arXiv subjects

Darshan Chalise

Publications and source records attributed to Darshan Chalise.

14 recordsLinked to original sources

arXiv2026

Dynamical diffraction formalism for imaging time-dependent diffuse scattering from coherent phonons with Dark-Field X-ray Microscopy

Coherent acoustic phonons, whose damping sets the upper bound of quality factors in acoustic resonators, play a critical role in advanced telecommunication and quantum information technologies. Yet, probing their decay in the GHz regime remains challenging using conventional surface-based techniques. Dark-field X-ray microscopy (DFXM) offers a solution by enabling through-depth, non-destructive and full-field imaging of strain fields and dislocations inside bulk materials with high spatial and angular resolution. We previously used kinematic diffraction theory to describe DFXM signals based on how the Bragg peak shifts due to the strain wave, allowing us to reconstruct the frequency spectrum of coherent phonons as a function of depth through the sample. The approach of tracking the Bragg peak shifts to study phonon dynamics, however, places an upper-bound to the highest phonon frequency that can be studied, determined by the spatial resolution of the measurement. In this work, we discuss how coherent phonon dynamics can be studied with DFXM from time-dependent intensity oscillation sidebands. This approach simultaneously allows studying coherent phonon dynamics in real and reciprocal space, overcoming frequency resolution limits imposed by the real-space resolution of Bragg-peak tracking. Using Takagi-Taupin dynamical diffraction formalism, we establish the spatial and reciprocal space resolution achievable for studying the coherent phonon dynamics and evaluate conditions for observing long-lived intensity oscillations. We close by proposing experimental strategies to optimize excitation bandwidths and reciprocal-space selectivity. The formalism in the paper enables the design of DFXM experiments for quantitative, frequency-resolved measurements of acoustic phonon decay and phonon-defect interactions in bulk crystalline materials.

cond-mat.mes-hall↗

arXiv2025

Computation and Sensitivity Analysis of the Deformation-Gradient Tensor Reconstruction in Dark-Field X-ray Microscopy

Spatially resolved strain measurements are crucial to understanding the properties of engineering materials. Although strain measurements utilizing techniques such as transmission electron microscopy and electron backscatter diffraction offer high spatial resolution, they are limited to surface or thin samples. X-ray diffraction methods, including Bragg Coherent Diffraction Imaging and X-ray topography, enable strain measurements deep inside bulk materials but face challenges in simultaneously achieving both high spatial resolution and large field-of-view. Dark-field X-ray Microscopy (DFXM) offers a promising solution with its ability to image bulk crystals at the nanoscale while offering a field-of-view approaching a few hundred $μ$m. However, an inverse modeling framework to explicitly relate the angular shifts in DFXM to the strain and lattice rotation tensors is lacking. In this paper, we develop such an inverse modeling formalism. Using the oblique diffraction geometry, enabling access to noncoplanar symmetry-equivalent reflections, we demonstrate that the reconstruction of the full deformation gradient tensor ($\mathbf{F^{(g)}}$) is possible. We also develop the computational framework to both forward calculate the anticipated angular shifts and reconstruct the average $\mathbf{F^{(g)}}$ for an individual pixel from DFXM experiments. Finally, utilizing the established formalism and computational framework, we present methods for sensitivity analysis to relate individual components of the rotation or strain tensor to specific angles of DFXM. The developed sensitivity analysis also enables explicit computation of the errors associated with the reconstruction of each component. The formalism, the computational framework, and the sensitivity analysis established in this paper should assist both the interpretation of past DFXM experiments and the design of future DFXM experiments.

cond-mat.mtrl-sci↗

arXiv2025

Planar 3$ω$ and 2$ω$ Method for Increased Sensitivity to Through-Plane Thermal Properties

Accurately measuring the thermal properties of buried interfaces is crucial for understanding heat transport in multilayered materials, particularly in applications such as batteries and integrated circuits. The conventional 3$ω$ method, which uses a line heater, has limited sensitivity to through-plane thermal properties due to lateral heat spreading, especially when a highly conductive layer overlays a resistive one. Additionally, when using a line heater, there is a lower limit to the frequency of heating, below which the analytical solution assuming infinite lateral dimension is not valid. This limits analytical interpretation of 2$ω$ temperature oscillation at lower frequencies where the sensitivity to the conductivity of a buried layer is greater. To overcome these limitations, we propose a planar 3$ω$ and 2$ω$ method that enhances the sensitivity to buried layers by ensuring planar heat flow. We implement this technique using a planar metallic heater across the entire sample and validate it experimentally against the analytical solution using Feldman's algorithm. We also discuss the practical implementation details of the approach, including ensuring uniform current distribution and the required sensor layout. Our results demonstrate improved measurement sensitivity for polymer layers in silicon stacks and buried interfaces in battery electrodes, with sensitivity improvements by factors of 2-5 compared to conventional technique using a line heater.

physics.app-ph↗

arXiv2024

X-ray induced grain boundary formation and grain rotation in Bi2Se3

Optimizing grain boundary characteristics in polycrystalline materials can improve their properties. Many processing methods have been developed for grain boundary manipulation, including the use of intense radiation in certain applications. In this work, we used X-ray free electron laser pulses to irradiate single-crystalline bismuth selenide (Bi2Se3) and observed grain boundary formation and subsequent grain rotation in response to the X-ray radiation. Our observations with simultaneous transmission X-ray microscopy and X-ray diffraction demonstrate how intense X- ray radiation can rapidly change size and texture of grains.

cond-mat.mtrl-sci↗

arXiv2024

Formalism to Image the Dynamics of Coherent and Incoherent Phonon with Dark-Field X-ray Microscopy using Kinematic Diffraction Theory

Dark-field X-ray microscopy (DFXM) is a novel X-ray imaging technique developed at synchrotrons to image along the diffracted beam with a real space resolution of ~100 nm and reciprocal space resolution of $10^{-4}$. Recent implementations of DFXM at X-ray free electron lasers (XFELs) have demonstrated DFXM's ability to visualize the real-time evolution of coherent GHz phonons produced by ultrafast laser excitation of metal transducers. Combining this with DFXM's ability to visualize strain fields due to dislocations makes it possible to study the interaction of GHz coherent phonons with the strain fields of dislocations, along with studying the damping of coherent phonons due to interactions with thermal phonons. For quantitative analysis of phonon-dislocation interactions and phonon damping, a formalism is required to relate phonon dynamics to the strains measured by DFXM. In this work, we use kinematic diffraction theory to simulate DFXM images of the specific coherent phonons in diamond that are generated by the ultrafast laser excitation of a metal transducer. We extend this formalism to also describe imaging of incoherent phonons of sufficiently high frequency, which are relevant for thermal transport, offering future opportunities for DFXM to image signals produced by thermal diffuse scattering. For both coherent and incoherent phonons, we discuss the optimal sampling of real space, reciprocal space and time, and the opportunities offered by the advances in DFXM optics.

cond-mat.mtrl-sci↗

arXiv2024

Improving nuclear magnetic resonance and electron spin resonance thermometry with size reduction of superparamagnetic iron oxide nanoparticles

Thermometry based on magnetic resonance has been extensively studied due to its important application in biomedical imaging. In our previous work, we showed that the spin-spin relaxation time (T2) of nuclear magnetic resonance (NMR) in water is a highly sensitive thermometer as T2 scales with the highly temperature-sensitive self-diffusion constant of water. In this work, in addition to temperature dependent self-diffusion constant of a fluid, we utilize the temperature dependent magnetization of 4 nm SPIONs to improve T2 sensitivity (4.96) by 1.4 times over self-diffusion (3.48) alone in hexane between 248 K and 333 K. To extend the application of NMR T2 thermometry to engineering systems, we also investigate the temperature dependence of T2 in mineral oil (Thermo Scientific, J62592), which exhibits remarkably high sensitivity (11.62) between 273 K and 353 K. This result implies that applications of NMR T2 thermometry in heat transfer fluids are promising. NMR thermometry, however, is generally not applicable to solids. Therefore, we also evaluate the potential of electron spin resonance (ESR) thermometry with SPIONs in solids between 100 K and 290 K, for potential temperature monitoring in biomedical and engineering applications. The size and concentration effects on ESR signals are studied systematically, and our results show that the temperature dependent linewidth follows a T^-2 law for 4 nm SPIONs, while the concentration of SPIONs has no impact on the temperature dependence of the ESR linewidth. The linewidth at room temperature at 9.4 GHz is 10.5 mT. Combining our NMR and ESR results, we find that to obtain higher temperature sensitivity in a magnetic resonance technique using SPIONs, SPION with a small magnetic moment, i.e., a small volume and reduced magnetization, are beneficial.

physics.app-ph↗

arXiv2023

Dark-Field X-ray Microscopy for 2D and 3D imaging of Microstructural Dynamics at the European X-ray Free Electron Laser

Dark field X-ray microscopy (DXFM) can visualize microstructural distortions in bulk crystals. Using the femtosecond X-ray pulses generated by X-ray free-electron lasers (XFEL), DFXM can achieve sub-{\mu}m spatial resolution and <100 fs time resolution simultaneously. In this paper, we demonstrate ultrafast DFXM measurements at the European XFEL to visualize an optically-driven longitudinal strain wave propagating through a diamond single crystal. We also present two DFXM scanning modalities that are new to the XFEL sources: spatially 3D and 2D axial-strain scans with sub-{\mu}m spatial resolution. With this progress in XFEL-based DFXM, we discuss new opportunities to study multi-timescale spatio-temporal dynamics of microstructures.

cond-mat.mes-hall↗

arXiv2023

Anisotropic thermal conductivity of high bandwidth memory

Thermal management of integrated circuits (ICs) is important to prevent thermal hotspots which are the leading cause of IC failure. Thermal management is even more critical in 3D integrated circuits (3D ICs) as the prevalence of thermal hotspots is expected to increase due to the presence of polymers and solder materials that are of low thermal conductivity. Understanding how thermal conductivity is affected by the presence of these materials is required for developing thermally aware IC design. The 3ω method can measure thermal conductivities spanning several orders of magnitude and is appropriate for measuring the thermal properties of layered structures such as 3D ICs. In this work, we use the 3ω method with planar and cylindrical heat flow geometries to determine thermal conductivities of the memory layers and layers with polymer and solder bumps in High Bandwidth Memory (HBM) Random Access Memory (RAM). We determine the in-plane thermal conductivity of the memory layers in HBM as 140 W/m-K, while the through-plane conductivity of the polymer/solder bump layer is 2 W/m-K. Combining the results of x-ray tomography and the 3-omega measurements, we estimate that the effective in-plane thermal conductivity of the overall HBM device is 100 W/m-K while the effective through-plane thermal conductivity is 7 W/m-K. Our results show that the presence of polymers and solder metals results in a significantly decreased through-plane thermal conductivity of a 3D IC compared to a single IC die. Improvement in the thermal performance of 3D ICs will require improvement in the thermal conductivity or the increased contact area of the solder metals used in 3D ICs.

physics.app-ph↗

arXiv2023

Temperature dependence of 7Li NMR relaxation rates in Li3InCl6, Li3YCl6, Li1.48Al0.48Ge1.52(PO4)3 and LiPS5Cl

Inorganic solid-state battery electrolytes show high ionic conductivities and enable the fabrication of all solid-state batteries. In this work, we present the temperature dependence of spin-lattice relaxation time (T1), spin-spin relaxation time (T2), and resonance linewidth of the 7Li nuclear magnetic resonance (NMR) for four solid-state battery electrolytes (Li3InCl6 (LIC), Li3YCl6 (LYC), Li1.48Al0.48Ge1.52(PO4)3 (LAGP) and LiPS5Cl (LPSC)) from 173 K to 403 K at a 7Li resonance frequency of 233 MHz, and from 253 K to 353 K at a 7Li resonance frequency of 291 MHz. Additionally, we measured the spin-lattice relaxation rates at an effective 7Li resonance frequency of 133 kHz using a spin-locking pulse sequence in the temperature range of 253 K to 353 K. In LPSC, the 7Li NMR relaxation is consistent with the Bloembergen-Pound-Purcell (BPP) theory of NMR relaxation of dipolar nuclei. In LIC, LYC and LAGP, the BPP theory does not describe the NMR relaxation rates for the temperature range and frequencies of our measurements. The presented NMR relaxation data assists in providing a complete picture of Li diffusion in the four solid-state battery electrolytes.

cond-mat.mtrl-sci↗

arXiv2023

Electron paramagnetic resonance of n-type silicon and germanium for applications in 3D thermometry

While several 2D thermometry techniques exist, there is a lack of 3D thermometry techniques that work for wide range of materials and offer good resolution in time, space and temperature. X-ray diffraction (XRD) and nuclear magnetic resonance (NMR) imaging can provide 3D temperature information. However, XRD is typically limited to crystalline materials while NMR is largely limited to liquids where the resonance lines are narrow. We investigate electron paramagnetic resonance (EPR) of n-type silicon and germanium for 3D thermometry. While in germanium the EPR linewidths are too broad, EPR linewidths in silicon are reasonably narrow and exhibit a strong temperature dependence. The temperature dependence of the spin-lattice relaxation rate (1/T1) of conduction electrons in n-type Si for low dopant concentrations follows a T^3 law due to phonon broadening. For heavily doped Si, which is desirable for good signal to noise ratio (SNR) for application in thermometry, impurity scattering is expected to decrease the temperature dependence of 1/T1. Our results show, in heavily doped n-type Si, spin-lattice relaxation induced by impurity scattering does not drastically decrease the temperature dependence of EPR linewidths. In P-doped Si with donor concentration of 7 x 10^18 /cm^3, the EPR linewidth has a T^(5/2) temperature dependence; the temperature dependence decreases to T^(3/2) when the donor concentration is 7 x 10^19 /cm^3. While the temperature dependence of linewidth decreases for heavier doping, EPR linewidth is still a sensitive thermometer. We define a figure of merit for SNR for thermometry from EPR linewidths of n-type Si and observe that increasing the doping results in a better SNR. Using effective medium theory, we show that EPR linewidth can be a sensitive thermometer for application in 3D thermometry with systems embedding microparticles of heavily doped n-type Si.

cond-mat.mtrl-sci↗

arXiv2023

Simultaneous mapping of temperature and hydration in proton exchange membrane of fuel cells using magnetic resonance imaging

The efficiency of a proton exchange membrane (PEM) fuel cell depends on the mobility of protons in the PEM, which is determined by the hydration and temperature of the membrane. While optical techniques or neutron or x-ray scattering techniques may be used to study the inhomogeneities in hydration and temperature in PEMs, these techniques cannot provide 3 dimensional spatial resolution in measuring layered PEMs. Due to their ability to provide non-invasive 3D images, spin-lattice relaxation time (T1) and spin-spin relaxation time (T2) contrast magnetic resonance imaging (MRI) of protons in PEMs have been suggested as methods to map hydration in the fuel cells. We show that while T1 and T2 imaging may be used to map hydration in PEMs under isothermal conditions, proton T1 and T2 are also a function of temperature. For PEM fuel cells, where current densities are large and thermal gradients are expected, T1 and T2 relaxation times cannot be used for mapping hydration. The chemical shift of the mobile proton is, however, a strong function of hydration but not temperature. Therefore, chemical shift imaging (CSI) can be used to map hydration. The diffusion constant of the mobile proton, which can be determined by pulsed field gradient NMR, increases with both temperature and hydration. Therefore, CSI followed by imaging of diffusion via pulsed field gradients can be used for separate mappings of hydration and temperature in PEMs. Here, we demonstrate a 16 x 16 pixel MRI mapping of hydration and temperature in Nafion PEMs with a spatial resolution of 1 mm x 1 mm, a total scan time of 3 minutes, a temperature resolution of 6 K, and an uncertainty in hydration within 15%. The demonstrated mapping can be generalized for imaging exchange membranes of any fuel cells or flow batteries.

cond-mat.mtrl-sci↗

arXiv2023

Highly sensitive and high throughput magnetic resonance thermometry using superparamagnetic nanoparticles

Magnetic resonance imaging (MRI) enables non-invasive 3D thermometry during thermal ablation of cancerous tumors. While T1 or T2 contrast MRI are relatively insensitive to temperature, techniques with greater temperature sensitivity such as chemical shift or diffusion imaging suffer from motional artifacts and long scan times. We describe an approach for highly sensitive and high throughput MR thermometry that is not susceptible to motional artifacts. We use superparamagnetic iron oxide nanoparticles (SPIONs) to spoil T2 of water protons. Motional narrowing results in proportionality between T2 and the diffusion constant, dependent only on the temperature in a specific environment. Our results show, for pure water, the nuclear magnetic resonance (NMR) linewidth and T2 follow the same temperature dependence as the self-diffusion constant of water. Thus, T2 mapping is a diffusion mapping in the presence of SPIONs, and T2 is a thermometer. For pure water, a T2 mapping of a 64 x 64 image (voxel size = 0.5 mm x 0.5 mm x 3 mm) in a 9.4 T MRI scanner resulted in a temperature resolution of 0.5 K for a scan time of 2 minutes. This indicates a highly sensitive and high throughput MR thermometry technique potentially useful for monitoring of biological tissues during thermal therapies or for diagnosis.

physics.med-ph↗

arXiv2022

Temperature mapping of stacked silicon dies from x-ray diffraction intensities

Increasing power densities in integrated circuits has led to an increased prevalence of thermal hotspots in integrated circuits. Tracking these thermal hotspots is imperative to prevent circuit failures. In 3D integrated circuits, conventional surface techniques like infrared thermometry are unable to measure 3D temperature distribution and optical and magnetic resonance techniques are difficult to apply due to the presence of metals and large current densities. X-rays offer high penetration depth and can be used to probe 3D structures. We report a method utilizing the temperature dependence of x-rays diffraction intensity via the Debye-Waller factor to simultaneously map the temperature of an individual silicon die that is a part of a stack of dies. Utilizing beamline 1-ID-E at the Advanced Photon Source (Argonne), we demonstrate for each individual silicon die, a temperature resolution of 3 K, a spatial resolution of 100 um x 400 um and a temporal resolution of 20 s. Utilizing a sufficiently high intensity laboratory source, e.g., from a liquid anode source, this method can be scaled down to laboratories for non-invasive temperature mapping of 3D integrated circuits.

physics.app-ph↗

arXiv2021

Good Solid-State Electrolytes Have Low, Glass-like Thermal Conductivity

Management of heat during charging and discharging of Li-ion batteries is critical for their safety, reliability, and performance. Understanding the thermal conductivity of the materials comprising batteries is crucial for controlling the temperature and temperature distribution in batteries. This work provides systemic quantitative measurements of the thermal conductivity of three important classes of solid electrolytes (oxides, sulfides, and halides) over the temperature range 150-350 K. Studies include the oxides Li1.5Al0.5Ge1.5(PO4)3 and Li6.4La3Zr1.4Ta0.6O12, sulfides Li2S-P2S5, Li6PS5Cl, and Na3PS4, and halides Li3InCl6 and Li3YCl6. Thermal conductivities of sulfide and halide solid electrolytes are in the range 0.45-0.70 W m-1 K-1; thermal conductivities of Li6.4La3Zr1.4Ta0.6O12 and Li1.5Al0.5Ge1.5(PO4)3 are 1.4 W m-1 K-1 and 2.2 W m-1 K-1, respectively. For most of the solid electrolytes studied in this work, the thermal conductivity increases with increasing temperature; i.e., the thermal conductivity has a glass-like temperature dependence. The measured room-temperature thermal conductivities agree well with the calculated minimum thermal conductivities indicating the phonon mean-free-paths in these solid electrolytes are close to an atomic spacing. We attribute the low, glass-like thermal conductivity of the solid electrolytes investigated to the combination of their complex crystal structures and the atomic-scale disorder induced by the materials processing methods that are typically needed to produce high ionic conductivities.

cond-mat.mtrl-sci↗