The increasing interest in developing nanodevices for biophysical and biomedical applications results in concerns about thermal management at interfaces between tissues and electronic devices. However, there is neither sufficient knowledge nor suitable tools for the characterization of thermal properties at interfaces between materials of contrasting mechanics, which are essential for design with reliability. Here we use computational simulations to quantify thermal transfer across the cell membrane–graphene interface. We find that the intercalated water displays a layered order below a critical value of ∼1 nm nanoconfinement, mediating the interfacial thermal coupling, and efficiently enhancing the thermal dissipation. We thereafter develop an analytical model to evaluate the critical value for power generation in graphene before significant heat is accumulated to disturb living tissues. These findings may provide a basis for the rational design of wearable and implantable nanodevices in biosensing and thermotherapic treatments where thermal dissipation and transport processes are crucial.

With the rise of atomic-scale devices such as molecular electronics and scanning probe microscopies, energy transport processes through molecular junctions have attracted notable research interest recently. In this work, heat dissipation and transport across diamond/benzene/diamond molecular junctions are explored by performing atomistic simulations. We identify the critical power Pcr to maintain thermal stability of the junction through efficient dissipation of local heat. We also find that the molecule–probe contact features a power-dependent interfacial thermal resistance RK in the order of 109 kW−1. Moreover, both Pcr and RK display explicit dependence on atomic structures of the junction, force and temperature. For instance, Pcr can be elevated in multiple-molecule junctions, and streching the junction enhances RK by a factor of 2. The applications of these findings in molecular electronics and scanning probing measurements are discussed, providing practical guidelines in their rational design.

Water transport through graphene-derived membranes has gained much interest recently due to its promising potential in filtration and separation applications. In this work, we explore water permeation in graphene oxide membranes using atomistic simulations and theoretical analysis, by considering flow through the interlayer gallery, expanded channels such as wrinkles of interedge spaces, and pores within the sheet. We find that, although flow enhancement can be established by nanoconfinement, fast water transport through pristine graphene channels is prohibited by a prominent side-pinning effect from capillaries formed within oxidized regions. We then discuss several flow enhancement mechanisms through the porous microstructures of graphene oxide membranes. These understandings are integrated into a complete picture to understand water permeation through the layer-by-layer and porous microstructure and can guide rational design of functional membranes for energy and environmental applications.

Recent experimental studies have revealed unconventional phase and transport behaviors of water confined within lamellar graphene oxide membranes, which hold great promise not only in improving our current understanding of nanoconfined water but also in developing high-performance filtration and separation applications. In this work, we explore molecular structures and diffusive dynamics of water intercalated between graphene or graphene oxide sheets. We identify the monolayer structured water between graphene sheets at temperature T below Tc = ∼315 K and an interlayer distance d = 0.65 nm, which is absent as the sheets are oxidized. The non-continuum collective diffusion of water intercalation between graphene layers facilitates fast molecular transport due to reduced wall friction. This solid-like structural order of intercalated water is disturbed as T or d increases to a critical value, with abnormal declines in the coefficients of collective diffusion. Based on a patched model of graphene oxide sheets consisting of spatially distributed pristine and oxidized regions, we conclude that the non-continuum collective diffusion of intercalated water can explain fast water permeation through graphene oxide membranes as reported in recent experimental studies, in stark contrast to the conventional picture of pressure-driven continuum flow with boundary slip, which has been widely adopted in literature but may apply only at high humidity or in the fully hydrated conditions.

Graphene-based paper materials attract particular interests recently owing to their outstanding properties, the key of which is their layer-by-layer hierarchical structures similar to many biological materials such as bone, teeth and nacre, combining intralayer strong sp2 bonds and interlayer crosslinks for efficient load transfer. Here we firstly study the mechanical properties of various interlayer and intralayer crosslinks through first-principles calculations, and then perform continuum model analysis for the overall mechanical properties of graphene-based paper materials. We find that there is a characteristic length scale l0, defined as , where D is the stiffness of the graphene sheet, h0 and G are height of interlayer crosslink and shear modulus respectively. When the size of the graphene sheets exceeds 3l0, the tension–shear (TS) chain model, which is widely used for nanocomposites, fails to predict the overall mechanical properties of the graphene-based papers. Instead we proposed here a deformable tension–shear (DTS) model by considering elastic deformation of graphene sheets, also the interlayer and intralayer crosslinks. The DTS is then applied to predict the mechanical properties of graphene papers under tensile loading. According to the results we thus obtain, optimal design strategies are proposed for graphene papers with ultrahigh stiffness, strength and toughness.