We present a novel experimental scheme for two-dimensional fluorescence-detected coherent spectroscopy (2D-FDCS) using a non-collinear beam geometry with the aid of "confocal imaging" of dynamic (population) grating and 27-step phase-cycling to extract the signal. This arrangement obviates the need for distinct experimental designs for previously developed transmission detected non-collinear two-dimensional coherent spectroscopy (2D-CS) and collinear 2D-FDCS. We also describe a novel method for absolute phasing of the 2D spectrum. We apply this method to record 2D spectra of a fluorescent dye in solution at room temperature and observe "spectral diffusion."

Here we report how ultrafast pulsed illumination at low average power results in a stable three-dimensional (3D) optical trap holding latex nanoparticles which is otherwise not possible with continuous wave lasers at the same power level. The gigantic peak power of a femtosecond pulse exerts a huge instantaneous gradient force that has been predicted theoretically earlier and implemented for microsecond pulses in a different context by others. In addition, the resulting two-photon fluorescence allows direct observation of trapping events by providing intrinsic 3D resolution.

The use of low-power high-repetition-rate ultrafast pulsed excitation in stable optical trapping of dielectric nanoparticles has been demonstrated in the recent past; the high peak power of each pulse leads to instantaneous trapping of a nanoparticle with fast inertial response and the high repetition-rate ensures repetitive trapping by successive pulses However, with such high peak power pulsed excitation under a tight focusing condition, nonlinear optical effects on trapping efficiency also become significant and cannot be ignored. Thus, in addition to the above mentioned repetitive instantaneous trapping, trapping efficiency under pulsed excitation is also influenced by the optical Kerr effect, which we theoretically investigate here. Using dipole approximation we show that with an increase in laser power the radial component of the trapping potential becomes progressively more stable but the axial component is dramatically modulated due to increased Kerr nonlinearity. We justify that the relevant parameter to quantify the trapping efficiency is not the absolute depth of the highly asymmetric axial trapping potential but the height of the potential barrier along the beam propagation direction. We also discuss the optimal excitation parameters leading to the most stable dipole trap. Our results show excellent agreement with previous experiments.

An effective z-scan setup with a minimum thermal effect is shown for intensity-dependent measure of two-photon absorption (TPA) with high-repetition rate lasers. Use of an additional intensity modulation with an optical chopper provides enough blanking time for a high-repetition rate laser to yield equally accurate results in TPA measurements compared to a low repetition laser. Extension of this method of thermal effect management with an optical chopper to emission studies also results in good correspondence for two-photon cross-section measurements from either z-scan or two-photon fluorescence techniques. The method also significantly enhances two-photon fluorescence, which could be promising for multiphoton microscopy.

We briefly review the coherent quantum beats observed in recent two-dimensional electronic spectroscopy experiments in a photosynthetic-light-harvesting antenna. We emphasize that the decay of the quantum beats in these experiments is limited by ensemble averaging. The in vivo dynamics of energy transport depends upon the local fluctuations of a single photosynthetic complex during the energy transfer time (a few picoseconds). Recent analyses suggest that it remains possible that the quantumcoherent motion may be robust under individual realizations of the environmentinduced fluctuations contrary to intuition obtained from condensed phase spectroscopic measurements and reduced density matrices. This result indicates that the decay of the observed quantum coherence can be understood as ensemble dephasing. We propose a fluorescence-detected single-molecule experiment with phase-locked excitation pulses to investigate the coherent dynamics at the level of a single molecule without hindrance by ensemble averaging. We discuss the advantages and limitations of this method. We report our initial results on bulk fluorescence-detected coherent spectroscopy of the Fenna-Mathews-Olson complex.