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Register a new userCapillary condensation under atomic-scale confinement
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Capillary condensation of water is ubiquitous in nature and technology. It routinely occurs in granular and porous media, can strongly alter such properties as adhesion, lubrication, friction and corrosion, and is important in many processes employed by microelectronics, pharmaceutical, food and other industries. The century-old Kelvin equation is commonly used to describe condensation phenomena and shown to hold well for liquid menisci with diameters as small as several nm. For even smaller capillaries that are involved in condensation under ambient humidity and, hence, of particular practical interest, the Kelvin equation is expected to break down, because the required confinement becomes comparable to the size of water molecules. Here we take advantage of van der Waals assembly of two-dimensional crystals to create atomic-scale capillaries and study condensation inside. Our smallest capillaries are less than 4 angstroms in height and can accommodate just a monolayer of water. Surprisingly, even at this scale, the macroscopic Kelvin equation using the characteristics of bulk water is found to describe accurately the condensation transition in strongly hydrophilic (mica) capillaries and remains qualitatively valid for weakly hydrophilic (graphene) ones. We show that this agreement is somewhat fortuitous and can be attributed to elastic deformation of capillary walls, which suppresses giant oscillatory behavior expected due to commensurability between atomic-scale confinement and water molecules. Our work provides a much-needed basis for understanding of capillary effects at the smallest possible scale important in many realistic situations.
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We show that condensation in a capped capillary slit is a continuous interfacial critical phenomenon, related intimately to several other surface phase transitions. In three dimensions (3d), the adsorption and desorption branches correspond to the unbinding of the meniscus from the cap and opening, respectively and are equivalent to 2d-like complete-wetting transitions. For dispersion forces, the singularities on the two branches are distinct, owing to the different interplay of geometry and intermolecular forces. In 2d we establish precise connection, or covariance, with 2d critical-wetting and wedge-filling transitions, i.e. we establish that certain interfacial properties in very different geometries are identical. Our predictions of universal scaling and covariance in finite capillaries are supported by extensive Ising model simulation studies in 2d and 3d.
Using grand canonical Monte Carlo simulations, we have explored the phenomenon of capillary condensation (CC) of Ar at the triple temperature inside infinitely long, cylindrical pores. Pores of radius R= 1 nm, 1.7 nm and 2.5 nm have been investigated, using a gas-surface interaction potential parameterized by the well-depth D of the gas on a planar surface made of the same material as that comprising the porous host. For strongly attractive situations, i.e., large D, one or more (depending on R) Ar layers adsorb successively before liquid fills the pore. For very small values of D, in contrast, negligible adsorption occurs at any pressure P below saturated vapor pressure P0; above saturation, there eventually occurs a threshold value of P at which the coverage jumps from empty to full, nearly discontinuously. Hysteresis is found to occur in the simulation data whenever abrupt CC occurs, i.e. for R>= 1.7 nm, and for small D when R=1nm. Then, the pore-emptying branch of the adsorption isotherm exhibits larger N than the pore-filling branch, as is known from many experiments and simulation studies. The relation between CC and wetting on planar surfaces is discussed in terms of a threshold value of D, which is about one-half of the value found for the wetting threshold on a planar surface. This finding is consistent with a simple thermodynamic model of the wetting transition developed previously.
The excess adsorption $Gamma $ in two-dimensional Ising strips $(infty times L)$ subject to identical boundary fields, at both one-dimensional surfaces decaying in the orthogonal direction $j$ as $-h_1j^{-p}$, is studied for various values of $p$ and along various thermodynamic paths below the critical point by means of the density-matrix renormalization-group method. The crossover behavior between the complete wetting and critical adsorption regimes, occurring in semi-infinite systems, are strongly influenced by confinement effects. Along isotherms $T=const$ the asymptotic power law dependences on the external bulk field, which characterize these two regimes, are undercut by capillary condensation. Along the pseudo first-order phase coexistence line of the strips, which varies with temperature, we find a broad crossover regime where both the thickness of the wetting film and $Gamma$ increase as function of the reduced temperature $tau$ but do not follow any power law. Above the wetting temperature the order parameter profiles are not slab-like but exhibit wide interfacial variations and pronounced tails. Inter alia, our explicit calculations demonstrate that, contrary to opposite claims by Kroll and Lipowsky [Phys. Rev. B {bf 28}, 5273 (1983)], for $p=2$ critical wetting transitions do exist and we determine the corresponding wetting phase diagram in the $(h_1,T)$ plane.
The thermodynamic uncertainty relation (TUR) is expected to hold in nanoscale electronic conductors, when the electron transport process is quantum coherent and the transmission probability is constant (energy and voltage independent). We present measurements of the electron current and its noise in gold atomic-scale junctions and confirm the validity of the TUR for electron transport in realistic quantum coherent conductors. Furthermore, we show that it is beneficial to present the current and its noise as a TUR ratio in order to identify deviations from noninteracting-electron coherent dynamics.
A Bose-Einstein condensate is the ground state of a dilute gas of bosons, such as atoms cooled to temperatures close to absolute zero. With much smaller mass, excitons (bound electron-hole pairs) are expected to condense at significantly higher temperatures. Here we study electrically generated interlayer excitons in MoSe2/WSe2 atomic double layers with density up to 10^12 cm-2. The interlayer tunneling current depends only on exciton density, indicative of correlated electron-hole pair tunneling. Strong electroluminescence (EL) arises when a hole tunnels from WSe2 to recombine with electron in MoSe2. We observe a critical threshold dependence of the EL intensity on exciton density, accompanied by a super-Poissonian photon statistics near threshold, and a large EL enhancement peaked narrowly at equal electron-hole densities. The phenomenon persists above 100 K, which is consistent with the predicted critical condensation temperature. Our study provides compelling evidence for interlayer exciton condensation in two-dimensional atomic double layers and opens up exciting opportunities for exploring condensate-based optoelectronics and exciton-mediated high-temperature superconductivity.
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