Effect of Twist Angle on Interfacial Thermal Transport in Two-Dimensional Bilayers.

Advances in two-dimensional (2D) devices require innovative approaches for manipulating transport properties. Analogous to the electrical and optical responses, it has been predicted that thermal transport across 2D materials can have a similar strong twist-angle dependence. Here, we report experimental evidence deviating from this understanding. In contrast to the large tunability in electrical transport, we measured an unexpected weak twist-angle dependence of interfacial thermal transport in MoS2 bilayers, which is consistent with theoretical calculations. More notably, we confirmed the existence of distinct regimes with weak and strong twist-angle dependencies for thermal transport, where, for example, a much stronger change with twist angles is expected for graphene bilayers. With atomic simulations, the distinct twist-angle effects on different 2D materials are explained by the suppression of long-wavelength phonons via the moiré superlattice. These findings elucidate the unique feature of 2D thermal transport and enable a new design space for engineering thermal devices.

Kinetics of Sorption in Hygroscopic Hydrogels.

Hygroscopic hydrogels hold significant promise for high-performance atmospheric water harvesting, passive cooling, and thermal management. However, a mechanistic understanding of the sorption kinetics of hygroscopic hydrogels remains elusive, impeding an optimized design and broad adoption. Here, we develop a generalized two-concentration model (TCM) to describe the sorption kinetics of hygroscopic hydrogels, where vapor transport in hydrogel micropores and liquid transport in polymer nanopores are coupled through the sorption at the interface. We show that the liquid transport due to the chemical potential gradient in the hydrogel plays an important role in the fast kinetics. The high water uptake is attributed to the expansion of hydrogel during liquid transport. Moreover, we identify key design parameters governing the kinetics, including the initial porosity, hydrogel thickness, and shear modulus. This work provides a generic framework of sorption kinetics, which bridges the knowledge gap between the fundamental transport and practical design of hygroscopic hydrogels.

Wetting States and Departure Diameters of Bubbles on Micro-/Nanostructured Surfaces.

Wetting states for droplets have been extensively investigated in the past. As the counter phase of the droplets, bubbles' wetting states have rarely been systematically explored. The wetting state of a bubble is closely related to its departure diameter, which plays significant roles in bubble-generated processes in boiling heat transfer and gas-evolving reactions. Based on the principle of minimum surface energy, we explicitly define three equilibrium wetting states (hemi-wicking state, Wenzel state, and Cassie-Baxter state) for bubbles on micro-/nanostructured surfaces in this paper. We analyze the three-phase contact line profiles for bubbles under these wetting states and propose theoretical models for predicting departure diameters of hemi-wicking-state bubble and Wenzel-state bubble on micro-/nanostructured surfaces. We identify competing effects of bubble departure in Wenzel state: the augmentation of contact line length due to the roughness, which would delay bubble departure, and the decrease of contact line length due to the reduced apparent contact angle, which would facilitate bubble departure. We demonstrate that hemi-wicking-state bubble exhibits a much smaller departure diameter on the textured surfaces. These findings are supported by numerical simulations by the three-dimensional (3D) multiple-relaxation-time lattice Boltzmann method. It is found that the length of the outermost contact lines instead of all contact lines determines the departure diameter of hemi-wicking-state bubble based on bubble detachment processes captured by our 3D numerical simulations. This work offers an avenue for the accurate prediction and control of bubble departure behaviors from micro-/nanostructured surfaces, and therefore can guide optimal designs of micro-/nanostructured surfaces in a variety of applications in boiling, desalination, and hydrogen production by electrolysis.

How Coalescing Bubbles Depart from a Wall.

Bubble evolution plays a fundamental role in boiling and gas-evolving electrochemical systems. One key stage is bubble departure, which is traditionally considered to be buoyancy-driven. However, conventional understanding cannot provide the full physical picture, especially for departure events with small bubble sizes commonly observed in water splitting and high heat flux boiling experiments. Here, we report a new regime of bubble departure owing to the coalescence of two bubbles, where the departure diameter can be much smaller than the conventional buoyancy limit. We show the significant reduction of the bubble base area due to the dynamics of the three-phase contact line during coalescence, which promotes bubble departure. More importantly, combining buoyancy-driven and coalescence-induced bubble departure modes, we demonstrate a unified relationship between the departure diameter and nucleation site density. By elucidating how coalescing bubbles depart from a wall, our work provides design guidelines for energy systems which can largely benefit from efficient bubble departure.

Transport-Based Modeling of Bubble Nucleation on Gas Evolving Electrodes.

Bubble nucleation is ubiquitous in gas evolving reactions that are instrumental for a variety of electrochemical systems. Fundamental understanding of the nucleation process, which is critical to system optimization, remains limited as prior works generally focused on the thermodynamics and have not considered the coupling between surface geometries and different forms of transport in the electrolytes. Here, we establish a comprehensive transport-based model framework to identify the underlying mechanism for bubble nucleation on gas evolving electrodes. We account for the complex effects on the electrical field, ion migration, ion diffusion, and gas diffusion arising from surface heterogeneities and gas pockets initiated from surface crevices. As a result, we show that neglecting these effects leads to significant underprediction of the energy needed for nucleation. Our model provides a non-monotonic relationship between the surface cavity size and the overpotential required for nucleation, which is physically more consistent than the monotonic relationship suggested by a traditional thermodynamics-based model. We also identify the significance of the gas diffuse layer thickness, a parameter controlled by external flow fields and overall electrode geometries, which has been largely overlooked in previous models. Our model framework offers guidelines for practical electrochemical systems whereby, without changing the surface chemistry, nucleation on electrodes can be tuned by engineering the cavity size and the gas diffuse layer thickness.

Thermal Expansion Coefficient of Monolayer Molybdenum Disulfide Using Micro-Raman Spectroscopy.

Atomically thin two-dimensional (2D) materials have shown great potential for applications in nanoscale electronic and optical devices. A fundamental property of these 2D flakes that needs to be well-characterized is the thermal expansion coefficient (TEC), which is instrumental to the dry transfer process and thermal management of 2D material-based devices. However, most of the current studies of 2D materials' TEC extensively rely on simulations due to the difficulty of performing experimental measurements on an atomically thin, micron-sized, and optically transparent 2D flake. In this work, we present a three-substrate approach to characterize the TEC of monolayer molybdenum disulfide (MoS2) using micro-Raman spectroscopy. The temperature dependence of the Raman peak shift was characterized with three different substrate conditions, from which the in-plane TEC of monolayer MoS2 was extracted on the basis of lattice symmetries. Independently from two different phonon modes of MoS2, we measured the in-plane TECs as (7.6 ± 0.9) × 10-6 K-1 and (7.4 ± 0.5) × 10-6 K-1, respectively, which are in good agreement with previously reported values based on first-principle calculations. Our work is not only useful for thermal mismatch reduction during material transfer or device operation but also provides a general experimental method that does not rely on simulations to study key properties of 2D materials.

Theoretical and experimental investigation of haze in transparent aerogels.

Haze in optically transparent aerogels severely degrades the visual experience, which has prevented their adoption in windows despite their outstanding thermal insulation property. Previous studies have primarily relied on experiments to characterize haze in aerogels, however, a theoretical framework to systematically investigate haze in porous media is lacking. In this work, we present a radiative transfer model that can predict haze in aerogels based on their physical properties. The model is validated using optical characterization of custom-fabricated, highly-transparent monolithic silica aerogels. The fundamental relationships between the aerogel structure and haze highlighted in this study could lead to a better understanding of light-matter interaction in a wide range of transparent porous materials and assist in the development of low-haze silica aerogels for high-performance glazing units to reduce building energy consumption.

Regularized pseudo-phase imaging for inspecting and sensing nanoscale features.

Recovering tiny nanoscale features using a general optical imaging system is challenging because of poor signal to noise ratio. Rayleigh scattering implies that the detectable signal of an object of size d illuminated by light of wavelength λ is proportional to d6/λ4, which may be several orders of magnitude weaker than that of additive and multiplicative perturbations in the background. In this article, we solve this fundamental issue by introducing the regularized pseudo-phase, an observation quantity for polychromatic visible light microscopy that seems to be more sensitive than conventional intensity images for characterizing nanoscale features. We achieve a significant improvement in signal to noise ratio without making any changes to the imaging hardware. In addition, this framework not only retains the advantages of conventional denoising techniques, but also endows this new measurand (i.e., the pseudo-phase) with an explicit physical meaning analogous to optical phase. Experiments on a NIST reference material 8820 sample demonstrate that we can measure nanoscale defects, minute amounts of tilt in patterned samples, and severely noise-polluted nanostructure profiles with the pseudo-phase framework even when using a low-cost bright-field microscope.

Multiscale Dynamic Growth and Energy Transport of Droplets during Condensation.

Condensation is an important physical process and has direct relevance for a range of engineering applications, including heat transfer, antifrosting, and self-cleaning. Understanding the mechanism of droplet growth during condensation is an important aspect, but past works have not typically considered the dynamics of the multiscale process. In this paper, we developed a dynamic growth model, which considers the continuous and multiscale nature of the droplet growth process from several nanometers to hundreds of microns. This model couples the transient phase change heat transfer and two-phase flow both inside and outside the droplet. Accordingly, the energy transport is distinct from the classical pure conduction model. We show that convection near the liquid-vapor interface and inside the droplets plays an increasingly important role as droplets grow and finally dominates the energy transport process. Driven by strong convection, the droplets mix well and the discrete layers of temperature observed in the pure conduction model disappear at the microscale. This model that considers convection can lead to over 4 times higher predicted overall heat transfer than that obtained with the pure conduction model. The interfacial mass flow through the liquid-vapor interface is the dominant factor responsible for the strong convection. We studied the critical radius where convection starts to have a significant influence on droplet growth under different subcooling temperatures and contact angles. Droplets have smaller critical radii under larger subcooling temperatures or larger contact angles, ranging from 0.5 to 20 µm. This work identifies the modes of energy transport in condensation at different scales, which not only enhances our fundamental understanding of individual droplet growth but provides design guidelines for various dropwise and jumping-droplet condensation research.

Autonomous Atmospheric Water Harvesting over a Wide RH Range Enabled by Super Hygroscopic Composite Aerogels.

Sorption-based atmospheric water harvesting (SAWH) offers a sustainable strategy to address the global freshwater shortage. However, obtaining sorbents with excellent performance over a wide relative humidity (RH) range and devices with fully autonomous water production remains challenging. Herein, magnesium chloride (MgCl2) is innovatively converted into super hygroscopic magnesium complexes(MC), which can effectively solve the problems of salt deliquescence and agglomeration. The MC are then integrated with photothermal aerogels composed of sodium alginate and carbon nanotubes (SA/CNTs) to form composite aerogels, which showed high water uptake over a wide RH range, reaching 5.43 and 0.27 kg kg-1 at 95% and 20% RH, respectively. The hierarchical porous structure enables the as-prepared SA/CNTs/MC to exhibit rapid absorption/desorption kinetics with 12 cycles per day at 70% RH, equivalent to a water yield of 10.0 L kg-1 day-1. To further realize continuous and practical freshwater production, a fully solar-driven autonomous atmospheric water generator is designed and constructed with two SA/CNTs/MC-based absorption layers, which can alternately conduct the water absorption/desorption process without any other energy consumption. The design provides a promising approach to achieving autonomous, high-performance, and scalable SAWH.

Unusual Temperature Dependence of Water Sorption in Semicrystalline Hydrogels.

Water vapor sorption is a ubiquitous phenomenon in nature and plays an important role in various applications, including humidity regulation, energy storage, thermal management, and water harvesting. In particular, capturing moisture at elevated temperatures is highly desirable to prevent dehydration and to enlarge the tunability of water uptake. However, owing to the thermodynamic limit of conventional materials, sorbents inevitably tend to capture less water vapor at higher temperatures, impeding their broad applications. Here, an inverse temperature dependence of water sorption in poly(ethylene glycol) (PEG) hydrogels, where their water uptake can be doubled with increasing temperature from 25 to 50 °C, is reported. With mechanistic modeling of water-polymer interactions, this unusual water sorption is attributed to the first-order phase transformation of PEG structures, and the key parameters for a more generalized strategy in materials development are identified. This work elucidates a new regime of water sorption with an unusual temperature dependence, enabling a promising engineering space for harnessing moisture and heat.

Three-Tier Hierarchical Structures for Extreme Pool Boiling Heat Transfer Performance.

Boiling is an effective energy-transfer process with substantial utility in energy applications. Boiling performance is described mainly by the heat-transfer coefficient (HTC) and critical heat flux (CHF). Recent efforts for the simultaneous enhancement of HTC and CHF have been limited by an intrinsic trade-off between them-HTC enhancement requires high nucleation-site density, which can increase bubble coalescence resulting in limited CHF enhancement. In this work, this trade-off is overcome by designing three-tier hierarchical structures. The bubble coalescence is minimized to enhance the CHF by defining nucleation sites with microcavities interspersed within hemi-wicking structures. Meanwhile, the reduced nucleation-site density is compensated for by incorporating nanostructures that promote evaporation for HTC enhancement. The hierarchical structures demonstrate the simultaneous enhancement of HTC and CHF up to 389% and 138%, respectively, compared to a smooth surface. This extreme boiling performance can lead to significant energy savings in a variety of boiling applications.

Highly efficient and salt rejecting solar evaporation via a wick-free confined water layer.

Recent advances in thermally localized solar evaporation hold significant promise for vapor generation, seawater desalination, wastewater treatment, and medical sterilization. However, salt accumulation is one of the key bottlenecks for reliable adoption. Here, we demonstrate highly efficient (>80% solar-to-vapor conversion efficiency) and salt rejecting (20 weight % salinity) solar evaporation by engineering the fluidic flow in a wick-free confined water layer. With mechanistic modeling and experimental characterization of salt transport, we show that natural convection can be triggered in the confined water. More notably, there exists a regime enabling simultaneous thermal localization and salt rejection, i.e., natural convection significantly accelerates salt rejection while inducing negligible additional heat loss. Furthermore, we show the broad applicability by integrating this confined water layer with a recently developed contactless solar evaporator and report an improved efficiency. This work elucidates the fundamentals of salt transport and offers a low-cost strategy for high-performance solar evaporation.

A unified approach and descriptor for the thermal expansion of two-dimensional transition metal dichalcogenide monolayers.

Two-dimensional (2D) materials have enabled promising applications in modern miniaturized devices. However, device operation may lead to substantial temperature rise and thermal stress, resulting in device failure. To address such thermal challenges, the thermal expansion coefficient (TEC) needs to be well understood. Here, we characterize the in-plane TECs of transition metal dichalcogenide (TMD) monolayers and demonstrate superior accuracy using a three-substrate approach. Our measurements confirm the physical range of 2D monolayer TECs and, hence, address the more than two orders of magnitude discrepancy in literature. Moreover, we identify the thermochemical electronegativity difference of compositional elements as a descriptor, enabling the fast estimation of TECs for various TMD monolayers. Our work presents a unified approach and descriptor for the thermal expansion of TMD monolayers, which can serve as a guideline toward the rational design of reliable 2D devices.

Toward Optimal Heat Transfer of 2D-3D Heterostructures via van der Waals Binding Effects.

Two-dimensional (2D) materials and their heterogeneous integration have enabled promising electronic and photonic applications. However, significant thermal challenges arise due to numerous van der Waals (vdW) interfaces limiting the dissipation of heat generated in the device. In this work, we investigate the vdW binding effect on heat transport through a MoS2-amorphous silica heterostructure. We show using atomistic simulations that the cross-plane thermal conductance starts to saturate with the increase of vdW binding energy, which is attributed to substrate-induced localized phonons. With these atomistic insights, we perform device-level heat transfer optimizations. Accordingly, we identify a regime, characterized by the coupling of in-plane and cross-plane heat transport mediated by vdW binding energy, where maximal heat dissipation in the device is achieved. These results elucidate fundamental heat transport through the vdW heterostructure and provide a pathway toward optimizing thermal management in 2D nanoscale devices.

Quasi-Newtonian Environmental Scanning Electron Microscopy (QN-ESEM) for Monitoring Material Dynamics in High-Pressure Gaseous Environments.

Environmental scanning electron microscopy (ESEM) is a powerful technique that enables imaging of diverse specimens (e.g., biomaterials, chemical materials, nanomaterials) in a hydrated or native state while simultaneously maintaining micro-to-nanoscale resolution. However, it is difficult to achieve high signal-to-noise and artifact-free secondary electron images in a high-pressure gaseous environment due to the intensive electron-gas collisions. In addition, nanotextured substrates can mask the signal from a weakly scattering sample. These drawbacks limit the study of material dynamics under extreme conditions and correspondingly our understanding in many fields. In this work, an imaging framework called Quasi-Newtonian ESEM is proposed, which introduces the concepts of quasi-force and quasi-work by referencing the scattering force in light-matter interactions, to break these barriers without any hardware changes. It is shown that quasi-force is a more fundamental quantity that has a more significant connection with the sample morphology than intensity in the strongly scattering regime. Experimental and theoretical studies on the dynamics of droplet condensation in a high-pressure environment (up to 2500 Pa) successfully demonstrate the effectiveness and robustness of the framework and that the overwhelmed signal of interest in ESEM images can be reconstructed through information stored in the time domain, i.e., frames captured at different moments.

Wide-Field Magnetic Field and Temperature Imaging Using Nanoscale Quantum Sensors.

The simultaneous imaging of magnetic fields and temperature (MT) is important in a range of applications, including studies of carrier transport and semiconductor device characterization. Techniques exist for separately measuring temperature (e.g., infrared (IR) microscopy, micro-Raman spectroscopy, and thermo-reflectance microscopy) and magnetic fields (e.g., scanning probe magnetic force microscopy and superconducting quantum interference devices). However, these techniques cannot measure magnetic fields and temperature simultaneously. Here, we use the exceptional temperature and magnetic field sensitivity of nitrogen vacancy (NV) spins in conformally coated nanodiamonds to realize simultaneous wide-field MT imaging at the device level. Our "quantum conformally attached thermo-magnetic" (Q-CAT) imaging enables (i) wide-field, high-frame rate imaging (100-1000 Hz); (ii) high sensitivity; and (iii) compatibility with standard microscopes. We apply this technique to study the industrially important problem of characterizing multifinger gallium nitride high-electron mobility transistors (GaN HEMTs). We spatially and temporally resolve the electric current distribution and resulting temperature rise, elucidating functional device behavior at the microscopic level. The general applicability of Q-CAT imaging serves as an important tool for understanding complex MT phenomena in material science, device physics, and related fields.

Enhanced Environmental Scanning Electron Microscopy Using Phase Reconstruction and Its Application in Condensation.

Environmental scanning electron microscopy (ESEM) is a broadly utilized nanoscale inspection technique capable of imaging wet or insulating samples. It extends the application of conventional scanning electron microscopy (SEM) and has been extensively used to study the behavior of liquid, polymer, and biomaterials by allowing for a gaseous environment. However, the presence of gas in the chamber can severely degrade the image resolution and contrast. This typically limits the ESEM operating pressure below 1000 Pa. The dynamic interactions, which require even-higher sensitivity and resolution, are particularly challenging to resolve at high-pressure conditions. Here, we present an enhanced ESEM technique using phase reconstruction to extend the limits of the ESEM operating pressure while improving the image quality, which is useful for sensing weak scattering from transparent or nanoscale samples. We applied this method to investigate the dynamics of condensing droplets, as an example case, which is of fundamental importance and has many industrial applications. We visualized dynamic processes such as single-droplet growth and droplet coalescence where the operating pressure range was extended from 1000 to 2500 Pa. Moreover, we detected the distribution of nucleation sites on the nanostructured surfaces. Such nanoscale sensing has been challenging previously due to the limitation of resolution and sensitivity. Our work provides a simple approach for high-performance ESEM imaging at high-pressure conditions without changes to the hardware and can be widely applied to investigate a broad range of static and dynamic processes.

Simultaneous measurement of temperature, stress, and electric field in GaN HEMTs with micro-Raman spectroscopy.

As semiconductor devices based on silicon reach their intrinsic material limits, compound semiconductors, such as gallium nitride (GaN), are gaining increasing interest for high performance, solid-state transistor applications. Unfortunately, higher voltage, current, and/or power levels in GaN high electron mobility transistors (HEMTs) often result in elevated device temperatures, degraded performance, and shorter lifetimes. Although micro-Raman spectroscopy has become one of the most popular techniques for measuring localized temperature rise in GaN HEMTs for reliability assessment, decoupling the effects of temperature, mechanical stress, and electric field on the optical phonon frequencies measured by micro-Raman spectroscopy is challenging. In this work, we demonstrate the simultaneous measurement of temperature rise, inverse piezoelectric stress, thermoelastic stress, and vertical electric field via micro-Raman spectroscopy from the shifts of the E2 (high), A1 longitudinal optical (LO), and E2 (low) optical phonon frequencies in wurtzite GaN. We also validate experimentally that the pinched OFF state as the unpowered reference accurately measures the temperature rise by removing the effect of the vertical electric field on the Raman spectrum and that the vertical electric field is approximately the same whether the channel is open or closed. Our experimental results are in good quantitative agreement with a 3D electro-thermo-mechanical model of the HEMT we tested and indicate that the GaN buffer acts as a semi-insulating, p-type material due to the presence of deep acceptors in the lower half of the bandgap. This implementation of micro-Raman spectroscopy offers an exciting opportunity to simultaneously probe thermal, mechanical, and electrical phenomena in semiconductor devices under bias, providing unique insight into the complex physics that describes device behavior and reliability. Although GaN HEMTs have been specifically used in this study to demonstrate its viability, this technique is applicable to any solid-state material with a suitable Raman response and will likely enable new measurement capabilities in a wide variety of scientific and engineering applications.