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Understanding and controlling vibrations in condensed matter is emerging as an essential necessity both at fundamental level and for the development of a broad variety of technological applications. Intelligent design of the band structure and transport properties of phonons at the nanoscale and of their interactions with electrons and photons impact the efficiency of nanoelectronic systems and thermoelectric materials, permit the exploration of quantum phenomena with micro- and nanoscale resonators, and provide new tools for spectroscopy and imaging. In this colloquium we assess the state of the art of nanophononics, describing the recent achievements and the open challenges in nanoscale heat transport, coherent phonon generation and exploitation, and in nano- and optomechanics. We also underline the links among the diverse communities involved in the study of nanoscale phonons, pointing out the common goals and opportunities.

In this study, we present a comprehensive analysis of the thermoelectric (TE) properties of highly c -axis-oriented thin films of layered misfit cobaltates Bi 2 Sr 2 Co 2 O y . The films exhibit a high c -axis orientation, facilitating precise measurements of electronic transport and TE properties along the a - b crystallographic plane. Our findings reveal that the presence of nearly stoichiometric oxygen content results in high thermopower with metallic conductivity, while the annealing of the films in a reduced oxygen atmosphere eliminates their metallic behavior. According to the well-established Heike's limit, the thermopower tends to become temperature independent when the thermal energy significantly exceeds the bandwidth, which provides a rough estimation of charge carrier density by using the Heike's formula. This observation suggests that the dominant contribution to the thermopower comes from the narrow Co-t 2g bands near the Fermi energy. Our study demonstrates that the calculated thermopower value using Heike's formula, based on the Hall electron density of the Bi 2 Sr 2 Co 2 O y thin films at 300 K, aligns well with the experimental results, shedding light on the intriguing TE properties of this family of layered cobaltate oxide films., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Effective thermal management of electronic devices encounters substantial challenges owing to the notable power densities involved. Here, we propose layered MoS 2 phononic crystals (PnCs) that can effectively reduce thermal conductivity (κ) with relatively small disruption of electrical conductivity (σ), offering a potential thermal management solution for nanoelectronics. These layered PnCs exhibit remarkable efficiency in reducing κ, surpassing that of Si and SiC PnCs with similar periodicity by ~100-fold. Specifically, in suspended MoS 2 PnCs, we measure an exceptionally low κ down to 0.1 watts per meter kelvin, below the amorphous limit while preserving the crystalline structure. These findings are supported by molecular dynamics simulations that account for the film thickness, porosity, and temperature. We demonstrate the approach efficiency by fabricating suspended heat-routing structures that effectively confine and guide heat flow in prespecified directions. This study underpins the immense potential of layered materials as directional heat spreaders, thermal insulators, and active components for thermoelectric devices.

Nanomaterials are driving advances in technology due to their oftentimes superior properties over bulk materials. In particular, their thermal properties become increasingly important as efficient heat dissipation is required to realize high-performance electronic devices, reduce energy consumption, and prevent thermal damage. One application where nanomaterials can play a crucial role is extreme ultraviolet (EUV) lithography, where pellicles that protect the photomask from particle contamination have to be transparent to EUV light, mechanically strong, and thermally conductive in order to withstand the heat associated with high-power EUV radiation. Free-standing carbon nanotube (CNT) films have emerged as candidates due to their high EUV transparency and ability to withstand heat. However, the thermal transport properties of these films are not well understood beyond bulk emissivity measurements. Here, we measure the thermal conductivity of free-standing CNT films using all-optical Raman thermometry at temperatures between 300 and 700 K. We find thermal conductivities up to 50 W m -1 K -1 for films composed of double-walled CNTs, which rises to 257 W m -1 K -1 when considering the CNT network alone. These values are remarkably high for randomly oriented CNT networks, roughly seven times that of single-walled CNT films. The enhanced thermal conduction is due to the additional wall, which likely gives rise to additional heat-carrying phonon modes and provides a certain resilience to defects. Our results demonstrate that free-standing double-walled CNT films efficiently dissipate heat, enhancing our understanding of these promising films and how they are suited to applications in EUV lithography.

This experimental study investigates thermal rectification via asymmetric far-field thermal radiation on a fused silica slab. An asymmetrical distribution of surface emissivity is created over the device by partially covering the fused silica with a 100 nm thick aluminum film. The slab is subjected to a thermal bias, and when this bias is reversed, a small temperature difference is observed between the different configurations. This temperature difference arises from the difference in emissivity between the aluminum layer and fused silica, resulting in the transfer of thermal energy to the surrounding environment through radiation. Experimental findings are supported by finite element simulations, which not only confirm the measured values but also provide valuable insights into the rectification efficiency of the system. The rectification efficiency is found to be approximately 50% at room temperature for a thermal bias of 140 K. Simulations, which are performed by considering different environmental conditions experienced by the radiation and free convection processes, provide further insight into the underlying thermal rectification mechanism. These simulations consider an environmental temperature of 4 K for thermal radiation and an ambient temperature of 294 K for free convection and reveal an enhanced rectification effect with a rectification efficiency up to 600% when a thermal bias of 195 K is applied. This result emphasizes the significance of considering both convection and radiation in the thermal management and rectification of asymmetric systems. The outcomes of this study further our understanding of the thermal rectification phenomenon. They also show the importance of system asymmetry, emissivity disparities, environmental conditions, and the interplay between convection and radiation. Furthermore, the findings have implications for heat transfer and rectification in asymmetric systems, offering potential applications in areas such as energy harvesting, thermal management, and heat transfer optimization in electronic devices., Competing Interests: The authors declare no competing financial interest., (© 2023 The Authors. Published by American Chemical Society.)

Artificially engineered 2D materials offer unique physical properties for thermal management, surpassing naturally occurring materials. Here, using van der Waals epitaxy, we demonstrate the ability to engineer extremely insulating thermal metamaterials based on atomically thin lattice-mismatched Bi 2 Se 3 /MoSe 2 superlattices and graphene/PdSe 2 heterostructures with exceptional thermal resistances (70-202 m 2 K/GW) and ultralow cross-plane thermal conductivities (0.012-0.07 W/mK) at room temperature, comparable to those of amorphous materials. Experimental data obtained using frequency-domain thermoreflectance and low-frequency Raman spectroscopy, supported by tight-binding phonon calculations, reveal the impact of lattice mismatch, phonon-interface scattering, size effects, temperature, and interface thermal resistance on cross-plane heat dissipation, uncovering different thermal transport regimes and the dominant role of long-wavelength phonons. Our findings provide essential insights into emerging synthesis and thermal characterization methods and valuable guidance for the development of large-area heteroepitaxial van der Waals films of dissimilar materials with tailored thermal transport characteristics.

Nanophononics has the potential for information transfer, in an analogous manner to its photonic and electronic counterparts. The adoption of phononic systems has been limited, due to difficulties associated with the generation, manipulation, and detection of phonons, especially at GHz frequencies. Existing techniques often require piezoelectric materials with an external radiofrequency excitation that are not readily integrated into existing CMOS infrastructures, while nonpiezoelectric demonstrations have been inefficient. In this Letter, we explore the optomechanical generation of coherent phonons in a suspended 2D silicon phononic crystal cavity with a guided mode around 6.8 GHz. By incorporating an air-slot into this cavity, we turn the phononic waveguide into an optomechanical platform that exploits localized photonic modes resulting from inherent fabrication imperfections for the transduction of mechanics. Such a platform exhibits very fine control of phonons using light, and is capable of coherent self-sustained phonon generation around 6.8 GHz, operating at room temperature. The ability to generate high frequency coherent mechanical vibrations within such a simple 2D CMOS-compatible system could be a first step towards the development of sources in phononic circuitry and the coherent manipulation of other solid-state properties.

Layered Bi-misfit cobaltates, such as Bi 2 Sr 2 Co 2 O y , are the natural superlattice of an electrically insulating rocksalt (RS) type Bi 2 Sr 2 O 4 layer and electrically conducting CoO 2 layer, stacked along the crystallographic c-axis. RS and CoO 2 layers are related through charge compensation reactions (or charge transfer). Therefore, thermoelectric transport properties are affected when doping or substitution is carried out in the RS layer. In this work, we have shown improved thermoelectric properties of spark plasma sintered Bi 2 Sr 2-x Ca x Co 2 O y alloys (x = 0, 0.3 and 0.5). The substitution of Ca atoms affects the thermal properties by introducing point-defect phonon scattering, while the electronic conductivity and thermopower remain unaltered.

This broad review summarizes recent advances and "hot" research topics in nanophononics and elastic, acoustic, and mechanical metamaterials based on results presented by the authors at the EUROMECH 610 Colloquium held on April 25-27, 2022 in Benicássim, Spain. The key goal of the colloquium was to highlight important developments in these areas, particularly new results that emerged during the last two years. This work thus presents a "snapshot" of the state-of-the-art of different nanophononics- and metamaterial-related topics rather than a historical view on these subjects, in contrast to a conventional review article. The introduction of basic definitions for each topic is followed by an outline of design strategies for the media under consideration, recently developed analysis and implementation techniques, and discussions of current challenges and promising applications. This review, while not comprehensive, will be helpful especially for early-career researchers, among others, as it offers a broad view of the current state-of-the-art and highlights some unique and flourishing research in the mentioned fields, providing insight into multiple exciting research directions., (© 2023 the author(s), published by De Gruyter, Berlin/Boston.)

Confining photons in cavities enhances the interaction between light and matter. In cavity optomechanics, this enables a wealth of phenomena ranging from optomechanically induced transparency to macroscopic objects cooled to their motional ground state. Previous work in cavity optomechanics employed devices where ubiquitous structural disorder played no role beyond perturbing resonance frequencies and quality factors. More generally, the interplay between disorder, which must be described by statistical physics, and optomechanical effects has thus far been unexplored. Here, we demonstrate how sidewall roughness in air-slot photonic-crystal waveguides can induce sufficiently strong backscattering of slot-guided light to create Anderson-localized modes with quality factors as high as half a million and mode volumes estimated to be below the diffraction limit. We observe how the interaction between these disorder-induced optical modes and in-plane mechanical modes of the slotted membrane is governed by a distribution of coupling rates, which can exceed g_{o}/2π∼200  kHz, leading to mechanical amplification up to self sustained oscillations via optomechanical backaction. Our Letter constitutes the first steps towards understanding optomechanics in the multiple-scattering regime and opens new perspectives for exploring complex systems with a multitude of mutually coupled degrees of freedom.

Phonons play a key role in the physical properties of materials, and have long been a topic of study in physics. While the effects of phonons had historically been considered to be a hindrance, modern research has shown that phonons can be exploited due to their ability to couple to other excitations and consequently affect the thermal, dielectric, and electronic properties of solid state systems, greatly motivating the engineering of phononic structures. Advances in nanofabrication have allowed for structuring and phonon confinement even down to the nanoscale, drastically changing material properties. Despite developments in fabricating such nanoscale devices, the proper manipulation and characterization of phonons continues to be challenging. However, a fundamental understanding of these processes could enable the realization of key applications in diverse fields such as topological phononics, information technologies, sensing, and quantum electrodynamics, especially when integrated with existing electronic and photonic devices. Here, we highlight seven of the available methods for the excitation and detection of acoustic phonons and vibrations in solid materials, as well as advantages, disadvantages, and additional considerations related to their application. We then provide perspectives towards open challenges in nanophononics and how the additional understanding granted by these techniques could serve to enable the next generation of phononic technological applications.

Controlling vibrations in solids is crucial to tailor their elastic properties and interaction with light. Thermal vibrations represent a source of noise and dephasing for many physical processes at the quantum level. One strategy to avoid these vibrations is to structure a solid such that it possesses a phononic stop band, that is, a frequency range over which there are no available elastic waves. Here we demonstrate the complete absence of thermal vibrations in a nanostructured silicon membrane at room temperature over a broad spectral window, with a 5.3-GHz-wide bandgap centred at 8.4 GHz. By constructing a line-defect waveguide, we directly measure gigahertz guided modes without any external excitation using Brillouin light scattering spectroscopy. Our experimental results show that the shamrock crystal geometry can be used as an efficient platform for phonon manipulation with possible applications in optomechanics and signal processing transduction., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

The substitution of extra virgin olive oil with other edible oils is the primary method for fraud in the olive-oil industry. Developing inexpensive analytical methods for confirming the quality and authenticity of olive oils is a major strategy towards combatting food fraud. Current methods used to detect such adulterations require complicated time- and resource-intensive preparation steps. In this work, a comparative study incorporating Raman and infrared spectroscopies, photoluminescence, and thermal-conductivity measurements of different sets of adulterated olive oils is presented. The potential of each characterization technique to detect traces of adulteration in extra virgin olive oils is evaluated. Concentrations of adulterant on the order of 5% can be detected in the Raman, infrared, and photoluminescence spectra. Small changes in thermal conductivity were also found for varying amounts of adulterants. While each of these techniques may individually be unable to identify impurity adulterants, the combination of these techniques together provides a holistic approach to validate the purity and authenticity of olive oils.

Passive radiative cooling (RC) enables the cooling of objects below ambient temperature during daytime without consuming energy, promising to be a game changer in terms of energy savings and CO 2 reduction. However, so far most RC surfaces are obtained by energy-intensive nanofabrication processes or make use of unsustainable materials. These limitations are overcome by developing cellulose films with unprecedentedly low absorption of solar irradiance and strong mid-infrared (mid-IR) emittance. In particular, a cellulose-derivative (cellulose acetate) is exploited to produce porous scattering films of two different thicknesses, L ≈ 30 µm (thin) and L ≈ 300 µm (thick), making them adaptable to above and below-ambient cooling applications. The thin and thick films absorb only ≈ 5 % ${\approx}5\%$ of the solar irradiance, which represents a net cooling power gain of at least 17 W m -2 , compared to state-of-the-art cellulose-based radiative-cooling materials. Field tests show that the films can reach up to ≈5 °C below ambient temperature, when solar absorption and conductive/convective losses are minimized. Under dryer conditions (water column = 1 mm), it is estimated that the films can reach average minimum temperatures of ≈7-8 °C below the ambient. The work presents an alternative cellulose-based material for efficient radiative cooling that is simple to fabricate, cost-efficient and avoids the use of polluting materials., (© 2022 The Authors. Advanced Science published by Wiley-VCH GmbH.)

Understanding heat flow in layered transition metal dichalcogenide (TMD) crystals is crucial for applications exploiting these materials. Despite significant efforts, several basic thermal transport properties of TMDs are currently not well understood, in particular how transport is affected by material thickness and the material's environment. This combined experimental-theoretical study establishes a unifying physical picture of the intrinsic lattice thermal conductivity of the representative TMD MoSe 2 . Thermal conductivity measurements using Raman thermometry on a large set of clean, crystalline, suspended crystals with systematically varied thickness are combined with ab initio simulations with phonons at finite temperature. The results show that phonon dispersions and lifetimes change strongly with thickness, yet the thinnest TMD films exhibit an in-plane thermal conductivity that is only marginally smaller than that of bulk crystals. This is the result of compensating phonon contributions, in particular heat-carrying modes around ≈0.1 THz in (sub)nanometer thin films, with a surprisingly long mean free path of several micrometers. This behavior arises directly from the layered nature of the material. Furthermore, out-of-plane heat dissipation to air molecules is remarkably efficient, in particular for the thinnest crystals, increasing the apparent thermal conductivity of monolayer MoSe 2 by an order of magnitude. These results are crucial for the design of (flexible) TMD-based (opto-)electronic applications., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Nanoelectro-opto-mechanical systems enable the synergistic coexistence of electrical, mechanical, and optical signals on a chip to realize new functions. Most of the technology platforms proposed for the fabrication of these systems so far are not fully compatible with the mainstream CMOS technology, thus, hindering the mass-scale utilization. We have developed a CMOS technology platform for nanoelectro-opto-mechanical systems that includes piezoelectric interdigitated transducers for electronic driving of mechanical signals and nanocrystalline silicon nanobeams for an enhanced optomechanical interaction. Room-temperature operation of devices at 2 GHz and with peak sensitivity down to 2.6 cavity phonons is demonstrated. Our proof-of-principle technology platform can be integrated and interfaced with silicon photonics, electronics, and MEMS devices and may enable multiple functions for coherent signal processing in the classical and quantum domains., Competing Interests: The authors declare no competing financial interest., (© 2022 American Chemical Society.)

The degree of thermal anisotropy affects critically key device-relevant properties of layered two-dimensional materials. Here, we systematically study the in-plane and cross-plane thermal conductivity of crystalline SnSe 2 films of varying thickness (16-190 nm) and uncover a thickness-independent thermal conductivity anisotropy ratio of about ∼8.4. Experimental data obtained using Raman thermometry and frequency domain thermoreflectance showed that the in-plane and cross-plane thermal conductivities monotonically decrease by a factor of 2.5 with decreasing film thickness compared to the bulk values. Moreover, we find that the temperature-dependence of the in-plane component gradually decreases as the film becomes thinner, and in the range from 300 to 473 K it drops by more than a factor of 2. Using the mean free path reconstruction method, we found that phonons with MFP ranging from ∼1 to 53 and from 1 to 30 nm contribute to 50% of the total in-plane and cross-plane thermal conductivity, respectively.

Precise patterning of 2D materials into micro- and nanostructures presents a considerable challenge and many efforts are dedicated to the development of processes alternative to the standard lithography. In this work we show a fabrication technique based on direct electron beam lithography (EBL) on MoS 2 on polydimethylsiloxane (PDMS) substrates. This easy and fast method takes advantage of the interaction of the electron beam with the PDMS, which at high enough doses leads to cross-linking and shrinking of the polymer. At the same time, the adhesion of MoS 2 to PDMS is enhanced in the exposed regions. The EBL acceleration voltages and doses are optimized in order to fabricate well-defined microstructures, which can be subsequently transferred to either a flexible or a rigid substrate, to obtain the negative of the exposed image. The reported procedure greatly simplifies the fabrication process and reduces the number of steps compared to standard lithography and etching. As no additional polymer, such as polymethyl methacrylate (PMMA) or photoresists, are used during the whole process the resulting samples are free of residues., Competing Interests: There are no conflicts of interest to declare., (This journal is © The Royal Society of Chemistry.)

Passive daytime radiative cooling has recently become an attractive approach to address the global energy demand associated with modern refrigeration technologies. One technique to increase the radiative cooling performance is to engineer the surface of a polar dielectric material to enhance its emittance at wavelengths in the atmospheric infrared transparency window (8-13 µm) by outcoupling surface-phonon polaritons (SPhPs) into free-space. Here we present a theoretical investigation of new surface morphologies based upon self-assembled silica photonic crystals (PCs) using an in-house built rigorous coupled-wave analysis (RCWA) code. Simulations predict that silica micro-sphere PCs can reach up to 73 K below ambient temperature, when solar absorption and conductive/convective losses can be neglected. Micro-shell structures are studied to explore the direct outcoupling of the SPhP, resulting in near-unity emittance between 8 and 10 µm. Additionally, the effect of material composition is explored by simulating soda-lime glass micro-shells, which, in turn, exhibit a temperature reduction of 61 K below ambient temperature. The RCWA code was compared to FTIR measurements of silica micro-spheres, self-assembled on microscope slides.

Two-dimensional materials, such as transition-metal dichalcogenides (TMDs), are attractive candidates for sensing applications due to their high surface-to-volume ratio, chemically active edges, and good electrical properties. However, their electrical response to humidity is still under debate and experimental reports remain inconclusive. For instance, in different studies, the impedance of MoS 2 -based sensors has been found to either decrease or increase with increasing humidity, compromising the use of MoS 2 for humidity sensing. In this work, we focus on understanding the interaction between water and TMDs. We fabricated and studied humidity sensors based on MoS 2 and WS 2 coated with copper chloride and silver nitrate. The devices exhibited high chemical stability and excellent humidity sensing performance in relative humidity between 4 and 80%, with response and recovery times of 2 and 40 s, respectively. We have systematically investigated the humidity response of the materials as a function of the type and amount of induced metal salt and observed the reverse action of sensing mechanisms. This phenomenon is explained based on a detailed structural analysis of the samples considering the Grotthuss mechanism in the presence of charge trapping, which was represented by an appropriate lumped-element model. Our findings open up a possibility to tune the electrical response in a facile manner and without compromising the high performance of the sensor. They offer an insight into the time-dependent performance and aging of the TMD-based sensing devices.

Optomechanical crystal cavities (OMC) have rich perspectives for detecting and indirectly analysing biological particles, such as proteins, bacteria and viruses. In this work we demonstrate the working principle of OMCs operating under ambient conditions as a sensor of submicrometer particles by optically monitoring the frequency shift of thermally activated mechanical modes. The resonator has been specifically designed so that the cavity region supports a particular family of low modal-volume mechanical modes, commonly known as -pinch modes-. These involve the oscillation of only a couple of adjacent cavity cells that are relatively insensitive to perturbations in other parts of the resonator. The eigenfrequency of these modes decreases as the deformation is localized closer to the centre of the resonator. Thus, by identifying specific modes that undergo a frequency shift that amply exceeds the mechanical linewidth, it is possible to infer if there are particles deposited on the resonator, how many are there and their approximate position within the cavity region. OMCs have rich perspectives for detecting and indirectly analysing biological particles, such as proteins, viruses and bacteria.

One strategy to decrease the incidence of hospital-acquired infections is to avoid the survival of pathogens in the environment by the development of surfaces with antimicrobial activity. To study the antibacterial behaviour of active surfaces, different approaches have been developed of which ISO 22916 is the standard. To assess the performance of different testing methodologies to analyse the antibacterial activity of hydrophobic surface patterned plastics as part of a Horizon 2020 European research project. Four different testing methods were used to study the antibacterial activity of a patterned film, including the ISO 22916 standard, the immersion method, the touch-transfer inoculation method, and the swab inoculation method, this latter developed specifically for this project. The non-realistic test conditions of the ISO 22916 standard showed this method to be non-appropriate in the study of hydrophobic patterned surfaces. The immersion method also showed no differences between patterned films and smooth controls due to the lack of attachment of testing bacteria on both surfaces. The antibacterial activity of films could be demonstrated by the touch-transfer and the swab inoculation methods, that more precisely mimicked the way of high-touch surfaces contamination, and showed to be the best methodologies to test the antibacterial activity of patterned hydrophobic surfaces. A new ISO standard would be desirable as the reference method to study the antibacterial behaviour of patterned surfaces.

The backscattering mean free path ξ, the average ballistic propagation length along a waveguide, quantifies the resistance of slow light against unwanted imperfections in the critical dimensions of the nanostructure. This figure of merit determines the crossover between acceptable slow-light transmission affected by minimal scattering losses and a strong backscattering-induced destructive interference when the waveguide length L exceeds ξ. Here, we calculate the backscattering mean free path for a topological photonic waveguide for a specific and determined amount of disorder and, equally relevant, for a fixed value of the group index n_{g} which is the slowdown factor of the group velocity with respect to the speed of light in vacuum. These two figures of merit, ξ and n_{g}, should be taken into account when quantifying the robustness of topological and conventional (nontopological) slow-light transport at the nanoscale. Otherwise, any claim on a better performance of topological guided light over a conventional one is not justified.

Heat dissipation and thermal management are central challenges in various areas of science and technology and are critical issues for the majority of nanoelectronic devices. In this review, we focus on experimental advances in thermal characterization and phonon engineering that have drastically increased the understanding of heat transport and demonstrated efficient ways to control heat propagation in nanomaterials. We summarize the latest device-relevant methodologies of phonon engineering in semiconductor nanostructures and 2D materials, including graphene and transition metal dichalcogenides. Then, we review recent advances in thermal characterization techniques, and discuss their main challenges and limitations.

The resonant enhancement of mechanical and optical interaction in optomechanical cavities enables their use as extremely sensitive displacement and force detectors. In this Letter, we demonstrate a hybrid magnetometer that exploits the coupling between the resonant excitation of spin waves in a ferromagnetic insulator and the resonant excitation of the breathing mechanical modes of a glass microsphere deposited on top. The interaction is mediated by magnetostriction in the ferromagnetic material and the consequent mechanical driving of the microsphere. The magnetometer response thus relies on the spectral overlap between the ferromagnetic resonance and the mechanical modes of the sphere, leading to a peak sensitivity of 850  pT Hz^{-1/2} at 206 MHz when the overlap is maximized. By externally tuning the ferromagnetic resonance frequency with a static magnetic field, we demonstrate sensitivity values at resonance around a few nT Hz^{-1/2} up to the gigahertz range. Our results show that our hybrid system can be used to build a high-speed sensor of oscillating magnetic fields.

Surface patterning technologies represent a worldwide growing industry, creating smart surfaces and micro/nanoscale device. The advent of large-area, high-speed imprinting technologies has created an ever-growing need for rapid and non-destructive dimensional metrology techniques to keep pace with the speed of production. Here we present a new real-time optical scatterometry technique, applicable at the mesoscale when optical inspection produces multiple orders of diffraction. We validate this method by inspecting multiple silicon gratings with a variety of structural parameters. These measurements are cross-referenced with FIB, SEM and scanning stylus profilometry. Finally, we measure thermally imprinted structures as a function of imprinting temperature in order to demonstrate the method suitable for in-line quality control in nanoimprint lithography.

The regulation of temperature is a major energy-consuming process of humankind. Today, around 15% of the global-energy consumption is dedicated to refrigeration and this figure is predicted to triple by 2050, thus linking global warming and cooling needs in a worrying negative feedback-loop. Here, an inexpensive solution is proposed to this challenge based on a single layer of silica microspheres self-assembled on a soda-lime glass. This 2D crystal acts as a visibly translucent thermal-blackbody for above-ambient radiative cooling and can be used to improve the thermal performance of devices that undergo critical heating during operation. The temperature of a silicon wafer is found to be 14 K lower during daytime when covered with the thermal emitter, reaching an average temperature difference of 19 K when the structure is backed with a silver layer. In comparison, the soda-lime glass reference used in the measurements lowers the temperature of the silicon by just 5 K. The cooling power of this simple radiative cooler under direct sunlight is found to be 350 W m -2 when applied to hot surfaces with relative temperatures of 50 K above the ambient. This is crucial to radiatively cool down devices, i.e., solar cells, where an increase in temperature has drastic effects on performance., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Novel thermoelectric materials developed for operation at room temperature must have similar or better performance along with being as ecofriendly as those commercially used, e.g. , Bi 2 Te 3 , in terms of their toxicity and cost. In this work, we present an in-depth study of the thermoelectric properties of epitaxial Nb-doped strontium titanate (SrTi 1- x Nb x O 3 ) thin films as a function of (i) doping concentration, (ii) film thickness and (iii) substrate type. The excellent crystal quality was confirmed by high resolution transmission electron microscopy and X-ray diffraction analysis. The thermoelectric properties were measured by the three-omega method (thermal conductivity) and van der Pauw method (electrical resistivity), complemented by Seebeck coefficient measurements. A maximum power factor of 8.9 × 10 -3 W m -1 K -2 and a thermoelectric figure of merit of 0.49 were measured at room temperature in 50 nm-thick films grown on lanthanum strontium aluminate. The mechanisms behind this high figure of merit are discussed in terms of a possible two-dimensional electron gas, increase of the effective mass of the electrons, electron filtering and change in strain due to different substrates. The overall enhancement of the thermoelectric properties suggests that SrTi 1- x Nb x O 3 is a very promising n-type candidate for room- to high-temperature applications., Competing Interests: There are not conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Pnictogen and chalcogenide compounds have been seen as high-potential materials for efficient thermoelectric conversion over the past few decades. It is also known that with nanostructuration, the physical properties of these pnictogen-chalcogenide compounds can be further enhanced towards a more efficient heat conversion. Here, we report the reduced thermal conductivity of a large ensemble of Bi2Te3 alloy nanowires (70 nm in diameter) with selenium for n-type and antimony for p-type (Bi2Te3-ySey and Bi2-xSbxTe3 respectively). The nanowire growth was carried out through electrodeposition in nanoporous aluminium oxide templates with high aspect ratios leading to a forest (109 per centimetre square) of nearly identical nanowires. The temperature dependence of thermal conductivity for the nanowire ensembles was acquired through a highly sensitive 3ω measurement technique. The change in the thermal conductivity of nanowires is largely affected by the roughness in addition to the size effect due to enhanced boundary scattering. The major factor that influences the thermal conductivity was found to be the ratio of the rms roughness to the correlation length of the nanowire. With a high Seebeck coefficient and electrical conductivity at room temperature, the overall thermoelectric figure of merit ZT allows the consideration of such forests of nanowires as efficient potential building blocks of future TE devices.

The synchronization of coupled oscillators is a phenomenon found throughout nature. Mechanical oscillators are paradigmatic examples, but synchronizing their nanoscaled versions is challenging. We report synchronization of the mechanical dynamics of a pair of optomechanical crystal cavities that, in contrast to previous works performed in similar objects, are intercoupled with a mechanical link and support independent optical modes. In this regime they oscillate in antiphase, which is in agreement with the predictions of our numerical model that considers reactive coupling. We also show how to temporarily disable synchronization of the coupled system by actuating one of the cavities with a heating laser, so that both cavities oscillate independently. Our results can be upscaled to more than two cavities and pave the way towards realizing integrated networks of synchronized mechanical oscillators.

In this work we study the effects of disorder on the thermal conductivity of porous 100 nm thick silicon membranes, in which the size, shape and position of the pores were varied randomly. Measurements using two-laser Raman thermometry on both non-patterned and porous membranes revealed more than a 10-fold reduction of the thermal conductivity compared to that of bulk silicon and a six-fold reduction compared to non-patterned membranes for the sample with random pore shapes. Using Monte Carlo methods we solved the Boltzmann transport equation for phonons and compared different possibilities of pore organization and its influence on the thermal conductivity of the samples. The simulations confirmed that the strongest reduction of thermal conductivity is achieved for a distribution of pores with arbitrary shapes that partially overlap. Up to a 15% reduction of the thermal conductivity with respect to the purely circular pores was predicted for a porous membrane with 37% filling fraction. The effect of the pore shape and distribution was further studied. Maps of temperature and heat flux distributions clearly showed that for particular pore placement heat transport can be efficiently blocked and hot spots can be found in narrow channels between pores. These findings have an impact on the fabrication of membrane-based thermoelectric devices, where low thermal conductivity is required. This work shows that for porous membranes with a given filling fraction the thermal conductivity can be further modified by introducing disorder in the shape and placement of the pores.

It is well known that by dispersing nanoparticles in a fluid, the thermal conductivity of the resulting nanofluid tends to increase with the concentration of nanoparticles. However, it is not clear what the mechanism behind this phenomenon is. Raman spectroscopy is a characterization technique connecting the molecular and macroscopic world, and therefore, it can unravel the puzzling effect exerted by the nanomaterial on the fluid. In this work, we report on a comparative study on the thermal conductivity, vibrational spectra and viscosity of graphene nanofluids based on three different amides: N , N -dimethylacetamide (DMAc); N , N -dimethylformamide (DMF); and N -methyl-2-pyrrolidinone (NMP). A set of concentrations of highly stable surfactant-free graphene nanofluids developed in-house was prepared and characterized. A correlation between the modification of the vibrational spectra of the fluids and an increase in their thermal conductivity in the presence of graphene was confirmed. Furthermore, an explanation of the non-modification of the thermal conductivity in graphene-NMP nanofluids is given based on its structure and a peculiar arrangement of the fluid.

The understanding of the mean free path (MFP) distribution of the energy carriers in materials (e.g., electrons, phonons, magnons, etc.) provides a key physical insight into their transport properties. In this context, MFP spectroscopy has become an important tool to describe the contribution of carriers with different MFP to the total transport phenomenon. In this work, we revise the MFP reconstruction technique and present a study on the impact of the regularization parameter on the MFP distribution of the energy carriers. By using the L-curve criterion, we calculate the optimal mathematical value of the regularization parameter. The effect of the change from the optimal value in the MFP distribution is analyzed in three case studies of heat transport by phonons. These results demonstrate that the choice of the regularization parameter has a large impact on the physical information obtained from the reconstructed accumulation function, and thus cannot be chosen arbitrarily. The approach can be applied to various transport phenomena at the nanoscale involving carriers of different physical nature and behavior.

Fundamental observations in physics ranging from gravitational wave detection to laser cooling of a nanomechanical oscillator into its quantum ground state rely on the interaction between the optical and the mechanical degrees of freedom. A key parameter to engineer this interaction is the spatial overlap between the two fields, optimized in carefully designed resonators on a case-by-case basis. Disorder is an alternative strategy to confine light and sound at the nanoscale. However, it lacks an a priori mechanism guaranteeing a high degree of colocalization due to the inherently complex nature of the underlying interference processes. Here, we propose a way to address this challenge by using GaAs/AlAs vertical distributed Bragg reflectors with embedded geometrical disorder. Because of a remarkable coincidence in the physical parameters governing light and motion propagation in these two materials, the equations for both longitudinal acoustic waves and normal-incidence light become practically equivalent for excitations of the same wavelength. This guarantees spatial overlap between the electromagnetic and displacement fields of specific photon-phonon pairs, leading to strong light-matter interaction. In particular, a statistical enhancement in the vacuum optomechanical coupling rate, g_{o}, is found, making this system a promising candidate to explore Anderson localization of high frequency (∼20  GHz) phonons enabled by cavity optomechanics. The colocalization effect shown here unlocks the access to unexplored localization phenomena and the engineering of light-matter interactions mediated by Anderson-localized states.

Hydrogel materials offer many advantages for chemical and biological sensoring due to their response to a small change in their environment with a related change in volume. Several designs have been outlined in the literature in the specific field of hydrogel-based optical sensors, reporting a large number of steps for their fabrication. In this work we present a three-dimensional, hydrogel-based sensor the structure of which is fabricated in a single step using thermal nanoimprint lithography. The sensor is based on a waveguide with a grating readout section. A specific hydrogel formulation, based on a combination of PEGDMA (Poly(Ethylene Glycol DiMethAcrylate)), NIPAAm (N-IsoPropylAcrylAmide), and AA (Acrylic Acid), was developed. This stimulus-responsive hydrogel is sensitive to pH and to water. Moreover, the hydrogel has been modified to be suitable for fabrication by thermal nanoimprint lithography. Once stimulated, the hydrogel-based sensor changes its topography, which is characterised physically by AFM and SEM, and optically using a specific optical set-up.

While the dispersion of nanomaterials is known to be effective in enhancing the thermal conductivity and specific heat capacity of fluids, the mechanisms behind this enhancement remain to be elucidated. Herein, we report on highly stable, surfactant-free graphene nanofluids, based on N,N-dimethylacetamide (DMAc) and N,N-dimethylformamide (DMF), with enhanced thermal properties. An increase of up to 48% in thermal conductivity and 18% in specific heat capacity was measured. The blue shift of several Raman bands with increasing graphene concentration in DMF indicates that there is a modification in the vibrational energy of the bonds associated with these modes, affecting all the molecules in the liquid. This result indicates that graphene has the ability to affect solvent molecules at long-range, in terms of vibrational energy. Density functional theory and molecular dynamics simulations were used to gather data on the interaction between graphene and solvent, and to investigate a possible order induced by graphene on the solvent. The simulations showed a parallel orientation of DMF towards graphene, favoring π-π stacking. Furthermore, a local order of DMF molecules around graphene was observed suggesting that both this special kind of interaction and the induced local order may contribute to the enhancement of the fluid's thermal properties.

Silicon on insulator photonics has offered a versatile platform for the recent development of integrated optomechanical circuits. However, there are some constraints such as the high cost of the wafers and limitation to a single physical device level. In the present work we investigate nanocrystalline silicon as an alternative material for optomechanical devices. In particular, we demonstrate that optomechanical crystal cavities fabricated of nanocrystalline silicon have optical and mechanical properties enabling non-linear dynamical behaviour and effects such as thermo-optic/free-carrier-dispersion self-pulsing, phonon lasing and chaos, all at low input laser power and with typical frequencies as high as 0.3 GHz.

Exposing graphene to a hydrogen post-etching process yields dendritic graphene shapes. Here, we demonstrate that similar dendritic structures can be achieved at long growth times without adding hydrogen externally. These shapes are not a result of a surface diffusion controlled growth but of the competing backward reaction (etching), which dominates the growth dynamics at long times due to an in situ rise in the hydrogen partial pressure. We have performed a systematic study on the growth of graphene as a function of time to identify the onset and gradual evolution of graphene shapes caused by etching and then demonstrated that the etching can be stopped by reducing the flow of hydrogen from the feed. In addition, we have found that the etching rate due to the in situ rise in hydrogen is strongly dependent on the confinement (geometrical confinement) of copper foil. Highly etched graphene with dendritic shapes was observed in unconfined copper foil regions while no etching was found in graphene grown in a confined reaction region. This highlights the effect of the dynamic reactant distribution in activating the in situ etching process during growth, which needs to be counteracted or controlled for large scale growth.

Nanotechnology, the manipulation of matter on atomic, molecular, and supramolecular scales, has become the most appealing strategy for biomedical applications and is of great interest as an approach to preventing microbial risks. In this study, we utilize the antimicrobial performance and the drug-loading ability of novel nanoparticles based on silicon oxide and strontium-substituted hydroxyapatite to develop nanocomposite antimicrobial films based on a poly(l-lactic acid) (PLLA) polymer. We also demonstrate that nanoimprint lithography (NIL), a process adaptable to industrial application, is a feasible fabrication technique to modify the surface of PLLA, to alter its physical properties, and to utilize it for antibacterial applications. Various nanocomposite PLLA films with nanosized (black silicon) and three-dimensional (hierarchical) hybrid domains were fabricated by thermal NIL, and their bactericidal activity against Escherichia coli and Staphylococcus aureus was assessed. Our findings demonstrate that besides hydrophobicity the nanoparticle antibiotic delivery and the surface roughness are essential factors that affect the biofilm formation., Competing Interests: The authors declare no competing financial interest.

We report on structural, compositional, and thermal characterization of self-assembled in-plane epitaxial Si 1-x Ge x alloy nanowires grown by molecular beam epitaxy on Si (001) substrates. The thermal properties were studied by means of scanning thermal microscopy (SThM), while the microstructural characteristics, the spatial distribution of the elemental composition of the alloy nanowires and the sample surface were investigated by transmission electron microscopy and energy dispersive x-ray microanalysis. We provide new insights regarding the morphology of the in-plane nanostructures, their size-dependent gradient chemical composition, and the formation of a 5 nm thick wetting layer on the Si substrate surface. In addition, we directly probe heat transfer between a heated scanning probe sensor and Si 1-x Ge x alloy nanowires of different morphological characteristics and we quantify their thermal resistance variations. We correlate the variations of the thermal signal to the dependence of the heat spreading with the cross-sectional geometry of the nanowires using finite element method simulations. With this method we determine the thermal conductivity of the nanowires with values in the range of 2-3 W m -1 K -1 . These results provide valuable information in growth processes and show the great capability of the SThM technique in ambient environment for nanoscale thermal studies, otherwise not possible using conventional techniques.

The highly anisotropic interactions in organic semiconductors together with the soft character of organic materials lead to strong coupling between nuclear vibrations and exciton dynamics, which potentially results in anomalous electrical, optical and optoelectrical properties. Here, we report on the Raman antenna effect from organic semiconducting nanobelts 6,13-dichloropentacene (DCP), resulting from the coupling of molecular excitons and intramolecular phonons. The highly ordered crystalline structure in DCP nanobelts enables the precise polarization-resolved spectroscopic measurement. The angle-dependent Raman spectroscopy under resonant excitation shows that all Raman modes from the skeletal vibrations of DCP molecule act like a nearly perfect dipole antenna I Raman ∝ cos 4 (θ - 90), with almost zero (maximum) Raman scattering parallel (perpendicular) to the nanobelt's long-axis. The Raman antenna effect in DCP nanobelt is originated from the coupling between molecular skeletal vibrations and intramolecular exciton and the confinement of intermolecular excitons. It dramatically enhances the Raman polarization ratio (ρ = I ‖ /I ⊥ > 25) and amplifies the anisotropy of the angle-dependent Raman scattering (κ Raman = I max /I min > 12) of DCP nanobelts. These findings have crucial implications for fundamental understanding on the exciton-phonon coupling and its effects on the optical properties of organic semiconductors.

The performance gain-oriented nanostructurization has opened a new pathway for tuning mechanical features of solid matter vital for application and maintained performance. Simultaneously, the mechanical evaluation has been pushed down to dimensions way below 1 μm. To date, the most standard technique to study the mechanical properties of suspended 2D materials is based on nanoindentation experiments. In this work, by means of micro-Brillouin light scattering we determine the mechanical properties, that is, Young modulus and residual stress, of polycrystalline few nanometers thick MoS 2 membranes in a simple, contact-less, nondestructive manner. The results show huge elastic softening compared to bulk MoS 2 , which is correlated with the sample morphology and the residual stress.

We report a record low thermal conductivity in polycrystalline MoS 2 obtained for ultrathin films with varying grain sizes and orientations. By optimizing the sulfurization parameters of nanometer-thick Mo layers, five MoS 2 films containing a combination of horizontally and vertically oriented grains, with respect to the bulk (001) monocrystal, were grown. From transmission electron microscopy, the average grain size, typically below 10 nm, and proportion of differently oriented grains were extracted. The thermal conductivity of the suspended samples was extracted from a Raman laser-power-dependent study, and the lowest value of thermal conductivity of 0.27 W m -1 K -1 , which reaches a similar value as that of Teflon, is obtained in a polycrystalline sample formed by a combination of horizontally and vertically oriented grains in similar proportion. Analysis by means of molecular dynamics and finite element method simulations confirm that such a grain arrangement leads to lower grain boundary conductance. We discuss the possible use of these thermal insulating films in the context of electronics and thermoelectricity.

Electrical forces are the background of all the interactions occurring in biochemical systems. From here and by using a combination of ab-initio and ad-hoc models, we introduce the first description of electric field profiles with intrabond resolution to support a characterization of single bond forces attending to its electrical origin. This fundamental issue has eluded a physical description so far. Our method is applied to describe hydrogen bonds (HB) in DNA base pairs. Numerical results reveal that base pairs in DNA could be equivalent considering HB strength contributions, which challenges previous interpretations of thermodynamic properties of DNA based on the assumption that Adenine/Thymine pairs are weaker than Guanine/Cytosine pairs due to the sole difference in the number of HB. Thus, our methodology provides solid foundations to support the development of extended models intended to go deeper into the molecular mechanisms of DNA functioning.

Heat conduction in silicon can be effectively engineered by means of sub-micrometre porous thin free-standing membranes. Tunable thermal properties make these structures good candidates for integrated heat management units such as waste heat recovery, rectification or efficient heat dissipation. However, possible applications require detailed thermal characterisation at high temperatures which, up to now, has been an experimental challenge. In this work we use the contactless two-laser Raman thermometry to study heat dissipation in periodic porous membranes at high temperatures via lattice conduction and air-mediated losses. We find the reduction of the thermal conductivity and its temperature dependence closely correlated with the structure feature size. On the basis of two-phonon Raman spectra, we attribute this behaviour to diffuse (incoherent) phonon-boundary scattering. Furthermore, we investigate and quantify the heat dissipation via natural air-mediated cooling, which can be tuned by engineering the porosity.Nanostructuring of silicon allows acoustic phonon engineering, but the mechanism of related thermal transport in these structures is not fully understood. Here, the authors study the heat dissipation in silicon membranes with periodic nanoholes and show the importance of incoherent scattering.

Achieving ultrasmall dimensions of materials and retaining high throughput are critical fabrication considerations for nanotechnology use. This article demonstrates an integrated approach for developing isolated sub-20 nm silicon oxide features through combined "top-down" and "bottom-up" methods: nanoimprint lithography (NIL) and block copolymer (BCP) lithography. Although techniques like those demonstrated here have been developed for nanolithographic application in the microelectronics processing industry, similar approaches could be utilized for sensor, fluidic, and optical-based devices. Thus, this article centers on looking at the possibility of generating isolated silica structures on substrates. NIL was used to create intriguing three-dimensional (3-D) polyhedral oligomeric silsesquioxane (POSS) topographical arrays that guided and confined polystyrene- block -poly(dimethylsiloxane) (PS- b -PDMS) BCP nanofeatures in isolated regions. A cylinder forming PS- b -PDMS BCP system was successfully etched using a one-step etching process to create line-space arrays with a period of 35 nm in confined POSS arrays. We highlight large-area (>6 μm) coverage of line-space arrays in 3-D topographies that could potentially be utilized, for example, in nanofluidic systems. Aligned features for directed self-assembly application are also demonstrated. The high-density, confined silicon oxide nanofeatures in soft lithographic templates over macroscopic areas illustrate the advantages of integrating distinct lithographic methods for attaining discrete features in the deep nanoscale regime., Competing Interests: The authors declare no competing financial interest.

Optical nonlinearities, such as thermo-optic mechanisms and free-carrier dispersion, are often considered unwelcome effects in silicon-based resonators and, more specifically, optomechanical cavities, since they affect, for instance, the relative detuning between an optical resonance and the excitation laser. Here, we exploit these nonlinearities and their intercoupling with the mechanical degrees of freedom of a silicon optomechanical nanobeam to unveil a rich set of fundamentally different complex dynamics. By smoothly changing the parameters of the excitation laser we demonstrate accurate control to activate two- and four-dimensional limit cycles, a period-doubling route and a six-dimensional chaos. In addition, by scanning the laser parameters in opposite senses we demonstrate bistability and hysteresis between two- and four-dimensional limit cycles, between different coherent mechanical states and between four-dimensional limit cycles and chaos. Our findings open new routes towards exploiting silicon-based optomechanical photonic crystals as a versatile building block to be used in neurocomputational networks and for chaos-based applications.