arXiv subjects

Nicola Mayer

Publications and source records attributed to Nicola Mayer.

9 recordsLinked to original sources

arXiv2026

Attosecond Transient Polarimetry

We introduce elliptical-dichroic attosecond transient absorption spectroscopy (eDATAS), an ultrafast attosecond spectroscopy technique in which an atomic gas is probed by elliptically polarized attosecond and near-infrared pulses with an arbitrary angle between the polarization ellipses and a varying time-delay. Using perturbation theory, we show that the transient absorption signal factorizes into form factors whose dependence on pulse ellipticities and polarization-ellipse orientations are governed entirely by dipole selection rules: ellipticity sets the amplitudes of the interfering multiphoton pathways, while the relative orientations of the ellipses control the phase. We reinterpret circular- and linear-dichroic attosecond transient absorption spectroscopy as limiting cases of eDATAS, and validate the theory through an eDATAS measurement in helium, finding excellent agreement. Finally, we demonstrate that eDATAS can also serve as an in situ measurement of the polarization state of the XUV field, avoiding the need for a dedicated XUV polarimeter.

physics.atom-ph↗

arXiv2026

Chiral moments make chiral measures

We develop a family of chiral measures to quantify the chirality of a distribution and assign it a handedness. Our measures are built using the tensorial moments of the distribution, which naturally encode its spatial character, not only via its angular shape consistently with existing multipolar-moment approaches, but also its radial dependence. We combine these tensorial moments into a rotationally-invariant pseudoscalar using a newly-defined cross product and triple product for arbitrary symmetric tensors. We analyze these measures for a variety of toy-model distributions, providing intuition for the geometry and guiding the choice of chiral measure optimal for a given distribution. We also apply our measures to a physically-motivated example coming from photoionization in polychromatic chiral light. Our work provides a robust, flexible, intuitive, highly geometrical, and physically-driven framework for understanding and quantifying the chirality of a wide variety of distributions, together with an open-source software package that makes this toolbox readily applicable for the analysis of numerical or experimental data.

physics.data-an↗

arXiv2025

Attosecond Optical Orientation

Circularly polarized light offers opportunities to probe symmetry-dependent properties of matter such as chirality and spin. Circular dichroism measurements typically require further intrinsic or extrinsic breaking of symmetry by e.g. enantiomeric excess, orientation, magnetic fields or direction-sensitive detectors. Here we introduce circular-dichroic attosecond transient absorption spectroscopy by leveraging the angular momentum of two circular-polarized pulses, both pump and probe, in an isotropic medium, optically orienting the angular momentum of excited states on an attosecond timescale. We investigate a circular-dichroic measurement of the attosecond transient absorption of He Rydberg states. By limiting the allowed pathways via dipole selection rules for co- and counter-rotating circular polarized NIR and XUV pulses, different spectral reshapings of the XUV transient absorption due to the AC Stark effect are observed. Paired with time-dependent Schrödinger equation calculations, the results show the role of selection and propensity rules and open up new opportunities to study coupling pathways of excited states as well as spin-dependent dynamics in atoms and beyond via attosecond optical orientation.

physics.atom-ph↗

arXiv2025

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↗

arXiv2024

Chiral topological light for detecting robust enantio-sensitive observables

The topological response of matter to electromagnetic fields is a property in high demand in materials design and metrology due to its robustness against noise and decoherence, stimulating recent advances in ultrafast photonics. Embedding topological properties into the enantio-sensitive optical response of chiral molecules could therefore enhance the efficiency and robustness of chiral optical discrimination. Here we achieve such a topological embedding by introducing the concept of chiral topological light~-- a light beam which displays chirality locally, with an azimuthal distribution of its handedness described globally by a topological charge. The topological charge is mapped onto the azimuthal intensity modulation of the non-linear optical response, where enantio-sensitivity is encoded into its spatial rotation. The spatial rotation is robust against intensity fluctuations and imperfect local polarization states of the driving field. Our theoretical results show that chiral topological light enables detection of percentage-level enantiomeric excesses in randomly oriented mixtures of chiral molecules, opening a way to new, extremely sensitive and robust chiro-optical spectroscopies with attosecond time resolution.

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↗

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↗

arXiv2016

Interference stabilization of autoionizing states in molecular $N_2$ studied by time- and angular-resolved photoelectron spectroscopy

An autoionizing resonance in molecular N$_2$ is excited by an ultrashort XUV pulse and probed by a subsequent weak IR pulse, which ionizes the contributing Rydberg states. Time- and angular-resolved photoelectron spectra recorded with a velocity map imaging spectrometer reveal two electronic contributions with different angular distributions. One of them has an exponential decay rate of $20\pm5$ fs, while the other one is shorter than 10 fs. This observation is interpreted as a manifestation of interference stabilization involving the two overlapping discrete Rydberg states. A formalism of interference stabilization for molecular ionization is developed and applied to describe the autoionizing resonance. The results of calculations reveal, that the effect of the interference stabilization is facilitated by rotationally-induced couplings of electronic states with different symmetry.

physics.atom-ph↗