We present detailed experimental and theoretical results on population transfer with frequency‐swept picosecond laser pulses. Here, we demonstrate that intense frequency‐swept pulses, when applied in the adiabatic limit, lead to both more efficient and more selective excitation than do unmodulated laser pulses. The experimental work is performed on quasi‐two‐level systems (pentacene/p‐terphenyl crystal and Na vapor), quasi‐three‐level systems (Na vapor), and on more complex multilevel systems (I2 vapor). We discuss the different characteristics of adiabatic population transfer in both few‐level, and multilevel cases, and, in particular, present computer calculations to explore the effects of molecular rotations in multilevel adiabatic population transfer.
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