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Updated: Nov 10, 2025

Ultrafast Time-resolved Near-IR Stimulated Raman Measurements of Functional π-conjugate Systems
Published on: February 10, 2020
Cascaded frequency conversion under nonlinear stimulated Raman adiabatic passage
Abstract:
A comprehensive study of two simultaneous three wave mixing processes, a second harmonic generation followed by difference frequency generation, under nonlinear stimulated Raman adiabatic passage (STIRAP) is presented. An input pump is up-converted to its second harmonic, which then gets down-converted to a signal and idler pair with frequencies lying very close to the input pump in such a manner that complete conversion from the pump to the signal and idler takes place without exciting the second harmonic under counterintuitive adiabatic passage. This process involves nonlinear STIRAP with a nonlinear dark state similar to atomic population transfers, and we bring an analogy from atomic systems to our nonlinear dynamics to linearize the problem and analytically obtain the adiabaticity condition required for complete conversion. We also show that the nonlinear STIRAP mechanism results in a large bandwidth of about 380 nm with almost complete conversion of the pump to the signal and idler.
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