTPG the CEP keeps this number almost unchanged, and only controls the partitioning of the recollisions between two orthogonal directions. This reduces the CEP-dependence of the HGS and decreases the spectral modulations. The CEP-resilience of the VTPG scheme holds promise for a variety of applications in attosecond science benefiting from quasicontinuous, helical HHG sources liberated from the necessity to stabilize the CEP of the laser.

physics.optics

Photoelectron chiral dichroism induced by lasers without helicity via chiral hole wave-packets

Photoelectron circular dichroism (PECD) is a method where randomly oriented chiral molecules are photoionized due to irradiation by circularly-polarized lasers, yielding large chiral signals in the photoelectron momentum distribution. Recently, PECD was explored with polarization-tailored light such as bi-chromatic and non-collinear drivers, which still produces significant chiral signals. Yet, all known PECD configurations to date exhibit non-zero time-local chirality. That is, they are driven by an intrinsically helical light source. Nonetheless, 'chiral' light can also be non-helical if its chirality manifests on longer timescales (e.g. an optical centrifuge). It remains unknown whether PECD can arise from non-helical coherent light. Here we predict that PECD indeed emerges from non-helical light by employing a train of linearly-polarized intense laser pulses with a rotating polarization axis, which are phase-coherent and time-delayed. We find strong PECD in the model chiral molecule CBrClFH under a wide parameter regime that can be optimized up to ~8% by tuning delays between pulses, suggesting quantum interference. We directly show that the physical mechanism for this type of PECD differs from the standard case, relying on a chiral hole attosecond wave-packet evolving in the molecule, induced by the first linear pulse. Our work shows that multiple mechanisms can give rise to PECD on longer timescales and provides a novel approach for ultrafast chirality spectroscopy and coherent chiral wave-packet manipulation.

physics.optics

Light's symmetry, asymmetry, and their role in nonlinear optics and ultrafast phenomena

The analysis of symmetries is extremely useful across science. In Physics, symmetries are used to derive conservation laws and selection rules for transitions in interacting systems. In the early days of nonlinear optics (NLO), symmetries were used to formulate a set of rules for photonic processes according to the medium's symmetries that are reflected in the NLO coefficient tensor. While this approach was believed to be complete and closed, the field has recently reignited as multi-color ultrashort laser pulses with tailored polarization and spatiotemporal structures become standard in NLO. A more complete theory has been recently emerging, which aims to incorporate all possible dynamical degrees of freedom of light: spin and orbital angular momentum, spatial structure, time-dependent polarizations, temporal envelopes, etc., in addition to the symmetries of the medium. This theoretical development is also accompanied by experimental advances that rely on tailored light beams that can now be generated with ever-increasing complexity, including topologies in real and a variety of synthetic dimensions, carrying poly-chromatic carrier waves, time-dependent varying angular momenta, local-chirality, and more. The nonlinear interactions between light fields with unique symmetries (or asymmetries) and matter is especially appealing, since that holds the key for developing new ultrafast spectroscopies with sub-femtosecond resolution, for exerting exact control over matter, and improving our fundamental understanding of how light and matter interact. We review these recent advances in this expanding field, focusing on the theory, its implications, and seminal experiments. We aim to establish a comprehensive database of symmetries and selection rules governing NLO light-matter interactions within the emerging new formalism, and invite the scientific community to contribute to this effort.

physics.optics

Chiral broadband High Harmonic Generation Source by Vectorial Time-Polarization-Gating

Chiral (highly helical) extreme ultraviolet (XUV) sources are pivotal for investigating chiroptical phenomena on the ultrafast electronic timescale. Table-top, coherent High Harmonic Generation (HHG)-based sources are particularly well-suited for these studies. However, chiral materials, such as organic chiral molecules and solid-state magnetic materials, exhibit fine spectral features which necessitate broadband radiation for their complete interrogation. The generation of radiation that is both broadband and helical through HHG presents a seemingly paradoxical challenge: while chiral HHG emission requires at least two recollisions occurring along different directions in the polarization plane, the Floquet limit might already be reached with as few as three recollisions, resulting in a sparse spectrum characterized by pronounced discrete harmonic peaks. Here we propose a straightforward scheme that enables the interrogation of fine spectral features, in principle restricted only by the resolution of the XUV spectrometer, with chiral XUV light. Our method is based on using a vectorial two-color driver with close central-frequencies with slight symmetry breaking. It integrates the time-gating and polarization-gating techniques to generate a vectorial driver which induces well-controlled bursts of recollisions, occurring along different directions in the polarization plane. The method satisfies the dual requirements of an XUV source which is both broadband and helical. We perform polarization scan and demonstrate that the broadband XUV radiation exhibits rapid modulations in its spectral ellipticity, and fast alternation in its spectral helicities. The phase of modulations could be controlled by introducing a slight symmetry breaking. This allows us to control and modulate the XUV polarization state, which should enable the detection of chiroptical signals with enhanced sensitivity.

physics.optics

New photonic conservation laws in parametric nonlinear optics

Conservation laws are one of the most generic and useful concepts in physics. In nonlinear optical parametric processes, conservation of photonic energy, momenta and parity often lead to selection rules, restricting the allowed polarization and frequencies of the emitted radiation. Here we present a new scheme to derive conservation laws in optical parametric processes in which many photons are annihilated and a single new photon is emitted. We then utilize it to derive two new such conservation laws. Conservation of reflection-parity (RP) arises from a generalized reflection symmetry of the polarization in a superspace, analogous to the superspace employed in the study of quasicrystals. Conservation of space-time-parity (STP) similarly arises from space-time reversal symmetry in superspace. We explore these new conservation laws numerically in the context of high harmonic generation and outline experimental set-ups where they can be tested.

physics.optics

Controlling the Bandwidth of High Harmonic Emission Peaks with the Spectral Polarization of the Driver

We demonstrate a High-Harmonic-Generation scheme which offers control over the bandwidth of the spectral peaks. The scheme uses a vectorial two-color driver with close central frequencies, generated by spectrally splitting a linearly-polarized input femtosecond-duration laser pulse and subsequent recombining the two halves after their polarizations are made cross-elliptical and counter-rotating. This results in the generation of new emission channels which coalesce into broad odd-integer HHG peaks, the bandwidth of each being proportional to the frequency difference between the two colors, to the harmonic order and inversely-proportional to the driver fields' ellipticities. Peak-broadening to the extent that a supercontinuum is formed is also demonstrated. This source will find use in HHG applications benefiting from high-flux broadband extreme ultra-violet radiation, such as attosecond transient absorption spectroscopy.

physics.optics

High Harmonic Generation without Tunnel-Ionization

A new High Harmonic Generation (HHG) scheme, which doesn't rely on Tunnel-Ionization as the ionization mechanism but rather on Single-Photon Ionization, is theoretically proposed and numerically demonstrated. The scheme uses two driver fields: an extreme-ultraviolet driver which induces the ionization, and a circularly-polarized, co-rotating, two-color infrared driver carried at a fundamental frequency and its second harmonic which induces the recollision. Using Classical and time-dependent Schr\"odinger equation simulations of a model Argon atom, we show that in this scheme ionization is essentially decoupled from recollision. Releasing the process from being Tunneling-dependent reduces its degree of nonlinearity, which offers new capabilities in attosecond science, such as generation of High Harmonics from highly-charged ions, or from specific deep core electronic levels. It is shown that the emitted high harmonics involve the absorption of photons of one color of the infrared driver, and the emission of photons of the second color. This calls for future examination of the possible correlations between the emitted high harmonics.

physics.atom-ph

Multi-scale dynamical symmetries and selection rules in nonlinear optics

Symmetries and their associated selection rules are extremely useful in all fields of science. In particular, for system that include electromagnetic (EM) fields interacting with matter, it has been shown that both of symmetries of matter and EM field's time-dependent polarization play a crucial role in determining the properties of linear and nonlinear responses. The relationship between the system's symmetry and the properties of its excitations facilitate precise control over light emission and enable ultrafast symmetry-breaking spectroscopy of variety of properties. Here. we formulate the first general theory that describes the macroscopic dynamical symmetries (including quasicrystal-like symmetries) of an EM vector field, revealing many new symmetries and selection rules in light-matter interactions. We demonstrate an example of multi-scale selection rules experimentally in the framework of high harmonic generation (HHG). This work waves the way for novel spectroscopic techniques in multi-scale system as well as for imprinting complex structures in EUV-X-ray beams, attosecond pulses, or the interacting medium itself.

physics.optics

Selection rules in symmetry-broken systems by symmetries in synthetic dimensions

Selection rules are often considered a hallmark of symmetry. When a symmetry is broken, e.g., by an external perturbation, the system exhibits selection rule deviations which are often analyzed by perturbation theory. Here, we employ symmetry-breaking degrees of freedom as synthetic dimensions, to demonstrate that symmetry-broken systems systematically exhibit a new class of symmetries and selection rules. These selection rules determine the scaling of a system's observables (to all orders in the strength of the symmetry-breaking perturbation) as it transitions from symmetric to symmetry-broken. We specifically analyze periodically driven (Floquet) systems subject to two driving fields, where the first field imposes a spatio-temporal symmetry, and the second field breaks it, imposing a symmetry in synthetic dimensions. We tabulate the resulting synthetic symmetries for (2+1)D Floquet group symmetries and derive the corresponding selection rules for high harmonic generation (HHG) and above-threshold ionization (ATI). Finally, we observe experimentally HHG selection rules imposed by symmetries in synthetic dimensions. The new class of symmetries & selection rules extends the scope of existing symmetry breaking spectroscopy techniques, opening new routes for ultrafast spectroscopy of phonon-polarization, spin-orbit coupling, and more.

physics.optics

High-order harmonics with frequency-varying polarization within each harmonic

We predict high-order harmonics in which the polarization within the spectral bandwidth of each harmonic varies continuously and significantly. For example, the interaction of counter-rotating circularly-polarized bichromatic drivers having close central frequencies with isotropic gas leads to the emission of polarization-fan harmonics which are nearly circularly-polarized in one tail of the harmonic peak, linear in the center of the peak and nearly circular with the opposite helicity in the opposite tail. Polarization fan harmonics are obtained as a result of multiple (at least two) head-on recollisions of electrons with their parent ions occurring from different angles. The process can be phase-matched using standard methods (e.g. pressure tuning phase matching) and maintains the single-atom polarization property through propagation. These polarization-fan harmonics may be used for exploring non-repetitive ultrafast chiral phenomena, e.g. dynamics of magnetic domains, in a single shot

physics.optics

Generation of phase-matched circularly-polarized extreme ultraviolet high harmonics for magnetic circular dichroism spectroscopy

Circularly-polarized extreme UV and X-ray radiation provides valuable access to the structural, electronic and magnetic properties of materials. To date, this capability was available only at large-scale X-ray facilities such as synchrotrons. Here we demonstrate the first bright, phase-matched, extreme UV circularly-polarized high harmonics and use this new light source for magnetic circular dichroism measurements at the M-shell absorption edges of Co. We show that phase matching of circularly-polarized harmonics is unique and robust, producing a photon flux comparable to the linearly polarized high harmonic sources that have been used very successfully for ultrafast element-selective magneto-optic experiments. This work thus represents a critical advance that makes possible element-specific imaging and spectroscopy of multiple elements simultaneously in magnetic and other chiral media with very high spatial and temporal resolution, using tabletop-scale setups.

physics.optics

Does high harmonic generation conserve angular momentum?

High harmonic generation (HHG) is a unique and useful process in which infrared or visible radiation is frequency up converted into the extreme ultraviolet and x ray spectral regions. As a parametric process, high harmonic generation should conserve the radiation energy, momentum and angular momentum. Indeed, conservation of energy and momentum have been demonstrated. Angular momentum of optical beams can be divided into two components: orbital and spin (polarization). Orbital angular momentum is assumed to be conserved and recently observed deviations were attributed to propagation effects. On the other hand, conservation of spin angular momentum has thus far never been studied, neither experimentally nor theoretically. Here, we present the first study on the role of spin angular momentum in extreme nonlinear optics by experimentally generating high harmonics of bi chromatic elliptically polarized pump beams that interact with isotropic media. While observing that the selection rules qualitatively correspond to spin conservation, we unequivocally find that the process of converting pump photons into a single high-energy photon does not conserve angular momentum, i.e. this process is not self contained. In one regime, we numerically find that this major fundamental discrepancy can be explained if the harmonic photons are emitted in pairs. Yet in another regime, the ionizing electron carries the missing angular momentum. The results presented here, apart from exploring the very foundations of HHG, are also important for a variety of applications, as our system exhibits full control over the harmonics polarization, from circular through elliptical to linear polarization, without comprising the efficiency of the process. This work paves the way for a broad range of applications with HHG, from ultrafast circular dichroism to zepto-clocks and to attosecond quantum optics.

physics.optics

Multiphoton Femtosecond Coherent Control in the Single-Cycle Regime

Coherent control of the atomic two-photon absorption with shaped single-cycle pulses is examined theoretically in the weak-field regime. The control over the stabilized carrier-envelope phase (CEP) of the pulses is determined as a key parameter allowing the full utilization of the ultrabroad pulse spectrum. This bandwidth is sufficient to provide besides the sequential two-photon pathways, additional Raman-type pathways coupling between the ground and the excited states. The interference between the different pathways is efficiently controlled via the control over the CEP. Simplified two-level model is analyzed in the frequency domain where the rational pulse shaping is applied. The developed intuition is applied to atomic Cs and verified by the exact numerical solution of time-dependent Schrodinger equation.

physics.atom-ph

Generation of Higher-Order Harmonics By Addition of a High Frequency XUV Radiation to the IR One

The irradiation of atoms by a strong IR laser field of frequency $ω$ results in the emission of odd-harmonics of $ω$ ("IR harmonics") up to some maximal cut-off frequency. The addition of an XUV field of frequency $\tilde{q}ω$ larger than the IR cut-off frequency to the IR driver field leads to the appearance of new higher-order harmonics ("XUV harmonics") $\tilde{q} \pm 2K, 2\tilde{q} \pm (2K-1), 3\tilde{q} \pm 2K,...$ ($K$ integer) which were absent in the spectra in the presence of the IR field alone. The mechanism responsible for the appearance of the XUV harmonics is analyzed analytically using a generalization of the semiclassical re-collision (three-step) model of high harmonic generation. It is shown that the emitted HHG radiation field can be written as a serie of terms, with the HHG field obtained from the three-step model in its most familiar context [P. B. Corkum, \textit{Phys. Rev. Lett.} {\bf 71}, 1994 (1993)] resulting from the zeroth-order term. The origin of the higher-order terms is shown to be the ac-Stark oscillations of the remaining ground electronic state which are induced by the XUV field. These terms are responsible for the appearance of the new XUV harmonics in the HGS. The XUV harmonics are formed by the same electron trajectories which form the IR harmonics and have the same emission times, but a much lower intensity than the IR harmonics, due to the small quiver amplitude of the ac-Stark oscillation. Nevertheless, this mechanism allows the extension of the cut-off in the HGS without the necessity of increasing the IR field intensity, as is verified by numerical time-dependent Schrödinger equation simulation of a Xe atom shined by a combination of IR and XUV field.

physics.atom-ph

Amplification of High Harmonics Using Weak Perturbative High Frequency Radiation

The mechanism underlying the substantial amplification of the high-order harmonics q \pm 2K (K integer) upon the addition of a weak seed XUV field of harmonic frequency qωto a strong IR field of frequency ωis analyzed in the framework of the quantum-mechanical Floquet formalism and the semiclassical re-collision model. According to the Floquet analysis, the high-frequency field induces transitions between several Floquet states and leads to the appearance of new dipole cross terms. The semiclassical re-collision model suggests that the origin of the enhancement lies in the time-dependent modulation of the ground electronic state induced by the XUV field.

physics.atom-ph

Calculations of time-dependent observables in non-Hermitian quantum mechanics: The problem and a possible solution

The solutions of the time independent Schrodinger equation for non-Hermitian (NH) Hamiltonians have been extensively studied and calculated in many different fields of physics by using L^2 methods that originally have been developed for the calculations of bound states. The existing non-Hermitian formalism breaks down when dealing with wavepackets(WP). An open question is how time dependent expectation values can be calculated when the Hamiltonian is NH ? Using the F-product formalism, which was recently proposed, [J. Phys. Chem., 107, 7181 (2003)] we calculate the time dependent expectation values of different observable quantities for a simple well known study test case model Hamiltonian. We carry out a comparison between these results with those obtained from conventional(i.e., Hermitian) quantum mechanics (QM) calculations. The remarkable agreement between these results emphasizes the fact that in the NH-QM, unlike standard QM, there is no need to split the entire space into two regions; i.e., the interaction region and its surrounding. Our results open a door for a type of WP propagation calculations within the NH-QM formalism that until now were impossible.

quant-ph

Adiabatic theorem for non-hermitian time-dependent open systems

In the conventional quantum mechanics (i.e., hermitian QM) the adia- batic theorem for systems subjected to time periodic fields holds only for bound systems and not for open ones (where ionization and dissociation take place) [D. W. Hone, R. Ketzmerik, and W. Kohn, Phys. Rev. A 56, 4045 (1997)]. Here with the help of the (t,t') formalism combined with the complex scaling method we derive an adiabatic theorem for open systems and provide an analytical criteria for the validity of the adiabatic limit. The use of the complex scaling transformation plays a key role in our derivation. As a numerical example we apply the adiabatic theorem we derived to a 1D model Hamiltonian of Xe atom which interacts with strong, monochromatic sine-square laser pulses. We show that the gener- ation of odd-order harmonics and the absence of hyper-Raman lines, even when the pulses are extremely short, can be explained with the help of the adiabatic theorem we derived.

physics.atom-ph