In atomically thin membranes, strain couples strongly to electrons, phonons, and photons. Although strain originating from uniform or global deformation has been widely studied, the impact of spatially localized mechanical perturbations on strain distribution remains less explored. Here, we investigate how localized tungsten carbide deposition via focused electron-beam-induced deposition (FEBID) modifies the strain landscape in suspended monolayer graphene membranes. Using spatially resolved mechanical resonance mode shape mapping and Raman spectroscopy, supported by finite element simulations, we find that the central deposit acts as a mechanically coupled local perturbation that redistributes the pre-existing strain into a more radially symmetric configuration with reduced angular anisotropy around the deposit. These findings demonstrate that FEBID-based local deposition can serve as a lithography-free approach for controlled strain modulation in suspended graphene, offering a practical platform for studying strain-coupled phenomena and designing strain-controlled nanoelectromechanical and optoelectronic systems.
We demonstrate controlled STM-induced modification/destruction of Ih-C60 supported on a Cu(111) surface, showing that the molecule is more resilient to high currents for bias voltages greater than ca. 3.5 V. This is due to the enhanced charge transport through the diffuse SAMO orbitals of the molecule with lower probability for electron-vibration coupling than found for resonant low bias transport through it-molecular orbitals. Experimental and theoretical DFT results demonstrate the destruction mechanism comes from C2 emission from the fullerene cage and the formation of smaller fullerenes via sequential emission of C2.
The two-dimensional nanomaterial, hexagonal boron nitride (hBN) was cleanly transferred via a blister-based laser-induced forward-transfer method. The transfer was performed utilizing femtosecond and nanosecond laser pulses for separation distances of 16 and 200 micrometers between a titanium donor film deposited on a glass substrate and a silicon/silicon dioxide receiver. Transfer efficiency was examined for isolated laser pulses as well as for series of overlapping pulses and single layer transfer was confirmed. It was found that hBN is transferable for all tested combinations of pulse duration and transfer distances. The results indicate that transfer proceeds via direct stamping for short donor-to-receiver distances while, for the larger distance, the material is ejected from the donor and lands on the receiver. Furthermore, with overlapping pulses, nanosecond laser pulses enable a successful printing of hBN lines while, for fs laser pulses, the Ti film can be locally disrupted by multiple pulses and molten titanium may be transferred along with the hBN flakes. For reproducibility, and to avoid contamination with metal deposits, low laser fluence transfer with ns pulses and transfer distances smaller than the blister height provide the most favourable and reproducible condition.
Fullerenes of extra-terrestrial origin may have been accessible as carbon sources for anaerobic microorganisms on the early Earth. Very little is known about how anaerobic microorganisms respond to and use fullerenes and their soluble derivatives. We present an investigation into the effects of fullerenes C60 and C70 and their hydroxylated fullerol derivatives on an environmentally relevant anaerobic community and a microbial isolate. Fullerenes and fullerols irradiated with 254 nm UV radiation for 2 weeks in the absence of oxygen to simulate UV irradiation under anoxia on early Earth were also assessed. The anaerobic community could grow using glucose in the presence of C60 up to 500 mg/mL without inhibitory effects on growth. Concentrations of C70 of 500 mg/ml were inhibitory. We attribute these results to the different chemical reactivity and photophysical properties of the fullerenes. The experiments suggest the potential for the use of C60 as a sole carbon source. Both C60 and C70 fullerols were inhibitory to growth in the presence of glucose, especially when exposed to light. When we exposed C60 fullerol suspensions to 254 nm UV radiation under an anoxic atmosphere, they become significantly more inhibitory to both the community and the isolate, but only if the cultures are grown under ambient light exposure. The anaerobic isolate was unable to grow on C60 alone, but after UV radiation exposure, the C60 photodegradation products served as a potentially accessible carbon source. Our data show that fullerenes and their derivatives are biologically active and capable of influencing growth in anoxic environments such as those that would have been prevalent on early Earth or in modern-day anoxic soils. Our results show that carbon sources such as these can be both beneficial or deleterious to life depending on their concentrations and environmental processing.
Warm dense matter (WDM) represents a highly excited state that lies at the intersection of solids, plasmas, and liquids and that cannot be described by equilibrium theories. The transient nature of this state when created in a laboratory, as well as the difficulties in probing the strongly coupled interactions between the electrons and the ions, make it challenging to develop a complete understanding of matter in this regime. In this work, by exciting isolated ∼8 nm copper nanoparticles with a femtosecond laser below the ablation threshold, we create uniformly excited WDM. Using photoelectron spectroscopy, we measure the instantaneous electron temperature and extract the electron-ion coupling of the nanoparticle as it undergoes a solid-to-WDM phase transition. By comparing with state-of-the-art theories, we confirm that the superheated nanoparticles lie at the boundary between hot solids and plasmas, with associated strong electron-ion coupling. This is evidenced both by a fast energy loss of electrons to ions, and a strong modulation of the electron temperature induced by strong acoustic breathing modes that change the nanoparticle volume. This work demonstrates a new route for experimental exploration of the exotic properties of WDM.
Weak interlayer couplings at 2D van der Waals (vdW) interfaces fundamentally distinguish out‐of‐plane charge flow, the information carrier in vdW‐assembled vertical electronic and optical devices, from the in‐plane band transport processes. Here, the out‐of‐plane charge transport behavior in 2D vdW semiconducting transition metal dichalcogenides (SCTMD) is reported. The measurements demonstrate that, in the high electric field regime, especially at low temperatures, either electron or hole carrier Fowler–Nordheim (FN) tunneling becomes the dominant quantum transport process in ultrathin SCTMDs, down to monolayers. For few‐layer SCTMDs, sequential layer‐by‐layer FN tunneling is observed to dominate the charge flow, thus serving as a material characterization probe for addressing the Fermi level positions and the layer numbers of the SCTMD films. Furthermore, it is shown that the physical confinement of the electron or hole carrier wave packets inside the sub‐nm thick semiconducting layers reduces the vertical quantum tunneling probability, leading to an enhanced effective mass of tunneling carriers.
The ultrafast-laser-induced solid–liquid phase transition in metals is still not clearly understood and its accurate quantitative description remains a challenge. Here, we systematically investigated, both experimentally and theoretically, the melting of gold by single femto- and picosecond near-infrared laser pulses. Two laser systems with wavelengths of 800 and 1030 nm and pulse durations ranging from 124 fs to 7 ps were used, and the damage and ablation thresholds were determined for each irradiation condition. The theoretical analysis was based on two-temperature modeling. Different expressions for the electron–lattice coupling rate and contribution of ballistic electrons were examined. In addition, the number of free electrons involved in the optical response is suggested to be dependent on the laser intensity and the influence of the fraction of involved electrons on the damage threshold was investigated. Only one combination of modelling parameters was able to describe consistently all the measured damage thresholds. Physical arguments are presented to explain the modeling results.
MoS2 nanoscrolls that have inner core radii of ∼250 nm are generated from MoS2 monolayers, and the optical and transport band gaps of the nanoscrolls are investigated. Photoluminescence spectroscopy reveals that a MoS2 monolayer, originally a direct gap semiconductor (∼1.85 eV (optical)), changes into an indirect gap semiconductor (∼1.6 eV) upon scrolling. The size of the indirect gap for the MoS2 nanoscroll is larger than that of a MoS2 bilayer (∼1.54 eV), implying a weaker interlayer interaction between concentric layers of the MoS2 nanoscroll compared to Bernal-stacked MoS2 few-layers. Transport measurements on MoS2 nanoscrolls incorporated into ambipolar ionic-liquid-gated transistors yielded a band gap of ∼1.9 eV. The difference between the transport and optical gaps indicates an exciton binding energy of 0.3 eV for the MoS2 nanoscrolls. The rolling up of 2D atomic layers into nanoscrolls introduces a new type of quasi-1D nanostructure and provides another way to modify the band gap of 2D materials.
Graphene oxides with different degrees of oxidation are prepared by controlling UV irradiation on graphene, and the charge transport and the evolution of the transport gap are investigated according to the extent of oxidation. With increasing oxygenous defect density nD, a transition from ballistic to diffusive conduction occurs at nD≃1012 cm−2 and the transport gap grows in proportion to nD. Considering the potential fluctuation related to the e−h puddle, the bandgap of graphene oxide is deduced to be Eg≃30nD(1012cm−2) meV. The temperature dependence of conductivity showed metal–insulator transitions at nD≃0.3×1012 cm−2, consistent with Ioffe–Regel criterion. For graphene oxides at nD≥4.9×1012 cm−2, analysis indicated charge transport occurred via 2D variable range hopping conduction between localized sp2 domain. Our work elucidates the transport mechanism at different extents of oxidation and supports the possibility of adjusting the bandgap with oxygen content.
The recent report of a p-type graphene(Gr)/carbon-nanotube(CNT) barristor facilitates the application of graphene barristors in the fabrication of complementary logic devices. Here, a complementary inverter is presented that combines a p-type Gr/CNT barristor with a n-type Gr/MoS2 barristor, and its characteristics are reported. A sub-nW (~0.2 nW) low-power inverter is demonstrated with a moderate gain of 2.5 at an equivalent oxide thickness (EOT) of ~15 nm. Compared to inverters based on field-effect transistors, the sub-nW power consumption was achieved at a much larger EOT, which was attributed to the excellent switching characteristics of Gr barristors.
1JILA, Department of Physics, University of Colorado and NIST, Boulder, Colorado 80309, USA 2Theoretical Division, Los Alamos National Laboratory, NM 87545, USA 3Kapteyn-Murnane Laboratories Inc., 4775 Walnut St #102, Boulder, CO 80301, USA 4Department of Chemistry, University of Colorado Boulder, CO 80309, USA 5Renewable and Sustainable Energy Institute, University of Colorado Boulder, CO 80309, USA 6EaStCHEM, School of Chemistry, Edinburgh University, David Brewster Road, Edinburgh EH9 3FJ, U.K. 7Molecular Foundary, Lawrence Berkeley National Laboratory, Berkeley, CA, USA. †Present address: Stanford PULSE Institute, SLAC National Accelerator Laboratory and Stanford University, Menlo Park, CA 94025, USA. *Email:Quynh.L.Nguyen@colorado.edu
The electrical performance of suspended few-layer MoTe2 field-effect-transistors with ionic liquid gating has been investigated. The suspended structure not only enhances the mobility of MoTe2 by removing the influence of the substrate but also allows ions to accumulate on both the top and the bottom surface of MoTe2. The consequent increase in the gate capacitance resulted in an improved subthreshold swing (∼73 mV/dec) and on–off ratio (106) at room temperature for suspended MoTe2 compared to substrate-supported devices. Suspended transistors with ionic liquid gating enable a larger charge density compared to ionic liquid gated supported devices and may provide a useful platform to study screening physics in 2D materials.
The arrangement of ionic liquids (ILs) within meso-porous ordered silica SBA-15 is revealed from nitrogen physisorption experiments combined with non-local density functional theory analysis of the pore structure and mean-field density functional theory (MFDFT). Using MFDFT on simple lattice models, we outline possible scenarios for IL distributions within the pores and conditions under which they originate. MFDFT predictions for nitrogen adsorption on these models of pore structures modified with ILs are in qualitative agreement with the experimental results. They demonstrate that the distribution of the ILs inside the pores of SBA-15 is sensitive to solid-fluid interactions, leading to different structures as a function of loading. This study also recommends the MFDFT and lattice models as a powerful framework for the interpretation of nitrogen sorption behavior, which complements the existing theoretical and experimental techniques to characterize the structure of supported ILs.
We have investigated the effect of an Al2O3passivation layer on the performance of few-layer WS2FETs. While the performance of WS2FETs is often limited by a substantial decrease in carrier mobility owing to charged impurities and a Schottky barrier between the WS2and metal electrodes, the introduction of an Al2O3overlayer by atomic layer deposition (ALD) suppressed the influence of charged impurities by high-κdielectric screening effect and reduced the effective Schottky barrier height. We argue that n-doping of WS2, induced by positive fixed charges formed at Al2O3/WS2interface during the ALD process, is responsible for the reduction of the effective Schottky barrier height in the devices. In addition, the Al2O3passivation layer protected the device from oxidation, and maintained stable electrical performance of the WS2FETs over 57 d. Thus, the ALD of Al2O3overlayer provides a facile method to enhance the performance of WS2FETs and to ensure ambient stability.
Experiments that probe the fundamental properties of endohedral fullerenes often require the preparation of molecular beams or thin films of the neutral molecules. It is challenging to cleanly sublime this class of molecules without producing some thermal degradation. We report combined gas phase and scanning tunnelling microscopy studies that probe the thermal decay of commercial [Li+C60]PF6- in a quartz ampoule and provide treatment conditions that will allow the sublimation of intact, neutral Li@C60 accompanied by a well-characterised component of neutral C60. The decay of the material at appropriate temperatures can be modelled with the assumption of a second order decay process in the oven yielding Arrhenius parameters that can predict the ratio of Li@C60 to C60 in the sublimed material.
The equipartition thickness provides a way to design advanced materials with task-specific surface properties and to predict their adsorption performance.
We publish three Roadmaps on photonic, electronic and atomic collision physics in order to celebrate the 60th anniversary of the ICPEAC conference. In Roadmap I, we focus on the light–matter interaction. In this area, studies of ultrafast electronic and molecular dynamics have been rapidly growing, with the advent of new light sources such as attosecond lasers and x-ray free electron lasers. In parallel, experiments with established synchrotron radiation sources and femtosecond lasers using cutting-edge detection schemes are revealing new scientific insights that have never been exploited. Relevant theories are also being rapidly developed. Target samples for photon-impact experiments are expanding from atoms and small molecules to complex systems such as biomolecules, fullerene, clusters and solids. This Roadmap aims to look back along the road, explaining the development of these fields, and look forward, collecting contributions from twenty leading groups from the field.
We have investigated the ionization and fragmentation of a metallo-endohedral fullerene, Sc3N@C80, using ultrashort (10 fs) x-ray pulses. Following selective ionization of a Sc (1s) electron (hν = 4.55 keV), an Auger cascade leads predominantly to either a vibrationally cold multiply charged parent molecule or multifragmentation of the carbon cage following a phase transition. In contrast to previous studies, no intermediate regime of C2 evaporation from the carbon cage is observed. A time-delayed, hard x-ray pulse (hν = 5.0 keV) was used to attempt to probe the electron transfer dynamics between the encapsulated Sc species and the carbon cage. A small but significant change in the intensity of Sc-containing fragment ions and coincidence counts for a delay of 100 fs compared to 0 fs, as well as an increase in the yield of small carbon fragment ions, may be indicative of incomplete charge transfer from the carbon cage on the sub-100 fs time scale.
The field of molecular electronics aims at advancing the miniaturization of electronic devices, by exploiting single molecules to perform the function of individual components. A molecular switch is defined as a molecule that displays stability in two or more states (e.g. "on" and "off" involving conductance, conformation etc.) and upon application of a controlled external perturbation, electric or otherwise, undergoes a reversible change such that the molecule is altered. Previous work has shown multi-state molecular switches with up to four and six distinct states. Using low temperature scanning tunnelling microscopy and spectroscopy, we report on a multi-state single molecule switch using the endohedral fullerene Li@C60 that displays 14 molecular states which can be statistically accessed. We suggest a switching mechanism that relies on resonant tunnelling via the superatom molecular orbitals (SAMOs) of the fullerene cage as a means of Li activation, thereby bypassing the typical vibronic excitation of the carbon cage that is known to cause molecular decomposition.