arXiv subjects

Parthapratim Biswas

Publications and source records attributed to Parthapratim Biswas.

At least 37 records · Page 2Linked to original sources

arXiv2015

Sculpting the band gap: a computational approach

Materials with optimized band gap are needed in many specialized applications. In this work, we demonstrate that Hellmann-Feynman forces associated with the gap states can be used to find atomic coordinates with a desired electronic density of states. Using tight-binding models, we show that this approach can be used to arrive at electronically designed models of amorphous silicon and carbon. We provide a simple recipe to include a priori electronic information in the formation of computer models of materials, and prove that this information may have profound structural consequences. An additional example of a graphene nanoribbon is provided to demonstrate the applicability of this approach to engineer 2-dimensional materials. The models are validated with plane-wave density functional calculations.

cond-mat.mtrl-sci↗

arXiv2010

Microstructure, vacancies and moments of nuclear magnetic resonance of hydrogenated amorphous silicon

Recent experiments on hydrogenated amorphous silicon using infrared absorption spectroscopy have indicated the presence of mono- and divacancy in samples for concentration of up to 14\% hydrogen. Motivated by this observation, we study the microstructure of hydrogen in two model networks of hydrogen-rich amorphous silicon with particular emphasis on the nature of the distribution (of hydrogen), the presence of defects, and the characteristic features of the nuclear magnetic resonance spectra at low and high concentration of hydrogen. Our study reveals the presence of vacancies, which are the built-in features of the model networks. The study also confirms the presence of various hydride configurations in the networks that include from silicon monohydrides and dihydrides to open chain-like structures, which have been observed in the infrared and nuclear magnetic resonance experiments. The broad and the narrow line widths of the nuclear magnetic resonance spectra are calculated from a knowledge of the distribution of spins (hydrogen) in the networks.

cond-mat.mtrl-sci↗

arXiv2010

Function reconstruction as a classical moment problem: A maximum entropy approach

We present a systematic study of the reconstruction of a non-negative function via maximum entropy approach utilizing the information contained in a finite number of moments of the function. For testing the efficacy of the approach, we reconstruct a set of functions using an iterative entropy optimization scheme, and study the convergence profile as the number of moments is increased. We consider a wide variety of functions that include a distribution with a sharp discontinuity, a rapidly oscillatory function, a distribution with singularities, and finally a distribution with several spikes and fine structure. The last example is important in the context of the determination of the natural density of the logistic map. The convergence of the method is studied by comparing the moments of the approximated functions with the exact ones. Furthermore, by varying the number of moments and iterations, we examine to what extent the features of the functions, such as the divergence behavior at singular points within the interval, is reproduced. The proximity of the reconstructed maximum entropy solution to the exact solution is examined via Kullback-Leibler divergence and variation measures for different number of moments.

math-ph↗

arXiv2009

Theoretical study of hydrogen microstructure in models of hydrogenated amorphous silicon

We study the distribution of hydrogen and various hydride configurations in realistic models of a-Si:H for two different concentration generated via experimentally constrained molecular relaxation approach (ECMR) [1]. The microstructure corresponding to low (< 10%) and high (> 20%) concentration of H atoms are addressed and are compared to the experimental results with particular emphasis on the size of H clusters and local environment of H atoms.The linewidths of the nuclear magnetic resonance (NMR) spectrum for the model configurations are calculated in order to compare to the experimental NMR data. Our study shows the presence of isolated hydrogen atoms, small and relatively large clusters with average proton-proton neighbor distance in the clusters around 1.6 to 2.4 Angstrom that have been observed in multiple quantum NMR experiments.

cond-mat.mtrl-sci↗

arXiv2009

Lyapunov exponent and natural invariant density determination of chaotic maps: An iterative maximum entropy ansatz

We apply the maximum entropy principle to construct the natural invariant density and Lyapunov exponent of one-dimensional chaotic maps. Using a novel function reconstruction technique that is based on the solution of Hausdorff moment problem via maximizing Shannon entropy, we estimate the invariant density and the Lyapunov exponent of nonlinear maps in one-dimension from a knowledge of finite number of moments. The accuracy and the stability of the algorithm are illustrated by comparing our results to a number of nonlinear maps for which the exact analytical results are available. Furthermore, we also consider a very complex example for which no exact analytical result for invariant density is available. A comparison of our results to those available in the literature is also discussed.

nlin.CD↗

arXiv2009

Atomistic modeling of amorphous silicon carbide: An approximate first-principles study in constrained solution space

Localized basis ab initio molecular dynamics simulation within the density functional framework has been used to generate realistic configurations of amorphous silicon carbide (a-SiC). Our approach consists of constructing a set of smart initial configurations that conform essential geometrical and structural aspects of the materials obtained from experimental data, which is subsequently driven via first-principles force-field to obtain the best solution in a reduced solution space. A combination of a priori information (primarily structural and topological) along with the ab-initio optimization of the total energy makes it possible to model large system size (1000 atoms) without compromising the quantum mechanical accuracy of the force-field to describe the complex bonding chemistry of Si and C. The structural, electronic and the vibrational properties of the models have been studied and compared to existing theoretical models and available data from experiments. We demonstrate that the approach is capable of producing large, realistic configurations of a-SiC from first-principles simulation that display excellent structural and electronic properties of a-SiC. Our study reveals the presence of predominant short-range order in the material originating from heteronuclear Si-C bonds with coordination defect concentration as small as 5% and the chemical disorder parameter of about 8%.

cond-mat.dis-nn↗

arXiv2008

Inverse approach to atomistic modeling: Applications to a-Si:H and g-GeSe2

We discuss an inverse approach for atomistic modeling of glassy materials. The focus is on structural modeling and electronic properties of hydrogenated amorphous silicon and glassy GeSe2 alloy. The work is based upon a new approach "experimentally constrained molecular relaxation (ECMR)". Unlike conventional approaches (such as molecular dynamics (MD) and Monte Carlo simulations(MC), where a potential function is specified and the system evolves either deterministically (MD) or stochastically (MC), we develop a novel scheme to model structural configurations using experimental data in association with density functional calculations. We have applied this approach to model hydrogenated amorphous silicon and glassy GeSe2. The electronic and structural properties of these models are compared with experimental data and models obtained from conventional molecular dynamics simulation.

cond-mat.dis-nn↗

arXiv2007

Experimentally Constrained Molecular Relaxation: The case of hydrogenated amorphous silicon

We have extended our experimentally constrained molecular relaxation technique (P. Biswas {\it et al}, Phys. Rev. B {\bf 71} 54204 (2005)) to hydrogenated amorphous silicon: a 540-atom model with 7.4 % hydrogen and a 611-atom model with 22 % hydrogen were constructed. Starting from a random configuration, using physically relevant constraints, {\it ab initio} interactions and the experimental static structure factor, we construct realistic models of hydrogenated amorphous silicon. Our models confirm the presence of a high frequency localized band in the vibrational density of states due to Si-H vibration that has been observed in a recent vibrational transient grating measurements on plasma enhanced chemical vapor deposited films of hydrogenated amorphous silicon.

cond-mat.mtrl-sci↗

arXiv2007

Real space information from Fluctuation electron microscopy: Applications to amorphous silicon

Ideal models of complex materials must satisfy all available information about the system. Generally, this information consists of experimental data, information implicit to sophisticated interatomic interactions and potentially other {\it a priori} information. By jointly imposing first-principles or tight-binding information in conjunction with experimental data, we have developed a method: Experimentally Constrained Molecular Relaxation (ECMR) that uses {\it all} of the information available. We apply the method to model medium range order in amorphous silicon using Fluctuation Electron microscopy (FEM) data as experimental information. The paracrystalline model of medium range order is examined, and a new model based on voids in amorphous silicon is proposed. Our work suggests that films of amorphous silicon showing medium range order (in FEM experiments) can be accurately represented by a continuous random network model with inhomogeneities consisting of ordered grains and voids dispersed in the network.

cond-mat.dis-nn↗

arXiv2004

Maximum entropy and the problem of moments: A stable algorithm

We present a technique for entropy optimization to calculate a distribution from its moments. The technique is based upon maximizing a discretized form of the Shannon entropy functional by mapping the problem onto a dual space where an optimal solution can be constructed iteratively. We demonstrate the performance and stability of our algorithm with several tests on numerically difficult functions. We then consider an electronic structure application, the electronic density of states of amorphous silica and study the convergence of Fermi level with increasing number of moments.

cond-mat.dis-nn↗

arXiv2004

Experimentally Constrained Molecular Relaxation: The Case of Glassy GeSe2

An ideal atomistic model of a disordered material should contradict no experiments,and should also be consistent with accurate force fields (either {\it ab initio}or empirical). We make significant progress toward jointly satisfying {\it both} of these criteria using a hybrid reverse Monte Carlo approach in conjunction with approximate first principles molecular dynamics. We illustrate the method by studying the complex binary glassy material g-GeSe$_2$. By constraining the model to agree with partial structure factors and {\it ab initio} simulation, we obtain a 647-atom model in close agreement with experiment, including the first sharp diffraction peak in the static structure factor. We compute the electronic state densities and compare to photoelectron spectroscopies. The approach is general and flexible.

cond-mat.mtrl-sci↗

arXiv2004

Inclusion of Experimental Information in First Principles Modeling of Materials

We propose a novel approach to model amorphous materials using a first principles density functional method while simultaneously enforcing agreement with selected experimental data. We illustrate our method with applications to amorphous silicon and glassy GeSe$_2$. The structural, vibrational and electronic properties of the models are found to be in agreement with experimental results. The method is general and can be extended to other complex materials.

cond-mat.mtrl-sci↗

arXiv2004

Reverse Monte Carlo modeling of amorphous silicon

An implementation of the Reverse Monte Carlo algorithm is presented for the study of amorphous tetrahedral semiconductors. By taking into account a number of constraints that describe the tetrahedral bonding geometry along with the radial distribution function, we construct a model of amorphous silicon using the reverse monte carlo technique. Starting from a completely random configuration, we generate a model of amorphous silicon containing 500 atoms closely reproducing the experimental static structure factor and bond angle distribution and in improved agreement with electronic properties. Comparison is made to existing Reverse Monte Carlo models, and the importance of suitable constraints beside experimental data is stressed.

cond-mat.dis-nn↗

arXiv2004

The electron-phonon coupling is large for localized states

From density functional calculations, we show that localized states stemming from defects or topological disorder exhibit an anomalously large electron-phonon coupling. We provide a simple analysis to explain the observation and perform a detailed study on an interesting system: amorphous silicon. We compute first principles deformation potentials (by computing the sensitivity of specific electronic eigenstates to individual classical normal modes of vibration). We also probe thermal fluctuations in electronic eigenvalues by first principles thermal simulation. We find a strong correlation between a static property of the network [localization, as gauged by inverse participation ratio (IPR)] and a dynamical property (the amplitude of thermal fluctuations of electron energy eigenvalues) for localized electron states. In particular, both the electron-phonon coupling and the variance of energy eigenvalues are proportional to the IPR of the localized state. We compare the results for amorphous Si to photoemission experiments. While the computations are carried out for silicon, very similar effects have been seen in other systems with disorder.

cond-mat.dis-nn↗

arXiv2003

Systematic Study of Electron Localization in an Amorphous Semiconductor

We investigate the electronic structure of gap and band tail states in amorphous silicon. Starting with two 216-atom models of amorphous silicon with defect concentration close to the experiments, we systematically study the dependence of electron localization on basis set, density functional and spin polarization using the first principles density functional code Siesta. We briefly compare three different schemes for characterizing localization: information entropy, inverse participation ratio and spatial variance. Our results show that to accurately describe defect structures within self consistent density functional theory, a rich basis set is necessary. Our study revealed that the localization of the wave function associated with the defect states decreases with larger basis sets and there is some enhancement of localization from GGA relative to LDA. Spin localization results obtained via LSDA calculations, are in reasonable agreement with experiment and with previous LSDA calculations on a-Si:H models.

cond-mat.dis-nn↗

arXiv2002

Vibrational properties of amorphous silicon from tight-binding O(N) calculation

We present an O(N) algorithm to study the vibrational properties of amorphous silicon within the framework of tight-binding approach. The dynamical matrix elements have been evaluated numerically in the harmonic approximation exploiting the short-range nature of the density matrix to calculate the vibrational density of states which is then compared with the same obtained from a standard O($N^4$) algorithm. For the purpose of illustration, an 1000-atom model is studied to calculate the localization properties of the vibrational eigenstates using the participation numbers calculation.

cond-mat.dis-nn↗

arXiv2001

Diffusion with random distribution of static traps

The random walk problem is studied in two and three dimensions in the presence of a random distribution of static traps. An efficient Monte Carlo method, based on a mapping onto a polymer model, is used to measure the survival probability P(c,t) as a function of the trap concentration c and the time t. Theoretical arguments are presented, based on earlier work of Donsker and Varadhan and of Rosenstock, why in two dimensions one expects a data collapse if -ln[P(c,t)]/ln(t) is plotted as a function of (lambda t)^{1/2}/ln(t) (with lambda=-ln(1-c)), whereas in three dimensions one expects a data collapse if -t^{-1/3}ln[P(c,t)] is plotted as a function of t^{2/3}lambda. These arguments are supported by the Monte Carlo results. Both data collapses show a clear crossover from the early-time Rosenstock behavior to Donsker-Varadhan behavior at long times.

cond-mat.stat-mech↗

arXiv2000

Efficient tight-binding Monte Carlo structural sampling of complex materials

While recent work towards the development of tight-binding and ab-initio algorithms has focused on molecular dynamics, Monte Carlo methods can often lead to better results with relatively little effort. We present here a multi-step Monte Carlo algorithm that makes use of the possibility of quickly evaluating local energies. For the thermalization of a 1000-atom configuration of {\it a}-Si, this algorithm gains about an order of magnitude in speed over standard molecular dynamics. The algorithm can easily be ported to a wide range of materials and can be dynamically optimized for a maximum efficiency.

cond-mat.stat-mech↗