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Label-free vibrational imaging of biological samples has attracted significant interest due to its integration of structural and chemical information. Vibrational infrared photothermal amplitude and phase signal (VIPPS) imaging provide label-free chemical identification by targeting the characteristic resonances of biological compounds that are present in the mid-infrared fingerprint region (3 µm - 12 µm). High contrast imaging of subcellular features and chemical identification of protein secondary structures in unlabeled and labeled fibroblast cells embedded in a collagen-rich extracellular matrix is demonstrated by combining contrast from absorption signatures (amplitude signals) with sensitive detection of different heat properties (lock-in phase signals). We present that the detectability of nano-sized cell membranes is enhanced to well below the optical diffraction limit since the membranes are found to act as thermal barriers. VIPPS offers a novel combination of chemical imaging and thermal diffusion characterization that paves the way towards label-free imaging of cell models and tissues as well as the study of intracellular heat dynamics.

Femtosecond micromachining offers a contact-free and mask-less technique for material patterning. With ultrafast laser irradiation, permanent modifications to the properties of single layer graphene through material ablation or defect introduction can be induced. Multiple femtosecond pulse interactions with a single layer graphene are studied and a low laser ablation threshold ~9.2 mJ/cm 2 is reported for a 15 second illumination time. Clean ablated structures are generated in such a multi pulse irradiation configuration at low pulse energies as an attractive alternative to ablation with single femtosecond, high energy pulses. For a fully ablated graphene hole, a radially symmetric region extending around 2 µm from the ablated edge is characterized by strong defect generation. Average distances between point-defects down to ~58 nm are derived and Raman spectroscopy implies that overall there is a strong resemblance to amorphous structures. For fluence values around 75% of the ablation threshold, modification with defect generation down to ~48 nm average defects lengths is reported, while the underlying graphene structure is maintained. Thus, depending on the laser parameter choice, the same laser configuration can be used to ablate graphene or to primarily introduce defect states. The presented findings offer interesting insights into femtosecond induced structural modifications of graphene that can lead to improved precision ablation and patterning of single-layer materials at the micro-and nano-scale. Further, this can be attractive for graphene or carbon-based device fabrication as well as sensor and transistor applications, where regions of varying carrier concentrations and different electrical, optical or physical properties are desired.

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We investigate the atomic rearrangement in graphene under femtosecond pulse illumination with reactive molecular dynamics simulations and compare with ultra-fast laser ablation experiments. To model the impact of the laser pulse irradiation, heat is locally applied to a selected area of the graphene layer and the resulting structural deformation is simulated as a function of time, providing a detailed understanding of the bond breaking process under laser illumination and subsequent re-equilibration after the pulse is turned off. Analysis of the atomic dynamics indicates that the types of defects formed depend on the pulse energy and exposure duration. By varying the exposed area, we determine that the shape of the ablated area is not only a function of the pulse energy, but also of the beam spot size and pulse repetition. Furthermore, we apply a machine learning approach to extrapolate our simulated data to experimental length scales and reproduce the trends in ablated area as a function of temperature. Our study provides a first step towards understanding the design parameters for graphene nano-patterning.