Optical dephasing of chromophores in an organic glass: picosecond photon echo and hole burning experiments

Abstract

The homogeneous optical dephasing time T2 for the organic glass system resorufin in ethanol is measured by picosecond twopulse photon echoes from 1.5 to I 1.4 K. A non-power law temperature dependence of T2 is measured. Non-photochemical hole burning (NPHB) linewidths are four times broader than the homogeneous linewidth, demonstrating that additional factors contribute to NPHB.

A Dynamical Transition in the Protein Myoglobin Observed by Infrared Vibrational Echo Experiments

“…Photon echo experiments on a 100 ps time scale and optical hole burning experiments on a 100 s time scale produce different pure dephasing widths. [38][39][40][41][42] The hole burning experiments yield broader pure dephasing line widths because of spectral diffusion caused by very slow processes that do not contribute to the photon echo experiments. 40,43,44 However, both types of experiments display the same T ∼1.3 temperature dependence of the pure dephasing contribution to the line width.…”

“…40,43,44 However, both types of experiments display the same T ∼1.3 temperature dependence of the pure dephasing contribution to the line width. [38][39][40][41][42] (The exponent varies somewhat depending on the glass.) In the W(CO) 6 /2MP system, vibrational pure dephasing in the supercooled liquid exhibits VTF behavior, which has its onset at T g .…”

Probing dynamics of complex molecular systems with ultrafast 2D IR vibrational echo spectroscopy

“…2,3 In 1964, the basic concepts inherent in the spin echo were extended to visible spectroscopy using the earliest pulsed lasers to perform ''photon echo'' experiments on electronic excited states. 4,5 Photon echoes have been widely used to study electronic excited state dynamics in systems such as low temperature crystals [6][7][8][9][10] and glasses, [11][12][13][14] proteins, [15][16][17] and photosynthetic chromophore clusters. 18,19 The advent of short pulse infrared (IR) sources made it possible to perform ''vibrational echo'' experiments on the vibrations of condensed mater systems such as liquids, glasses and proteins beginning in the early 1990's.…”

Tunneling Systems in Amorphous and Crystalline Solids

“…The temperature dependence of the quasi-homogeneous linewidths as measured using hole burning by Thijssen et al (1982) and using the photon echo technique by Walsh et al (1986) is approximately linear. In the most extensively investigated organic glasses and polymers, an algebraic temperature dependence was found with an exponent of a ~ 1.3 (see Volker (1989), and references therein).…”

“…But this interpretation changed dramatically after the discovery of a huge discrepancy between the "homogeneous" linewidth of the same impurity in the same glassy host, as measured by two different techniques: Two-pulse photon echo and persistent hole burning (Molenkamp and Wiersma (1985), Walsh et al (1986), Berg et al (1987a)). Spectral diffusion was conceived as a minor addition to the homogeneous linewidth.…”