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Emilio Pisanty

Publications and source records attributed to Emilio Pisanty.

At least 19 recordsLinked to original sources

Geometric Control of Cat States in High Harmonic Generation

High-harmonic generation (HHG) provides a powerful platform for exploring the interaction between intense laser fields and matter on ultrafast timescales. Beyond its conventional description in terms of emitted radiation and electron dynamics, a fully quantum treatment of HHG reveals that the nonlinear light-matter interaction can modify the quantum state of the driving field itself, establishing correlations between the fundamental and harmonic modes. This perspective opens new possibilities for using HHG as a tool to engineer and control nonclassical states of light. In this work, we investigate the geometric properties of optical Schroedinger cat states generated in HHG via conditioning and post-selection. By analyzing the coherent-state displacements induced by different structured driving fields, we characterize the resulting phase-space evolution and the associated geometric phases of the generated quantum states. Particular emphasis is placed on how the polarization and spatial-mode structure of the driving light influence the geometry and evolution of displaced coherent states. Our results demonstrate that structured light offers a versatile means of controlling the geometric dynamics of HHG-generated cat states across the parameter space. Furthermore, we discuss the prospects for realizing genuinely topological optical cat states by exploiting more complex structured light configurations.

physics.optics

2D quantum-path interference in high-harmonic generation driven by highly-bichromatic fields

We experimentally observe a new type of quantum-path interference, in two-dimensions (2D-QPI), in high-harmonic generation (HHG) driven by an orthogonally-polarised highly-bichromatic field. This regime is marked by comparable intensities of the two orthogonal colours. In this highly-bichromatic regime, we demonstrate that 2D-QPI is encoded in the measured harmonic intensity modulations with respect to the relative phase of the two-colour field. The modulations of the odd-order harmonics show a monomodal behaviour, whereas the even harmonics are modulated in a bimodal structure. Our calculations using the strong-field approximation and saddle-point method disentangle contributions from multiple quantum orbits in this HHG regime, revealing that the dipole response for both odd and even harmonics inherits the dynamic symmetry of the orthogonally-polarised driving field. This new type of 2D-QPI offers a novel route to HHG spectroscopy of attosecond electron dynamics by lifting up the dimensionality of the quantum paths involved in the interference.

quant-ph

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

A universal approach to saddle-point methods in attosecond science

Light-matter interactions within the strong-field regime, where intense laser fields can ionise a target via tunnelling, give rise to fascinating phenomena such as the generation of high-order harmonic radiation (HHG). On the atomic scale, these strong-field processes are described in terms of highly-oscillatory time integrals which are often approximated using saddle-point methods. These methods simultaneously simplify the calculations and let us understand the physical processes in terms of semi-classical electron trajectories, or quantum orbits. However, applying saddle-point methods for HHG driven by polychromatic laser fields without clear dynamical symmetries has remained challenging. Here we introduce Picard-Lefschetz theory as a universal and robust link between the time integrals and the semi-classical trajectories. The continuous deformation of the integration contour towards so-called Lefschetz thimbles allows an exact evaluation of the integral, as well as the identification of relevant quantum orbits, for arbitrary driving fields. The latter is realised via the ``necklace algorithm'', a novel solution to the open problem of determining the relevance of saddle points for a two-dimensional integral, which we introduce here. We demonstrate the versatility and rigour of Picard-Lefschetz methods by studying Stokes transitions and spectral caustics arising in HHG driven by two-colour laser fields. For example, we showcase a quantum-orbit analysis of the colour switchover, which links the regime of perturbative two-colour fields with that of fully bichromatic driving fields. With this work, we set the foundation for a rigorous application of quantum-orbit based approaches in attosecond science that enables the interpretation of state-of-the-art experimental setups, and guides the design of future ones.

quant-ph

Quantum tunnelling without a barrier

Tunneling is an iconic concept that captures the peculiarity of quantum dynamics but, despite its ubiquity, questions remain. We focus on strong-field tunneling, which is vital to all attosecond science. We find an unexpected optical tunneling event that happens when the instantaneous electric field vanishes and there is no barrier. This event arises from a color switchover in a strongly polychromatic field. The tunneling without a barrier reveals the disconnect between the standard intuition built on the picture of a quasistatic barrier and the nonadiabatic nature of the process.

quant-ph

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

Topological phase transitions via attosecond x-ray absorption spectroscopy

We present a numerical experiment that demonstrates the possibility to capture topological phase transitions via an x-ray absorption spectroscopy scheme. We consider a Chern insulator whose topological phase is tuned via a second-order hopping. We perform time-dynamics simulations of the out-of-equilibrium laser-driven electron motion that enables us to model a realistic attosecond spectroscopy scheme. In particular, we use an ultrafast scheme with a circularly polarized IR pump pulse and an attosecond x-ray probe pulse. A laser-induced dichroism-type spectrum shows a clear signature of the topological phase transition. We are able to connect these signatures with the Berry structure of the system. This work extend the applications of attosecond absorption spectroscopy to systems presenting a non-trivial topological phase.

physics.optics

Nonclassical states of light after high-harmonic generation in semiconductors: a Bloch-based perspective

High-harmonic generation has emerged as a pivotal process in strong-field physics, yielding extreme ultraviolet radiation and attosecond pulses with a wide range of applications. Furthermore, its emergent connection with the field of quantum optics has revealed its potential for generating non-classical states of light. Here, we investigate the process of high-harmonic generation in semiconductors under a quantum optical perspective while using a Bloch-based solid-state description. Through the implementation of quantum operations based on the measurement of high-order harmonics, we demonstrate the generation of non-classical light states similar to those found when driving atomic systems. These states are characterized using diverse quantum optical observables and quantum information measures, showing the influence of electron dynamics on their properties. Additionally, we analyze the dependence of their features on solid characteristics such as the dephasing time and crystal orientation, while also assessing their sensitivity to changes in driving field strength. This study provides insights into HHG in semiconductors and its potential for generating non-classical light sources.

quant-ph

Entanglement and non-classical states of light in a strong-laser driven solid-state system

The development of sources delivering non-classical states of light is one of the main needs for applications of optical quantum information science. Here, we demonstrate the generation of non-classical states of light using strong-laser fields driving a solid-state system, by using the process of high-order harmonic generation, where an electron tunnels out of the parent site and, later on, recombines on it emitting high-order harmonic radiation, at the expense of affecting the driving laser field. Since in solid-state systems the recombination of the electron can be delocalized along the material, the final state of the electron determines how the electromagnetic field gets affected because of the laser-matter interaction, leading to the generation of entanglement between the electron and the field. These features can be enhanced by applying conditioning operations, i.e., quantum operations based on the measurement of high-harmonic radiation. We study non-classical features present in the final quantum optical state, and characterize the amount of entanglement between the light and the electrons in the solid. The work sets the foundation for the development of compact solid-state-based non-classical light sources using strong-field physics.

quant-ph

Strong laser physics, non-classical light states and quantum information science

Strong laser physics is a research direction that relies on the use of high-power lasers and has led to fascinating achievements ranging from relativistic particle acceleration to attosecond science. On the other hand, quantum optics has been built on the use of low photon number sources and has opened the way for groundbreaking discoveries in quantum technology, advancing investigations ranging from fundamental tests of quantum theory to quantum information processing. Despite the tremendous progress, until recently these directions have remained disconnected. This is because, the majority of the interactions in the strong-field limit have been successfully described by semi-classical approximations treating the electromagnetic field classically, as there was no need to include the quantum properties of the field to explain the observations. The link between strong laser physics, quantum optics, and quantum information science has been developed in the recent past. Studies based on fully quantized and conditioning approaches have shown that intense laser--matter interactions can be used for the generation of controllable entangled and non-classical light states. This achievement opens the way for a vast number of investigations stemming from the symbiosis of strong laser physics, quantum optics, and quantum information science. Here, after an introduction to the fundamentals of these research directions, we report on the recent progress in the fully quantized description of intense laser--matter interaction and the methods that have been developed for the generation of non-classical light states and entangled states. Also, we discuss the future directions of non-classical light engineering using strong laser fields, and the potential applications in ultrafast and quantum information science.

quant-ph

Strong laser fields and their power to generate controllable high-photon-number coherent-state superpositions

Recently, intensely driven laser-matter interactions have been used to connect the fields of strong laser field physics with quantum optics by generating non-classical states of light. Here, we make a further key step and show the potential of strong laser fields for generating controllable high-photon-number coherent-state superpositions. This has been achieved by using two of the most prominent strong-laser induced processes: high-harmonic generation and above-threshold ionization. We show how the obtained coherent-state superpositions change from an optical Schrödinger "cat" state to a "kitten" state by changing the atomic density in the laser-atom interaction region, and we demonstrate the generation of a 9-photon shifted optical "cat" state which, to our knowledge, is the highest photon number optical "cat" state experimentally reported. Our findings anticipate the development of new methods that naturally lead to the creation of high-photon-number controllable coherent-state superpositions, advancing investigations in quantum technology.

quant-ph

Conservation of a Half-Integer Angular Momentum in Nonlinear Optics with a Polarization Möbius Strip

Symmetries and conservation laws of energy, linear momentum and angular momentum play a central role in physics, in particular in nonlinear optics. Recently, light fields with non trivial topology, such as polarization Möbius strips or torus-knot beams, have been unveiled. They cannot be associated to well-defined values of orbital and spin angular momenta (OAM and SAM), but are invariant under coordinated rotations, i.e. rotational symmetries that are generated by the generalized angular momentum (GAM) operator, a mixture of the OAM and SAM operators. The discovery of the GAM, which at variance with integer-valued OAM and SAM, can have arbitrary value, and raises the question of its conservation in nonlinear optical processes. By driving high harmonic generation with a polarization Möbius strip and implementing novel OAM characterization methods in the XUV range, we experimentally observe the conservation of the GAM, each harmonic carrying a precise half-integer GAM charge equal to that of the fundamental field multiplied by the harmonic order. The GAM is thus revealed as the appropriate quantum number to describe nonlinear processes driven by light fields containing topological polarization singularities.

physics.optics

Optical polarization skyrmionic fields in free space

We construct optical beams in free space with robust skyrmionic structures in their polarization fields, both in the electric spin vector for near-circular fields and in the polarization direction for near-linear fields, and for both Bloch (spiral) and Néel (hedgehog) textures. These structures are made possible by the spin-orbit coupling of tightly-focused nonparaxial optics as applied to higher-order Full-Poincaré beams, as well as by standing-wave configurations comprising forwards- and backwards-propagating waves. Our constructions show near-uniform circular and linear polarizations, providing a high degree of topological protection in the absence of nonlinear interactions.

physics.optics

A systematic construction of Gaussian basis sets for the description of laser field ionization and high-harmonic generation

A precise understanding of mechanisms governing the dynamics of electrons in atoms and molecules subjected to intense laser fields has a key importance for the description of attosecond processes such as the high-harmonic generation and ionization. From the theoretical point of view, this is still a challenging task, as new approaches to solve the time-dependent Schrödinger equation with both good accuracy and efficiency are still emerging. Until recently, the purely numerical methods of real-time propagation of the wavefunction using finite grids have been frequently and successfully used to capture the electron dynamics in small one- or two-electron systems. However, as the main focus of attoscience shifts toward many-electron systems, such techniques are no longer effective and need to be replaced by more approximate but computationally efficient ones. In this paper, we explore the increasingly popular method of expanding the wavefunction of the examined system into a linear combination of atomic orbitals and present a novel systematic scheme for constructing an optimal Gaussian basis set suitable for the description of excited and continuum atomic or molecular states. We analyze the performance of the proposed basis sets by carrying out a series of time-dependent configuration interaction calculations for the hydrogen atom in fields of intensity varying from $5 \times 10^{13}\:\rm W/cm^2$ to $5 \times 10^{14}\:\rm W/cm^2$. We also compare the results with the data obtained using Gaussian basis sets proposed previously by other authors.

physics.chem-ph

High photon number entangled states and coherent state superposition from the extreme-ultraviolet to the far infrared

We present a theoretical demonstration on the generation of entangled coherent states and of coherent state superpositions, with photon numbers and frequencies orders of magnitude higher than those provided by the current technology. This is achieved by utilizing a quantum mechanical multimode description of the single- and two-color intense laser field driven process of high harmonic generation in atoms. It is found that all field modes involved in the high harmonic generation process are entangled, and upon performing a quantum operation, leads to the generation of high photon number optical cat states spanning from the far infrared to the extreme-ultraviolet spectral region. This provides direct insights into the quantum mechanical properties of the optical field in intense laser matter interaction. Finally, these states can be considered as a new resource for fundamental tests of quantum theory, quantum information processing or sensing with non-classical states of light.

quant-ph

Generation of optical Schrödinger cat states in intense laser-matter interactions

The physics of intense laser-matter interactions is described by treating the light pulses classically, anticipating no need to access optical measurements beyond the classical limit. However, the quantum nature of the electromagnetic fields is always present. Here, we demonstrate that intense laser-atom interactions may lead to the generation of highly non-classical light states. This was achieved by using the process of high-harmonic generation in atoms, in which the photons of a driving laser pulse of infrared frequency are up-converted into photons of higher frequencies in the extreme ultraviolet spectral range. The quantum state of the fundamental mode after the interaction, when conditioned on the high-harmonic generation, is a so-called Schrödinger cat state, which corresponds to a superposition of two distinct coherent states: the initial state of the laser and the coherent state reduced in amplitude that results from the interaction with atoms. The results open the path for investigations towards the control of the non-classical states, exploiting conditioning approaches on physical processes relevant to high-harmonic generation.

physics.optics

Enantiosensitive steering of free-induction decay

Chiral discrimination, a problem of vital importance, has recently become an emerging frontier in ultrafast physics, with remarkable progress achieved in multiphoton and strong-field regimes. Rydberg excitations, unavoidable in the strong-field regime and intentional for few-photon processes, arise in all these approaches. Here we show how to harness this ubiquitous feature by introducing a new phenomenon, enantiosensitive free-induction decay, steered by a tricolour chiral field at a gentle intensity, structured in space and time. We demonstrate theoretically that an excited chiral molecule accumulates an enantiosensitive phase due to perturbative interactions with the tricolour chiral field, resulting in a spatial phase gradient steering the free-induction decay in opposite directions for opposite enantiomers. Our work introduces a general, extremely sensitive, all-optical, enantiosensitive detection technique which avoids strong fields and takes full advantage of recent advances in structuring light.

physics.optics

Dialogue on analytical and ab initio methods in attoscience

The perceived dichotomy between analytical and ab initio approaches to theory in attosecond science is often seen as a source of tension and misconceptions. This Topical Review compiles the discussions held during a round-table panel at the 'Quantum Battles in Attoscience' CECAM virtual workshop, to explore the sources of tension and attempt to dispel them. We survey the main theoretical tools of attoscience -- covering both analytical and numerical methods -- and we examine common misconceptions, including the relationship between ab initio approaches and the broader numerical methods, as well as the role of numerical methods in 'analytical' techniques. We also evaluate the relative advantages and disadvantages of analytical as well as numerical and ab initio methods, together with their role in scientific discovery, told through the case studies of two representative attosecond processes: non-sequential double ionisation and resonant high-harmonic generation. We present the discussion in the form of a dialogue between two hypothetical theoreticians, a numericist and an analytician, who introduce and challenge the broader opinions expressed in the attoscience community.

quant-ph