arXiv subjects

Michael A. Susner

Publications and source records attributed to Michael A. Susner.

At least 19 recordsLinked to original sources

arXiv2026

Nonlinear Photocurrent Spectroscopy and Polarization-Tunable Shift Current in the Layered Semiconductor $\mathrm{CuScP_2S_6}$

The class of layered metal thiophosphates and selenophosphates are emerging as promising candidates for non-linear photonic and optoelectronic applications. Here we report one-photon absorption (1PA) and two-photon absorption (2PA) induced photocurrents in $CuScP_2S_6$, establishing it as an optoelectronically-active non-centrosymmetric semiconductor. Spectrally-resolved 1PA and 2PA photoresponsivity paired with photoluminescence and differential reflectance measurements reveal a band gap of 2.35 eV, several higher energy interband transitions, and sub-band gap multiphoton excitonic transitions. Vertical graphite/$CuScP_2S_6$/graphite devices exhibit zero-bias photocurrent with a polarity controlled by both photon energy and optical polarization orientation within the ab-plane. This sign-dependence combined with a characteristic power-law transition from linear to square-root scaling are consistent with a shift-current origin to this bulk photovoltaic effect (BPVE). These findings establish $CuScP_2S_6$ as a multi-functional platform for polarization-sensitive non-linear optoelectronics.

cond-mat.mtrl-sci↗

arXiv2026

Scalable, Simple, and Versatile Encapsulation of 2D Materials and Devices

Air-sensitive 2D materials present a fundamental challenge for device integration. Encapsulation is often required to preserve intrinsic properties, yet conventional protection strategies often fail for thicker layers and complicate fabrication. Here, we demonstrate that electron-beam (e-beam) evaporated aluminum oxide ($\mathrm{AlO}_x$) serves as both an effective encapsulation layer and a platform for direct device fabrication. Unlike transfer-based approaches, this scalable method is compatible with thicker flakes and full device or wafer coverage. It requires no stacking procedures and enables contacts without post-encapsulation etching. Using rare-earth tritellurides ($\mathrm{RTe}_3$, R = La, Er), semimetallic $\mathrm{WTe}_2$, and superconducting $\mathrm{FeTe}_x\mathrm{Se}_{1-x}$, we show that $\mathrm{AlO}_x$ suppresses oxidation and preserves intrinsic optical and electronic properties. We establish substrate-dependent optimization of encapsulation across a range of flake thicknesses, demonstrate that ultrathin $\mathrm{AlO}_x$ preserves $\mathrm{WTe}_2$'s plasmonic response and maintains superconducting performance in $\mathrm{FeTe}_x\mathrm{Se}_{1-x}$. Thus we overcome the longstanding tradeoff between encapsulation and straightforward device fabrication in fragile quantum materials.

cond-mat.mes-hall↗

arXiv2026

A high-entropy form of $R$Mn$_6$Sn$_6$ with distinct magnetotransport regimes correlated to different magnetic structures

The kagome $R$Mn$_6$Sn$_6$ material family has attracted significant attention as high-temperature metallic magnets with a host of different magnetic orderings and anisotropy. Theoretical studies point to the rare-earth ($R$) as the determining factor for both the direction of magnetic anisotropy and the type of magnetic ordering in a given compound. This motivates studying high-entropy forms of $R$Mn$_6$Sn$_6$ to examine how the interplay of several rare-earth elements leads to different magnetic states in a single crystal. Here, we present a rare-earth mix of Tb, Dy, Ho, Er, Tm, and Lu that produces phase transitions from a paramagnet to an easy-plane ferrimagnet (FiM) below $T_{\text{C}}$ = 380 K, then to a FiM easy-axis state at $T_{\text{SR1}}$ = 207 K, to a canted FiM ground state below $T_{\text{SR2}}$ = 79 K. This behavior is consistent with previously reported high-entropy $R$Mn$_6$Sn$_6$ compounds; however, uniquely, the rare-earth mix studied here exhibits a broad transition from easy-plane to easy-axis anisotropy from 270 K to 170 K, and reveals a nonmonotonic magnetoresistance. Using neutron scattering data, we found that both observations correlate with an incommensurate modulated contribution to the spin state due to competing rare-earth interactions. This magnetoresistive behavior and the correlated spin structures underscore the potential for rare-earth engineering of magnetism.

cond-mat.mtrl-sci↗

arXiv2026

Lanthanide Ion Electronic Structure Controls Magnetic Excitations in Topological Quantum Ferrimagnets $LnMn_{6}Sn_{6}$ (Ln = Tb, Dy, Ho)

The $LnMn_{6}Sn_{6}$ family of topological magnets is a promising platform for next-generation spintronic and magnonic technologies. However, the influence of the lanthanide ion ($Ln^{3+}$) on the excited-state spin dynamics, or magnons, remains a critical knowledge gap. Here, we present the first comparative study of the magnetic dynamics in $LnMn_{6}Sn_{6}$ materials (Ln = Tb, Dy, Ho) using Brillouin light scattering. Our findings reveal a direct correlation between the lanthanide ion's intrinsic properties and the magnon behavior. We demonstrate that the magnon frequency in the absence of an applied magnetic field is primarily dictated by the strength of the lanthanide exchange coupling, as modeled by its relationship with the de Gennes factor. The response of the magnon to an applied field is influenced by material's gyromagnetic ratio and the overall anisotropy of the material, which are dictated by total angular momentum and the anisotropy of the lanthanide sublattice, respectively. These results establish that simple lanthanide substitution provides a powerful and predictable method for tuning magnon properties, enabling the rational design of materials for advanced technological applications.

cond-mat.mtrl-sci↗

arXiv2026

Non-local low energy neutral excitations in a strongly disordered triangular Mott magnet Cr$_3$Se$_2$Br$_5$

Understanding if low-energy excitations can remain itinerant in the presence of strong disorder remains a central challenge in frustrated quantum magnets, where disorder is generally expected to localize excitations through Anderson-like mechanisms. Here we report the emergence of charge-neutral itinerant excitations in a van der Waals compound Cr$_3$Se$_2$Br$_5$, a strongly disordered $S = 3/2$ Mott insulator with a frustrated triangular lattice. Structural analysis reveals substantial intrinsic disorder arising from Cr-site deficiency and Se/Br-site mixing, which appear to be fixed and cannot be readily tuned. No long-range magnetic order or conventional glassy behavior is observed. In addition to its highly insulating nature, the magnetic specific heat C_mag/T and thermal conductivity \k{appa}_xx/T both exhibit linear temperature dependencies with substantial finite intercepts. In particular, a sizeable field-independent residual term $κ/T \approx 0.03~\mathrm{W\,m^{-1}\,K^{-2}}$ is observed, providing compelling evidence of itinerant low-energy excitations that carry entropy without charge. These findings conceptually advance our understanding of quantum matter by demonstrating a rare regime where the interplay of disorder, frustration, and electronic correlations actively reshapes the nature of low-energy excitations, allowing itinerant neutral excitations to coexist with strong intrinsic disorder.

cond-mat.str-el↗

arXiv2026

Raman and Terahertz Spectroscopy of Low-Frequency Chiral Phonons in Amino Acids

Chiral phonons are mirror-symmetric vibrations that correspond to twisting and rotational motions of atoms. In chiral biomolecules, they correspond to low-energy terahertz (THz)-range vibrations of the molecular segments involving dozens of atoms whose energies are sensitive to the chirality of the molecules and local atomic geometries. Here we present spectral signatures of chiral phonons in circularly polarized low-frequency Raman and Raman optical activity (ROA) spectra from crystals of several amino acids in different enantiomeric forms. Along with complementary THz circular dichroism (TCD) measurements, our ROA data reveal two sets of bisignate peaks in valine, alanine, tyrosine and proline between 1 and 4.5 THz that are more intense than the ROA peaks in the fingerprint region. Density functional theory (DFT) calculations on L-alanine attribute these modes to twisting and shearing molecular motions. The strong agreement between the ROA and TCD data demonstrates the power of these complementary vibrational spectroscopy techniques to identify chiral phonons in biomolecules, and offers new insights into their vibrational properties and interactions with circularly polarized light.

cond-mat.mtrl-sci↗

arXiv2026

Magnetism and magnetoelastic effect in 2D van der Waals multiferroic CuCrP2S6

We report a magnetic and neutron diffraction study on the ground state magnetism and field evolution of single crystal van der Waals multiferroic CuCrP2S6. The ordered moments align along the b axis in the A-type antiferromagnetic configuration with a spin-flop transition along the same direction. Field application along a introduces a smooth transition to a fully-polarized ferromagnetic state via in-plane spin rotation. These findings resolve the ambiguity of the ground state magnetization direction in CuCrP2S6 and uncover its field responses, providing a firm basis for future magnetoelectric study. A magnetoelastic coupling effect connecting the interlayer spacing and the magnetic order was further revealed, highlighting the out-of-plane strain as an effective control knob for tuning magnetism both in this system and in related van der Waals magnets.

cond-mat.str-el↗

arXiv2026

Highly Efficient Second/Third Harmonic Generation in van der Waals Layered Material AgScP2S6 with Anisotropic Polarization and Temperature Dependence

Single-crystal X-ray diffraction and nonlinear optical measurements, especially second- and third-harmonic generation (SHG/THG) are comprehensively investigated for the van der Waals layered material AgScP2S6 with a non-centrosymmetric P31c (159) space group. Linear optical constants are extracted using spectroscopic ellipsometry and applied in fitting the harmonic generation behavior. Polarization-resolved SHG and THG measurements exhibit pronounced anisotropy, with emission patterns well-described by theoretical models derived from the khi(2) and khi(3) tensor elements. The material demonstrates exceptionally high nonlinear susceptibilities, with khi(2) ~ 10^(-8) m/V and khi(3) ~ 10^(-17) m^2/V^2 which is a few orders of magnitude greater than comparable 2D materials reported in the literature. Temperature-dependent SHG and THG measurements from 300 K to 25 K reveal exponential decay in harmonic signal intensities, attributed to reduced carrier mobility, with no evidence of structural phase transitions, consistent with results from single crystal diffraction and heat capacity measurements. Polarization-resolved SHG and THG measurements also reveal distinct orientation and ellipticity trends, highlighting the anisotropic nonlinear tensor contributions and contrasting polarization selection rules in the material. These results establish AgScP2S6 as a high-performance, thermally stable, and highly anisotropic nonlinear candidate material suitable for compact photonic applications such as ultrafast optical modulators, polarization-sensitive detectors, and wavelength-tunable light sources.

cond-mat.mtrl-sci↗

arXiv2025

Engineering the Magnetocaloric Effect in Nd$T_4$B

We present a comprehensive study of the magnetocaloric effect (MCE) in the Nd$T_4$B system where $T$ = Fe, Co, and Ni. These compounds are ferromagnetic kagome materials with tunable ordering temperatures, transition width, and magnetic moments depending on the choice of transition metal. Thus, they are good candidates for investigating the MCE. We characterize the MCE using standard metrics and construct ternary phase diagrams as functions of Fe, Co, and Ni concentrations. Using these phase diagrams, we engineer the composition NdFe$_{1.15}$Co$_{0.46}$Ni$_{2.39}$B to maximize the MCE. Interestingly, the Nd$T_4$B system shows a notable entropy change over a wide temperature range ($\sim$10 to 650 K), and particular compositions have notable MCEs spanning hundreds of Kelvin, making this a suitable system to study for technologies used in a wide range of temperatures. In a few cases, we observe a two-peak MCE. These two transitions, releasing comparable entropy, provide an interesting platform to study for applications in multi-stage cooling.

cond-mat.mtrl-sci↗

arXiv2025

Adjudicating Conduction Mechanisms in High Performance Carbon Nanotube Fibers

The performance of carbon nanotube (CNT) cables, a contender for copper-wire replacement, is tied to its metallic and semi-conducting-like conductivity responses with temperature; the origin of the semi-conducting-like response however is an underappreciated incongruity in literature. With controlled aspect-ratio and doping-degree, over 61 unique cryogenic experiments including anisotropy and Hall measurements, CNT cable performance is explored at extreme temperatures (65 mK) and magnetic fields (60 T). A semi-conducting-like conductivity response with temperature becomes temperature-independent approaching absolute-zero, uniquely demonstrating the necessity of heterogeneous fluctuation induced tunneling; complete de-doping leads to localized hopping, contrasting graphite's pure metallic-like response. High-field magneto-resistance (including +22% longitudinal magneto-resistance near room-temperature) is analyzed with hopping and classical two-band models, both similarly yielding a parameter useful for conductor development. Varying field-orientation angle uncovers two-and four-fold symmetries from Aharonov-Bohm-like corrections to curvature-induced bandgap. Tight-binding calculations using Green's Function formalism model large-scale, coherent transport in commensurate CNT bundles in magnetic field, revealing non-uniform transmission across bundle cross-sections with doping restoring uniformity; independent of doping, transport in bundle-junction-bundle systems are predominantly from CNTs adjacent to the other bundle. The final impact is predicting the ultimate conductivity of heterogeneous CNT cables using temperature and field-dependent transport, surpassing conductivity of traditional metals.

cond-mat.mtrl-sci↗

arXiv2025

Spin-lattice entanglement in $\mathbf{CoPS}_3$

Complex chalcogenides in the $M$PS$_3$ family of materials ($M$ = Mn, Fe, Co, and Ni) display remarkably different phase progressions depending upon the metal center orbital filling, character of the P-P linkage, and size of the van der Waals gap. There is also a stacking pattern and spin state difference between the lighter and heavier transition metal-containing systems that places CoPS$_3$ at the nexus of these activities. Despite these unique properties, this compound is under-explored. Here, we bring together Raman scattering spectroscopy and infrared absorption spectroscopy with X-ray techniques to identify a structural component to the 119 K magnetic ordering transition as well as a remarkable lower temperature set of magnon-phonon pairs that engage in avoided crossings along with a magnetic scattering continuum that correlates with phonon lifetime effects. These findings point to strong spin-phonon entanglement as well as opportunities to control these effects under external stimuli.

cond-mat.str-el↗

arXiv2025

Observation of giant remnant polarization in ultrathin AlScN at cryogenic temperatures

The discovery of wurtzite ferroelectrics opens new frontiers in polar materials, yet their behavior at cryogenic temperatures remains unexplored. Here, we reveal unprecedented ferroelectric properties in ultrathin (10 nm) Al$_{0.68}$Sc$_{0.32}$N (AlScN) at cryogenic temperatures where the properties are fundamentally distinct from those of conventional oxide ferroelectrics. At 12 K, we demonstrate a giant remnant polarization exceeding 250 $μ$C/cm$^2$ -- more than twice that of any known ferroelectric -- driven by an enhanced c/a ratio in the wurtzite structure. Our devices sustain remarkably high electric fields (~13 MV/cm) while maintaining reliable switching, achieving over 104 polarization reversal cycles at 12 K. Critically, this breakdown field strength approaches that of passive dielectric materials while maintaining ferroelectric functionality. The extraordinary polarization enhancement and high-field stability at cryogenic temperatures contrasts sharply with oxide ferroelectrics, establishing wurtzite ferroelectrics as a distinct class of polar materials with implications spanning fundamental physics to cryogenic non-volatile memory and quantum technologies.

cond-mat.mtrl-sci↗

arXiv2025

Anomalous Raman scattering in layered AgCrP$_2$Se$_6$: Helical modes and excitation energy-dependent intensities

Structural anisotropy in layered two-dimensional materials can lead to highly anisotropic optical absorption which, in turn, can profoundly a^ect their phonon modes. These e^ects include lattice orientation-dependent and excitation energy-dependent mode intensities that can enable new phononic and optoelectronic applications. Here, we report anomalous Raman spectra in single-crystalline AgCrP$_2$Se$_6$, a layered antiferromagnetic material. Density functional theory calculations and experimental measurements reveal several unique features in the Raman spectra of bulk and exfoliated AgCrP$_2$Se$_6$ crystals including three helical vibrational modes. These modes exhibit large Raman optical activities (circular intensity di^erences) in bulk AgCrP$_2$Se$_6$, which progressively decrease with thickness. We also observe strong excitation energy dependent peak intensities as well as a decrease in anti-Stokes peak intensities at room temperature with increasing excitation energy, resulting in an apparent cooling by up to 220 K. All of these anomalies in bulk and exfoliated flakes are attributed to the unique ABC layer stacking structure of AgCrP$_2$Se$_6$ and to the smaller unit cell volume that causes hybridization between the Se and Ag/Cr electron densities, resulting in charge transfer and strongly a^ecting the electron-phonon coupling. This work thus positions AgCrP$_2$Se$_6$ as an exciting new 2D material for optical and phononic applications.

cond-mat.mes-hall↗

arXiv2025

Thermal and dimensional stability of photocatalytic material ZnPS$_3$ under extreme environmental conditions

Zinc phosphorus trisulfide (ZnPS$_3$), a promising material for photocatalysis and energy storage, is shown in this study to exhibit remarkable stability under extreme conditions. We explore its optical and structural properties under high pressure and cryogenic temperatures using photoluminescence (PL) spectroscopy, Raman scattering, and density functional theory (DFT). Our results identify a pressure-induced phase transition starting at 6.75 GPa and stabilizing by 12.5 GPa, after which ZnPS$_3$ demonstrates robust stability across a broad pressure range of 15 to 100 GPa. DFT calculations predict a semiconductor-to-semimetal transition at 100 GPa, while PL measurements reveal defect-assisted emissions that quench under pressure due to enhanced non-radiative recombination. At cryogenic temperatures, PL quenching intensifies as non-radiative processes dominate, driven by a rising Grüneisen parameter and reduced phonon population. Cryogenic X-ray diffraction (XRD) also reveals a high mean thermal expansion coefficient (TEC) of (4.369 $\pm$ 0.393) $\times$ 10$^{-5}$ K$^{-1}$, among the highest reported for 2D materials. This unique combination of tunable electronic properties under low pressure and high thermal sensitivity makes ZnPS$_3$ a strong candidate for sensing applications in extreme environments.

cond-mat.mtrl-sci↗

arXiv2024

Defect-Induced Strain-Tunable Photoluminescence in AgScP$_2$S$_6$

Metal thiophosphates (MTPs) are a large family of 2D materials that exhibit large structural and chemical diversity. They also show promise for applications in energy harvesting and photodetection. Strain and defect engineering have previously been demonstrated as useful mechanisms to tune several properties of MTPs such as resistivity, magnetic state, and electronic band gap. However, the effect of these stimuli on engineering tunable light emission in MTPs remains unexplored. Here, we show experimentally that structural defects in metal thiophosphate AgScP$_2$S$_6$ are prominent in exhibiting photoluminescence, which is likely driven by the defect-state-to-conduction-band transitions and can be further tuned by temperature-induced strain gradients.

physics.optics↗

arXiv2023

Investigating strain between phase-segregated domains in Cu-deficient CuInP2S6

CuInP2S6 (CIPS) is an emerging layered ferroelectric material with a TC above room temperature. When synthesized with Cu deficiencies (i.e., Cu1-xIn1+x/3P2S6), the material segregates into CIPS and In4/3P2S6 (IPS) self-assembled heterostructures within the same single crystal. This segregation results in significant in-plane and out-of-plane strains between the CIPS and IPS phases as the volume fraction of CIPS (IPS) domains shrink (grow) with decreasing Cu fraction. Here, we synthesized CIPS with varying amounts of Cu (x = 0, 0.2, 0.3, 0.4, 0.5, 0.7, 0.8 and 1) and measured the strains between the CIPS and IPS phases through the evolution of the respective Raman, infrared, and optical reflectance spectra. Density functional theory calculations revealed vibrational modes unique to the CIPS and IPS phases, which can be used to distinguish between the two phases through two-dimensional Raman mapping. A comparison of the composition-dependent frequencies and intensities of the CIPS and IPS Raman peaks showed interesting trends with decreasing CIPS phase fraction (i.e., Cu/In ratio). Our data reveal red- and blue-shifted Raman and infrared peak frequencies that we correlate to lattice strains arising from the segregation of the material into CIPS and IPS chemical domains. The strain is highest for a Cu/In ratio of 0.33 (Cu0.4In1.2P2S6), which we attribute to equal and opposite strains exerted by the CIPS and IPS phases on each other. In addition, bandgaps extracted from the optical reflectance spectra revealed a decrease in values, with the lowest value (~ 2.3 eV) for Cu0.4In1.2P2S6.

cond-mat.mtrl-sci↗

arXiv2023

Pressure-Induced Insulator-to-Metal Transition in van der Waals compound CoPS$_3$

We have studied the insulator-to-metal transition and crystal structure evolution under high pressure in the van der Waals compound CoPS$_3$ through $\textit{in-situ}$ electrical resistance, Hall resistance, magnetoresistance, X-ray diffraction, and Raman scattering measurements. CoPS$_3$ exhibits a $C2/m$ $\rightarrow$ $P\overline{3}$ structural transformation at 7 GPa accompanied by a 2.9$\%$ reduction in the volume per formula unit. Concomitantly, the electrical resistance decreases significantly, and CoPS$_3$ becomes metallic. This metallic CoPS$_3$ is a hole-dominant conductor with multiple conduction bands. The linear magnetoresistance and the small volume collapse at the metallization suggest the incomplete high-spin $\rightarrow$ low-spin transition in the metallic phase. Thus, the metallic CoPS$_3$ possibly possesses an inhomogeneous magnetic moment distribution and short-range magnetic ordering. This report summarizes the comprehensive phase diagram of $M$PS$_3$ ($M$ = V, Mn, Fe, Co, Ni, and Cd) that metalize under pressures.

cond-mat.str-el↗

arXiv2022

Phonon anharmonicity in Cu-based layered thiophosphates

In this work, we performed temperature-dependent Raman spectroscopy studies on three layered metal thiophosphates: CuInP2S6, CuCrP2S6, and CuInP2S6-In4/3P2S6 heterostructures. These materials are emerging multiferroics, with CuInP2S6 and CuInP2S6-In4/3P2S6 exhibiting room temperature ferrielectric polarization while CuCrP2S6 is both anti-ferroelectric and antiferromagnetic at low temperatures (<145 and <30 K, respectively). We studied two prominent peaks in the Raman spectra of these compounds, namely their P-P and P-S stretching modes. First order linear fits to the mode softening yielded coefficients similar to other layered materials. Furthermore, analysis of the phonon decay revealed the dominant role of anharmonic effects rather than thermal expansion. In particular, the decay of the optical phonons was found to be governed by three-phonon processes in CuInP2S6 and CuCrP2S6 and by the four-phonon process in the CuInP2S6-In4/3P2S6 heterostructures. These phonon lifetimes were found to be less than 1 ps, indicating high scattering rates and showing the potential for these materials to be used in thermoelectric applications.

cond-mat.mtrl-sci↗