arXiv subjects

Rupali Jindal

Publications and source records attributed to Rupali Jindal.

5 recordsLinked to original sources

arXiv2026

Correlated-Electron Theory of Triplet-Triplet Multiexciton States in Polypentacene

We present correlated-electron calculations of optical spin-singlet and triplet-triplet multiexciton states in three- and four-unit pentacene oligomers as microscopic models for polypentacene. The calculations use the Pariser-Parr-Pople Hamiltonian, multiple-reference singles and doubles configuration interaction, and a molecular exciton basis that resolves Frenkel, charge-transfer, and triplet-pair (T1T1) configurations in real space. We find that the complete set of 1(T1T1) eigenstates lies in a narrow, nearly degenerate energy window near the lowest optical exciton and that no eigenstate can be identified with a single localized triplet-pair configuration. Instead, each triplet-pair eigenstate is a quantum superposition of configurations containing all accessible intertriplet separations. This electronic structure explains the perceived absence of intramolecular triplet diffusion in pentacene oligomers, polypentacene, and polytetracene solutions, while leaving open the possibility of intermolecular singlet fission in films with appreciable interchain interactions.

cond-mat.mtrl-sci↗

arXiv2025

Comment on "Superconductivity and Mott Physics in Organic Charge Transfer Materials"

Menke et al. recently claimed that superconductivity (SC) in the $κ$-phase organic charge-transfer solids (CTS) can be understood within the two-dimensional half-filled anisotropic triangular-lattice Hubbard model. Experimentally, $κ$-CTS are mostly but not always antiferromagnetic (AFM) at ambient pressure and SC appears under pressure. In apparent agreement with this observation, Menke et al. found AFM ground states for small $t/U$ and SC over a small region at the interface of AFM and Fermi liquid ground states with increasing $t/U$ at fixed $t'/t$, where $U$ is the Hubbard repulsion. Menke et al's computational results directly contradict those obtained using exact diagonalization and Path Integral Renormalization Group approaches. It is clearly of interest to determine the origin of this discrepancy, especially in view of the facts that (a) related arguments continue to persist in the context of cuprate SC superconductivity (which however involves doping), and (b) there exist CTS in which SC is not proximate to AFM, but is separated by an intermediate charge-disproportionated phase. Here we show that Menke et al's conclusion regarding SC is incorrect and originates from a flawed assumption.

cond-mat.supr-con↗

arXiv2024

First-Principles Study of Penta-CN2 Quantum Dots for Efficient Hydrogen Evolution Reaction

The objective of our research is to investigate the electrocatalytic properties of novel metal-free quantum dots (QDs) composed of the recently discovered 2D material penta-CN2, with the aim of replacing costly and scarce catalysts such as Pt and Pd. Employing a first-principles density functional theory (DFT) based approach, the geometries of the three penta-CN2 quantum dots (QDs) of increasing sizes, 3 x 3, 3 x 4, 4 x 4 are optimized. Through comprehensive analysis, our research extensively explored the structural stability of penta-CN2 QDs, delved into their electronic properties, and assessed their catalytic performance concerning the Hydrogen Evolution Reaction (HER). Notably, the H-adsorbed penta-CN2 QDs exhibit a significant reduction in the HOMO-LUMO gap (E_{g}) ranging from 35% to 49% compared to the pristine QD. Next, we investigated their catalytic performance relevant to HER, using well-known descriptors: (i) adsorption energy, (ii) over-potential, (iii) Gibbs free energy and (iv) exchange current density along with the volcano curve. As far as size dependence of the catalytic performance is concerned, the value of Delta G^{(av)} is minimum for 3 x 3 penta-CN2 QD, with those of 3 x 4 and 4 x 4 QDs being slightly larger. Our calculations predict a high value of exchange current density 2.24 x 10^{-3} A-cm^{-2} for one of the sites (N11 for 3 x 3 QD), which we believe will lead to significantly enhanced HER properties. Our research outcomes hold great promise in advancing the discovery of abundant, non-toxic, and cost-effective catalysts for HER, playing a vital role in facilitating large-scale hydrogen production.

cond-mat.mtrl-sci↗

arXiv2023

A first-principles study of the electronic, vibrational, and optical properties of planar SiC quantum dots

With the reported synthesis of a fully planar 2D silicon carbide (SiC) allotrope, the possibilities of its technological applications are enormous. Recently, several authors have computationally studied the structures and electronic properties of a variety of novel infinite periodic SiC monolayers, in addition to the honeycomb one. In this work, we perform a systematic first-principles investigation of the geometry, electronic structure, vibrational, and optical absorption spectra of several finite, but, fully planar structures of SiC, i.e., 0D quantum dots (QDs). The sizes of the studied structures are in the 1.20--2.28 nm range, with their computed HOMO(H)-LUMO(L) gaps ranging from 0.66 eV to 4.09 eV, i.e., from the IR to the UV region of the spectrum. The H-L gaps in the SiC QDs are larger as compared to the band gaps of the corresponding monolayers, confirming the quantum confinement effects. In spite of covalent bonding in the QDs, Mulliken charge analysis reveals that Si atoms exhibit positive charges, whereas the C atoms acquire negative charges, due to the different electron affinities of the two atoms. Furthermore, a strong structure property relationship is observed with fingerprints both in the vibrational and optical spectra. The wide range of H-L gaps in different SiC QDs makes them well-suited for applications in fields such as photocatalysis, light-emitting diodes, and solar cells.

cond-mat.mtrl-sci↗

arXiv2022

Density Functional Theory Study of the Hydrogen Evolution Reaction in Haeckelite Boron Nitride Quantum Dots

To satisfy rising energy needs and to handle the forthcoming worldwide climate transformation, major research attention has been drawn to environmentally friendly, renewable, and abundant energy resources. Hydrogen plays an ideal and significant role is such resources, due to its non-carbon-based energy and production through clean energy. In this work, we have explored the catalytic activity of a newly predicted haeckelite boron nitride quantum dot (haeck-BNQD), constructed from the infinite BN sheet, for its utilization in hydrogen production. Density functional theory calculations are employed to investigate geometry optimization, electronic and adsorption mechanism of haeck-BNQD using Gaussian16 package, employing the hybrid B3LYP and wB97XD functionals, along with 6- 31G(d,p) basis set. A number of physical quantities such as HOMO/LUMO energies, the density of states, hydrogen atom adsorption energies, Mulliken populations, Gibbs free energy, work functions, overpotentials, etc., have been computed and analyzed in the context of the catalytic performance of haeck-BNQD for the hydrogen-evolution reaction (HER). Based on our calculations, we predict that the best catalytic performance will be obtained for H adsorption on top of the squares or the octagons of haeck-BNQD. We hope that our prediction of the most active catalytic sites on haeck-BNQD for HER will be put to test in future experiments.

cond-mat.mtrl-sci↗