Welcome to the Frandsen Group!

About the Group

We are an experimental condensed matter physics group focused on investigating the structure and magnetism of fascinating--and often technologically promising--materials, such as superconductors, strongly correlated electron systems, multiferroics, magnetocalorics, molten salts for nuclear reactors, and more. We use beams of neutrons, x-rays, and muons produced at large-scale accelerator facilities to probe the atomic and magnetic correlations in these materials, together with advanced computational modeling to gain quantitative insight into the spatial arrangement of atoms and spins in a given material. Specific techniques include atomic and magnetic pair distribution function (PDF) analysis of neutron/x-ray total scattering data and muon spin relaxation/rotation (μSR). Interested and motivated undergraduate and prospective graduate students are encouraged to reach out to learn more about our research and find opportunities to participate.

Research Projects

Thermoelectrics, Magnetocalorics, and Multiferroics--Oh My!

This project focuses on the connection between the local atomic and magnetic structure and the energy-relevant properties of magnetocaloric, thermoelectric, and multiferroic materials. Magnetocaloric materials exhibit large temperature changes with the application and removal of a magnetic field, offering promising applications in solid-state refrigeration and waste heat harvesting. Thermoelectric materials experience an electrical voltage when subjected to a temperature gradient or vice versa, also providing novel routes for energy-efficient cooling and waste heat harvesting. Multiferroic materials show cross-order coupling between electric polarization and magnetic order, potentially enabling unique functionalities for energy transformation, information science, and signal processing. We are using combined atomic and magnetic pair distribution function analysis, together with muon spin spectroscopy, to establish the local atomic and magnetic structure of representative compounds for these material classes and better understand the origin of their outstanding properties. In the process, we are developing new experimental and computational methods for magnetic pair distribution function analysis, which will be widely applicable to many other materials, as well. Funding: US Department of Energy, Early Career program.

Promoting Many-Body Quantum Entanglement in Geometrically Frustrated Magnets with Disorder

Quantum information technologies rely on quantum entanglement, or the intrinsic linking of one quantum object to another. An important research objective is to gain a fundamental understanding of many-body quantum entanglement involving large numbers of quantum objects. Certain magnetic materials known as geometrically frustrated magnets provide a valuable platform for this topic of study because they may exhibit many-body-entanglement at low temperature. This project advances the search for promising quantum-entangled frustrated magnets through a systematic investigation of the role of atomic-scale disorder in promoting or hindering many-body entanglement. The results illuminate strategies for utilizing disorder to promote quantum-entangled ground states and contribute to a deeper understanding of many-body quantum entanglement in general. Funding: US National Science Foundation LEAPS Program.

Novel magnets, Magnetic Nanoparticles, Metal-Insulator Transitions, High-Entropy Materials, and More

We maintain broad interest and involvement in structural studies of numerous material systems where knowledge of the local atomic and magnetic structure can add value. We have ongoing projects on novel magnets such as altermagnets and low-dimensional magnets, magnetic nanoparticles, Mott insulator systems and materials with metal-insulator transitions, high-entropy alloys and oxides, and more. We are always open to collaborations on interesting material systems.

Selected Publications

Volume-wise destruction of the antiferromagnetic Mott insulating state through quantum tuning

Benjamin A. Frandsen (et al.)

RENiO3 (RE=rare-earth element) and V2O3 are archetypal Mott insulator systems. When tuned by chemical substitution (RENiO3) or pressure (V2O3), they exhibit a quantum phase transition (QPT) between an antiferromagnetic Mott insulating state and a paramagnetic metallic state. Because novel physics often appears near a Mott QPT, the details of this transition, such as whether it is first or second order, are important. Here, we demonstrate through muon spin relaxation/rotation (μSR) experiments that the QPT in RENiO3 and V2O3 is first order: the magnetically ordered volume fraction decreases to zero at the QPT, resulting in a broad region of intrinsic phase separation, while the ordered magnetic moment retains its full value until it is suddenly destroyed at the QPT. These findings bring to light a surprising universality of the pressure-driven Mott transition, revealing the importance of phase separation and calling for further investigation into the nature of quantum fluctuations underlying the transition.

Investigating short-range magnetic correlations in real space with the magnetic pair distribution function (mPDF)

Benjamin Frandsen (et al.)

μSR investigation of a new diluted magnetic semiconductor Li(Zn,Mn,Cu)As with Mn and Cu codoping at the same Zn sites

B A Frandsen (et al.)

We report the successful synthesis and characterization of a new type I–II–V bulk form diluted magnetic semiconductor (DMS) Li(Zn,Mn,Cu)As, in which charge and spin doping are decoupled via (Cu,Zn) and (Mn,Zn) substitution at the same Zn sites. Ferromagnetic transition temperature up to ∼33 K has been observed with a coercive field ∼40 Oe for the 12.5% doping level. μ SR measurements confirmed that the magnetic volume fraction reaches nearly 100% at 2 K, and the mechanism responsible for the ferromagnetic interaction in this system is the same as other bulk form DMSs.

Verification of Anderson Superexchange in MnO via Magnetic Pair Distribution Function Analysis and ab initio Theory

Benjamin A. Frandsen (et al.)

We present a temperature-dependent atomic and magnetic pair distribution function (PDF) analysis of neutron total scattering measurements of antiferromagnetic MnO, an archetypal strongly correlated transition-metal oxide. The known antiferromagnetic ground-state structure fits the low-temperature data closely with refined parameters that agree with conventional techniques, confirming the reliability of the newly developed magnetic PDF method. The measurements performed in the paramagnetic phase reveal significant short-range magnetic correlations on a

\sim 1 nm

length scale that differ substantially from the low-temperature long-range spin arrangement. Ab initio calculations using a self-interaction-corrected local spin density approximation of density functional theory predict magnetic interactions dominated by Anderson superexchange and reproduce the measured short-range magnetic correlations to a high degree of accuracy. Further calculations simulating an additional contribution from a direct exchange interaction show much worse agreement with the data. The Anderson superexchange model for MnO is thus verified by experimentation and confirmed by ab initiotheory.

Antiferromagnetism and hidden order in isoelectronic doping of URu₂Si₂

B. A. Frandsen (et al.)

We present muon spin rotation
(
μ
SR
)
and susceptibility measurements on single crystals of isoelectronically doped
URu
2
−
x
T
x
Si
2
(T = Fe, Os) for doping levels up to 50%. Zero field (ZF)
μ
SR
measurements show long-lived oscillations demonstrating that an antiferromagnetic state exists down to low doping levels for both Os and Fe dopants. The measurements further show an increase in the internal field with doping for both Fe and Os. Comparison of the local moment-hybridization crossover temperature from susceptibility measurements and our magnetic transition temperature shows that changes in hybridization, rather than solely chemical pressure, are important in driving the evolution of magnetic order with doping.

The synthesis and characterization of 1 1 1 1 type diluted ferromagnetic semiconductor (La_1-xCa_x)(Zn_1-xMn_x)AsO

B A Frandsen (et al.)

We report the synthesis and characterization of a bulk form diluted magnetic semiconductor, (La1−x Ca x )(Zn1−y Mn y )AsO, with a layered crystal structure isostructural to that of the 1 1 1 1 type Fe-based high-temperature superconductor LaFeAsO and the antiferromagnetic LaMnAsO. With Ca and Mn codoping into LaZnAsO, the ferromagnetic ordering occurs below the Curie temperature ~30 K. Taking advantage of the decoupled charge and spin doping, we investigate the influence of carrier concentration on the ferromagnetic ordering state. For a fixed Mn concentration of 10%, increases from 24 K to 30 K when the Ca concentration increases from 5% to 10%. Further increase of Ca concentration reduces both the coercive field and saturation moment. Muon spin relaxation measurements confirm the ferromagnetically ordered state, and clearly demonstrate that (La1−x Ca x )(Zn1−y Mn y )AsO shares a common mechanism for the ferromagnetic exchange interaction with (Ga,Mn)As. Neutron scattering measurements show no structural transition in (La0.90Ca0.10)(Zn0.90Mn0.10)AsO below 300 K.