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Atomic Resolution Observations of Nanoparticle Surface Dynamics and Instabilities Enabled by Artificial Intelligence
Authors:
Peter A. Crozier,
Matan Leibovich,
Piyush Haluai,
Mai Tan,
Andrew M. Thomas,
Joshua Vincent,
Sreyas Mohan,
Adria Marcos Morales,
Shreyas A. Kulkarni,
David S. Matteson,
Yifan Wang,
Carlos Fernandez-Granda
Abstract:
Nanoparticle surface structural dynamics is believed to play a significant role in regulating functionalities such as diffusion, reactivity, and catalysis but the atomic-level processes are not well understood. Atomic resolution characterization of nanoparticle surface dynamics is challenging since it requires both high spatial and temporal resolution. Though ultrafast transmission electron micros…
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Nanoparticle surface structural dynamics is believed to play a significant role in regulating functionalities such as diffusion, reactivity, and catalysis but the atomic-level processes are not well understood. Atomic resolution characterization of nanoparticle surface dynamics is challenging since it requires both high spatial and temporal resolution. Though ultrafast transmission electron microscopy (TEM) can achieve picosecond temporal resolution, it is limited to nanometer spatial resolution. On the other hand, with the high readout rate of new electron detectors, conventional TEM has the potential to visualize atomic structure with millisecond time resolutions. However, the need to limit electron dose rates to reduce beam damage yields millisecond images that are dominated by noise, obscuring structural details. Here we show that a newly developed unsupervised denoising framework based on artificial intelligence enables observations of metal nanoparticle surfaces with time resolutions down to 10 ms at moderate electron dose. On this timescale, we find that many nanoparticle surfaces continuously transition between ordered and disordered configurations. The associated stress fields can penetrate below the surface leading to defect formation and destabilization making the entire nanoparticle fluxional. Combining this unsupervised denoiser with electron microscopy greatly improves spatio-temporal characterization capabilities, opening a new window for future exploration of atomic-level structural dynamics in materials.
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Submitted 2 August, 2024; v1 submitted 24 July, 2024;
originally announced July 2024.
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NLP for Knowledge Discovery and Information Extraction from Energetics Corpora
Authors:
Francis G. VanGessel,
Efrem Perry,
Salil Mohan,
Oliver M. Barham,
Mark Cavolowsky
Abstract:
We present a demonstration of the utility of NLP for aiding research into energetic materials and associated systems. The NLP method enables machine understanding of textual data, offering an automated route to knowledge discovery and information extraction from energetics text. We apply three established unsupervised NLP models: Latent Dirichlet Allocation, Word2Vec, and the Transformer to a larg…
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We present a demonstration of the utility of NLP for aiding research into energetic materials and associated systems. The NLP method enables machine understanding of textual data, offering an automated route to knowledge discovery and information extraction from energetics text. We apply three established unsupervised NLP models: Latent Dirichlet Allocation, Word2Vec, and the Transformer to a large curated dataset of energetics-related scientific articles. We demonstrate that each NLP algorithm is capable of identifying energetic topics and concepts, generating a language model which aligns with Subject Matter Expert knowledge. Furthermore, we present a document classification pipeline for energetics text. Our classification pipeline achieves 59-76\% accuracy depending on the NLP model used, with the highest performing Transformer model rivaling inter-annotator agreement metrics. The NLP approaches studied in this work can identify concepts germane to energetics and therefore hold promise as a tool for accelerating energetics research efforts and energetics material development.
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Submitted 10 February, 2024;
originally announced February 2024.
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Multiple exciton generation in VO2
Authors:
S. R. Sahu,
S. Khan,
A. Tripathy,
K. Dey,
N. Bano,
S. Raj Mohan,
M. P. Joshi,
S. Verma,
B. T. Rao,
V. G. Sathe,
D. K. Shukla
Abstract:
Multiple exciton generation (MEG) is a widely studied phenomenon in semiconductor nanocrystals and quantum dots, aimed at improving the energy conversion efficiency of solar cells. MEG is the process wherein incident photon energy is significantly larger than the band gap, and the resulting photoexcited carriers relax by generating additional electron-hole pairs, rather than decaying by heat dissi…
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Multiple exciton generation (MEG) is a widely studied phenomenon in semiconductor nanocrystals and quantum dots, aimed at improving the energy conversion efficiency of solar cells. MEG is the process wherein incident photon energy is significantly larger than the band gap, and the resulting photoexcited carriers relax by generating additional electron-hole pairs, rather than decaying by heat dissipation. Here, we present an experimental demonstration of MEG in a prototype strongly correlated material, VO2, through photocurrent spectroscopy and ultrafast transient reflectivity measurements, both of which are considered the most prominent ways for detecting MEG in working devices. The key result of this paper is the observation of MEG at room temperature (in a correlated insulating phase of VO2), and the estimated threshold for MEG is 3Eg. We demonstrate an escalated photocurrent due to MEG in VO2, and quantum efficiency is found to exceed 100%. Our studies suggest that this phenomenon is a manifestation of expeditious impact ionization due to stronger electron correlations and could be exploited in a large number of strongly correlated materials.
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Submitted 23 October, 2023;
originally announced October 2023.
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Ab initio Molecular Dynamics Simulation of Threshold Displacement Energies and Defect Formation Energies in Y4Zr3O12
Authors:
Sruthi Mohan,
Gurpreet Kaur,
C. David,
B. K. Panigrahi,
G. Amarendra
Abstract:
Ab initio molecular dynamics simulations using VASP was employed to calculate threshold displacement energies and defect formation energies of Y4Zr3O12 δ-phase, which is the most commonly found phase in newly developed Zr and Al-containing ODS steels. The Threshold displacement energy (Ed) values are determined to be 28 eV for Zr3a primary knock-on atom along [111] direction, 40 eV for Zr18f atoms…
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Ab initio molecular dynamics simulations using VASP was employed to calculate threshold displacement energies and defect formation energies of Y4Zr3O12 δ-phase, which is the most commonly found phase in newly developed Zr and Al-containing ODS steels. The Threshold displacement energy (Ed) values are determined to be 28 eV for Zr3a primary knock-on atom along [111] direction, 40 eV for Zr18f atoms along [111] direction and 50 eV for Y recoils along [110] direction. Minimum Ed values for O and O' atoms are 13 eV and 16 eV respectively. The displacement energies of anions are much smaller compared to cations, thus suggesting that anion disorder is more probable than cation disorder. All directions except the direction in which inherent structural vacancies are aligned, cations tend to occupy another cation site. The threshold displacement energies are larger than that of Y2Ti2O7, the conventional precipitates in Ti containing ODS steels. Due to the partial occupancy of Y and Zr in the 18f position, the antisite formation energy is negligibly small, and it may help the structure to withstand more disorder upon irradiation. These results convey that Zr/Al ODS alloys, which have better corrosion resistance properties compared to the conventional Ti-ODS alloys, may also possess superior radiation resistance.
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Submitted 31 May, 2021;
originally announced May 2021.
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Effect of Zr and Al Addition on Nanocluster Formation in Oxide Dispersion Strenghthened Steel-an ab initio Study
Authors:
Sruthi Mohan,
Gurpreet Kaur,
B. K. Panigrahi,
C. David,
G. Amarendra
Abstract:
Conventional Oxide dispersion strengthened steels are characterized by thermally stable, high density of Y-Ti-O nanoclusters, which are responsible for their high creep strength. Ti plays a major role in obtaining a high density of ultrafine particles of optimum size range of 2-10 nm. In Al-containing ODS steels developed for corrosion resistance, Y-Al-O clusters formed are of size range 20 -100 n…
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Conventional Oxide dispersion strengthened steels are characterized by thermally stable, high density of Y-Ti-O nanoclusters, which are responsible for their high creep strength. Ti plays a major role in obtaining a high density of ultrafine particles of optimum size range of 2-10 nm. In Al-containing ODS steels developed for corrosion resistance, Y-Al-O clusters formed are of size range 20 -100 nm, and Ti fails in making dispersions finer in the presence of Al. Usage of similar alloying elements like Zr in place of Ti is widely considered. In this study, binding energies of different stages of Y-Zr-O-Vacancy and Y-Al-O-Vacancy complexes in the bcc Iron matrix are studied by first-principle calculations. It is shown that in all the stages of formation, Y-Zr-O-Vacancy clusters have higher binding energy than Y-Al-O-Vacancy clusters and hence in ferritic steel containing both Zr and Al, Y-Zr-O-Vacancy clusters are more stable and more favored to nucleate than Y-Al-O-Vacancy clusters. The bonding nature in each stage is analyzed using charge density difference plots for the plausible reason for higher stability of Y-Zr-O-Vacancy clusters.
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Submitted 31 May, 2021;
originally announced May 2021.
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Experimental validation of density functional theory calculations on the Zr/Al oxide nanocluster formation in bcc Fe
Authors:
Sruthi Mohan,
Gurpreet Kaur,
C. David,
R. Vijay,
G. Amarendra
Abstract:
Ab initio simulations carried out in different atomic cluster configurations in bcc Fe matrix containing Zr and Al suggest energetic favorability of Y-Zr-O phase nucleation, preferably with trigonal Y4Zr3O12 structure. Subsequently, the HRTEM investigation of the as-prepared Fe - 14 Cr-0.3 Y2O3 - 0.6 Zr - 4Al oxide dispersion strengthened (ODS) alloy shows 78% of precipitates with Y4Zr3O12 structu…
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Ab initio simulations carried out in different atomic cluster configurations in bcc Fe matrix containing Zr and Al suggest energetic favorability of Y-Zr-O phase nucleation, preferably with trigonal Y4Zr3O12 structure. Subsequently, the HRTEM investigation of the as-prepared Fe - 14 Cr-0.3 Y2O3 - 0.6 Zr - 4Al oxide dispersion strengthened (ODS) alloy shows 78% of precipitates with Y4Zr3O12 structure, thereby confirming the predictive power of ab initio simulations on the secondary formation in multi-component alloys.
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Submitted 2 March, 2022; v1 submitted 27 May, 2021;
originally announced May 2021.
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Correlation between anion defects and ion beam induced luminescence in Y4Zr3O12
Authors:
Sruthi Mohan,
Gurpreet Kaur,
Sachin Srivastava,
P. Magudapathy,
C. David,
G. Amarendra
Abstract:
Potential applications of Zr/Al ODS alloys vests on the irradiation stability of the Y4Zr3O12 dispersoids. Fundamental studies to identify the type of defects are important in order to recognize pathways for damage alleviation. In this context, studies relating to identification of point defects and their clusters by in-situ ionoluminescence spectroscopy were taken up. The ionoluminescence spectru…
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Potential applications of Zr/Al ODS alloys vests on the irradiation stability of the Y4Zr3O12 dispersoids. Fundamental studies to identify the type of defects are important in order to recognize pathways for damage alleviation. In this context, studies relating to identification of point defects and their clusters by in-situ ionoluminescence spectroscopy were taken up. The ionoluminescence spectrum acquired during 100 keV He+ ion irradiation shows two prominent bands, at 330 nm and 415 nm. Using density functional theory calculations with HSE06 hybrid exchange correlation functional, the luminescent bands have been identified to be arising due to native and irradiation induced oxygen vacancy defects in charged and neutral configurations.
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Submitted 22 May, 2021;
originally announced May 2021.
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Interfacial strain relief by periodic dislocation doublets emerging from rotationally related orientation relationships of Y4Zr3O12 dispersions in ferrite matrix
Authors:
Sruthi Mohan,
Alphy George,
R. Vijay,
C. David,
G. Amarendra
Abstract:
The trigonal/bcc orientation relationships (ORs) and their likelihood of occurrence are extensively studied using dispersed Y4Zr3O12nano-precipitates in bcc Fe matrix by means of transmission electron microscopy, image simulations, and a crystallographic model. Two orientation relationships related by a rotation:[1-20]||[111] with (21-2)||(-110) and [1-20]||[111] with (00-3)||(-110), are establish…
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The trigonal/bcc orientation relationships (ORs) and their likelihood of occurrence are extensively studied using dispersed Y4Zr3O12nano-precipitates in bcc Fe matrix by means of transmission electron microscopy, image simulations, and a crystallographic model. Two orientation relationships related by a rotation:[1-20]||[111] with (21-2)||(-110) and [1-20]||[111] with (00-3)||(-110), are established and periodic arrays of misfit dislocation doublets are identified at the strained interface in (110) for both ORs. Further eighteen energetically feasible ORs in Y4Zr3O12/bcc system are deduced by combining stereographic projections, which include the two predominant ORs in this study and other ORs in literature. The orientation relationship which generates the interface with a minimum number of dislocation doublets is the most frequent.
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Submitted 6 May, 2021;
originally announced May 2021.
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Developing and Evaluating Deep Neural Network-based Denoising for Nanoparticle TEM Images with Ultra-low Signal-to-Noise
Authors:
Joshua L. Vincent,
Ramon Manzorro,
Sreyas Mohan,
Binh Tang,
Dev Y. Sheth,
Eero P. Simoncelli,
David S. Matteson,
Carlos Fernandez-Granda,
Peter A. Crozier
Abstract:
A deep convolutional neural network has been developed to denoise atomic-resolution TEM image datasets of nanoparticles acquired using direct electron counting detectors, for applications where the image signal is severely limited by shot noise. The network was applied to a model system of CeO2-supported Pt nanoparticles. We leverage multislice image simulations to generate a large and flexible da…
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A deep convolutional neural network has been developed to denoise atomic-resolution TEM image datasets of nanoparticles acquired using direct electron counting detectors, for applications where the image signal is severely limited by shot noise. The network was applied to a model system of CeO2-supported Pt nanoparticles. We leverage multislice image simulations to generate a large and flexible dataset for training and testing the network. The proposed network outperforms state-of-the-art denoising methods by a significant margin both on simulated and experimental test data. Factors contributing to the performance are identified, including most importantly (a) the geometry of the images used during training and (b) the size of the network's receptive field. Through a gradient-based analysis, we investigate the mechanisms learned by the network to denoise experimental images. This shows that the network exploits global and local information in the noisy measurements, for example, by adapting its filtering approach when it encounters atomic-level defects at the nanoparticle surface. Extensive analysis has been done to characterize the network's ability to correctly predict the exact atomic structure at the nanoparticle surface. Finally, we develop an approach based on the log-likelihood ratio test that provides a quantitative measure of the agreement between the noisy observation and the atomic-level structure in the network-denoised image.
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Submitted 17 March, 2021; v1 submitted 19 January, 2021;
originally announced January 2021.
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Probing defect states in few-layer MoS$_{2}$ by conductance fluctuation spectroscopy
Authors:
Suman Sarkar,
K. Lakshmi Ganapathi,
Sangeneni Mohan,
Aveek Bid
Abstract:
Despite the concerted effort of several research groups, a detailed experimental account of defect dynamics in high-quality single- and few-layer transition metal dichalcogenides remain elusive. In this paper we report an experimental study of the temperature dependence of conductance and conductance-fluctuations on several few-layer MoS$_{2}$ exfoliated on hexagonal boron nitride and covered by a…
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Despite the concerted effort of several research groups, a detailed experimental account of defect dynamics in high-quality single- and few-layer transition metal dichalcogenides remain elusive. In this paper we report an experimental study of the temperature dependence of conductance and conductance-fluctuations on several few-layer MoS$_{2}$ exfoliated on hexagonal boron nitride and covered by a capping layer of high-$κ$ dielectric HfO$_{2}$. The presence of the high-$κ$ dielectric made the device extremely stable against environmental degradation as well as resistant to changes in device characteristics upon repeated thermal cycling enabling us to obtain reproducible data on the same device over a time-scale of more than one year. Our device architecture helped bring down the conductance fluctuations of the MoS$_2$ channel by orders of magnitude compared to previous reports. The extremely low noise levels in our devices made in possible to detect the generation-recombination noise arising from charge fluctuation between the sulphur-vacancy levels in the band gap and energy-levels at the conductance band-edge. Our work establishes conduction fluctuation spectroscopy as a viable route to quantitatively probe in-gap defect levels in low-dimensional semiconductors.
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Submitted 3 July, 2019;
originally announced July 2019.
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Dielectric Engineering of HfO2 Gate Stacks Towards Normally-ON and Normally-OFF GaN HEMTs on Silicon
Authors:
Hareesh Chandrasekar,
Sandeep Kumar,
K. L. Ganapathi,
Shreesha Prabhu,
Surani Bin Dolmanan,
Sudhiranjan Tripathy,
Srinivasan Raghavan,
K. N. Bhat,
Sangeneni Mohan,
R. Muralidharan,
Navakanta Bhat,
Digbijoy N. Nath
Abstract:
We report on the interfacial electronic properties of HfO2 gate dielectrics both, with GaN towards normally-OFF recessed HEMT architectures and the AlGaN barrier for normally-ON AlGaN/GaN MISHEMTs for GaN device platforms on Si. A conduction band offset of 1.9 eV is extracted for HfO2/GaN along with a very low density of fixed bulk and interfacial charges. Conductance measurements on HfO2/GaN MOSC…
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We report on the interfacial electronic properties of HfO2 gate dielectrics both, with GaN towards normally-OFF recessed HEMT architectures and the AlGaN barrier for normally-ON AlGaN/GaN MISHEMTs for GaN device platforms on Si. A conduction band offset of 1.9 eV is extracted for HfO2/GaN along with a very low density of fixed bulk and interfacial charges. Conductance measurements on HfO2/GaN MOSCAPs reveal an interface trap state continuum with a density of 9.37x1012 eV-1cm-2 centered at 0.48 eV below EC. The forward and reverse current densities are shown to be governed by Fowler-Nordheim tunneling and Poole-Frenkel emission respectively. Normally-ON HfO2/AlGaN/GaN MISHEMTs exhibit negligible shifts in threshold voltage, transconductances of 110mS/mm for 3 μm gate length devices, and three-terminal OFF-state gate leakage currents of 20 nA/mm at a VD of 100 V. Dynamic capacitance dispersion measurements show two peaks at the AlGaN/GaN interface corresponding to slow and fast interface traps with a peak Dit of 5.5x1013 eV-1cm-2 and 1.5x1013 eV-1cm-2 at trap levels 0.55 eV and 0.46 eV below EC respectively. The HfO2/AlGaN interface exhibits a peak Dit of 4.4x1013 eV-1cm- 2 at 0.45 eV below EC.
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Submitted 12 August, 2017;
originally announced August 2017.
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Structure and Giant Magnetoresistance of Electrodeposited Co/Cu Multilayers Prepared by Two-Pulse (G/P) and Three-Pulse (G/P/G) Plating
Authors:
N. Rajasekaran,
L. Pogány,
Á. Révész,
B. G. Tóth,
S. Mohan,
L. Péter,
I. Bakonyi
Abstract:
The giant magnetoresistance (GMR) was investigated for electrodeposited Co/Cu multilayers. In order to better understand the formation of individual layers and their influence on GMR, multilayers produced by two different deposition strategies were compared. One series of Co(2 nm)/Cu(tCu) multilayers with tCu ranging from 0.5 nm to 6 nm was produced with the conventional two-pulse plating by using…
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The giant magnetoresistance (GMR) was investigated for electrodeposited Co/Cu multilayers. In order to better understand the formation of individual layers and their influence on GMR, multilayers produced by two different deposition strategies were compared. One series of Co(2 nm)/Cu(tCu) multilayers with tCu ranging from 0.5 nm to 6 nm was produced with the conventional two-pulse plating by using a galvanostatic/potentiostatic (G/P) pulse combination for the magnetic/non-magnetic layer deposition, respectively, whereby the Cu layer deposition was carried out at the electrochemically optimized potential. Another Co(2 nm)/Cu(tCu) multilayer series with the same tCu range was prepared with the help of a G/P/G pulse combination. In this latter case, first a bilayer of Co(2 nm)/Cu(6 nm) was deposited in each cycle as in the G/P mode after which a third G pulse was applied with a small anodic current to dissolve part of the 6 nm thick Cu layer in order to ensure the targeted tCu value. The comparison of the two series revealed that the G/P/G pulse combination yields multilayers for which GMR can be obtained even at such low nominal Cu layer thicknesses where G/P multilayers already exhibit bulk-like anisotropic magnetoresistance only. Surface roughness measurements by atomic force microscopy revealed that the two kinds of pulse combination yield different surface roughness values which correlate with the structural quality of the multilayers as indicated by the absence or presence of multilayer satellite reflections in the X-ray diffraction patterns. The results of multilayer chemical analysis revealed that mainly an increased Cu content of the magnetic layer is responsible for the onset of SPM regions in the form of Co segregations in the G/P/G multilayers with small Cu layer thicknesses.
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Submitted 17 April, 2017;
originally announced April 2017.
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Giant magnetoresistance and structure of electrodeposited Co/Cu multilayers: the influence of layer thicknesses and Cu deposition potential
Authors:
N. Rajasekaran,
J. Mani,
B. G. Tóth,
G. Molnár,
S. Mohan,
L. Péter,
I. Bakonyi
Abstract:
The giant magnetoresistance (GMR) and structure was investigated for electrodeposited Co/Cu multilayers prepared by a conventional galvanostatic/potentiostatic pulse combination from a pure sulfate electrolyte with various layer thicknesses, total multilayer thickness and Cu deposition potential. X-ray diffraction (XRD) measurements revealed superlattice satellite reflections for many of the multi…
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The giant magnetoresistance (GMR) and structure was investigated for electrodeposited Co/Cu multilayers prepared by a conventional galvanostatic/potentiostatic pulse combination from a pure sulfate electrolyte with various layer thicknesses, total multilayer thickness and Cu deposition potential. X-ray diffraction (XRD) measurements revealed superlattice satellite reflections for many of the multilayers having sufficiently large thickness (at least 2 nm) of both constituent layers. The bilayer repeats derived from the positions of the visible superlattice reflections were typically 10-20% higher than the nominal values.The observed GMR was found to be dominated by the multilayer-like ferromagnetic (FM) contribution even for multilayers without visible superlattice satellites. There was always also a modest superparamagnetic (SPM) contribution to the GMR and this term was the largest for multilayers with very thin (0.5 nm) magnetic layers containg apparently a small amount of magnetically decoupled SPM regions. No oscillatory GMR behavior with spacer thickness was observed at any magnetic layer thickness. The saturation of the coercivity as measured by the peak position of the MR(H) curves indicated a complete decoupling of magnetic layers for large spacer thicknesses. The GMR increased with total multilayer thickness which could be ascribed to an increasing SPM contribution to the GMR due to an increasing surface roughness, also indicated by the increasing coercivity. For multilayers with Cu layers deposited at more and more positive potentials, the GMRFM term increased and the GMRSPM term decreased. At the same time, a corresponding reduction of surface roughness measured with atomic force microscopy indicated an improvement of the multilayer structural quality which was, however, not accompanied by an increase of the superlattice reflection intensities.
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Submitted 3 February, 2017;
originally announced February 2017.
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Influence of morphological inhomogeneity induced carrier diffusion on transient photocurrent pulse shape in organic thin films
Authors:
S. Raj Mohan,
Manoranjan P. Singh,
M. P. Joshi,
L. M. Kukreja
Abstract:
The influence of film morphology induced carrier diffusion on the broadening of the time-of-flight transient photo-current pulse was investigated using Monte Carlo simulation in organic thin films. Assuming the Gaussian Disorder Model for the charge transport the simulation of the time-of-flight photo-current pulse shape was carried out for homogeneous and inhomogeneous films by varying the overal…
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The influence of film morphology induced carrier diffusion on the broadening of the time-of-flight transient photo-current pulse was investigated using Monte Carlo simulation in organic thin films. Assuming the Gaussian Disorder Model for the charge transport the simulation of the time-of-flight photo-current pulse shape was carried out for homogeneous and inhomogeneous films by varying the overall energetic disorder of the system. In the case of homogeneous system, the value of the tail broadening parameter (W) of the photocurrent pulse is found to decrease upon decreasing the energetic disorder. The observed behavior is explained by using the temporal evolution of carrier diffusion coefficient. In case of the inhomogeneous system, upon decreasing the overall energetic disorder of the system the value of W initially attained a maximum before it started to decrease. This is attributed to the morphology dependent carrier diffusion in the latter case. This study elicits the importance of the influence of the film morphology induced carrier diffusion on the experimentally measured shape of the time-of-flight transient photo-current pulses, which is found to be generally ignored.
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Submitted 8 August, 2013;
originally announced August 2013.
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Monte Carlo Simulation of Carrier Diffusion in Organic Thin Films with Morphological Inhomogeneity
Authors:
S. Raj Mohan,
Manoranjan P. Singh,
M. P. Joshi,
L. M. Kukreja
Abstract:
Monte Carlo simulation was carried out to understand the influence of morphological inhomogeneity on carrier diffusion in organic thin films. The morphological inhomogeneity was considered in the simulation by incorporating the regions of low energetic disorder in a host lattice of high energetic disorder which decreases the overall energetic disorder of the system. For the homogeneous films, the…
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Monte Carlo simulation was carried out to understand the influence of morphological inhomogeneity on carrier diffusion in organic thin films. The morphological inhomogeneity was considered in the simulation by incorporating the regions of low energetic disorder in a host lattice of high energetic disorder which decreases the overall energetic disorder of the system. For the homogeneous films, the carrier diffusion was found to decrease upon decreasing the energetic disorder. In contrast to this, in the case of inhomogeneous films the carrier diffusion enhanced upon decreasing the overall energetic disorder, up to an optimum value and beyond which the carrier diffusion decreased. Through our simulation, we observed that the behavior of carrier diffusion in the inhomogeneous case is due to the morphology dependent carrier spreading, which acts in addition to the thermal and non-thermal field assisted diffusion mechanisms. This morphological dependence of carrier spreading arises due to the generation of packets of carriers with different jump rates, which is after effect of slow relaxation of the carriers generated in the less disordered regions of inhomogeneous system. Our simulation of morphology dependent carrier spreading and its influence on the basic diffusion process provide deeper insight into the charge transport mechanisms in organic thin films.
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Submitted 25 October, 2013; v1 submitted 7 August, 2013;
originally announced August 2013.
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Growth and characterization of n-type electron-induced ferromagnetic semiconductor (In,Fe)As
Authors:
Pham Nam Hai,
Le Duc Anh,
Shyam Mohan,
Tsuyoshi Tamegai,
Masaya Kodzuka,
Tadakatsu Ohkubo,
Kazuhiro Hono,
Masaaki Tanaka
Abstract:
We show that by introducing isoelectronic iron (Fe) magnetic impurities and Beryllium (Be) double-donor atoms into InAs, it is possible to grow a n-type ferromagnetic semiconductor (FMS) with the ability to control ferromagnetism by both Fe and independent carrier doping by low-temperature molecular-beam epitaxy. We demonstrate that (In,Fe)As doped with electrons behaves as an n-type electron-indu…
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We show that by introducing isoelectronic iron (Fe) magnetic impurities and Beryllium (Be) double-donor atoms into InAs, it is possible to grow a n-type ferromagnetic semiconductor (FMS) with the ability to control ferromagnetism by both Fe and independent carrier doping by low-temperature molecular-beam epitaxy. We demonstrate that (In,Fe)As doped with electrons behaves as an n-type electron-induced FMS. This achievement opens the way to realize novel spin-devices such as spin light-emitting diodes or spin field-effect transistors, as well as helps understand the mechanism of carrier-mediated ferromagnetism in FMSs.
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Submitted 3 September, 2012;
originally announced September 2012.
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Magnetic and transport properties of iron-platinum arsenide Ca10(Pt4-δAs8)(Fe2-xPtxAs2)5 single crystal
Authors:
Qing-Ping Ding,
Yuji Tsuchiya,
Shyam Mohan,
Toshihiro Taen,
Yasuyuki Nakajima,
Tsuyoshi Tamegai
Abstract:
We report superconducting properties of single crystalline Ca10(Pt4-δAs8)(Fe2-xPtxAs2)5 by X-ray diffraction, magnetization, resistivity, and magneto-optical imaging measurements. The magnetization measurements reveal fish-tail hysteresis loop and relatively high critical current density Jc ~ 0.8\times105 A/cm2 at low temperatures. The exponential temperature dependence of Jc, which arises from no…
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We report superconducting properties of single crystalline Ca10(Pt4-δAs8)(Fe2-xPtxAs2)5 by X-ray diffraction, magnetization, resistivity, and magneto-optical imaging measurements. The magnetization measurements reveal fish-tail hysteresis loop and relatively high critical current density Jc ~ 0.8\times105 A/cm2 at low temperatures. The exponential temperature dependence of Jc, which arises from nonlinear effective flux-creep activation energy, has been observed. Upper critical field determined by resistive transition shows a relatively large anisotropy. The magneto-optical images reveal homogenous current flow within the crystal.
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Submitted 1 March, 2012;
originally announced March 2012.
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Instability of vortex-antivortex interface in optimally-doped Ba(Fe_{1-x}Co_{x})_{2}As_{2}
Authors:
Shyam Mohan,
Yuji Tsuchiya,
Yasuyuki Nakajima,
Tsuyoshi Tamegai
Abstract:
We explore the flux front patterns during virgin penetration and after remagnetization in the iron-based superconductor Ba(Fe_{1-x}Co_{x})_{2}As_{2}. After remagnetization we observe an instability characterized by turbulent dynamics at the vortex-antivortex boundary. Associated with the turbulent flux boundary a band of excess current density is observed. The turbulence is contrasted with the ins…
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We explore the flux front patterns during virgin penetration and after remagnetization in the iron-based superconductor Ba(Fe_{1-x}Co_{x})_{2}As_{2}. After remagnetization we observe an instability characterized by turbulent dynamics at the vortex-antivortex boundary. Associated with the turbulent flux boundary a band of excess current density is observed. The turbulence is contrasted with the instability observed in the cuprate superconductors. Our results suggest turbulent instability at the vortex-antivortex interface may be a common feature in all remagnetized type-II superconductors.
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Submitted 13 September, 2011;
originally announced September 2011.
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Magneto-optical imaging and transport properties of FeSe superconducting tapes prepared by diffusion method
Authors:
Q. P. Ding,
S. Mohan,
Y. Tsuchiya,
T. Taen,
Y. Nakajima,
T. Tamegai
Abstract:
High-quality FeSe tapes have been prepared by using a diffusion method. By adjusting the reaction temperature and the thickness systematically, a transport critical current density as high as 600 A/cm2 at 4.2 K under self field is achieved. Magneto-optical images indicate considerable distribution of Tc and weak-link features in the FeSe tape. This study gives some insight into how to improve the…
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High-quality FeSe tapes have been prepared by using a diffusion method. By adjusting the reaction temperature and the thickness systematically, a transport critical current density as high as 600 A/cm2 at 4.2 K under self field is achieved. Magneto-optical images indicate considerable distribution of Tc and weak-link features in the FeSe tape. This study gives some insight into how to improve the quality and performance of FeSe tapes and other superconducting tapes prepared through diffusion method further.
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Submitted 9 September, 2011;
originally announced September 2011.
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Improving the efficiency of organic light emitting diodes by use of a diluted light-emitting layer
Authors:
S. H. Mohan,
K. Garre,
N. Bhandari,
M. Cahay
Abstract:
The use of a thin mixed layer consisting of an inert diluent material and a light emitting material between the hole-transport layer and electron-transport layer of organic light-emitting diodes leads to an increase in the external quantum efficiency. The efficiency improvement is highly dependent on the thickness of the diluted light-emitting layer and driving current. Significant improvement see…
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The use of a thin mixed layer consisting of an inert diluent material and a light emitting material between the hole-transport layer and electron-transport layer of organic light-emitting diodes leads to an increase in the external quantum efficiency. The efficiency improvement is highly dependent on the thickness of the diluted light-emitting layer and driving current. Significant improvement seen at low current densities is explained in terms of effective hole confinement by the mixed layer while a modest decreases in efficiency at higher current densities may be attributed to luminescence quenching at the hole-transport layer/inert diluents material interface. The phenomena are demonstrated with three different inert diluents materials. A maximum external quantum efficiency improvement of about 40% is found for a diluted light-emitting layer thickness between 40 Å and 60 Å.
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Submitted 13 July, 2011;
originally announced July 2011.
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Low-temperature Synthesis of FeTe0.5Se0.5 Polycrystals with a High Transport Critical Current Density
Authors:
Qing-Ping Ding,
Shyam Mohan,
Yuji Tsuchiya,
Toshihiro Taen,
Yasuyuki Nakajima,
Tsuyoshi Tamegai
Abstract:
We have prepared high-quality polycrystalline FeTe0.5Se0.5 at temperature as low as 550°C. The transport critical current density evaluated by the current-voltage characteristics is over 700 A/cm2 at 4.2 K under zero field, which is several times larger than FeTe0.5Se0.5 superconducting wires. The critical current density estimated from magneto-optical images of flux penetration is also similar to…
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We have prepared high-quality polycrystalline FeTe0.5Se0.5 at temperature as low as 550°C. The transport critical current density evaluated by the current-voltage characteristics is over 700 A/cm2 at 4.2 K under zero field, which is several times larger than FeTe0.5Se0.5 superconducting wires. The critical current density estimated from magneto-optical images of flux penetration is also similar to this value. The upper critical field of the polycrystalline FeTe0.5Se0.5 at T = 0 K estimated by Werthamer-Helfand-Hohenberg theory is 585 kOe, which is comparable to that of single crystals. This study gives some insight into how to improve the performance of FeTe0.5Se0.5 superconducting wires.
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Submitted 9 March, 2011;
originally announced March 2011.
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Transport and magnetic properties of Co-doped BaFe_{2}As_{2} epitaxial thin films
Authors:
Shyam Mohan,
Toshihiro Taen,
Hidenori Yagyuda,
Yasuyuki Nakajima,
Tsuyoshi Tamegai,
Takayoshi Katase,
Hidenori Hiramatsu,
Hideo Hosono
Abstract:
We report resistivity, Hall coefficient, current-voltage characteristics, and magneto-optical imaging measurements of epitaxial Co-doped BaFe_{2}As_{2} thin films deposited on MgO(001) substrate. The Hall resistivity of the films has a substantial contribution arising from anomalous Hall effect of ferromagnetic components. The critical current density (J_{c}) of the films is ~2 MA/cm^{2} at low te…
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We report resistivity, Hall coefficient, current-voltage characteristics, and magneto-optical imaging measurements of epitaxial Co-doped BaFe_{2}As_{2} thin films deposited on MgO(001) substrate. The Hall resistivity of the films has a substantial contribution arising from anomalous Hall effect of ferromagnetic components. The critical current density (J_{c}) of the films is ~2 MA/cm^{2} at low temperatures. Differential magneto-optical images of the remanent state give similar J_{c} values and also exhibit presence of extended defects in the film.
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Submitted 2 August, 2010; v1 submitted 2 August, 2010;
originally announced August 2010.
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Driven weak to strong pinning crossover in partially nanopatterned 2H-NbSe2 single crystal
Authors:
Gorky Shaw,
Jaivardhan Sinha,
Shyam Mohan,
S. S. Banerjee
Abstract:
Investigations into the heterogeneous pinning properties of the vortex state created by partially nano-patterning single crystals of 2H-NbSe2 reveal an atypical magnetization response which is significantly drive dependent. Analysis of the magnetization response shows non-monotonic behavior of the magnetization relaxation rate with varying magnetic field sweep rate. With all the patterned pinning…
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Investigations into the heterogeneous pinning properties of the vortex state created by partially nano-patterning single crystals of 2H-NbSe2 reveal an atypical magnetization response which is significantly drive dependent. Analysis of the magnetization response shows non-monotonic behavior of the magnetization relaxation rate with varying magnetic field sweep rate. With all the patterned pinning centers saturated with vortices, we find that the pinning force experienced by the vortices continues to increase with increasing drive. Our studies reveal an unconventional dynamic weak to strong pinning crossover where the flow of the vortex state appears to be hindered or jammed as it is driven harder through the interstitial voids in the patterned pinning lattice.
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Submitted 31 May, 2010;
originally announced May 2010.
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Giant low frequency velocity fluctuations in a driven vortex lattice
Authors:
Shyam Mohan,
Jaivardhan Sinha,
S. S. Banerjee,
A. K. Sood,
S. Ramakrishnan,
A. K. Grover
Abstract:
The driven state of a well-ordered flux line lattice in a single crystal of 2H-NbSe2 in the time domain has revealed the presence of substantial fluctuations in velocity, with large and distinct time periods (~ seconds). A superposition of a periodic drive in the driven vortex lattice causes distinct changes in these fluctuations. We propose that prior to onset of the peak effect there exist hit…
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The driven state of a well-ordered flux line lattice in a single crystal of 2H-NbSe2 in the time domain has revealed the presence of substantial fluctuations in velocity, with large and distinct time periods (~ seconds). A superposition of a periodic drive in the driven vortex lattice causes distinct changes in these fluctuations. We propose that prior to onset of the peak effect there exist hithertofore unexplored regime of coherent dynamics, with unexpected behaviour in velocity fluctuations.
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Submitted 1 October, 2009;
originally announced October 2009.
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Monte Carlo simulation of charge transport in disordered organic systems using buffer lattice at boundary
Authors:
S. Raj Mohan,
Manoranjan P. Singh,
M. P. Joshi
Abstract:
In this article, we present an alternative method for simulating charge transport in disordered organic materials by using a buffer lattice at the boundary. This method does not require careful tracking of carrier's hopping pattern across boundaries. Suitability of this method is established by reproducing the field dependence of mobility, carrier relaxation and carrier diffusion in disordered org…
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In this article, we present an alternative method for simulating charge transport in disordered organic materials by using a buffer lattice at the boundary. This method does not require careful tracking of carrier's hopping pattern across boundaries. Suitability of this method is established by reproducing the field dependence of mobility, carrier relaxation and carrier diffusion in disordered organic systems obtained by simulating the charge transport for the full length of the systems along the field direction without and boundary condition. The significance of the buffer lattice is emphasized by simulating field dependence of mobility without using a buffer lattice, which results in negative field dependence of mobiltiy (NFDM) at low field regime due to the extra bias the carrier gains from the neglected hops and boundaries along field direction.
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Submitted 14 November, 2018; v1 submitted 8 September, 2009;
originally announced September 2009.
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Interacting nanopatterned pins: barriers towards creating interstitial vortices
Authors:
Gorky Shaw,
Shyam Mohan,
Jaivardhan Sinha,
S. S. Banerjee
Abstract:
We show that by nano-patterning a superconductor (NbSe2 single crystal) with an array of blind holes produces significant magnetic field sweep rate dependent metastable magnetization response. Our results are explained on the basis of a unique collective action of the blind holes pins which creates a barrier against vortex redistribution inside the sample. We propose that this barrier leads to a…
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We show that by nano-patterning a superconductor (NbSe2 single crystal) with an array of blind holes produces significant magnetic field sweep rate dependent metastable magnetization response. Our results are explained on the basis of a unique collective action of the blind holes pins which creates a barrier against vortex redistribution inside the sample. We propose that this barrier leads to a phase separation creating distinct population of vortices viz., those pinned on blind holes and those confined in the interstitials between the holes.
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Submitted 10 November, 2008;
originally announced November 2008.
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Criticality of tuning in athermal phase transitions
Authors:
U. Chandni,
Arindam Ghosh,
H. S. Vijaya,
S. Mohan
Abstract:
We experimentally address the importance of tuning in athermal phase transitions, which are triggered only by a slowly varying external field acting as tuning parameter. Using higher order statistics of fluctuations, a singular critical instability is detected for the first time in spite of an apparent universal self-similar kinetics over a broad range of driving force. The results as well as th…
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We experimentally address the importance of tuning in athermal phase transitions, which are triggered only by a slowly varying external field acting as tuning parameter. Using higher order statistics of fluctuations, a singular critical instability is detected for the first time in spite of an apparent universal self-similar kinetics over a broad range of driving force. The results as well as the experimental technique are likely to be of significance to many slowly driven non-equilibrium systems from geophysics to material science which display avalanche dynamics.
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Submitted 1 November, 2008;
originally announced November 2008.
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Signature of Martensite transformation on conductivity noise in thin films of NiTi shape memory alloys
Authors:
Chandni. U,
Arindam Ghosh,
H. S. Vijaya,
S. Mohan
Abstract:
Slow time-dependent fluctuations, or noise, in the electrical resistance of dc magnetron sputtered thin films of Nickel Titanium shape memory alloys have been measured. Even in equilibrium, the noise was several orders of magnitude larger than that of simple diffusive metallic films, and was found to be non-monotonic around the martensitic transformation regime. The results are discussed in term…
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Slow time-dependent fluctuations, or noise, in the electrical resistance of dc magnetron sputtered thin films of Nickel Titanium shape memory alloys have been measured. Even in equilibrium, the noise was several orders of magnitude larger than that of simple diffusive metallic films, and was found to be non-monotonic around the martensitic transformation regime. The results are discussed in terms of dynamics of structural defects, which also lay foundation to a new noise-based characterization scheme of martensite transformation.
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Submitted 1 November, 2008;
originally announced November 2008.
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Negative electric field dependence of mobility in TPD doped Polystyrene
Authors:
S. Raj Mohan,
M. P. Joshi,
Manoranjan P. Singh
Abstract:
A total negative field dependence of hole mobility down to low temperature was observed in N,N'-diphenyl-N,N'-bis(3-methylphenyl)-(1,1'-biphenyl)-4,4'diamine (TPD) doped in Polystyrene. The observed field dependence of mobility is explained on the basis of low values of energetic and positional disorder present in the sample. The low value of disorder is attributed to different morphology of the…
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A total negative field dependence of hole mobility down to low temperature was observed in N,N'-diphenyl-N,N'-bis(3-methylphenyl)-(1,1'-biphenyl)-4,4'diamine (TPD) doped in Polystyrene. The observed field dependence of mobility is explained on the basis of low values of energetic and positional disorder present in the sample. The low value of disorder is attributed to different morphology of the sample due to aggregation/crystallization of TPD. Monte Carlo simulations were also performed to understand the influence of aggregates on charge transport in disordered medium with correlated site energies. The simulation supports our experimental observations and justification on the basis of low values of disorder parameters.
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Submitted 24 July, 2008;
originally announced July 2008.
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Mapping giant magnetic fields around dense solid plasmas by high resolution magneto-optical microscopy
Authors:
Jaivardhan Sinha,
Shyam Mohan,
S. S. Banerjee,
Subhendu Kahaly,
G. Ravindra Kumar
Abstract:
We investigate distribution of magnetic fields around dense solid plasmas generated by intense p-polarized laser (~10^{16} W.cm^{-2}, 100 fs) irradiation of magnetic tapes, using high sensitivity magneto optical microscopy. We present evidence for giant axial magnetic fields and map out for the first time the spatial distribution of these fields. By using the axial magnetic field distribution as…
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We investigate distribution of magnetic fields around dense solid plasmas generated by intense p-polarized laser (~10^{16} W.cm^{-2}, 100 fs) irradiation of magnetic tapes, using high sensitivity magneto optical microscopy. We present evidence for giant axial magnetic fields and map out for the first time the spatial distribution of these fields. By using the axial magnetic field distribution as a diagnostic tool we uncover evidence for angular momentum associated with the plasma. We believe this study holds significance for investigating the process under which a magnetic material magnetizes or demagnetizes under the influence of ultrashort intense laser pulses.
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Submitted 4 October, 2007;
originally announced October 2007.
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Charge transport in disordered organic solids: A Monte Carlo simulation study on the effects of film morphology
Authors:
S. Raj Mohan,
M. P. Joshi,
Manoranjan P. Singh
Abstract:
The influence of ordered regions (micro crystallites and aggregates) in the other wise disordered polymer host matrix on field and temperature dependence of mobility (μ) has been simulated. Increase in concentration of ordered regions leads to increase in magnitude of mobility and in high field regime the saturation of the mobility occurs at lower electric field strength. The influence of differ…
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The influence of ordered regions (micro crystallites and aggregates) in the other wise disordered polymer host matrix on field and temperature dependence of mobility (μ) has been simulated. Increase in concentration of ordered regions leads to increase in magnitude of mobility and in high field regime the saturation of the mobility occurs at lower electric field strength. The influence of different mean and standard deviation of Gaussian density of states (DOS) of ordered regions on the field dependence of mobility was studied and found to be significant only at higher concentrations. Weak influence of these parameters at low concentrations are attributed to the strong interface effects due to the difference in the standard deviation of DOS of two regions (host and ordered region) and shallow trapping effect by ordered regions. For all the parameters of ordered regions under investigation the temperature dependence of mobility (logμ) and the slope of logμ Vs E^{1/2} plot show 1/T^2 dependence.
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Submitted 4 July, 2007;
originally announced July 2007.
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Instabilities in the vortex matter and the peak effect phenomenon
Authors:
Shyam Mohan,
Jaivardhan Sinha,
S. S. Banerjee,
Yuri Myasoedov
Abstract:
In single crystals of 2H-NbSe2, we identify for the first time a crossover from weak collective to strong pinning regime in the vortex state which is not associated with the peak effect phenomenon. Instead, we find the crossover is associated with anomalous history dependent magnetization response. In the field (Bdc) - temperature (T) vortex matter phase diagram we demarcate this pinning crossov…
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In single crystals of 2H-NbSe2, we identify for the first time a crossover from weak collective to strong pinning regime in the vortex state which is not associated with the peak effect phenomenon. Instead, we find the crossover is associated with anomalous history dependent magnetization response. In the field (Bdc) - temperature (T) vortex matter phase diagram we demarcate this pinning crossover boundary. We also delineate another boundary which separates the strong pinning region from a thermal fluctuation dominated regime, and find that PE appears on this boundary.
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Submitted 5 January, 2007;
originally announced January 2007.
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A frictional Cosserat model for the slow shearing of granular materials
Authors:
L. S. Mohan,
K. Kesava Rao,
Prabhu R. Nott
Abstract:
A rigid-plastic Cosserat model for slow frictional flow of granular materials, proposed by us in an earlier paper, has been used to analyze plane and cylindrical Couette flow. In this model, the hydrodynamic fields of a classical continuum are supplemented by the couple stress and the intrinsic angular velocity fields. The balance of angular momentum, which is satisfied implicitly in a classical…
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A rigid-plastic Cosserat model for slow frictional flow of granular materials, proposed by us in an earlier paper, has been used to analyze plane and cylindrical Couette flow. In this model, the hydrodynamic fields of a classical continuum are supplemented by the couple stress and the intrinsic angular velocity fields. The balance of angular momentum, which is satisfied implicitly in a classical continuum, must be enforced in a Cosserat continuum. As a result, the stress tensor could be asymmetric, and the angular velocity of a material point may differ from half the local vorticity. An important consequence of treating the granular medium as a Cosserat continuum is that it incorporates a material length scale in the model, which is absent in frictional models based on a classical continuum. Further, the Cosserat model allows determination of the velocity fields uniquely in viscometric flows, in contrast to classical frictional models. Experiments on viscometric flows of dense, slowly deforming granular materials indicate that shear is confined to a narrow region, usually a few grain diameters thick, while the remaining material is largely undeformed. This feature is captured by the present model, and the velocity profile predicted for cylindrical Couette flow is in good agreement with reported data. When the walls of the Couette cell are smoother than the granular material, the model predicts that the shear layer thickness is independent of the Couette gap $H$ when the latter is large compared to the grain diameter $d_p$. When the walls are of the same roughness as the granular material, the model predicts that the shear layer thickness varies as $(H/d_p)^{1/3}$ in the limit $(H/d_p) \gg 1$, for plane shear under gravity and cylindrical Couette flow.
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Submitted 27 July, 2001;
originally announced July 2001.
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A frictional Cosserat model for the flow of granular materials through a vertical channel
Authors:
L. Srinivasa Mohan,
Prabhu R. Nott,
K. Kesava Rao
Abstract:
A rigid-plastic Cosserat model has been used to study dense, fully developed flow of granular materials through a vertical channel. Frictional models based on the classical continuum do not predict the occurrence of shear layers, at variance with experimental observations. This feature has been attributed to the absence of a material length scale in their constitutive equations. The present mode…
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A rigid-plastic Cosserat model has been used to study dense, fully developed flow of granular materials through a vertical channel. Frictional models based on the classical continuum do not predict the occurrence of shear layers, at variance with experimental observations. This feature has been attributed to the absence of a material length scale in their constitutive equations. The present model incorporates such a material length scale by treating the granular material as a Cosserat continuum. Thus localised couple stresses exist and the stress tensor is asymmetric. The velocity profiles predicted by the model are in close agreement with available experimental data. The predicted dependence of the shear layer thickness on the width of the channel is in reasonable agreement with data. In the limit of the ratio of the particle diameter to the half-width of the channel being small, the model predicts that the shear layer thickness scaled by the particle diameter grows.
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Submitted 13 April, 1999;
originally announced April 1999.