Enhanced magnetic anisotropy of iridium dimers on antisite defects of two-dimensional transition-metal dichalcogenides.

The combination of transition-metal (TM) elements with two-dimensional (2D) transition-metal dichalcogenides (TMDs) provides an effective route to realizing a 2D controllable magnetic order, leading to significant applications in multifunctional nanospintronics. However, in most TM atoms@TMDs nanostructures, it is challenging for the magnetic anisotropy energy (MAE) to exceed 30 meV when affected by the crystal field. Hence, the stronger magnetic anisotropy of TMDs has yet to be developed. Here, utilizing first-principle calculations based on density functional theory (DFT), a feasible method to enhance the MAEs of TMDs via configurating iridium dimers (Ir2) on 2D traditional and Janus TMDs with antisite defects is reported. Calculations revealed that 28 of the 54 configurations considered possessed structure-dependent MAEs of >60 meV per Ir2 in the out-of-plane direction, suggesting the potential for applications at room temperature. We also showed the ability to tune the MAE further massively by applying a biaxial strain as well as the surface asymmetric polarization reversal of Janus-type substrates. This approach led to changes to >80 meV per Ir2. This work provides a novel strategy to achieve tunable large magnetic anisotropy in 2D TMDs. It also extends the functionality of antisite-defective TMDs, thereby providing theoretical support for the development of magnetic nanodevices.

Observation of giant non-reciprocal charge transport from quantum Hall states in a topological insulator.

Symmetry breaking in quantum materials is of great importance and can lead to non-reciprocal charge transport. Topological insulators provide a unique platform to study non-reciprocal charge transport due to their surface states, especially quantum Hall states under an external magnetic field. Here we report the observation of non-reciprocal charge transport mediated by quantum Hall states in devices composed of the intrinsic topological insulator Sn-Bi1.1Sb0.9Te2S, which is attributed to asymmetric scattering between quantum Hall states and Dirac surface states. A giant non-reciprocal coefficient of up to 2.26 × 105 A-1 is found. Our work not only reveals the properties of non-reciprocal charge transport of quantum Hall states in topological insulators but also paves the way for future electronic devices.

Light-induced giant enhancement of nonreciprocal transport at KTaO3-based interfaces.

Nonlinear transport is a unique functionality of noncentrosymmetric systems, which reflects profound physics, such as spin-orbit interaction, superconductivity and band geometry. However, it remains highly challenging to enhance the nonreciprocal transport for promising rectification devices. Here, we observe a light-induced giant enhancement of nonreciprocal transport at the superconducting and epitaxial CaZrO3/KTaO3 (111) interfaces. The nonreciprocal transport coefficient undergoes a giant increase with three orders of magnitude up to 105 A-1 T-1. Furthermore, a strong Rashba spin-orbit coupling effective field of 14.7 T is achieved with abundant high-mobility photocarriers under ultraviolet illumination, which accounts for the giant enhancement of nonreciprocal transport coefficient. Our first-principles calculations further disclose the stronger Rashba spin-orbit coupling strength and the longer relaxation time in the photocarrier excitation process, bridging the light-property quantitative relationship. Our work provides an alternative pathway to boost nonreciprocal transport in noncentrosymmetric systems and facilitates the promising applications in opto-rectification devices and spin-orbitronic devices.

Oxidation behavior and atomic structural transition of size-selected coalescence-resistant tantalum nanoclusters.

Herein a series of size-selected TaN(N = 147, 309, 561, 923, 1415, 2057, 6525, 10 000, 20 000) clusters are generated using a gas-phase condensation cluster beam source equipped with a lateral time-of-flight mass-selector. Aberration-corrected scanning transmission electron microscopy (AC-STEM) imaging reveals good thermal stability of TaNclusters in this study. The oxidation-induced amorphization is observed from AC-STEM imaging and further demonstrated through x-ray photoelectron spectroscopy and energy-dispersive spectroscopy. The oxidized Ta predominantly exists in the +5 oxidation state and the maximum spontaneous oxidation depth of the Ta cluster is observed to be 5 nm under prolonged atmosphere exposure. Furthermore, the size-dependent sintering and crystallization processes of oxidized TaNclusters are observed with anin situheating technique, and eventually, ordered structures are restored. As the temperature reaches 1300 °C, a fraction of oxidized Ta309clusters exhibit decahedral and icosahedral structures. However, the five-fold symmetry structures are absent in larger clusters, instead, these clusters exhibit ordered structures resembling those of the crystalline Ta2O5films. Notably, the sintering and crystallization process occurs at temperatures significantly lower than the melting point of Ta and Ta2O5, and the ordered structures resulting from annealing remain well-preserved after six months of exposure to ambient conditions.

Defect-induced helicity dependent terahertz emission in Dirac semimetal PtTe2 thin films.

Nonlinear transport enabled by symmetry breaking in quantum materials has aroused considerable interest in condensed matter physics and interdisciplinary electronics. However, achieving a nonlinear optical response in centrosymmetric Dirac semimetals via defect engineering has remained a challenge. Here, we observe the helicity dependent terahertz emission in Dirac semimetal PtTe2 thin films via the circular photogalvanic effect under normal incidence. This is activated by a controllable out-of-plane Te-vacancy defect gradient, which we unambiguously evidence with electron ptychography. The defect gradient lowers the symmetry, which not only induces the band spin splitting but also generates the giant Berry curvature dipole responsible for the circular photogalvanic effect. We demonstrate that the THz emission can be manipulated by the Te-vacancy defect concentration. Furthermore, the temperature evolution of the THz emission features a minimum in the THz amplitude due to carrier compensation. Our work provides a universal strategy for symmetry breaking in centrosymmetric Dirac materials for efficient nonlinear transport.

Magnetotransport spectroscopy of electroburnt graphene nanojunctions.

We have reported the precise methodology for fabricating graphene quantum dots through electroburning and performed measurements on the Coulomb blockade and oscillation phenomena. The diameters of graphene quantum dots can be estimated to range from several to tens of nanometers, utilizing the disk capacitance model and the two-dimensional quantum well model. By subjecting the quantum dots to a vertical magnetic field, an obvious alteration in conductance can be detected at the point of resonance tunneling. This observed phenomenon can be attributed to the modification in the density of states of Landau levels within the graphene leads. Moreover, by manipulating the gate voltage, it is possible to regulate the Fermi level of the lead, resulting in distinct magnetoresistance of different electron states. The presence of this lead effect may potentially disrupt the magnetic response analysis of graphene-based single-molecule transistors, necessitating a comprehensive theoretical examination to mitigate such interference.

Electrically controlled nonvolatile switching of single-atom magnetism in a Dy@C84 single-molecule transistor.

Single-atom magnetism switching is a key technique towards the ultimate data storage density of computer hard disks and has been conceptually realized by leveraging the spin bistability of a magnetic atom under a scanning tunnelling microscope. However, it has rarely been applied to solid-state transistors, an advancement that would be highly desirable for enabling various applications. Here, we demonstrate realization of the electrically controlled Zeeman effect in Dy@C84 single-molecule transistors, thus revealing a transition in the magnetic moment from 3.8 µ B to 5.1 µ B for the ground-state GN at an electric field strength of 3 - 10 MV/cm. The consequent magnetoresistance significantly increases from 600% to 1100% at the resonant tunneling point. Density functional theory calculations further corroborate our realization of nonvolatile switching of single-atom magnetism, and the switching stability emanates from an energy barrier of 92 meV for atomic relaxation. These results highlight the potential of using endohedral metallofullerenes for high-temperature, high-stability, high-speed, and compact single-atom magnetic data storage.

[Mandibular condyle localization in orthognathic surgery based on mandibular movement trajectory and its preliminary accuracy verification].

OBJECTIVE: To establish and assess the precision of pre-surgical condyle position planning using mandibular movement trajectory data for orthognathic surgery. METHODS: Skull data from large-field cone beam computed tomography (CBCT) and dental oral scan data were imported into IVSPlan 1.0.25 software for 3D reconstruction and fusion, creating 3D models of the maxilla and mandible. Trajectory data of mandibular movement were collected using a mandibular motion recorder, and the data were integrated with the jaw models within the software. Subsequently, three-dimensional trajectories of the condyle were obtained through matrix transformations, rendering them visually accessible. A senior oral and maxillofacial surgeon with experience in both diagnosis and treatment of temporomandibular joint disease and orthognathic surgery selected the appropriate condyle position using the condyle movement trajectory interface. During surgical design, the mobile mandibular proximal segment was positioned accordingly. Routine orthognathic surgical planning was completed by determining the location of the mandibular distal segment, which was based on occlusal relationships with maxilla and facial aesthetics. A virtual mandible model was created by integrating data from the proximal and distal segment bone. Subsequently, a solid model was generated through rapid prototyping. The titanium plate was pre-shaped on the mandibular model, and the screw hole positions were determined to design a condylar positioning guide device. In accordance with the surgical plan, orthognathic surgery was performed, involving mandibular bilateral sagittal split ramus osteotomy (SSRO). The distal segment of the mandible was correctly aligned intermaxillary, while the proximal bone segment was positioned using the condylar positioning guide device and the pre-shaped titanium plate. The accuracy of this procedure was assessed in a study involving 10 patients with skeletal class Ⅱ malocclusion. Preoperative condyle location planning and intraoperative positioning were executed using the aforementioned techniques. CBCT data were collected both before the surgery and 2 weeks after the procedure, and the root mean square (RMS) distance between the preope-rative design position and the actual postoperative condyle position was analyzed. RESULTS: The RMS of the condyle surface distance measured was (1.59±0.36) mm (95%CI: 1.35-1.70 mm). This value was found to be significantly less than 2 mm threshold recommended by the expert consensus (P < 0.05). CONCLUSION: The mandibular trajectory may play a guiding role in determining the position of the mandibular proximal segment including the condyle in the orthognathic surgery. Through the use of a condylar positioning guide device and pre-shaped titanium plates, the condyle positioning can be personalized and customized with clinically acceptable accuracy.

Investigation of the accuracy of dynamic condylar position: A model study.

OBJECTIVES: To evaluate dynamic condylar positions by integrating mandibular movement recording data and cone-beam computed tomography (CBCT) and to investigate its accuracy via dynamic model experiments. METHODS: A polyvinyl chloride skull model was utilized. A robot arm was used to operate the mandible to perform mouth opening, closing, protrusion, and lateral movements. A recording device, worn on the skull, was used to record the dynamic process and an optical position tracking (OPT) system was used to simultaneously trace the movements. A self-developed software module was used to evaluate the dynamic condylar position by integrating the dynamic tracing data and a virtual skull model derived from CBCT images. Errors were defined as differences between the dynamic coordinates of six landmarks around the condylar area derived from the software module (test) and OPT system (gold standard). RESULTS: The condylar position errors were 0.76 ± 0.31, 0.55 ± 0.15, and 0.68 ± 0.23 mm for mouth opening, bilateral, and protrusion movements, respectively. Furthermore, the errors for small, moderate, and large mouth opening movements were 0.62 ± 0.19, 0.69 ± 0.29, and 0.94 ± 0.31 mm, respectively. The errors for all movements, except for large mouth opening, were significantly less than 1 mm (P < 0.05). The error was not different from 1 mm in the large mouth opening movement (P > 0.05). CONCLUSIONS: Our developed method of achieving dynamic condylar position by integrating mandibular movement recording data and CBCT images is clinically reliable. CLINICAL SIGNIFICANCE: This study proved the reliability of evaluating dynamic condylar position using a commercial dynamic recording instrument and CBCT images.

Influence of ligands on the optical properties of rod-shaped Au25 nanoclusters.

In this study, we successfully synthesized rod-shaped [Au25(PPh3)10(S-Adm)5Cl2]2+ nanoclusters using kinetic controls. The complete molecular structure was determined by single-crystal X-ray crystallography and electrospray ionization mass spectrometry. In comparison with the previously reported [Au25(PPh3)10(PET)5Cl2]2+ clusters, both nanoclusters have an icosahedral composition of Au13 linked by Au atoms that share a vertex, but [Au25(PPh3)10(S-Adm)5Cl2]2+ clusters appear elongated due to the rigidity of adamantane. We conducted ultraviolet-visible spectrophotometry (UV-vis) measurements of [Au25(PPh3)10(PET)5Cl2]2+ and [Au25(PPh3)10(S-Adm)5Cl2]2+ in dichloromethane solvent to elucidate the modulation of the cluster properties of different ligands. The lowest energy absorption peak of [Au25(PPh3)10(S-Adm)5Cl2]2+ shifted to lower energies compared to the [Au25(PPh3)10(PET)5Cl2]2+ clusters in UV-vis measurements. Temperature-dependent absorption measurements revealed that [Au25(PPh3)10(S-Adm)5Cl2]2+ clusters were less affected by temperature compared to [Au25(PPh3)10(PET)5Cl2]2+. This result is attributed to the exciton phonon coupling of [Au25(PPh3)10(S-Adm)5Cl2]2+ clusters being weaker than [Au25(PPh3)10(PET)5Cl2]2+ clusters. Furthermore, the absorption spectra of [Au25(PPh3)10(PET)5Cl2]2+ and [Au25(PPh3)10(S-Adm)5Cl2]2+ clusters were measured using different types of solutions, and it was found that the lowest energy absorption peaks of [Au25(PPh3)10(S-Adm)5Cl2]2+ were shifted and affected by the solution at room temperature, which suggested that the [Au25(PPh3)10(S-Adm)5Cl2]2+ clusters with solution hydrogen bonds also interacted strongly at room temperature. Theoretical calculations show that changes in ligands affect the differences in the molecular orbitals and structures of the clusters, which cause changes in the optical properties.

Tunable optical topological transitions of plasmon polaritons in WTe2 van der Waals films.

Naturally existing in-plane hyperbolic polaritons and the associated optical topological transitions, which avoid the nano-structuring to achieve hyperbolicity, can outperform their counterparts in artificial metasurfaces. Such plasmon polaritons are rare, but experimentally revealed recently in WTe2 van der Waals thin films. Different from phonon polaritons, hyperbolic plasmon polaritons originate from the interplay of free carrier Drude response and interband transitions, which promise good intrinsic tunability. However, tunable in-plane hyperbolic plasmon polariton and its optical topological transition of the isofrequency contours to the elliptic topology in a natural material have not been realized. Here we demonstrate the tuning of the optical topological transition through Mo doping and temperature. The optical topological transition energy is tuned over a wide range, with frequencies ranging from 429 cm-1 (23.3 microns) for pure WTe2 to 270 cm-1 (37.0 microns) at the 50% Mo-doping level at 10 K. Moreover, the temperature-induced blueshift of the optical topological transition energy is also revealed, enabling active and reversible tuning. Surprisingly, the localized surface plasmon resonance in skew ribbons shows unusual polarization dependence, accurately manifesting its topology, which renders a reliable means to track the topology with far-field techniques. Our results open an avenue for reconfigurable photonic devices capable of plasmon polariton steering, such as canaling, focusing, and routing, and pave the way for low-symmetry plasmonic nanophotonics based on anisotropic natural materials.

Broadband and Spectrally Selective Photothermal Conversion through Nanocluster Assembly of Disordered Plasmonic Metasurfaces.

Plasmonic metasurfaces have been realized for efficient light absorption, thereby leading to photothermal conversion through nonradiative decay of plasmonic modes. However, current plasmonic metasurfaces suffer from inaccessible spectral ranges, costly and time-consuming nanolithographic top-down techniques for fabrication, and difficulty of scale-up. Here, we demonstrate a new type of disordered metasurface created by densely packing plasmonic nanoclusters of ultrasmall size on a planar optical cavity. The system either operates as a broadband absorber or offers a reconfigurable absorption band right across the visible region, resulting in continuous wavelength-tunable photothermal conversion. We further present a method to measure the temperature of plasmonic metasurfaces via surface-enhanced Raman spectroscopy (SERS), by incorporating single-walled carbon nanotubes (SWCNTs) as an SERS probe within the metasurfaces. Our disordered plasmonic system, generated by a bottom-up process, offers excellent performance and compatibility with efficient photothermal conversion. Moreover, it also provides a novel platform for various hot-electron and energy-harvesting functionalities.

Slice Visualization for Imaging Nanocluster Transformations.

Metal nanoclusters have served as an emerging class of modular nanomaterials. Several efficient strategies have been proposed for transforming cluster precursors into new nanoclusters with customized structures and enhanced performance. However, such nanocluster transformations have still been in a "blind box" state, meaning that the existing intermediates were hard to track with atomic precision. Herein, we present a "slice visualization" approach for in-depth imaging of the nanocluster transformation from Au1Ag24(SR)18 to Au1Ag30(SR)20. With this approach, two cluster intermediates, namely, Au1Ag26(SR)19 and Au1Ag28(SR)20, were monitored with atomic precision. The four nanoclusters constituted a correlated Au1Ag24+2n (n = 0, 1, 2, and 3) cluster series with comparable structural features─the same Au1Ag12 icosahedral kernel but evolutionary peripheral motif structures. The mechanism of nanocluster structure growth was mapped in detail─insertion of Ag2(SR)1 or Ag-induced assembly of surface subunits. The presented "slice visualization" approach not only contributes an ideal cluster platform for in-depth investigations of structure-property correlations but also hopefully acts as a powerful means for obtaining clear information on nanocluster structure evolution.

Processing Optimization of Shear Thickening Fluid Assisted Micro-Ultrasonic Machining Method for Hemispherical Mold Based on Integrated CatBoost-GA Model.

Micro-electro-mechanical systems (MEMS) hemispherical resonant gyroscopes are used in a wide range of applications in defense technology, electronics, aerospace, etc. The surface roughness of the silicon micro-hemisphere concave molds (CMs) inside the MEMS hemispherical resonant gyroscope is the main factor affecting the performance of the gyroscope. Therefore, a new method for reducing the surface roughness of the micro-CM needs to be developed. Micro-ultrasonic machining (MUM) has proven to be an excellent method for machining micro-CMs; shear thickening fluids (STFs) have also been used in the ultra-precision polishing field due to their perfect processing performance. Ultimately, an STF-MUM polishing method that combines STF with MUM is proposed to improve the surface roughness of the micro-CM. In order to achieve the excellent processing performance of the new technology, a Categorical Boosting (CatBoost)-genetic algorithm (GA) optimization model was developed to optimize the processing parameters. The results of optimizing the processing parameters via the CatBoost-GA model were verified by five groups of independent repeated experiments. The maximum absolute error of CatBoost-GA is 7.21%, the average absolute error is 4.69%, and the minimum surface roughness is reduced by 28.72% compared to the minimum value of the experimental results without optimization.

Enhanced Superconductivity and Upper Critical Field in Ta-Doped Weyl Semimetal Td -MoTe2.

2D transition metal dichalcogenides are promising platforms for next-generation electronics and spintronics. The layered Weyl semimetal (W,Mo)Te2 series features structural phase transition, nonsaturated magnetoresistance, superconductivity, and exotic topological physics. However, the superconducting critical temperature of the bulk (W,Mo)Te2 remains ultralow without applying a high pressure. Here, the significantly enhanced superconductivity is observed with a transition temperature as large as about 7.5 K in bulk Mo1- x Tax Te2 single crystals upon Ta doping (0 ≤ x ≤ 0.22), which is attributed to an enrichment of density of states at the Fermi level. In addition, an enhanced perpendicular upper critical field of 14.5 T exceeding the Pauli limit is also observed in Td -phase Mo1- x Tax Te2 (x = 0.08), indicating the possible emergence of unconventional mixed singlet-triplet superconductivity owing to the inversion symmetry breaking. This work provides a new pathway for exploring the exotic superconductivity and topological physics in transition metal dichalcogenides.

Light-Induced Mott-Insulator-to-Metal Phase Transition in Ultrathin Intermediate-Spin Ferromagnetic Perovskite Ruthenates.

Light control of emergent quantum phenomena is a widely used external stimulus for quantum materials. Generally, perovskite strontium ruthenate SrRuO3 has an itinerant ferromagnetism with a low-spin state. However, the phase of intermediate-spin (IS) ferromagnetic metallic state has never been seen. Here, by means of UV-light irradiation, a photocarrier-doping-induced Mott-insulator-to-metal phase transition is shown in a few atomic layers of perovskite IS ferromagnetic SrRuO3- δ . This new metastable IS metallic phase can be reversibly regulated due to the convenient photocharge transfer from SrTiO3 substrates to SrRuO3- δ ultrathin films. These dynamical mean-field theory calculations further verify such photoinduced electronic phase transformation, owing to oxygen vacancies and orbital reconstruction. The optical manipulation of charge-transfer finesse is an alternative pathway toward discovering novel metastable phases in strongly correlated systems and facilitates potential light-controlled device applications in optoelectronics and spintronics.

Large Exchange Bias Effect and Coverage-Dependent Interfacial Coupling in CrI3/MnBi2Te4 van der Waals Heterostructures.

Igniting interface magnetic ordering of magnetic topological insulators by building a van der Waals heterostructure can help to reveal novel quantum states and design functional devices. Here, we observe an interesting exchange bias effect, indicating successful interfacial magnetic coupling, in CrI3/MnBi2Te4 ferromagnetic insulator/antiferromagnetic topological insulator (FMI/AFM-TI) heterostructure devices. The devices originally exhibit a negative exchange bias field, which decays with increasing temperature and is unaffected by the back-gate voltage. When we change the device configuration to be half-covered by CrI3, the exchange bias becomes positive with a very large exchange bias field exceeding 300 mT. Such sensitive manipulation is explained by the competition between the FM and AFM coupling at the interface of CrI3 and MnBi2Te4, pointing to coverage-dependent interfacial magnetic interactions. Our work will facilitate the development of topological and antiferromagnetic devices.

Electrical devices designed based on inorganic clusters.

The idea of exploring the bottom brink of material science has been carried out for more than two decades. Clusters science is the frontmost study of all nanoscale structures. Being an example of 0-dimensional quantum dot, nanocluster serves as the bridge between atomic and conventionally understood solid-state physics. The forming mechanism of clusters is found to be the mutual effects of electronic and geometric configuration. It is found that electronic shell structure influences the properties and geometric structure of the cluster until its size becomes larger, where electronic effects submerge in geometric structure. The discrete electronic structures depend on the size and conformation of clusters, which can be controlled artificially for potential device applications. Especially, small clusters with a size of 1-2 nm, whose electronic states are possibly discrete enough to overcome thermal fluctuations, are expected to build a single-electron transistor with room temperature operation. However, exciting as the progress may be seen, cluster science still falls within the territory of merely the extension of atomic and molecular science. Its production rate limits the scientific and potential application research of nanoclusters. It is suggested in this review that the mass-produce ability without losing the atomic precision selectivity would be the milestone for nanoclusters to advance to material science.

Observation of Magnetism-Induced Topological Edge State in Antiferromagnetic Topological Insulator MnBi4Te7.

Breaking time reversal symmetry in a topological insulator may lead to quantum anomalous Hall effect and axion insulator phase. MnBi4Te7 is a recently discovered antiferromagnetic topological insulator with TN ∼ 12.5 K, which is composed of an alternatively stacked magnetic layer (MnBi2Te4) and nonmagnetic layer (Bi2Te3). By means of scanning tunneling spectroscopy, we clearly observe the electronic state present at a step edge of a magnetic MnBi2Te4 layer but absent at nonmagnetic Bi2Te3 layers at 4.5 K. Furthermore, we find that as the temperature rises above TN the edge state vanishes, while the point defect induced state persists upon an increase in temperature. These results confirm the observation of magnetism-induced edge states. Our analysis based on an axion insulator theory reveals that the nontrivial topological nature of the observed edge state.

Hierarchical structural complexity in atomically precise nanocluster frameworks.

The supramolecular chemistry of nanoclusters is a flourishing area of nano-research; however, the controllable assembly of cluster nano-building blocks in different arrays remains challenging. In this work, we report the hierarchical structural complexity of atomically precise nanoclusters in micrometric linear chains (1D array), grid networks (2D array) and superstructures (3D array). In the crystal lattice, the Ag29(SSR)12(PPh3)4 nanoclusters can be viewed as unassembled cluster dots (Ag29-0D). In the presence of Cs+ cations, the Ag29(SSR)12 nano-building blocks are selectively assembled into distinct arrays with different oxygen-carrying solvent molecules-Cs@Ag29(SSR)12(DMF) x as 1D linear chains (Ag29-1D), Cs@Ag29(SSR)12(NMP) x as 2D grid networks (Ag29-2D), and Cs@Ag29(SSR)12(TMS) x as 3D superstructures (Ag29-3D). Such self-assemblies of these Ag29(SSR)12 units have not only been observed in their crystalline state, but also in their amorphous state. Due to the diverse surface structures and crystalline packing modes, these Ag29-based assemblies manifest distinguishable optical absorptions and emissions in both solutions and crystallized films. Furthermore, the surface areas of the nanocluster crystals are evaluated, the maximum value of which occurs when the cluster nano-building blocks are assembled into 2D arrays (i.e. Ag29-2D). Overall, this work presents an exciting example of the hierarchical assembly of atomically precise nanoclusters by simply controlling the adsorbed molecules on the cluster surface.