Picosecond kilohertz-class cryogenically cooled multistage Yb-doped chirped pulse amplifier.

A multistage cryogenic chirped pulse amplifier has been developed, utilizing two different Yb-doped gain materials in subsequent amplifier stages. A Yb:GSAG regenerative amplifier followed by a Yb:YAG power amplifier is able to deliver pulses with a broader bandwidth than a system using only one of these two gain media throughout. We demonstrate 90 mJ of pulse energy (113 W of average power) uncompressed and 67 mJ (84 W of average power) compressed at 1.25 kHz pulse repetition frequency, 3.0 ps FWHM Gaussian pulse width, and near-diffraction-limited (M2<1.3) beam quality.

Femtosecond dynamics of exciton localization: self-trapping from the small to the large polaron limit.

We use femtosecond vibrational wavepacket techniques to time-resolve the coupled electronic and vibrational dynamics of exciton self-trapping in a series of materials in which the relative strength of the electron-phonon coupling can be compositionally tuned from the small to the large polaron limit. Transient absorption experiments are carried out in the quasi-one-dimensional halide-bridged mixed-valence transition metal linear chain complexes [Pt(en)2][Pt(en)2X2]⋅(ClO4)4 (en=ethylenediamine, C2H8N2) with X=Cl, Br and I. In each complex, we detect the formation of the self-trapped exciton through the appearance of its characteristic red-shifted optical absorption, and find that self-trapping occurs on a time scale of the order of a single vibrational period of the optical phonon mode that dominates the self-trapping dynamics. The associated optical phonon response, detected as wavepacket oscillations that modulate the exciton absorption, shows a significant softening of the optical phonon frequency compared to that of the unexcited system. The degree of softening is found to vary significantly with coupling strength, ranging from more than 40% in the strongly coupled chloride-bridged complex to less than 20% in the weakly coupled iodide-bridged complex. We relate these results to the extent of electronic delocalization by comparison with the electronic properties of the ground states of the materials and with the properties of their equilibrated self-trapped electronic states predicted by theoretical modeling.

Vibrational spectroscopy of structurally relaxed self-trapped excitons via excited-state resonant impulsive stimulated Raman spectroscopy.

We probe the vibrational modes of the equilibrated self-trapped exciton (STE) in the mixed-valence linear chain material [Pt(en)(2)][Pt(en)(2)Br(2)]·(ClO(4))(4) using resonantly enhanced impulsive stimulated Raman excitation of the excited electronic state. In these measurements, excitons are created by photoexcitation of the optical intervalence charge transfer band, and after a delay to allow self-trapping and equilibration, the metastable STE is impulsively excited and probed within its red-shifted absorption band. The pump-pump-probe response reveals wavepacket oscillations at a frequency of 125 cm(-1) that are assigned to a Raman-active mode of the STE having Br-Pt-Br symmetric stretching character. This frequency is shifted from the 171 cm(-1) symmetric stretch Raman frequency of the ground electronic state, and from the previously observed 110 cm(-1) wavepacket modulation that accompanies the formation of the STE from the initially excited electronic state, reflecting a new component of the structural relaxation of the exciton.

Mode calculations in asymmetrically aberrated laser resonators using the Huygens-Fresnel kernel formulation.

A theoretical framework is presented for calculating three-dimensional resonator modes of both stable and unstable laser resonators. The resonant modes of an optical resonator are computed using a kernel formulation of the resonator round-trip Huygens-Fresnel diffraction integral. To substantiate the validity of this method, both stable and unstable resonator mode results are presented. The predicted lowest loss and higher order modes of a semi-confocal stable resonator are in agreement with the analytic formulation. Higher order modes are determined for an asymmetrically aberrated confocal unstable resonator, whose lowest loss unaberrated mode is consistent with published results. The three-dimensional kernel method provides a means to evaluate multi-mode configurations with two-dimensional aberrations that cannot be decomposed into one-dimensional representations.