Label-free multimodal coherent anti-Stokes Raman scattering analysis of microparticles in unconstrained microfluidics.

Fast, label-free optical identification and quantification of biomolecules and other relevant biological materials in microfluidic devices and the vascular system will play a major role in liquid biopsy and related diagnoses. An optical microscope probing simultaneously non-linear coherent anti-Stokes Raman scattering (CARS) and linear scattering (LS) was used to probe microparticles in aqueous solutions flowed unconstrained in microfluidic channels. Despite the optical complexity of these systems, where out-of-focus microparticles randomly impede CARS and LS, and where water CARS generates a substantial background, we demonstrate that in-focus microparticles can be individually and unambiguously detected when CARS and LS are co-analyzed. The ability to chemically discriminate microscale features in optically realistic flows supports the relevance of multimodal CARS platforms for liquid biopsy.

Reversible switching among three adsorbate configurations in a single [2.2]paracyclophane-based molecule.

Single 4,7,12,15-tetrakis(4'-dimethylaminostyryl)[2.2]paracyclophane molecules adsorb on NiAl(110) in different configurations. When the symmetry axes of the molecules are properly oriented with respect to the surface lattice, three adsorbate states of different conductance can be reversibly induced and directly imaged with a scanning tunneling microscope. Couplings between tunneling electrons and adsorbate vibrational and electronic states are primarily responsible for the transformation. However, change from low to high conductance configuration can also be triggered by electric field in the junction.

Chemical imaging of single 4,7,12,15-tetrakis[2.2]paracyclophane by spatially resolved vibrational spectroscopy.

Single 4,7,12,15-tetrakis[2.2]paracyclophane were deposited on NiAl(110) surface at 11 K. Two adsorbed species with large and small conductivities were detected by the scanning tunneling microscope (STM). Their vibrational properties were investigated by inelastic electron tunneling spectroscopy (IETS) with the STM. Five vibrational modes were observed for the species with the larger conductivity. The spatially resolved vibrational images for the modes show striking differences, depending on the coupling of the vibrations localized on different functional groups within the molecule to the electronic states of the molecule. The vibrational modes are assigned on the basis of ab initio calculations. No IETS signal is resolved from the species with the small conductivity.

Atomic scale conductance induced by single impurity charging.

A scanning tunneling microscope was used to probe electron transport through an alkali doped C(60) monolayer crystal on Al(2)O(3) grown by the oxidation of NiAl(110). Each individual alkali atom forms a localized complex with the neighboring C(60) molecules. Charging of the complex induces a substantial rise in the current that persists outside the physical dimensions of the complex. This induction of the current rise is characterized by spatially resolved spectroscopy and mapping of the differential conductance (dI/dV) in the vicinity of the complex.