Optical stark effects in j-aggregate-metal hybrid nanostructures exhibiting a strong exciton-surface-plasmon-polariton interaction.

We report on the observation of optical Stark effects in J-aggregate-metal hybrid nanostructures exhibiting strong exciton-surface-plasmon-polariton coupling. For redshifted nonresonant excitation, pump-probe spectra show short-lived dispersive line shapes of the exciton-surface-plasmon-polariton coupled modes caused by a pump-induced Stark shift of the polariton resonances. For larger coupling strengths, the sign of the Stark shift is reversed by a transient reduction in normal mode splitting. Our studies demonstrate an approach to coherently control and largely enhance optical Stark effects in strongly coupled hybrid systems. This may be useful for applications in ultrafast all-optical switching.

Selective breaking of bonds in water with intense, 2-cycle, infrared laser pulses.

One of the holy grails of contemporary science has been to establish the possibility of preferentially breaking one of several bonds in a molecule. For instance, the two O-H bonds in water are equivalent: given sufficient energy, either one of them is equally likely to break. We report bond-selective molecular fragmentation upon application of intense, 2-cycle pulses of 800 nm laser light: we demonstrate up to three-fold enhancement for preferential bond breaking in isotopically substituted water (HOD). Our experimental observations are rationalized by means of ab initio computations of the potential energy surfaces of HOD, HOD(+), and HOD(2+) and explorations of the dissociation limits resulting from either O-H or O-D bond rupture. The observations we report present a formidable theoretical challenge that need to be taken up in order to gain insights into molecular dynamics, strong field physics, chemical physics, non-adiabatic processes, mass spectrometry, and time-dependent quantum chemistry.

Ultrasmall bullets of light--focusing few-cycle light pulses to the diffraction limit.

We demonstrate an essentially dispersion-free and diffraction-limited focusing of few-cycle laser pulses through all-reflective microscope objectives. By transmitting 6-fs-pulses from a Ti:sapphire oscillator through an all-reflective 0.5 NA objective, we reach a focus with a beam diameter of 1.0 µm, preserving the time structure of the pulses. The temporal and spatial pulse profile is recorded simultaneously using a novel tip-enhanced electron emission autocorrelator, indicating a focal volume of these pulses of only 1.8 µm3. We anticipate that the demonstrated technique is of considerable interest for inducing and probing optical nonlinearities of individual nanostructures.

Ultrafast manipulation of strong coupling in metal-molecular aggregate hybrid nanostructures.

We demonstrate an ultrafast manipulation of the Rabi splitting energy Ω(R) in a metal-molecular aggregate hybrid nanostructure. Femtosecond excitation drastically alters the optical properties of a model system formed by coating a gold nanoslit array with a thin J-aggregated dye layer. Controlled and reversible transient switching from strong (Ω(R) ≃ 55 meV) to weak (Ω(R) ≈ 0) coupling on a sub-ps time scale is directly evidenced by mapping the nonequilibrium dispersion relations of the coupled excitations. Such a strong, externally controllable coupling of excitons and surface plasmon polaritons is of considerable interest for ultrafast all-optical switching applications in nanoscale plasmonic circuits.

Coherent exciton-surface-plasmon-polariton interaction in hybrid metal-semiconductor nanostructures.

We report measurements of a coherent coupling between surface plasmon polaritons (SPP) and quantum well excitons in a hybrid metal-semiconductor nanostructure. The hybrid structure is designed to optimize the radiative exciton-SPP interaction which is probed by low-temperature, angle-resolved, far-field reflectivity spectroscopy. As a result of the coupling, a significant shift of approximately 7 meV and an increase in broadening by approximately 4 meV of the quantum well exciton resonance are observed. The experiments are corroborated by a phenomenological coupled-oscillator model predicting coupling strengths as large as 50 meV in structures with optimized detunings between the coupled exciton and SPP resonances. Such a strong interaction can, e.g., be used to enhance the luminescence yield of semiconductor quantum structures or to amplify SPP waves.

Classification of human lung carcinomas by mRNA expression profiling reveals distinct adenocarcinoma subclasses.

We have generated a molecular taxonomy of lung carcinoma, the leading cause of cancer death in the United States and worldwide. Using oligonucleotide microarrays, we analyzed mRNA expression levels corresponding to 12,600 transcript sequences in 186 lung tumor samples, including 139 adenocarcinomas resected from the lung. Hierarchical and probabilistic clustering of expression data defined distinct subclasses of lung adenocarcinoma. Among these were tumors with high relative expression of neuroendocrine genes and of type II pneumocyte genes, respectively. Retrospective analysis revealed a less favorable outcome for the adenocarcinomas with neuroendocrine gene expression. The diagnostic potential of expression profiling is emphasized by its ability to discriminate primary lung adenocarcinomas from metastases of extra-pulmonary origin. These results suggest that integration of expression profile data with clinical parameters could aid in diagnosis of lung cancer patients.