arXiv subjects

Gopal Dixit

Publications and source records attributed to Gopal Dixit.

At least 37 records · Page 2Linked to original sources

arXiv2022

Probing phonon-driven symmetry alterations in graphene via high-harmonic spectroscopy

High-harmonic spectroscopy has become an essential ingredient in probing various ultrafast electronic processes in solids with sub-cycle temporal resolution. Despite its immense importance, sensitivity of high-harmonic spectroscopy to phonon dynamics in solids is not well known. This work addresses this critical question and demonstrates the potential of high-harmonic spectroscopy in probing intertwined phonon-electron dynamics in solids. A pump pulse excites in-plane optical phonon modes in monolayer graphene and a circularly polarised pulse is employed to probe the excited phonon dynamics that generates higher-order harmonics. We show that the coherent phonon dynamics alters the dynamical symmetry of graphene with the probe pulse and leads the generations of the symmetry-forbidden harmonics. Moreover, sidebands associated with the prominent harmonic peaks are generated as a result of the coherent dynamics. It is found that the symmetries and the characteristic timescale of the excited phonon mode determine the polarisation and positions of these sidebands. Present work opens an avenue in time-resolved probing of phonon-driven processes and dynamical symmetries in solids with sub-cycle temporal resolution.

physics.optics↗

arXiv2022

High-Harmonic Spectroscopy of Coherent Lattice Dynamics in Graphene

High-harmonic spectroscopy of solids is a powerful tool, which provides access to both electronic structure and ultrafast electronic response of solids, from their band structure and density of states, to phase transitions, including the emergence of the topological edge states, to the PetaHertz electronic response. However, in spite of these successes, high harmonic spectroscopy has hardly been applied to analyse the role of coherent femtosecond lattice vibrations in the attosecond electronic response. Here we study coherent phonon excitations in monolayer graphene to show how high-harmonic spectroscopy can be used to detect the influence of coherent lattice dynamics, particularly longitudinal and transverse optical phonon modes, on the electronic response. Coherent excitation of the in-plane phonon modes results in the appearance of sidebands in the spectrum of the emitted harmonic radiation. We show that the spectral positions and the polarisation of the sideband emission offer a sensitive probe of the dynamical symmetries associated with the excited phonon modes. Our work brings the key advantage of high harmonic spectroscopy -- the combination of sub-femtosecond to tens of femtoseconds temporal resolution -- to the problem of probing phonon-driven electronic response and its dependence on the dynamical symmetries in solids.

physics.optics↗

arXiv2021

Controlling Valley-Polarisation in Graphene via Tailored Light Pulses

Analogous to charge and spin, electrons in solids endows an additional degree of freedom: the valley pseudospin. Two-dimensional hexagonal materials such as graphene exhibit two valleys, labelled as $\mathbf{K}$ and $\mathbf{K}^{\prime}$. These two valleys have the potential to realise logical operations in two-dimensional materials. Obtaining the desired control over valley polarisation between the two valleys is a prerequisite for the logical operations. Recently, it was shown that two counter-rotating circularly polarised laser pulses can induce a significant valley-polarisation in graphene. The main focus of the present work is to optimise the valley polarisation in monolayer graphene by controlling different laser parameters, such as wavelength, intensity ratio, frequency ratio and sub-cycle phase in two counter-rotating circularly polarised laser setup. Moreover, an alternate approach, based on single or few-cycle linearly polarised laser pulse, is also explored to induce significant valley polarisation in graphene. Our work could help experimentalists to choose a suitable method with optimised parameter space to obtain the desired control over valley polarisation in monolayer graphene.

cond-mat.mes-hall↗

arXiv2021

Imaging charge-migration in chiral molecules using time-resolved x-ray diffraction

Four-dimensional imaging of charge migration is crucial to the understanding of several ubiquitous processes in nature. The present work focuses on imaging of charge migration in an oriented epoxypropane: a chiral molecule. A linearly polarized pulse is used to induce the charge migration, which is imaged by time-resolved x-ray diffraction. It is found that the total time-resolved diffraction signals are significantly different for both enantiomers. Furthermore, a connection between time-resolved x-ray diffraction and the electronic continuity equation is discussed by analyzing the time-dependent diffraction signal and the time derivative of the total electron density in the momentum space.

physics.chem-ph↗

arXiv2021

High-Harmonic Generation from Monolayer and Bilayer Graphene

High-harmonic generation (HHG) in solids is an emerging method to probe ultrafast electron dynamics in solids at attosecond timescale. In this work, we study HHG from monolayer and bilayer graphene. Bilayer graphenes with AA and AB stacking are considered in this work. It is found that the monolayer and bilayer graphenes exhibit significantly different harmonic spectra. The difference in the spectra is attributed to the interlayer coupling between the two layers. Also, the intraband and interband contributions to the total harmonic spectrum play a significant role. Moreover, interesting polarization and ellipticity dependence are noticed in total harmonic spectrum for monolayer and bilayer graphene.

physics.optics↗

arXiv2021

Light-Induced Valleytronics in Pristine Graphene

Electrons in two-dimensional hexagonal materials have valley degree of freedom, which can be used to encode and process quantum information. The valley-selective excitations, governed by the circularly polarised light resonant with the material's band-gap, continues to be the foundation of valleytronics. It is often assumed that achieving valley selective excitation in pristine graphene with all-optical means is not possible due to the inversion symmetry of the system. Here we demonstrate that both valley-selective excitation and valley-selective high-harmonic generation can be achieved in pristine graphene by using the combination of two counter-rotating circularly polarized fields, the fundamental and its second harmonic. Controlling the relative phase between the two colours allows us to select the valleys where the electron-hole pairs and higher-order harmonics are generated. We also describe an all-optical method for measuring valley polarization in graphene with a weak probe pulse. This work offers a robust recipe to write and read valley-selective electron excitations in materials with zero bandgap and zero Berry curvature.

cond-mat.mes-hall↗

arXiv2021

High harmonic spectroscopy of disorder-induced Anderson localization

Exponential localization of wavefunctions in lattices, whether in real or synthetic dimensions, is a fundamental wave interference phenomenon. Localization of Bloch-type functions in space-periodic lattice, triggered by spatial disorder, is known as Anderson localization and arrests diffusion of classical particles in disordered potentials. In time-periodic Floquet lattices, exponential localization in a periodically driven quantum system similarly arrests diffusion of its classically chaotic counterpart in the action-angle space. Here we demonstrate that nonlinear optical response allows for clear detection of the disorder-induced phase transition between delocalized and localized states. The optical signature of the transition is the emergence of symmetry-forbidden even-order harmonics: these harmonics are enabled by Anderson-type localization and arise for sufficiently strong disorder even when the overall charge distribution in the field-free system spatially symmetric. The ratio of even to odd harmonic intensities as a function of disorder maps out the phase transition even when the associated changes in the band structure are negligibly small.

cond-mat.dis-nn↗

arXiv2021

Four-Dimensional Imaging of Lattice Dynamics using Inelastic Scattering

Time-resolved mapping of lattice dynamics in real- and momentum-space is essential to understand better several ubiquitous phenomena such as heat transport, displacive phase transition, thermal conductivity, and many more. In this regard, time-resolved diffraction and microscopy methods are employed to image the induced lattice dynamics within a pump-probe configuration. In this work, we demonstrate that inelastic scattering methods, with the aid of theoretical simulation, are competent to provide similar information as one could obtain from the time-resolved diffraction and imaging measurements. To illustrate the robustness of the proposed method, our simulated result of lattice dynamics in germanium is in excellent agreement with the time-resolved x-ray diffuse scattering measurement performed using x-ray free-electron laser. For a given inelastic scattering data in energy and momentum space, the proposed method is useful to image in-situ lattice dynamics under different environmental conditions of temperature, pressure, and magnetic field. Moreover, the technique will profoundly impact where time-resolved diffraction within the pump-probe setup is not feasible, for instance, in inelastic neutron scattering.

cond-mat.str-el↗

arXiv2020

Controlling polarization of attosecond pulses with plasmonic-enhanced bichromatic counter-rotating circularly polarised fields

The use of bichromatic counter-rotating laser field is known to generate high-order harmonics with non-zero ellipticity. By combining such laser field with a plasmonic-enhanced spatially inhomogeneous field, we propose a way to influence the sub-cycle dynamics of the high-harmonic generation process. Using the numerical solution of the time-dependent Schr{ö}dinger equation combined with classical trajectory Monte Carlo simulations, we show that the change of the direction and the strength of the plasmonic field selectively enhances or suppresses certain recombining electron trajectories. This in turn modifies the ellipticity of the emitted attosecond pulses.

physics.atom-ph↗

arXiv2020

Angle-Resolved Attosecond Streaking of Twisted Attosecond Pulses

The present work focuses on the characterisation of the amount of orbital angular momentum (OAM) encoded in the twisted attosecond pulses via energy- and angle-resolved attosecond streaking in pump-probe setup. It is found that the photoelectron spectra generated by the linearly polarised twisted pulse with different OAM values exhibit angular modulations, whereas circularly polarised twisted pulse yields angular isotropic spectra. It is demonstrated that the energy- and angle-resolved streaking spectra are sensitive to the OAM values of the twisted pulse. Moreover, the different combinations of the polarisation of the twisted pump pulse and strong infrared probe pulse influence the streaking spectra differently. The characterisation of the OAM carrying twisted attosecond pulses opens up the possibility to explore helical light-matter interaction on attosecond timescale.

physics.atom-ph↗

arXiv2020

Signatures of the orbital angular momentum of an infrared light beam in the two-photon transition matrix element: A step toward attosecond chronoscopy of photoionization

We present a theory of time-resolved photoionisation in the presence of a vortex beam. In a pump-probe setup, an extreme ultraviolet or an x-ray pump pulse triggers ionization, which is probed by a synchronized infrared pulse with non-zero orbital angular momentum. We show, how this property of the probe pulse affects the electron dynamics upon ionization, in a way that is independent of the initial and final angular momentum states of the ionizing system.

physics.atom-ph↗

arXiv2020

High-Harmonic generation from spin-polarised defects in solids

Generation of high-order harmonics in gases enabled to probe the attosecond electron dynamics in atoms and molecules with unprecedented resolution. Extending the techniques developed originally for atomic and molecular gases to solid state materials requires a fundamental understanding of the physics that has been partially addressed theoretically. Here we employ time-dependent density-functional theory to investigate how the electron dynamics resulting in high-harmonic emission in monolayer hexagonal boron nitride is affected by the presence of vacancies. We show how these realistic spin-polarised defects modify the harmonic emission, and demonstrate that important differences exist between harmonics from a pristine solid and a defected-solid. In particular, we found that the different spin channels are affected differently because of the presence of the spin-polarized point defect, and that localisation of the wavefunction, the geometry of the defect and the electron-electron interaction are all important ingredients to describe high-harmonic generation in defected-solids. We show that different vacancies lead to qualitatively different effects, thus opening the door to the high-harmonic imaging of spin-polarised defects in solids.

physics.optics↗

arXiv2020

Probing Electronic Fluxes via Time-Resolved X-ray Scattering

The current flux density is a vector field that can be used to describe theoretically how electrons flow in a system out-of-equilibrium. In this work, we unequivocally demonstrate that the signal obtained from time-resolved X-ray scattering does not only map the time-evolution of the electronic charge distribution, but also encodes information about the associated electronic current flux density. We show how the electronic current flux density qualitatively maps the distribution of electronic momenta and reveals the underlying mechanism of ultrafast charge migration processes, while also providing quantitative information about the timescales of electronic coherences.

physics.atom-ph↗

arXiv2020

Influence of vacancy defects in solid high-order harmonic generation

The present work discusses the impact of vacancy defects in solid high-order harmonic generation. The total energy cutoff of the high-order harmonic spectrum increases as a function of concentration of vacancy defects, and the total spectrum gradually turns into a single slanted spectrum without having an abrupt transition between primary and secondary plateaus. The spectral intensity of the below-band-gap harmonics in a solid with vacancy defects is enhanced significantly in comparison to the harmonics in a pristine solid. The changes in the harmonic spectra are understood in terms of their effective band structures. The presence of vacancy defects breaks the translational symmetry of the unit cell locally. As a consequence of this, new defect states appear, which open additional paths for the electron dynamics. The ill-resolved electron trajectories in the Gabor profile confirm the interference of additional paths. Moreover, the single slanted high-order harmonic spectrum carries a unique signature of vacancy defects in comparison to the high-order harmonic spectrum corresponding to solids with defects such as underdoping or overdoping.

physics.optics↗

arXiv2019

Direct Numerical Observation of Real-Space Recollision in High-Harmonic Generation from Solids

Real-space picture of electron recollision with the parent ion guides our understanding of the highly nonlinear response of atoms and molecules to intense low-frequency laser fields. It is also among several leading contestants for the dominant mechanism of high harmonic generation (HHG) in solids, where it is typically viewed in the momentum space, as the recombination of the conduction band electron with the valence band hole, competing with another HHG mechanism, the strong-field driven Bloch oscillations. In this work, we use numerical simulations to directly test and confirm the real-space recollision picture as the key mechanism of HHG in solids. Our tests take advantage of the well-known characteristic features in the molecular harmonic spectra, associated with the real-space structure of the molecular ion. We show the emergence of analogous spectral features when similar real-space structures are present in the periodic potential of the solid-state lattice. This work demonstrates the capability of HHG imaging of spatial structures of a unit cell in solids.

physics.optics↗

arXiv2019

Probing molecular chirality via laser-induced electronic fluxes

Chirality is ubiquitous in nature and of fundamental importance in science. The present work focuses on understanding the conditions required to modify the chirality during ultrafast electronic motion by bringing enantiomers out-of-equilibrium. Different kinds of ultrashort linearly-polarised laser pulses are used to drive an ultrafast charge migration process by the excitation of a small number of low-lying excited states from the ground electronic state of S- and R-epoxypropane. Control over chiral electron dynamics is achieved by choosing the different orientations of the linearly polarised pulse. We find that chirality breaking electric fields are only possible in oriented molecules, and that charge migration remains chiral when the polarisation of the field lies in the mirror plane defining the enantiomer pair, or when it is strictly perpendicular to it. Ultimately, the presence or the absence of a mirror symmetry for the enantiomer pair in the external field determines the chiral properties of the charge migration process.

physics.chem-ph↗

arXiv2018

Simultaneous control of harmonic yield and energy cutoff of high-harmonic generation using seeded plasmonic-enhanced fields

We study high-order harmonic generation (HHG) driven by seeded plasmonic-enhanced fields. On one hand, plasmonic-enhanced fields have shown a great potential to extend the HHG cutoff, an instrumental pre-requisite for the generation of attosecond pulses. On another hand, the use of XUV seeds appears to have a considerable potential to improve the HHG conversion efficiency, which is typically modest when a unique fundamental laser pulse is employed. By mixing these two sources, we show it is possible to, simultaneously, boost the HHG cutoff and to increase the harmonic photon flux. The combination of these features potentially enables to generate intense and spectrally broad attosecond pulse trains.

physics.atom-ph↗

arXiv2018

Control of helicity of high-harmonic radiation using bichromatic circularly polarized laser fields

High-harmonic generation in two-colour ($ω-2ω$) counter-rotating circularly polarised laser fields opens the path to generate isolated attosecond pulses and attosecond pulse trains with controlled ellipticity. The generated harmonics have alternating helicity, and the ellipticity of the generated attosecond pulse depends sensitively on the relative intensities of two adjacent, counter-rotating harmonic lines. For the $s$-type ground state, such as in Helium, the successive harmonics have nearly equal amplitude, yielding isolated attosecond pulses and attosecond pulse trains with linear polarisation, rotated by 120$^{\circ}$ from pulse to pulse. In this work, we suggest a solution to overcome the limitation associated with the $s$-type ground state. It is based on modifying the three propensity rules associated with the three steps of the harmonic generation process: ionisation, propagation, and recombination. We control the first step by seeding high harmonic generation with XUV light tuned well below the ionisation threshold, which generates virtual excitations with the angular momentum co-rotating with the $ω$-field. We control the propagation step by increasing the intensity of the $ω$-field relative to the $2ω$-field, further enhancing the chance of the $ω$-field being absorbed versus the $2ω$-field, thus favouring the emission co-rotating with the seed and the $ω-$field. We demonstrate our proposed control scheme using Helium atom as a target and solving time-dependent Schr{ö}dinger equation in two and three-dimensions.

physics.optics↗