The nonlinear mechanical response of monolayer graphene on polyethylene terephthalate (PET) is characterised using in‐situ Raman spectroscopy and atomic force microscopy. While interfacial stress transfer leads to tension in graphene as the PET substrate is stretched, retraction of the substrate during unloading imposes compression in the graphene. Two interfacial failure mechanisms, shear sliding under tension and buckling under compression, are identified. Using a nonlinear shear‐lag model, the interfacial shear strength is found to range between 0.46 and 0.69 MPa. The critical strain for onset of interfacial sliding is ∼0.3%, while the maximum strain that can be transferred to graphene ranges from 1.2% to 1.6% depending on the interfacial shear strength and graphene size. Beyond a critical compressive strain of around −0.7%, buckling ridges are observed after unloading. The results from this work provide valuable insight and design guidelines for a broad spectrum of applications of graphene and other 2D nanomaterials, such as flexible and stretchable electronics, strain sensing, and nanocomposites.

Van der Waals adhesion between graphene and various substrates has an important impact on the physical properties, device applications and nanomanufacturing processes of graphene. Here we report a general, high-throughput and reliable method that can measure adhesion energies between ultraflat graphene and a broad range of materials using atomic force microscopy with a microsphere tip. In our experiments, only van der Waals force between the tip and a graphene flake is measured. The Maugis-Dugdale theory is employed to convert the measured adhesion force using AFM to the adhesion energy. The ultraflatness of monolayer graphene on mica eliminates the effect of graphene surface roughness on the adhesion, while roughness of the microsphere tip is addressed by the modified Rumpf model. Adhesion energies of monolayer graphene to SiO2 and Cu are obtained as 0.46 and 0.75 J m(-2), respectively. This work provides valuable insight into the mechanism of graphene adhesion and can readily extend to the adhesion measurement for other 2D nanomaterials.

Streaking of photoelectrons with optical lasers has been widely used for temporal characterization of attosecond extreme ultraviolet pulses. Recently, this technique has been adapted to characterize femtosecond x-ray pulses in free-electron lasers with the streaking imprinted by farinfrared and Terahertz (THz) pulses. Here, we report successful implementation of THz streaking for time-stamping of an ultrashort relativistic electron beam of which the energy is several orders of magnitude higher than photoelectrons. Such ability is especially important for MeV ultrafast electron diffraction (UED) applications where electron beams with a few femtosecond pulse width may be obtained with longitudinal compression while the arrival time may fluctuate at a much larger time scale. Using this laser-driven THz streaking technique, the arrival time of an ultrashort electron beam with 6 fs (rms) pulse width has been determined with 1.5 fs (rms) accuracy. Furthermore, we have proposed and demonstrated a non-invasive method for correction of the timing jitter with femtosecond accuracy through measurement of the compressed beam energy, which may allow one to advance UED towards sub-10 fs frontier far beyond the ∼100 fs (rms) jitter.

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In low-dimensional systems with strong electronic correlations, the application of an ultrashort laser pulse often yields novel phases that are otherwise inaccessible. The central challenge in understanding such phenomena is to determine how dimensionality and many-body correlations together govern the pathway of a non-adiabatic transition. To this end, we examine a layered compound, 1T-TiSe2, whose three-dimensional charge-density-wave (3D CDW) state also features exciton condensation due to strong electron-hole interactions. We find that photoexcitation suppresses the equilibrium 3D CDW while creating a nonequilibrium 2D CDW. Remarkably, the dimension reduction does not occur unless bound electron-hole pairs are broken. This relation suggests that excitonic correlations maintain the out-of-plane CDW coherence, settling a long-standing debate over their role in the CDW transition. Our findings demonstrate how optical manipulation of electronic interaction enables one to control the dimensionality of a broken-symmetry order, paving the way for realizing other emergent states in strongly correlated systems.