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Arpin, Paul C.

Publications and source records attributed to Arpin, Paul C..

Spatiotemporal dispersion compensation for a 200-THz noncollinear optical parametric amplifier

A noncollinear optical parametric amplifier (NOPA) can produce few-cycle femtosecond laser pulses that are ideally suited for time-resolved optical spectroscopy measurements. However, the nonlinear-optical process giving rise to ultrabroadband pulses is susceptible to spatiotemporal dispersion problems. Here, we detail refinements, including chirped-pulse amplification (CPA) and pulse-front matching (PFM), that minimize spatiotemporal dispersion and thereby improve the properties of ultrabroadband pulses produced by a NOPA. Here, the description includes a rationale behind the choices of optical and optomechanical components, as well as assessment protocols. We demonstrate these techniques using a 1 kHz, second-harmonic Ti:sapphire pump configuration, which produces ~5-fs duration pulses that span from about 500 to 800 nm with a bandwidth of about 200 THz. To demonstrate the utility of the CPA-PFM-NOPA, we measure vibrational quantum beats in the transient–absorption spectrum of methylene blue, a dye molecule that serves as a reference standard.

47 OTHER INSTRUMENTATION↗

Perturbative theoretical model of electronic transient circular dichroism spectroscopy of molecular aggregates

A chiral analog of transient absorption spectroscopy, transient circular dichroism (TCD) spectroscopy is an emerging time-resolved method. Both spectroscopic methods can probe the electronic transitions of a sample, and TCD is additionally sensitive to the dynamic aspects of chirality, such as those induced by molecular excitons. Here, we develop a theoretical description of TCD for electronic multi-level models in which the pump pulse is linearly polarized and probe pulse is alternately left- and right-circularly polarized. We derive effective response functions analogous to those often used to describe other four-wave mixing methods and then simulate and analyze TCD spectra for three representative multi-level electronic model systems. We elaborate on the presence and detection of the spectral signatures of electronic coherences.

77 NANOSCIENCE AND NANOTECHNOLOGY↗