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DOE OSTI2025

In-plane thermal conductivity and the applicability of the Wiedemann–Franz law in dilute AlCu thin films

The Wiedemann–Franz (WF) law correlates heat and charge transport in metals. However, the validity of this correlation remains an open-ended question, especially in the context of inelastic scattering at room temperature. To address this gap in knowledge, we perform independent measurements of the in-plane thermal and electrical conductivities across four AlCu (0.5% Cu) films [thickness (⁠h⁠) ≈ 174, 98, 53, and 24 nm] using optical pump–probe metrologies and four-point probe techniques, respectively. For in-plane thermal conductivity measurements, we utilize time-domain thermoreflectance, in both concentric and beam-offset configurations, and the time-resolved magneto-optic Kerr effect. Our results show that the WF law overpredicts the thermal conductivity by at least ∼10% in all films, thus demonstrating modest deviations in predicted thermal conductivity when applying the WF law to dilute AlCu films. Using infrared variable angle spectroscopic ellipsometry, we demonstrate increased electron scattering rates in the thinnest film (⁠⁠h⁠ ≈ 24 nm), indicating electron-boundary scattering drives the reduction in in-plane thermal conductivity. Furthermore, this is generally an elastic scattering process, which is supported by our thermal conductivity measurements and analysis.

Electrical conductivity↗

DOE OSTI2020

Numerical simulation of the beam self-cleaning process in a multimode graded-index fibre during propagation of a pump wave and a Stokes component

A model of coupled modes is proposed, which makes it possible to describe the propagation of a pump wave and a Stokes component in a multimode graded-index fibre. A decrease in the depression in the centre of the profile of the pump wave intensity distribution as a result of the influence of Kerr effects and random linear coupling of modes is demonstrated. (paper)

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Disentangling electronic, lattice, and spin dynamics in the chiral helimagnet Cr 1/3 NbS 2

We investigate the static and ultrafast magneto-optical response of the hexagonal chiral helimagnet Cr 1/3 NbS 2 above and below the helimagnetic ordering temperature. The presence of a magnetic easy plane contained within the crystallographic $ab$-plane is confirmed, while degenerate optical pump-probe experiments reveal significant differences in the dynamic between the parent, NbS 2 , and Cr-intercalated compounds. Time-resolved magneto-optical Kerr effect measurements show a two-step demagnetization process, where an initial, subpicosecond relaxation and subsequent buildup (τ > 50ps) in the demagnetization dynamic scale similarly with increasing pump fluence. Despite theoretical evidence for partial gapping of the minority spin channel, suggestive of possible half-metallicity in Cr 1/3 NbS 2 , such a long demagnetization dynamic likely results from spin-lattice relaxation as opposed to minority state blocking. However, comparison of the two-step demagnetization process in Cr 1/3 NbS 2 with other 3d intercalated transition metal dichalcogenides reveals a behavior that is unexpected from conventional spin-lattice relaxation, and may be attributed to the complicated interaction of local moments with itinerant electrons in this material system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Transient magnetoelastic coupling in CrSBr

Recent research has revealed remarkable properties of the two-dimensional (2D) van der Waals layered crystal CrSBr, which is both a semiconductor and an A-type antiferromagnet. Here, in this study, we show the role of strong magnetoelastic coupling in the generation and propagation of coherent magnons in CrSBr. Time- and spatially resolved magneto-optical Kerr effect microscopy reveals two time-varying transient strain fields induced by out-of-plane transverse and in-plane longitudinal lattice displacements. These transient strain fields launch coherent wavepackets of magnons, optical and acoustic, at 24.6 ± 0.8 and 33.4 ± 0.5GHz, respectively. These findings suggest mechanisms for controlling and manipulating coherent magnons from distinct magnetoelastic couplings in this 2D van der Waals magnetic semiconductor.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Anisotropic X-Ray Scattering of Transiently Oriented Water

We study the structural dynamics of liquid water by time-resolved anisotropic x-ray scattering under the optical Kerr effect condition. In this way, we can separate the anisotropic scattering decay of 160 fs from the delayed temperature increase of ~ 0.1 K occurring at 1 ps and quantify transient changes in the O-O pair distribution function. Polarizable molecular dynamics simulations reproduce well the experiment, indicating transient alignment of molecules along the electric field, which shortens the nearest-neighbor distances. In addition, analysis of the simulated water local structure provides evidence that two hypothesized fluctuating water configurations exhibit different polarizability.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Revealing the Origin of Time-Reversal Symmetry Breaking in Fe-Chalcogenide Superconductor FeTe 1 - x Se x

We report that recently evidence has emerged in the topological superconductor Fe-chalcogenide FeTe 1-x Se x for time-reversal symmetry breaking (TRSB), the nature of which has strong implications on the Majorana zero modes (MZM) discovered in this system. It remains unclear however whether the TRSB resides in the topological surface state (TSS) or in the bulk, and whether it is due to an unconventional TRSB superconducting order parameter or an intertwined order. Here by performing in superconducting FeTe 1-x Se x crystals both surface-magneto-optic-Kerr effect (SMOKE) measurements using a Sagnac interferometer and bulk magnetic susceptibility measurements, we pinpoint the TRSB to the TSS, where we also detect a Dirac gap. Further, we observe surface TRSB in non-superconducting FeTe 1-x Se x of nominally identical composition, indicating that TRSB arises from an intertwined surface ferromagnetic (FM) order. The observed surface FM bears striking similarities to the two-dimensional (2D) FM found in 2D van der Waals crystals, and is highly sensitive to the exact chemical composition, thereby providing a means for optimizing the conditions for Majorana particles that are useful for robust quantum computing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Possible unconventional surface superconductivity in the half-Heusler compound YPtBi

Here, we report an extensive study of the noncentrosymmetric half-Heusler superconductor YPtBi, revealing an unusual relation between bulk superconductivity and the possible appearance of surface superconductivity on the (111) oriented surface, at temperatures up to three times the bulk transition temperature. Transport measurements confirmed the low carrier density of the material and its bulk superconducting transition, which was also observed in ac susceptibility through mutual inductance (MI) measurements. However, a weak signature of superconductivity in the MI measurements appeared much above the bulk transition temperature, which was further observed in scanning tunneling spectroscopy, pointing to a possible surface superconducting state. Polar Kerr effect measurements suggest that while the bulk superconductor may exhibit an unusual nodal superconducting state, only the surface state breaks time reversal symmetry. Complementary tunneling measurements on LuPtBi are used to establish the observations on YPtBi, while density-functional theory calculations may shed light on the origin of this unusual surface state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Free-space confocal magneto-optical spectroscopies at milliKelvin temperatures

We describe the operation of a free-space confocal optical microscope operated in a dilution refrigerator. The microscope is installed on a cold insertable probe to enable fast sample exchange while the refrigerator is held at low temperatures. A vector magnet provides a 6 T field normal to the sample and 1 T fields at arbitrary angles. A variety of optical microscopies and spectroscopies, including photoluminescence, Raman, magneto-optical Kerr effect, and spin relaxometry measurements are described, and some of the challenges associated with performing these measurements at milliKelvin temperatures are explored.

Lawrie, B. J.↗

DOE OSTI2020

Ferromagnetic order beyond the superconducting dome in a cuprate superconductor

According to conventional wisdom, the extraordinary properties of the cuprate high-temperature superconductors arise from doping a strongly correlated antiferromagnetic insulator. The highly overdoped cuprates—whose doping lies beyond the dome of superconductivity—are considered to be conventional Fermi liquid metals. We report the emergence of itinerant ferromagnetic order below 4 kelvin for doping beyond the superconducting dome in thin films of electron-doped La 2– x Ce x CuO 4 (LCCO). The existence of this ferromagnetic order is evidenced by negative, anisotropic, and hysteretic magnetoresistance, hysteretic magnetization, and the polar Kerr effect, all of which are standard signatures of itinerant ferromagnetism in metals. This surprising result suggests that the overdoped cuprates are strongly influenced by electron correlations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Multicomponent superconducting order parameter in UTe 2

An unconventional superconducting state was recently discovered in uranium ditelluride (UTe 2 ), in which spin-triplet superconductivity emerges from the paramagnetic normal state of a heavy-fermion material. The coexistence of magnetic fluctuations and superconductivity, together with the crystal structure of this material, suggests that a distinctive set of symmetries, magnetic properties, and topology underlie the superconducting state. Here, we report observations of a nonzero polar Kerr effect and of two transitions in the specific heat upon entering the superconducting state, which together suggest that the superconductivity in UTe 2 is characterized by a two-component order parameter that breaks time-reversal symmetry. These data place constraints on the symmetries of the order parameter and inform the discussion on the presence of topological superconductivity in UTe 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

hhg v1.0

The program simulates the non-linear propagation of a laser pulse through a gas medium and calculates the emission of harmonic radiation. The computational model includes the optical Kerr-effect and multiphoton ionization of the gas resulting in plasma dynamics.

Schroeder, Christian [Lawrence Berkeley National L↗

DOE OSTI2022

Antiferromagnetic-configuration–dependent high harmonic generation in bilayer CrI 3

Abstract Bilayer CrI 3 accommodates both interlayer antiferromagnetic (AFM) and intralayer ferromagnetic couplings. Different alignments of intralayer ferromagnetic orders would lead to almost degenerate AFM configurations, which are insensitive to conventional techniques such as VSM and magneto-optical Kerr effect. Here, we demonstrate high harmonic generation (HHG) as a feasible means to detect the AFM configurations in bilayer CrI 3 with AB and stacking orders. When the intralayer magnetic moments are aligned along the z -axis, the AB stacked bilayer CrI 3 cancels the 3 n -order harmonics under the circularly polarized laser field. However, the stacked bilayer contains both even and odd harmonic. The 3 n -order harmonics are recovered as the intralayer magnetic moments of AB bilayer are in-plane aligned. For an in-plane linearly polarized laser field, the stacking bilayer with the magnetic moments along the x -axis contains both the even and odd harmonics in each component. However, when the magnetic moments are along the y -axis, the perpendicular component of HHG cancels out for the linearly polarized laser field along the x -axis. More interestingly, when the linearly polarized laser field is along the y -axis, the parallel component includes only the odd harmonics while the perpendicular component contains only the even harmonics. Our study provides HHG as a potential tool to detect AFM configurations.

Physics↗

DOE OSTI2024

Extreme-value statistics in nonlinear optics

We show that, although nonlinear optics may give rise to a vast multitude of statistics, all these statistics converge, in their extreme-value limit, to one of a few universal extreme-value statistics. Specifically, in the class of polynomial nonlinearities, such as those found in the Kerr effect, weak-field harmonic generation, and multiphoton ionization, the statistics of the nonlinear-optical output converges, in the extreme-value limit, to the exponentially tailed, Gumbel distribution. Exponentially growing nonlinear signals, on the other hand, such as those induced by parametric instabilities and stimulated scattering, are shown to reach their extreme-value limits in the class of the Fréchet statistics, giving rise to extreme-value distributions (EVDs) with heavy, manifestly nonexponential tails, thus favoring extreme-event outcomes and rogue-wave buildup.

Zheltikov, Aleksei M. (ORCID:0000000291380576)↗

DOE OSTI2025

Single-element balanced detector giving 65 dB CMRR at 30 MHz

We present a simple design for a single-element balanced detector (BD) that utilizes optical fibers in the sensing and reference channels with path length differences set to detect the differential signal at a desired frequency. With this approach, we easily achieve a common-mode rejection ratio of 65 dB, corresponding to the shot-noise limit of our setup. The CMRR demonstration is made in the MHz frequency range but could be extended to the kHz or GHz range. Using a single detector, the BD achieves stable CMRR over extended periods and does not require careful matching of detectors and amplification electronics. We demonstrate the single-element balanced detector design using the optical Kerr effect induced by a 30 MHz pulsed laser, showing a significant improvement over similar experiments using a commercial balanced detector.

Badilla-Nunez, Kelly [Georgia Institute of Technol↗

DOE OSTI2020

The transient properties of 2D magnets: from mechanical exfoliation to ultrafast optical spectroscopy of CrX 3 materials

The discovery of two-dimensional (2D) systems hosting intrinsic long-range magnetic order represents a seminal achievement, adding to the already diverse array of physics supported by layered van der Waals (vdW) materials. This finding has spurred great interest among the research community, with efforts aimed at uncovering their fundamental properties and light- matter interactions. A prototypical example of a 2D magnetic material is Crl 3 , where the strong relationship between crystalline structure and magnetic order, along with strong light- matter interactions, provide a promising platform to explore the nature of couplings between magnetism and the other degrees of freedom at the 2D limit. In this report, we highlight our efforts involving the use of time-resolved magneto-optical Kerr effect (TR-MOKE) spectroscopy to probe the magnetization and vibrational dynamics of Crl 3 . These measurements reveal evidence of strong exchange-mediated coupling between lattice vibrations and spin oscillations. Additionally, we discuss our related efforts to explore other material from the Chromium trihalide family through mechanical exfoliation to support subsequent optical spectroscopy investigations.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Ferroelectric Large Polarons and Defect Tolerance in Multi-Component Lead Halide Perovskites

Solvation plays a pivotal role in chemistry and biology. A solid-state analogy of solvation is polaron formation, but the magnitude of Coulomb screening is typically an order-of-magnitude weaker than that of solvation in aqueous solutions. Here the PI aims to explore a new class of polarons, the ferroelectric large polaron, which allows efficient Coulomb screening of an electron or hole by extended ordering of dipoles from symmetry-broken unit cells. This kind of local ordering is reflected in the ferroelectric-like THz dielectric responses of lead halide perovskites (LHPs) and may be partially responsible for their exceptional optoelectronic performances. A charge carrier may be localized to and/or induce the formation of nanoscale domain boundaries of locally ordered dipoles in a ferroelectric or paraelectric material, i.e., crystal structure with polar unit cells or polar fluctuations. The ability to form ferroelectric large polarons can result in the efficient screening of charge carriers from scattering with other charge carriers, with charged defects, and with longitudinal optical phonons, thus contributing to enhanced optoelectronic properties. During the past funding period, the PI has explored efficient charge carrier screening in three-dimensional (3D) LHP crystals and has developed the ferroelectric large polaron model to explain a range of carrier properties in these materials. The PI has also developed a new experimental tool, two-dimensional optical Kerr effect (2D-OKE), which is particularly powerful in probing photophysical properties with exquisite energy resolution at or near the bandgap. During the next funding periods, the PI aims to establish the applicability of the ferroelectric large polaron proposal as a general principle for the design/search of defect tolerant semiconductors in optoelectronics. Preliminary experiments on model semiconductor systems beyond LHPs have demonstrated the feasibility of the proposed research.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Free-space confocal magneto-optical spectroscopies at milliKelvin temperatures

Lawrie, Benjamin↗

DOE OSTI2023

Spin-carrier coupling induced ferromagnetism and giant resistivity peak in EuCd 2 P 2

EuCd 2 P 2 is notable for its unconventional transport: upon cooling the metallic resistivity changes slope and begins to increase, ultimately 100-fold, before returning to its metallic value. Surprisingly, this giant peak occurs at 18 K, well above the Néel temperature (T N ) of 11.5 K. Here, using a suite of sensitive probes of magnetism, including resonant x-ray scattering and magneto-optical polarimetry, we have discovered that ferromagnetic order onsets above T N in the temperature range of the resistivity peak. The observation of inverted hysteresis in this regime shows that ferromagnetism is promoted by coupling of localized spins and itinerant carriers. The resulting carrier localization is confirmed by optical conductivity measurements.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗