Eur. Phys. J. D 14, 147-155 (2001)
https://doi.org/10.1007/s100530170212

General theory of population transfer by adiabatic rapid passage with intense, chirped laser pulses

University of Florida, Quantum Theory Project, P.O. Box 118435, Gainesville, FL 32611–8435, USA

Corresponding author: ^a krause@qtp.ufl.edu

Received: 6 September 2000
Revised: 25 September 2000
Published online: 15 May 2001

Abstract

We present a general theory of adiabatic rapid passage (ARP) with intense, linearly chirped laser pulses. For pulses with a Gaussian profile and a fixed bandwidth, we derive a rigorous formula for the maximum temporal chirp rate that can be sustained by the pulse. A modified Landau-Zener formula displays clearly the relationships among the pulse parameters. This formula is used to derive the optimal conditions for efficient, robust population transfer. As illustrations of the theory, we present results for two- and four-level systems, and selective vibronic excitation in the I₂ molecule. We demonstrate that population transfer with chirped pulses is more robust and more selective than population transfer with transform-limited pulses.