Local Probe Research Articles

A convenient approach to characterizing model uncertainty with application to early dark energy solutions of the Hubble tension

ABSTRACT Despite increasingly precise observations and sophisticated theoretical models, the discrepancy between measurements of H0 from the cosmic microwave background or from baryon acoustic oscillations combined with big bang nucleosynthesis versus those from local distance ladder probes – commonly known as the ‘H0 tension’ – continues to perplex the scientific community. To address this tension, early dark energy (EDE) models have been proposed as alternatives to Lambda cold dark matter, as they can change the observed sound horizon and the inferred Hubble constant from measurements based on this. In this paper, we investigate the use of Bayesian model averaging (BMA) to evaluate EDE as a solution to the H0 tension. BMA consists of assigning a prior to the model and deriving a posterior as for any other unknown parameter in a Bayesian analysis. BMA can be computationally challenging in that one must approximate the joint posterior of both model and parameters. Here, we present a computational strategy for BMA that exploits existing Markov chain Monte Carlo software and combines model-specific posteriors post hoc. In application to a comprehensive analysis of cosmological data sets, we quantify the impact of EDE on the H0 discrepancy. We find an EDE model probability of ${\sim} 90~{{\ \rm per\ cent}}$ whenever we include the H0 measurement from Type Ia supernovae in the analysis, whereas the other data show a strong preference for the standard cosmological model. We finally present constraints on common parameters marginalized over both cosmological models. For reasonable priors on models with and without EDE, the H0 tension is reduced by at least 20 per cent.

Fluid-structure interaction in phaco-emulsification based cataract surgery

Cataract scatters the light as it enters the eye, blurs images and severely interferes people's daily activities. The only effective therapy is cataract surgery, in which the clouded lens is phacoemulsified and removed. However, an aberrant iris distortion, namely intra-operative floppy iris syndrome (IFIS), is not uncommon in the phacoemulsification process, and it greatly degrades the surgical outcomes. Despite its great impact, the mechanism of IFIS has seldom been explored from the mechanics viewpoint. This study constitutes the first exploration into IFIS mechanism within the torsional-irrigation/aspiration (T-I/A) combined mode, from the perspective of fluid-structure coupling, employing our newly developed fluid-structure interaction (FSI) simulation framework. The impacts of several factors, including probe type and position, irrigation and aspiration (I/A), iris stiffness and lens presence, are evaluated in two different torsional-irrigation/aspiration (T-I/A) combined configurations, corresponding to the scenarios of coaxial and bimanual I/A operations. Results reveal that by altering the probe's location in anterior chamber, three distinct modes of iris dynamics are recognized and defined as repulsion (RP), attraction (AT), and adhesion (AH) modes according to the relative iris-probe location. Among them, RP mode, where the iris is repelled by the probe, is preferred to ensure the safety of the iris. Furthermore, IFIS could be alleviated by stiffening iris, reducing I/A strength and choosing coaxial I/A device. These interventions result in the contraction of the damaging AH zone towards the iris root, occurring at approximately one-fourth (coaxial case), one-fifth (coaxial case), and one-fourth of the iris length, achieved by quadrupling iris stiffness, ceasing I/A flow, and utilizing coaxial I/A device, respectively. However, the risk of IFIS is only marginally impacted by the lens presence. Our findings gain a deeper insight into the iris dynamics in T-I/A mode from fluid-iris interaction viewpoint, which may provide valuable guidance for the surgical protocol operation.

Interplay between transition-metal K-edge XMCD, slight structural distortions and magnetism in a series of trimetallic (CoxNi(1-x))4[Fe(CN)6]3/8 Prussian blue analogues.

The magnetic properties of a series of trimetallic (Co,Ni)Fe Prussian blue analogues (PBAs) were investigated by SQUID magnetometry and X-ray magnetic circular dichroism (XMCD) at the three transition metal (TM) K-edges. In turn, the PBA trimetallic series was used as a tool in order to better understand the information contained in TM K-edge XMCD and particularly the chemical nature of the probed species (extended sub-lattice or localized entities). The results show that the magnetic behavior of the compounds is dictated by competing exchange interactions between the Co-Fe and Ni-Fe pairs, without spin frustration. They also show that XMCD at the TM K-edge is a local atomic probe of the element at the N side of the cyanide bridge and a local probe of the absorbing atom and its first magnetic neighbors on the C side of the bridge. At last, XMCD at the TM K-edge turns out to be highly sensitive to very small structural distortions.

A Concept for Preoperative and Intraoperative Molecular Imaging and Detection for Assessing Extent of Disease of Solid Tumors.

The authors propose a concept of "systems engineering," the approach to assessing the extent of diseased tissue (EODT) in solid tumors. We modeled the proof of this concept based on our clinical experience with colorectal carcinoma (CRC) and gastrinoma that included short and long-term survival data of CRC patients. This concept, applicable to various solid tumors, combines resources from surgery, nuclear medicine, radiology, pathology, and oncology needed for preoperative and intraoperative assessments of a patient's EODT. The concept begins with a patient presenting with biopsy-proven cancer. An appropriate preferential locator (PL) is a molecule that preferentially binds to a cancer-related molecular target (i.e., tumor marker) lacking in non-malignant tissue and is the essential element. Detecting the PL after an intravenous injection requires the PL labeling with an appropriate tracer radionuclide, a fluoroprobe, or both. Preoperative imaging of the tracer's signal requires molecular imaging modalities alone or in combination with computerized tomography (CT). These include positron emission tomography (PET), PET/CT, single-photon emission computed tomography (SPECT), SPECT/CT for preoperative imaging, gamma cameras for intraoperative imaging, and gamma-detecting probes for precise localization. Similarly, fluorescent-labeled PLs require appropriate cameras and probes. This approach provides the surgeon with real-time information needed for R0 resection.

Determination of local pH in CO2 electroreduction.

The electrocatalytic conversion of CO2 and H2O into fuels and valuable chemicals has gained significant interest as a prospective method for the storage of renewable energy and the utilization of captured CO2. In the process of electroreduction of CO2, pH near the surface of the electrocatalysts plays an important role in the catalytic selectivity and activity. However, to elucidate the local pH effect on the fundamental reaction mechanism and modify the catalytic CO2 reduction performance, the localized pH determination method is highly desirable. In this minireview, we present the recent advances in the strategies of the local pH probe for CO2 electrolysis in both H-type cell reactors and GDE-type flow electrolyzers, followed with a better understanding of the local reaction environment in CO2 reduction. Additionally, pertinent advantages and drawbacks of the different localized pH probe techniques are discussed, and perspectives on future research efforts are also provided in this minireview.

Hamiltonian learning with real-space impurity tomography in topological moiré superconductors

Extracting Hamiltonian parameters from available experimental data is a challenge in quantum materials. In particular, real-space spectroscopy methods such as scanning tunneling spectroscopy allow probing electronic states with atomic resolution, yet even in those instances extracting the effective Hamiltonian is an open challenge. Here we show that impurity states in modulated systems provide a promising approach to extracting non-trivial Hamiltonian parameters of a quantum material. We show that by combining the real-space spectroscopy of different impurity locations in a moiré topological superconductor, modulations of exchange and superconducting parameters can be inferred via machine learning. We demonstrate our strategy with a physically-inspired harmonic expansion combined with a fully-connected neural network that we benchmark against a conventional convolutional architecture. We show that while both approaches allow extracting exchange modulations, only the former approach allows inferring the features of the superconducting order. Our results demonstrate the potential of machine learning methods to extract Hamiltonian parameters by real-space impurity spectroscopy as local probes of a topological state.

Testing Distributions of Huge Objects

We initiate a study of a new model of property testing that is a hybrid of testing properties of distributions and testing properties of strings. Specifically, the new model refers to testing properties of distributions, but these are distributions over huge objects (i.e., very long strings). Accordingly, the model accounts for the total number of local probes into these objects (resp., queries to the strings) as well as for the distance between objects (resp., strings), and the distance between distributions is defined as the earth mover's distance with respect to the relative Hamming distance between strings. We study the query complexity of testing in this new model, focusing on three directions. First, we try to relate the query complexity of testing properties in the new model to the sample complexity of testing these properties in the standard distribution testing model. Second, we consider the complexity of testing properties that arise naturally in the new model (e.g., distributions that capture random variations of fixed strings). Third, we consider the complexity of testing properties that were extensively studied in the standard distribution testing model: Two such cases are uniform distributions and pairs of identical distributions.

Pattern of Endothelialization in Left Atrial Appendage Occluder by Optic Coherence Tomography: A Pilot Study.

Implantation of the left atrial appendage occluder (LAAO) has been proven to prevent stroke effectively in patients with atrial fibrillation who cannot tolerate anticoagulants. Incomplete endothelization of LAAO may cause device-related thrombus, and currently no good image modality exists to clearly see LAAO endothelialization. We aimed to use coronary optic coherence tomography (OCT) to visualize LAAO endothelialization. We enrolled 14 patients (72.8±9.4 years old) undergoing pulmonary vein isolation with a preexisting LAAO implanted more than 1 year ago (5 Watchman and 9 Amulet). After pulmonary vein isolation, we did OCT via steerable sheath and coronary guiding catheter to adjust OCT probe location and injected contrast medium to visualize the LAAO surface. Invitro testing was also performed to see the bare occluder. Invitro OCT showed the surface of the bare device as an interrupted granule pattern, which included the Watchman surface polytetrafluoroethylene membrane string, Amulet disc metal strut, and inner polytetrafluoroethylene membrane string. In the implanted Watchman, OCT showed endothelialization as a smooth surface layer with noninterrupted coarser granules. In the implanted Amulet, OCT showed endothelialization as thin (early) or thick (late) endothelialization layer covering struts with OCT shadows. Among patients with Watchman, 2 showed no, 2 early, and 1 complete endothelialization. Among patients with Amulet, 2 showed no, 3 early, and 4 late endothelialization. We demonstrated the feasibility of OCT to visualize LAAO endothelization with high resolution. Further studies are needed to determine antithrombotic regimens if incomplete endothelization is detected. A new OCT catheter may be designed specifically for LAAO.

Cellular Visualization of G-Quadruplex RNA via Fluorescence- Lifetime Imaging Microscopy.

Over the past decade, appreciation of the roles of G-quadruplex (G4) structures in cellular regulation and maintenance has rapidly grown, making the establishment of robust methods to visualize G4s increasingly important. Fluorescent probes are commonly used for G4 detection in vitro; however, achieving sufficient selectivity to detect G4s in a dense and structurally diverse cellular environment is challenging. The use of fluorescent probes for G4 detection is further complicated by variations of probe uptake into cells, which may affect fluorescence intensity independently of G4 abundance. In this work, we report an alternative small-molecule approach to visualize G4s that does not rely on fluorescence intensity switch-on and, thus, does not require the use of molecules with exclusive G4 binding selectivity. Specifically, we have developed a novel thiazole orange derivative, TOR-G4, that exhibits a unique fluorescence lifetime when bound to G4s compared to other structures, allowing G4 binding to be sensitively distinguished from non-G4 binding, independent of the local probe concentration. Furthermore, TOR-G4 primarily colocalizes with RNA in the cytoplasm and nucleoli of cells, making it the first lifetime-based probe validated for exploring the emerging roles of RNA G4s in cellulo.

Polar Polymorphism: A New Intermediate Structure toward the Thin-Film Phase in Asymmetric Benzothieno[3,2-b][1]-benzothiophene Derivatives.

Understanding structure and polymorphism is relevant for any organic device optimization, and it is of particular relevance in 7-decyl-2-phenyl[1]benzothieno[3,2-b][1]benzothiophene (Ph-BTBT-10) since high carrier mobility in Ph-BTBT-10 thin films has been linked to the structural transformation from the metastable thin-film phase to the thermodynamically stable bilayer structure via thermal annealing. We combine here a systematic nanoscale morphological analysis with local Kelvin probe force microcopy (KPFM) that demonstrates the formation of a polar polymorph in thin films as an intermediate structure for thicknesses lower than 20 nm. The polar structure develops with thickness a variable amount of structural defects in the form of individual flipped molecules (point defects) or sizable polar domains, and evolves toward the reported nonpolar thin-film phase. The direct experimental evidence is supported by electronic structure density functional theory calculations. The structure of the film has dramatic effects on the electronic properties, leading to a decrease in the film work function (by up to 1 eV) and a considerable broadening of the occupied molecular orbitals, attributed to electrostatic disorder. From an advanced characterization point of view, KPFM stands out as a valuable tool for evaluating electrostatic disorder and the conceivable emergence of polar polymorphs in organic thin films. The emergence of polar assemblies introduces a critical consideration for other asymmetric BTBT derivatives, which may be pivotal to understanding the structure-property relationships in organic field-effect transistors (OFETs). A precise determination of any polar assemblies close to the dielectric interface is critical for the judicious design and upgrading of high-performance OFETs.

Investigation of the impact of probes and internals on power and flow in stirred tank reactors

This study characterises the power requirements and flow patterns in several commercial stirred tank bioreactors with working volumes ranging from 60 mL to 1 L, and investigates the isolated impact of internals, i.e. baffles and probes, on the power number, P0. Results show that the presence of probes leads to a rise of the turbulent power number, P0, equivalent to the presence of baffles, and as the number of internals increases the variation of P0 gets smaller until it plateaus for large probe quantity and high-volume blockage. Internals have a greater impact on flow with radial flow impellers, causing a significant increase in P0 in comparison to axial flow impellers. An experimental and computational flow dynamics study is also conducted to investigate the interaction between the probe wake and the impeller trailing vortices, and an estimate is provided of the form drag from the pressure distribution acting on the probe, with a good agreement to the corresponding power number increase. A comparison between P0 data obtained from conventional-cylindrical and novel-streamlined probe configurations shows that optimising probe geometry and location with respect to the incoming flow can be an effective approach for reducing power requirements, local values energy dissipation rate and stress levelsinside the tank. This study provides valuable insights into the impact of internal components and flow type on power input per unit volume, P/V, in small-scale bioreactors and supports the development of more robust scaling procedures for the biopharma industry.

Understanding LiNiO2 Electronic Structure and Redox Mechanism by Raman and X-Ray Techniques

LiNiO2 (LNO) is considered a very promising and high energy density alternative to Co-containing Li-ion battery cathodes. It is also the benchmarked cathode material of the European BIGMAP project, which aim is to combine advance operando characterization, computational modelling and artificial intelligence in order to accelerate the research and development of new generation batteries.However, the material suffers from several degradation issues resulting in fading cell performance. In particular, the presence of highly reactive Ni4+ species at the electrode/electrolyte interface1, Ni dissolution from the cathode leading to the loss of active material 2, and O2 release at high voltage are the major drawbacks precluding commercial applications. A recent in situ study1 has shown that O2 release compromises the structural stability and triggers reactions with ethylene carbonate (EC), prompting CO2evolution3,4.In parallel, solid state physics community is also largely interested into LiNiO2 in the framework of a larger investigation around the electronic and atomic structure of nickelates, in particular rare-earth nickelates. This interest rises from the fact that there is still no consensus on the atomic/electronic structure of LiNiO2, while different descriptions exist in literature. Local probe techniques demonstrate the distortion of NiO6 octahedra, and there are two on-going theories for explaining the presence of this distortion: (i) Ni3+ (t2g6 eg1) Jahn-Teller (JT) distortion, (ii) 2 Ni3+ → Ni2+ + Ni4+ bond disproportionation (BD)5. Surprisingly, the local order distortion does not result in the long-range distortion, the mechanism behind this phenomenon is not completely understood.In this contribution we present a detailed study of LNO cathode material by operando Raman and X-ray absorption spectroscopy (XAS) at the Ni K-edge, ex situ X-ray emission spectroscopy (XES) and resonant Inelastic X-ray scattering (RIXS). Distinguishing between JT and BD models is challenging, and therefore NaNiO2 reference is used, which is isoelectronic material to LiNiO2, and is known to feature long-range JT distortion.While XAS is widely established technique to probe local structure and transition metal oxidation state, RIXS is useful for assessing d-d transitions and bond disproportionation. Operando Raman spectroscopy is an excellent tool for studying phase transitions in Li-ion battery cathodes and is therefore complementary to the employed X-ray techniques6. It provides information on two characteristic for layered oxides crystalline phonon modes A1g and Eg, and sheds light on both short-range order and cationic/anionic redox. The penetration depth is estimated as top few hundred nanometers of around five micrometres sized secondary particle, therefore near-surface area is probed. The results show a complex behaviour of band positions and intensities during cycling (figure 1), corresponding to four phases transformations. Notably the peaks intensities increase considerably, while the widths are decreased, which is evidence of increased order upon material delithiation, and is in agreement with the Extended X-ray Absorption Fine Structure (EXAFS). Raman is also used to evaluate the contribution of anionic redox, since all the reduced oxygen species (superoxide, peroxide and molecular oxygen) have well-known Raman-active modes.To conclude, we demonstrate how a combination of multiple vibrational and X-rays based spectroscopies provides a better understanding of both LNO ground state electronic structure and redox mechanism. This increased fundamental understanding will stimulate the design of better strategies for prevention of the material degradation and improved cycle retention.

Mapping Pressure- and Temperature-Induced Structural and Magnetic Transitions in Perovskite PrNiO3 with Local and Long-Range Probes

Mapping Pressure- and Temperature-Induced Structural and Magnetic Transitions in Perovskite PrNiO₃ with Local and Long-Range Probes

Identifying Chern numbers of superconductors from local measurements

Fascination in topological materials originates from their remarkable response properties and exotic quasiparticles which can be utilized in quantum technologies. In particular, large-scale efforts are currently focused on realizing topological superconductors and their Majorana excitations. However, determining the topological nature of superconductors with current experimental probes is an outstanding challenge. This shortcoming has become increasingly pressing due to rapidly developing designer platforms which are theorized to display very rich topology and are better accessed by local probes rather than transport experiments. We introduce a robust machine learning protocol for classifying the topological states of two-dimensional (2D) chiral superconductors and insulators from local density of states (LDOS) data. Since the LDOS can be measured with standard experimental techniques, our protocol contributes to overcoming the almost three decades standing problem of identifying the topological phase of 2D superconductors with broken time-reversal symmetry.

Local probing of eddy current correlated with magnetic properties

Recently, the development of long-range electric vehicles with effective electric motors has drawn considerable attention. The key to achieving such electric vehicles development is power saving, which has served as an essential motive for development of new magnetic materials. In this regard, further improvement of magnetic materials requires deep insight into the existence of eddy currents, which are primary contributors toward power loss in practical applications. Therefore, exploring the key effects of eddy currents on overall magnetic properties is essential. Here, we demonstrate clearly distinguished eddy current distributions being influenced by local magnetic properties via multidimensional magnetic force microscopy. Using our model systems, we explored the key role of an insulation layer and magnetic domains on eddy current dependent magnetic properties. In particular, we visualized the correlation between the eddy current and magnetic domain/domain wall. Therefore, our approach provides detailed characterization of eddy current, particularly related to the underlying contributions of local magnetic properties, offering crucial insights for improvement of electric motors.

Electrostatic Impact of Brefeldin A on Thiocyanate Probes Surrounding the Interface of Arf1-BFA-ARNO4M, a Protein-Drug-Protein Complex.

Protein-protein interactions regulate many cellular processes, making them ideal drug candidates. Design of such drugs, however, is hindered by a lack of understanding of the factors that contribute to the interaction specificity. Specific protein-protein complexes possess both structural and electrostatic complementarity, and while structural complementarity of protein complexes has been extensively investigated, fundamental understanding of the complicated networks of electrostatic interactions at these interfaces is lacking, thus hindering the rational design of orthosterically binding small molecules. To better understand the electrostatic interactions at protein interfaces and how a small molecule could contribute to and fit within that environment, we used a model protein-drug-protein system, Arf1-BFA-ARNO4M, to investigate how small molecule brefeldin A (BFA) perturbs the Arf1-ARNO4M interface. By using nitrile probe labeled Arf1 sites and measuring vibrational Stark effects as well as temperature dependent infrared shifts, we measured changes in the electric field and hydrogen bonding at this interface upon BFA binding. At all five probe locations of Arf1, we found that the vibrational shifts resulting from BFA binding corroborate trends found in Poisson-Boltzmann calculations of surface potentials of Arf1-ARNO4M and Arf1-BFA-ARNO4M, where BFA contributes negative electrostatic potential to the protein interface. The data also corroborate previous hypotheses about the mechanism of interfacial binding and confirm that alternating patches of hydrophobic and polar interactions lead to BFA binding specificity. These findings demonstrate the impact of BFA on this protein-protein interface and have implications for the design of other interfacial drug candidates.

Multiple potential drop measurement – A new method for crack detection and crack length measurement

The Direct Current Potential Drop Method (DCPDM) is widely used for crack detection and crack length measurement in fatigue experiments. Unfortunately, crack length measurements are only possible when a calibration for a specified crack initiation site and potential probe location is available. Investigations by Hartweg and Bär (2019) as well as Nahbein and Bär (2022) on notched round specimens equipped with three potential probes placed in a distance of 120° on the circumference have shown that the crack initiation site can be determined using a simple vector-based model. In this model the normal vector of a plane span by the three potentials is calculated in cylindrical coordinates. In the present work a more detailed investigation of crack initiation and propagation is undertaken to show the possibilities offered by this method. During fatigue tests with the simultaneous measurement of the three potential drops using amplifiers of the control electronics, overloads were introduced in fixed intervals to mark the crack front on the fracture surface. The measurement of both crack depth and fractured area allows a calibration of the potential drop measurement. The calibration was performed on the radius coordinate n of the normal vector using a function suggested by Tiedemann (2016). The multiple potential drop measurement enables an early detection of crack initiation as well as a location of the crack initiation site on the circumference of the specimen. Using the Tiedemann function fitted to the measured data, it is possible to determine the crack length independent of the crack initiation site on the circumference of the specimen.

Analysis of the first coronagraphic multi-band observations of a sungrazing comet

Context. Between 24 and 25 December 2021 a sungrazing comet (SOHO-4341) approached the Sun, being observed by “classical” visible light (VL) coronagraphs on board the SOHO and STEREO missions, and also by the innovative Metis coronagraph on board the ESA-NASA Solar Orbiter mission in the VL and ultraviolet (UV H I Lyman-α) band. Aims. We show how VL data acquired by the Metis coronagraph can be combined with those provided by other space-based coronagraphs to reconstruct the comet orbit, but also to provide information on the dust composition from the polarized VL emission. Moreover, we show how the UV emission can be employed to measure local plasma parameters of the ambient solar wind. Methods. By using the comet positions tracked with VL Metis images (with spatial resolution that is four times better than UV), the UV images (with a time cadence that is five times faster than VL) have been coaligned to maximize the signal-to-noise ratio in the UV band. The local electron density ne was measured from the observed exponential decay of the UV Lyman-α intensity along the tail, while the solar wind speed vwind was measured from the UV Lyman-α tail inclination with respect to the cometary orbital path deprojected in 3D. Moreover, the proton kinetic temperature Tk was also obtained by the aperture angle of the UV Lyman-α tail. Results. When the comet was at an average heliocentric distance of 14.3 R⊙, the comet had a radial speed of 155 km s−1 and a tangential speed of 59 km s−1. The comet had a UV Lyman-α tail extending in the anti-solar direction over more than 1.5 R⊙. From the analysis of the tail shape in UV we obtained the local solar wind speed (vwind = 190 km s−1), electron density (ne = 1.5 × 104 cm−3), and proton temperature (Tk = 1.2 × 106 K). Moreover, theoretical analysis of the measured UV Lyman-α intensity allowed us to estimate the radius of the cometary nucleus (Rcom = 65 m) and the water outgassing rate (QH2O = 4.8 × 1028 molec s−1). Conclusions. These results show that sungrazing comets are unique “local probes” for the ambient coronal plasma, providing measurements that are not as affected by the line-of-sight integration effects as those provided by remote sensing instruments, in regions of the Heliosphere that are not explored in situ by the ongoing space missions.

Bound states of Dirac fermions in the presence of a Fermi velocity modulation

We investigate the effect of a position-dependent Fermi velocity on the electronic properties of two-dimensional Dirac materials. A physical Fermi velocity distribution, which approaches a finite value at infinity and experiences a modulation near x = 0, is considered. Such a position-dependent Fermi velocity could be realized in the curved graphene or by applying strain. It is shown that the bound states are absent in the presence of a pure Fermi velocity modulation without an electrostatic potential well. However, an extra electrostatic potential modulation could produce the bound states. A set of discrete energy level spectrum and the corresponding wave functions are obtained by solving the Dirac equation exactly. Local probes such as scanning tunnel microscopy should be able to observe the predicted bound states in two-dimensional materials.

Local probe-induced structural isomerization in a one-dimensional molecular array

Synthesis of one-dimensional molecular arrays with tailored stereoisomers is challenging yet has great potential for application in molecular opto-, electronic- and magnetic-devices, where the local array structure plays a decisive role in the functional properties. Here, we demonstrate the construction and characterization of dehydroazulene isomer and diradical units in three-dimensional organometallic compounds on Ag(111) with a combination of low-temperature scanning tunneling microscopy and density functional theory calculations. Tip-induced voltage pulses firstly result in the formation of a diradical species via successive homolytic fission of two C-Br bonds in the naphthyl groups, which are subsequently transformed into chiral dehydroazulene moieties. The delicate balance of the reaction rates among the diradical and two stereoisomers, arising from an in-line configuration of tip and molecular unit, allows directional azulene-to-azulene and azulene-to-diradical local probe structural isomerization in a controlled manner. Furthermore, our theoretical calculations suggest that the diradical moiety hosts an open-shell singlet with antiferromagnetic coupling between the unpaired electrons, which can undergo an inelastic spin transition of 91 meV to the ferromagnetically coupled triplet state.