Picosecond spectroscopy: The first 20 years

Lasers were at first operating in the pulsed mode. That was the ruby, Cr/sup 3+/, emitting at 694.3 nm with a few kilowatts power, several microseconds time width, and a rather broad non-smooth-spiky-intensity profile. Even with such a primitive laser source, several noteworthy, novel experiments were performed such as two photon processes and second harmonic generation. The advent of Q-switch lasers by means of dyes, Kerr cells and electro-optic crystals introduced the era of high power lasers and laser spectroscopy. The high intensity and rather smooth intensity versus time profile pulses emitted by ruby and Nd/sup 3+//glass lasers provided excellent means for non-linear spectroscopy studies and nanosecond Raman spectroscopy, a field which flourished ten years later. In the mid-sixties, the He/Ne laser was mode locked, and shortly thereafter, the Nd/sup 3+//glass laser was also mode locked and shown to emit picosecond duration pulses. This paper presents what one observes on the screen of an oscilloscope once a laser is set up so as to generate picosecond pulses by use of either a saturable absorbing dye or solid state modulator. What is seen is, of course, a train of pulses. It is characteristic of these pulses that their intensity is extremely high, in the gigawatt region. In this particular case, the band width is approximately twenty to thirty wavenumbers. The method utilized to measure the picosecond pulses, initially, was the two photon method. This paper also gives a more graphic illustration how this technique operates. This same procedure provides an extremely simple technique which the author believes made possible the initial development of the picosecond spectroscopy field