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A detailed examination of stimulated pump-probe measurements of vibrational population relaxation

Review of Scientific Instruments, ISSN: 0034-6748, Vol: 67, Issue: 12, Page: 4085-4091
1996
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We have developed and demonstrated a pump-probe laser spectroscopic scheme to measure ground state vibrational population relaxation. There are two significant advantages to this technique over alternative measurement methods. The first is that the detection sensitivity of the pump-probe method is limited by the shot noise present on the probe laser and the second is that, because of the manner in which the ground state vibration(s) are populated, it is possible to interrogate T processes for degenerate donor-acceptor conditions. We detail in this article the form of the experimental stimulated signal, the effect of the detection scheme used, and the consequences of spontaneous (Boltzmann) population of ground state vibrations. A central conclusion of this work is that, even for small signal limit pump-probe experiments, absorption, stimulated emission, and spontaneous emission all play important roles in collectively determining the form of the experimental signal. © 1996 American Institute of Physics.

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