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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Continuum model of strong light-matter coupling for molecular polaritons

Strong coupling between light and matter generates hybrid polariton modes. We present a continuum formalism that expresses the polariton modes in terms of light and matter densities of states (DOS). We derive exact expressions for the light and matter DOS for a planar cavity containing a strongly dispersive dielectric.We show that these DOS depend exclusively on the linear response of the cavity components, i.e., the reflectance of the mirrors and the susceptibility of the dielectric. Here, we further show that, within the strong coupling regime, the light and matter DOS are well approximated by coupled mode theory. Altogether, our continuum formalism offers a unified treatment of polaritons that connects the framework of light-matter coupling with that of linear dispersion.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Methane Adsorption on Heteroatom-Modified Maquettes of Porous Carbon Surfaces

Experimental and theoretical studies disagree on the energetics of methane adsorption on carbon materials. However, this information is critical for the rational design and optimization of the structure and composition of adsorbents for natural gas storage. The delicate nature of dispersion interactions, polarization of both the adsorbent and the adsorbate, interplay between H-bonding and tetrel bonding, and induced dipole/Coulomb interactions inherent to methane physisorption require computational treatment at the highest possible level of theory. In this study, we employed the smallest reasonable computational model, a maquette of porous carbon surfaces with a central site for substitution and methane binding. The most accurate predictions of methane adsorption energetics were achieved by electron-correlated molecular orbital theory CCSD(T) and hybrid density functional theory MN15 calculations employing a saturated, all-electron basis set. Here, the characteristic geometry of methane adsorption on a carbon surface (“lander approach”) arises due to bonding interactions of the adsorbent π-system with the proximal H–C bonds of methane, in addition to tetrel bonding between the antibonding orbital of the distal C–H bond and the central atom of the maquette (C, B, or N). The polarization of the electron density, structural deformations, and the comprehensive energetic analysis clearly indicate a ∼3 kJ mol –1 preference for methane binding on the N-substituted maquette. The B-substituted maquette showed a comparable or lower binding energy than the unsubstituted, pure C model, depending on the level of theory employed. The calculated thermodynamic results indicate a strategy for incorporating electron-enriched substitutions (e.g., N) into carbon materials as a way to increase methane storage capacity over electron-deficient (e.g., B) modifications. The thermochemical analysis was revised for establishing a conceptual agreement between the experimental isosteric heat of adsorption and the binding enthalpies from statistical thermodynamics principles.

03 NATURAL GAS↗
NASA NTRS2010

NASA Tech Briefs, October 2010

Topics covered include: Hybrid Architecture Active Wavefront Sensing and Control; Carbon-Nanotube-Based Chemical Gas Sensor; Aerogel-Positronium Technology for the Detection of Small Quantities of Organic and/or Toxic Materials; Graphene-Based Reversible Nano-Switch/Sensor Schottky Diode; Inductive Non-Contact Position Sensor; High-Temperature Surface-Acoustic-Wave Transducer; Grid-Sphere Electrodes for Contact with Ionospheric Plasma; Enabling IP Header Compression in COTS Routers via Frame Relay on a Simplex Link; Ka-Band SiGe Receiver Front-End MMIC for Transponder Applications; Robust Optimization Design Algorithm for High-Frequency TWTs; Optimal and Local Connectivity Between Neuron and Synapse Array in the Quantum Dot/Silicon Brain; Method and Circuit for In-Situ Health Monitoring of Solar Cells in Space; BGen: A UML Behavior Network Generator Tool; Platform for Post-Processing Waveform-Based NDE; Electrochemical Hydrogen Peroxide Generator; Fabrication of Single, Vertically Aligned Carbon Nanotubes in 3D Nanoscale Architectures; Process to Create High-Fidelity Lunar Dust Simulants; Lithium-Ion Electrolytes Containing Phosphorous-Based, Flame-Retardant Additives; InGaP Heterojunction Barrier Solar Cells; Straight-Pore Microfilter with Efficient Regeneration; Determining Shear Stress Distribution in a Laminate; Self-Adjusting Liquid Injectors for Combustors; Handling Qualities Prediction of an F-16XL-Based Reduced Sonic Boom Aircraft; Tele-Robotic ATHLETE Controller for Kinematics - TRACK; Three-Wheel Brush-Wheel Sampler; Heterodyne Interferometer Angle Metrology; Aligning Astronomical Telescopes via Identification of Stars; Generation of Optical Combs in a WGM Resonator from a Bichromatic Pump; Large-Format AlGaN PIN Photodiode Arrays for UV Images; Fiber-Coupled Planar Light-Wave Circuit for Seed Laser Control in High Spectral Resolution Lidar Systems; On Calculating the Zero-Gravity Surface Figure of a Mirror; Optical Modification of Casimir Forces for Improved Function of Micro- and Nano-Scale Devices; Analysis, Simulation, and Verification of Knowledge-Based, Rule-Based, and Expert Systems; Core and Off-Core Processes in Systems Engineering; Digital Reconstruction Supporting Investigation of Mishaps; and Template Matching Approach to Signal Prediction.

Source record↗
DOE OSTI2025

Origin of Large Effective Phonon Magnetic Moments in Monolayer MoS 2

Recent helicity-resolved magneto-Raman spectroscopy measurement demonstrates large effective phonon magnetic moments of ~2.5 μ B in monolayer MoS 2 , highlighting resonant excitation of bright excitons as a feasible route to activate Γ-point circularly polarized phonons in transition metal dichalcogenides. However, a microscopic picture of this intriguing phenomenon remains lacking. In this work, we show that an orbital transition between the split conduction bands (Δ 0 = 4 meV) of MoS 2 couples to the doubly degenerate E" phonon mode (Ω 0 = 33 meV), forming two hybridized states. Our phononic and electronic Raman scattering measurements capture these two states: (i) one with predominantly phonon contribution in the helicity-switched channels and (ii) one with primarily orbital contribution in the helicity-conserved channels. An orbital-phonon coupling model successfully reproduces the large effective magnetic moments of the circularly polarized phonons and explains their thermodynamic properties. Strikingly, the Raman mode from the orbital transition is superimposed on a strong quasi-elastic scattering background, indicating the presence of spin fluctuations. As a result, the electrons excited to the conduction bands through the exciton exhibit paramagnetic behavior although MoS 2 is generally considered as a nonmagnetic material. By depositing nanometer-thickness nickel thin films on monolayer MoS 2 , we tune the electronic structure so that the A exciton perfectly overlaps with the 633 nm laser. The optimization of resonance excitation leads to pronounced tunability of the orbital-phonon hybridized states. Our results generalize the orbital-phonon coupling model of effective phonon magnetic moments to material systems beyond the paramagnets and magnets.

2D transition metal dichalcogenide↗
DOE OSTI2021

Hybrid gausslet/Gaussian basis sets

We introduce hybrid gausslet/Gaussian basis sets, where a standard Gaussian basis is added to a gausslet basis in order to increase accuracy near the nuclei while keeping the spacing of the grid of gausslets relatively large. The Gaussians are orthogonalized to the gausslets, which are already orthonormal, and approximations are introduced to maintain the diagonal property of the two electron part of the Hamiltonian so that it continues to scale as the second power of the number of basis functions rather than the fourth. We introduce several corrections to the Hamiltonian designed to enforce certain exact properties, such as the values of certain two-electron integrals. We also introduce a simple universal energy correction that compensates for the incompleteness of the basis stemming from the electron–electron cusps based on the measured double occupancy of each basis function. We perform a number of Hartree Fock and full configuration interaction (full-CI) test calculations on two electron systems and Hartree Fock on a ten-atom hydrogen chain to benchmark these techniques. The inclusion of the cusp correction allows us to obtain complete basis set full-CI results for the two electron cases at the level of several micro-Hartrees, and we see similar apparent accuracy for Hartree Fock on the ten-atom hydrogen chain.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Probing Coherent States of Light and Matter in Two-Dimensional Semiconductors. Final Report

The ability to enhance light-matter interactions in engineered optical environments is well-established in micro- and nano-photonics. New classes of materials bring new rich correlations between spin, momentum, and light polarization that can be exploited in these photonic systems for information processing and low-power electronics. Interfacing these novel material features with strong optical interactions suggests the compelling capability to create hybrid light-matter systems harnessing low-energy and protected material properties such as spin. The long-term objective of this program was to investigate the interplay between pseudospin in 2D materials and light, revealing new coherent phenomena. The materials studied are the monolayer transition metal dichalcogenides (TMDs), which support polarization-sensitive optical transitions when isolated to a single sub-nanometer crystal layer in thickness. In particular, monolayer TMD semiconductors such as MoS 2 exhibit degenerate valleys in momentum space with distinct spin character. These valleys can be separately addressed by circularly polarized light, providing a tool for manipulation. Integrating this valley pseudospin of excitons in monolayer TMDs with engineered strong optical excitations to create novel coherent phenomena was a key long-term goal of this research. The scope of this research primarily focused on studying light-matter interactions of valley-sensitive excitations in monolayer TMDs. The scope also included the integration of monolayer materials that support valley-polarized emission into photonic devices. This approach extends prior work on exciton-polaritons in 2D materials toward a platform with far more control and improved light input and output characteristics to aid scalability of these polarization-sensitive phenomena to many-body, long-range optical networks. During the course of the five-year Early Career program, the approaches led to successful progress on each proposed aim. Initial successful work seeded additional research that developed from the main themes, while this program focus evolved toward coherent manipulation of valley polaritons and integration with photonics. Both of these advanced topics set the stage for new capabilities in future innovative research. The results of this project provide advances in materials and methods relevant for new visions of opto-electronics and photonics that can improve information processing in an era of increased focus on quantum and coherent phenomena. The research has also contributed to the training of two postdoctoral scholars and five graduate students.

2D Materials↗
DOE OSTI2020

Spin-orbit-proximitized ferromagnetic metal by monolayer transition metal dichalcogenide: Atlas of spectral functions, spin textures, and spin-orbit torques in Co/MoSe 2 , Co/WSe 2 and Co/TaSe 2 heterostructures

In this work, the heterostructures composed of an ultrathin ferromagnetic metal (FM) and a material hosting strong spin-orbit (SO) coupling are the principal resource for SO torque and spin-to-charge conversion nonequilibrium effects in spintronics. The key quantity in theoretical description of these effects is nonequilibrium spin density, which can appear on any monolayer of the heterostructure through which the current is flowing as long as the monolayer bands are affected by the native or proximity induced SO coupling. Here we demonstrate how hybridization of wave functions of Co layer and a monolayer of transition metal dichalcogenides (TMDs)—such as semiconducting MoSe 2 and WSe 2 or metallic TaSe 2 —can lead to dramatic transmutation of electronic and spin structure of Co within some distance away from its interface with TMD, when compared to the bulk of Co or its surface in contact with a vacuum. This is due to proximity induced SO splitting of Co bands encoded in the spectral functions and spin textures on its monolayers, which we obtain using noncollinear density functional theory (ncDFT) combined with equilibrium Green function (GF) calculations. In fact, SO splitting is present due to structural inversion asymmetry of the bilayer—i.e., just the presence of the interface—even if SO coupling within TMD monolayer is artificially switched off in ncDFT calculations. However, switching it on makes the effects associated with proximity SO coupling within Co layer about five times larger. Injecting spin-unpolarized charge current through SO-proximitized monolayers of Co generates nonequilibrium spin density over them, so that its cross product with the magnetization of Co determines SO torque. The SO torque computed via first-principles quantum transport methodology, which combines ncDFT with nonequilibrium GF calculations, can be used as the screening parameter to identify optimal combination of materials and their interfaces for applications in spintronics. In particular, we identify heterostructure two-monolayer-Co/monolayer-WSe 2 as the most optimal one, at least in the clean limit.

2-dimensional systems↗
DOE OSTI2020

Recent Developments in the General Atomic and Molecular Electronic Structure System

A discussion of many of the recently implemented features of GAMESS (General Atomic and Molecular Electronic Structure System) and LibCChem (the C++ CPU/GPU library associated with GAMESS) is presented. These features include fragmentation methods like the fragment molecular orbital, effective fragment potential and effective fragment molecular orbital methods, hybrid MPI/OpenMP approaches to Hartree-Fock and resolution of the identity second order perturbation theory. Many new coupled cluster theory methods have been implemented in GAMESS, as have multiple levels of density functional/tight binding theory. The role of accelerators, especially graphical processing units, is discussed in the context of the new features of LibCChem, as is the associated problem of power consumption as the power of computers increases dramatically. The process by which a complex program suite like GAMESS is maintained and developed is considered. Future developments are briefly summarized.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Magic-Angle Twisted Bilayer Graphene as a Topological Heavy Fermion Problem

Magic-angle (θ=1.05°) twisted bilayer graphene (MATBG) has shown two seemingly contradictory characters: the localization and quantum-dot-like behavior in STM experiments, and delocalization in transport experiments. We construct a model, which naturally captures the two aspects, from the Bistritzer-MacDonald (BM) model in a first principle spirit. A set of local flat-band orbitals (f) centered at the AA-stacking regions are responsible to the localization. A set of extended topological semimetallic conduction bands (c), which are at small energetic separation from the local orbitals, are responsible to the delocalization and transport. The topological flat bands of the BM model appear as a result of the hybridization of f and c electrons. This model then provides a new perspective for the strong correlation physics, which is now described as strongly correlated f electrons coupled to nearly free c electrons—we hence name our model as the topological heavy fermion model. Using this model, we obtain the U(4) and U(4)×U(4) symmetries of Refs. [1–5] as well as the correlated insulator phases and their energies. Simple rules for the ground states and their Chern numbers are derived. Moreover, features such as the large dispersion of the charge ±1 excitations [2,6,7], and the minima of the charge gap at the Γ M point can now, for the first time, be understood both qualitatively and quantitatively in a simple physical picture. Our mapping opens the prospect of using heavy-fermion physics machinery to the superconducting physics of MATBG.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Screened Range-Separated Hybrid Functional with Polarizable Continuum Model Overcomes Challenges in Describing Triplet Excitations in the Condensed Phase Using TDDFT

Long range-corrected (LRC) or range-separated hybrid (RSH) functionals where the long-range (LR) limit of electronic interactions is set to the exact exchange have been shown to correct the tendency of traditional density functional theory (DFT) to underestimate the frontier orbital gap. Consequently, the use of such functionals in calculating electronic excited states using linear response based time-dependent DFT (TDDFT) has been successful in correcting the tendency for underestimating the energies of charge transfer states by DFT-based calculations. More recently formulations of functionals that attenuate the LR limit to address condensed-phase effects to polarize the electronic density have been reported. In particular screened RSH (SRSH) combined with polarizable continuum model (PCM) was benchmarked successfully in reproducing the fundamental gap and charge transfer state energies of molecular systems in the condensed phase. Here we use SRSH-PCM to address triplet excited states, and show its success in obtaining correspondence of the low-lying triplet states to the singlet–triplet gap in a similar way that the fundamental orbital gap corresponds to electron removal and addition energies. Importantly, the accuracy of the SRSH-PCM in calculating triplet excitations stands on the polarization consistent framework in addressing the scalar dielectric constant and without affecting the optimal tuning by triplet energies. Finally, the prospect of even further improving the SRSH-PCM accuracy in calculating triplet states can be achieved by optimal tuning on the basis of the spin multiplicity gap.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Delocalized polaron and Burstein-Moss shift induced by Li in α–V 2 O 5 : A DFT + DMFT study

For this work, we performed density functional theory (DFT)+U and dynamical mean field theory (DMFT) calculations with a continuous-time quantum Monte Carlo impurity solver to investigate the electronic properties of V 2 O 5 and Li x V 2 O 5 (x = 0.125 and 0.25). Pristine V 2 O 5 is a charge-transfer insulator with strong O p–V d hybridization, and it exhibits a large band gap (E gap ) as well as a nonzero conduction-band (CB) gap.We show that the band gap, the number of d electrons of vanadium, N d , and the CB gap for V 2 O 5 obtained from our DMFT calculations are in excellent agreement with the experimental values. While the DFT +U approach replicates the experimental band gap, it overestimates the value of N d and underestimates the CB gap. In the presence of low Li doping, the electronic properties of V 2 O 5 are mainly driven by a polaronic mechanism, and electron spin resonance and electron nuclear double resonance spectroscopies observed the coexistence of free and bound polarons. Notably, our DMFT results identify both polaron types, with the bound polaron being energetically preferred, while the DFT +U method only predicts the free polaron. Our DMFT analysis also reveals that increased Li doping leads to electron filling in the conduction band, shifting the Fermi level. This result is consistent with the observed Burstein-Moss shift upon enhanced Li doping, and we thus demonstrate that the DFT + DMFT approach can be used for an accurate and realistic description of strongly correlated materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Ultrafast Dynamics of Plasmon-Coupled Excitons in Semiconducting Nanoplatelets

Exciton-plasmon coupling in nanomaterials produces many relevant phenomena for photonics applications including increased light-matter interactions, enhanced radiative rates of quantum emitters, and coherent energy exchange. In the case of exciton coupling to surface plasmon polaritons (SPPs), dispersive interactions controlled by the wavevector of optical excitation create the opportunity for tunable optical emission. Strong temporal impacts on exciton lifetimes can also occur in coupled systems, creating the opportunity for ultrafast control of exciton lifetime via changes in electronic coupling magnitude to a dispersive SPP. The coupling strength can be impacted by the morphology of the nanomaterials. Here, in this study, we utilize colloidal semiconductor nanoplatelets deposited onto thin silver plasmonic films, and compare the results to semiconductor quantum dots deposited on the silver films. We map the dispersion of the coupled systems and measure the ultrafast transient absorption response of the coupled systems. Due to the larger interaction areas of the nanoplatelets that lie flat on the silver films, a greater degree of coupling is found for the nanoplatelets, and much faster temporal responses are found as compared to quantum dots. Fresnel theory calculations that incorporate heavy and light hole features can reproduce the dispersion of the nanoplatelet-silver film, and a simple three-state model is developed to provide insights into the nature of the coupling at different photon energies along the dispersion curve.

colloidal semiconductor nanoplatelets↗
DOE OSTI2024

2D material platform for overcoming the amplitude–phase tradeoff in ring resonators

Compact and high-speed electro-optic phase modulators play a vital role in various large-scale applications including optical computing, quantum and neural networks, and optical communication links. Conventional electro-refractive phase modulators such as silicon (Si), III-V and graphene on Si suffer from a fundamental tradeoff between device length and optical loss that limits their scaling capabilities. High-finesse ring resonators have been traditionally used as compact intensity modulators, but their use for phase modulation has been limited due to the high insertion loss associated with the phase shift. Here, we show that high-finesse resonators can achieve a strong phase shift with low insertion loss by simultaneous modulation of the real and imaginary parts of the refractive index, to the same extent, i.e., Δ n Δ k ∼1. To implement this strategy, we demonstrate an active hybrid platform that combines a low-loss SiN ring resonator with 2D materials such as graphene and transition metal dichalcogenide [tungsten disulphide (WSe 2 )], which induces a strong change in the imaginary and real parts of the index. Our platform consisting of a 25 µm long Gr-Al 2 O 3 -WSe 2 capacitor embedded on a SiN ring of 50 µm radius (∼8% ring coverage) achieves a continuous phase shift of (0.46±0.05) π radians with an insertion loss (IL) of 3.18±0.20 dB and a transmission modulation (Δ T Ring ) of 1.72±0.15dB at a probe wavelength ( λ p ) of 1646.18 nm. We find that our Gr-Al 2 O 3 -WSe 2 capacitor exhibits a phase modulation efficiency ( V π 2 ⋅ L ) of 0.530±0.016V⋅cm and can support an electro-optic bandwidth of 14.9±0.1GHz. We further show that our platform can achieve a phase shift of π radians with an IL of 5 dB and a minimum Δ T of 0.046 dB. We demonstrate the broadband nature of the binary phase response, by measuring a phase shift of (1.00±0.10) π radians, with an IL of 5.20±0.31dB and a minimal Δ T Ring of 0.015±0.006dB for resonances spanning from 1564 to 1650 nm. This SiN–2D hybrid platform provides the design for compact and high-speed reconfigurable circuits with graphene and transition metal dichalcogenide (TMD) monolayers that can enable large-scale photonic systems.

Datta, Ipshita (ORCID:0000000318842882)↗
DOE OSTI2021

Too big, too small, or just right? A benchmark assessment of density functional theory for predicting the spatial extent of the electron density of small chemical systems

Multipole moments are the first-order responses of the energy to spatial derivatives of the electric field strength. The quality of density functional theory prediction of molecular multipole moments thus characterizes errors in modeling the electron density itself, as well as the performance in describing molecules interacting with external electric fields. However, only the lowest non-zero moment is translationally invariant, making the higher-order moments origin-dependent. Therefore, instead of using the 3 × 3 quadrupole moment matrix, we utilize the translationally invariant 3 × 3 matrix of second cumulants (or spatial variances) of the electron density as the quantity of interest (denoted by K). The principal components of K are the square of the spatial extent of the electron density along each axis. A benchmark dataset of the principal components of K for 100 small molecules at the coupled cluster singles and doubles with perturbative triples at the complete basis set limit is developed, resulting in 213 independent K components. The performance of 47 popular and recent density functionals is assessed against this Var213 dataset. Several functionals, especially double hybrids, and also SCAN and SCAN0 predict reliable second cumulants, although some modern, empirically parameterized functionals yield more disappointing performance. The H, Li, and Be atoms, in particular, are challenging for nearly all methods, indicating that future functional development could benefit from the inclusion of their density information in training or testing protocols.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Ubiquity of amplitude-modulated magnetic ordering in the H - T phase diagram of the frustrated non-Fermi-liquid YbAgGe

YbAgGe contains a magnetic geometrically frustrated kagome-like lattice that also features significant local single-ion anisotropy. The electronic state is established by hybridization of 4f and conduction electrons leading to heavy electronic masses. The competition between these various interactions leads to nontrivial behavior under external magnetic field, including a sequence of magnetic phase transitions, non-Fermi-liquid states, and possibly a quantum critical point. We present a series of neutron diffraction experiments performed in the mK temperature range and under magnetic fields up to 8 T in the hexagonal plane, revealing the microscopic nature of the first four subsequent magnetic states of this phase diagram. The magnetic phases are associated with the propagation vectors K 1 =($\frac{1}{3}$ 0 $\frac{1}{3}$) for H < 2 T, K 2 = (0 0 0.32) for 2 T < H < 3 T, K 1 = ($\frac{1}{3}$ 0 $\frac{1}{3}$) for 3 T < H < 4.5 T and k 3 = (0.195 0.195 0.38) for 4.5 T < H < 7 T. Our structural refinements reveal a strong modulation of the magnetic moment amplitude in all phases. We observe that the ordered moments of the three magnetically different Yb sites become increasingly different in field, which complies with the principle local anisotropy directions relative to the field direction. While the ordered moments are aligned predominantly in the hexagonal plane, we also find a significant out-of-plane component and a ferromagnetic contribution above 2 T. Here we discuss possible scenarios that may evolve around the phase boundary at 4.5 T, which is associated with putative quantum criticality as identified by various bulk probes. We propose further steps that are required to better understand the microscopic interactions in this material.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Switching of Hybrid Improper Ferroelectricity in Oxide Double Perovskites

In ABO 3 -type perovskite oxides with Pnma symmetry, rotation (Q R+ , a 0 a 0 c + ) and tilt (Q T , a – a – c 0 ) of BO 6 octahedra are the two primary order parameters. These order parameters establish an inherent trilinear coupling with anti-ferroelectric A-site displacement (Q AFE ) to form the low-symmetry phase. The symmetry is further lowered in double perovskite oxides (DPOs) due to A/A' cation ordering. It in turn makes these systems polar via hybrid improper ferroelectric mechanism, primarily driven by Q R+ and Q T . Naturally, it has been believed that functionalities such as polarization can also be switched by tuning these primary order parameters. However, mystery around finding switching mechanism still remains. Our study based on density functional theory calculations combined with finite-temperature molecular dynamics simulations shows that the polarization switching is a two-step process, driven by out-of-phase rotation (Q R– , a 0 a 0 c – when Q T = 0 or, a – a – b – when Q T ≠ 0). A series of polar DPOs such as KLnFeOsO 6 [Ln = Sm, Gd, Dy, Tm (lanthanides) and Y (rare earth)], all belonging to P2 1 symmetry, are considered in this investigation. The polarization switching P ($\overrightarrow{P}$) occurs at a very high temperature of ~1150 K through a phase transition, from a polar (P2 1 ) phase with $\overrightarrow{P}$(+) to $\overrightarrow{P}$(-) via a non-polar P4/n phase. The switching itself is metastable in nature. The switching (both polarization and spin state) is only observed for a very short period of time (~23 ps) that poses limitation on using such a mechanism in memory device realization. We demonstrate a concurrent heating–cooling procedure to overcome such shortcoming. In conclusion, simulations conducted at 600 K further imply that long lasting switching can be achieved, at least for 1.2 ns for 600 K, and ideally for an infinite time, if the material is heated just above the T c followed by rapid cooling to a temperature below T c .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Interplay of Kondo physics with incommensurate charge density waves in CeTe 3

CeTe 3 is a 2-dimensional (2D) Van der Waals (VdW) material with incommensurate charge density waves (CDW), extremely high transition temperature (T CDW ), and a large momentum-dependent CDW gap that leaves a significant portion of the Fermi surface intact. It is also considered to be a weak Kondo system, a property unexpected for a material with incommensurate CDW, where each atomic site is slightly different. Here, we study the properties of the CDW state in several RTe3 (R is rare earth) materials and examine the hybridization of itinerant states with the localized Ce 4f multiplet in CeTe 3 by using angle resolved photoemission spectroscopy. We find that the renormalization of the itinerant states originating from the hybridization with the deeper localized 4f states at −260 meV is k−dependent and extends to the Fermi level. As these localized states are far from the Fermi level, the observed hybridization affects the effective masses only marginally and does not lead to heavy fermions. However, since the same renormalizing mechanism normally leads to the heavy fermion physics when the localized 4f states are near the Fermi level, our observation of its strong k−dependence suggests that this could be the reason for discrepancy between the heavy masses in specific heat and light ones in Shubnikov de Haas oscillations, often observed in heavy fermions.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Stability, electronic quantum states, and magnetic interactions of Er 3+ ions in Ga 2 ⁢O 3

Here, we report an ab initio study of phase stability, defect formation, electronic structure, and multiple magnetic, Dzyaloshinskii-Moriya, optical, hyperfine, and crystal field interactions in erbium (Er)-doped wide band gap 𝛼- and 𝛽-gallium oxides (Ga 2 ⁢O 3 ), critically important to make a foundation for both optoelectronic and quantum information applications. The chemical, structural, mechanical, and dynamical stabilities of the pristine phases are confirmed from respective negative formation energies, negative cohesive energies, favorable elastic constants, and positive phonon frequencies. The phonon dispersions indicate that the Ga-O bonds are uniform in the 𝛼-phase, while they vary in the 𝛽-phase due to the anisotropic polyhedral movement. The defect formation energy analysis confirms that both Er-doped 𝛼- and 𝛽−Ga 2 ⁢O 3 prefer Er 3+ (neutral) state. The underestimated band gaps of the pristine phases from standard density functional theory (DFT) calculations as compared to experimental values are corrected by employing the hybrid functional calculations, resulting in the indirect band gaps of 5.21 eV in 𝛼−Ga 2 ⁢O 3 and 4.94 eV in 𝛽−Ga 2 ⁢O 3 . The site preference energy analysis indicates partial occupation of Er in the octahedral site of Ga. The anisotropic nature of hyperfine tensor coefficients of Er is similar in both phases, which may be due to the occupation of Er in the same octahedral Ga site. On the other hand, the calculated magnetic exchange interaction between two Er dopants is negative for 𝛼 and positive for 𝛽, indicating an antiferromagnetic (AFM) ground state in the former and a ferromagnetic (FM) ground state in the latter. Large values of Dzyaloshinskii-Moriya interactions (DMIs) are obtained along the 𝑥 direction in the 𝛼 and along the 𝑦 direction in the 𝛽. The large DMI may support exotic magnetic textures, a promising direction for spintronic applications. The analysis of dielectric constants and refractive indices of both pristine and Er-doped phases shows a good agreement with available experimental values. The calculated optical anisotropy is slightly higher in 𝛽 than those in 𝛼, which is due to the involvement of lower symmetry in 𝛽. The crystal field coefficients (CFCs) calculated from DFT are used to analyze 4⁢𝑓 multiplets and 4⁢𝑓 −4⁢𝑓 transitions. Thus calculated lowest energy level of the first excited state to the lowest energy level of the ground state is about 1.53 µ⁢m, which is in a good agreement with available experiments, and it falls within the quantum telecommunication wavelength range.

3-dimensional systems↗