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Title: Coherent phase control of resonance-mediated (2+1) three-photon absorption

Abstract

Femtosecond coherent phase control of resonance mediated (2+1) three-photon absorption is studied both theoretically and experimentally. The regime is perturbative of third order. The photoexcitation coherently combines elements of both nonresonant and resonance-mediated multiphoton transitions. By proper simple pulse shaping the three-photon absorption in Na is effectively controlled experimentally, enhanced up to {approx}300% of the absorption induced by the transform-limited pulse. It is achieved by phase manipulating intra- and intergroup interferences involving two groups of three-photon excitation pathways: (i) on resonance and (ii) near resonance with the intermediate resonance state accessed by nonresonant two-photon transition.

Authors:
; ; ;  [1]
  1. Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa 32000, (Israel)
Publication Date:
OSTI Identifier:
20982219
Resource Type:
Journal Article
Resource Relation:
Journal Name: Physical Review. A; Journal Volume: 75; Journal Issue: 3; Other Information: DOI: 10.1103/PhysRevA.75.031401; (c) 2007 The American Physical Society; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; ABSORPTION; CONTROL; DISTURBANCES; EXCITATION; INTERFERENCE; INTERMEDIATE RESONANCE; MULTI-PHOTON PROCESSES; PHOTON-ATOM COLLISIONS; PHOTONS; PULSES; SODIUM

Citation Formats

Gandman, Andrey, Chuntonov, Lev, Rybak, Leonid, and Amitay, Zohar. Coherent phase control of resonance-mediated (2+1) three-photon absorption. United States: N. p., 2007. Web. doi:10.1103/PHYSREVA.75.031401.
Gandman, Andrey, Chuntonov, Lev, Rybak, Leonid, & Amitay, Zohar. Coherent phase control of resonance-mediated (2+1) three-photon absorption. United States. doi:10.1103/PHYSREVA.75.031401.
Gandman, Andrey, Chuntonov, Lev, Rybak, Leonid, and Amitay, Zohar. Thu . "Coherent phase control of resonance-mediated (2+1) three-photon absorption". United States. doi:10.1103/PHYSREVA.75.031401.
@article{osti_20982219,
title = {Coherent phase control of resonance-mediated (2+1) three-photon absorption},
author = {Gandman, Andrey and Chuntonov, Lev and Rybak, Leonid and Amitay, Zohar},
abstractNote = {Femtosecond coherent phase control of resonance mediated (2+1) three-photon absorption is studied both theoretically and experimentally. The regime is perturbative of third order. The photoexcitation coherently combines elements of both nonresonant and resonance-mediated multiphoton transitions. By proper simple pulse shaping the three-photon absorption in Na is effectively controlled experimentally, enhanced up to {approx}300% of the absorption induced by the transform-limited pulse. It is achieved by phase manipulating intra- and intergroup interferences involving two groups of three-photon excitation pathways: (i) on resonance and (ii) near resonance with the intermediate resonance state accessed by nonresonant two-photon transition.},
doi = {10.1103/PHYSREVA.75.031401},
journal = {Physical Review. A},
number = 3,
volume = 75,
place = {United States},
year = {Thu Mar 15 00:00:00 EDT 2007},
month = {Thu Mar 15 00:00:00 EDT 2007}
}
  • We study in detail coherent phase control of femtosecond resonance-mediated (2+1) three-photon absorption and its dependence on the spectral bandwidth of the excitation pulse. The regime is the weak-field regime of third perturbative order. The corresponding interference mechanism involves a group of three-photon excitation pathways that are on resonance with the intermediate state and a group of three-photon excitation pathways that are near resonant with it. The model system of the study is atomic sodium (Na), for which experimental and numerical-theoretical results are obtained. Prominent among the results is our finding that with simple proper pulse shaping an increase inmore » the excitation bandwidth leads to a corresponding increase in the enhancement of the three-photon absorption over the absorption induced by the (unshaped) transform-limited pulse. For example, here, a 40 nm bandwidth leads to an order-of-magnitude enhancement over the transform-limited absorption.« less
  • We theoretically and experimentally demonstrate the quantum coherent control of the resonance-mediated two-photon absorption in rare-earth ions by the phase-shaped femtosecond laser pulse. Our theoretical results show that the resonance-mediated two-photon absorption can be effectively controlled, but the control efficiency depends on the laser repetition rate in real experiment due to the long lifetime and the short decoherence time of the excited state, and the larger laser repetition rate yields the lower control efficiency. These theoretical results are experimentally confirmed in glass sample doped with Er{sup 3+} by utilizing the femtosecond lasers with low repetition rate of 1 kHz and highmore » repetition rate of 80 MHz.« less
  • The effect of phase modulation of a femtosecond light pulse on three-photon absorption in a diatomic system is studied. Direct three-photon transitions between the initial and final electronic states are considered. The total populations of the final electronic state are calculated for different modulation types as functions of the parameter describing modulation. It is found that the effect of modulation on the three-photon excitation probability substantially depends on the modulation regime. The results of calculations are compared with available experimental data. (nonlinear optical phenomena)
  • We show theoretically and experimentally that two-photon coherent control in a V-shape three-level system projects a one-photon coherent transient in a simple two-level system. The second- and third-order spectral phase terms of a shaped laser pulse play the roles of time and quadratic spectral phase, respectively, in conventional coherent transients. In a three-pulse coherent control experiment of atomic rubidium, the phase and amplitude of controlled transition probability is retrieved from a two-dimensional Fourier-transform spectral peak. It is hoped that this control scheme may harness coherent control capability on multidimensional Fourier-transform spectroscopy.
  • The photochemical reaction dynamics of chlorine dioxide (OClO) are investigated using absorption and resonance Raman spectroscopy. The first Raman spectra of gaseous OClO obtained directly on resonance with the {sup 2}B{sub 1}-{sup 2}A{sub 2} electronic transition are reported. Significant scattering intensity is observed for all vibrational degrees of freedom (the symmetric stretch, bend, and asymmetric stretch), demonstrating that structural evolution occurs along all three normal coordinates following photoexcitation. The experimentally measured absorption and resonance Raman intensities are compared to the intensities predicted using both empirical and ab initio models for the optically active {sup 2}A{sub 2} surface. Comparison of themore » experimental and theoretical absorption spectra demonstrates that the frequencies and intensities of transitions involving the asymmetric stretch are well reproduced by the empirical model characterized by a double-minimum along the asymmetric stretch. However, the ab initio model is also found to reproduce a subset of the experimental intensities. In addition, the extremely large resonance Raman intensity of the asymmetric stretch overtone transition is predicted by both models. The results presented here taken in combination with the model for the {sup 2}A{sub 2} surface in condensed environments suggest that the phase-dependent photochemical reactivity of OClO is due to environment-dependent excited-state structural evolution along the asymmetric stretch coordinate.« less