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At least 757 records · Page 42
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Highly Conjugated Porphyrin Arrays Enable Optical Resolution of Ferromagnetic and Antiferromagnetic Aligned States of the Triplet Exciton and an Incorporated Stable Radical

Well-defined photogenerated molecular spin systems have potential utility in spintronics and quantum information science (QIS). Because molecular magnetic, optical, and electronic properties can be controlled by design, diverse spin systems can be prepared at modest temperatures. Photogenerated molecular spin systems often involve states prepared from the interaction of excitons and charges. Resolving the nature of electron spin alignment in photogenerated spin states described by the coupling of a triplet exciton and a stable radical commonly relies on EPR spectroscopy. Here, we describe ethyne-bridged (porphinato)metal ( PM n ) oligomers that incorporate a macrocycle-bound Cu(II) radical center. Upon photoexcitation of such PM n arrays, a singdoublet ( 2 S 1 ) state is formed; ultrafast internal conversion (IC) then produces a tripdoublet ( 2 T 1 ) state, which undergoes intersystem crossing (ISC) to produce a tripquartet ( 4 T 1 ) state, before relaxation to the ground state ( 2 S 0 ). These highly conjugated Cu(II) radical-containing PMn arrays enable direct observation of copper porphyrin 2 T 1 → 4 T 1 ISC dynamics from the biexponential decay of the near-infrared (NIR) 2,4 T 1 → 2,4 T n transient absorption manifold. Multireference n-electron valence perturbation theory (NEVPT2) computations illuminate how PM n electronic structure controls the relaxation dynamics of these long-lived (>10 ns) electronically excited multiplet states. These studies show that highly conjugated and polarizable porphyrin arrays incorporating stable spin centers provide rare π-delocalized systems where the ferromagnetic and antiferromagnetic alignment between a triplet exciton and a stable radical are both spectrally resolved and addressable using transient optical spectroscopy at wavelengths exceeding 1 μm, providing new opportunities to QIS.

14 SOLAR ENERGY↗
DOE OSTI2020

Performance of an atomic mean-field spin–orbit approach within exact two-component theory for perturbative treatment of spin–orbit coupling

The paper reports development of an atomic mean-field (AMF) spin–orbit approach within the spin-free exact two-component theory in its one-electron variant (SFX2C-1e), a new relativistic quantum-chemical method for treating spin-orbit coupling in molecules. The effective one-electron spin–orbit integral matrix in the four-component representation is assembled as a direct sum of one-centre spin–orbit integral matrices with the mean-field two-electron contributions evaluated using atomic SFX2C-1e Hartree–Fock density matrices. It is then transformed into two-component representation using analytic SFX2C-1e energy derivative formulation. The resulting two-component spin–orbit integral matrix is by design suitable for use in perturbative calculations of spin–orbit coupling, treating SFX2C-1e wavefunctions as unperturbed states. The accuracy of the present AMF approach has been demonstrated using benchmark calculations of spin–orbit splittings for representative diatomic radicals at the equation-of-motion coupled-cluster singles and doubles level. In conclusion, to demonstrate the applicability and accuracy of the present perturbative spin–orbit scheme in calculations of challenging heavy-element containing systems, a thorough computational investigation of six low-lying electronic states of ThO+ is reported.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Magnetoresistance effects in a spin-fermion model for multilayers

Here, we consider a spin-fermion model consisting of free electrons coupled to classical spins where the latter are embedded in a quasi-one-dimensional superlattice structure consisting of spin blocks separated by spinless buffers. Using a spiral ansatz for the spins, we study the effect of the electron mediated Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction on the $\textit{T}$ = 0 ground state of the system. We find that the RKKY interaction can lead to ferromagnetic, antiferromagnetic, or intermediate spiral phases for different system parameters. When the width is much larger than the length of the individual blocks, the spiral phases are suppressed, and the ground state oscillates between ferromagnetic and antiferromagnetic orders as the size of the buffer regions is varied. This is accompanied by a corresponding oscillation in the Drude weight reflecting an increased conductivity in the ferromagnetic state compared to the antiferromagnetic one. These results are reminiscent of classic giant magnetoresistance phenomena observed in a similar geometry of thin sandwiched magnetic and nonmagnetic layers. Our analysis provides a robust framework for understanding the role of the RKKY interaction on the ground-state order and corresponding transport properties of such systems, extending beyond the conventional perturbative regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Predicting magnetic properties of single-molecule magnets from self-interaction-free density-functional theory (Final Report)

In this project we investigated electronic structure of an intermediate-sized copper-based molecule and magnetic and hyperfine properties of several small non-magnetic and magnetic molecules including transition-metal elements by applying self-interaction corrections to density functional theory (DFT). In a sufficient number of cases, DFT-calculated electronic structure and magnetic properties of single-molecule magnets qualitatively differ from corresponding experimental data. This is partly due to self-interacting electrons within the DFT formalism. Recently, an efficient method to correct the self-interactions was proposed, i.e., Fermi-Lowdin prbital (FLO) based self-interaction corrected (SIC) methodology, within DFT. Henceforth, this method is referred to as FLO-SIC method which exists in FLOSIC code. We used this FLO-SIC method for our studies of electronic structure and magnetic and hyperfine properties of small magnetic molecules and non-magnetic molecules. Our study will provide insight into predictions of magnetic properties of single-molecule magnets where self-interaction corrections play a critical role. There are two components of this project. In the first work, we studied the electronic structure of a planar mononuclear Cu-based molecule in two oxidation states, using DFT with the FLO-SIC method. We chose this system because it is small enough and it includes a transition metal element. We found that the standard FLO-SIC method takes too much compute time even for the small transition-metal molecule and so we slightly modified the method in order to expedite the process. In the dianionic state, we found that the FLO-SIC spin density agrees quantitatively with accurate quantum chemistry methods, while DFT spin density without self-interaction corrections are severely deviated from the quantum chemistry methods. We also showed that the energy gap between the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) of the dianionic state is larger than that of the monoanionic state. This result is consistent with experimental data. In the second work, we investigated how the interaction between the electron spin and nuclear spin is affected by electron self-interactions within small non-magnetic and magnetic molecules. Such an interaction is called hyperfine interaction. For molecules without significant orbital angular momentum, the hyperfine interaction consists of Fermi contact and dipolar interaction terms. Since the Fermi contact term depends on electron spin density at the nuclear site, it would be highly affected by self-interaction corrections. Therefore, we calculated the hyperfine interaction for the small molecules using DFT with the slightly modified expedited FLO-SIC method which was obtained in the first work, and compared the results to experimental data and DFT calculations without self-interaction corrections. We found significant improvement of the Fermi contact term computed using the FLO-SIC method for small magnetic molecules. Overall, the first and second work provided positive outlook of application of the FLO-SIC method to magnetic molecules and systems including transition-metal elements.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Crystal structure and magnetism of actinide oxides: a review

In actinide systems, the 5f electrons experience a uniquely delicate balance of effects and interactions having similar energy scales, which are often difficult to properly disentangle. This interplay of factors such as the dual nature of 5f-states, strong electronic correlations, and strong spin–orbit coupling results in electronically unusual and intriguing behavior such as multi-k antiferromagnetic ordering, multipolar ordering, Mott-physics, mixed valence configurations, and more. Despite the inherent allure of their exotic properties, the exploratory science of even the more basic, binary systems like the actinide oxides has been limited due to their toxicity, radioactivity, and reactivity. In this article, we provide an overview of the available synthesis techniques for selected binary actinide oxides, including the actinide dioxides, sesquioxides, and a selection of higher oxides. For these oxides, here we also review and evaluate the current state of knowledge of their crystal structures and magnetic properties. In many aspects, substantial knowledge gaps exist in the current body of research on actinide oxides related to understanding their electronic ground states. Bridging these gaps is vital for improving not only a fundamental understanding of these systems but also of future nuclear technologies. To this end, we note the experimental techniques and necessary future investigations which may aid in better elucidating the nature of these fascinating systems.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Electronic anisotropy and rotational symmetry breaking at a Weyl semimetal/spin ice interface

In magnetic pyrochlore materials, the interplay of spin-orbit coupling, electronic correlations, and geometrical frustration gives rise to exotic quantum phases, including topological semimetals and spin ice. While these phases have been observed in isolation, the interface-driven phenomena emerging from their interaction have never been realized previously. Here, we report on the discovery of interfacial electronic anisotropy and rotational symmetry breaking at a heterostructure consisting of the Weyl semimetal Eu 2 Ir 2 O 7 and spin ice Dy 2 Ti 2 O 7 . Subjected to magnetic fields, we unveil a sixfold anisotropic transport response that is theoretically accounted by a Kondo-coupled heterointerface, where the spin ice’s field-tuned magnetism induces electron scattering in the Weyl semimetal’s topological Fermi-arc states. Furthermore, at elevated magnetic fields, we reveal a twofold anisotropic response indicative of the emergence of a symmetry-broken many-body state. This discovery showcases the potential of pyrochlore frustrated magnet/topological semimetal heterostructures in search of emergent interfacial phenomena.

Science & Technology - Other Topics↗
DOE OSTI2022

Measuring the Electric Dipole Moment of the Electron in a Two-Energy Spin-Transparent Storage Ring

We will present a new design of a two-energy storage ring for low energy (0.2 to 2 MeV) polarized electron bunches [1]. The new design is based on the transparent spin methodology that cancels the spin precession due to the magnetic dipole moment at any energy while allowing for spin precession induced by the fundamental physics of interest to accumulate. The buildup of the vertical component of beam polarization can be measured using standard Mott polarimetry that is optimal at low electron energy. These rings can be used to measure the permanent electric dipole moment of the electron, relevant to CP violation and matter-antimatter asymmetry in the universe, and to search for dark energy and ultra-light dark matter.

Suleiman, R.↗
DOE OSTI2022

Measuring the Electric Dipole Moment of the Electron in a Two-Energy Spin-Transparent Storage Ring

We will present a new design of a two-energy storage ring for low energy (0.2 to 2 MeV) polarized electron bunches [1]. The new design is based on the transparent spin methodology that cancels the spin precession due to the magnetic dipole moment at any energy while allowing for spin precession induced by the fundamental physics of interest to accumulate. The buildup of the vertical component of beam polarization can be measured using standard Mott polarimetry that is optimal at low electron energy. These rings can be used to measure the permanent electric dipole moment of the electron, relevant to CP violation and matter-antimatter asymmetry in the universe, and to search for dark energy and ultra-light dark matter.

Suleiman, R.↗
DOE OSTI2024

Photo-induced non-collinear interlayer RKKY coupling in bulk Rashba semiconductors

Abstract The interplay between light-matter, spin-orbit, and magnetic interactions allows the investigation of light-induced magnetic phenomena that are otherwise absent without irradiation. We present our analysis of light-driven effects on the interlayer exchange coupling mediated by a bulk Rashba semiconductor in a magnetic multilayer. The collinear magnetic exchange coupling mediated by the photon-dressed spin-orbit coupled electrons of BiTeI develops light-induced oscillation periods and displays new decay power laws, both of which are enhanced with an increasing light-matter coupling. For magnetic layers with non-collinear magnetization, we find a non-collinear magnetic exchange coupling uniquely generated by light-driving of the multilayer. As the non-collinear magnetic exchange coupling mediated by the photon-dressed electrons of BiTeI is unique to the irradiated system and it is enhanced with increasing light-matter coupling, this effect offers a promising platform of investigation of light-driven effects on magnetic phenomena in spin-orbit coupled systems. In this platform, light properties, such as its intensity, can serve as external knobs for inducing non-collinear couplings of the interlayer exchange and for modulating the collinear couplings. Both of these effects signify the photo-generated modification in the spin textures of spin-orbit coupled electrons in BiTeI.

Physics↗
DOE OSTI2026

Current-Driven Symmetry Breaking and Spin–Orbit Polarization in Chiral Wires

The spin dynamics of electrons in chiral molecular systems remains a topic of intense interest, particularly regarding whether geometric chirality inherently induces spin polarization in current-carrying electrons. In this work, we employ ab initio real-time time-dependent density functional theory (rt-TDDFT) to directly simulate the interplay among charge current, spin, and orbital. This realtime tracking extends beyond perturbative treatments, and we analyze how nonequilibrium currents effectively lift the symmetry constraints of screw rotation and time-reversal symmetry. We find that the emergence of spin and orbital angular momenta is dynamically correlated with a concomitant loss of translational (linear) momentum, which we interpret as an intrinsic consequence of current-driven symmetry lowering. The implications of this mechanism for chirality-induced spin selectivity and spintronics device design are discussed.

chiral wire↗
DOE OSTI2021

Nonclassical Spin Transfer Effects in an Antiferromagnet

We simulate scattering of electrons by a chain of antiferromagnetically coupled quantum Heisenberg spins, to analyze spin-transfer effects not described by the classical models of magnetism. Our simulations demonstrate efficient excitation of dynamical states that would be forbidden by the semiclassical symmetries, such as generation of multiple magnetic excitation quanta by a single electron. Furthermore, quantum interference of spin wave functions enables generation of magnetization dynamics with amplitudes exceeding the transferred magnetic moment. Here, the efficiency of excitation is almost independent of the electron spin polarization, and is governed mainly by the transfer of energy. Nonclassical spin transfer may thus enable efficient electronic control of antiferromagnets not limited by the classical constraints.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Spin phase diagram of the interacting quantum Hall liquid

Measurement of the ground-state spin polarization of quantum systems offers great potential for the discovery and characterization of correlated electronic states. However, spin polarization measurements have mainly involved optical and NMR techniques that perturb the delicate ground states and, for quantum Hall systems, have provided conflicting results. In this work we present spin-resolved pulsed tunnelling (SRPT) that precisely determines the phase diagram of the ground-state spin polarization as a function of magnetic field and Landau level (LL) filling factor ($ν$) with negligible perturbation to the system. Our phase diagram shows a variety of polarized, unpolarized and topological spin states in the lowest (N = 0) LL, which can largely be described by a weakly interacting composite fermion (CF) model7. However, the phase diagram shows unexpected behaviour in the N = 1 LL. We observe fully polarized $ν$ = 5/2 and 8/3 states but a partially depolarized $ν$ = 7/3 state. This behaviour deviates from the conventional theoretical picture of weakly interacting fractional quasiparticles, but instead suggests unusual electronic correlations and the possibility of new non-Abelian phases. The results establish SRPT as a powerful technique for investigating correlated electron phenomena.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Origin of Ferromagnetic Exchange Coupling in Donor–Acceptor Biradical Analogues of Charge-Separated Excited States

A new donor–acceptor biradical complex, Tp Cum,Me Zn(SQ-VD) (Tp Cum,Me Zn + = zinc(II) hydro-tris(3-cumenyl-5-methylpyrazolyl)borate complex cation; SQ = orthosemiquinone; VD = oxoverdazyl), which is a ground-state analogue of a charge-separated excited state, has been synthesized and structurally characterized. Here, the magnetic exchange interaction between the S = 1/2 SQ and the S = 1/2 VD within the SQ-VD biradical ligand is observed to be ferromagnetic, with $J_{SQ-VD}$ = +77 cm –1 (H = -2$J_{SQ-VD}\bar{S}_{SQ}·\bar{S}_{VD}$) determined from an analysis of the variable-temperature magnetic susceptibility data. The pairwise biradical exchange interaction in Tp Cum,Me Zn(SQ-VD) can be compared with that of the related donor–acceptor biradical complex Tp Cum,Me Zn(SQ-NN) (NN = nitronyl nitroxide, S = 1/2), where $J_{SQ-NN}$ ≅ +550 cm –1 . This represents a dramatic reduction in the biradical exchange by a factor of ~7, despite the isolobal nature of the VD and NN acceptor radical SOMOs. Computations assessing the magnitude of the exchange were performed using a broken-symmetry density functional theory (DFT) approach. These computations are in good agreement with those computed at the CASSCF NEVPT2 level, which also reveals an S = 1 triplet ground state as observed in the magnetic susceptibility measurements. A combination of electronic absorption spectroscopy and CASSCF computations has been used to elucidate the electronic origin of the large difference in the magnitude of the biradical exchange coupling between Tp Cum,Me Zn(SQ-VD) and Tp Cum,Me Zn(SQ-NN). A Valence Bond Configuration Interaction (VBCI) model was previously employed to highlight the importance of mixing an SQ SOMO → NNLUMO charge transfer configuration into the electronic ground state to facilitate the stabilization of the high-spin triplet (S = 1) ground state in Tp Cum,Me Zn(SQ-NN). Here, CASSCF computations confirm the importance of mixing the pendant radical (e.g., VD, NN) LUMO (VD LUMO and NN LUMO ) with the SOMO of the SQ radical (SQ SOMO ) for stabilizing the triplet, in addition to spin polarization and charge transfer contributions to the exchange. An important electronic structure difference between Tp Cum,Me Zn(SQ-VD) and Tp Cum,Me Zn(SQ-NN), which leads to their different exchange couplings, is the reduced admixture of excited states that promote ferromagnetic exchange into the Tp Cum,Me Zn(SQ-VD) ground state, and the intrinsically weaker mixing between the VD LUMO and the SQ SOMO compared to that observed for Tp Cum,Me Zn(SQ-NN), where this orbital mixing is significant. The results of this comparative study contribute to a greater understanding of biradical exchange interactions, which are important to our understanding of excited-state singlet–triplet energy gaps, electron delocalization, and the generation of electron spin polarization in both the ground and excited states of (bpy)Pt(CAT-radical) complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Fluctuation-induced odd-frequency spin-triplet pairing in a disordered electron liquid

Here we consider a two-dimensional disordered conductor in the regime when the superconducting phase is destroyed by the magnetic field. We analyze a combination of fluctuations of different origin which results in an effective interaction amplitude suitable for a spontaneous s-wave odd-frequency pairing instability. We observe that the end point of the superconductivity is a quantum critical point separating the conventional superconducting phase from a state with the odd-frequency spin-triplet pairing instability. We speculate that this could shed light on a rather mysterious insulating state observed in strongly disordered superconducting films in a broad region of the magnetic fields.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Essential role of magnetic frustration in the phase diagrams of doped cobaltites

Doped perovskite cobaltites (e.g., La 1–x Sr x CoO 3 ) have been extensively studied for their spin-state physics, electronic inhomogeneity, and insulator-metal transitions. Ferromagnetically interacting spin-state polarons emerge at low x in the phase diagram of these compounds, eventually yielding long-range ferromagnetism. The onset of long-range ferromagnetism (x≈0.18) is substantially delayed relative to polaron percolation (x≈0.05), however, generating a troubling inconsistency. Here, in this study, Monte Carlo simulations of a disordered classical spin model are used to establish that previously ignored magnetic frustration is responsible for this effect, enabling faithful reproduction of the magnetic phase diagram.

36 MATERIALS SCIENCE↗
NASA NTRS1987

A study of reduced chromium content in a nickel-base superalloy via element substitution and rapid solidification processing

A study of reduced chromium content in a nickel base superalloy via element substitution and rapid solidification processing was performed. The two elements used as partial substitutes for chromium were Si and Zr. The microstructure of conventionally solidified materials was characterized using microscopy techniques. These alloys were rapidly solidified using the chill block melt spinning technique and the rapidly solidified microstructures were characterized using electron microscopy. The spinning technique and the rapidly solidified microstructures was assessed following heat treatments at 1033 and 1272 K. Rapidly solidified material of three alloys was reduced to particulate form and consolidated using hot isostatic pressing (HIP). The consolidated materials were also characterized using microscopy techniques. In order to evaluate the relative strengths of the consolidated alloys, compression tests were performed at room temperature and 1033 K on samples of as-HIPed and HIPed plus solution treated material. Yield strength, porosity, and oxidation resistance characteristics are given and compared.

Powers, William O.↗
DOE OSTI2023

Importance of Dispersion in the Molecular Geometries of Mn(III) Spin-Crossover Complexes

The computational investigation of the molecular geometries of a pair of manganese(III) spin-crossover complexes is reported. For the geometry of the quintet high-spin state, density functionals significantly overestimate Mn–Namine bond distances, although the geometry for the triplet intermediate-spin state is well described. Here, comparisons with several wave function-based methods demonstrate that this error is due to the limited ability of commonly used density functionals to recover dispersion beyond a certain extent. Among the methods employed for geometry optimization, restricted open-shell Møller–Plesset perturbation theory (MP2) appropriately describes the high-spin geometry but results in a slightly shorter Mn–O distance in both spin states. On the other hand, extended multistate complete active space second-order perturbation theory (XMS-CASPT2) provides a good description of the geometry for the intermediate-spin state but also sufficiently recovers dispersion, performing well for the high-spin state. Despite the fact that the electronic structure of both spin states is dominated by one-electron configuration, XMS-CASPT2 offers a balanced approach, leading to molecular geometries with much better agreement with experiment than MP2 and DFT. A scan along the Mn–N amine bond demonstrates that for these complexes coupled cluster methods (i.e., DLPNO-CCSD(T)) also yield bond distances in agreement with experiment while multiconfiguration pair density functional theory (MC-PDFT) is unable to recover dispersion well enough, analogous to single-reference DFT.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗