Transition metal doping is commonly used for altering the properties of solid-state materials to suit applications in science and technology. Partially filled $d$ -shells of transition metal atoms lead to electronic states with diverse spatial and spin symmetries. Chromium(III) cations have shown great potential for designing laser materials and, more recently, for developing spin qubits in quantum applications. They also represent an intriguing class of chemical systems with strongly correlated multi-reference excited states, due to the $d^3$ electron configuration. These states are difficult to describe accurately using single-reference quantum chemical methods such as density functional theory (DFT), the most commonly used method to study the electronic structures of solid-state systems. Recently, the periodic effective Hamiltonian of crystal field (pEHCF) method has been shown to overcome some limitations arising in the calculations of excited $d$ -states. In this work, we assess the suitability of DFT and pEHCF to calculate the electronic structure and $d$ - $d$ excitations of chromium(III) dopants in wide band gap host materials. The results will aid computational development of novel transition metal-doped materials and provide a deeper understanding of the complex nature of transition metal dopants in solids.Transition metal doping is commonly used for altering the properties of solid-state materials to suit applications in science and technology. Partially filled $d$-shells of transition metal atoms lead to electronic states with diverse spatial and spin symmetries. Chromium(III) cations have shown great potential for designing laser materials and, more recently, for developing spin qubits in quantum applications. They also represent an intriguing class of chemical systems with strongly correlated multi-reference excited states, due to the $d^3$ electron configuration. These states are difficult to describe accurately using single-reference quantum chemical methods such as density functional theory (DFT), the most commonly used method to study the electronic structures of solid-state systems. Recently, the periodic effective Hamiltonian of crystal field (pEHCF) method has been shown to overcome some limitations arising in the calculations of excited $d$-states. In this work, we assess the suitability of DFT and pEHCF to calculate the electronic structure and $d$-$d$ excitations of chromium(III) dopants in wide band gap host materials. The results will aid computational development of novel transition metal-doped materials and provide a deeper understanding of the complex nature of transition metal dopants in solids.

cond-mat.mtrl-sciCross-listedarXiv:2512.07398Dec 9, 2025

How to Be a Relativistic Spacetime State Realist

Noel Swanson

According to spacetime state realism (SSR), the fundamental ontology of a quantum mechanical world consists of a state-valued field evolving in four-dimensional spacetime. One chief advantage it claims over rival wave-function realist views is its natural compatibility with relativistic quantum field theory (QFT). I argue that the original density operator formulation of SSR cannot be extended to QFTs where the local observables form type III von Neumann algebras. Instead, I propose a new formulation of SSR in terms of a presheaf of local state spaces dual to the net of local observables studied by algebraic QFT. 1. Introduction 2. Spacetime State Realism in Quantum Field Theory 2.1. Equivalence thesis 3. Entanglement and the Type III Property 3.1. No-Go Lemma 1 3.2. No-Go Lemma 2 4. State Space Axioms for Quantum Field Theory 4.1. Revised equivalence thesis 5. DiscussionAccording to spacetime state realism (SSR), the fundamental ontology of a quantum mechanical world consists of a state-valued field evolving in four-dimensional spacetime. One chief advantage it claims over rival wave-function realist views is its natural compatibility with relativistic quantum field theory (QFT). I argue that the original density operator formulation of SSR cannot be extended to QFTs where the local observables form type III von Neumann algebras. Instead, I propose a new formulation of SSR in terms of a presheaf of local state spaces dual to the net of local observables studied by algebraic QFT. 1. Introduction 2. Spacetime State Realism in Quantum Field Theory 2.1. Equivalence thesis 3. Entanglement and the Type III Property 3.1. No-Go Lemma 1 3.2. No-Go Lemma 2 4. State Space Axioms for Quantum Field Theory 4.1. Revised equivalence thesis 5. Discussion

The British Journal for the Philosophy of ScienceJul 31, 201816 citations

Robust Optical Coherence in a Chemically Tunable Eu(III) Molecular Crystal

Suma Al-Hunaishi, Senthil Kumar Kuppusamy, Yisheng Lei +8 more

Chemical substitution o!ers a powerful route to tune molecular quantum materials, but its e!ects on optical decoherence extend beyond the simple dilution of interacting emitters; here, we investigate these e!ects in the molecular crystal [Eu(III)(TMHD)3(phen)], its dilution series in the isostructural host [Y(TMHD)3(phen)], and a partially deuterated analogue. The optical inhomogeneous linewidth of the 7F0 ↔ 5D0 transition near 580.4 nm exhibits a pronounced concentration dependence, ranging from 6 to 20 GHz, while the transition frequency shifts by up to ↗25 GHz across the dilution series. In contrast, the homogeneous linewidth measured by two-pulse photon echoes remains in the 50–130 kHz regime at 1.4 K, and shows a non-monotonic dependence on Eu(III) content. Partial phenanthroline deuteration also leaves the homogeneous linewidth essentially unchanged. Spectral-di!usion and temperature-dependent photon-echo measurements identify non-magnetic fluctuations of the molecular environment as the dominant residual dephasing channel. In contrast to rigid inorganic rare-earth hosts, the molecular crystal lattice supports low-frequency lattice modes that can dynamically modulate the anisotropic Eu(III) crystal field, while the extrapolated zero-temperature linewidth is most likely limited by electric-field perturbations. These results establish Eu(III) molecular crystals as chemically tunable materials with robust optical coherence and show that chemical dilution simultaneously reshapes static disorder, lattice dynamics, and decoherence, identifying molecular-lattice rigidity and electrostatic stability as central design parame-Chemical substitution o!ers a powerful route to tune molecular quantum materials, but its e!ects on optical decoherence extend beyond the simple dilution of interacting emitters; here, we investigate these e!ects in the molecular crystal [Eu(III)(TMHD)3(phen)], its dilution series in the isostructural host [Y(TMHD)3(phen)], and a partially deuterated analogue. The optical inhomogeneous linewidth of the 7F0 ↔ 5D0 transition near 580.4 nm exhibits a pronounced concentration dependence, ranging from 6 to 20 GHz, while the transition frequency shifts by up to ↗25 GHz across the dilution series. In contrast, the homogeneous linewidth measured by two-pulse photon echoes remains in the 50–130 kHz regime at 1.4 K, and shows a non-monotonic dependence on Eu(III) content. Partial phenanthroline deuteration also leaves the homogeneous linewidth essentially unchanged. Spectral-di!usion and temperature-dependent photon-echo measurements identify non-magnetic fluctuations of the molecular environment as the dominant residual dephasing channel. In contrast to rigid inorganic rare-earth hosts, the molecular crystal lattice supports low-frequency lattice modes that can dynamically modulate the anisotropic Eu(III) crystal field, while the extrapolated zero-temperature linewidth is most likely limited by electric-field perturbations. These results establish Eu(III) molecular crystals as chemically tunable materials with robust optical coherence and show that chemical dilution simultaneously reshapes static disorder, lattice dynamics, and decoherence, identifying molecular-lattice rigidity and electrostatic stability as central design parame-

Aug 27, 20260 citations

Transition metal doping is commonly used for altering the properties of solid-state materials to suit applications in science and technology. Partially filled

d

-shells of transition metal atoms lead to electronic states with diverse spatial and spin symmetries. Chromium(III) cations have shown great potential for designing laser materials and, more recently, for developing spin qubits in quantum applications. They also represent an intriguing class of chemical systems with strongly correlated multi-reference excited states, due to the

d^3

electron configuration. These states are difficult to describe accurately using single-reference quantum chemical methods such as density functional theory (DFT), the most commonly used method to study the electronic structures of solid-state systems. Recently, the periodic effective Hamiltonian of crystal field (pEHCF) method has been shown to overcome some limitations arising in the calculations of excited

d

-states. In this work, we assess the suitability of DFT and pEHCF to calculate the electronic structure and

d

d

excitations of chromium(III) dopants in wide band gap host materials. The results will aid computational development of novel transition metal-doped materials and provide a deeper understanding of the complex nature of transition metal dopants in solids.