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Rohit P. Prasankumar

Publications and source records attributed to Rohit P. Prasankumar.

At least 19 recordsLinked to original sources

Quantized Photocurrents in Gapless Topological Matter

The quantum Hall effect establishes that topology can fix a material response to integer multiples of fundamental constants when an energy gap isolates the relevant symmetry-protected electronic states. Whether such universal quantization can also emerge in gapless matter, where topological bands coexist with a continuum of metallic excitations, has remained a fundamental question in the field of quantum materials. Chiral topological semimetals provide a unique setting in which to explore this principle; when optical transitions are confined to a single chiral node, the resulting circular photogalvanic effect is predicted to be quantized by the topological charge of the node. In real materials, however, this nonlinear optical phenomenon has remained experimentally elusive, obscured by trivial band transitions, insufficient energy separation between node pairs, and their relative positions with respect to the Fermi level. Here we observe a quantized circular photogalvanic effect in the chiral topological semimetal Rh0.95Ni0.05Si. Band engineering via Ni substitution opens a photon-energy window dominated by interband optical transitions at the {\Gamma}-point multifold node. This allows circularly polarized near- to mid-infrared pulses to drive a helicity-odd terahertz response that manifests three hallmarks of quantization: a sharp onset, a photon-energy-independent plateau governed by the magnitude of the monopole charge, and an abrupt long-wavelength cutoff imposed by Pauli blocking. Our work thus establishes an all-optical analogue of the quantum Hall effect and a new paradigm to realize topological quantization in gapless matter.

cond-mat.mtrl-sci

Anharmonic lattice dynamics and superconductivity in strained bulk and surface niobium

Using first-principles calculations, we investigate how homogeneous strain and crystallographic surface orientation modify the vibrational and superconducting properties of niobium. For bulk Nb, tensile strain strongly softens the phonon spectrum and enhances the electron--phonon coupling, increasing the superconducting transition temperature from 9.5 K at equilibrium to 14.5 K at $\sim\!6\%$ lattice expansion. For the low-index Nb(001), Nb(110), and Nb(111) surfaces, harmonic phonon calculations exhibit imaginary modes, showing that anharmonic lattice effects are essential. To treat these effects efficiently, we train Nb-specific machine-learning interatomic potentials on bulk and slab first-principles configurations and use them to accelerate stochastic self-consistent harmonic approximation calculations, thereby obtaining anharmonically renormalized phonon modes that are combined with density-functional perturbation theory electron--phonon matrix elements to construct the Eliashberg spectral function. Among the clean free-standing slabs considered here, Nb(001) exhibits the strongest electron--phonon coupling and the highest calculated transition temperature of 10.0 K, while Nb(110) and Nb(111) show progressively reduced pairing strength. Finally, by analyzing the Eliashberg spectral function and the functional derivative $δT_\text{c}/δα^2F(ω)$, we identify the phonon energy ranges most effective for superconducting pairing. Our results show that strain, surface termination, and anharmonic phonon renormalization provide complementary and interrelated microscopic routes for tuning superconductivity in Nb.

cond-mat.supr-con

Ambient-pressure 151-K superconductivity in HgBa2Ca2Cu3O8+δ via pressure quench

Superconductivity has been a vigorously researched topic since its discovery in 1911. Raising the superconducting transition temperature (Tc) has been the main driving force behind such long-sustained efforts due to its potential for impacting humanity and the fundamental knowledge gained from understanding this macroscopic coherent quantum state at high temperatures. The successful development of high-Tc superconductivity will make possible extraordinarily efficient generation, delivery, and utilization of energy, and could also enable the development of controlled fusion while impacting other burgeoning fields like quantum computation and quantum electronics. However, progress has been hindered by a longstanding plateau in the record ambient-pressure Tc, unchanged since 1993. Subsequent significant advancements in Tc have been achieved only under high pressures, preventing the realization of superconductivity's full potential. To directly address this challenge, we developed a pressure-quench protocol (PQP) to stabilize pressure-induced/-enhanced superconducting states at ambient pressure. Here we achieve a record ambient-pressure Tc of 151 K in the cuprate HgBa2Ca2Cu3O8+δ via PQP. The experimental results are further supported by synchrotron X-ray diffraction measurements and phonon and electronic structure calculations. This breakthrough opens new avenues for stabilizing and exploring ambient-pressure high-Tc superconducting states and other quantum states that have been previously only accessible under pressure, paving the way for deeper understanding and practical applications of high-Tc superconductivity and beyond.

cond-mat.supr-con

High-pressure stabilization of Mg2IrH7: Structural proximity to high-Tc superconductivity

Mg$_2$IrH$_6$ is a metastable complex metal hydride with a predicted superconducting transition temperature as high as 170 K at ambient pressure. Following the synthesis of isomorphic, insulating Mg$_2$IrH$_5$ at low pressure, higher-pressure studies were conducted to investigate the phase behavior and compound formation in this system. X-ray diffraction and Raman spectroscopic measurements indicate that cubic Mg$_2$IrH$_7$ is stabilized above ca. 40 GPa and coexists with a related hexagonal hydride with likely composition near Mg$_2$IrH$_5$. Electrical transport measurements show that the cubic Mg$_2$IrH$_7$ is insulating, in agreement with ab initio predictions, and persists during room-temperature decompression until $\sim$20 GPa before reverting back to the cubic Mg$_2$IrH$_5$. The experimental results confirm ground-state structure predictions in the Mg-Ir-H system, and the formation of two nearly identical phases with surrounding compositions opens new opportunities to access superconducting Mg$_2$IrH$_6$ through non-equilibrium processing pathways.

cond-mat.supr-con

Inverse Isotope Effect in the Ternary Perovskite Hydride SrPdH/D$_{2.9}$: A Signature of Quantum Zero-Point Fluctuations

Guided by first-principles calculations, we demonstrate superconductivity in the ternary perovskite hydride SrPdH$_{3-x}$, synthesized at low pressure. Structural characterization via neutron diffraction reveals the near-stoichiometric composition SrPdD$_{2.9(2)}$ with 96\% deuterium site occupancy. Subsequent transport and magnetic susceptibility measurements establish onset superconducting transitions at $T_\text{c} = \SI{2.1}{K} $ (H) and $T_\text{c} = \SI{2.2}{K} $ (D), exhibiting an inverse isotope effect that our first-principles calculations attribute predominantly to quantum zero-point motion. The excellent agreement between theory and experiment with respect to thermodynamic stability and superconducting properties provides important validation for theory-guided superconductor discovery. This work establishes superconductivity in the perovskite hydride structural prototype -- expanding the limited family of experimentally realized ternary hydride superconductors -- and demonstrates the importance of quantum nuclear motion on the accurate theoretical treatment of low-pressure hydride superconductors.

cond-mat.supr-con

Polar enhancement of optical nonlinearities and domain-driven second harmonic contrast in bismuth telluro-halide van der Waals crystals

The BiTeX family of polar van der Waals (vdW) semiconductors offers a unique platform for exploring the interplay between polar crystalline structure and nonlinear optical phenomena. Here, we utilize second harmonic generation (SHG) polarimetry to demonstrate giant anisotropic optical nonlinearities in BiTeBr and BiTeI driven by contributions to the crystals' nonlinear polarizability originating from their permanent dipole moment. In addition, using SHG microscopy, we show that BiTeI displays a distinctive SHG spatial texture consisting of thread-like regions of reduced harmonic intensity. These features demark the boundaries between phase and anti-phase polar domains, confirmed via piezoresponse force microscopy and are attributable to disorder-driven restoration of inversion symmetry and concomitant optical interference effects. Our results unveil the power of polarization-resolved SHG microscopy in elucidating the intricate relationship between structure, symmetry, and nonlinear optical responses in polar vdW materials and highlight the promise of BiTeX as a material platform for domain-engineered nanoscale nonlinear photonics.

physics.optics

First-principles evidence for conventional superconductivity in a quasicrystal approximant

Quasicrystals (QCs) host long-range order without translational symmetry, a regime in which the very foundations of BCS theory are not straightforwardly applicable, yet experiments on QCs and their approximant crystals (ACs) point to conventional, $s$-wave, electron-phonon coupled superconductivity. Here we test the predictive power of the electron-phonon framework in a representative decagonal AC from first principles. Using state-of-the-art \textit{ab initio} methods, we compute the superconducting properties of the recently discovered AC Al$_{13}$Os$_4$ and quantitatively reproduce its bulk $T_\text{c}$. This constitutes, to our knowledge, the first \textit{ab initio} determination of $T_\text{c}$ for an AC and establishes that the electron-phonon framework is predictive in these systems as well. Using the generalized quasichemical approximation for alloy modeling in the decagonal Al--Os family, we predict tunable superconductivity in Al$_{13}$Os$_{4-x}$Re$_x$ and Al$_{13}$Os$_{4-x}$Ir$_x$; in particular, Al$_{13}$Re$_4$ is dynamically stable and estimated to have a $T_\text{c}$ about 30% above Al$_{13}$Os$_4$. Finally, we discuss the role of ACs as high-fidelity proxies for their parent QCs. Although long-range quasiperiodicity may introduce subtle electronic features, our findings indicate that the key ingredients for superconductivity are already encoded in the local structural motifs preserved by the AC. This places the Al--Os and Al--Re families among the most promising candidates for the highest-$T_\text{c}$ quasicrystalline superconductivity.

cond-mat.supr-con

Cavity-altered superconductivity

Is it feasible to alter the ground state properties of a material by engineering its electromagnetic environment? Inspired by theoretical predictions, experimental realizations of such cavity-controlled properties without optical excitation are beginning to emerge. Here, we devised and implemented a novel platform to realize cavity-altered materials. Single crystals of hyperbolic van der Waals (vdW) compounds provide a resonant electromagnetic environment with enhanced density of photonic states and prominent mode confinement. We interfaced hexagonal boron nitride (hBN) with the molecular superconductor $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br ($κ$-ET). The frequencies of infrared (IR) hyperbolic modes of hBN match the IR-active carbon-carbon stretching molecular resonance of ($κ$-ET) implicated in superconductivity. Nano-optical data supported by first-principles molecular Langevin dynamics simulations confirm the presence of resonant coupling between the hBN hyperbolic cavity modes and the carbon-carbon stretching mode in ($κ$-ET). Meissner effect measurements via magnetic force microscopy demonstrate a strong suppression of superfluid density near the hBN/($κ$-ET) interface. Non-resonant control heterostructures, including RuCl$_3$/($κ$-ET) and hBN/$\text{Bi}_2\text{Sr}_2\text{CaCu}_2\text{O}_{8+x}$, do not display the superfluid suppression. These observations suggest that hBN/($κ$-ET) realizes a cavity-altered superconducting ground state. Our work highlights the potential of dark cavities devoid of external photons for engineering electronic ground state properties of complex quantum materials.

cond-mat.supr-con

Single layer clathrane: A potential superconducting two-dimensional (2D) hydrogenated metal borocarbide

We propose a new family of two-dimensional (2D) metal-borocarbide clathrane superconductors, derived from three-dimensional (3D) MM$^\prime$B$_6$C$_6$ clathrates. First-principles calculations reveal that hydrogen passivation and surface metal decoration stabilize the M$_2$M$^\prime$B$_8$C$_8$H$_8$ monolayers. These 2D systems exhibit tunable superconductivity governed by hole concentration, structural anisotropy, and electron-phonon coupling. We find that in-plane anisotropy competes with superconductivity, reducing \tc\ despite favorable doping. Biaxial strain mitigates this anisotropy, enhances Fermi surface nesting, and increases \tc\ by an average of 15.5~K. For example, the \tc\ of Sr$_3$B$_8$C$_8$H$_8$ is predicted to increase from 11.3~K to 22.2~K with strain engineering. These findings identify 2D clathranes as promising, strain-tunable superconductors and highlight design principles for optimizing low-dimensional superconducting materials.

cond-mat.supr-con

Vacancy-free cubic superconducting NbN enabled by quantum anharmonicity

Niobium nitride (NbN) is renowned for its exceptional mechanical, electronic, magnetic, and superconducting properties. The ideal 1:1 stoichiometric $δ$-NbN cubic phase, however, is known to be dynamically unstable, and repeated experimental observations have indicated that vacancies are necessary for its stabilization. In this work, we demonstrate that when the structure is fully relaxed and allowed to distort under quantum anharmonic effects, a previously unreported stable cubic phase with space group $P\bar{4}3m$ emerges - 65 meV/atom lower in free energy than the ideal $δ$ phase. This discovery is enabled by state-of-the-art first-principles calculations accelerated by machine-learned interatomic potentials. To evaluate the vibrational and superconducting properties with quantum anharmonic effects accounted for, we use the stochastic self-consistent harmonic approximation (SSCHA) and molecular dynamics spectral energy density (SED) methods. Electron-phonon coupling calculations based on the SSCHA phonon dispersion yield a superconducting transition temperature of $T_\text{c}$ = 20 K, which aligns closely with experimentally reported values for near-stoichiometric NbN. These findings challenge the long-held assumption that vacancies are essential for stabilizing cubic NbN and point to the potential of synthesizing the ideal 1:1 stoichiometric phase as a route to achieving enhanced superconducting performance in this technologically significant material.

cond-mat.supr-con

Prediction and Synthesis of Mg$_4$Pt$_3$H$_6$: A Metallic Complex Transition Metal Hydride Stabilized at Ambient Pressure

The low-pressure stabilization of superconducting hydrides with high critical temperatures ($T_c$s) remains a significant challenge, and experimentally verified superconducting hydrides are generally constrained to a limited number of structural prototypes. Ternary transition-metal complex hydrides (hydrido complexes)-typically regarded as hydrogen storage materials-exhibit a large range of compounds stabilized at low pressure with recent predictions for high-$T_c$ superconductivity. Motivated by this class of materials, we investigated complex hydride formation in the Mg-Pt-H system, which has no known ternary hydride compounds. Guided by ab initio structural predictions, we successfully synthesized a novel complex transition-metal hydride, Mg$_4$Pt$_3$H$_6$, using laser-heated diamond anvil cells. The compound forms in a body-centered cubic structural prototype at moderate pressures between 8-25 GPa. Unlike the majority of known hydrido complexes, Mg$_4$Pt$_3$H$_6$ is metallic, with formal charge described as 4[Mg]$^{2+}$.3[PtH$_2$]$^{2-}$. X-ray diffraction (XRD) measurements obtained during decompression reveal that Mg$_4$Pt$_3$H$_6$ remains stable upon quenching to ambient conditions. Magnetic-field and temperature-dependent electrical transport measurements indicate ambient-pressure superconductivity with $T_c$ (50%) = 2.9 K, in reasonable agreement with theoretical calculations. These findings clarify the phase behavior in the Mg-Pt-H system and provide valuable insights for transition-metal complex hydrides as a new class of hydrogen-rich superconductors.

cond-mat.supr-con

Creation, stabilization, and study at ambient pressure of pressure-induced superconductivity in Bi$_{0.5}$Sb$_{1.5}$Te$_3$

In light of breakthroughs in superconductivity under high pressure, and considering that record critical temperatures (T$_c$s) across various systems have been achieved under high pressure, the primary challenge for higher Tc should no longer solely be to increase T$_c$ under extreme conditions but also to reduce, or ideally eliminate, the need for applied pressure in retaining pressure-induced or -enhanced superconductivity. The topological semiconductor Bi$_{0.5}$Sb$_{1.5}$Te$_3$ (BST) was chosen to demonstrate our approach to addressing this challenge and exploring its intriguing physics. Under pressures up to ~ 50 GPa, three superconducting phases (BST-I, -II, and -III) were observed. A superconducting phase in BST-I appears at ~ 4 GPa, without a structural transition, suggesting the possible topological nature of this phase. Using the pressure-quench protocol (PQP) recently developed by us, we successfully retained this pressure-induced phase at ambient pressure and revealed the bulk nature of the state. Significantly, this demonstrates recovery of a pressure-quenched sample from a diamond anvil cell at room temperature with the pressure-induced phase retained at ambient pressure. Other superconducting phases were retained in BST-II and -III at ambient pressure and subjected to thermal and temporal stability testing. Superconductivity was also found in BST with T$_c$ up to 10.2 K, the record for this compound series. While PQP maintains superconducting phases in BST at ambient pressure, both depressurization and PQP enhance its T$_c$, possibly due to microstructures formed during these processes, offering an added avenue to raise T$_c$. These findings are supported by our density-functional theory calculations.

cond-mat.supr-con

Synthesis of Mg$_2$IrH$_5$: A potential pathway to high-$T_c$ hydride superconductivity at ambient pressure

Following long-standing predictions associated with hydrogen, high-temperature superconductivity has recently been observed in several hydride-based materials. Nevertheless, these high-$T_c$ phases only exist at extremely high pressures, and achieving high transition temperatures at ambient pressure remains a major challenge. Recent predictions of the complex hydride Mg$_{2}$IrH$_{6}$ may help overcome this challenge with calculations of high-$T_c$ superconductivity (65 K$~<~T_c~<~$ 170 K) in a material that is stable at atmospheric pressure. In this work, the synthesis of Mg$_{2}$IrH$_{6}$ was targeted over a broad range of $P$-$T$ conditions, and the resulting products were characterized using X-ray diffraction (XRD) and vibrational spectroscopy, in concert with first-principles calculations. The results indicate that the charge-balanced complex hydride Mg$_{2}$IrH$_{5}$ is more stable over all conditions tested up to ca 28 GPa. The resulting hydride is isostructural with the predicted superconducting Mg$_{2}$IrH$_{6}$ phase except for a single hydrogen vacancy, which shows a favorable replacement barrier upon insertion of hydrogen into the lattice. Bulk Mg$_{2}$IrH$_{5}$ is readily accessible at mild $P$-$T$ conditions and may thus represent a convenient platform to access superconducting Mg$_{2}$IrH$_{6}$ via non-equilibrium processing methods.

cond-mat.supr-con

Twisted nonlinear optics in monolayer van der Waals crystals

In addition to a plethora of emergent phenomena, the spatial topology of optical vortices enables an array of applications spanning communications to quantum photonics. Nonlinear optics is essential in this context, providing access to an infinitely large set of quantum states associated with the orbital angular momentum of light. Nevertheless, the realization of such processes have failed to keep pace with the ever-growing need to shrink the fundamental length-scale of photonic technologies to the nanometer regime6. Here, we push the boundaries of vortex nonlinear optics to the ultimate limits of material dimensionality. By exploiting second and third-order frequency-mixing processes in semiconducting monolayers, we demonstrate the independent manipulation of the wavelength, orbital angular momentum, and spatial distribution of vortex light-fields. Due to the atomically-thin nature of the host quantum material, this control spans a broad spectral bandwidth in a highly-integrable platform, unconstrained by the traditional limits of bulk nonlinear optical materials. Our work heralds a new avenue for ultra-compact and scalable hybrid nanotechnologies empowered by twisted nonlinear light-matter interactions in van der Waals quantum nanomaterials.

physics.optics

Machine learning assisted prediction of organic salt structure properties

We demonstrate a machine learning-based approach which predicts the properties of crystal structures following relaxation based on the unrelaxed structure. Use of crystal graph singular values reduces the number of features required to describe a crystal by more than an order of magnitude compared to the full crystal graph representation. We construct machine learning models using the crystal graph singular value representations in order to predict the volume, enthalpy per atom, and metal versus semiconducting phase of DFT-relaxed organic salt crystals based on randomly generated unrelaxed crystal structures. Initial base models are trained to relate 89,949 randomly generated structures of salts formed by varying ratios of 1,3,5-triazine and HCl with the corresponding volumes, enthalpies per atom, and phase of the DFT-relaxed structures. We further demonstrate that the base model is able to extrapolate to new chemical systems with the inclusion of 2,000 to 10,000 crystal structures from the new system. After training a single model with a large number of data points, extension can be done at significantly lower cost. The constructed machine learning models can be used to rapidly screen large sets of randomly generated organic salt crystal structures and efficiently downselect the structures most likely to be experimentally realizable. The models can be used either as a stand-alone crystal structure predictor or incorporated into more sophisticated workflows as a filtering step.

cond-mat.mtrl-sci

Light-Driven Nanoscale Vectorial Currents

Controlled charge flows are fundamental to many areas of science and technology, serving as carriers of energy and information, as probes of material properties and dynamics, and as a means of revealing or even inducing broken symmetries. Emerging methods for light-based current control offer promising routes beyond the speed and adaptability limitations of conventional voltage-driven systems. However, optical generation and manipulation of currents at nanometer spatial scales remains a basic challenge and a crucial step towards scalable optoelectronic systems for microelectronics and information science. Here, we introduce vectorial optoelectronic metasurfaces in which ultrafast light pulses induce local directional charge flows around symmetry-broken plasmonic nanostructures, with tunable responses and arbitrary patterning down to sub-diffractive nanometer scales. Local symmetries and vectorial current distributions are revealed by polarization- and wavelength-sensitive electrical readout and terahertz (THz) emission, while spatially-tailored global currents are demonstrated in the direct generation of elusive broadband THz vector beams. We show that in graphene, a detailed interplay between electrodynamic, thermodynamic, and hydrodynamic degrees of freedom gives rise to rapidly-evolving nanoscale driving forces and charge flows under extreme temporal and spatial confinement. These results set the stage for versatile patterning and optical control over nanoscale currents in materials diagnostics, THz spectroscopies, nano-magnetism, and ultrafast information processing.

cond-mat.mes-hall

Revealing Charge Carrier Dynamics and Transport in Te-Doped GaAsSb and GaAsSbN Nanowires by Correlating Ultrafast Terahertz Spectroscopy and Optoelectronic Characterization

Recent advances in the growth of III-V semiconductor nanowires (NWs) hold great promise for nanoscale optoelectronic device applications. Recently, it was found that a small amount of nitrogen (N) incorporation in III-V semiconductor NWs can effectively red-shift their wavelength of operation and tailor their electronic properties for specific applications. However, understanding the impact of N incorporation on non-equilibrium charge carrier dynamics and transport in semiconducting NWs is critical in achieving efficient semiconducting NW devices. In this work, ultrafast optical pump-terahertz (THz) probe spectroscopy (OPTP) and electrical characterization have been used to study non-equilibrium carrier dynamics and equilibrium transport in Te-doped GaAsSb and dilute nitride GaAsSb NWs, with the goal of correlating these results with their photo-response under bias and their low-frequency noise characteristics. Nitrogen incorporation in GaAsSb NWs led to a significant increase in the carrier scattering rate, resulting in a severe reduction in carrier mobility. Carrier recombination lifetimes of 33 ps and 147 ps in GaAsSbN and GaAsSb NWs, respectively, were determined using ultrafast OPTP measurements. The reduction in the carrier lifetime and photoinduced optical conductivities are due to the presence of N-induced defects, leading to deterioration in the electrical and optical characteristics of dilute nitride NWs relative to the non-nitride NWs. Finally, we observed a very fast rise time of ~ 2 ps for both NW materials, directly impacting their potential use as high-speed photodetectors.

cond-mat.mes-hall

Manipulation of Exciton Dynamics in Single-Layer WSe2 Using a Toroidal Dielectric Metasurface

Recent advances in emerging atomically thin transition metal dichalcogenide semiconductors with strong light-matter interactions and tunable optical properties provide novel approaches for realizing new material functionalities. Coupling two-dimensional semiconductors with all-dielectric resonant nanostructures represents an especially attractive opportunity for manipulating optical properties in both the near-field and far-field regimes. Here, by integrating single-layer WSe2 and titanium oxide (TiO2) dielectric metasurfaces with toroidal resonances, we realized robust exciton emission enhancement over one order of magnitude at both room and low temperatures. Furthermore, we could control exciton dynamics and annihilation by using temperature to tailor the spectral overlap of excitonic and toroidal resonances, allowing us to selectively enhance the Purcell effect. Our results provide rich physical insight into the strong light-matter interactions in single-layer TMDs coupled with toroidal dielectric metasurfaces, with important implications for optoelectronics and photonics applications.

cond-mat.mes-hall