arXiv subjects

Pulickel M. Ajayan

Publications and source records attributed to Pulickel M. Ajayan.

At least 19 recordsLinked to original sources

arXiv2026

Diamond-to-graphite transformation under hypersonic impact

Diamond to graphite transformation is a complex kinetically driven process which has been studied under various conditions for its fundamental importance. We report the transformation of diamond embedded ceramic matrix composites during hypersonic impact. Diamond particles embedded in cubic boron nitride matrix provide a superhard composite that was subjected to high impact collisions of metal projectiles travelling at speeds reaching Mach 8.45. Our observations suggest that the energy absorption and fracture of the composite is primarily enabled via the phase change of diamond into graphite. Characterization of the impact-fractured composite shows transformed diamond particles and provides details of the shock-induced phase transformation and the nature of diamond-graphite interfaces formed during rapid phase change. The study provides new understanding of phase transformation of diamond under extreme conditions.

cond-mat.mtrl-sci↗

arXiv2026

Quantum Dot Moiré from Crossed MoS2 Nanoribbons

Twisted atomically thin layers have attracted much attention for Moiré potential and correlated quantum phenomena. However, existing Moiré superlattices have largely been limited to extensive wavefunction without lateral confinement. Here we introduce a new platform where 1D nanoribbons of 2D MoS2 grown by vapor deposition can be easily superposed at various angles from stacking and transferring, to form Moiré quantum dots at their intersections with unique exciton physics. Angle-dependent Moiré intersections show enhanced exciton emission at commensurate angle 22 deg, which demonstrates faster relaxation at the cryogenic temperature. A size-dependent study further exhibits a reduced exciton energy and soften out-of-plane interlayer coupling for smaller Moiré areas. Our results reveal exciton physics turnability via precise overlapping of 1D nanoribbons.

cond-mat.mtrl-sci↗

arXiv2026

Atomically-Thin Tsumoite (BiTe) based All-Photonic-Isolator, Information Converter, and Logic-Gate

Two-dimensional tsumoite (BiTe), a polymorph of Bi2Te3, has emerged as a promising candidate for nonlinear photonic devices owing to its strong spin-orbit coupling, tunable bandgap, and high carrier mobility characteristics. This work presents a thorough examination of the third-order nonlinear optical response of BiTe dispersions using spatial self-phase modulation (SSPM) spectroscopy. The nonlinear refractive index (n2) and third-order nonlinear susceptibility are quantitatively derived from the diffraction ring patterns, demonstrating third-order nonlinear susceptibility values, similar to or surpassing those of advanced 2D materials. The temporal development and distortion of the SSPM rings are examined using the wind-chime model, and thermal factors influencing the SSPM pattern are analyzed. First-principles electronic band structure studies reveal that the elevated nonlinear susceptibility arises from band dispersion. Direct correlation between carrier transport and third-order nonlinear susceptibility is established. Utilizing these qualities, all photonic devices, including a photonic isolator based on a 2D BiTe-2D hBN heterostructure, are depicted to show asymmetric propagation. A photonic information converter and a logic gate are designed using the cross-phase modulation technique. These findings establish 2D BiTe nanostructure as a formidable nonlinear optical platform for advanced photonic signal processing and integrated photonic applications.

physics.optics↗

arXiv2026

Optical spin defect pairs in cubic boron nitride

Room-temperature optically active solid-state spin defects are widely known to be useful in quantum sensing applications, however, only a select range of materials have been found to host such systems. Recent measurements in the van der Waals material hexagonal boron nitride (hBN) have shown optically detected magnetic resonance (ODMR) with spin-1/2-like signatures can be explained by a charge transfer mechanism where charges move between adjacent defects forming weakly coupled spin pairs. Interestingly, these ODMR signatures have been reported in a variety of materials aside from hBN, suggesting the spin pair model provides a potentially material agnostic approach for enabling ODMR. Here, we test whether the charge transfer mechanism is supported in a different crystal phase, and report on ODMR signatures in cubic boron nitride (cBN), showing all the characteristic properties identified in hBN are preserved. We consider a selection of different cBN samples of varying size and observe ODMR from a single sub-micron cBN particle, paving the way towards sensing applications. This work further expands understanding of the ubiquity of optical spin defect pairs, and establishes the potential for exploring quantum technologies with a wider range of materials.

cond-mat.mes-hall↗

arXiv2025

From Glaphene to Glaphynes: A Hybridization of 2D Silica Glass and Graphynes

Hybrid two-dimensional (2D) materials have attracted increasing interest as platforms for tailoring electronic properties through interfacial design. Very recently, a novel hybrid 2D material termed glaphene, which combines monolayers of 2D silica glass and graphene, was experimentally realized. Inspired by glaphenes, we proposed a new class of similar structures named glaphynes, which are formed by stacking SiO$_2$ monolayers onto $α$-, $β$-, and $γ$-graphynes. Graphynes are 2D carbon allotropes with the presence of acetylenic groups (triple bonds). The glaphynes' structural and electronic properties were investigated using the density functional tight-binding (DFTB) method, as implemented in the DFTB+ package. Our analysis confirms their energetic and structural stability. We have observed that in the case of glaphynes, the electronic proximity effect can indeed open the electronic band gap, but not for all cases, even with the formation of Si-O-C bonds between silica and graphynes.

cond-mat.mtrl-sci↗

arXiv2025

Controlled Growth of Bronze Telluride for Scalable Thermoelectric Energy Harvesting

With the growing demand for sustainable and decentralized energy solutions, thermoelectric energy harvesting has emerged as a promising technology for directly converting waste heat into electricity through solid state, environmentally friendly means. Among copper chalcogenides, Cu2Te is a notable p-type material due to its degenerate semiconducting nature and low thermal conductivity. In this study, we present a sustainable synthesis strategy for Sn-doped Cu2Te referred to as bronze telluride (BT) via a chemical vapor deposition (CVD) assisted tellurization process using pre-alloyed Cu Sn (bronze) powder. The resulting BT exhibited an enhanced thermoelectric figure of merit (ZT) of 1 at 500 K. To assess practical applicability, BT was integrated with n type galena (PbS) in a cascaded p n thermoelectric module, which generated 2.8 mV across a temperature gradient of 35 K, demonstrating its potential for medium- to high-temperature waste heat recovery. Furthermore, thermodynamic calculations and density functional theory (DFT) simulations provided insights into the formation mechanism of Cu2Te and the thermoelectric behaviour of BT. This work introduces an efficient, scalable, and environmentally responsible pathway for developing copper-based thermoelectric materials using industrially relevant precursors.

cond-mat.mtrl-sci↗

arXiv2025

Sub-nm Curvature Unlocks Quantum Flexoelectricity in Graphene

Flexoelectricity, polarization induced by strain gradients, is especially pronounced in two-dimensional (2D) materials due to their mechanical flexibility and sensitivity to mechanical deformation. In nanostructures with sub-nm curvature, this effect is governed by quantum-mechanical polarization and electrostatic modulation, not merely classical lattice distortion. Here, we present the first direct experimental and theoretical demonstration of large intrinsic quantum flexoelectricity in graphene nanowrinkles, exhibiting polarization densities (P_{th} ~ 4 C/m^{2}, P_{exp} ~ 1 C/m^{2}) that exceed those of mesoscale systems by 5 to 7 orders of magnitude. These nanowrinkles, with sub-nm radii of curvature at their apex, undergo atomic-level buckling and result in localized strain fields, as confirmed by sub-micron Raman spectroscopy. These curvatures create an asymmetry to π-orbital interactions across the atomic layer, which, in turn, leads to localized polarization densities. Kelvin probe force microscopy reveals curvature-dependent work function shifts consistent with flexoelectric polarization, while conductive atomic force microscopy detects reproducible flexoelectric currents exhibiting a threshold voltage (Φth ~1 V) that matches the band offset predicted by ab initio calculations (~1.2 V). Together, these results confirm how flexoelectric dipoles reshape the local electronic potential. Graphene nanowrinkles thus provide a pristine platform for uncovering quantum-mechanical flexoelectricity: a fundamentally ubiquitous effect, whose study in the simplest crystalline material can illuminate electromechanical behavior across condensed matter, soft matter, and biological systems.

cond-mat.mes-hall↗

arXiv2025

Structural Stability of Sulfur Depleted MoS2

Transition metal dichalcogenides (TMDs), particularly monolayer MoS2, have received increased attention in materials science and have been exploited in diverse applications from photonics to catalysis. Defects in TMDs play a crucial role in modulating their properties, and understanding defect-induced dynamics is of great importance. This study investigates the dynamics of sulfur depletion in defective monolayer MoS2, which yields stable MoS monolayers. Various defect sizes, temperature regimes, and substrate effects were investigated. Through comprehensive classical molecular (ReaxFF) molecular dynamics (MD) and ab initio MD (AIMD) simulations, we elucidate the dynamics of sulfur vacancy formation in MoS2 lattices. After removing all sulfur atoms from the top layer, several sulfur atoms from the bottom layer spontaneously migrate to the top layer as a response to increase structural stability, thus creating a MoSx alloy. These findings deepen our understanding of defect dynamics in TMDs, offering valuable insights into the controlled engineering of their properties for nanotechnology applications.

cond-mat.mtrl-sci↗

arXiv2025

Anomalous properties of spark plasma sintered boron nitride solids

Hexagonal boron nitride (h-BN) is a brittle ceramic with a layered structure, however, recent experiments have suggested that inter-layer structural engineering could be key to new structural and functional properties. Here we report the scalable bulk synthesis of high-density crystalline h-BN solids, by using high-temperature spark plasma sintering (SPS) of h-BN powders, which show high values of mechanical strength, ductility, dielectric constant, thermal conductivity, and exceptional neutron radiation shielding capability. Through exhaustive characterizations we reveal that SPS induces non-basal plane crystallinity, twisting of layers, and facilitates inter-grain fusion with a high degree of in-plane alignment across macroscale dimensions, resulting in near-theoretical density and improved properties. Our findings highlight the importance of material design, via new approaches such as layer twisting and interlayer interconnections, to create novel ceramics with properties that could go beyond their intrinsic limits.

cond-mat.mtrl-sci↗

arXiv2025

Room-Temperature High-Purity Single Photon Emission from Carbon-Doped Boron Nitride Thin Films

Hexagonal boron nitride (hBN) has emerged as an excellent host material for generating room temperature single photons exhibiting high brightness and spin-photon entanglement. However, challenges in improving purity, stability, and scalability limit its use in quantum technologies. Here, we demonstrate highly pure and stable single photon emitters (SPEs) in hBN by directly growing carbon-doped, centimeter-scale hBN thin films using the pulsed laser deposition (PLD) method. These SPEs exhibit room temperature operation with polarized emission, achieving a g(2)(0) value of 0.015, which is among the lowest reported for room temperature SPEs and the lowest achieved for hBN SPEs. It also exhibits high brightness ( around 0.5 million counts per second), remarkable stability during continuous operation (> 15 minutes), and a Debye-Waller factor of 45%. First-principles calculations reveal unique carbon defects responsible for these properties, enabled by PLD's low-temperature synthesis and in-situ doping. Our results demonstrate an effective method for large-scale production of high-purity, stable SPEs in hBN, enabling robust quantum optical sources for various applications.

physics.app-ph↗

arXiv2025

Attosecond Inner-Shell Lasing at Angstrom Wavelengths

Since the invention of the laser nonlinear effects such as filamentation, Rabi-cycling and collective emission have been explored in the optical regime leading to a wide range of scientific and industrial applications. X-ray free electron lasers (XFELs) have led to the extension of many optical techniques to X-rays for their advantages of angstrom scale spatial resolution and elemental specificity. One such example is XFEL driven population inversion of 1s core hole states resulting in inner-shell K$α$ (2p to 1s) X-ray lasing in elements ranging from neon to copper, which has been utilized for nonlinear spectroscopy and development of next generation X-ray laser sources. Here we show that strong lasing effects, similar to those observed in the optical regime, can occur at 1.5 to 2.1 angstrom wavelengths during high intensity (> ${10^{19}}$ W/cm${^{2}}$) XFEL driven inner-shell lasing and superfluorescence of copper and manganese. Depending on the temporal substructure of the XFEL pump pulses(containing ${~10^{6}}$ - ${10^{8}}$ photons) i, the resulting inner-shell X-ray laser pulses can exhibit strong spatial inhomogeneities as well as spectral splitting, inhomogeneities and broadening. Through 3D Maxwell Bloch theory we show that the observed spatial inhomogeneities result from X-ray filamentation, and that the spectral splitting and broadening is driven by Rabi cycling with sub-femtosecond periods. Our simulations indicate that these X-ray pulses can have pulse lengths of less than 100 attoseconds and coherence properties that open the door for quantum X-ray optics applications.

physics.optics↗

arXiv2024

Ion-Assisted Nanoscale Material Engineering in Atomic Layers

Achieving deterministic control over the properties of low-dimensional materials with nanoscale precision is a long-sought goal. Mastering this capability has a transformative impact on the design of multifunctional electrical and optical devices. Here, we present an ion-assisted synthetic technique that enables precise control over the material composition and energy landscape of two-dimensional (2D) atomic crystals. Our method transforms binary transition metal dichalcogenides (TMDs), like MoSe$_2$, into ternary MoS$_{2α}$Se$_{2(1-α})$ alloys with systematically adjustable compositions, $α$. By piecewise assembly of the lateral, compositionally modulated MoS$_{2α}$Se$_{2(1-α)}$ segments within 2D atomic layers, we present a synthetic pathway towards the realization of multi-compositional designer materials. Our technique enables the fabrication of complex structures with arbitrary boundaries, dimensions as small as 30 nm, and fully customizable energy landscapes. Our optical characterizations further showcase the potential for implementing tailored optoelectronics in these engineered 2D crystals.

cond-mat.mtrl-sci↗

arXiv2024

Non-thermal Magnetic Deicing Using Two-Dimensional Chromium Telluride

Two-dimensional (2D) chromium telluride Cr2Te3 exhibits strong ferromagnetic ordering with high coercivity at low temperatures and paramagnetic behaviour when approaching room temperature. The spin states of monolayer Cr2Te3 show ferromagnetic ordering in the ground state, and in-situ Raman analysis shows reversible structure transformation and hence a ferromagnetic to paramagnetic transition during low-temperature heating cycles (0 - 25 °C). The magnetic phase transition near room temperature in the 2D Cr2Te3 prompted the exploration of these layered materials for energy application. We demonstrate that the low-temperature ferromagnetic behavior can be used to magnetically deice material surfaces using an external magnetic source, avoiding the use of harsh chemicals and high temperatures. The hydrophobic nature and dipole interactions of H2O molecules with the surface of the 2D Cr2Te3 coating aid in the condensation of ice droplets formed on the surface. First-principles calculations also confirm the observed crystal structure, surface interaction, and magnetic properties of 2D Cr2Te3.

cond-mat.mtrl-sci↗

arXiv2024

Graphene Terahertz Devices for Sensing and Communication

Graphene-based terahertz (THz) devices have emerged as promising platforms for a variety of applications, leveraging graphene's unique optoelectronic properties. This review explores recent advancements in utilizing graphene in THz technology, focusing on two main aspects: THz molecular sensing and THz wave modulation. In molecular sensing, the environment-sensitive THz transmission and emission properties of graphene are utilized for enabling molecular adsorption detection and biomolecular sensing. This capability holds significant potential, from the detection of pesticides to DNA at high sensitivity and selectivity. In THz wave modulation, crucial for next-generation wireless communication systems, graphene demonstrates remarkable potential in absorption modulation when gated. Novel device structures, spectroscopic systems, and metasurface architectures have enabled enhanced absorption and wave modulation. Furthermore, techniques such as spatial phase modulation and polarization manipulation have been explored. From sensing to communication, graphene-based THz devices present a wide array of opportunities for future research and development. Finally, advancements in sensing techniques not only enhance biomolecular analysis but also contribute to optimizing graphene's properties for communication by enabling efficient modulation of electromagnetic waves. Conversely, developments in communication strategies inform and enhance sensing capabilities, establishing a mutually beneficial relationship.

physics.optics↗

arXiv2024

From Pure Mathematics to Macroscale Applications: The Genesis of Schwarzites

Schwarzites are porous (spongy-like) carbon allotropes with negative Gaussian curvatures. They were proposed by Mackay and Terrones inspired by the works of the German mathematician Hermann Schwarz on Triply-Periodic Minimal Surfaces (TPMS). This review presents and discusses the history of schwarzites and their place among curved carbon nanomaterials. We summarized the main works on schwarzites available in the literature. We discuss their unique structural, electronic, thermal, and mechanical properties. Although the synthesis of carbon-based schwarzites remains elusive, the recent advances in the synthesis of zeolite-templates nanomaterials bring them closer to reality. Atomic-based models of schwarzites have been translated into macroscale ones that have been 3D printed. These 3D printed models have been exploited in many real-world applications, including water remediation and biomedical ones.

cond-mat.mtrl-sci↗

arXiv2023

Non-linear optics at twist interfaces in h-BN/SiC heterostructures

Understanding the emergent electronic structure in twisted atomically thin layers has led to the exciting field of twistronics. However, practical applications of such systems are challenging since the specific angular correlations between the layers must be precisely controlled and the layers have to be single crystalline with uniform atomic ordering. Here, we suggest an alternative, simple and scalable approach where nanocrystalline two-dimensional (2D) film on three-dimensional (3D) substrates yield twisted-interface-dependent properties. Ultrawide-bandgap hexagonal boron nitride (h-BN) thin films are directly grown on high in-plane lattice mismatched wide-bandgap silicon carbide (4H-SiC) substrates to explore the twist-dependent structure-property correlations. Concurrently, nanocrystalline h-BN thin film shows strong non-linear second-harmonic generation and ultra-low cross-plane thermal conductivity at room temperature, which are attributed to the twisted domain edges between van der Waals stacked nanocrystals with random in-plane orientations. First-principles calculations based on time-dependent density functional theory manifest strong even-order optical nonlinearity in twisted h-BN layers. Our work unveils that directly deposited 2D nanocrystalline thin film on 3D substrates could provide easily accessible twist-interfaces, therefore enabling a simple and scalable approach to utilize the 2D-twistronics integrated in 3D material devices for next-generation nanotechnology.

cond-mat.mtrl-sci↗

arXiv2023

Unravelling the room temperature growth of two-dimensional h-BN nanosheets for multifunctional applications

Room temperature growth of two-dimensional van der Waals (2D-vdW) materials is indispensable for state-of-the-art nanotechnology. The low temperature growth supersedes the requirement of elevated growth temperature accompanied with high thermal budgets. Moreover, for electronic applications, low or room temperature growth reduces the possibility of intrinsic film-substrate interfacial thermal diffusion related deterioration of functional properties and consequent device performance. Here, we demonstrated the growth of ultrawide-bandgap boron nitride (BN) at room temperature by using the pulsed laser deposition (PLD) process and demonstrated various functionalities for potential applications. Comprehensive chemical, spectroscopic and microscopic characterization confirms the growth of ordered nanosheet-like hexagonal BN. Functionally, nanosheets show hydrophobicity, high lubricity (low coefficient of friction), low refractive index within the visible to near-infrared wavelength range, and room temperature single-photon quantum emission. Our work unveils an important step that brings a plethora of applications potential for room temperature grown h-BN nanosheets as it can be feasible on any given substrate, thus creating a scenario for h-BN on demand at frugal thermal budget.

physics.app-ph↗

arXiv2023

Structural, optical, and thermal properties of BN thin films grown on diamond via pulsed laser deposition

Heterostructures based on ultrawide-bandgap (UWBG) semiconductors (bandgap >4.0 eV), boron nitride (BN) and diamond are important for next-generation high-power electronics. However, in-situ hetero-epitaxy of BN/diamond or vice-versa remains extremely challenging, due to their non-trivial growth kinetics. Here, we have grown BN thin film on (100) single crystal diamond by pulsed laser deposition and investigated its structural and magnetic properties, optical refractive index, and thermal conductivity. Structural characterizations confirm the mixed (stable hexagonal and metastable cubic) phase growth. Film shows diamagnetic behavior at room temperature. It displays anisotropic refractive index within the visible-to-near-infrared wavelength range. The room temperature cross-plane thermal conductivity of BN is ~1.53 W/(mK), and the thermal conductance of the BN/diamond interface is ~20 MW/(m2K). Our findings are useful for various device related applications based on UWBG BN/diamond heterostructures.

physics.app-ph↗