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DOE OSTI2024

Real-space visualization of atomic displacements in a long-wavelength charge density wave using cryogenic 4D-STEM

EuA⁢l 4 , a known skyrmion magnet, represents a class of materials that show complex electronic behaviors involving long-wavelength charge density wave (CDW). Here we realize direct real-space imaging of the concomitant periodic lattice distortion (PLD) with picometer precision in EuA⁢l 4 . Simultaneous imaging of microstructure, polarization, and interatomic distance is made possible using cryogenic four-dimensional scanning transmitting electron microscopy (cryo-4DSTEM). With this approach, we determined that the PLD in EuA⁢l 4 incorporates two out-of-phase atomic displacement modes on the Eu and Al sublattices. The PLD introduces periodic local symmetry fluctuations from the average symmetry of the bulk EuA⁢l 4 crystal. This critical local structural insight helps understanding of charge-spin-lattice couplings behind the intertwined quantum order in EuA⁢l 4 . Furthermore, our results also demonstrate cryo-4DSTEM as an indispensable approach for probing CDW and related quantum materials at low temperatures.

Ni, Haoyang↗

DOE OSTI2025

Quantitative approaches for multiscale structural analysis with atomic resolution electron microscopy

Atomic-resolution imaging with scanning transmission electron microscopy is a powerful tool for characterizing the nanoscale structure of materials, in particular features such as defects, local strains, and symmetry-breaking distortions. In addition to advanced instrumentation, the effectiveness of the technique depends on computational image analysis to extract meaningful features from complex datasets recorded in experiments, which can be complicated by the presence of noise and artifacts, small or overlapping features, and the need to scale analysis over large representative areas. Here, we present image analysis approaches which synergize real and reciprocal space information to efficiently and reliably obtain meaningful structural information with picometer scale precision across hundreds of nanometers of material from atomic-resolution electron microscope images. Damping superstructure peaks in reciprocal space allows symmetry-breaking structural distortions to be disentangled from other sources of inhomogeneity and measured with high precision. Real-space fitting of the wavelike signals resulting from Fourier filtering enables absolute quantification of lattice parameter variations and strain, as well as the uncertainty associated with these measurements. Implementations of these algorithms are made available as an open source python package.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Capturing 3D atomic defects and phonon localization at the 2D heterostructure interface

The three-dimensional (3D) local atomic structures and crystal defects at the interfaces of heterostructures control their electronic, magnetic, optical, catalytic, and topological quantum properties but have thus far eluded any direct experimental determination. Here, we use atomic electron tomography to determine the 3D local atomic positions at the interface of a MoS 2 -WSe 2 heterojunction with picometer precision and correlate 3D atomic defects with localized vibrational properties at the epitaxial interface. We observe point defects, bond distortion, and atomic-scale ripples and measure the full 3D strain tensor at the heterointerface. By using the experimental 3D atomic coordinates as direct input to first-principles calculations, we reveal new phonon modes localized at the interface, which are corroborated by spatially resolved electron energy-loss spectroscopy. We expect that this work will pave the way for correlating structure-property relationships of a wide range of heterostructure interfaces at the single-atom level.

42 ENGINEERING↗

DOE OSTI2020

Giant piezoelectricity in oxide thin films with nanopillar structure

High-performance piezoelectric materials are critical components for electromechanical sensors and actuators. For more than 60 years, the main strategy for obtaining large piezoelectric response has been to construct multiphase boundaries, where nanoscale domains with local structural and polar heterogeneity are formed, by tuning complex chemical compositions. We used a different strategy to emulate such local heterogeneity by forming nanopillar regions in perovskite oxide thin films. We obtained a giant effective piezoelectric coefficient d 33 , f * of ~1098 picometers per volt with a high Curie temperature of ~450°C. Our lead-free composition of sodium-deficient sodium niobate contains only three elements (Na, Nb, and O). The formation of local heterogeneity with nanopillars in the perovskite structure could be the basis for a general approach to designing and optimizing various functional materials.

Science & Technology - Other Topics↗

DOE OSTI2022

Relaxor ferroelectric polymer exhibits ultrahigh electromechanical coupling at low electric field

Electromechanical (EM) coupling—the conversion of energy between electric and mechanical forms—in ferroelectrics has been used for a broad range of applications. Ferroelectric polymers have weak EM coupling that severely limits their usefulness for applications. Here, we introduced a small amount of fluorinated alkyne (FA) monomers (<2 mol %) in relaxor ferroelectric poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene) (PVDF-TrFE-CFE) terpolymer that markedly enhances the polarization change with strong EM coupling while suppressing other polarization changes that do not contribute to it. Under a low–dc bias field of 40 megavolts per meter, the relaxor tetrapolymer has an EM coupling factor (k 33 ) of 88% and a piezoelectric coefficient (d 33 ) >1000 picometers per volt. These values make this solution-processed polymer competitive with ceramic oxide piezoelectrics, with the potential for use in distinct applications.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Quantum critical electro-optic and piezo-electric nonlinearities

Although electro-optic (EO) nonlinearities are essential for many quantum and classical photonics applications, a major challenge is inefficient modulation in cryogenic environments. Guided by the connection between phase transitions and nonlinearity, we identify the quantum paraelectric perovskite SrTiO 3 as a strong cryogenic EO [>500 picometers per volt (pm/V)] and piezo-electric material (>90 picocoulombs per newton) at T = 5 K, at frequencies to at least 1 megahertz. Furthermore, by tuning SrTiO 3 toward quantum criticality, we more than double the EO and piezo-electric effects, demonstrating a linear Pockels coefficient above 1000 pm/V. Furthermore, our results probe the link between quantum phase transitions, dielectric susceptibility, and nonlinearity, unlocking opportunities in cryogenic optical and mechanical systems and providing a framework for discovering new nonlinear materials.

Anderson, Christopher P. [Stanford University, CA ↗

DOE OSTI2022

Heterodyne spectrometer sensitivity limit for quantum networking

We report optical heterodyne detection-based spectrometers are attractive due to their relatively simple construction and ultrahigh resolution. Here we demonstrate a proof-of-principle single-mode optical-fiber-based heterodyne spectrometer that has picometer resolution and quantum-limited sensitivity around 1550 nm. Moreover, we report a generalized quantum limit of detecting broadband multispectral-temporal-mode light using heterodyne detection, which provides a sensitivity limit on a heterodyne detection-based optical spectrometer. We then compare this sensitivity limit to several spectrometer types and dim light sources of interest such as spontaneous parametric downconversion, Raman scattering, and spontaneous four-wave mixing. We calculate that the heterodyne spectrometer is significantly less sensitive than a single-photon detector and is unable to detect these dim light sources, except for the brightest and narrowest-bandwidth examples.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Sensitivity Limitation of an Optical Heterodyne Spectrometer

We show an optical heterodyne spectrometer with picometer resolution and high sensitivity. Moreover, we report the quantum limit of detecting multi-mode light using heterodyne detection, and compare it to a typical down conversion source output.

Chapman, Joseph↗

DOE OSTI2025

Compare low-gain 1D and 3D models toward a storage ring-based X-ray free-electron-laser oscillator

Fourth-generation diffraction-limited synchrotron light sources (DL-SLS) present a compelling platform for advanced light source applications due to their ultra-low emittance (around tens of picometers), sub-micrometer beam stability, and high repetition rates (greater than 1 MHz). Despite these advantages, fundamental limitations, such as long bunch durations (tens of picoseconds), large relative energy spread (~10⁻³), and low peak current (<300 A), have hindered their effectiveness in free-electron laser (FEL) applications. Using a low-gain three-dimensional (3D) model based on NSLS-II upgrade lattice parameters, we demonstrate that a 6% single-pass gain is achievable with an optimized transverse gradient undulator (TGU). Concurrently, recent advances in X-ray optics—specifically, a four-mirror bow-tie resonator utilizing diamond mirrors and beryllium compound refractive lenses (CRLs)—enable total round-trip losses below 4% and an output coupling efficiency near 1%, rendering a Storage Ring based X-ray FEL oscillator (XFELO) a realistic possibility. In the 3D framework, the TGU effectively mitigates the detrimental effects of large energy spread by spatially dispersing the beam, leading to enhanced gain relative to conventional one-dimensional (1D) models. We establish both analytical and numerical connections between the 1D and 3D descriptions, leveraging GENESIS simulations to map equivalent gain conditions. While 1D resonance is defined in the energy domain, the 3D TGU system shifts the resonance dependence to transverse gradient and dispersion parameters. Once optimized, this framework allows predictive modeling using 1D formulas, which can then be validated through full 3D simulations.

43 PARTICLE ACCELERATORS↗

DOE OSTI2025

Enhanced Monte Carlo Simulations for Electron Energy Loss Mitigation in Real-Space Nanoimaging of Thick Biological Samples and Microchips

High-resolution imaging using Transmission Electron Microscopy (TEM) is essential for applications such as grain boundary analysis, microchip defect characterization, and biological imaging. However, TEM images are often compromised by electron energy spread and other factors. In TEM mode, where the objective and projector lenses are positioned downstream of the sample, electron–sample interactions cause energy loss, which adversely impacts image quality and resolution. This study introduces a simulation tool to estimate the electron energy loss spectrum (EELS) as a function of sample thickness, covering electron beam energies from 300 keV to 3 MeV. Leveraging recent advances in MeV-TEM/STEM technology, which includes a state-of-the-art electron source with 2-picometer emittance, an energy spread of 3 × 10 -5 , and optimized beam characteristics, we aim to minimize energy spread. By integrating EELS capabilities into the BNL Monte Carlo (MC) simulation code for thicker samples, we evaluate electron beam parameters to mitigate energy spread resulting from electron–sample interactions. Based on our simulations, we propose an experimental procedure for quantitively distinguishing between elastic and inelastic scattering. The findings will guide the selection of optimal beam settings, thereby enhancing resolution for nanoimaging of thick biological samples and microchips.

36 MATERIALS SCIENCE↗

NASA NTRS1999

Laser Interferometer Space Antenna (LISA) Far Field Phase Patterns

The Laser Interferometer Space Antenna (LISA) for the detection of Gravitational Waves is a very long baseline interferometer, which will measure the changes in the distance of a five million kilometer arm to picometer accuracies. Knowledge of the phase deviations from a spherical wave and what causes these deviations are needed considerations in (as a minimum) the design of the telescope and in determining pointing requirements. Here we will present the far field phase deviations from a spherical wave for given Zernike aberrations of the exit pupil and discuss how these results affect the choice of a telescope design.

Waluschka, Eugene↗

NASA NTRS2000

SIM Configuration Evolution

The Space Interferometry Mission (SIM) is a space-based 10 m baseline Michelson interferometer. Planned for launch in 2005 aboard a Delta III launch vehicle, or equivalent, its primary objective is to measure the positions of stars and other celestial objects with an unprecedented accuracy of 4 micro arc seconds. With such an instrument, tremendous advancement can be expected in our understanding of stellar and galactic dynamics. Using triangulation from opposite sides of the orbit around the sun (i.e. by using parallax) one can measure the distance to any observable object in our galaxy. By directly measuring the orbital wobble of nearby stars, the mass and orbit of planets can be determined over a wide range of parameters. The distribution of velocity within nearby galaxies will be measurable. Observations of these and other objects will improve the calibration of distance estimators by more than an order of magnitude. This will permit a much better determination of the Hubble Constant as well as improving our overall understanding of the evolution of the universe. SIM has undergone several transformations, especially over the past year and a half since the start of Phase A. During this phase of a project, it is desirable to perform system-level trade studies, so the substantial evolution of the design that has occurred is quite appropriate. Part of the trade-off process has addressed two major underlying architectures: SIM Classic; and Son of SIM. The difference between these two architectures is related to the overall arrangement of the optical elements and the associated metrology system. Several different configurations have been developed for each architecture. Each configuration is the result of design choices that are influenced by many competing considerations. Some of the more important aspects will be discussed. The Space Interferometry Mission has some extremely challenging goals: millikelvin thermal stability, nanometer stabilization of optics, picometer measurement of wavefront, and others. In order to meet these goals, a significant amount of technological development is required. Although there has been a program operating for about a decade developing technologies specifically to address the challenges of space-based interferometry, there still remains a tremendous effort to achieve the incredible accuracy required of SIM. The projected viability of some of these areas has influenced design choices during the evolution of the many configurations that have been developed. For instance, the perceived complexity of the IR laser metrology system used to measure and control the positions of key optical elements was the strongest discriminator between the two architectures, and led to a decision to select SOS rather than Classic in early 1998. More recently, an appreciation of the sensitivity to beam-walk within the SOS architecture is forcing a reconsideration of that decision. At the time of submission of this abstract, there is some hope that a full-aperture metrology system may alleviate this issue. In addition to describing the current configuration of SIM, the influence of a few selected areas on the evolution of the configuration will be discussed.

Aaron, Kim M.↗

NASA NTRS2001

MEMS Memory Elements

This paper presents a design example that illustrates the potential of microelectromechanical systems (MEMS) to perform the mechanical positioning required for addressing stored data and to enable an entirely new mechanism for reading and writing magnetic data. Specifically, MEMS sensors and actuators can be used to achieve active servo control of the separation between magnetic probe tips and a media surface with sub-nanometer accuracy. This allows mechanical position to be used to selectively write magnetic marks in a continuous thin-film magnetic media. In addition, MEMS sensors can be used to measure the separation between a magnetic probe tip and the media with a noise floor of roughly 22 picometers, allowing them to be used as position sensors in a magnetic force microscope (MFM) style data detection system.

Carley, L. Richard↗

NASA NTRS2002

LISA Optics Model

The LISA experiment has six telescopes, in three spacecraft, in orbit about the sun. There is a continuous laser link between all of the spacecraft. Because of the large, 5 million kilometer distances, between the spacecraft and the need to perform picometer level interferometry and the fact that the optical system is dynamic precludes the use of standard optical codes in the design and analysis of this optical system. A detailed description of the approach used to model all of the optics, in the spacecraft in orbit, is presented and the ability of this model to analyze requirements is discussed. A dynamic computer simulation will be shown to illustrate the laser link and the effects of this dynamic environment on the interferometry.

Waluschka, Eugene↗

NASA NTRS2002

LISA Telescope Sensitivity Analysis

The Laser Interferometer Space Antenna (LISA) for the detection of Gravitational Waves is a very long baseline interferometer which will measure the changes in the distance of a five million kilometer arm to picometer accuracies. As with any optical system, even one with such very large separations between the transmitting and receiving, telescopes, a sensitivity analysis should be performed to see how, in this case, the far field phase varies when the telescope parameters change as a result of small temperature changes.

Waluschka, Eugene↗

NASA NTRS2003

Precision Pointing for the Laser Interferometry Space Antenna Mission

The Laser Interferometer Space Antenna (LISA) mission is a planned NASA-ESA gravitational wave detector consisting of three spacecraft in heliocentric orbit. Lasers are used to measure distance fluctuations between proof masses aboard each spacecraft to the picometer level over a 5 million kilometer separation. Each spacecraft and its two laser transmit/receive telescopes must be held stable in pointing to less than 8 nanoradians per root Hertz in the frequency band 0.1-100 mHz. The pointing error is sensed in the received beam and the spacecraft attitude is controlled with a set of micro-Newton thrusters. Requirements, sensors, actuators, control design, and simulations are described.

Hyde, T. Tupper↗

NASA NTRS2002

LISA Optics Model

The Laser Interferometer Space Antenna (LISA) experiment has six telescopes, in three spacecraft, in orbit about the sun. There is a continuous two-way laser link between all of the spacecraft. The ability to make sub picometer level performance predictions about the interferometry for such a large optical system which has major subassemblies separated by 5 million kilometer distances which are constantly moving with respect to each other requires a slight extension of existing optical analysis techniques. To see this a description of the approach used to model all of the optics, in the spacecraft in orbit, is presented and the ability of this model to analyze requirements is discussed.

Waluschka, Eugene↗

NASA NTRS2003

Precision Pointing for the Laser Interferometry Space Antenna Mission

Hyde, T. Tupper↗