Searcharxiv⌕ Search

arXiv subjects

Alok Shukla

Publications and source records attributed to Alok Shukla.

At least 55 records · Page 3Linked to original sources
arXiv2024

On sequency-complete and sequency-ordered matrices

The concept of sequency holds a fundamental significance in signal analysis using Walsh basis functions. In this study, we closely examine the concept of sequency and explore the properties of sequency-complete and sequency-ordered matrices. We obtain results on cardinalities of sets containing sequency-complete and sequency-ordered matrices of arbitrary sizes. We present methods for obtaining interesting classes of sequency-complete and sequency-ordered matrices of arbitrary sizes. We also provide results on the sequencies of columns in tensor products involving two or more matrices.

math.CO↗
arXiv2023

High Capacity Hydrogen Storage on Zirconium decorated γ-graphyne: A systematic first-principles study

In this work, we investigate the hydrogen-storage properties of Zr-decorated $γ$-graphyne monolayer employing Density Functional Theory (DFT) for green energy storage. We predict that each Zr atom decorated on graphyne sheet (2D) can adsorb up to seven H$_2$ molecules with an average adsorption energy of -0.44 eV/H$_2$, leading to a hydrogen gravimetric density of 7.95 wt%, and desorption temperature of 574 K, particularly suited to fuel-cell applications. Decorated Zr atom strongly attached to graphyne due to charge transfer from Zr to graphyne sheet. Hydrogen molecules adsorb on Zr decorated graphyne with Kubas type of interaction. The 4.05 eV diffusion energy barrier between Zr decorated position, and its neighboring pores may avoid the metal-metal (Zr-Zr) clustering. The stability of Zr+$γ$-graphyne is confirmed by performing ab-initio molecular dynamics simulations at room temperature and at estimated average desorption temperature. Hence, our calculations show Zr functionalized on $γ$-graphyne could be a promising solid-state hydrogen storage material.

cond-mat.mtrl-sci↗
arXiv2023

Tuning the electronic and optical properties of hg-C$_3$N$_4$, quantum dots with edge-functionalization: A computational perspective

In this work, we have systematically investigated the structural, electronic, vibrational and optical properties of the edge-functionalized hg-C3N4 quantum dots with the aim of exploring their possible applications in solar cells and other optoelectronic devices such as light-emitting diodes. The functional groups considered in this work are methyl (-CH$_3$), fluorine (-F), and oxygenated groups such as aldehyde (-CHO), carboxyl (-COOH), ketone (-COCH$_3$), and hydroxyl (-OH) groups. The edge-functionalization resulted in significant tuning of the electronic, vibrational, and optical properties. Thus, their structural fingerprints are present in both their vibrational and optical properties, thereby allowing their detection both in the Raman as well as optical spectroscopies. It is observed that edge functionalization broadens the energy range of optical absorption, leading to coverage of most of the ultraviolet and visible regions. This implies that the edge-functionalization of hg-C$_3$N$_4$ quantum dots can be used in a variety of optoelectronic devices such as solar cells and light emitting diodes.

cond-mat.mtrl-sci↗
arXiv2023

Defect-driven tunable electronic and optical properties of two-dimensional silicon carbide

Recently, an atomic-scale two-dimensional silicon carbide monolayer has been synthesized {[}Polley \emph{et al., }Phys. Rev. Lett. \textbf{130},076203 (2023){]} which opens up new possibilities for developing next-generation electronic and optoelectronic devices. Our study predicts the pristine SiC monolayer to have an ``indirect'' band gap of 3.38 eV $(K\rightarrow M)$ and a ``direct'' band gap of 3.43 eV $(K\rightarrow K)$ calculated using the HSE06 functional. We performed a detailed investigation of the various possible defects (i.e., vacancies, foreign impurities, antisites, and their various combinations) on the structural stability, electronic, and optical properties of the SiC monolayer using a first-principles based density-functional theory (DFT) and molecular dynamics (MD) simulations. A number of physical quantities such as the formation energy, electronic band gap, and the effective masses of charge carriers, have been calculated. We report that the SiC monolayer has a very low formation energy of 0.57 eV and can be stabilized on TaC \{111\} film by performing the surface slab energy and interfacial adhesion energy calculations. Nitrogen doping is predicted to be the most favorable defect in silicon carbide monolayer due to its very low formation energy, indicating high thermodynamic stability. An interesting transition from semiconducting to metallic state is observed for $N_{C}$ and $Al_{Si}$ defective systems. For the pristine SiC monolayer, we find that the conduction band is nearly flat in the $M\rightarrow K$ direction, leading to a high effective mass of $3.48m_{o}$. A significant red shift in the absorption edge, as well as the occurrence of additional absorption peaks due to the defects, have been observed in the lower energy range of the spectrum.

cond-mat.mtrl-sci↗
arXiv2023

Potential reversible hydrogen storage in Li-decorated carbon allotrope PAI-Graphene: A first-principles study

Two-dimensional porous carbon nanomaterials are proven to be promising hydrogen storage substrates as they possess high surface area, large number of active sites, low molecular mass, and hydrogen molecules can be adsorbed on both sides of these materials. By performing first-principles density functional theory-based calculations, we report ultrahigh reversible hydrogen uptake in lithium decorated 2D carbon allotrope PAI-graphene, which is formed of a regular pattern of polymerized as-indacenes (PAI). We found that a single unit cell of PAI-graphene can be decorated by 8 Li atoms, in which each Li atom can reversibly adsorb 4 hydrogen molecules, leading to 15.7 % of H uptake, remarkably higher than the DOE demand of 6.5 %. Li atom donates its valence 2s-electron to PAI-graphene and gets ionized. The adsorption energies of the various H2 attached to Li-atom are found to be suitable for reversible use during practical applications. Hydrogen molecules get attached to the ionized metal atom by electrostatic interactions. An energy barrier of 1.48 eV is present for the diffusion of Li atoms between the two most stable adsorption sites which justifies the absence of the clustering of Li atoms.

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↗
arXiv2023

Improving Hydrogen evolution catalytic activity of 2D carbon allotrope Biphenylene with B, N, P doping: Density Functional Theory Investigations

Using a first principles approach, we studied the hydrogen evolution reaction activity of newly synthesized biphenylene and B, N, P decorated biphenylene sheet. hydrogen evolution reaction activity of pristine biphenylene sheet is not encouraging, as it is similar to pristine graphene. The Gibbs free energy and overpotential of P(N) doped on biphenylene sheet are 0.022 (-0.092) eV and 22 (92) mV, respectively. The reported Gibbs free energy and overpotential of Pt are 0.9 eV and 90 mV. Hence doping of P(N) atom on top of biphenylene sheet improves hydrogen evolution reaction activity much better (near to) Pt metal. We analyzed the adsorption mechanism of dopants (B, N, P) and hydrogen with Bader charge analysis and density of states analysis. P and N-decoration on biphenylene sheet change its electronic structure so that one obtains improved hydrogen evolution reaction activity for P and N-doped biphenylene sheet. Furthermore, the stability of N, P decorated biphenylene at room temperature with ab initio molecular dynamics and formation energy near that of biphenylene indicate experimental feasibility. We have compared all our best hydrogen evolution reaction activity results in the reaction coordinate and volcano plots of pristine, B, N, and P-doped BPh sheets. They indicate that P-doped biphenylene is a metal-free, powerful catalyst for hydrogen evolution reaction activities.

cond-mat.mtrl-sci↗
arXiv2023

Engineering the electronic, magnetic, and optical properties of GaP monolayer by substitutional doping: a first-principles study

In this paper we present a thorough first-principles based density functional theory study of the structural stability, electronic, magnetic, and optical properties of pristine and doped gallium phosphide (GaP) monolayers. The pristine GaP monolayer is found to have a periodically buckled structure, with an indirect band gap of 2.15 eV. The doping by X (B, Al, In, C, Si, Ge, Sn, Zn, Cd) at the Ga site, and Y (N, As, Sb, O, S, Se, Te, Zn, Cd) at the P site is considered, and an indirect to direct transition is observed after doping by In at the Ga site. For several cases, significant changes in the band gap are seen after doping, while system becomes metallic when O is substituted at the P site. The spin-polarized band structures are calculated for the monolayers with doping-induced magnetism, and we find that for some cases a direct band gap appears for one of the spin orientations. For such cases, we investigate the intriguing possibility of spin-dependent optical properties. Furthermore for several cases, the band gap is very small for one of the spin orientations, suggesting the possibility of engineering half metallicity by doping. For the layers with direct band gaps, the calculated optical absorption spectra are found to span a wide energy range in the visible and ultraviolet regions. The calculated formation energies of both the pristine and doped structures are quite small, indicating that the laboratory realization of such structures is quite feasible. On the whole, our results suggest that the doped GaP monolayer is a material with potentially a wide range of applications in nanoelectronics, spintronics, optoelectronics, solar cells, etc.

cond-mat.mtrl-sci↗
arXiv2023

A quantum approach for digital signal processing

We propose a novel quantum approach to signal processing, including a quantum algorithm for low-pass and high-pass filtering, based on the sequency-ordered Walsh-Hadamard transform. We present quantum circuits for performing the sequency-ordered Walsh-Hadamard transform, as well as quantum circuits for low-pass, high-pass, and band-pass filtering. Additionally, we provide a proof of correctness for the quantum circuit designed to perform the sequency-ordered Walsh-Hadamard transform. The performance and accuracy of the proposed approach for signal filtering were illustrated using computational examples, along with corresponding quantum circuits, for DC, low-pass, high-pass, and band-pass filtering. Our proposed algorithm for signal filtering has a reduced gate complexity and circuit depth of $O (\log_2 N)$, compared to at least $O ((\log_2 N )^2)$ associated with Quantum Fourier Transform (QFT) based filtering (excluding state preparation and measurement costs). In contrast, classical Fast Fourier Transform (FFT) based filtering approaches have a complexity of $O (N \log_2 N )$. This shows that our proposed approach offers a significant improvement over QFT-based filtering methods and classical FFT-based filtering methods. Such enhanced efficiency of our proposed approach holds substantial promise across several signal processing applications by ensuring faster computations and efficient use of resources via reduced circuit depth and lower gate complexity.

quant-ph↗
arXiv2023

A quantum algorithm for counting zero-crossings

We present a zero-crossings counting problem that is a generalization of the Bernstein-Vazirani problem. The goal of this problem is to count the number of zero-crossings (or sign changes) in a special type of sequence S, whose definition depends upon a secret string. A quantum algorithm is presented to solve this problem. The proposed quantum algorithm requires only one oracle query to solve the problem, whereas a classical algorithm would need at least n oracle queries, where $2^n$ is the size of the sequence S. In addition to solving the zero-crossings counting problem, we also give a quantum circuit for performing the Walsh-Hadamard transforms in sequency ordering. The Walsh-Hadamard transform in sequency ordering is used in a wide range of scientific and engineering applications, including in digital signal and image processing. Therefore, the proposed quantum circuit for computing the Walsh-Hadamard transforms in sequency ordering may be helpful in quantum computing algorithms for applications for which the computation of the Walsh-Hadamard transform in sequency ordering is required.

quant-ph↗
arXiv2023

Influence of native defects on magneto-optoelectronic properties of $α$-MoO$_{3}$

Semiconducting oxides possess a variety of intriguing electronic, optical, and magnetic properties, and native defects play a crucial role in these systems. In this study, we study the influence of native defects on these properties of $α$-MoO$_{3}$ using the first-principles density functional theory (DFT) calculations. From the formation energy calculations, it is concluded that Mo vacancies are difficult to form in the system, while O and Mo-O co-vacancies are energetically quite favorable. We further find that vacancies give rise to mid-gap states (trap states) that remarkably affect the magneto-optoelectronic properties of the material. Our calculations indicate that a single Mo vacancy leads to half-metallic behavior, and also induces a large magnetic moment of 5.98 $μ_{B}$. On the other hand, for the single O vacancy case, the band gap disappears completely, but the system remains in a non-magnetic state. For Mo-O co-vacancies of two types considered in this work, a reduced band gap is found, along with an induced magnetic moment of 2.0 $μ_{B}$. Furthermore, a few finite peaks below the main band edge are observed in the absorption spectra of configurations with Mo and O vacancies, while they are absent in the Mo-O co-vacancies of both types, just like in the pristine state. From the ab-initio molecular dynamics simulations, stability and sustainability of induced magnetic moment at room temperate is verified. Our findings will enable the development of defect strategies that maximize the functionality of the system, and further help in designing highly efficient magneto-optoelectronic and spintronic devices.

cond-mat.mtrl-sci↗
arXiv2023

On Using Non-Kekule' Triangular Graphene Quantum Dots for Scavenging Hazardous Sulfur Hexafluoride Components

The goal of the present study is to explore how the size and functionalization of graphene quantum dots (GQDs) affect their sensing capabilities. Specifically, we investigated the adsorption of SO$_2$, SOF$_2$, SO$_2$F$_2$, and SF$_6$ on GQDs that were functionalized with -CH$_3$, - COCH$_3$, and -NH$_2$. We used density functional theory to analyze the electronic properties of these functionalized GQDs and found that the functionalization significantly altered their electronic properties. For example, the B3LYP H-L gap of pristine triangulene was 3.9eV, while the H-L gap of functionalized triangulene ranged from 2.8 eV-3.6 eV (using the B3LYP functional). Our results indicate that -NH2 functionalized phenalenyl and triangulene provide strong interaction with SO$_2$, with adsorption energies of -0.429 eV and -0.427 eV, respectively. These adsorption properties exhibit physisorption, leading to high gas sensitivity and superior recovery time. The findings of this study provide new insights into the potential use of GQDs for detecting the decomposed constituents of sulfur hexafluoride, which can be beneficial for assessing the operation status of SF$_6$ insulated devices. Overall, our calculations suggest that functionalized GQDs can be employed in gas insulated systems for partial discharge detection.

physics.chem-ph↗
arXiv2023

Highly Efficient Hydrogen Storage of Sc Decorated Biphenylene Monolayer near Ambient-temperature: An Ab-initio Simulation

The energy demands for the growing development of society need to be catered with alternative and green fuels like hydrogen energy for a lasting and sustainable culture. One essential component of the hydrogen economy is the efficiency of its storage. We have studied the hydrogen-storage capability on a recently synthesized Biphenylene (BPh) decorated with Sc using the first-principles density functional theory (DFT) and ab-initio molecular dynamics (AIMD) techniques. Scandium attaches BPh sheet strongly with binding energy -3.84 eV, and single Sc decorated on BPh can absorb a maximum of five H$_2$ molecules resulting in a high gravimetric weight percentage of 11.07, which is significantly higher than DoE's ultimate criteria (6.5 wt%). Using van't Hoff equation, strongly and weakly attached hydrogens correspond to desorption temperatures of 200 K and 397 K with an average of 305 K. The high binding of Sc to BPh is due to charge donation of 3d orbital of Sc to 2p orbital of C. The interactions between absorbed H$_2$ and BPh+Sc are due to charge transfer from 3d-orbital of Sc to $σ$* bond of H$_2$ molecules and backdonation from $σ$ bond of H$_2$ to empty 3d-orbital of Sc known as Kubas type interaction. Furthermore, phonon and AIMD simulation confirm BPh+Sc stability, and the presence of an energy barrier shows no probability of Sc-Sc clustering on BPh. So theoretically stable BPh+Sc showing high gravimetric weight percentage with an average 305 K desorption temperature, might be a potential candidate for solidstage hydrogen devices.

cond-mat.mtrl-sci↗
arXiv2023

Improvement in the Performance and Efficiency on Self-Deficient CaTiO$_3$: Towards Sustainable and Affordable New-Generation Solar Cells

Thin films of pure and self-deficient calcium titanites i.e., CaTiO$_3$, Ca$_{1-α}$TiO$_3$, CaTi$_{1-β}$O$_3$ and CaTiO$_{3-γ}$ have been deposited on ITO substrate using dip coating method. X-ray diffraction and Scanning electron Microscopy (SEM) analysis confirm the structural and morphology of all deposited thin films. Photocurrent measurement has been done, and it is observed that during the incidence of UV light on the as-prepared device (i.e., in the "ON" state), a significant increase in photocurrent (IUV) at zero voltage was observed in case of O deficient CaTiO$_3$, while in case of Ti and Ca deficient thin films smaller values of photocurrents were seen. Responsivity and detectivity of deposited thin films of all self-deficient CaTiO3 were found to be maximum in the UV region while they also showed smaller contributions in the visible range possibly due to the presence of self-deficiency. The self-deficient sample exhibits lower resistance (higher recombination rate) than the pure sample at low voltage, but at higher voltage, it is almost identical. Furthermore, theoretical calculations have been performed using the first-principles density-functional theory to validate the experimental findings on self-deficient CaTiO$_3$. Incident-photon-to-current efficiency (IPCE) and current density have also been measured for all deficient CaTiO$_3$ samples. Maximum IPCE have been found in the range 25%-28% for Ti and O deficient samples in the UV range (280- 400 nm). We argue that first-principles DFT calculations combined with the experimental measurements on self-deficient CaTiO$_3$ thin films offer a reliable way to enhance the performance of perovskite-based solar devices.

cond-mat.mtrl-sci↗
arXiv2023

Room Temperature d$^0$ Ferromagnetism in Carbon Doped LaH$_3$: Insights From Density Functional Theory Simulations

Employing the state-of-the-art Density Functional Theory with both GGA and hybrid HSE06 functional along with the incorporation of spin-orbit coupling, we have engineered stable room temperature ferromagnetism in non-magnetic LaH$_3$ through C substitution at octahedral and tetrahedral H sites where the induced magnetic moment is mostly contributed by 2p orbital of C atom. It is interesting that the magnetic signature is switched on with an impurity concentration as low as 1.04 at% with a magnetic moment of $\approx$ 1.0 $μ_B$ per impurity, where the localized behavior of the 2p states of C along with significant exchange splitting energy can be attributed as the origin of the induced magnetic moment. The verification of the Stoner criterion in the material further confirmed the onset of ferromagnetism in the system, and the computed Curie temperature is found to be well above room temperature. Reduced formation energy and requirement of lower impurity concentration ensure practical feasibility towards a spintronic device where room temperature ferromagnetism is established from the non-magnetic host and the dopant.

cond-mat.mtrl-sci↗
arXiv2023

Benchmarking Gaussian Basis Sets in Quantum-Chemical Calculations of Photoabsorption Spectra of Light Atomic Clusters

The choice of Gaussian basis functions for computing the ground-state properties of molecules, and clusters, employing wave-function-based electron-correlated approaches, is a well-studied subject. However, the same cannot be said when it comes to the excited-state properties of such systems, in general, and optical properties, in particular. The aim of the present study is to understand how the choice of basis functions affects the calculations of linear optical absorption in clusters, qualitatively, and quantitatively. For this purpose, we have calculated linear optical absorption spectra of several small charged and neutral clusters, namely, Li$_{2}$, Li$_{3}$, Li$_{4}$, B$_{2}^{+}$, B$_{3}^{+}$, Be$_{2}^{+}$, and Be$_{3}^{+}$, using a variety of Gaussian basis sets. The calculations were performed within the frozen-core approximation, and a rigorous account of electron correlation effects in the valence sector was taken by employing various levels of configuration interaction (CI) approach both for the ground and excited states. Our results on the peak locations in the absorption spectra of Li$_{3}$ and Li$_{4}$ are in very good agreement with the experiments. Our general recommendation is that for excited-state calculations, it is very important to utilize those basis sets which contain augmented functions. Relatively smaller aug-cc-pVDZ basis sets also yield high-quality results for photoabsorption spectra, and are recommended for such calculations if the computational resources are limited.

physics.chem-ph↗
arXiv2023

Highly Sensitive and Self Powered Ultraviolet Photo Detector based on ZnO Nanorods Coated with TiO$_2$

Nanorods (NRs) of crystalline ZnO coated with thin layers of TiO$_2$(ZnO@TiO$_2$) were fabricated with the help of the spin coating technique followed by the hydrothermal method. Scanning electron microscopy (SEM) and X-ray diffraction analysis confirms the morphology and structural stability of as-prepared NRs. The optical band gaps of the NRs were estimated, and a clear blue shift toward the UV region has been detected. When UV light falls on as-prepared device (i.e., in the "ON" state), a significant increase in photocurrent (I$_{UV}$) at zero voltage supply was observed from 6 $μ$A to 17 $μ$A while in the "OFF" state, the dark current (I$_{dark}$), increases from 0.08 $μ$A to 0.6 $μ$A with ZnO@TiO$_2$ NRs as compared to bare ZnO NRs respectively. Responsivity and detectivity of TiO$_2$ coated ZnO NRs based device found maximum in UV region unlike bare ZnO NRs. Enhanced photocurrent achieved by the growth of TiO$_2$ layers on ZnO NRs is 250 $μ$A as compared to bare ZnO NRs for which it is 35 $μ$A at 10 V voltage supply under the ultraviolet irradiation (illumination intensity of 1 mW/cm$^2$). Furthermore, theoretical calculations have been performed using the first-principles density-functional theory to understand the effects of heterostructure NRs on the electronic and optical properties of TiO$_2$ coated ZnO.

physics.app-ph↗
arXiv2022

Influence of Defects on the Valley Polarization Properties of Monolayer MoS$_{2}$ Grown by Chemical Vapor Deposition

Here, the underlying mechanisms behind valley de-polarization is investigated in chemical vapor deposited 1L-MoS$_{2}$. Temperature dependent polarization resolved photoluminescence spectroscopy was carried out on as-grown, transferred and capped samples. It has been found that the momentum scattering of the excitons due to the sulfur-vacancies attached with air-molecule defects has a strong influence on the valley de-polarization process. Our study reveals that at sufficiently low densities of such defects and temperatures, long range electron-hole exchange mediated intervalley transfer due to momentum scattering via Maialle-Silva-Sham (MSS) mechanism of excitons is indeed the most dominant spin-flip process as suggested by T. Yu et al. The rate of momentum scattering of the excitons due to these defects is found to be proportional to the cube root of the density of the defects. Intervalley transfer process of excitons involving $Γ$-valley also has significance in the valley de-polarization process specially when the layer has tensile strain or high density of $V_S$ defects as these perturbations reduce $K$ to $Γ$-energy separation. Band-structural calculations carried out within the density functional theory framework validate this finding. Experimental results further suggest that exchange interactions with the physisorbed air molecules can also result in the intervalley spin-flip scattering of the excitons, and this process gives an important contribution to valley depolarization, specially at the strong scattering regime.

physics.optics↗