ABSTRACT
Frequency recognition algorithm for multiple exposures (FRAME) is a high-speed videography technique that exposes a dynamic object to time-varying structured illumination (SI) and captures two-dimensional transients in a single shot. Conventional FRAME requires light splitting to increase the number of frames per shot, thereby resulting in optical loss and a limited number of frames per shot. Here, we propose and demonstrate a novel FRAME method which overcomes these problems by utilizing an interferometer to generate a time-varying SI without light splitting. Combining this method with a pulsed laser enables low-cost, high-speed videography on a variety of timescales from microseconds.
ABSTRACT
Nonlinear optical microscopy allows for rapid high-resolution microscopy with image contrast generated from the intrinsic properties of the sample. Established modalities, such as multiphoton excited fluorescence and second/third-harmonic generation, can be combined with other nonlinear techniques, such as coherent Raman spectroscopy, which typically allow chemical imaging of a single resonant vibrational mode of a sample. Here, we utilize a single ultrafast laser source to obtain broadband coherent Raman spectra on a microscope, together with other nonlinear microscopy approaches on the same instrument. We demonstrate that the coherent Raman modality allows broadband measurement (>1000 cm-1), with high spectral resolution (<5 cm-1), with a rapid spectral acquisition rate (3-12 kHz). This enables Raman hyperspectral imaging of kilo-pixel images at >11 frames per second.
ABSTRACT
We report a broadband refractive index measurement method based on a higher harmonic generation tabletop coherent extreme ultraviolet source. We measured the complex refractive index of a sample material by measuring the interference pattern produced by a bare double slit and comparing this with the pattern produced by another double slit with one slit covered by the sample material. We validated the method by measuring the complex refractive index of aluminum in the photon energy range of 63-78 eV using a neon gas jet. The measurement system had errors of less than 0.02%.
ABSTRACT
We demonstrate ultra-broadband Fourier-transform coherent anti-Stokes Raman scattering (FT-CARS) spectroscopy spanning over 3,000 cm-1 with a rapid-scan Michelson interferometer at a scan rate of 24,000 spectra/s. Using sub-10-fs optical pulses from a mode-locked laser, we measure broad CARS spectrum covering both the fingerprint region (500-1,800 cm-1) and the C-H, N-H, O-H stretching region (2,700-3,600 cm-1). To the best of our knowledge, this is the first demonstration of coherent Raman scattering spectroscopy covering over 3,000 cm-1 at a scan rate of more than 10,000 spectra/s. Our system holds the potential for high-speed or high-throughput label-free chemical analysis, such as investigating non-repetitive chemical dynamics, taking large area images of materials or biological specimens, or counting and sorting a large number of heterogeneous cells.
ABSTRACT
We combine sub-20 fs transient absorption spectroscopy with state-of-the-art computations to study the ultrafast photoinduced dynamics of trans-azobenzene (AB). We are able to resolve the lifetime of the ππ* state, whose decay within ca. 50 fs is correlated to the buildup of the nπ* population and to the emergence of coherences in the dynamics, to date unobserved. Nonlinear spectroscopy simulations call for the CNN in-plane bendings as the active modes in the subps photoinduced coherent dynamics out of the ππ* state. Radiative to kinetic energy transfer into these modes drives the system to a high-energy planar nπ*/ground state conical intersection, inaccessible upon direct excitation of the nπ* state, that triggers an ultrafast (0.45 ps) nonproductive decay of the nπ* state and is thus responsible for the observed Kasha rule violation in UV excited trans-AB. On the other hand, cis-AB is built only after intramolecular vibrational energy redistribution and population of the NN torsional mode.
