arXiv subjects

Daniel A. Rehn

Publications and source records attributed to Daniel A. Rehn.

12 recordsLinked to original sources

arXiv2026

Field-induced magnetic phase transition driven by a ground state level-crossing in CsErSe$_2$

We report a comprehensive study of the low-temperature magnetic properties of the insulating rare-earth triangular magnet CsErSe$_2$. We uncover a field-induced level crossing at the crystal electric field (CEF) ground state, which gives rise to a first order phase transition as well as to distinctive magnetic properties. This crossing is identified by the accurate determination of the single-ion Hamiltonian, the reliability of which is substantially enhanced by field-dependent optical spectroscopy that directly tracks the Zeeman splittings of Kramers doublets. We also observe spontaneous antiferromagnetic ordering in CsErSe$_2$ below $T_N \approx 110$ mK, and resolve the corresponding magnetic structure using elastic neutron scattering. We discuss how the rich magnetic behavior of CsErSe$_2$ arises from the interplay of non-trivial field-dependent single-ion physics and spontaneous ordering, and highlight the implications of these results for understanding magnetic phenomena across a wide range of insulating rare-earth magnets.

cond-mat.str-el↗

arXiv2026

Defect assignment of the clock site in $^{229}\text{Th:CaF}_2$

The performance of solid-state $^{229}\text{Th}$ nuclear clocks depends sensitively on the microscopic environment of the thorium nucleus in the host crystal. Here we reassess the dominant quadrupole-split thorium site in $^{229}\text{Th:CaF}_2$, which has been assigned to a thorium dimer in recent spectroscopic work. Thermodynamic estimates, density functional theory calculations, and electric-field-gradient comparisons instead favor an isolated $\text{Th}^{4+}$ substitution on a $\text{Ca}^{2+}$ site charge-compensated by two nearby fluorine interstitials in a relaxed $90^\circ$ motif. The same calculation identifies a higher-energy mixed-shell interstitial motif as a plausible minor site. The clock-active quadrupole-split site is therefore controlled by local fluoride compensation rather than unavoidable thorium aggregation. This defect assignment also has implications for achievable linewidths and provides a microscopic basis for reducing broadening in solid-state nuclear clocks.

physics.atom-ph↗

arXiv2026

Ab initio calculations of $^{229}$Th band-to-band internal conversion rate in $^{229}$ThO$_2$

We present an ab initio calculation of the band-to-band internal-conversion rate of the $\hbarω_{\rm nuc} \approx 8.35$ eV isomeric transition in $^{229}$ThO$_2$. Because the nuclear transition energy exceeds the electronic band gap of ThO$_2$, the isomer can decay nonradiatively by resonantly promoting a valence electron into the conduction band. We formulate this process as a Brillouin-zone sum over vertical interband transitions weighted by local Th-centered hyperfine matrix elements, which are evaluated directly from all-electron full-potential linearized augmented-plane-wave Bloch spinors. A finite nuclear magnetization model is included to regularize the short-range hyperfine interaction and to account for the Bohr-Weisskopf effect. After applying scissor shifts to span the experimentally reported ThO$_2$ band gaps, we find calculated internal-conversion lifetimes in the range of $1-16~μ{\rm s}$. The lifetime increases strongly as the band gap approaches $ω_{\rm nuc}$ because the resonant interband phase space at the nuclear transition energy is reduced. For the larger reported ThO$_2$ gaps, the calculated lifetime is comparable to the measured conversion-electron Mössbauer lifetime [Nature 648, 300 (2025)]. Our analysis implies that choosing solid-state hosts with band-gap values slightly lower than $ω_{\rm nuc}$ can optimize solid-state nuclear clock performance with internal-conversion electron readout.

nucl-th↗

arXiv2025

$^{229}$Th Nuclear Spectroscopy in an Opaque Material: Laser-Based Conversion Electron Mössbauer Spectroscopy of $^{229}$ThO$_2$

Here, we report the first demonstration of laser-induced conversion electron Mössbauer spectroscopy of the $^{229}$Th nuclear isomeric state, which provides the ability to probe the nuclear transition in a material that is opaque to light resonant with the nuclear transition. Specifically, we excite the nuclear transition in a thin ThO$_2$ sample whose band gap ($\sim$ 6 eV) is considerably smaller than the nuclear isomeric state energy (8.4 eV). As a result, the excited nucleus can quickly decay by internal conversion, resulting in the ejection of electrons from the surface. By collecting these conversion electrons, nuclear spectroscopy can be recorded. Unlike fluorescence spectroscopy, this technique is compatible with materials whose work function is less than the nuclear transition energy, opening a wider class of systems to study. Further, because ThO$_2$ can be made from spinless isotopes and the internal conversion decay process reduces the isomeric state lifetime to only $\sim$10 $μ$s, allowing $\sim$10$^8$ relative reduction in clock interrogation time, a conversion-electron-based nuclear clock could lead to a $\sim$10$^4$ reduction in clock instability.

physics.atom-ph↗

arXiv2025

Explaining the extra crystal field mode in ACeX2

A growing list of Ce-based magnets have shown an extra and heretofore unexplained crystal electric field (CEF) mode at high energies. We describe a process whereby an optical phonon can produce a split CEF mode well above the phonon energy. We use density functional theory and point-charge model calculations to estimate the phonon distortions and coupling to model this effect in KCeO$_2$, showing that it accounts for the extra CEF mode observed. This mechanism is generic, and may explain the extra modes observed on a variety of Ce$^{3+}$ compounds.

cond-mat.str-el↗

arXiv2025

Theoretical study of high harmonic generation in monolayer NbSe$_2$

High harmonic generation (HHG) is a powerful probe of electron dynamics on attosecond to femtosecond timescales and has been successfully used to detect electronic and structural changes in solid-state quantum materials, including transition metal dichalcogenides (TMDs). Among TMDs, bulk NbSe2 exhibits charge density wave (CDW) order below 33 K and becomes superconducting below 7.3 K. Monolayer NbSe2 is therefore interesting as a material whose different structural and electronic properties could be probed via HHG. Here, we predict the HHG response of the pristine 2H and CDW phases of monolayer NbSe2 using real-time time-dependent density functional theory under the application of a simulated laser pulse excitation. We find that due to the lack of inversion symmetry in both monolayer phases, it is possible to excite even harmonics and that the even harmonics appear as the transverse components of the current response under excitations polarized along the zigzag direction of the monolayer, while odd harmonics arise from the longitudinal current response in all excitation directions. This suggests that the even and odd harmonic response can be controlled via the polarization of the probing field, opening an avenue for potentially useful applications in opto-electronic devices.

cond-mat.mtrl-sci↗

arXiv2023

Relativistic materials from an alternative viewpoint

Electrons in materials containing heavy elements are fundamentally relativistic and should in principle be described using the Dirac equation. However, the current standard for treatment of electrons in such materials involves density functional theory methods originally formulated from the Schrödinger equation. While some extensions of the Schrödinger-based formulation have been explored, such as the scalar relativistic approximation with or without spin-orbit coupling, these solutions do not provide a way to fully account for all relativistic effects of electrons, and the language used to describe such solutions are still based in the language of the Schrödinger equation. In this article, we provide a different method for translating between the Dirac and Schrödinger viewpoints in the context of a Coulomb potential. By retaining the Dirac four-vector notation and terminology in taking the non-relativistic limit, we see a much deeper connection between the Dirac and Schrödinger equation solutions that allow us to more directly compare the effects of relativity in the angular and radial functions. Through this viewpoint, we introduce the concepts of densitals and Dirac spherical harmonics that allow us to translate more easily between the Dirac and Schrödinger solutions. These concepts allow us to establish a useful language for discussing relativistic effects in materials containing elements throughout the full periodic table and thereby enable a more fundamental understanding of the effects of relativity on electronic structure.

cond-mat.mtrl-sci↗

arXiv2021

OpenSesame tutorial

OpenSesame is a program for generating tabular equations of state (EOS), with capabilities for multiphase EOS construction. In this tutorial, we provide an overview of how to run OpenSesame to construct a multiphase EOS. We discuss some general features of OpenSesame, followed by a description of sample input files required for multiphase EOS construction. We also discuss how to extract data from EOS tables in order to compare to experimental data, with an example using the OpenSesame GUI. Lastly, we provide a description of how to generate ASCII-formatted EOS tables most often used by hydro code users.

cond-mat.mtrl-sci↗

arXiv2021

Effect of Ionic Disorder on the Principal Shock Hugoniot

The effect of ionic disorder on the principal Hugoniot is investigated using Multiple Scattering Theory to very high pressure (Gbar). Calculations using molecular dynamics to simulate ionic disorder, are compared to those with a fixed crystal lattice, for both carbon and aluminum. For the range of conditions considered here, we find that ionic disorder is most important at the onset of shell ionization and that at higher pressures, the subtle effect of the ionic environment is overwhelmed by the larger number of ionized electrons with higher thermal energies.

physics.plasm-ph↗

arXiv2021

Multiphase tin equation of state using density functional theory

We perform density functional theory (DFT) calculations of five solid phases and the liquid phase of tin. The calculations include cold curves of the five solid phases, phonon calculations in the quasi-harmonic approximation over a range of volumes for each solid phase, and DFT-based molecular dynamics (DFT-MD) calculations of the liquid phase. Using the DFT results, we construct a tabular multiphase SESAME equation of state for tin, referred to as SESAME 2162. Comparisons to experimental data are made and show a high level of agreement in isobaric data, isothermal data, shock data, and phase boundary measurements, including measurements of the melt curve. The 2162 EOS will be useful for hydrodynamics simulations and has been designed with an eye toward hydrodynamics simulations that incorporate materials strength models and allow for modeling of the kinetics of phase transitions.

cond-mat.mtrl-sci↗

arXiv2019

Reversible Electrochemical Phase Change in Monolayer to Bulk MoTe2 by Ionic Liquid Gating

Transition metal dichalcogenides (TMDs) exist in various crystal structures with semiconducting, semi-metallic, and metallic properties. The dynamic control of these phases is of immediate interest for next generation electronics such as phase change memories. Of the binary Mo and W-based TMDs, MoTe2 is attractive for electronic applications because it has the lowest energy difference (40 meV) between the semiconducting (2H) and semi-metallic (1T') phases, allowing for MoTe2 phase change by electrostatic doping. Here we report phase change between the 2H and 1T' polymorphs of MoTe2 in thicknesses ranging from the monolayer case to effective bulk (73nm) using an ionic liquid electrolyte at room temperature and in air. We find consistent evidence of a partially reversible 2H-1T' transition using in-situ Raman spectroscopy where the phase change occurs in the top-most layers of the MoTe2 flake. We find a thickness-dependent transition voltage where higher voltages are necessary to drive the phase change for thicker flakes. We also show evidence of electrochemical activity during the gating process by observation of Te metal deposition. This finding suggests the formation of Te vacancies which have been reported to lower the energy difference between the 2H and 1T' phase, potentially aiding the phase change process. Our discovery that the phase change can be achieved on the surface layer of bulk materials reveals that this electrochemical mechanism does not require isolation of a single layer and the effect may be more broadly applicable than previously thought.

cond-mat.mtrl-sci↗

arXiv2014

Analytic Framework for Students' Use of Mathematics in Upper-Division Physics

Many students in upper-division physics courses struggle with the mathematically sophisticated tools and techniques that are required for advanced physics content. We have developed an analytical framework to assist instructors and researchers in characterizing students' difficulties with specific mathematical tools when solving the long and complex problems that are characteristic of upper-division. In this paper, we present this framework, including its motivation and development. We also describe an application of the framework to investigations of student difficulties with direct integration in electricity and magnetism (i.e., Coulomb's Law) and approximation methods in classical mechanics (i.e., Taylor series). These investigations provide examples of the types of difficulties encountered by advanced physics students, as well as the utility of the framework for both researchers and instructors.

physics.ed-ph↗