RESUMEN
Ice, one of the most enigmatic materials on Earth, exhibits diverse polymorphism, with research mainly focusing on the most commonly observed phases: hexagonal ice (Ih), cubic ice (Ic), and stacking-disordered ice (Isd). While their formation or structural changes are crucial for advancements in cloud science, climate modeling, and cryogenic technology, the molecular mechanisms driving these phenomena remain unexplored. Herein, utilizing cryogenic transmission electron microscopy, we investigate the formation of ice at two different temperatures, demonstrating a size-dependent phase shift from Ic to Isd. Furthermore, a relatively metastable cubic phase in Isd transitions to a hexagonal phase under electron beam radiation. This transition, facilitated by crystal defects, contrasts with perfect crystalline Ic, which maintains its original phase, emphasizing the importance of defects in polymorphic phase transitions. Our findings provide novel insights on phase control during the ice growth processes and polymorphic phase transitions from the cubic-to-hexagonal phases.
RESUMEN
Single-molecule techniques are powerful microscopy methods that provide new insights into biological processes. Liquid-phase transmission electron microscopy (LP-TEM) is an ideal single-molecule technique for overcoming the poor spatiotemporal resolution of optical approaches. However, single-molecule LP-TEM is limited by several challenges such as electron-beam-induced molecular damage, difficulty in identifying biomolecular species, and a lack of analytical approaches for conformational dynamics. Herein, a single-molecule graphene liquid-cell TEM (GLC-TEM) technique that enables the investigation of real-time structural perturbations of intact amyloid fibrils is presented. It is demonstrated that graphene membranes significantly extend the observation period of native amyloid beta proteins without causing oxidative damage owing to electron beams, which is necessary for imaging. Stochastic and time-resolved investigations of single fibrils reveal that structural perturbations in the early fibrillar stage are responsible for the formation of various amyloid polymorphs. The advantage of observing structural behavior in real time with unprecedented resolution will potentially make GLC-TEM a complementary approach to other single-molecule techniques.
Asunto(s)
Grafito , Grafito/química , Amiloide/química , Electrones , Péptidos beta-Amiloides , Microscopía Electrónica de TransmisiónRESUMEN
We report the synthesis of ethylenediamine-intercalated NbSe2 and Li-ethylenediamine-intercalated MoSe2 single crystals with increased interlayer distances and their electronic structures measured by means of angle-resolved photoemission spectroscopy (ARPES). X-ray diffraction patterns and transmission electron microscopy images confirm the successful intercalation and an increase in the interlayer distance. ARPES measurement reveals that intercalated NbSe2 shows an electronic structure almost identical to that of monolayer NbSe2. Intercalated MoSe2 also returns the characteristic feature of the monolayer electronic structure, a direct band gap, which generates sizable photoluminescence even in the bulk form. Our results demonstrate that the properties and phenomena of the monolayer transition metal dichalcogenides can be achieved with large-scale bulk samples by blocking the interlayer interaction through intercalation.
RESUMEN
Graphene liquid cell electron microscopy (GLC-EM), a cutting-edge liquid-phase EM technique, has become a powerful tool to directly visualize wet biological samples and the microstructural dynamics of nanomaterials in liquids. GLC uses graphene sheets with a one carbon atom thickness as a viewing window and a liquid container. As a result, GLC facilitates atomic-scale observation while sustaining intact liquids inside an ultra-high-vacuum transmission electron microscopy chamber. Using GLC-EM, diverse scientific results have been recently reported in the material, colloidal, environmental, and life science fields. Here, the developments of GLC fabrications, such as first-generation veil-type cells, second-generation well-type cells, and third-generation liquid-flowing cells, are summarized. Moreover, recent GLC-EM studies on colloidal nanoparticles, battery electrodes, mineralization, and wet biological samples are also highlighted. Finally, the considerations and future opportunities associated with GLC-EM are discussed to offer broad understanding and insight on atomic-resolution imaging in liquid-state dynamics.
Asunto(s)
Grafito , Nanopartículas , Suministros de Energía Eléctrica , Microscopía Electrónica , Microscopía Electrónica de TransmisiónRESUMEN
Graphene liquid cell transmission electron microscopy allows in situ observation of nanomaterial dynamics in a liquid environment. However, this method suffers from both random formation and small size of liquid pockets. Here, we introduce facile and mass-producible graphene-sealed well-type liquid cells with rational designs. The developed liquid cell structure and its formation mechanism depending on hole diameter (d)/spacer thickness (h) ratio are systematically analyzed. Finally, we show its high-resolution imaging and chemical analysis capability for nanoparticles and biomaterial applications. This work will provide an enhanced liquid cell platform for diverse liquid environmental studies.