Showing 1–50 of 71 results for author: Nandy, A

Reentrant localization transition, quantum butterfly and robust edge modes in aperiodic zig-zag ladder

Authors: Sayan Bhattacharya, Rhiddha Acharjee, Atanu Nandy

Abstract: Low dimensional tight-binding lattices in presence of quasiperiodic disorder generally exhibits localization transition. The system supports diffusive modes upto a limiting strength of disorder and all the eigenstates become localized beyond that critical strength thereby quenching the kinetic signature of the wavepacket. However, moving away from this situation, we demonstrate that with minimal l… ▽ More Low dimensional tight-binding lattices in presence of quasiperiodic disorder generally exhibits localization transition. The system supports diffusive modes upto a limiting strength of disorder and all the eigenstates become localized beyond that critical strength thereby quenching the kinetic signature of the wavepacket. However, moving away from this situation, we demonstrate that with minimal long-range off-diagonal modulation, the eigenspectrum again may offer delocalization of electronic states for some subtle combination of kinetic parameters of the Hamiltonian leading to a second quantum phase change. The localization transitions are associated with the obvious presence of single-particle mobility edges. Multifractal energy landscape also shows quantum butterfly pattern with the in-gap robust edge modes. The re-emerging localization transition is manifested through the evaluation of inverse participation ratio, eigenspectrum and a pertinent quantum dynamical study. △ Less

Submitted 4 July, 2026; originally announced July 2026.

Spin-reorientation as a switch for electronic topology in van der Waals ferromagnets

Authors: Satyabrata Bera, Sudipta Chatterjee, Suman Kalyan Pradhan, Subhadip Pradhan, Arnab Bera, Sk Kalimuddin, Ashis K. Nandy, Mintu Mondal

Abstract: The interplay between spin reorientation and topological electronic structure in two-dimensional (2D) van der Waals (vdW) ferromagnets is central to understanding how magnetic anisotropy shapes charge transport. Although spin-reorientation transitions (SRTs) are common in 2D metallic ferromagnets, their impact on electronic-topology-driven thermodynamic and transport properties remains largely une… ▽ More The interplay between spin reorientation and topological electronic structure in two-dimensional (2D) van der Waals (vdW) ferromagnets is central to understanding how magnetic anisotropy shapes charge transport. Although spin-reorientation transitions (SRTs) are common in 2D metallic ferromagnets, their impact on electronic-topology-driven thermodynamic and transport properties remains largely unexplored. Here we investigate this issue in Fe$_4$GeTe$_2$ (F4GT), a room-temperature quasi-2D vdW ferromagnet, using temperature-dependent magnetization, specific heat, magnetotransport, and thermoelectric measurements. Magnetization and specific heat establish a reorientation of the magnetic easy axis near $T_{\mathrm{SRT}} \sim 100$~K, in addition to ferromagnetic ordering at $T_C \sim 270$~K. Across the SRT, the Seebeck coefficient and anisotropic magnetoresistance show clear anomalies, indicating Fermi-surface reconstruction. The magnetoresistance exhibits a two-step field dependence: a low-field enhancement near the SRT associated with scattering from canted spins and evolving domains, followed by a higher-field negative response as spin fluctuations are suppressed. The simultaneous sign change of the ordinary Hall coefficient $R_0$ and the sharp anomaly in the anomalous Hall resistivity $ρ^{A}_{yx}$ further point to a temperature-driven modification of the underlying band topology. Analysis of the anomalous Hall conductivity $σ^{A}_{xy}$ and the scaling of $ρ^{A}_{yx}$ shows that the Berry-curvature-driven anomalous Hall response below $T_{\mathrm{SRT}}$ is strongly modified above the transition. Our results identify spin reorientation as an internal control parameter for switching between distinct topological transport regimes in a 2D vdW ferromagnet, providing a symmetry-controlled route to engineer spin-polarized electronic states and domain-texture-driven functionalities. △ Less

Submitted 20 March, 2026; originally announced March 2026.

Unusual magnetic and charge transport properties in In-Substituted Half-Metallic Kagome Ferromagnet Co3Sn2S2

Authors: Karan Singh, Subhadip Pradhan, K. Mukherjee, Ashis Kumar Nandy, Subhendra D. Mahanti, D. Topwal

Abstract: The kagome ferromagnet Co3Sn2S2 has been studied extensively for its unusual topology of electronic bands, origin of ferromagnetism and strong coupling between magnetism and charge transport. To understand the role of nonmagnetic element Sn, we have investigated magnetic, transport, and electronic structure of the isostructural compound Co3SnInS2, where all the Sn (divalent) atoms in the Co3Sn Kag… ▽ More The kagome ferromagnet Co3Sn2S2 has been studied extensively for its unusual topology of electronic bands, origin of ferromagnetism and strong coupling between magnetism and charge transport. To understand the role of nonmagnetic element Sn, we have investigated magnetic, transport, and electronic structure of the isostructural compound Co3SnInS2, where all the Sn (divalent) atoms in the Co3Sn Kagome layer are replaced by In (trivalent) atoms. We find long-range ferromagnetic order is nearly quenched in Co3SnInS2. The system exhibits predominantly antiferromagnetic correlations with only a very small net magnetic moment and turns ferromagnetic in the presence of an external magnetic field. Transport measurements show a semiconducting behaviour at low temperatures. Magnetoresistance shows a nonmonotonic field dependence, changing from negative to positive with increasing magnetic field. An anomalous Hall effect is observed, but its magnitude is significantly reduced compared to Co3Sn2S2 where the topological character of the Fermi surface plays a dominant role. These results indicate that substitution of Sn by In in the Co3Sn plane not only suppresses the topological electronic features of the transport electrons but drives the system away from the ferromagnetic Half-metallicity to an almost nonmagnetic semiconducting state with unusual paramagnetic response. Electronic structure calculations are consistent with some of these observations. △ Less

Submitted 3 March, 2026; originally announced March 2026.

Emergence of a hidden-order phase well below the charge density wave transition in a topological Weyl semimetal (TaSe$_4$)$_2$I

Authors: Sk Kalimuddin, Sudipta Chatterjee, Arnab Bera, Satyabrata Bera, Deep Singha Roy, Soham Das, Tuhin Debnath, Ashis K. Nandy, Shishir K. Pandey, Mintu Mondal

Abstract: The emergence of a charge density wave (CDW) in a Weyl semimetal -- a correlated topological phase, is exceptionally rare in condensed matter systems. In this context, the quasi-one-dimensional type-III Weyl semimetal (TaSe$_4$)$_2$I undergoes a CDW transition at $T_{\mathrm{CDW}} \approx 263$~K, providing an exceptional platform to investigate correlated topological CDW states. Here, we uncover a… ▽ More The emergence of a charge density wave (CDW) in a Weyl semimetal -- a correlated topological phase, is exceptionally rare in condensed matter systems. In this context, the quasi-one-dimensional type-III Weyl semimetal (TaSe$_4$)$_2$I undergoes a CDW transition at $T_{\mathrm{CDW}} \approx 263$~K, providing an exceptional platform to investigate correlated topological CDW states. Here, we uncover an additional hidden-order phase transition at $T^* \sim 100$ K, well below the CDW onset, using low-frequency resistance noise spectroscopy, electrical transport, and thermoelectric measurements. This transition is characterized by a sharp enhancement in the noise exponent ($α$) and variance of resistance fluctuations. Analysis of higher-order statistics of resistance fluctuations reveals the correlated dynamics underlying the transition. A pronounced anomaly in the Seebeck coefficient near $T^*$ further suggests a Fermi surface reconstruction. First-principles calculations reveal a structural distortion from the high-symmetry $I422$ phase to a low-symmetry $C2$ phase, via an intermediate $I4$ symmetry. This leads to renormalization of the electronic structure near the Fermi level and opening of a bandgap in the hidden-order phase. These findings demonstrate a previously unidentified correlated phase transition in the topological CDW-Weyl semimetal (TaSe$_4$)$_2$I, enriching the phase diagram of this material and establishing it as an ideal platform for studying intertwined electronic and structural orders. △ Less

Submitted 9 January, 2026; v1 submitted 19 December, 2025; originally announced December 2025.

Comments: 15 pages including 11 figures (6 main and 5 supporting)

Journal ref: Phys. Rev. B 113, 045114 (2026)

Evaluating Large Language Models in Scientific Discovery

Authors: Zhangde Song, Jieyu Lu, Yuanqi Du, Botao Yu, Thomas M. Pruyn, Yue Huang, Kehan Guo, Xiuzhe Luo, Yuanhao Qu, Yi Qu, Yinkai Wang, Haorui Wang, Jeff Guo, Jingru Gan, Parshin Shojaee, Di Luo, Andres M Bran, Gen Li, Qiyuan Zhao, Shao-Xiong Lennon Luo, Yuxuan Zhang, Xiang Zou, Wanru Zhao, Yifan F. Zhang, Wucheng Zhang , et al. (31 additional authors not shown)

Abstract: Large language models (LLMs) are increasingly applied to scientific research, yet prevailing science benchmarks probe decontextualized knowledge and overlook the iterative reasoning, hypothesis generation, and observation interpretation that drive scientific discovery. We introduce a scenario-grounded benchmark that evaluates LLMs across biology, chemistry, materials, and physics, where domain exp… ▽ More Large language models (LLMs) are increasingly applied to scientific research, yet prevailing science benchmarks probe decontextualized knowledge and overlook the iterative reasoning, hypothesis generation, and observation interpretation that drive scientific discovery. We introduce a scenario-grounded benchmark that evaluates LLMs across biology, chemistry, materials, and physics, where domain experts define research projects of genuine interest and decompose them into modular research scenarios from which vetted questions are sampled. The framework assesses models at two levels: (i) question-level accuracy on scenario-tied items and (ii) project-level performance, where models must propose testable hypotheses, design simulations or experiments, and interpret results. Applying this two-phase scientific discovery evaluation (SDE) framework to state-of-the-art LLMs reveals a consistent performance gap relative to general science benchmarks, diminishing return of scaling up model sizes and reasoning, and systematic weaknesses shared across top-tier models from different providers. Large performance variation in research scenarios leads to changing choices of the best performing model on scientific discovery projects evaluated, suggesting all current LLMs are distant to general scientific "superintelligence". Nevertheless, LLMs already demonstrate promise in a great variety of scientific discovery projects, including cases where constituent scenario scores are low, highlighting the role of guided exploration and serendipity in discovery. This SDE framework offers a reproducible benchmark for discovery-relevant evaluation of LLMs and charts practical paths to advance their development toward scientific discovery. △ Less

Submitted 7 May, 2026; v1 submitted 17 December, 2025; originally announced December 2025.

The interplay of magnetic order with the electronic scattering and crystal-field effects in a metallic ferromagnet

Authors: Payel Shee, Tanaya Halder, Chia-Jung Yang, Nainish Tickoo, Ratiranjan Samal, Ruta Kulkarni, Shishir K. Pandey, Vikas Kashid, Ashis K. Nandy, Arumugam Thamizhavel, Anamitra Mukherjee, Shovon Pal

Abstract: The interplay between magnetic order, charge dynamics, and crystal field excitations underpins the emergent ground states of rare-earth intermetallics. Using time-domain terahertz spectroscopy, we probe this coupling in PrSi, a metallic ferromagnet. The optical response exhibits pronounced Drude-Smith behavior over a broad temperature range, indicating persistent carrier scattering. A classical Ko… ▽ More The interplay between magnetic order, charge dynamics, and crystal field excitations underpins the emergent ground states of rare-earth intermetallics. Using time-domain terahertz spectroscopy, we probe this coupling in PrSi, a metallic ferromagnet. The optical response exhibits pronounced Drude-Smith behavior over a broad temperature range, indicating persistent carrier scattering. A classical Kondo-lattice model (CKLM) attributes this non-Drude conductivity to scattering of itinerant electrons by localized magnetic moments, persisting down to temperatures well below the magnetic ordering scale. At lower temperatures, beyond the scope of CKLM, our experiment reveals that the response is dominated by crystal-field excitations, with sharp transitions at 0.6 THz and 1.54 THz. The mode at 1.54 THz shows a dynamic correlation with the onset of ferromagnetic order, marking the onset of a crystal-field-governed low temperature regime. △ Less

Submitted 15 December, 2025; originally announced December 2025.

Localization, transport, flux induced extended modes and mobility edge in a self-similar corral substrate

Authors: Sayan Bhattacharya, Rhiddha Acharjee, Atanu Nandy

Abstract: We address that a single-band tight-binding Hamiltonian defined on a self-similar corral substrate can give rise to a set of non-diffusive localized modes that follow the same hierarchical distribution. As the lattice, the spatial extent of quantum prison containing a cluster of atomic sites is dependent on the generation of fractal structure. Apart from the quantum imprisonment of the excitation,… ▽ More We address that a single-band tight-binding Hamiltonian defined on a self-similar corral substrate can give rise to a set of non-diffusive localized modes that follow the same hierarchical distribution. As the lattice, the spatial extent of quantum prison containing a cluster of atomic sites is dependent on the generation of fractal structure. Apart from the quantum imprisonment of the excitation, a magnetic flux threading each elementary plaquette is shown to destroy the boundedness and generate an absolutely continuous sub-band populated by resonant eigen functions. Flux induced engineering of quantum states is corroborated through the evaluation of inverse participation ratio and quantum transport. Moreover, the robustness of the extended states has been checked in presence of diagonal disorder and off-diagonal anisotropy. Flux modulated single-particle mobility edge is characterized through mutlifractal analysis. Quantum interference is the essential issue, reported here, that manipulates the kinematics of the excitation and this is manifested by the workout of persistent current. △ Less

Submitted 6 December, 2025; originally announced December 2025.

Quantum Spin Hall Effect and Su-Schrieffer-Heeger Model Implementation in Novel C3N-based Dumbbell Morphologies

Authors: Deep Mondal, Arka Bandyopadhyay, Atanu Nandy, Debnarayan Jana

Abstract: Two-dimensional carbon nitride materials have been the center of attention for their diverse usage in energy harvesting, environmental remediation and nanoelectronic applications. A broad range of utilities with decent synthetic plausibility have made this family a sweet spot to dive into, whereas the underlying analytical aspects are yet to have prominence. Recently, using the machinaries of firs… ▽ More Two-dimensional carbon nitride materials have been the center of attention for their diverse usage in energy harvesting, environmental remediation and nanoelectronic applications. A broad range of utilities with decent synthetic plausibility have made this family a sweet spot to dive into, whereas the underlying analytical aspects are yet to have prominence. Recently, using the machinaries of first principles, we reported a family of six different structures C3NX with a unique dumbbell-shaped morphology, functionalizing the recently synthesized monolayer of C3N. Here we have critically explored the non-trivial topological phases of the semimetallic Dumbbell C3NX sheets and nanoribbons. Spin-orbit coupling induced gap across the Fermi level, its subsequent tuning via an external electric field, portrayal of band inversion from the Berry curvature distribution and the evaluation of topological index using the Wannier charge center (WCC) firmly establishes the traces of topological footprint. The real space decimation scheme and Green function technique evaluate the underlying spectral information with corresponding transport characteristics. Fascinating features of these quasi-1D systems are observed utilizing the Su-Schrieffer-Heeger (SSH) model where different twisted phases reveal distinct topological signatures even in a low atomic mass system like DB C4N. △ Less

Submitted 6 December, 2025; originally announced December 2025.

Report number: Volume 40, October 2024, 102360

Paradoxical Topological Soliton Lattice in Anisotropic Frustrated Chiral Magnets

Authors: Sayan Banik, Nikolai S. Kiselev, Ashis K. Nandy

Abstract: Two-dimensional chiral magnets are known to host a variety of skyrmions, characterized by an integer topological charge. However, these systems typically favor uniform lattices as a thermodynamically stable phase composed of either skyrmions (Q = -1) or antiskyrmions (Q = 1). In isotropic chiral magnets, skyrmion-antiskyrmion coexistence is typically transient due to mutual annihilation, making th… ▽ More Two-dimensional chiral magnets are known to host a variety of skyrmions, characterized by an integer topological charge. However, these systems typically favor uniform lattices as a thermodynamically stable phase composed of either skyrmions (Q = -1) or antiskyrmions (Q = 1). In isotropic chiral magnets, skyrmion-antiskyrmion coexistence is typically transient due to mutual annihilation, making the observation of a stable, long-range ordered lattice a significant challenge. Here, we address this challenge by demonstrating a skyrmion-antiskyrmion lattice as a magnetic field-induced topological ground state in chiral magnets with competing anisotropic interactions, specifically Dzyaloshinskii-Moriya and frustrated exchange interactions. This unique lattice exhibits a net-zero global topological charge due to the balanced populations of skyrmions and antiskyrmions. Furthermore, density functional theory and spin-lattice simulations identify 2Fe/InSb(110) as an ideal candidate material for realizing this phase. This finding reveals new possibilities for manipulating magnetic solitons and establishes anisotropic frustrated chiral magnets as a promising material class for future spintronic applications. △ Less

Submitted 26 October, 2025; originally announced October 2025.

Journal ref: Adv. Sci. 13, no. 5: e14568 (2026)

Skyrmion-Antiskyrmion Lattice: A Net-Zero Topological Phase in Low-Symmetry Frustrated Chiral Magnets

Authors: Sayan Banik, Ashis K. Nandy

Abstract: We report the discovery of a thermodynamically stable skyrmion-antiskyrmion lattice in two-dimensional heterostructures, a novel state exhibiting a net-zero global topological charge owing to an equal population of skyrmions and antiskyrmions. This surprising coexistence of oppositely charged solitons remarkably circumvents their anticipated annihilation. We demonstrate the formation and evolution… ▽ More We report the discovery of a thermodynamically stable skyrmion-antiskyrmion lattice in two-dimensional heterostructures, a novel state exhibiting a net-zero global topological charge owing to an equal population of skyrmions and antiskyrmions. This surprising coexistence of oppositely charged solitons remarkably circumvents their anticipated annihilation. We demonstrate the formation and evolution of this phase in Fe films on C1v -symmetric (110) surfaces of GaAs and CdTe semiconductors. Specifically, we reveal a series of magnetic field-induced phase transitions: cycloidal spin-spiral to skyrmion-antiskyrmion lattice to conical spin-spiral to ferromagnet. The remarkable stability of the net-zero lattice is attributed to symmetry-enforced anisotropic magnetic interactions. Lowering interfacial symmetry to C1v thus enables frustrated chiral magnets, uniquely manifesting in thermodynamically stable net-zero topological soliton lattices, as revealed by our findings. △ Less

Submitted 17 September, 2025; originally announced September 2025.

Journal ref: Physical Review B 112, L140404 (2025)

The Rise of Generative AI for Metal-Organic Framework Design and Synthesis

Authors: Chenru Duan, Aditya Nandy, Shyam Chand Pal, Xin Yang, Wenhao Gao, Yuanqi Du, Hendrik Kraß, Yeonghun Kang, Varinia Bernales, Zuyang Ye, Tristan Pyle, Ray Yang, Zeqi Gu, Philippe Schwaller, Shengqian Ma, Shijing Sun, Alán Aspuru-Guzik, Seyed Mohamad Moosavi, Robert Wexler, Zhiling Zheng

Abstract: Advances in generative artificial intelligence are transforming how metal-organic frameworks (MOFs) are designed and discovered. This Perspective introduces the shift from laborious enumeration of MOF candidates to generative approaches that can autonomously propose and synthesize in the laboratory new porous reticular structures on demand. We outline the progress of employing deep learning models… ▽ More Advances in generative artificial intelligence are transforming how metal-organic frameworks (MOFs) are designed and discovered. This Perspective introduces the shift from laborious enumeration of MOF candidates to generative approaches that can autonomously propose and synthesize in the laboratory new porous reticular structures on demand. We outline the progress of employing deep learning models, such as variational autoencoders, diffusion models, and large language model-based agents, that are fueled by the growing amount of available data from the MOF community and suggest novel crystalline materials designs. These generative tools can be combined with high-throughput computational screening and even automated experiments to form accelerated, closed-loop discovery pipelines. The result is a new paradigm for reticular chemistry in which AI algorithms more efficiently direct the search for high-performance MOF materials for clean air and energy applications. Finally, we highlight remaining challenges such as synthetic feasibility, dataset diversity, and the need for further integration of domain knowledge. △ Less

Submitted 15 August, 2025; originally announced August 2025.

Comments: 10 pages, 5 figures

Journal ref: Matter (2026)

Field-free superconducting diode effect in two-dimensional Shiba lattices

Authors: Sayak Bhowmik, Dibyendu Samanta, Ashis K. Nandy, Arijit Saha, Sudeep Kumar Ghosh

Abstract: The superconducting diode effect (SDE) refers to non-reciprocal transport, where current flows without resistance in one direction but becomes resistive in the opposite direction, but its typical reliance on magnetic field hinders scalability and device integration. In this article, we present a theoretical framework for realizing a field-free SDE based on a two-dimensional (2D) Shiba lattice feat… ▽ More The superconducting diode effect (SDE) refers to non-reciprocal transport, where current flows without resistance in one direction but becomes resistive in the opposite direction, but its typical reliance on magnetic field hinders scalability and device integration. In this article, we present a theoretical framework for realizing a field-free SDE based on a two-dimensional (2D) Shiba lattice featuring a conical spin texture. Using the real-space Bogoliubov-de Gennes (BdG) calculations, we illustrate that the conical spin configuration alone is sufficient to break the necessary inversion and time reversal symmetries, enabling nonreciprocal supercurrent flow without any external magnetic field, yielding diode efficiency exceeding 40%. Furthermore, we find that the efficiency of such a diode effect becomes strongly dependent on the direction of current flow, revealing a pronounced angular dependence that can be tuned by varying the pitches of the spin texture along the two spatial lattice directions. Our findings offer a pathway toward scalable, field-free superconducting components for non-dissipative electronics and quantum technologies. △ Less

Submitted 14 August, 2025; originally announced August 2025.

Comments: 9 pages, 5 figures, Supplementary material is included, Comments are welcome

Emergent Quasiparticles \& Field-Tuned RIXS Spectra in a Trimerized Spin-1/2 Chain

Authors: Subhajyoti Pal, Pradeep Thakur, Ashis Kumar Nandy, Anamitra Mukherjee

Abstract: We investigate spin-flip excitations in the spin-1/2 trimer chain $\rm{Cu_3(P_2O_6OH)_2}$, featuring an antiferromagnetic exchange motif $J_1$-$J_1$-$J_2$ with $J_1 < J_2$. Using density matrix renormalization group (DMRG) simulations, we demonstrate that single-spin-flip processes induced by resonant inelastic X-ray scattering (RIXS) generate emergent gapless modes governed by the underlying trim… ▽ More We investigate spin-flip excitations in the spin-1/2 trimer chain $\rm{Cu_3(P_2O_6OH)_2}$, featuring an antiferromagnetic exchange motif $J_1$-$J_1$-$J_2$ with $J_1 < J_2$. Using density matrix renormalization group (DMRG) simulations, we demonstrate that single-spin-flip processes induced by resonant inelastic X-ray scattering (RIXS) generate emergent gapless modes governed by the underlying trimer periodicity alongside distinct high-energy excitations. By combining exact diagonalization and real-space renormalization group (RG) techniques, we attribute these features to fractionalized spinons and composite quasiparticles arising from one- and two-trimer excitations. Furthermore, we show that multi-spin RIXS excitations yield experimentally distinguishable spectral signatures of composite modes absent in single-spin-flip spectra. At the field-induced 1/3 magnetization plateau, single-spin-flip RIXS spectra evolves with the magnetic field to favor spin-polarized composite quasiparticles. This trend culminates in a gapless spectrum of spin-1 excitations beyond the plateau, paving the way for field-tuned Bose condensation of composite modes. △ Less

Submitted 29 May, 2025; originally announced May 2025.

Building-Block Aware Generative Modeling for 3D Crystals of Metal Organic Frameworks

Authors: Chenru Duan, Aditya Nandy, Sizhan Liu, Yuanqi Du, Liu He, Yi Qu, Haojun Jia, Jin-Hu Dou

Abstract: Metal-organic frameworks (MOFs) marry inorganic nodes, organic edges, and topological nets into programmable porous crystals, yet their astronomical design space defies brute-force synthesis. Generative modeling holds ultimate promise, but existing models either recycle known building blocks or are restricted to small unit cells. We introduce Building-Block-Aware MOF Diffusion (BBA MOF Diffusion),… ▽ More Metal-organic frameworks (MOFs) marry inorganic nodes, organic edges, and topological nets into programmable porous crystals, yet their astronomical design space defies brute-force synthesis. Generative modeling holds ultimate promise, but existing models either recycle known building blocks or are restricted to small unit cells. We introduce Building-Block-Aware MOF Diffusion (BBA MOF Diffusion), an SE(3)-equivariant diffusion model that learns 3D all-atom representations of individual building blocks, encoding crystallographic topological nets explicitly. Trained on the CoRE-MOF database, BBA MOF Diffusion readily samples MOFs with unit cells containing 1000 atoms with great geometric validity, novelty, and diversity mirroring experimental databases. Its native building-block representation produces unprecedented metal nodes and organic edges, expanding accessible chemical space by orders of magnitude. One high-scoring [Zn(1,4-TDC)(EtOH)2] MOF predicted by the model was synthesized, where powder X-ray diffraction, thermogravimetric analysis, and N2 sorption confirm its structural fidelity. BBA-Diff thus furnishes a practical pathway to synthesizable and high-performing MOFs. △ Less

Submitted 13 May, 2025; originally announced May 2025.

Anomalous Hall and Nernst effect switching via staggered rotation in a kagome antiferromagnetic semimetal

Authors: Subhadip Pradhan, Kartik Samanta, Ashis K. Nandy

Abstract: The intricate interplay between magnetism and the topology of electronic structures provides a rich avenue for tailoring materials with unique and potent anomalous transport properties. In this paper, we present a strategy for inducing robust Berry curvature and anomalous transverse conductivity in noncollinear antiferromagnets through an unconventional approach termed ``small \textit{staggered ro… ▽ More The intricate interplay between magnetism and the topology of electronic structures provides a rich avenue for tailoring materials with unique and potent anomalous transport properties. In this paper, we present a strategy for inducing robust Berry curvature and anomalous transverse conductivity in noncollinear antiferromagnets through an unconventional approach termed ``small \textit{staggered rotation} of spin". Considering noncollinear Mn$_3$Sn, we demonstrate that the positive vector chirality antiferromagnetic configuration, typically associated with a vanishing anomalous Hall effect and Nernst effect, can be manipulated to exhibit finite anomalous Hall conductivity (AHC) and anomalous Nernst conductivity (ANC) through \textit{staggered rotation}. Furthermore, we illustrate that the value and sign of both the AHC and ANC can be tuned through \textit{staggered rotation}. This tuning is intricately influenced by the spin-orbit coupling (SOC) induced gapped nodal line, revealing the critical role of electronic structure modifications in achieving precise control over transport properties. △ Less

Submitted 3 December, 2024; originally announced December 2024.

Comments: 9 pages, 7 figures

Non-equilibrium active noise enhances generative memory in diffusion models

Authors: Agnish Kumar Behera, Alexandra Lamtyugina, Aditya Nandy, Daiki Goto, Carlos Floyd, Suriyanarayanan Vaikuntanathan

Abstract: Generative diffusion models have emerged as powerful tools for sampling high-dimensional distributions, yet they typically rely on white gaussian noise and noise schedules to destroy and reconstruct information. Here, we demonstrate that driving the generative process out of equilibrium using active, temporally correlated noise sources fundamentally alters the information thermodynamics of the sys… ▽ More Generative diffusion models have emerged as powerful tools for sampling high-dimensional distributions, yet they typically rely on white gaussian noise and noise schedules to destroy and reconstruct information. Here, we demonstrate that driving the generative process out of equilibrium using active, temporally correlated noise sources fundamentally alters the information thermodynamics of the system. We show that coupling the data to an active non-Markovian bath creates a `memory effect' where high-level semantic information (such as class identity or molecular metastability) is stored in the temporal correlations of auxiliary degrees of freedom. Using Fisher information analysis, we prove that this active mechanism significantly retards the rate of information decay compared to passive Brownian motion. Crucially, this memory effect facilitates an earlier and more robust symmetry breaking (speciation) during the reverse generative process, allowing the system to resolve multi-scale structures, reminiscent of metastable states in molecular configurations that are washed out in the typical noising processes. Our results suggest that non-equilibrium protocols, inspired by active matter physics, offer a thermodynamically distinct and potentially advantageous pathway for recovering high-dimensional energy landscapes using generative diffusion. △ Less

Submitted 28 January, 2026; v1 submitted 11 November, 2024; originally announced November 2024.

Comments: 24 pages, 15 figures

Unified strategy of flat band engineering, electronic transport and other spectral properties for different kagome ribbon variants

Authors: Atanu Nandy

Abstract: We address the problem of flat band engineering in different prototypes of quasi-one dimensional kagome network through a generalized analytical proposition worked out within the tight-binding formalism. Exact fabrication of single particle eigenstates with localized as well as diffusive modes is reported through the demonstration of such unified methodology by virtue of a simple real space decima… ▽ More We address the problem of flat band engineering in different prototypes of quasi-one dimensional kagome network through a generalized analytical proposition worked out within the tight-binding formalism. Exact fabrication of single particle eigenstates with localized as well as diffusive modes is reported through the demonstration of such unified methodology by virtue of a simple real space decimation formalism in such interesting variants of ribbon shaped geometry. The description provides a common platform to investigate the band dispersion including the overall spectral portrait and associated physical aspects of those quasi-one dimensional lattices. Exact detection of dispersionless flat band mode and its tunability are reported as a direct consequence of the analytical prescription. Analytical work out is justified through the numerical evaluation of density of eigenstates, electronic transmission behavior, inverse participation ratio, persistent current study, Aharanov-Bohm oscillation in the transmittance and other related issues. An obvious analogous extension in the context photonics concludes our description. △ Less

Submitted 2 November, 2024; originally announced November 2024.

Comments: 15 pages, 22 eps figures

Current-induced spin polarisation in Rashba-Dresselhaus systems under different point groups

Authors: Akash Dey, Ashis K. Nandy, Kush Saha

Abstract: Non-magnetic materials without inversion symmetry typically exhibit strong Rashba spin-orbit coupling (SOC), enabling the well-known Rashba Edelstein effect where an external electrical current induces transverse spin polarisation. In this study, we demonstrate that electrically induced spin polarisation in non-magnetic materials, for example, electronic systems within quantum-well geometries, can… ▽ More Non-magnetic materials without inversion symmetry typically exhibit strong Rashba spin-orbit coupling (SOC), enabling the well-known Rashba Edelstein effect where an external electrical current induces transverse spin polarisation. In this study, we demonstrate that electrically induced spin polarisation in non-magnetic materials, for example, electronic systems within quantum-well geometries, can significantly be influenced by the system's point-group symmetries, such as $C_n$ and $C_{nv}$. These symmetries allow various linear and higher-order momentum, $k-$varying SOC Hamiltonian. Specifically, we show that surfaces having $C_{n}$ point-group symmetry, which permits specific linear and cubic Rashba and Dresselhaus SOC terms, can lead to both orthogonal and non-orthogonal spin polarisations with respect to the applied field. In contrast, surfaces with $C_{nv}$ symmetry exhibit only transverse spin polarisation, regardless of the linear and cubic SOC terms. We further find contrasting spin polarisation for cubic-in-$k$ SOC as compared to the linear-in-$k$ SOC when energy is varied, for example, through doping. Additionally, we show that the surfaces with $C_{n}$ symmetry may exhibit persistent spin current, depending on the relative strength between different momentum-dependent SOC terms. Our finding emphasizes the significance of crystal symmetry in understanding and manipulating induced spin polarisation in noncentrosymmetric materials, especially in surface/interface systems. △ Less

Submitted 12 December, 2024; v1 submitted 9 August, 2024; originally announced August 2024.

Comments: 27 pages, 8 figures

Journal ref: New J. Phys. 27 013024 (2025)

Optimizing one dimensional superconducting diodes: Interplay of Rashba spin-orbit coupling and magnetic fields

Authors: Sayak Bhowmik, Dibyendu Samanta, Ashis K. Nandy, Arijit Saha, Sudeep Kumar Ghosh

Abstract: The superconducting diode effect (SDE) refers to the non-reciprocal nature of the critical current (maximum current that a superconductor can withstand before turning into a normal metal) of a superconducting device. Here, we investigate SDE in helical superconductors with broken inversion and time-reversal symmetry, focusing on a prototypical Rashba nanowire device proximitized by an s-wave super… ▽ More The superconducting diode effect (SDE) refers to the non-reciprocal nature of the critical current (maximum current that a superconductor can withstand before turning into a normal metal) of a superconducting device. Here, we investigate SDE in helical superconductors with broken inversion and time-reversal symmetry, focusing on a prototypical Rashba nanowire device proximitized by an s-wave superconductor and subjected to external magnetic fields. Using a self-consistent Bogoliubov-de Gennes mean-field formalism, we analyze the interplay between linear and higher-order spin-orbit coupling (SOC), bulk supercurrents, and external magnetic fields. Our results demonstrate that Rashba nanowires with only linear SOC can achieve incredibly large diode efficiencies > 45% through the interplay of longitudinal and transverse magnetic fields. Notably, higher-order SOC introduces qualitatively different behavior, enabling finite diode efficiency even in the absence of a longitudinal Zeeman field due to inherent energy dispersion asymmetry. We present a comprehensive phase diagram of the device elucidating the emergent Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) superconducting state and demonstrate that proximitized Rashba nanowires offer a versatile, practical platform for SDE, with potential realizations in existing material systems. These results provide crucial insights for optimizing SDE in nanoscale superconducting devices, paving the way for next-generation dissipationless quantum electronics. △ Less

Submitted 24 July, 2024; v1 submitted 17 July, 2024; originally announced July 2024.

Comments: 9 pages, 8 figures. Comments are welcome

Journal ref: Commun Phys 8, 260 (2025)

Terahertz crystal electric field transitions in a Kondo-lattice antiferromagnet

Authors: Payel Shee, Chia-Jung Yang, Shishir Kumar Pandey, Ashis Kumar Nandy, Ruta Kulkarni, Arumugam Thamizhavel, Manfred Fiebig, Shovon Pal

Abstract: Hybridization between the localized f-electrons and the delocalized conduction electrons together with the crystal electric field (CEF) play a determinant role in governing the many-body ground state of a correlated-electron system. Here, we investigate the low-energy CEF states in CeAg_2Ge_2, a prototype Kondo-lattice antiferromagnet where Kondo correlation is found to exist within the antiferrom… ▽ More Hybridization between the localized f-electrons and the delocalized conduction electrons together with the crystal electric field (CEF) play a determinant role in governing the many-body ground state of a correlated-electron system. Here, we investigate the low-energy CEF states in CeAg_2Ge_2, a prototype Kondo-lattice antiferromagnet where Kondo correlation is found to exist within the antiferromagnetic phase. Using time-domain THz reflection spectroscopy, we show the first direct evidence of two low-energy CEF transitions at 0.6 THz (2.5 meV) and 2.1 THz (8.7 meV). The presence of low-frequency infrared-active phonon modes further manifests as a Fano-modified lineshape of the 2.1 THz CEF conductivity peak. The temporal spectral weights obtained directly from the THz time traces, in addition, corroborate the corresponding CEF temperature scales of the compound. △ Less

Submitted 30 January, 2024; originally announced January 2024.

Comments: 10 pages, 6 figures

Pressure-Driven Transitions in La2CoTiO6: Antiferromagnetic Insulator to Nonmagnetic Metal via Antiferromagnetic Metal in a Double Perovskite Oxide

Authors: Sromona Nandi, Subhadip Pradhan, Ashis K. Nandy, Rudra Sekhar Manna

Abstract: In double perovskite oxides (A$_2$BB$^\prime$O$_6$), magnetism often arises from diluted magnetic lattices, created by combining a perovskite structure with localized 3$d$ magnetic elements (B) alongside another perovskite lattice containing nearly nonmagnetic delocalized 4$d$/$5d$ elements (B$^\prime$). Alternatively, the magnetic lattice can consist entirely of 3$d$ elements, with one being comp… ▽ More In double perovskite oxides (A$_2$BB$^\prime$O$_6$), magnetism often arises from diluted magnetic lattices, created by combining a perovskite structure with localized 3$d$ magnetic elements (B) alongside another perovskite lattice containing nearly nonmagnetic delocalized 4$d$/$5d$ elements (B$^\prime$). Alternatively, the magnetic lattice can consist entirely of 3$d$ elements, with one being completely nonmagnetic with $d^0$ state. La$_2$CoTiO$_6$ (LCTO), a representative double perovskite oxide, contains Ti in a nonmagnetic state with a $d^0$ electron configuration due to its $4^+$ oxidation state. Experimental evidence shows that LCTO possesses a monoclinic structure (space group $P2_1/n$) and behaves as an antiferromagnet with a Néel temperature of 14.6 K. Through first-principle electronic structure calculations, we uncover that adjusting external hydrostatic pressure induces a sequence of phase transitions: from antiferromagnetic insulator (AFM-I) to antiferromagnetic metal (AFM-M), and ultimately to itinerant nonmagnetic metal (NM-M). The transition from AFM-I to AFM-M at $\sim$ 42 GPa pressure coincides with a shift in spin states, moving from a high-spin (HS) state to a low-spin (LS) state, while Co retains a $d^7$ configuration. Distortion within the monoclinic structure under pressure plays a pivotal role in the spin-state transition. At the AFM-I to AFM-M transition, we observe a sharp decrease in the ratio of the octahedral volumes occupied by Co and Ti. Such change in ratio is linked to variations in octahedral volumes, akin to a breathing mode distortion. We explore the impact of the breathing mode distortion by examining a highly symmetric theoretical structure (space-group $I4/mmm$), achieved by optimizing the structure with all $\angle${Co-O-Ti} angles set to 180$^{\circ}$. △ Less

Submitted 26 July, 2024; v1 submitted 9 October, 2023; originally announced October 2023.

Journal ref: Phys. Rev. B 110, 085101 (2024)

Second-order topological superconductor via noncollinear magnetic texture

Authors: Pritam Chatterjee, Arnob Kumar Ghosh, Ashis K. Nandy, Arijit Saha

Abstract: We put forth a theoretical framework for engineering a two-dimensional (2D) second-order topological superconductor (SOTSC) by utilizing a heterostructure: incorporating noncollinear magnetic textures between an $s$-wave superconductor and a 2D quantum spin Hall insulator. It stabilizes the higher order topological superconducting phase, resulting in Majorana corner modes (MCMs) at four corners of… ▽ More We put forth a theoretical framework for engineering a two-dimensional (2D) second-order topological superconductor (SOTSC) by utilizing a heterostructure: incorporating noncollinear magnetic textures between an $s$-wave superconductor and a 2D quantum spin Hall insulator. It stabilizes the higher order topological superconducting phase, resulting in Majorana corner modes (MCMs) at four corners of a 2D domain. The calculated non-zero quadrupole moment characterizes the bulk topology. Subsequently, through a unitary transformation, an effective low-energy Hamiltonian reveals the effects of magnetic textures, resulting in an effective in-plane Zeeman field and spin-orbit coupling. This approach provides a qualitative depiction of the topological phase, substantiated by numerical validation within exact real-space model. Analytically calculated effective pairings in the bulk illuminate the microscopic behavior of the SOTSC. The comprehension of MCM emergence is supported by a low-energy edge theory, which is attributed to the interplay between effective pairings of $(p_x + p_y)$-type and $(p_x + i p_y)$-type. Our extensive study paves the way for practically attaining the SOTSC phase by integrating noncollinear magnetic textures. △ Less

Submitted 29 January, 2024; v1 submitted 24 August, 2023; originally announced August 2023.

Comments: This is the published version

Journal ref: Phys. Rev. B (Letter) 109, L041409 (2024)

Anomalous Hall effect induced by Berry curvature in topological nodal-line van der Waals ferromagnet Fe$_4$GeTe$_2$

Authors: Satyabrata Bera, Sudipta Chatterjee, Subhadip Pradhan, Suman Kalyan Pradhan, Sk Kalimuddin, Arnab Bera, Ashis K. Nandy, Mintu Mondal

Abstract: The exploration of nontrivial transport phenomena associated with the interplay between magnetic order and spin-orbit coupling (SOC), particularly in van der Waals (vdW) systems has gained a resurgence of interest due to their easy exfoliation, ideal for two-dimensional (2D) spintronics. We report the near room temperature quasi-2D ferromagnet, Fe$_4$GeTe$_2$ from the iron-based vdW family (Fe… ▽ More The exploration of nontrivial transport phenomena associated with the interplay between magnetic order and spin-orbit coupling (SOC), particularly in van der Waals (vdW) systems has gained a resurgence of interest due to their easy exfoliation, ideal for two-dimensional (2D) spintronics. We report the near room temperature quasi-2D ferromagnet, Fe$_4$GeTe$_2$ from the iron-based vdW family (Fe$_n$GeTe$_2$, $n$=3,4,5), exhibiting a large anomalous Hall conductivity (AHC), $σ^A_{xy}$ $\sim$ 490 $Ω^{-1}\textrm{cm}^{-1}$ at 2 K. The near quadratic behavior of anomalous Hall resistivity ($ρ^{A}_{xy}$) with the longitudinal resistivity ($ρ_{xx}$) suggests that a dominant AHC contribution is coming from an intrinsic Berry curvature (BC) mechanism. Concomitantly, the electronic structure calculations reveal a large BC arising from SOC induced gaped nodal lines around the Fermi level, governing such large AHC property. Moreover, we also report an exceptionally large anomalous Hall angle ($\simeq$ 10.6\%) and Hall factor ($\simeq$ 0.22 V$^{-1}$) values which so far, are the largest in compared to those for other members in this vdW family. △ Less

Submitted 18 August, 2023; originally announced August 2023.

Comments: 7 pages, 4 figures, supplementary

Localization property of a periodic chain of atoms with aperiodically coupled quantum dots

Authors: Atanu Nandy

Abstract: The spectral landscape and the transport property of a translationally invariant network with side-coupled quantum dots are demonstrated within the tight-binding framework. For periodic environment band structure is demonstrated analytically in details. Moreover, if the side-coupling here follows a typical quasiperiodic Aubry-Andre-Harper type of modulation then such off-diagonal disorder invites… ▽ More The spectral landscape and the transport property of a translationally invariant network with side-coupled quantum dots are demonstrated within the tight-binding framework. For periodic environment band structure is demonstrated analytically in details. Moreover, if the side-coupling here follows a typical quasiperiodic Aubry-Andre-Harper type of modulation then such off-diagonal disorder invites an exotic spectral feature for this model quantum system. We perform an in-depth numerical analysis followed by the evaluation of the density of eigenstates and the inverse participation ratio. The description shows that this network creates a typical self-similar kind of multifractal pattern in the energy landscape. The impacts of the strength of such aperiodic connectivity and the slowness parameter are reported in this analysis. In the present era of advanced technology and lithography techniques all such non-trivial results definitely throw an achievable challenge to the experimentalists to study the localization of excitation in such network △ Less

Submitted 20 March, 2023; originally announced March 2023.

Comments: 5 pages (brief communication as conference publication), Proceedings of International Conference on Recent Trends in Physics and Allied Sciences, Vol. No. 1, Page-73-77 (2023), ISBN-978-93-89817-84-3

Topological Superconductivity by Engineering Noncollinear Magnetism in Magnet/ Superconductor Heterostructures: A Realistic Prescription for 2D Kitaev Model

Authors: Pritam Chatterjee, Sayan Banik, Sandip Bera, Arnob Kumar Ghosh, Saurabh Pradhan, Arijit Saha, Ashis K. Nandy

Abstract: We report on a realistic and rather general scheme where noncollinear magnetic textures proximitized with the most common $s$-wave superconductor can appear as the alternative to $p$-wave superconductor{--}the prime proposal to realize two-dimensional (2D) Kitaev model for topological superconductors (TSCs) hosting Majorana flat edge mode (MFEM). A general minimal Hamiltonian suitable for magnet/s… ▽ More We report on a realistic and rather general scheme where noncollinear magnetic textures proximitized with the most common $s$-wave superconductor can appear as the alternative to $p$-wave superconductor{--}the prime proposal to realize two-dimensional (2D) Kitaev model for topological superconductors (TSCs) hosting Majorana flat edge mode (MFEM). A general minimal Hamiltonian suitable for magnet/superconductor heterostructures reveals robust MFEM within the gap of Shiba bands due to the emergence of an effective ``$p_x+p_y$"-type $p$-wave pairing, spatially localized at the edges of a 2D magnetic domain of spin-spiral. We finally verify this concept by considering Mn (Cr) monolayer grown on a $s$-wave superconducting substrate, Nb(110) under strain (Nb(001)). In both 2D cases, the antiferromagnetic spin-spiral solutions exhibit robust MFEM at certain domain edges that is beyond the scope of the trivial extension of 1D spin-chain model in 2D. This approach, particularly when the MFEM appears in the TSC phase for such heterostructure materials, offers a perspective to extend the realm of the TSC in 2D. △ Less

Submitted 12 March, 2024; v1 submitted 7 March, 2023; originally announced March 2023.

Comments: This is the published version

Journal ref: Phys. Rev. B (Letter) 109, L121301 (2024)

Tunable caging of excitation in decorated Lieb-ladder geometry with long range connectivity

Authors: Atanu Nandy

Abstract: Controlled Aharonov-Bohm caging of wave train is reported in a quasi-one dimensional version of Lieb geometry with next nearest neighbor hopping integral within the tight-binding framework. This longer wavelength fluctuation is considered by incorporating periodic, quasi-periodic or fractal kind of geometry inside the skeleton of the original network. This invites exotic eigenspectrum displaying a… ▽ More Controlled Aharonov-Bohm caging of wave train is reported in a quasi-one dimensional version of Lieb geometry with next nearest neighbor hopping integral within the tight-binding framework. This longer wavelength fluctuation is considered by incorporating periodic, quasi-periodic or fractal kind of geometry inside the skeleton of the original network. This invites exotic eigenspectrum displaying a distribution of flat band states. Also a subtle modulation of external magnetic flux leads to a comprehensive control over those non-resonant modes. Real space renormalization group method provides us an exact analytical prescription for the study of such tunable imprisonment of excitation. The non-trivial tunability of external agent is important as well as challenging in the context of experimental perspective. △ Less

Submitted 2 January, 2023; originally announced January 2023.

Comments: 11 pages, 25 eps figures

Higher order exchange driven noncoplanar magnetic state and large anomalous Hall effects in electron doped kagome magnet Mn$_3$Sn

Authors: Charanpreet Singh, Sk Jamaluddin, Ashis K. Nandy, Masashi Tokunaga, Maxim Avdeev, Ajaya K. Nayak

Abstract: Owing to the geometrical frustration, Mn$_3 $Sn exhibits a 120$^{\circ}$ in-plane triangular antiferromagnetic (AFM) order with a large anomalous Hall effect (AHE). Here, we present a combined theoretical and experimental study to demonstrate that the in-plane AFM structure in Mn$_3 $Sn can be significantly modified to a tunable noncoplanar magnetic state by suitable electron doping. With the help… ▽ More Owing to the geometrical frustration, Mn$_3 $Sn exhibits a 120$^{\circ}$ in-plane triangular antiferromagnetic (AFM) order with a large anomalous Hall effect (AHE). Here, we present a combined theoretical and experimental study to demonstrate that the in-plane AFM structure in Mn$_3 $Sn can be significantly modified to a tunable noncoplanar magnetic state by suitable electron doping. With the help of Density Functional Theory calculations we show that the presence of higher-order exchange interactions in the system leads to the stabilization of the noncoplanar magnetic ground state, which is further established by neutron diffraction study in the Fe-doped Mn$_3 $Sn sample. Interestingly, we find a large scalar spin chirality (SSC) induced topological AHE that can be significantly tuned with the degree of non-coplanarity. We carry out 60~T magnetic and Hall resistivity measurements to demonstrate the contribution of SSC to the observed AHE. We also illustrate a simultaneous manipulation of dual order in the system, where the AHE arising from the in-plane 120$^{\circ}$ triangular AFM order can switch its sign without affecting the AHE generated by the SSC. The present study opens up a new direction to explore novel quantum phenomena associated with the coexistence of multiple orders. △ Less

Submitted 23 November, 2022; originally announced November 2022.

Journal ref: npj Quantum Mater. 9, 43 (2024)

A Database of Ultrastable MOFs Reassembled from Stable Fragments with Machine Learning Models

Authors: Aditya Nandy, Shuwen Yue, Changhwan Oh, Chenru Duan, Gianmarco G. Terrones, Yongchul G. Chung, Heather J. Kulik

Abstract: High-throughput screening of large hypothetical databases of metal-organic frameworks (MOFs) can uncover new materials, but their stability in real-world applications is often unknown. We leverage community knowledge and machine learning (ML) models to identify MOFs that are thermally stable and stable upon activation. We separate these MOFs into their building blocks and recombine them to make a… ▽ More High-throughput screening of large hypothetical databases of metal-organic frameworks (MOFs) can uncover new materials, but their stability in real-world applications is often unknown. We leverage community knowledge and machine learning (ML) models to identify MOFs that are thermally stable and stable upon activation. We separate these MOFs into their building blocks and recombine them to make a new hypothetical MOF database of over 50,000 structures that samples orders of magnitude more connectivity nets and inorganic building blocks than prior databases. This database shows an order of magnitude enrichment of ultrastable MOF structures that are stable upon activation and more than one standard deviation more thermally stable than the average experimentally characterized MOF. For the nearly 10,000 ultrastable MOFs, we compute bulk elastic moduli to confirm these materials have good mechanical stability, and we report methane deliverable capacities. Our work identifies privileged metal nodes in ultrastable MOFs that optimize gas storage and mechanical stability simultaneously. △ Less

Submitted 25 October, 2022; originally announced October 2022.

Low-cost machine learning approach to the prediction of transition metal phosphor excited state properties

Authors: Gianmarco Terrones, Chenru Duan, Aditya Nandy, Heather J. Kulik

Abstract: Photoactive iridium complexes are of broad interest due to their applications ranging from lighting to photocatalysis. However, the excited state property prediction of these complexes challenges ab initio methods such as time-dependent density functional theory (TDDFT) both from an accuracy and a computational cost perspective, complicating high throughput virtual screening (HTVS). We instead lev… ▽ More Photoactive iridium complexes are of broad interest due to their applications ranging from lighting to photocatalysis. However, the excited state property prediction of these complexes challenges ab initio methods such as time-dependent density functional theory (TDDFT) both from an accuracy and a computational cost perspective, complicating high throughput virtual screening (HTVS). We instead leverage low-cost machine learning (ML) models to predict the excited state properties of photoactive iridium complexes. We use experimental data of 1,380 iridium complexes to train and evaluate the ML models and identify the best-performing and most transferable models to be those trained on electronic structure features from low-cost density functional theory tight binding calculations. Using these models, we predict the three excited state properties considered, mean emission energy of phosphorescence, excited state lifetime, and emission spectral integral, with accuracy competitive with or superseding TDDFT. We conduct feature importance analysis to identify which iridium complex attributes govern excited state properties and we validate these trends with explicit examples. As a demonstration of how our ML models can be used for HTVS and the acceleration of chemical discovery, we curate a set of novel hypothetical iridium complexes and identify promising ligands for the design of new phosphors. △ Less

Submitted 18 September, 2022; originally announced September 2022.

Observation of anisotropic Dirac cones in the topological material Ti2Te2P

Authors: Gyanendra Dhakal, Firoza Kabir, Ashis K. Nandy, Alex Aperis, Anup Pradhan Sakhya, Subhadip Pradhan, Klauss Dimitri, Christopher Sims, Sabin Regmi, M. Mofazzel Hosen, Yangyang Liu, Luis Persaud, Dariusz Kaczorowski, Peter M. Oppeneer, Madhab Neupane

Abstract: Anisotropic bulk Dirac (or Weyl) cones in three dimensional systems have recently gained intense research interest as they are examples of materials with tilted Dirac (or Weyl) cones indicatig the violation of Lorentz invariance. In contrast, the studies on anisotropic surface Dirac cones in topological materials which contribute to anisotropic carrier mobility have been limited. By employing angl… ▽ More Anisotropic bulk Dirac (or Weyl) cones in three dimensional systems have recently gained intense research interest as they are examples of materials with tilted Dirac (or Weyl) cones indicatig the violation of Lorentz invariance. In contrast, the studies on anisotropic surface Dirac cones in topological materials which contribute to anisotropic carrier mobility have been limited. By employing angle-resolved photoemission spectroscopy and first-principles calculations, we reveal the anisotropic surface Dirac dispersion in a tetradymite material Ti2Te2P on the (001) plane of the Brillioun zone. We observe the quasi-elliptical Fermi pockets at the M -point of the Brillouin zone forming the anisotropic surface Dirac cones. Our calculations of the Z2 indices confirm that the system is topologically non-trivial with multiple topological phases in the same material. In addition, the observed nodal-line like feature formed by bulk bands makes this system topologically rich. △ Less

Submitted 15 September, 2022; originally announced September 2022.

Comments: 21 pages, 17 figures, Supplementary Information included

Journal ref: Phys. Rev. B 106, 125124 (2022)

Ligand additivity relationships enable efficient exploration of transition metal chemical space

Authors: Naveen Arunachalam, Stefan Gugler, Michael G. Taylor, Chenru Duan, Aditya Nandy, Jon Paul Janet, Ralf Meyer, Jonas Oldenstaedt, Daniel B. K. Chu, Heather J. Kulik

Abstract: To accelerate exploration of chemical space, it is necessary to identify the compounds that will provide the most additional information or value. A large-scale analysis of mononuclear octahedral transition metal complexes deposited in an experimental database confirms an under-representation of lower-symmetry complexes. From a set of around 1000 previously studied Fe(II) complexes, we show that t… ▽ More To accelerate exploration of chemical space, it is necessary to identify the compounds that will provide the most additional information or value. A large-scale analysis of mononuclear octahedral transition metal complexes deposited in an experimental database confirms an under-representation of lower-symmetry complexes. From a set of around 1000 previously studied Fe(II) complexes, we show that the theoretical space of synthetically accessible complexes formed from the relatively small number of unique ligands is significantly (ca. 816k) larger. For the properties of these complexes, we validate the concept of ligand additivity by inferring heteroleptic properties from a stoichiometric combination of homoleptic complexes. An improved interpolation scheme that incorporates information about cis and trans isomer effects predicts the adiabatic spin-splitting energy to around 2 kcal/mol and the HOMO level to less than 0.2 eV. We demonstrate a multi-stage strategy to discover leads from the 816k Fe(II) complexes within a targeted property region. We carry out a coarse interpolation from homoleptic complexes that we refine over a subspace of ligands based on the likelihood of generating complexes with targeted properties. We validate our approach on 9 new binary and ternary complexes predicted to be in a targeted zone of discovery, suggesting opportunities for efficient transition metal complex discovery. △ Less

Submitted 12 September, 2022; originally announced September 2022.

Active Learning Exploration of Transition Metal Complexes to Discover Method-Insensitive and Synthetically Accessible Chromophores

Authors: Chenru Duan, Aditya Nandy, Gianmarco Terrones, David W. Kastner, Heather J. Kulik

Abstract: Transition metal chromophores with earth-abundant transition metals are an important design target for their applications in lighting and non-toxic bioimaging, but their design is challenged by the scarcity of complexes that simultaneously have optimal target absorption energies in the visible region as well as well-defined ground states. Machine learning (ML) accelerated discovery could overcome… ▽ More Transition metal chromophores with earth-abundant transition metals are an important design target for their applications in lighting and non-toxic bioimaging, but their design is challenged by the scarcity of complexes that simultaneously have optimal target absorption energies in the visible region as well as well-defined ground states. Machine learning (ML) accelerated discovery could overcome such challenges by enabling screening of a larger space, but is limited by the fidelity of the data used in ML model training, which is typically from a single approximate density functional. To address this limitation, we search for consensus in predictions among 23 density functional approximations across multiple rungs of Jacobs ladder. To accelerate the discovery of complexes with absorption energies in the visible region while minimizing MR character, we use 2D efficient global optimization to sample candidate low-spin chromophores from multi-million complex spaces. Despite the scarcity (i.e., approx. 0.01\%) of potential chromophores in this large chemical space, we identify candidates with high likelihood (i.e., > 10\%) of computational validation as the ML models improve during active learning, representing a 1,000-fold acceleration in discovery. Absorption spectra of promising chromophores from time-dependent density functional theory verify that 2/3 of candidates have the desired excited state properties. The observation that constituent ligands from our leads have demonstrated interesting optical properties in the literature exemplifies the effectiveness of our construction of a realistic design space and active learning approach. △ Less

Submitted 15 September, 2022; v1 submitted 10 August, 2022; originally announced August 2022.

A Transferable Recommender Approach for Selecting the Best Density Functional Approximations in Chemical Discovery

Authors: Chenru Duan, Aditya Nandy, Ralf Meyer, Naveen Arunachalam, Heather J. Kulik

Abstract: Approximate density functional theory (DFT) has become indispensable owing to its cost-accuracy trade-off in comparison to more computationally demanding but accurate correlated wavefunction theory. To date, however, no single density functional approximation (DFA) with universal accuracy has been identified, leading to uncertainty in the quality of data generated from DFT. With electron density f… ▽ More Approximate density functional theory (DFT) has become indispensable owing to its cost-accuracy trade-off in comparison to more computationally demanding but accurate correlated wavefunction theory. To date, however, no single density functional approximation (DFA) with universal accuracy has been identified, leading to uncertainty in the quality of data generated from DFT. With electron density fitting and transfer learning, we build a DFA recommender that selects the DFA with the lowest expected error with respect to gold standard but cost-prohibitive coupled cluster theory in a system-specific manner. We demonstrate this recommender approach on vertical spin-splitting energy evaluation for challenging transition metal complexes. Our recommender predicts top-performing DFAs and yields excellent accuracy (ca. 2 kcal/mol) for chemical discovery, outperforming both individual transfer learning models and the single best functional in a set of 48 DFAs. We demonstrate the transferability of the DFA recommender to experimentally synthesized compounds with distinct chemistry. △ Less

Submitted 21 July, 2022; originally announced July 2022.

Tailoring phase transition from topological superconductor to trivial superconductor induced by magnetic textures of a spin-chain on a $p$-wave superconductor

Authors: Pritam Chatterjee, Saurabh Pradhan, Ashis K. Nandy, Arijit Saha

Abstract: We theoretically investigate the phase transition from a non-trivial topological $p$-wave superconductor to a trivial $s$-wave like superconducting phase through a gapless phase, driven by different magnetic textures as an one-dimensional spin-chain impurity, e.g. Bloch-type, in-plane and out-of-plane Néel-type spin-chains etc. In our proposal, the chain of magnetic impurities is placed on a spin-… ▽ More We theoretically investigate the phase transition from a non-trivial topological $p$-wave superconductor to a trivial $s$-wave like superconducting phase through a gapless phase, driven by different magnetic textures as an one-dimensional spin-chain impurity, e.g. Bloch-type, in-plane and out-of-plane Néel-type spin-chains etc. In our proposal, the chain of magnetic impurities is placed on a spin-triplet $p$-wave superconductor where we obtain numerically as well as analytically an effective $s$-wave like pairing due to spin rotation, resulting in gradual destruction of the Majorana zero modes present in the topological superconducting phase. In particular, when the impurity spins are antiferromagnetically aligned i.e. spiral wave vector $G_{s}=π$, the system becomes an effective $s$-wave superconductor without Majorana zero modes in the local density of states. The Shiba bands, on the other hand, formed due to the overlapping of Yu-Shiba-Rusinov states play a crucial role in this topological to trivial superconductor phase transition, confirmed by the sign change in the minigap within the Shiba bands. We also characterize this topological phase transition via gap closing and winding number analysis. Moreover, interference of the Shiba bands exhibiting oscillatory behavior within the superconducting gap, $-Δ_{p}$ to $Δ_{p}$, as a function of $G_{s}$, also reflects an important evidence for the formation of an effective $s$-wave pairing. Such oscillation is absent in the $p$-wave regime. △ Less

Submitted 5 March, 2023; v1 submitted 30 June, 2022; originally announced June 2022.

Comments: This is the published version

Journal ref: Phys. Rev. B 107, 085423 (2023)

Vector Chirality $κ$ Driven Topological Phase Transition and the Associated Anomalous Hall Conductivity Tuning in a Non-Collinear Antiferromagnet

Authors: Subhadip Pradhan, Kartik Samanta, Kush Saha, Ashis K. Nandy

Abstract: Based on the first-principles electronic structure calculations and subsequent symmetry adapted effective low-energy $\textbf{k.p}$ theory, we show the switching of the vector chirality, $κ$, in a noncollinear antiferromagnet (AFM), Mn$_3$Sn, as an unconventional route to topological phase transition from a nodal-ring to a Weyl point semimetal. Specifically, we find that the switching of $κ$ leads… ▽ More Based on the first-principles electronic structure calculations and subsequent symmetry adapted effective low-energy $\textbf{k.p}$ theory, we show the switching of the vector chirality, $κ$, in a noncollinear antiferromagnet (AFM), Mn$_3$Sn, as an unconventional route to topological phase transition from a nodal-ring to a Weyl point semimetal. Specifically, we find that the switching of $κ$ leads to gaping out an elliptic nodal-ring everywhere at the Fermi-level except for a pair of points on the ring. As a consequence, the topological phase transition switches the anomalous Hall conductivity (AHC) from zero to a giant value. Furthermore, we theoretically demonstrate how the controlled manipulation of the chiral AFM order keeping $κ$ unaltered favors unusual rotation of Weyl-points on the ring. This in turn enables us to tune in-plane components of the AHC by a collective uniform rotations of spins in the AFM unit cell. △ Less

Submitted 27 September, 2023; v1 submitted 30 June, 2022; originally announced June 2022.

Comments: 6 pages, 3 figures

Journal ref: Commun Phys 6, 272 (2023)

Putting Density Functional Theory to the Test in Machine-Learning-Accelerated Materials Discovery

Authors: Chenru Duan, Fang Liu, Aditya Nandy, Heather J. Kulik

Abstract: Accelerated discovery with machine learning (ML) has begun to provide the advances in efficiency needed to overcome the combinatorial challenge of computational materials design. Nevertheless, ML-accelerated discovery both inherits the biases of training data derived from density functional theory (DFT) and leads to many attempted calculations that are doomed to fail. Many compelling functional ma… ▽ More Accelerated discovery with machine learning (ML) has begun to provide the advances in efficiency needed to overcome the combinatorial challenge of computational materials design. Nevertheless, ML-accelerated discovery both inherits the biases of training data derived from density functional theory (DFT) and leads to many attempted calculations that are doomed to fail. Many compelling functional materials and catalytic processes involve strained chemical bonds, open-shell radicals and diradicals, or metal-organic bonds to open-shell transition-metal centers. Although promising targets, these materials present unique challenges for electronic structure methods and combinatorial challenges for their discovery. In this Perspective, we describe the advances needed in accuracy, efficiency, and approach beyond what is typical in conventional DFT-based ML workflows. These challenges have begun to be addressed through ML models trained to predict the results of multiple methods or the differences between them, enabling quantitative sensitivity analysis. For DFT to be trusted for a given data point in a high-throughput screen, it must pass a series of tests. ML models that predict the likelihood of calculation success and detect the presence of strong correlation will enable rapid diagnoses and adaptation strategies. These "decision engines" represent the first steps toward autonomous workflows that avoid the need for expert determination of the robustness of DFT-based materials discoveries. △ Less

Submitted 5 May, 2022; originally announced May 2022.

Journal ref: Journal of Physical Chemistry Letters, 2021, 12, 19, 4628-4637

Ligand Additivity and Divergent Trends in Two Types of Delocalization Errors from Approximate Density Functional Theory

Authors: Yael Cytter, Aditya Nandy, Akash Bajaj, Heather J. Kulik

Abstract: Despite its widespread use, the predictive accuracy of density functional theory (DFT) is hampered by delocalization errors, especially for correlated systems such as transition-metal complexes. Two complementary tuning strategies have been developed to reduce delocalization error: eliminating the global curvature with respect to charge addition or removal, and computing a linear response Hubbard… ▽ More Despite its widespread use, the predictive accuracy of density functional theory (DFT) is hampered by delocalization errors, especially for correlated systems such as transition-metal complexes. Two complementary tuning strategies have been developed to reduce delocalization error: eliminating the global curvature with respect to charge addition or removal, and computing a linear response Hubbard U as a measure of local curvature at the metal center at fixed charge and applying it to the transition-metal complex in a DFT+U framework. We investigate the relationship between the two measures of delocalization error as we manipulate the ligand field strength by varying the number of strong-field ligands in a series of heteroleptic complexes or by geometrically constraining the metal-ligand bond length in homoleptic octahedral complexes. We show that across these sets of complexes with varying ligand fields, an inverse relationship generally exists between global and local curvatures. We find that effects of ligand substitution on both measures of delocalization are typically additive, but the two quantities seldom coincide. The observation of ligand additivity suggests opportunities for evaluating errors on homoleptic complexes to infer corrections for lower-symmetry complexes. △ Less

Submitted 7 April, 2022; originally announced April 2022.

Machine learning models predict calculation outcomes with the transferability necessary for computational catalysis

Authors: Chenru Duan, Aditya Nandy, Husain Adamji, Yuriy Roman-Leshkov, Heather J. Kulik

Abstract: Virtual high throughput screening (VHTS) and machine learning (ML) have greatly accelerated the design of single-site transition-metal catalysts. VHTS of catalysts, however, is often accompanied with high calculation failure rate and wasted computational resources due to the difficulty of simultaneously converging all mechanistically relevant reactive intermediates to expected geometries and elect… ▽ More Virtual high throughput screening (VHTS) and machine learning (ML) have greatly accelerated the design of single-site transition-metal catalysts. VHTS of catalysts, however, is often accompanied with high calculation failure rate and wasted computational resources due to the difficulty of simultaneously converging all mechanistically relevant reactive intermediates to expected geometries and electronic states. We demonstrate a dynamic classifier approach, i.e., a convolutional neural network that monitors geometry optimization on the fly, and exploit its good performance and transferability for catalyst design. We show that the dynamic classifier performs well on all reactive intermediates in the representative catalytic cycle of the radical rebound mechanism for methane-to-methanol despite being trained on only one reactive intermediate. The dynamic classifier also generalizes to chemically distinct intermediates and metal centers absent from the training data without loss of accuracy or model confidence. We rationalize this superior model transferability to the use of on-the-fly electronic structure and geometric information generated from density functional theory calculations and the convolutional layer in the dynamic classifier. Combined with model uncertainty quantification, the dynamic classifier saves more than half of the computational resources that would have been wasted on unsuccessful calculations for all reactive intermediates being considered. △ Less

Submitted 2 March, 2022; originally announced March 2022.

Defect Modulated Band Modification in Ion Implanted MgO Crystal: Experimental and Ab Initio Calculations

Authors: Sourav Bhakta, Subhadip Pradhan, Ashis K. Nandy, Pratap K. Sahoo

Abstract: Defects creation and annihilation is a fundamental concept in device fabrication. This report studies the optical bandgap modification in MgO by MeV Ni ion irradiation-induced defect states between valance and conduction band. Ion implantation on MgO single crystal produces substitutional defect states along with F (anionic vacancy center), $F_2$, other oxygen vacancy center and V (cationic vacanc… ▽ More Defects creation and annihilation is a fundamental concept in device fabrication. This report studies the optical bandgap modification in MgO by MeV Ni ion irradiation-induced defect states between valance and conduction band. Ion implantation on MgO single crystal produces substitutional defect states along with F (anionic vacancy center), $F_2$, other oxygen vacancy center and V (cationic vacancy center) centers confirmed from absorption and photoluminescence spectra that can be applied as filament in valance charge memory based resistive random access memories. The variation of optical bandgap with Ni ion fluences is ascertained by modifying the electronic band structure. Density Functional Theory (DFT) calculation assists in understanding the evolution of electronic band structure for vacancies and substitutional defects consisting of MgO structures. △ Less

Submitted 14 February, 2022; originally announced February 2022.

Microscopic Origin Of Room Temperature Ferromagnetism in a Double Perovskite Sr$_2$FeReO$_6$: a first principle and model Hamiltonian study

Authors: Shishir K. Pandey, Ashis K. Nandy, Poonam Kumari, Priya Mahadevan

Abstract: The puzzling observation of room temperature ferromagnetism in double perovskites (A$_2$BB$'$O$_6$), despite having the magnetic lattice of B-ions diluted by non-magnetic B$'$-ions, have been examined for Sr$_2$FeReO$_6$. {\it Ab-initio} spin spiral electronic structure calculations along various high symmetry directions in reciprocal space are used to determine the exchange interactions entering… ▽ More The puzzling observation of room temperature ferromagnetism in double perovskites (A$_2$BB$'$O$_6$), despite having the magnetic lattice of B-ions diluted by non-magnetic B$'$-ions, have been examined for Sr$_2$FeReO$_6$. {\it Ab-initio} spin spiral electronic structure calculations along various high symmetry directions in reciprocal space are used to determine the exchange interactions entering an extended Heisenberg model, which is then solved classically using Monte Carlo simulations to determine the ferromagnetic transition temperature T$_c$. We find that one must consider onsite Coulomb interactions at the nonmagnetic Re sites ($U$) in order to obtain a T$_c$ close to the experimental value. Analysis of the $ab$-$initio$ electronic structure as well as an appropriate model Hamiltonian trace the origin of enhancement in T$_c$ with $U$ to the enhanced exchange splitting that is introduced at these sites. This in turn destabilizes the antiferromagnetic exchange channels, thereby enhancing the T$_c$. The role of occupancy at the non-magnetic sites is examined by contrasting with the case of Sr$_2$FeMoO$_6$. △ Less

Submitted 2 February, 2022; originally announced February 2022.

Two Wrongs Can Make a Right: A Transfer Learning Approach for Chemical Discovery with Chemical Accuracy

Authors: Chenru Duan, Daniel B. K. Chu, Aditya Nandy, Heather J. Kulik

Abstract: Appropriately identifying and treating molecules and materials with significant multi-reference (MR) character is crucial for achieving high data fidelity in virtual high throughput screening (VHTS). Nevertheless, most VHTS is carried out with approximate density functional theory (DFT) using a single functional. Despite development of numerous MR diagnostics, the extent to which a single value of… ▽ More Appropriately identifying and treating molecules and materials with significant multi-reference (MR) character is crucial for achieving high data fidelity in virtual high throughput screening (VHTS). Nevertheless, most VHTS is carried out with approximate density functional theory (DFT) using a single functional. Despite development of numerous MR diagnostics, the extent to which a single value of such a diagnostic indicates MR effect on chemical property prediction is not well established. We evaluate MR diagnostics of over 10,000 transition metal complexes (TMCs) and compare to those in organic molecules. We reveal that only some MR diagnostics are transferable across these materials spaces. By studying the influence of MR character on chemical properties (i.e., MR effect) that involves multiple potential energy surfaces (i.e., adiabatic spin splitting, $ΔE_\mathrm{H-L}$, and ionization potential, IP), we observe that cancellation in MR effect outweighs accumulation. Differences in MR character are more important than the total degree of MR character in predicting MR effect in property prediction. Motivated by this observation, we build transfer learning models to directly predict CCSD(T)-level adiabatic $ΔE_\mathrm{H-L}$ and IP from lower levels of theory. By combining these models with uncertainty quantification and multi-level modeling, we introduce a multi-pronged strategy that accelerates data acquisition by at least a factor of three while achieving chemical accuracy (i.e., 1 kcal/mol) for robust VHTS. △ Less

Submitted 11 January, 2022; originally announced January 2022.

Molecular orbital projectors in non-empirical jmDFT recover exact conditions in transition metal chemistry

Authors: Akash Bajaj, Chenru Duan, Aditya Nandy, Michael G. Taylor, Heather J. Kulik

Abstract: Low-cost, non-empirical corrections to semi-local density functional theory are essential for accurately modeling transition metal chemistry. Here, we demonstrate the judiciously-modified density functional theory (jmDFT) approach with non-empirical U and J parameters obtained directly from frontier orbital energetics on a series of transition metal complexes. We curate a set of nine representativ… ▽ More Low-cost, non-empirical corrections to semi-local density functional theory are essential for accurately modeling transition metal chemistry. Here, we demonstrate the judiciously-modified density functional theory (jmDFT) approach with non-empirical U and J parameters obtained directly from frontier orbital energetics on a series of transition metal complexes. We curate a set of nine representative Ti(III) and V(IV) $d^1$ transition metal complexes and evaluate their flat plane errors along the fractional spin and charge lines. We demonstrate that while jmDFT improves upon both DFT+U and semi-local DFT with the standard atomic orbital projectors (AOPs), it does so inefficiently. We rationalize these inefficiencies by quantifying hybridization in the relevant frontier orbitals for both the case of fractional spins and fractional charges. To overcome these limitations, we introduce a procedure for computing a molecular orbital projector (MOP) basis for use with jmDFT. We demonstrate this single set of $d^1$ MOPs to be suitable for nearly eliminating all energetic delocalization error and static correlation error. In all cases, the MOP jmDFT outperforms AOP jmDFT, and it eliminates most flat plane errors at non-empirical values. Unlike widely employed DFT+U or hybrid functionals, jmDFT nearly eliminates energetic delocalization error and static correlation error within a non-empirical framework. △ Less

Submitted 29 December, 2021; originally announced December 2021.

Tailoring flat bands and topological phases in a multi-strand Creutz network

Authors: Amrita Mukherjee, Atanu Nandy, Shreekantha Sil, Arunava Chakrabarti

Abstract: We prove that, a suitable correlation between the system parameters can trigger topological phase transition and flat bands in a multi strand Creutz ladder network, when a staggered second neighbor interaction is included along the x axis. An appropriate change of basis maps such a finite N strand mesh into N or N 1 decoupled Su Schrieffer Heeger chains, depending onNeven or odd. A simple intuitiv… ▽ More We prove that, a suitable correlation between the system parameters can trigger topological phase transition and flat bands in a multi strand Creutz ladder network, when a staggered second neighbor interaction is included along the x axis. An appropriate change of basis maps such a finite N strand mesh into N or N 1 decoupled Su Schrieffer Heeger chains, depending onNeven or odd. A simple intuitive method, using a real space decimation scheme turns out to be very powerful in analytically extracting the flat bands, explaining their degeneracy or a lifting of the same. Our results are analytically exact, and may inspire experiments in photonics and ultracold atomic systems. △ Less

Submitted 11 November, 2021; originally announced November 2021.

Comments: 9 pages, 8 figures

Audacity of huge: overcoming challenges of data scarcity and data quality for machine learning in computational materials discovery

Authors: Aditya Nandy, Chenru Duan, Heather J. Kulik

Abstract: Machine learning (ML)-accelerated discovery requires large amounts of high-fidelity data to reveal predictive structure-property relationships. For many properties of interest in materials discovery, the challenging nature and high cost of data generation has resulted in a data landscape that is both scarcely populated and of dubious quality. Data-driven techniques starting to overcome these limit… ▽ More Machine learning (ML)-accelerated discovery requires large amounts of high-fidelity data to reveal predictive structure-property relationships. For many properties of interest in materials discovery, the challenging nature and high cost of data generation has resulted in a data landscape that is both scarcely populated and of dubious quality. Data-driven techniques starting to overcome these limitations include the use of consensus across functionals in density functional theory, the development of new functionals or accelerated electronic structure theories, and the detection of where computationally demanding methods are most necessary. When properties cannot be reliably simulated, large experimental data sets can be used to train ML models. In the absence of manual curation, increasingly sophisticated natural language processing and automated image analysis are making it possible to learn structure-property relationships from the literature. Models trained on these data sets will improve as they incorporate community feedback. △ Less

Submitted 2 November, 2021; originally announced November 2021.

MOFSimplify: Machine Learning Models with Extracted Stability Data of Three Thousand Metal-Organic Frameworks

Authors: A. Nandy, G. Terrones, N. Arunachalam, C. Duan, D. W. Kastner, H. J. Kulik

Abstract: We report a workflow and the output of a natural language processing (NLP)-based procedure to mine the extant metal-organic framework (MOF) literature describing structurally characterized MOFs and their solvent removal and thermal stabilities. We obtain over 2,000 solvent removal stability measures from text mining and 3,000 thermal decomposition temperatures from thermogravimetric analysis data.… ▽ More We report a workflow and the output of a natural language processing (NLP)-based procedure to mine the extant metal-organic framework (MOF) literature describing structurally characterized MOFs and their solvent removal and thermal stabilities. We obtain over 2,000 solvent removal stability measures from text mining and 3,000 thermal decomposition temperatures from thermogravimetric analysis data. We assess the validity of our NLP methods and the accuracy of our extracted data by comparing to a hand-labeled subset. Machine learning (ML, i.e. artificial neural network) models trained on this data using graph- and pore-geometry-based representations enable prediction of stability on new MOFs with quantified uncertainty. Our web interface, MOFSimplify, provides users access to our curated data and enables them to harness that data for predictions on new MOFs. MOFSimplify also encourages community feedback on existing data and on ML model predictions for community-based active learning for improved MOF stability models. △ Less

Submitted 16 September, 2021; originally announced September 2021.

Deciphering Cryptic Behavior in Bimetallic Transition Metal Complexes with Machine Learning

Authors: Michael G. Taylor, Aditya Nandy, Connie C. Lu, Heather J. Kulik

Abstract: The rational tailoring of transition metal complexes is necessary to address outstanding challenges in energy utilization and storage. Heterobimetallic transition metal complexes that exhibit metal-metal bonding in stacked "double decker" ligand structures are an emerging, attractive platform for catalysis, but their properties are challenging to predict prior to laborious synthetic efforts. We de… ▽ More The rational tailoring of transition metal complexes is necessary to address outstanding challenges in energy utilization and storage. Heterobimetallic transition metal complexes that exhibit metal-metal bonding in stacked "double decker" ligand structures are an emerging, attractive platform for catalysis, but their properties are challenging to predict prior to laborious synthetic efforts. We demonstrate an alternative, data-driven approach to uncovering structure-property relationships for rational bimetallic complex design. We tailor graph-based representations of the metal-local environment for these heterobimetallic complexes for use in training of multiple linear regression and kernel ridge regression (KRR) models. Focusing on oxidation potentials, we obtain a set of 28 experimentally characterized complexes to develop a multiple linear regression model. On this training set, we achieve good accuracy (mean absolute error, MAE, of 0.25 V) and preserve transferability to unseen experimental data with a new ligand structure. We trained a KRR model on a subset of 330 structurally characterized heterobimetallics to predict the degree of metal-metal bonding. This KRR model predicts relative metal-metal bond lengths in the test set to within 5%, and analysis of key features reveals the fundamental atomic contributions (e.g., the valence electron configuration) that most strongly influence the behavior of complexes. Our work provides guidance for rational bimetallic design, suggesting that properties including the formal shortness ratio should be transferable from one period to another. △ Less

Submitted 29 July, 2021; originally announced July 2021.

Using Machine Learning and Data Mining to Leverage Community Knowledge for the Engineering of Stable Metal-Organic Frameworks

Authors: Aditya Nandy, Chenru Duan, Heather J. Kulik

Abstract: Although the tailored metal active sites and porous architectures of MOFs hold great promise for engineering challenges ranging from gas separations to catalysis, a lack of understanding of how to improve their stability limits their use in practice. To overcome this limitation, we extract thousands of published reports of the key aspects of MOF stability necessary for their practical application:… ▽ More Although the tailored metal active sites and porous architectures of MOFs hold great promise for engineering challenges ranging from gas separations to catalysis, a lack of understanding of how to improve their stability limits their use in practice. To overcome this limitation, we extract thousands of published reports of the key aspects of MOF stability necessary for their practical application: the ability to withstand high temperatures without degrading and the capacity to be activated by removal of solvent molecules. From nearly 4,000 manuscripts, we use natural language processing and automated image analysis to obtain over 2,000 solvent-removal stability measures and 3,000 thermal degradation temperatures. We analyze the relationships between stability properties and the chemical and geometric structures in this set to identify limits of prior heuristics derived from smaller sets of MOFs. By training predictive machine learning (ML, i.e., Gaussian process and artificial neural network) models to encode the structure-property relationships with graph- and pore-structure-based representations, we are able to make predictions of stability orders of magnitude faster than conventional physics-based modeling or experiment. Interpretation of important features in ML models provides insights that we use to identify strategies to engineer increased stability into typically unstable 3d-containing MOFs that are frequently targeted for catalytic applications. We expect our approach to accelerate the time to discovery of stable, practical MOF materials for a wide range of applications. △ Less

Submitted 24 June, 2021; originally announced June 2021.

Representations and Strategies for Transferable Machine Learning Models in Chemical Discovery

Authors: Daniel R. Harper, Aditya Nandy, Naveen Arunachalam, Chenru Duan, Jon Paul Janet, Heather J. Kulik

Abstract: Strategies for machine-learning(ML)-accelerated discovery that are general across materials composition spaces are essential, but demonstrations of ML have been primarily limited to narrow composition variations. By addressing the scarcity of data in promising regions of chemical space for challenging targets like open-shell transition-metal complexes, general representations and transferable ML m… ▽ More Strategies for machine-learning(ML)-accelerated discovery that are general across materials composition spaces are essential, but demonstrations of ML have been primarily limited to narrow composition variations. By addressing the scarcity of data in promising regions of chemical space for challenging targets like open-shell transition-metal complexes, general representations and transferable ML models that leverage known relationships in existing data will accelerate discovery. Over a large set (ca. 1000) of isovalent transition-metal complexes, we quantify evident relationships for different properties (i.e., spin-splitting and ligand dissociation) between rows of the periodic table (i.e., 3d/4d metals and 2p/3p ligands). We demonstrate an extension to graph-based revised autocorrelation (RAC) representation (i.e., eRAC) that incorporates the effective nuclear charge alongside the nuclear charge heuristic that otherwise overestimates dissimilarity of isovalent complexes. To address the common challenge of discovery in a new space where data is limited, we introduce a transfer learning approach in which we seed models trained on a large amount of data from one row of the periodic table with a small number of data points from the additional row. We demonstrate the synergistic value of the eRACs alongside this transfer learning strategy to consistently improve model performance. Analysis of these models highlights how the approach succeeds by reordering the distances between complexes to be more consistent with the periodic table, a property we expect to be broadly useful for other materials domains. △ Less

Submitted 20 June, 2021; originally announced June 2021.

Ring-localized states, radial aperiodicity and quantum butterflies on a Cayley tree

Authors: Amrita Mukherjee, Atanu Nandy, Arunava Chakrabarti

Abstract: We present an analytical method, based on a real space decimation scheme, to extract the exact eigenvalues of a macroscopically large set of pinned localized excitations in a Cayley tree fractal network. Within a tight binding scheme we exploit the above method to scrutinize the effect of a deterministic deformation of the network, first through a hierarchical distribution in the values of the nea… ▽ More We present an analytical method, based on a real space decimation scheme, to extract the exact eigenvalues of a macroscopically large set of pinned localized excitations in a Cayley tree fractal network. Within a tight binding scheme we exploit the above method to scrutinize the effect of a deterministic deformation of the network, first through a hierarchical distribution in the values of the nearest neighbor hopping integrals, and then through a radial Aubry Andre Harper quasiperiodic modulation. With increasing generation index, the inflating loop less tree structure hosts pinned eigenstates on the peripheral sites that spread from the outermost rings into the bulk of the sample, resembling the spread of a forest fire, lighting up a predictable set of sites and leaving the rest unignited. The penetration depth of the envelope of amplitudes can be precisely engineered. The quasiperiodic modulation yields hitherto unreported quantum butterflies, which have further been investigated by calculating the inverse participation ratio for the eigenstates, and a multifractal analysis. The applicability of the scheme to photonic fractal waveguide networks is discussed at the end. △ Less

Submitted 22 November, 2020; originally announced November 2020.

Comments: 7 pages, 7 figures

Journal ref: Physica E 134, 114911 (2021)

Pressure controlled trimerization for switching of anomalous Hall effect in triangular antiferromagnet Mn$_3$Sn

Authors: Charanpreet Singh, Vikram Singh, Gyandeep Pradhan, Velaga Srihari, Himanshu Kumar Poswal, Ramesh Nath, Ashis K. Nandy, Ajaya K. Nayak

Abstract: Here, we present a detailed theoretical and experimental study on the pressure induced switching of anomalous Hall effect (AHE) in the triangular antiferromagnetic (AFM) compound Mn$_3$Sn. Our theoretical model suggests pressure driven significant splitting of the in-plane Mn bond lengths $i.e.$ an effective trimerization, which in turn stabilizes a helical AFM ground state by modifying the inter-… ▽ More Here, we present a detailed theoretical and experimental study on the pressure induced switching of anomalous Hall effect (AHE) in the triangular antiferromagnetic (AFM) compound Mn$_3$Sn. Our theoretical model suggests pressure driven significant splitting of the in-plane Mn bond lengths $i.e.$ an effective trimerization, which in turn stabilizes a helical AFM ground state by modifying the inter-plane exchange parameters in the system. We experimentally demonstrate that the AHE in Mn$_3$Sn reduces from 5$μΩ$ cm at ambient pressure to zero at an applied pressure of about 1.5 GPa. Furthermore, our pressure dependent magnetization study reveals that the conventional triangular AFM ground state of Mn$_3$Sn systematically transforms into the helical AFM phase where the symmetry does not support a non-vanishing Berry curvature required for the realization of a finite AHE. The pressure dependent x-ray diffraction (XRD) study rules out any role of structural phase transition in the observed phenomenon. In addition, the temperature dependent in-plane lattice parameter at ambient pressure is found to deviate from the monotonic behavior when the system enters into the helical AFM phase, thereby, supporting the proposed impact of trimerization in controlling the AHE. We believe that the present study makes an important contribution towards understanding the stabilization mechanism of different magnetic ground states in Mn$_3$Sn and related materials for their potential applications pertaining to AHE switching. △ Less

Submitted 20 November, 2020; originally announced November 2020.

Journal ref: Phys. Rev. Research 2, 043366 (2020)