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At least 307 records · Page 17

Many-body perturbation theory with hybrid density functional theory starting points accelerated by adaptively compressed exchange

We report on the use of the adaptively compressed exchange (ACE) operator to accelerate many-body perturbation theory (MBPT) calculations, including G 0 W 0 and the Bethe–Salpeter equation (BSE), for hybrid density functional theory starting points. We show that by approximating the exact exchange operator with the low-rank ACE operator, substantial computational savings can be achieved with systematically controllable errors in the quasiparticle energies computed with full-frequency G 0 W 0 and the optical absorption spectra and vertical excitation energies computed by solving the BSE within density matrix perturbation theory. Our implementation makes use of the ACE-accelerated electronic Hamiltonian to carry out both G 0 W 0 and BSE without explicitly computing empty states. We show the robustness of the approach and present the computational gains obtained on both the central processing unit and graphics processing unit nodes. In conclusion, our work will facilitate the exploration and evaluation of fine-tuned hybrid starting points aimed at enhancing the accuracy of MBPT calculations without involving computationally demanding self-consistency in Hedin’s equations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Studying Open Quantum Systems Relevant to Chemistry on a Trapped-Ion Quantum Simulator (Final Technical Report)

This project advances the trapped-ion quantum simulator as a versatile platform for studying open quantum system phenomena. We aim to contribute to the emerging quantum simulation toolkits and enable simulation of nanoscale energy processes. Trapped-ion platforms offer unique capabilities: their vibrational motion can be precisely manipulated, measured, and coherently coupled to auxiliary qubits. The vibrational mode can function both as a highly sensitive quantum sensor and a programmable environment bath. Using this platform, we achieved three major outcomes. First, we demonstrated using the vibrational mode as an ultrasensitive probe for testing fundamental physics, including possible nonlinear quantum mechanics effects. Second, we established that these modes can act as controllable baths in which tunable noise and loss can enhance or modify energy-transfer dynamics, providing the experimental preparation toward studying mechanisms relevant to chemical reactions and light-harvesting systems. Third, by introducing controllable nonlinear gain and loss, we showed theoretically how simulations using trapped ions can model vibrationally-assisted energy transport in a non‐Hermitian quantum system comprising a chromophore dimer weakly coupled to a vibrational mode. Exploring the non‐Hermitian dynamics of the whole system including vibrations, we found that energy transfer accompanied by absorption of phonons from a vibrational mode can be significantly enhanced near an exceptional point. This theoretical work on simulation of energy transfer processes in driven non‐Hermitian quantum systems revealed an interesting novel path to study open quantum systems dynamics under conditions of gain and loss. We then further explored the benefits of controllable gain and loss with an experimental realization of quantum analogs of nonlinear oscillators, namely, the van der Pol oscillator. Here we observed mutual synchronization mediated by collective dissipation between two oscillators. In parallel, we explored related quantum networking protocols using the same trapped-ion platform, developing fast, high-fidelity schemes for distributing entanglement. Together, these achievements show that trapped-ion vibrational modes provide a highly programmable and high-fidelity platform for investigating complex dissipative quantum behavior, while enabling new approaches to remote quantum sensing, energy science, and nonlinear quantum dynamics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Spectral phase singularity and topological behavior in perfect absorption

Perfect absorbers, which can achieve total absorption of all incoming energy, have been extensively studied in the last decades for various important technologies in general wave systems. Here, we show that perfect absorption (PA) is generically associated with topological spectral phase singularity (SPS), carrying conserved and tunable quantized topological invariants in spectral space. The order of topological invariant $\tilde{v}$ depends on the number of degenerate outgoing channels. Two commonly studied absorbers, mirror-backed and all-dielectric structures, are reexamined from a topological perspective to reveal the generation, evolution, and annihilation of SPSs with $\tilde{v}$ = ±1 or even high orders (i.e., $\tilde{v}$ = ±2,±4). A strategy based on charge conservation of SPSs to design dual-band perfect absorbers has been established. Our findings establish the topological origin of the robust existence of PA. More broadly, in this letter, we highlight topology as the fundamental property of conventional scattering behaviors. Finally, this insight could lead to opportunities in applications such as biosensing, topological metasurfaces, and micro/nano thermal radiation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Probing Distinctive Redox Mechanism in Ni-Rich Cathode Via Real-Time Quick X-Ray Absorption Spectroscopy

X-ray radiation damage on the measuring system has been a critical issue regularly for a long-time exposure to X-ray beam during the in operando characterizations, which is particularly severe when the applied X-ray energy is near the absorption edges (M, L, K, etc.) of the interest element. Here, to minimize the negative effects raised by beam radiation, we employ quick X-ray absorption spectroscopy (QXAS) to study the electrochemical reaction mechanism of a Ni-rich layered structure cathode for lithium-ion batteries. With the advanced QXAS technique, the electronic structure and local coordination environment of the transition metals (TMs) are monitored in-operando with limited radiation damage. Compared to the conventional step-mode X-ray absorption spectroscopy, the QXAS can provide more reliable oxidation state change and more detailed local structure evolutions surrounding TMs (Ni and Co) in Ni-rich layered oxides. By leveraging these advantages of QXAS, we demonstrated that the Ni dominates the electrochemical process with the Co being almost electrochemically inactive. Reversible Ni ions movement between TMs sites and Li sites is also revealed by the time-resolved QXAS technique.

25 ENERGY STORAGE↗

Multi-crystal native-SAD phasing at 5 keV with a helium environment

De novo structure determination from single-wavelength anomalous diffraction using native sulfur or phospho­rus in biomolecules (native-SAD) is an appealing method to mitigate the labor-intensive production of heavy-atom derivatives and seleno­methio­nyl substitutions. The native-SAD method is particularly attractive for membrane proteins, which are difficult to produce and often recalcitrant to grow into decent-sized crystals. Native-SAD uses lower-energy X-rays to enhance anomalous signals from sulfur or phospho­rus. However, at lower energies, the scattering and absorption of air contribute to the background noise, reduce the signals and are thus adverse to native-SAD phasing. We have previously demonstrated native-SAD phasing at an energy of 5 keV in air at the NSLS-II FMX beamline. Here, the use of a helium path developed to reduce both the noise from background scattering and the air absorption of the diffracted X-ray beam are described. The helium path was used for collection of anomalous diffraction data at 5 keV for two proteins: thaumatin and the membrane protein TehA. Although anomalous signals from each individual crystal are very weak, robust anomalous signals are obtained from data assembled from micrometre-sized crystals. The thaumatin structure was determined from 15 microcrystals and the TehA structure from 18 microcrystals. These results demonstrate the usefulness of a helium environment in support of native-SAD phasing at 5 keV.

59 BASIC BIOLOGICAL SCIENCES↗

Dicyanobenzothiadiazole (DCBT) Organic Dye as a Visible Light Absorbing Strong Photoinduced Oxidant with a 16 Microsecond Long–Lived Excited State

Strong photoinduced oxidants are important to organic synthesis and solar energy conversion, to chemical fuels or electric. For these applications, visible light absorption is important to solar energy conversion and long–lived excited states are needed to drive catalysis. With respect to these desirable qualities, a series of five 5,6–dicyano[2,1,3]benzothiadiazole (DCBT) dyes are examined as organic chromophores that can serve as strong photooxidants in catalytic systems. The series utilizes a DCBT core with aryl groups on the periphery with varying electron donation strengths relative to the core. The dyes are studied via both steady–state and transient absorption and emission studies. Additionally, computational analysis, voltammetry, crystallography, and absorption spectroelectrochemistry are also used to better understand the behavior of these dyes. Ultimately, a strong photooxidant is arrived at with an exceptionally long excited state lifetime for an organic chromophore of 16 µs. Finally, the long–lived excited state photosensitizer is well–suited for use in catalysis, and visible light driven photosensitized water oxidation is demonstrated using a water–soluble photosensitizer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Calibration of a versatile multi-energy soft x-ray diagnostic for WEST long pulse plasmas

A compact multi-energy soft x-ray diagnostic is being installed on the W Environment in Steady-state Tokamak (WEST), which was designed and built to test ITER-like tungsten plasma facing components in a long pulse (~1000 s) scenario. The diagnostic consists of a pinhole camera fielded with the PILATUS3 photon-counting Si-based detector (≲100 kpixel). The detector has sensitivity in the range 1.6–30 keV and enables energy discrimination, providing a higher energy resolution than conventional systems with metal foils and diodes with adequate space and time resolution (≲1 cm and 2 ms). The lower-absorption cut-off energy is set independently on each one of the ~100 kpixels, providing a unique opportunity to measure simultaneously the plasma emissivity in multiple energy ranges and deduce a variety of plasma parameters (e.g., T e , n Z , and ΔZ eff ). The energy dependence of each pixel is calibrated here over the range 3–22 keV. The detector is exposed to a variety of monochromatic sources—fluorescence emission from metallic targets—and for each pixel, the lower energy threshold is scanned to calibrate the energy dependence. The data are fit to a responsivity curve (“S-curve”) that determines the mapping between the possible detector settings and the energy response for each pixel. Here, the calibration is performed for three energy ranges: low (2.3–6 keV), medium (4.5–13.5 keV), and high (5.4–21 keV). We determine the achievable energy resolutions for the low, medium, and high energy ranges as 330 eV, 640 eV, and 950 eV, respectively. The main limitation for the energy resolution is found to be the finite width of the S-curve.

47 OTHER INSTRUMENTATION↗

Recyclable Design for Retaining High Solar Absorptivity of the Media in CSP

Efficient thermal energy storage is pivotal to lowering the levelized cost of electricity (LCOE) for Concentrating Solar Power (CSP) plants. In solid-particle systems, however, prolonged high-temperature service degrades particle solar absorptivity, eroding overall efficiency. This project demonstrates a hydrogen-assisted recovery process that reliably restores absorptivity to >90 %, offering a practical route to sustain long-term CSP performance. Bench-scale investigations mapped the reduction kinetics of optically faded particles across hydrogen concentrations, temperatures, and residence times. Coupling mass-spectrometric monitoring with machine-learning optimization minimized energy demand while maximizing absorptivity gain. The resulting process window—moderate hydrogen partial pressures, 15–30 min dwell times, and temperatures well below initial calcination levels—cuts energy consumption well below that of incumbent re-blackening methods. A prototype recovery reactor processed multiple 2 kg batches with repeatable outcomes, confirming scalability and operational robustness. Integrated techno-economic analysis indicates material and operating cost reductions exceeding 15 % relative to conventional particle replacement or chemical re-coating, translating directly into lower LCOE for next-generation CSP facilities. By uniting fundamental reaction-kinetics insight with pragmatic engineering, this work advances the solid-particle pathway, delivering a cost-effective, field-deployable solution to one of CSP’s key durability challenges and strengthening the commercial outlook for high-temperature renewable power.

14 SOLAR ENERGY↗

Evolution from Tunneling to Hopping Mediated Triplet Energy Transfer from Quantum Dots to Molecules

Efficient energy transfer is particularly important for multiexcitonic processes like singlet fission and photon upconversion. Observation of the transition from short-range tunneling to long-range hopping during triplet exciton transfer from CdSe nanocrystals to anthracene is reported here. This is firmly supported by steady- state photon upconversion measurements, a direct proxy for the efficiency of triplet energy transfer (TET), as well as transient absorption measurements. When phenylene bridges are initially inserted between a CdSe nanocrystal donor and anthracene acceptor, the rate of TET decreases exponentially, commensurate with a decrease in the photon upconversion quantum efficiency from 11.6% to 4.51% to 0.284%, as expected from a tunneling mechanism. However, as the rigid bridge is increased in length to 4 and 5 phenylene units, photon upconversion quantum efficiencies increase again to 0.468% and 0.413%, 1.5–1.6 fold higher than that with 3 phenylene units (using the convention where the maximum upconversion quantum efficiency is 100%). This suggests a transition from exciton tunneling to hopping, resulting in relatively efficient and distance-independent TET beyond the traditional 1 nm Dexter distance. Transient absorption spectroscopy is used to confirm triplet energy transfer from CdSe to transmitter, and the formation of a bridge triplet state as an intermediate for the hopping mechanism. Lastly, this first observation of the tunneling-to-hopping transition for long-range triplet energy transfer between nanocrystal light absorbers and molecular acceptors suggests that these hybrid materials should further be explored in the context of artificial photosynthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tritium adsorption and absorption on (100) and (001) surfaces of pure and tin defective zirconium

Zirconium alloys such as zircaloy-4 are used as tritium (T) getter materials in tritium-producing burnable absorber rods (TPBARs) due to their ability to capture T, thereby forming metal hydrides. Developing an understanding of T adsorption onto zircaloy prior to diffusion into the subsurface is relevant for rational tritium getter and TPBAR design, to improve material properties for nuclear applications. Herein, density functional theory calculations revealed the preferred binding sites for T adsorption on Zr(001) and Zr(100). The energy barriers of T transfer, along the surface and from the surface to the subsurface were computed. The adsorption properties of Zr(001) were found to be superior to those of Zr(100). Surface tin impurities were found to strongly repel T. The presence of subsurface and surface tin resulted in higher absorption energy barriers for both the forward and reverse processes. Based on the calculated energy barriers, a surface to surface T diffusion coefficient of 9.53 × 10 -10 m 2 s -1 is expected for pristine Zr(001). Finally, a surface to subsurface T diffusion coefficient on the order of 10 -13 m 2 s -1 is predicted in pristine Zr, decreasing to 10 -19 m 2 s -1 for the transfer with a subsurface tin impurity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The influence of hydrothermal synthesis temperature on the electronic structure and luminescence property of Cr-doped ZnGa 2 O 4 nanoparticles

Cr-doped ZnGa 2 O 4 (CZGO) is a near-infrared-emitting material with long-lasting persistent luminescence. This unique property makes it a great candidate in optical imaging and sensing for various biomedical applications. Nanosized CZGO can be synthesized via a hydrothermal approach, but the reaction temperatures reported in existing literature vary from 120°C to 220°C, approaching the highest temperature allowed for a standard autoclave vessel. The reason for choosing a particular hydrothermal synthesis temperature has rarely been discussed, and it is unclear whether the resulting CZGO possess the same optical properties. This work compares CZGO nanoparticles synthesized at temperatures from the lowest reported 120°C and to as high as 220°C. We find that although all the synthesized CZGO are light emitting, they exhibit different luminescence intensities and respond differently to the change of excitation energy. X-ray absorption fine structure (XAFS) analysis is employed to investigate the local chemical environment around Zn, Ga and Cr, respectively. We found synthesis temperature strongly influences the Ga species formed in these particles. The energy transfer mechanism is further elucidated using X-ray excited optical luminescence (XEOL) in combination with element-specific XAFS. Two energy transfer paths are identified, which explains the different excitation energy dependencies of the observed photoluminescence.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Correlating Surface Processing of Nb Superconducting RF Cavities with the Evolution of Surface Electronic States

Superconducting-radio frequency (RF) cavities provide an efficient way to accelerate particle beams with extremely high acceleration gradients while generating very small power dissipation. The few nanometers of the surface play a critical role in defining the RF performance of superconducting Nb based cavities. Over the past two decades, several pioneering surface treatment and processing methods have emerged, enabling remarkable improvements in superconducting cavity performance by simultaneously achieving high quality factors with increasing maximum acceleration gradients. These processing approaches include chemical polishing, distinct multi-step thermal treatments under ultra-high vacuum (UHV) conditions over low to high temperature regimes, as well as high-temperature treatments under controlled nitrogen atmospheres. Beyond their macroscopic impact on RF performance, these methods produce distinct surface oxide configurations characterized by different valence states, oxide thicknesses, chemical uniformity, and oxygen concentration profiles extending into the near-surface bulk of niobium. In this work, we are trying to understand how the surface-processing methods and the resulting oxide/oxygen profiles affect the electronic structure of surface and the mechanism of superconductivity. Using a combination of X-ray photoemission and X-ray absorption spectroscopies, we investigate how the valence-band structure and the electronic density of states (DoS) near the Fermi level evolve under different surface treatments. By employing tunable photon energies across multiple elemental absorption edges, we use resonant photoemission to disentangle and identify the elemental contributions to specific valence-band features. Our observations show that different surface-processing methods lead to distinct temperature evolutions of the DoS and valence-band states near the Fermi level. Our results suggest variations in different Nb-O orbital hybridizations in distinct processes and point towards the possibility of different underlying mechanisms of superconductivity governed by surface chemistry and oxide configuration. We also correlate these distinct superconducting mechanisms with RF cavity performance, specifically focusing on measured surface resistance, the nature of the Q-slope, and quench fields observed in superconducting RF measurements. These results will enable us to identify the potential limiting factors and relevant controllable parameters that can be further optimized to improve the performance of superconducting RF cavities.

Tripathi, Malvika [Fermilab] (ORCID:00000001989251↗

Natural Charge-Transfer Analysis: Eliminating Spurious Charge-Transfer States in Time-Dependent Density Functional Theory via Diabatization, with Application to Projection-Based Embedding

For many types of vertical excitation energies, linear-response time-dependent density functional theory (LR-TDDFT) offers a useful degree of accuracy combined with unrivaled computational efficiency, although charge-transfer excitation energies are often systematically and dramatically underestimated, especially for large systems and those that contain explicit solvent. As a result, low energy electronic spectra of solution-phase chromophores often contain tens to hundreds of spurious charge-transfer states, making LR-TDDFT needlessly expensive in bulk solution. More nefariously, intensity borrowing by the low-energy charge-transfer states can affect intensities of the valence excitations even if those excitation energies are accurate. At higher excitation energies, it is difficult to distinguish spurious CT states from genuine charge-transfer-to-solvent (CTTS) excitations. In this work, we introduce an automated diabatization scheme that enables fast and effective screening of the CTTS acceptor space in bulk solution. Our procedure introduces the concept of “natural charge-transfer orbitals”, which provide a means to isolate characteristic pairs of orbitals that are most likely to participate in a CTTS excitation. The projection of these orbitals onto solvent-centered virtual orbitals provides a criterion for defining the most important solvent molecules in a given excitation. We apply this method to analyze an ab initio molecular dynamics (MD) trajectory of I-(aq) and report the lowest-energy CTTS band in the absorption spectrum. Our results are in excellent agreement with experimental measurements for bulk I-(aq), and only one-third of the water molecules in the I-(H2O)96 simulation cell need to be described with LR-TDDFT in order to obtain excitation energies that are converged to < 0.1 eV. The tools introduced herein will improve the accuracy, efficiency, and usability of LR-TDDFT in solution-phase environments

Carter-Fenk, Kevin D.↗

Enhancement of vibrationally assisted energy transfer by proximity to exceptional points, probed by fluorescence-detected vibrational spectroscopy

Emulation of energy transfer processes in natural systems on quantum platforms can further our understanding of complex dynamics in nature. One notable example is the demonstration of vibrationally assisted energy transfer (VAET) on a trapped-ion quantum emulator, which offers insights for the energetics of light harvesting. In this work, we expand the study of VAET simulation with trapped ions to a non-Hermitian quantum system comprising a 𝒫⁢𝑇-symmetric chromophore dimer weakly coupled to a vibrational mode. We first characterize exceptional points (EPs) and non-Hermitian features of the excitation energy transfer processes in the absence of the vibration, finding a degenerate pair of second-order EPs. Exploring the non-Hermitian dynamics of the whole system including vibrations, we find that energy transfer accompanied by absorption of phonons from a vibrational mode can be significantly enhanced near such a degenerate EP. Our calculations reveal a unique spectral feature accompanying the coalescing of eigenstates and eigenenergies that provides a unique approach to probe the degenerate EP by fluorescence-detected vibrational spectroscopy. Enhancement of the VAET process near the EP is found to be due to maximal favorability of phonon absorption at the degenerate EP, enabling multiple simultaneous excitations. Our work on improving VAET processes in non-Hermitian quantum systems paves the way for leveraging non-Hermiticity in quantum dynamics related to excitation energy transfer.

Non-Hermitian systems↗

Electro-physical properties of surface-barrier diodes on low-resistance n-Cd 0.96 Mn 0.04 Te 0.96 Se 0.04 crystals

The electro-physical properties of Cd 0.96 Mn 0.04 Te 0.96 Se 0.04 n-type conductivity single crystals with relatively low resistivity were studied. The determined resistivity of semiconductor single crystals Cd 0.96 Mn 0.04 Te 0.96 Se 0.04 n-type conductivity is equal to ρ≈2 Ω-cm at 293K. The activation energy of dark conductivity, measured from the temperature dependence of the resistivity of the In/Cd 0.96 Mn 0.04 Te 0.96 Se 0.04 /In structure, is equal to ΔE≈0.11eV. From optical measurements of the absorption coefficient from the energy of photons in the region of large α, the band-gap width of the single crystal was found, which is equal to E g =1.53eV. Diode structures of Ni/Cd 0.96 Mn 0.04 Te 0.96 Se 0.04 /In obtained by vacuum sputtering of Ni on the surface of a single crystal n-Cd 0.96 Mn 0.04 Te 0.96 Se 0.04 were manufactured and studied. Here, the rectification coefficient at a voltage of U=1V is equal to 10 8 . Within the framework of the Sah-Noys-Shockley carrier generation-recombination model, a quantitative match of the experimental measurements of the volt-ampere characteristics with the calculation was achieved.

(Cd,Mn)(Te,Se)↗

Solution Chemistry of Copper(II) Binding to Substituted 8-Hydroxyquinolines

8-Hydroxyquinolines (8HQs) are a family of lipophilic metal ion chelators that have been used in a range of analytical and pharmaceutical applications over the last 100 years. More recently, CQ (clioquinol; 5-chloro-7-iodo-8-hydroxyquinoline) and PBT2 (5,7-dichloro-2-[(dimethylamino)methyl]-8-hydroxyquinoline) have undergone clinical trials for the treatment of Alzheimer’s disease and Huntington’s disease. Because CQ and PBT2 appear to redistribute metals into cells, these compounds have been redefined as copper and zinc ionophores. Despite the attention surrounding the clinical trials and the clear link between 8HQs and metals, the fundamental solution chemistry of how these compounds bind divalent metals such as copper and zinc, as well as their mechanism(s) of action in mammalian systems, remains poorly understood. Here, we used a combination of X-ray absorption spectroscopy (XAS), high-energy resolution fluorescence detected (HERFD) XAS, electron paramagnetic resonance (EPR), and UV–visible absorption spectroscopies to investigate the aqueous solution chemistry of a range of 8HQ derivatives. To circumvent the known solubility issues with 8HQ compounds and their complexes with Cu(II), and to avoid the use of abiological organic solvents, we have devised a surfactant buffer system to investigate these Cu(II) complexes in aqueous solution. Our study comprises the first comprehensive investigation of the Cu(II) complexes formed with many 8HQs of interest in aqueous solution, and it provides the first structural information on some of these complexes. We find that halogen substitutions in 8HQ derivatives appear to have little effect on the Cu(II) coordination environment; 5,7-dihalogenated 8HQ conformers all have a pseudo square planar Cu(II) bound by two quinolin-8-olate anions, in agreement with previous studies. Conversely, substituents in the 2-position of the 8HQ moiety appear to cause significant distortions from the typical square-planar-like coordination of most Cu(II)-bis-8HQ complexes, such that the 8HQ moieties in the Cu(II)-bis-8HQ complex are rotated approximately 30–40° apart in a “propeller-like” arrangement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Photocarrier Dynamics in MoTe 2 Nanofilms with 2 H and Distorted 1 T Lattice Structures

Molybdenum telluride (MoTe 2 ), an emerging layered two-dimensional (2D) material, possesses excellent phase-changing properties. Previous studies revealed its reversible transition between 2H and 1T' phases with a transition energy as small as 35 meV. Since 1T'-MoTe 2 is metallic, it can serve as an electrical contact for semiconducting 2H-MoTe 2 -based optoelectronic devices. Here, the photocarrier dynamics in MoTe 2 nanofilms synthesized by a one-step method and with coexisting multiple phases are investigated by transient absorption measurements. Both the energy relaxation time and the recombination lifetime of the excitons are shorter in the 1T'-MoTe 2 compared to its 2H phase. Furthermore, these results provide information on the different photocarrier dynamical properties of these two phases, which is important for future 2D optoelectronic and phase-change electronic devices based on MoTe 2 .

36 MATERIALS SCIENCE↗

Satellites, core hole excitations, and spin-resolved electronic structure in the spectroscopy of half-metallic CrO 2

Photoelectron satellites—the structures appearing on the low kinetic or high binding-energy side of the “main” or “elastic” photopeak—betray the complex many-body interactions set in motion by the sudden creation of the core hole. In this work, we demonstrate, using the technologically important ferromagnetic half-metal CrO 2 , how such satellites can manifest themselves in other core-level spectroscopies of the material and how they can reveal important details pertinent to its electronic structure. Specifically, we identify a fluorescence satellite in the Cr 𝐿 3 resonant x-ray-emission spectra that radiates at a constant emission energy across the Cr 𝐿 3 x-ray edge with energy ≈1.3 eV above the ordinary valence fluorescence. Here, we provide evidence that this feature arises from the valence recombination of the Cr 2⁢𝑝 core hole “dressed” by the same shakeup charge-transfer process present in both the Cr x-ray photoelectron and the Cr x-ray absorption spectra with its energy uniquely measuring the exchange splitting of the Cr 3⁢𝑑 level. Further analysis of the x-ray emission data reveals three additional features that radiate at constant loss energy that are attributed to combinations of Cr 3⁢𝑑⁢(𝑡 2⁢𝑔 ) → Cr 3⁢𝑑⁢(𝑡 2⁢𝑔 ), charge-transfer O 2⁢𝑝→Cr 3⁢𝑑, and crystal-field Cr⁢ 3⁢𝑑⁡(𝑡 2⁢𝑔 )→Cr⁢ 3⁢𝑑⁡(𝑒 𝑔 ) excitations. These assignments and their energies are supported by density-functional theory calculations, the accuracy of which we demonstrate by hard x-ray valence-photoemission measurements. Atomic multiplet calculations, which include crystal-field effects, help interpret x-ray photoelectron and x-ray absorption spectra of the covalently mixed Cr ion. Resonant Cr K-𝐿 2,3 ⁢𝐿 2,3 Auger-electron emission spectra support a ligand-to-metal nature of the charge-transfer process while highlighting the charge sensitivity differences between photon-in/electron-out and photon-in/photon-out spectroscopies.

36 MATERIALS SCIENCE↗