arXiv subjects

Jivesh Kaushal

Publications and source records attributed to Jivesh Kaushal.

9 recordsLinked to original sources

arXiv2025

Unlocking klockmannite: formation of colloidal quasi-2D CuSe nanocrystals and photo-physical properties arising from crystal anisotropy

Copper selenide is an exceptional quasi-layered monolithic material that exhibits both semiconducting and metallic properties in adjacent visible and near-infrared (NIR) spectral ranges. Here we introduce a thiol-free colloidal synthesis for generating quasi-2D klockmannite copper selenide nanocrystals via hot injection method, achieving shape control by tuning the injection temperature and precursor concentrations without any additional ligands. This approach produces large klockmannite nanosheets with lateral sizes from 200 nm to several micrometres, as well as uniform triangular nanoplatelets with sizes of 12-25 nm that are monocrystalline and display strong NIR plasmonic absorption. The spectral features of the anisotropic klockmannite phase in the NIR have been analysed using complex-scaled discrete dipole approximation (CSDDA) calculations, which reveal pronounced optical anisotropy and the emergence of hyperbolic regime. The combined effect of propagating and evanescent fields is regarded as the underlying reason of such modes in the hyperbolic domain. Finally, the ultrafast photophysical behaviour of the material in klockmannite phase is examined, including hot-hole cooling, trapping, and coherent phonons generation. Our findings emphasize the important role of the intrinsic crystal anisotropy in governing the physical properties of nanoscale klockmannite.

cond-mat.mtrl-sci↗

arXiv2025

Multipole expansion for dispersion forces -- watch this trace

Light-matter interaction models invariably rely on the multipole expansion of the electromagnetic potentials generated by complex charge distributions. These multipoles are typically taken to be traceless, however, for a correct evaluation of dispersion forces at all distances, the validity of this assumption has to be checked carefully. Here, we revisit the concept of dispersion forces on an atom near a dielectric surface from the perspective of macroscopic quantum electrodynamics and find that, beyond the quadrupole, the multipoles cannot always be taken as fully traceless. In particular, we show that the trace of the octupole moment contributes to Casimir-Polder interactions beyond the electrostatic regime.

quant-ph↗

arXiv2024

Effects of higher-order Casimir-Polder interactions on Rydberg atom spectroscopy

In the extreme near-field, when the spatial extension of the atomic wavefunction is no longer negligible compared to the atom-surface distance, the dipole approximation is no longer sufficient to describe Casimir-Polder interactions. Here we calculate the higher-order, quadrupole and octupole, contributions to Casimir-Polder energy shifts of Rydberg atoms close to a dielectric surface. We subsequently investigate the effects of these higher-order terms in thin-cell and selective reflection spectroscopy. Beyond its fundamental interest, this new regime of extremely small atom surface separations is relevant for quantum technology applications with Rydberg or surface-bound atoms interfacing with photonic platforms.

physics.atom-ph↗

arXiv2018

Ultrafast Preparation and Detection of Ring Currents in Single Atoms

Quantum particles can penetrate potential barriers by tunneling (1). If that barrier is rotating, the tunneling process is modified (2,3). This is typical for electrons in atoms, molecules or solids exposed to strong circularly polarized laser pulses (4,5). Here we measure how the transmission probability through a rotating tunnel depends on the sign of the magnetic quantum number m of the electron and thus on the initial sense of rotation of its quantum phase. We further show that the electron keeps part of that rotary motion on its way through the tunnel by measuring m-dependent modification of the electron emission pattern. These findings are relevant for attosecond metrology as well as for interpretation of strong field electron emission from atoms and molecules (6-13) and directly demonstrates the creation of ring currents in bound states of ions with attosecond precision. In solids, this could open a way to inducing and controlling ring-current related topological phenomena (14).

physics.atom-ph↗

arXiv2015

Opportunities for detecting ring currents using the attoclock set-up

Strong field ionization by circularly polarized laser fields from initial states with internal orbital momentum has interesting propensity rule: electrons counter-rotating with respect to the laser field can be liberated more easily than co-rotating electrons [Barth and Smirnova PRA 84, 063415, 2011}]. Here we show that application of few-cycle IR pulses allows one to use this propensity rule to detect ring currents associated with such quantum states, by observing angular shifts of the ejected electrons. Such shifts present the main observable of the attoclock method. We use time-dependent Analytical $R$-Matrix (A$R$M) theory to show that the attoclock measured angular shifts of an electron originating from two counter-rotating orbitals ($p^{+}$ and $p^{-}$) are noticeably different. Our work opens new opportunities for detecting ring currents excited in atoms and molecules, using the attoclock set-up.

physics.atom-ph↗

arXiv2015

Spin-Orbit Larmor Clock for Ionisation Times in One-Photon and Strong-Field Regimes

Photoionisation is a process where absorption of one or several photons liberates an electron and creates a hole in a quantum system, such as an atom or a molecule. Is it faster to remove an electron using one or many photons, and how to define this time? Here we introduce a clock that allows us to define ionisation time for both one-photon and many-photon ionisation regimes. The clock uses the interaction of the electron or hole spin with the magnetic field created by their orbital motion, known as the spin-orbit interaction. The angle of spin precession in the magnetic field records time. We use the combination of analytical theory and ab-initio calculations to show how ionisation delay depends on the number of absorbed photons, how it appears in the experiment and what electron dynamics it signifies. In particular, we apply our method to calculate the derived time delays in tunnelling regime of strong-field ionisation.

quant-ph↗

arXiv2015

Interpreting Attoclock Measurements of Tunnelling Times

Resolving in time the dynamics of light absorption by atoms and molecules, and the electronic rearrangement this induces, is among the most challenging goals of attosecond spectroscopy. The attoclock is an elegant approach to this problem, which encodes ionization times in the strong-field regime. However, the accurate reconstruction of these times from experimental data presents a formidable theoretical challenge. Here, we solve this problem by combining analytical theory with ab-initio numerical simulations. We apply our theory to numerical attoclock experiments on the hydrogen atom to extract ionization time delays and analyse their nature. Strong field ionization is often viewed as optical tunnelling through the barrier created by the field and the core potential. We show that, in the hydrogen atom, optical tunnelling is instantaneous. By calibrating the attoclock using the hydrogen atom, our method opens the way to identify possible delays associated with multielectron dynamics during strong-field ionization.

physics.atom-ph↗

arXiv2013

Time-resolving electron-core dynamics during strong field ionization in circularly polarized fields

Electron-core interactions play a key role in strong-field ionization and the formation of photoelectron spectra. We analyse the temporal dynamics of strong field ionization associated with these interactions using the time-dependent analytical R-matrix (ARM) method, developed in our previous work [J. Kaushal and O. Smirnova, Phys. Rev. A 88, 013421 (2013)]. The approach is fully quantum but includes the concept of trajectories. However, the trajectories are not classical in the sense that they have both real and imaginary components all the way to the detector. We show that the imaginary parts of these trajectories, which are usually ignored, have a clear physical meaning and are crucial for the correct description of electron-core interactions after ionization. In particular, they give rise to electron deceleration, as well as dynamics associated with electron recapture and release. Our approach is analytical and time-dependent, and allows one to gain access to the electron energy distribution and ionization yield as a function of time. Thus we can also rigorously answer the question: when is ionization completed?

physics.atom-ph↗

arXiv2013

Non-adiabatic Coulomb effects in strong field ionisation in circularly polarised laser fields

We develop the recently proposed analytical R-matrix (ARM) method to encompass strong field ionisation by circularly polarised fields, for atoms with arbitrary binding potentials. Through ARM, the effect of the potential can now be included consistently both during and after ionisation, providing a complete picture for the effects of the long-range potential. We find that the Coulomb effects modify the ionisation dynamics in several ways, including modification of (i) the ionisation (exit) times, (ii) the initial conditions for the electron continuum dynamics, (iii) the "tunnelling angle", at which the electron "enters" the barrier, and (iv) the electron drift momentum. We derive analytical expressions for the Coulomb-corrected ionisation times, initial velocities, momentum shifts and ionisation rates in circularly polarised fields, for arbitrary angular momentum of the initial state. We also analyse how the non-adiabatic Coulomb effects modify (i) the calibration of the attoclock in the angular streaking method, and (ii) the ratio of ionisation rates from $p^{-}$ and $p^{+}$ orbitals.

physics.atom-ph↗