Atomic Images Research Articles

Energetic neutral atom imaging reveals nearly 11-year cycle of the ring current of Saturn

The drift motion of energetic charged particles can generate an azimuthal electric current around the planet known as the ring current, which regulates the field configuration of the magnetosphere. However, limited coverage of in-situ measurements makes it challenging to investigate the long-term variations of the global ring current. Taking advantage of the energetic neutral atom (ENA) imaging onboard the Cassini mission, we present a nearly 11-year cycle of the suprathermal ring current populations in Saturn’s magnetosphere. We find that the peak location of the suprathermal ring current in local time oscillates between post-midnight and pre-midnight sectors, and its intensity minimizes during the solar maximum. These results indicate that the modulation of the suprathermal ring current is closely related to the solar cycle. Our analysis also offers a preview of the ring current at other giant planets, such as Jupiter, which will be imaged by ENA cameras onboard the JUICE mission.

Discrimination of thrombus types in ischemic stroke using Dual-Energy CT

ObjectiveThis study explores the clinical utility of dual-energy computed tomography (DECT) in discriminating thrombus types in ischemic stroke. MethodsPatients with acute ischemic stroke who underwent brain DECT non-contrast scanning and brain CT perfusion (CTP) before thrombectomy were included, and the thrombus composition was analyzed by postoperative pathology. DECT data was conducted to reconstruct polychromatic images and effective atomic number images. Computed tomography (CT) values, effective atomic numbers, and spectral curve slopes of the thrombus were measured and calculated. Thrombus attenuation increase was obtained from CTP data. Parameters were compared between red blood cell (RBC)-dominant thrombi and fibrin/platelet (F/P)-dominant thrombi. Thresholds, sensitivity, specificity, and area under the curve (AUC) were analyzed to distinguish these thrombi. The associations between DECT parameters and proportion of RBCs were analyzed by Spearman’s correlation. ResultsPathological analysis of 42 enrolled patients revealed 24 cases of RBC-dominant thrombi and 18 cases of F/P-dominant thrombi. Effective atomic numbers, spectral curve slopes, and polychromatic images CT values were significantly higher in the RBC-dominant thrombi group compared with the F/P-dominant thrombi group. Although the average thrombus attenuation increase was greater in the F/P-dominant thrombi group, this difference was not statistically significant. Among the DECT parameters, polychromatic images CT values had the greatest AUC at 0.924 (0.848–0.999) for discriminating RBC-dominant and F/P-dominant thrombi, with a threshold of 59 HU, sensitivity of 79.2 %, and specificity of 94.4 %. The combined diagnostic AUC reached 0.938 (0.863–1.012), with 87.5 % sensitivity and 94.4 % specificity. DECT polychromatic images CT values, effective atomic numbers, and spectral curve slopes were significantly correlated with proportion of RBCs (r = 0.673, 0.574, and 0.571, all p < 0.01). ConclusionDECT non-contrast scan parameters are associated with thrombus composition, which could be effective in distinguishing between RBC-dominant and F/P-dominant thrombi.

Enhanced Bulk Photovoltaic Effect of Single-Domain Freestanding BiFeO3 Membranes.

The bulk photovoltaic effect (BPVE), which uniquely exists in non-centrosymmetric materials, has been received extensive attention recently due to its potential to overcome the theoretical Shockley-Queisser limit in traditional p-n junction solar cells. Here, freestanding single-domain BiFeO3 membranes are exfoliated from miscut SrTiO3 substrates by dissolving Sr3Al2O6 sacrificial layers, and transferred on SiO2/Si substrates. This study finds that the freestanding BiFeO3 membranes maintain the single-domain structure and exhibits the significantly enhanced bulk photovoltaic response (≈200% enhancement), compared to the strained BiFeO3 films. The comprehensive atomic imaging analyses manifest that the freestanding BiFeO3 membrane demonstrates the bigger noncentral ion (Fe) displacement, which results in the larger in-plane ferroelectric polarization and substantial increase in the BPVE photocurrent. This work not only provides an effective approach to enhance the BPVE of ferroelectric oxide films, but also can potentially promote the exploration of BPVE of oxide membranes integrated with silicon-based or 2D electronics.

Seebeck Coefficient Modulation of Graphene Grown on Faceted Cu Surfaces

The thermoelectric properties of polycrystalline copper (Cu) surfaces partially covered with graphene grown by Joule‐heating chemical vapor deposition using scanning thermoelectric microscopy are investigated. Atomic‐resolution atomic force microscopy topographic images of graphene grown on Cu(100) surfaces showed a 1D stripe pattern of Moiré superlattices, while thermoelectric voltage images clearly distinguish wrinkle defects caused by thermal mismatch between graphene and Cu substrate. Regions of different signs were found in the thermoelectric voltage image of the graphene island, which are attributed to the faceted surface of the Cu substrate. In addition, faceted surfaces consisting of low‐ and high‐index Cu surfaces are formed on the Cu grain to minimize the surface energy. Due to these structural changes, charge transfer and chemical interactions at the interface between the graphene and Cu facets affect the electronic structure of the graphene, which is understood as the observed Seebeck coefficients with different signs in the thermoelectric microscopy measurements, which are sensitive to the local density of states.

Deep Learning Enhanced in Situ Atomic Imaging of Ion Migration at Crystalline-Amorphous Interfaces.

Improving the performance of energy storage, neuromorphic computing, and more applications requires an in-depth understanding of ion transport at interfaces, which are often hindered by facile atomic reconfiguration at working conditions and limited characterization capability. Here, we construct an in situ double-tilt electric manipulator inside an aberration-corrected scanning transmission electron microscope. Coupled with deep learning-based image enhancement, atomic images are enhanced 3-fold compared to traditional methods to observe the potassium ion migration and microstructure evolution at the crystalline-amorphous interface in antimony selenide. Potassium ions form stable anisotropic insertion sites outside the (Sb4Se6) chain, with a few potassium ions present within the moieties. Combined experiments and density functional theory calculations reveal a reaction pathway of forming a novel metastable state during potassium ion insertion, followed by recovery and unexpected chirality changes at the interface upon potassium ion extraction. Our unique methodology paves the way for facilitating the improvement and rational design of nanostructured materials.

Atomic force microscopy wide-field scanning imaging using homography matrix optimization

During the offline combination of multiple atomic force microscopy (AFM) images, changes in probe displacement can be affected by dynamic noise, leading to dislocation and tearing in the stitching. To overcome this, we designed a homography matrix optimization method to describe the relative positional relationship between images by constructing the original image matrix and applying singular value decomposition to denoise the homography matrix. Additionally, we implemented a scale-invariant feature transform (SIFT) to extract feature points. To verify the effectiveness of this method, the SIFT + RANSAC (R), SIFT + affine transformation (AT), and oriented FAST and rotated BRIEF (ORB) algorithms were compared with the proposed algorithm. The experimental results demonstrate that the proposed method precisely computes the transformation matrix, thereby guaranteeing the geometric consistency of mosaic imaging. The proposed method preserves the intricate details of the original image and enhances the stitching quality of wide-field images.

Synthesis, characterization and corrosion inhibition evaluation of a new chalcone derivative 2-3-(3-hydroxyphenyl)-1-[4-(1H-imidazol-1-yl) phenyl] prop-2-en-1-one for mild steel corrosion in 1M HCl assessment with DFT and MD studies

The prime objective of the work focuses on the synthesis of novel chalcone derivative, the 2-3-(3-hydroxyphenyl)-1-[4-(1H-imidazol-1-yl) phenyl] prop-2-en-1-one (HIPP) and study its corrosion inhibition for mild steel in 1M HCl. Various spectroscopic techniques such as IR, 1H-NMR, 13C-NMR, and mass spectroscopy were used to confirm the formation of the synthesized chalcone. Distinct electrochemical techniques like potentiodynamic Tafel polarization and impedance spectroscopy were employed to investigate HIPP in 1M HCl as a mild steel corrosion inhibitor. The synthesized chalcone was checked in a temperature range varying from 30° C to 60° C. With increasing quantities of HIPP, it is noticed that there is an enhancement in calculated corrosion inhibition efficiency. The maximum inhibition efficiency obtained was found to be 94.3 % in the presence of 100 ppm at room temperature. Surface morphology of unhindered and inhibited HIPP was analysed using scanning electron microscopy (SEM), atomic force microscopy (AFM) and water contact angle (WCA) measurements. SEM investigation revealed that the inhibitor effectively protects the metal surface from aggressive corrosion. Atomic force microscopic images show the corroded MS surface roughness in the presence of HIPP reduced from 342.1 nm to 174.3 nm. Furthermore, the inhibitor's adsorption through electron-donor acceptor interactions was revealed by DFT calculations and MD studies.

Perspective: imaging atomic step geometry to determine surface terminations of kagome materials and beyond

Here we review scanning tunneling microscopy research on the surface determination for various types of kagome materials, including 11-type (CoSn, FeSn, FeGe), 32-type (Fe3Sn2), 13-type (Mn3Sn), 135-type (AV3Sb5, A = K, Rb, Cs), 166-type (TbMn6Sn6, YMn6Sn6 and ScV6Sn6), and 322-type (Co3Sn2S2 and Ni3In2Se2). We first demonstrate that the measured step height between different surfaces typically deviates from the expected value of ±0.4 ∼0.8Å, which is owing to the tunneling convolution effect with electronic states and becomes a serious issue for Co3Sn2S2 where the expected Sn-S interlayer distance is 0.6Å. Hence, we put forward a general methodology for surface determination as atomic step geometry imaging, which is fundamental but also experimentally challenging to locate the step and to image with atomic precision. We discuss how this method can be used to resolve the surface termination puzzle in Co3Sn2S2. This method provides a natural explanation for the existence of adatoms and vacancies, and beyond using unknown impurity states, we propose and use designer layer-selective substitutional chemical markers to confirm the validity of this method. Finally, we apply this method to determine the surface of a new kagome material Ni3In2Se2, as a cousin of Co3Sn2S2, and we image the underlying kagome geometry on the determined Se surface above the kagome layer, which directly visualizes the p-d hybridization physics. We emphasize that this general method does not rely on theory, but the determined surface identity can provide guidelines for first-principles calculations with adjustable parameters on the surface-dependent local density of states and quasi-particle interference patterns.

Growth Mechanism of Carbon Nanotubes Revealed by in situ Transmission Electron Microscopy.

Elucidating the growth mechanism of carbon nanotubes (CNTs) is critical to obtaining CNTs with desired structures and tailored properties for their practical applications. With atomic resolution imaging, in situ transmission electron microscopy (TEM) has been a key technique to reveal the microstructure and dynamics of CNTs in real time. In this review, recent advances in the development of in situ TEM with different types of environmental reactors will be introduced. The catalytic growth mechanisms of CNTs revealed by in situ TEM under realistic conditions are discussed from fundamental thermodynamics and kinetics to the detailed nucleation, growth, and termination mechanisms, including the state and phase of active catalysts, interfacial connections between catalyst and growing CNTs, and catalyst-related growth kinetics of CNTs. Great progresses have been made on how a CNT nucleates, grows and terminates, focusing on the interface dynamics and kinetic fluctuations. Finally, challenges and future directions for understanding the atomic dynamics under the real growth conditions are proposed. It is expected that breakthroughs in the fundamental growth mechanisms will pave the way to the ultimate goal of designing and controlling the atomic structures of CNTs for their applications in various devices.

Surface sensitivity of atomic resolution secondary electron imaging

Surface sensitivity of atomic resolution secondary electron imaging

Quadrupole Coupling of Circular Rydberg Qubits to Inner Shell Excitations.

Divalent atoms provide excellent means for advancing control in Rydberg atom-based quantum simulation and computing due to the second optically active valence electron available. Particularly promising in this context are circular Rydberg atoms, for which long-lived ionic core excitations can be exploited without suffering from detrimental autoionization. Here, we report the implementation of electric quadrupole coupling between the metastable 4D_{3/2} level and a very high-n (n=79) circular Rydberg qubit, realized in doubly excited ^{88}Sr atoms prepared from an optical tweezer array. We measure the kHz-scale differential level shift on the circular Rydberg qubit via beat-node Ramsey interferometry comprising spin echo. Observing this coupling requires coherent interrogation of the Rydberg states for more than 100 μs, which is assisted by tweezer trapping and circular state lifetime enhancement in a black-body radiation suppressing capacitor. Further, we find no noticeable loss of qubit coherence under continuous photon scattering on the ion core, paving the way for laser cooling and imaging of Rydberg atoms. Our results demonstrate access to weak electron-electron interactions in Rydberg atoms and expand the quantum simulation toolbox for optical control of highly excited circular state qubits via ionic core manipulation.

Piezo tube stacked scanning tunneling microscope for use in extreme and confined environments

Scanning Tunneling Microscopy (STM) is widely used for observing atomic structures due to its ultra-high spatial resolution. As the core units of STM, the coarse stepper motor and imaging unit, have conflicting size requirements for piezo tubes. Longer piezo tubes yield greater output force and easier movement for the motor, while shorter tubes enhance imaging precision and stability for the scanner. Traditional STMs typically employ a large piezo tube for coarse stepping and a smaller one for independent imaging to address this issue. Here, we present the new design of a piezo tube stacked STM, in which two independent piezo tubes act together during tip-sample approach process and only one shorter tube works during scanning imaging. Both tubes are fixed to the framework, ensuring high rigidity and compactness. The new design enables us to achieve both coarse stepping and imaging functions with a total length of only 25 mm for the two tubes, effectively reducing the length of whole STM, facilitating its integration into narrow low-temperature spaces for imaging applications. Using this device, we obtained high-quality atomic images of graphite sample surfaces at room temperature. Continuous scanning imaging of the same area on Au film at 300 K demonstrates the STM’s high stability in both X-Y and Z directions. Atomic images, I-V spectra, and di/dv spectra obtained at 2 K on graphite surface illustrate the excellent application potential of this device in low-temperature environments. Finally, atomic images obtained of graphite in sweeping the magnetic fields from 0 T to 11 T in a huge vibrational dry magnet prove the new STM’s excellent performance in extreme conditions.

Investigation on Junction Contacts of Semiconducting Carbon Nanotube Networks Using Conductive Atomic Force Microscopy.

Semiconductor single-walled carbon nanotube (s-SWNT) networks have gained prominence in electronic devices due to their cost-effectiveness, relatively production-naturality, and satisfactory performance. Configuration, density, and resistance of SWNT-SWNT junctions are considered crucial factors influencing the overall conductivity of s-SWNT networks. In this study, we present a method for inferring the lower bounds of the SWNT-SWNT junction resistance in s-SWNT networks based on conductive atomic force microscopy TUNA images. This method further enables the proposal of a classification for SWNT-SWNT junctions based on the current behavior relative to their surroundings. The three types of SWNT-SWNT junctions are denoted as (i) true contact (T), (ii) poor contact (P), and (iii) false contact (F). Of them, the true and poor contacts, respectively, represent good and poor electrical contact for the subject SWNT-SWNT junctions whose electrical conductivity hardly improves under external tip pressure, while that of the false contact can be further improved by external pressure. Statistical analysis demonstrates that while T-type junctions make a significant contribution to network conductivity, their proportion accounts for only approximately 40%. The P-type and F-type junctions, which constitute over 60% of the total, may be a contributing factor that constrains the overall conductivity of the s-SWNT networks. The height ratio of the junction to the sum of two SWNTs was also observed to exhibit variations among the three types. Finally, we propose a three-dimensional model to elucidate the formation mechanism underlying each type of junction. The present study provides insights into the performance of spontaneous contacts between s-SWNTs in the networks, and the systematic image acquisition and junction classification processes may provide support for future advancements in these networks.

Real-Space Tilting Method for Atomic Resolution STEM Imaging of Nanocrystalline Materials.

Atomic-resolution scanning transmission electron microscopy (STEM) characterization requires precise tilting of the specimen to a high symmetric zone axis, which is usually processed in reciprocal space by following the diffraction patterns. However, for small-sized nanocrystalline materials, their diffraction patterns are often too faint to guide the tilting process. Here, a simple and effective tilting method is developed based on the diffraction contrast change of the shadow image in the Ronchigram. The misorientation angle of the specimen can be calculated and tilted to the zone axis based on the position of the shadow image with lowest intensity. This method requires no prior knowledge of the sample and the maximum misorientation angle that can be corrected is >±6.9° with sub-mrad accuracy. It operates in real space, without recording the diffraction patterns of the specimens, making it particularly effective for nanocrystalline materials. Combined with the scripting to control the microscope, the sample can be automatically tilted to the zone axis under low dose conditions (<0.17 e-Å- 2s-1), facilitating the imaging of beam sensitive materials such as zeolites or metal-organic frameworks. This automated tilting method can significantly contribute to the atomic-scale characterization of the nanocrystalline materials by STEM imaging.

Atomic resolution scanning transmission electron microscopy at liquid helium temperatures for quantum materials

Fundamental quantum phenomena in condensed matter, ranging from correlated electron systems to quantum information processors, manifest their emergent characteristics and behaviors predominantly at low temperatures. This necessitates the use of liquid helium (LHe) cooling for experimental observation. Atomic resolution scanning transmission electron microscopy combined with LHe cooling (cryo-STEM) provides a powerful characterization technique to probe local atomic structural modulations and their coupling with charge, spin and orbital degrees-of-freedom in quantum materials. However, achieving atomic resolution in cryo-STEM is exceptionally challenging, primarily due to sample drifts arising from temperature changes and noises associated with LHe bubbling, turbulent gas flow, etc. In this work, we demonstrate atomic resolution cryo-STEM imaging at LHe temperatures using a commercial side-entry LHe cooling holder. Firstly, we examine STEM imaging performance as a function of He gas flow rate, identifying two primary noise sources: He-gas pulsing and He-gas bubbling. Secondly, we propose two strategies to achieve low noise conditions for atomic resolution STEM imaging: either by temporarily suppressing He gas flow rate using the needle valve or by acquiring images during the natural warming process. Lastly, we show the applications of image acquisition methods and image processing techniques in investigating structural phase transitions in Cr2Ge2Te6, CuIr2S4, and CrCl3. Our findings represent an advance in the field of atomic resolution electron microscopy imaging for quantum materials and devices at LHe temperatures, which can be applied to other commercial side-entry LHe cooling TEM holders.

Development of a liquid-helium free cryogenic sample holder with mK temperature control for autonomous electron microscopy

The automated and autonomous cryogenic transmission electron microscopy (Cryo-EM) demands a sample holder capable of maintaining temperatures below 10 K with precise control, long holding times, and minimal helium use. Rising to this challenge, we initiated an ambitious project to develop a novel closed-cycle cryocooler-based cryogenic sample holder that operates without the use of liquid helium and the consumption of gaseous helium. This article presents the design, construction, and experimental testing of the initial prototype, which achieves an ultimate temperature of 5.6 K with exceptional stability close to 1mK, while providing a wide temperature control range from 295 K to 5.6 K, marking a clear advancement in cryo-EM holder development. While the prototype was not designed for atomic resolution imaging and thus lacks a sturdy support system to mitigate mechanical vibrations from the cryocooler's pulsed tube, this innovative approach successfully demonstrates proof of concept. It offers unprecedented capabilities for state-of-the-art cryogenic microscopy and microanalysis in materials and biological sciences.

Detailed structural analyses and viscoelastic properties of nano-fibrillated bacterial celluloses

Nano-fibrillated bacterial cellulose (NFBC) can be prepared by cultivating a cellulose-producing bacterium in a medium containing a dispersant under agitating and aerobic conditions. Although NFBCs have various applications, their detailed structure and physical properties have not been clarified. Therefore, in this study, we performed detailed structural and physical property analyses of NFBCs to advance their potential applications. Atomic force microscopy and image analysis showed that the average fiber length of NFBCs was approximately 17 µm and fiber widths were 10–15 nm; the aspect ratios of NFBCs were > 1000, which are >10-fold higher than that of 2,2,6,6-tetramethylpioeridine-1-oxyl-oxidized cellulose nanofiber. Shear viscosity measurements showed that the NFBCs exhibited shear-thinning flow behavior even at low concentrations (0.01 wt%). Frequency sweep measurements showed that the storage modulus values were greater than the loss modulus values in the measured frequency range, indicating that the NFBCs were in a stable gel state. Thus, the NFBCs exhibited significantly longer fiber lengths, larger aspect ratios, and excellent viscoelastic properties based on these unique structural features. Our findings will help develop novel applications utilizing the ultrahigh aspect ratio unique to NFBC and its viscoelastic properties.

Merging Mesoscale Magnetotail Features and Ground B‐Field Perturbation Network Connectivity During Substorm Activity

AbstractThe connection between the magnetosphere and ionosphere is particularly dynamic during substorms. Mesoscale features in the magnetotail are consistent with substorm activity, including magnetic reconnection in the tail, flow channels, and particle injections. Observations of substorm related phenomena can be made using energetic neutral atom (ENA) imagers, in situ satellite measurements, and ground based magnetic field perturbation measurements. Analysis of the 10 October 2014 isolated substorm event is presented. Comparison of the spatial and temporal dynamics of the features seen in equatorial maps generated from ENA data are made with inner magnetosphere in situ measurements and ionospheric features with network analysis of the SuperMAG data. An MHD simulation of the event using OpenGGCM is also compared with the data.

Engineering Novel Amphiphilic Platinum(IV) Complexes to Co-Deliver Cisplatin and Doxorubicin.

In this study, we report a novel platinum-doxorubicin conjugate that demonstrates superior therapeutic indices to cisplatin, doxorubicin, or their combination, which are commonly used in cancer treatment. This new molecular structure (1) was formed by conjugating an amphiphilic Pt(IV) prodrug of cisplatin with doxorubicin. Due to its amphiphilic nature, the Pt(IV)-doxorubicin conjugate effectively penetrates cell membranes, delivering both cisplatin and doxorubicin payloads intracellularly. The intracellular accumulation of these payloads was assessed using graphite furnace atomic absorption spectrometry and fluorescence imaging. Since the therapeutic effects of cisplatin and doxorubicin stem from their ability to target nuclear DNA, we hypothesized that the amphiphilic Pt(IV)-doxorubicin conjugate (1) would effectively induce nuclear DNA damage toward killing cancer cells. To test this hypothesis, we used flow the cytometric analysis of phosphorylated H2AX (γH2AX), a biomarker of nuclear DNA damage. The Pt(IV)-doxorubicin conjugate (1) markedly induced γH2AX in treated MDA-MB-231 breast cancer cells, showing higher levels than cells treated with either cisplatin or doxorubicin alone. Furthermore, MTT cell viability assays revealed that the enhanced DNA-damaging capability of complex 1 resulted in superior cytotoxicity and selectivity against human cancer cells compared to cisplatin, doxorubicin, or their combination. Overall, the development of this amphiphilic Pt(IV)-doxorubicin conjugate represents a new form of combination therapy with improved therapeutic efficacy.

The Deposition of Lead on a Pt(100) Electrode and the Effects on the Oxidation of Formic Acid

The electrodeposition of foreign metals on a platinum (Pt) electrode can be used to alter the electrochemical properties of the modified electrode. The current study employed in situ scanning tunneling microscopy (STM) to characterize the spatial structures of a monolayer and multilayer lead (Pb) electrodeposited on an ordered Pt(100) electrode in 0.1 M perchloric acid (HClO4) with and without formic acid under potential control. The Pt(100) bead crystal used in this study was pretreated by a modified annealing and quenching method, producing a long-range ordered, unreconstructed (1 × 1) surface. The underpotential deposition (UPD) of Pb on the Pt(100) electrode resulted in a pair of sharp and reversible peak at 0.5 V (vs. Ag/AgCl), prior to the bulk deposition at E < -0.45 V in 0.1 M HClO4 + 1 mM Pb(ClO4)2. Cyclic potential sweeping in the UPD regimes resulted in a stable voltammogram, but bulk Pb deposition led to varying morphologies of the profiles. Atomic resolution STM images were obtained to reveal a well-ordered Pt(100)-(√2 × √2)R45°-Pb structure and elongated rows of Pb aggregates and local (√2 × 2√2) R45° in the initial and final stages of Pb UPD, respectively. Bulk Pb deposition at E < -0.5 V led to a crystalline Pb film, but a roughened Pt(100) surface was imaged after the Pb deposit was anodically stripped. The activity of the Pt(100) electrode toward formic acid oxidation was nearly tripled after being modified with a sub-monolayer of Pb, and increased by another 20 % when it was loaded with multilayer Pb.