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Applied Physics Letters

Proposed picosecond excited-state measurement method using a tunable-laser-induced grating

Anthony E.. Siegman

Published Jan 1, 1977• 37 citations
Publisher

Abstract

This letter analyzes a suggested technique for studying excited atomic or molecular states on a picosecond to subpicosecond time scale by using tunable laser beams, without requiring ultrafast laser pulses or optical detectors. In the proposed technique the frequency transform of the impulse response of an excited state is determined by measuring the diffraction of a cw probe laser beam from a moving excited-state grating induced by two intersecting tunable excitation beams, as the frequency difference between the two cw excitation beams is varied.

DOI
10.1063/1.89216

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This letter analyzes a suggested technique for studying excited atomic or molecular states on a picosecond to subpicosecond time scale by using tunable laser beams, without requiring ultrafast laser pulses or optical detectors. In the proposed technique the frequency transform of the impulse response of an excited state is determined by measuring the diffraction of a cw probe laser beam from a moving excited-state grating induced by two intersecting tunable excitation beams, as the frequency difference between the two cw excitation beams is varied.
I. A new technique utilizing the electro-optic frequency switching of a single mode ( 6 Mhz) dye laser was used to observe free induction decay and optical nutation in iodine gas and optical nutation in an organic mixed crystal (pentacene in p-terphenyl) at low temperature. A new technique, incoherent resonance decay (IRO) was also developed. These experiments allow one to determine T_1 and T_2, the longitudinal and transverse relaxation times of the excited ensemble, in analogy with magnetic resonance. For I_2(g) at O∙C; T_l = 2.3 x 10^(-7) sec, T_2 ≃ 1 x 10^(-7) sec. These techniques are limited to a time scale > 10 nsec. II. The construction and characterization of cw, mode-locked dye laser capable of putting out a continuous train of reproducible sub-picosecond pulses is described. Experiments utilizing this laser for the measurement of picosecond coherent transients and time resolved absorption spectroscopy are proposed.
Recent advances in the development of synchronously mode-locked dye-laser systems have permitted the first low-power measurement of the time-resolved dephasing dynamics of a Raman active molecular vibration. Excitation and delayed probing of the coherent ensemble of vibrators is accomplished with the help of synchronized picosecond pulse trains from two independently tunable mode-locked dye lasers. A new probe technique, based on a gain measurement, is employed that provides a signal that scales linearly with the coherent vibrational amplitude. We demonstrate this technique with the first measurement of the dephasing dynamics of the normal mode (656.5 cm−1) of CS2 in the liquid state. An exponential decay with time constant 20±1 psec is obtained for the isotropic component of the coherent scattering.
A simple method for observing coherent optical-transient phenomena is described. Effects such as photon echoes and free induction decay (FID) should allow studies of the dynamic properties of atoms, molecules, and solids on a time scale ranging from milliseconds to \ensuremath{\sim} 50 ps. The frequency of a cw dye laser is switched with an intracavity electro-optic modulator, producing in an external sample coherent transients which are detected in the forward beam. Measurements of long dephasing times are possible, as in FID, because the laser can oscillate indefinitely at the new frequency following a step-function switching pulse. Measurements of short decay times are also practical because the switching time is not restricted by the laser gain or cavity ringing time. In addition, the dye's dephasing time of a few picoseconds or less is too rapid to interfere with these observations. Since the pulse sequence can be preselected, the entire class of coherent optical transients is accessible. The method thus incorporates all of the advantages inherent in Stark switching, including heterodyne detection and high sensitivity, without being restricted to Stark-tunable systems. Laser frequency switching is discussed also in terms of a theoretical model which exposes the time-dependent properties of a phase-modulated cavity mode. Dephasing studies have been carried out thus far in atomic and molecular gases and low-temperature solids containing inorganic impurity ions or large organic molecules. The utility of the FID effect is emphasized where precise dephasing times are obtained from time-frequency Fourier transformation of FID signals using a digital computer. The first quantitative and detailed test of FID theory is provided by these experimental techniques.
We propose a new technique for measuring the frequency stability of cw laser radiation. The technique relies on using the laser to be tested as a coupling laser in a scheme of electromagnetically-induced transparency (EIT), either on a or a ladder system. A second, frequency tunable laser (stabilization of this laser is not needed) is used both to act as the EIT probe laser, and to form an atomic frequency reference spectrum. The frequency stability is monitored via the frequency deviation of the EIT resonance with respect to an atomic reference frequency. We also present an improved dichroic atomic vapor laser lock (DAVLL) method for frequency stabilization based on a nanocell with a thickness.