arXiv subjects

Himadri S. Chakraborty

Publications and source records attributed to Himadri S. Chakraborty.

31 records · Page 2Linked to original sources

arXiv2016

Effects of exchange-correlation potentials on the density functional description of C_60 versus C_240 photoionization

We study the photoionization properties of the C_60 versus C_240 molecule in a spherical jellium frame of density functional method. Two different approximations to the exchange-correlation (xc) functional are used: (i) The Gunnerson-Lundqvist parametrization [Phys. Rev. B 13, 4274 (1976)] with an explicit correction for the electron self-interaction (SIC) and (ii) a gradient-dependent augmentation of (i) by using the van Leeuwen and Baerends model potential [Phys. Rev. A 49, 2421 (1994)], in lieu of SIC, to implicitly restore electrons' asymptotic properties. Ground state results from the two schemes for both molecules show differences in the shapes of mean-field potentials and bound-level properties. The choice of a xc scheme also significantly alters the dipole single-photoionization cross sections obtained by an abinitio method that incorporates linear-response dynamical correlations. Differences in the structures and ionization responses between C_60 and C_240 uncover the effect of molecular size on the underlying physics. Analysis indicates that the collective plasmon resonances with the gradient-based xc-option produce results noticeably closer to the experimental data available for C_60.

physics.atm-clus↗

arXiv2016

Attosecond delay of xenon $4d$ photoionization at the giant resonance and Cooper minimum

A Kohn-Sham time-dependent local-density-functional scheme is utilized to predict attosecond time delays of xenon 4d photoionization that involves the 4d giant dipole resonance and Cooper minimum. The fundamental effect of electron correlations to uniquely determine the delay at both regions is demonstrated. In particular, for the giant dipole resonance, the delay underpins strong collective effect, emulating the recent prediction at C60 giant plasmon resonance [T. Barillot et al, Phys. Rev. A 91, 033413 (2015)]. For the Cooper minimum, a qualitative similarity with a photorecombination experiment near argon 3p minimum [S. B. Schoun et al, Phys. Rev. Lett. 112, 153001 (2014)] is found. The result should encourage attosecond measurements of Xe 4d photoemission.

physics.atom-ph↗

arXiv2015

Coherence of Auger and inter-Coulombic decay processes in the photoionization of Ar@C60 versus Kr@C60

For the asymmetric spherical dimer of an endohedrally confined atom and a host fullerene, an innershell vacancy of either system can decay through the continuum of an outer electron hybridized between the systems. Such decays, viewed as coherent superpositions of the single-center Auger and two-center inter-Coulombic (ICD) amplitudes, are found to govern leading decay mechanisms in noble-gas endofullerenes, and are likely omnipresent in this class of nanomolecules. A comparison between resulting autoionizing resonances calculated in the photoionization of Ar@C60 and Kr@C60 exhibits details of the underlying processes.

physics.atm-clus↗

arXiv2015

Attosecond time delay in valence photoionization and photorecombination of argon: a TDLDA study

We determine and analyze the quantum phases and time delays in photoionization and photorecombination of valence 3p and 3s electrons of argon using the Kohn-Sham local density functional approach. The time-dependent local density approximation (TDLDA) is used to account for the electron correlation. Resulting attosecond Wigner-Smith time delays show excellent agreements with two recent independent experiments on argon that measured the relative 3s-3p time delay in photoionization [Physical Review Letters {\bf 106}, 143002 (2011)] and the delay in 3p photorecombination [Physical Review Letters {\bf 112}, 153002 (2014)]

physics.atom-ph↗

arXiv2015

Fullerene photoemission time delay explores molecular cavity in attoseconds

Photoelectron spectroscopy earlier probed oscillations in C60 valence emissions, producing series of minima whose energy separation depends on the molecular cavity. We show here that the quantum phase at these cavity minima exhibits variations from strong electron correlations in C60, causing rich structures in the emission time delay. Hence, these minima offer unique spectral zones to directly explore multielectron forces via attosecond RABITT interferometry not only in fullerenes, but also in clusters and nanostructures for which such minima are likely abundant.

physics.atm-clus↗

arXiv2014

Photoionization of bonding and antibonding-type atom-fullerene hybrid states in Cd@C$_{60}$ vs Zn@C$_{60}$60

Powerful hybridization of the Cd 4$d$ state with the $d$-angular momentum state of C$_{60}$ $π$ symmetry is found in the local density approximation (LDA) structure of Cd@C$_{60}$ ground state. The photoionization of the resulting symmetric and antisymmetric levels are computed using the time dependent LDA method to include electron correlations. Cross sections exhibit effects of the C$_{60}$ plasmonic motion coherently coupled to the diffraction-type cavity oscillations induced by local emissions from C$_{60}$. The Cd@C$_{60}$ results exhibit a substantial difference from our previous results for Zn@C$_{60}$.

physics.atm-clus↗

arXiv2013

Resonant Auger-intercoulombic hybridized decay in the photoionization of endohedral fullerenes

Considering the photoionization of Ar@C60, we predict resonant femtosecond decays of both Ar and C60 vacancies through the continua of atom-fullerene hybrid final states. The resulting resonances emerge from the interference between simultaneous autoionizing and intercoulombic decay (ICD) processes. For Ar 3s-->np excitations, these resonances are far stronger than the Ar-to-C60 resonant ICDs, while for C60 excitations they are strikingly larger than the corresponding Auger features. The results indicate the power of hybridization to enhance decay rates, and modify lifetimes and line profiles.

physics.atm-clus↗

arXiv2013

Time delay in the recoiling valence-photoemission of Ar endohedrally confined in C$_{60}$

Effects of confinement and electron correlations on the relative time delay between the 3s and 3p photoemissions of Ar confined endohedrally in C$_{60}$ are investigated using the time dependent local density approximation - a method that is also found to mostly agree with recent time delay measurements between the 3s and 3p subshells in atomic Ar. At energies in the neighborhood of 3p Cooper minimum, correlations with C$_{60}$ electrons are found to induce opposite temporal effects in the emission of Ar 3p hybridized symmetrically versus that of Ar 3p hybridized antisymmetrically with C$_{60}$. A recoil-type interaction model mediated by the confinement is found to best describe the phenomenon.

physics.atom-ph↗

arXiv2003

Evidence for parallel confinement in resonant charge transfer of negative hydrogen ion near metal surfaces

Using a wave packet propagation approach, we find that the resonant charge transfer process of H^- near a Cu(111) surface is strongly influenced by transient hybrid states. These states originate from an ion-induced confinement parallel to the surface together with the surface-localization character of the metal potential along the surface normal. The lowest members of these states have lifetimes of the order of interaction times in typical particle-surface scattering experiments. The propagation of the electron probability density provides clear evidence for this effect in visualizing the evolution and the decay of these transient states.

physics.atom-ph↗

arXiv2003

Interchannel coupling effects in the spin polarization of energetic photoelectrons

Effects of the interchannel coupling on the spin polarization of energetic photoelectrons emitted from atomic Ne valence subshells are examined. Like previously obtained results for cross sections and angular distributions, the photoelectron spin polarization parameters too are found considerably influenced by the coupling. The result completes a series of studies to finally conclude that the independent particle description is inadequate for the {\em entire} range of photoionization dynamics over the {\em full} spectral energy domain

physics.atom-ph↗

arXiv2001

Oscillations in the photocurrent from quantum dots: Geometric information from reciprocal spectra

We demonstrate that the current of photoelectrons from a quantum dot exhibits oscillations as a function of the photon energy owing to the predominant ionization from the dot boundary. In the Fourier reciprocal space of the photoelectron wave vector these oscillations reveal frequencies connected to the confinement range. We attribute the oscillation in the recent photocurrent measurements by Fry et al. (PRL 84, 733 (2000)) to this phenomenon. Angle-resolved and angle-integrated experiments with the focus on directly imaging the confining potential are suggested.

cond-mat.mes-hall↗

arXiv2001

Energetic photoionization of neutral and ionic metal clusters

We show, with an example of Na_92, that for jellium metal clusters the interference of fast electron-waves emitted from equivalent sites on the cluster edge produces monochromatic oscillations in all photoionization observables as a function of the photoelectron momentum; the effect is equivalent to the usual dispersion phenomenon. In dealing with formalisms, a serious consequence of the inadequacy of self-interaction corrected local density-functional theory in correctly accounting for the exchange interaction is identified. We also briefly discuss the influence of the ionicity of the residual core on photospectra by considering the neutral member with N=58 and and the ionic member with N=52 of the Na_58 iso-jellium series, where N is the number of valence electrons. A few final remarks on possible implications of these results on other quantum systems of delocalized electrons are made.

physics.atom-ph↗

arXiv2001

Spurious oscillations from local self-interaction correction in high energy photoionization calculations for metal clusters

We find that for simple metal clusters a single-electron description of the ground state employing self-interaction correction (SIC) in the framework of local-density approximation strongly contaminates the high energy photoionization cross sections with spurious oscillations for a subshell containing node(s). This effect is shown connected to the unphysical structure that SIC generates in ensuing state-dependent radial potentials around a position where the respective orbital density attains nodal zero. Non-local Hartree-Fock that exactly eliminates the electron self-interaction is found entirely free from this effect. It is inferred that while SIC is largely unimportant in high photon-energies, any implementation of it within the local frame can induce unphysical oscillations in the high energy photospectra of metal clusters pointing to a general need for caution in choosing appropriate theoretical tools.

physics.atm-clus↗