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The Journal of Chemical Physics

Broadband population inversion by phase modulated pulses

Jean Baum, Robert Tycko, Alexander Pines

Published Nov 1, 1983• 117 citations
Publisher

Abstract

We present a class of continuously phase modulated radiation pulses that result in coherent population inversion over a large range of transition frequencies. The continuously modulated pulses can be approximated by sequences of discrete phase shifted pulses. Simulations of the inversion properties of the continuously modulated pulses and of the discrete pulse sequences are given.

DOI
10.1063/1.446381

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We present a class of continuously phase modulated radiation pulses that result in coherent population inversion over a large range of transition frequencies. The continuously modulated pulses can be approximated by sequences of discrete phase shifted pulses. Simulations of the inversion properties of the continuously modulated pulses and of the discrete pulse sequences are given.
We describe a class of continuously phase-modulated radiation pulses that result in coherent population inversion on resonance as well as over a large range of transition frequencies and radiation field strengths. This is a population-inversion analogy to self-induced transparency. Simulations of the inversion properties of the modulated inversion pulse (MIP) are presented. It is shown that the inversion behavior can be explained by treating the MIP as a highly efficient adiabatic sweep. Criteria for establishing adiabaticity are discussed in detail. Finally, a method is presented for generating a sequence of phase-shifted radio-frequency pulses, from the continuously modulated pulse, which can be implemented on modern NMR and coherent optical spectrometers; experimental confirmation is given.
Frequency swept pulses are used to invert population over a broad band of transition frequencies without the need for a precise calibration of the pulse amplitude. As long as the adiabatic approximation is valid, population is adiabatically inverted at each individual transition frequency of the swept range. Even though this picture fails to be true when the adiabatic approximation breaks down, population inversion can still be achieved for an appreciable range of transition frequencies and field amplitudes. We discuss population inversion in an ensemble of two-level systems by a frequency-swept pulse, the so-called constant adiabaticity pulse, without invoking the adiabatic approximation. The equations of motion are integrated by a seminumerical method to analyze population inversion in the regime where usually the adiabatic approximation is applied. The effects of resonance offset and variable pulse amplitude are described by an average Hamiltonian expansion to discuss pulse performance beyond the validity of the adiabatic approximation. As a function of the adiabaticity parameter (reciprocal of the pulse area), the inversion bandwidth increases in a stepwise fashion due to the consecutive cancellation of average Hamiltonians. The first inversion over a finite range of transition frequencies and pulse amplitudes is shown to occur for an adiabaticity parameter of 1/15.
We propose a technique for coherent population inversion of a two-state system, which uses an amplitude-modulated pulse. In the modulation-free adiabatic basis, the modulation introduces oscillating interaction between the adiabatic states. In a second rotating-wave approximation picture, this oscillating interaction induces a pair of level crossings between the energies of the adiabatic states if the modulation frequency is chosen appropriately. By suitably offsetting the modulation with respect to the center of the pulse, one can make the modulation act only in the vicinity of one of these crossings. In a higher-order adiabatic basis, this crossing shows up as an avoided crossing between the energies of the higher-order adiabatic states. As a result robust and efficient population transfer can be achieved between the adiabatic states, and hence, between the original bare states. We derive analytically the conditions on the interaction parameters for this technique and verify them with numerical simulations. Possible experimental implementations are discussed.
We introduce a method to rotate arbitrarily the excitation profile of universal broadband composite pulse sequences for robust high-fidelity population inversion. These pulses compensate deviations in any experimental parameter (e.g., pulse amplitude, pulse duration, detuning from resonance, Stark shifts, unwanted frequency chirp, etc.) and are applicable with any pulse shape. The rotation allows one to achieve higher-order robustness to any combination of pulse area and detuning errors at no additional cost. The latter can be particularly useful, e.g., when detuning errors are due to Stark shifts that are correlated with the power of the applied field. We demonstrate the efficiency and universality of these composite pulses by experimental implementation for rephasing of atomic coherences in a Pr3+:Y2SiO5{\text{Pr}}^{3+}\text{:}{\text{Y}}_{2}{\text{SiO}}_{5}Pr3+:Y2​SiO5​ crystal.