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  1. We argue that one can associate a pseudo-time with sequences of configurations generated in the course of classical Monte Carlo simulations for a single-minimum bound state if the sampling is optimal. Hereby, the sampling rates can be, under special circumstances, calibrated against the relaxation rate and frequency of motion of an actual physical system. The latter possibility is linked to the optimal sampling regime being a universal crossover separating two distinct suboptimal sampling regimes analogous to the physical phenomena of diffusion and effusion, respectively. Bound states break symmetry; one may thus regard the pseudo-time as a quantity emerging together with the bound state. Conversely, when transport among distinct bound states takes place—thus restoring symmetry—a pseudo-time can no longer be defined. One can still quantify activation barriers if the latter barriers are smooth, but simulation becomes impractically slow and pertains to overdamped transport only. Specially designed Monte Carlo moves that bypass activation barriers—so as to accelerate sampling of the thermodynamics—amount to effusive transport and lead to severe under-sampling of transition-state configurations that separate distinct bound states while destroying the said universality. Implications of the present findings for simulations of glassy liquids are discussed.

    Free, publicly-accessible full text available March 29, 2024
  2. Access to well-defined, model-like, non-noble metal intermetallic compound nanomaterials (<10 nm) with phase pure bulk, bulk-like 1st-atomic-layer surface composition, and unique electronic and surface chemical properties is critical for the fields of catalysis, electronics, and sensor development. Non-noble metal intermetallic compounds are compositionally ordered solid compounds composed of transition metals and semimetals or post-transition metals. Their synthesis as model-like high-surface-area supported nanoparticles is challenging due to the elevated reactivity of the constituent elements and their interaction with the support material. In this study, we have developed a systematic understanding of the fundamental phenomena that control the synthesis of these materials such that phase pure bulk nanoparticles (<10 nm) may be produced with bulk-like surface terminations. The effects of the precursor and support choice, chemical potential of H 2 , reduction temperature, and annealing procedures were investigated to understand the fundamental kinetics of particle formation and interactions that dictate phase purity and stability and 1st-atomic-layer surface composition. The understanding developed may serve as a foundation for further developing advanced synthesis procedures for well-defined nanoparticles with increasing compositional complexity.
    Free, publicly-accessible full text available June 6, 2023
  3. Free, publicly-accessible full text available July 1, 2023
  4. Abstract

    The development of integrated semiconductor lasers has miniaturized traditional bulky laser systems, enabling a wide range of photonic applications. A progression from pure III-V based lasers to III-V/external cavity structures has harnessed low-loss waveguides in different material systems, leading to significant improvements in laser coherence and stability. Despite these successes, however, key functions remain absent. In this work, we address a critical missing function by integrating the Pockels effect into a semiconductor laser. Using a hybrid integrated III-V/Lithium Niobate structure, we demonstrate several essential capabilities that have not existed in previous integrated lasers. These include a record-high frequency modulation speed of 2 exahertz/s (2.0 × 1018Hz/s) and fast switching at 50 MHz, both of which are made possible by integration of the electro-optic effect. Moreover, the device co-lases at infrared and visible frequencies via the second-harmonic frequency conversion process, the first such integrated multi-color laser. Combined with its narrow linewidth and wide tunability, this new type of integrated laser holds promise for many applications including LiDAR, microwave photonics, atomic physics, and AR/VR.

  5. Thioamides are ‘single-atom’ isosteres of amide bonds that have found broad applications in organic synthesis, biochemistry and drug discovery. In this New Talent themed issue, we present a general strategy for activation of N–C(S) thioamide bonds by ground-state-destabilization. This concept is outlined in the context of a full study on transamidation of thioamides with nucleophilic amines, and relies on (1) site-selective N -activation of the thioamide bond to decrease resonance and (2) highly chemoselective nucleophilic acyl addition to the thioamide CS bond. The follow-up collapse of the tetrahedral intermediate is favored by the electronic properties of the amine leaving group. The ground-state-destabilization concept of thioamides enables weakening of the N–C(S) bond and rationally modifies the properties of valuable thioamide isosteres for the development of new methods in organic synthesis. We fully expect that in analogy to the burgeoning field of destabilized amides introduced by our group in 2015, the thio amide bond ground-state-destabilization activation concept will find broad applications in various facets of chemical science, including metal-free, metal-catalyzed and metal-promoted reaction pathways.
  6. Abstract

    Ultrahigh surface-to-volume ratio in nanoscale materials, could dramatically facilitate mass transport, leading to surface-mediated diffusion similar to Coble-type creep in polycrystalline materials. Unfortunately, the Coble creep is just a conceptual model, and the associated physical mechanisms of mass transport have never been revealed at atomic scale. Akin to the ambiguities in Coble creep, atomic surface diffusion in nanoscale crystals remains largely unclear, especially when mediating yielding and plastic flow. Here, by using in situ nanomechanical testing under high-resolution transmission electron microscope, we find that the diffusion-assisted dislocation nucleation induces the transition from a normal to an inverse Hall-Petch-like relation of the strength-size dependence and the surface-creep leads to the abnormal softening in flow stress with the reduction in size of nanoscale silver, contrary to the classical “alternating dislocation starvation” behavior in nanoscale platinum. This work provides insights into the atomic-scale mechanisms of diffusion-mediated deformation in nanoscale materials, and impact on the design for ultrasmall-sized nanomechanical devices.