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Two-color high-harmonic generation from relativistic plasma mirrors

July 7, 2023|

Circularly polarized x-rays have a number of microscopy applications that leverage the rotational nature of some physical systems, one of the most common applications being magnetic dichroism of nanoscale magnetic devices. Generating circularly polarized x-rays, particularly coherent x-rays with ultrafast pulse durations is practically difficult and inefficient. One of the major successes of STROBE was the development of not just one, but two mechanisms for generating circularly polarized x-rays using light at moderate intensities in the strong field regime. In this work, we lay the foundation for scaling analogous mechanisms into the relativistic regime. In this regime, the energy cutoff can be much higher than in the strong field. Performing numerical simulations, we confirm that despite the physical mechanism being completely different at relativistic intensities, the same conservation laws observed in the earlier STROBE work are still valid in the relativistic regime. Experiments are being planned to demonstrate this mechanism in the lab, which can leverage new facilities such as the NSF ZEUS which would enable high single shot flux in dichroism experiments.

N. F. Beier, F. F. Dollar, “Two-color high-harmonic generation from relativistic plasma mirrors,” Physical Review E, 108, 015201, (2023). DOI: 10.1103/physreve.108.015201

Predicting heat flow in 3D semiconductor nanosystems

May 17, 2023|

Nanostructuring on length scales corresponding to phonon mean free paths provides control over heat flow in semiconductors and makes it possible, in principle, to engineer their thermal properties. However, this is currently not feasible because there is no general description for heat flow in 3D nanostructured semiconductors. In recent research, STROBE scientists used short wavelength extreme ultraviolet beams to study heat transport in a silicon metalattice with deep nanoscale features. They observed dramatically reduced thermal conductivity relative to bulk—about x50 times less than current model predictions. To explain this, they developed a new predictive theory that incorporates the idea that heat-carrying lattice vibrations can behave like a fluid—spreading out instead of just moving ballistically in straight lines. Moreover, this new theory of heat transport can be used to predict and engineer phonon transport in many other 3D nanosystems including nanowires and nanomeshes, that are of great interest for next-generation energy-efficient devices.

McBennett, A. Beardo, E. Nelson, B. Abad, T. Frazer, A. Adak, B. Li, H. Kapteyn, M. Murnane, J. Knobloch, "Universal Behavior of Highly Confined Heat Flow in Semiconductor Nanosystems: From Nanomeshes to Metalattices," Nano Letters 23, 2129 (2023).

Relationships between Compositional Heterogeneity and Electronic Spectra of (Ga1−xZnx)(N1−xOx) Nanocrystals Revealed by Valence Electron Energy Loss Spectroscopy

April 17, 2023|

Many ternary and quaternary semiconductors have been made in nanocrystalline forms for a variety of applications, but we have little understanding of how well their ensemble properties reflect the properties of individual nanocrystals. STROBE researchers at CU Boulder examined electronic structure heterogeneities in nanocrystals of (Ga1−xZnx)(N1−xOx), a semiconductor that splits water under visible illumination. They used valence electron energy loss spectroscopy (VEELS) in a scanning transmission electron microscope to map out electronic spectra of (Ga1−xZnx)(N1−xOx) nanocrystals with a spatial resolution of 8 nm. They examine three samples with varying degrees of intraparticle and interparticle compositional heterogeneity and ensemble optical spectra that range from a single band gap in the visible to two band gaps, one in the visible and one in the UV. The VEELS spectra resemble the ensemble absorption spectra for a sample with a homogeneous elemental distribution and a single band gap and, more interestingly, one with intraparticle compositional heterogeneity and two band gaps. They observe spatial variation in VEELS spectra only with significant interparticle compositional heterogeneity. Hence, they reveal the conditions under which the ensemble spectra reveal the optical properties of individual (Ga1−xZnx)(N1−xOx) particles. More broadly, they illustrate how VEELS can be used to probe electronic heterogeneities in compositionally complex nanoscale semiconductors.

B. F. Hammel, L. G. Hall, L. M. Pellows, O. M. Pearce, P. Tongying, S. Yazdi, G. Dukovic, “Relationships between Compositional Heterogeneity and Electronic Spectra of (Ga1-xZnX)(N1-xOX) Nanocrystals Revealed by Valence Electron Energy Loss Spectroscopy,” The Journal of Physical Chemistry C, 127, 7762-7771, (2023). DOI: 10.1021/acs.jpcc.3c00572

The Swirling Spins of Hedgehogs

January 24, 2023|

Though microscopes have been in use for centuries, there is still much that we cannot see at the smallest length scales. Current microscopies range from the simple optical microscopes used in high school science classes, to x-ray microscopes that can image through visibly-opaque objects, to electron microscopes that use electrons instead of light to capture images of vaccines and viruses. However, there is a great need to see beyond the static structure of an object—to be able capture how a nano- or biosystem functions in real time, or to visualize magnetic fields on nanometer scales. A team of researchers from the STROBE Center have been working together to overcome these challenges. STROBE is an NSF Science and Technology Center that is building the microscopes of tomorrow. A large multidisciplinary team from the Miao and Osher groups from UCLA, the Kapteyn-Murnane group at CU Boulder, Ezio Iacocca from CU Colorado Springs, David Shapiro and collaborators at Lawrence Berkley National Laboratory, and the Badding and Crespi groups from Pennsylvania State University. They developed and implemented a new method to use x-ray beams to capture the 3D magnetic texture in a material with very high 10-nanometer spatial resolution for the first time (published in Nature Nanotechnology, see reference below).

Hedgehogs and Anti-Hedgehogs

The team investigated a nanostructured magnetic sample, consisting of tiny spheres of nickel, only ~30nm across, connected together by slender few-nm “necks” of nickel, that together form a structure called a magnetic metalattice. This complex nanostructured magnet is expected to produce swirling magnetic fields with topological spin textures that are far more complex than in a uniform magnet. These are called 3D topological magnetic monopoles – or hedgehogs, due to their spiny shape in magnetic rotation – if the magnetic field points outward. Conversely, they can be thought of anti-hedgehogs if the magnetic field points inward.  However, until recently, there was no experimental method to measure the 3D spin texture at the deep nanoscale. Using advanced algorithms to recover the image, and a microscope at the x-ray synchrotron light source at the Lawrence Berkley National Laboratory, the researchers overcame these challenges.

Imaging spin textures is extremely important, as it can help physicists to better understand magnetism at a fundamental level, and to design more energy-efficient data storage, memory, and nanodevices.  Using electron microscopy, one can capture beautiful 2D images of a static spin-texture, but it is challenging to capture a full 3D image. In the past, other scientists were able to capture a 3D image at a spatial resolution of about 100 nanometers, but they had to make assumptions about the sample to extract the 3D image. With this new technique, researchers do not have to make any assumptions.

Armed with this new visualization technique, the team of researchers is excited to study spin textures further. STROBE is developing tabletop setups and helping with national facilities that can capture the static and dynamic spin texture in materials. All algorithms developed for this data analysis will be open-sourced soon. In this experiment, as with others, they found that collaboration is key for moving scientific progress forward.

A. RanaC. LiaoE. IacoccaJ. ZouM. PhamX. LuE. SubramanianY. LoS. A. RyanC. S. BevisR. M. KarlA. J. GlaidJ. RableP. MahaleJ. HirstT. OstlerW. LiuC. M. O’LearyY. YuK. BustilloH. OhldagD. A. ShapiroS. YazdiT. E. MalloukS. J. OsherH. C. KapteynV. H. CrespiJ. V. BaddingY. TserkovnyakM. M. MurnaneJ. Miao, ""Three-dimensional topological magnetic monopoles and their interactions in a ferromagnetic meta-lattice," Nature Nanotechnology(2023)DOI: 10.1038/s41565-022-01311-0

Three-dimensional topological magnetic monopoles and their interactions in a ferromagnetic meta-lattice

January 23, 2023|

Topological magnetic monopoles (TMMs), also known as hedgehogs or Bloch points, are three-dimensional (3D) nonlocal spin textures that are robust to thermal and quantum fluctuations due to their topology. Understanding their properties is of fundamental interest and practical applications. However, it has been difficult to directly observe the 3D magnetization vector field of TMMs and probe their interactions at the nanoscale. Now, a STROBE team from UCLA, CU Boulder, UC Berkeley and LBNL collaborated with the Penn State MRSEC reports the creation of 138 stable TMMs at the specific sites of a ferromagnetic meta-lattice at room temperature. They developed 3D soft x-ray vector ptychography to determine the magnetization vector and emergent magnetic field of the TMMs with a 3D spatial resolution of 10 nm. This spatial resolution is comparable to the magnetic exchange length of transition metals, enabling them to probe monopole-monopole interactions. The team found that the TMM and anti-TMM pairs are separated by 18.3±1.6 nm, while the TMM and TMM, anti-TMM and anti-TMM pairs are stabilized at comparatively longer distances of 36.1±2.4 nm and 43.1±2.0 nm, respectively. They also observed virtual TMMs created by magnetic voids in the meta-lattice. This work demonstrates that ferromagnetic meta-lattices could be used as a new platform to create and investigate the interactions and dynamics of TMMs. Furthermore, it is expected that soft x-ray vector ptychography can be broadly applied to quantitatively image 3D vector fields in magnetic and anisotropic materials at the nanoscale.

A. Rana, C. Liao, E. Iacocca, J. Zou, M. Pham, X. Lu, E. Subramanian, Y. Lo, S. A. Ryan, C. S. Bevis, R. M. Karl, A. J. Glaid, J. Rable, P. Mahale, J. Hirst, T. Ostler, W. Liu, C. M. O’Leary, Y. Yu, K. Bustillo, H. Ohldag, D. A. Shapiro, S. Yazdi, T. E. Mallouk, S. J. Osher, H. C. Kapteyn, V. H. Crespi, J. V. Badding, Y. Tserkovnyak, M. M. Murnane, J. Miao, “Three-dimensional topological magnetic monopoles and their interactions in a ferromagnetic meta-lattice,” Nature Nanotechnology, 18, 227-232, (2023). DOI: 10.1038/s41565-022-01311-0

Deep-Learning Electron Diffractive Imaging

January 6, 2023|

Coherent diffractive imaging (CDI) is revolutionizing the physical and biological science fields by first measuring the diffraction patterns of nano-crystals or non-crystalline samples and then inverting them to high-resolution images. The well-known phase problem is solved by the combination of coherent illumination and iterative computational algorithms. In particular, ptychography – a powerful scanning CDI method – has found wide applications with synchrotron radiation, high harmonic generation, electron and optical microscopy. However, iterative algorithms are not only computationally expensive, but also require practitioners to get algorithmic training to optimize the parameters and obtain satisfactory results. These difficulties  have thus far prevented CDI from being accessible to an even broader user community. Here we demonstrated deep learning CDI using convolutional neural networks (CNNs) trained only by simulated data. The CNNs are subsequently used to directly retrieve the phase images of monolayer graphene, twisted hexagonal boron nitride and a Au nanoparticle from experimental electron diffraction patterns without any iteration. Quantitative analysis shows that the phase images recovered by the CNNs have comparable quality to those reconstructed by a conventional iterative method and the resolution of the phase images by the CNNs is in the range of 0.71-0.53 Å. Looking forward, we expect that deep learning CDI could become an important tool for real-time, atomic-scale imaging of a wide range of samples across different disciplines.    

D. J. Chang, C. M. O’Leary, C. Su, D. A. Jacobs, S. Kahn, A. Zettl, J. Ciston, P. Ercius, J. Miao, “Deep-Learning Electron Diffractive Imaging,” Physical Review Letters, 130, 016101, (2023). DOI: 10.1103/physrevlett.130.016101

Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations

December 5, 2022|

In ultrafast electron diffraction (UED) experiments, accurate retrieval of time-resolved structural parameters, such as atomic coordinates and thermal displacement parameters, requires an accurate scattering model. In this article, we demonstrated dynamical scattering models that are suitable for matching ultrafast electron diffraction (UED) signals from single-crystal films and retrieving the lattice temperature dynamics. We first described the computational approaches used, including both a multislice and a Bloch wave method, and introduced adaptations to account for key physical parameters. We then illustrated the role of dynamical scattering in UED of single-crystal films by comparing static and temperature-dependent diffraction signals calculated using kinematical and dynamical models for gold films of varying thicknesses and rippling as well as varying electron probe energy. Lastly, we applied these models to analyze relativistic UED measurements of single-crystal gold films recorded at the High Repetition-rate Electron Scattering (HiRES) beamline of Lawrence Berkeley National Laboratory. Our results showed the importance of a dynamical scattering theory for quantitative analysis of UED and demonstrated models that can be practically applied to single-crystal materials and heterostructures.

D. B. Durham, C. Ophus, K. M. Siddiqui, A. M. Minor, D. Filippetto, “Accurate quantification of lattice temperature dynamics from ultrafast electron diffraction of single-crystal films using dynamical scattering simulations,” Structural Dynamics, 9, 064302, (2022). DOI: 10.1063/4.0000170

Assessing student engagement with teamwork in an online, large-enrollment course-based undergraduate research experience in physics

October 25, 2022|

Over the last decade, course-based undergraduate research experiences (CUREs) have been recognized as a way to improve undergraduate science, technology, engineering, and mathematics education by engaging students in authentic research practices. One of these authentic practices is participating in teamwork and collaboration, which is increasingly considered to be an important component of undergraduate research experiences and laboratory classes. For example, the American Association of Physics Teachers Recommendations for the Undergraduate Physics Laboratory Curriculum suggest that one of the goals for students in physics labs should be to develop “interpersonal communication skills” through “teamwork and collaboration.” Teamwork can have tremendous benefits for students, including increased motivation, creativity, and reflection; however, it can also pose an array of new social and environmental challenges, such as differing styles of communication, levels of commitment, and understanding of concepts. It can also be difficult for lab course instructors to evaluate and assess. In this work, we study student teamwork in a large-enrollment physics CURE. The CURE was specifically designed to emphasize teamwork as a scientific practice. We use the two sources of data, the adaptive instrument for regulation of emotions questionnaire and students’ written memos to future researchers, to measure the students’ teamwork goals, challenges, self, co-, and socially shared regulations, and perceived goal attainment. We find that students overwhelmingly achieved their teamwork goals by overcoming obstacles using primarily socially shared regulatory strategies, and that the vast majority of students felt teamwork was an essential part of their research experience. We discuss implications for the design of future CUREs and lab courses and for lab instructors desiring to assess teamwork in their own courses.

A. Werth, et al., "Assessing student engagement with teamwork in an online, large-enrollment course-based undergraduate research experience in physics," Physical Review Physics Education Research18020128(2022). DOI: 10.1103/physrevphyseducres.18.020128

Structural and Elastic Properties of Nanostructured Materials Extracted Via Nondestructive Coherent Extreme UV Scatterometry and Electron Tomography

September 2, 2022|

Semiconductor metalattices consisting of a linked network of 3D nanostructures with periodicities on length scales <100nm can enable tailored functional properties due to their complex nanostructuring. For example, by controlling both the porosity and pore size, thermal transport in these phononic metalattices can be tuned—making them promising candidates for efficient thermoelectrics or thermal rectifiers. Thus, the ability to characterize the porosity, and other physical properties, of metalattices is critical but challenging, due to their nanoscale structure and thickness. To date, only metalattices with high porosities, close to the close-packing fraction of hard spheres, have been studied experimentally. Recently, a STROBE team characterized the porosity, thickness, and elastic properties of a low-porosity, empty-pore silicon metalattices for the first time. Laser-driven nanoscale surface acoustic waves were probed by EUV scatterometry to nondestructively measure the acoustic dispersion in these thin silicon metalattice layers. The Young’s modulus, porosity and metalattice layer thickness were then extracted. These advanced characterization techniques are critical for informed and iterative fabrication of energy-efficient devices based on nanostructured metamaterials.

Knobloch et al., “Structural and elastic properties of empty-pore metalattices extracted via nondestructive coherent extreme UV scatterometry and electron tomography, ACS Applied Materials and Interfaces 14, 41316 (2022). Abad et al., “Nondestructive measurements of the mechanical and structural properties of nanostructured metalattices,” Nano Letters 20, 3306 (2020). DOI: 10.1021/acs.nanolett.0c00167

Unveiling the spontaneous blistering of graphene

March 22, 2022|

The outstanding electrical and optical properties of graphene are intricately linked to its extraordinary mechanical behaviors. We report that for monolayer and few-layer graphene on common silicon and glass substrates, acidic solutions induce fast, spontaneous generation of solution-enclosing blisters/bubbles. Using interference reflection microscopy (IRM), a method we developed to visualize graphene structure and defects with outstanding contrast, we monitor the blister-generating process in situ, and show that at pH<~2, nanoscale to micrometer-sized graphene blisters, up to ~100 nm in height, are universally generated with high surface coverages on hydrophilic, but not hydrophobic, surfaces. The spontaneously generated blisters are highly dynamic, with growth, merging, and reconfiguration occurring at second-to-minute time scales. Moreover, we show that in this dynamic system, graphene behaves as a semipermeable membrane that allows the relatively free passing of water, impeded passing of the NaCl solute, and no passing of large dye molecules. Consequently, the blister volumes can be fast and reversibly modulated by the solution osmotic pressure.

Li, B. et al., "Dynamic, spontaneous blistering of substrate-supported graphene in acidic solutions," ACS Nano, 16, 6145-6152, 2022. DOI: 10.1021/acsnano.1c11616
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