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International Conference on Ultrafast Phenomena

Programmable Wavefunction Engineering in Cs Rydberg States

P. H. Bucksbaum, Douglass W. Schumacher, Dan Pinkos, J. H. Hoogenraad, Jeffrey L. Krause, Kent R. Wilson

Published Jan 1, 1994• 0 citations
Publisher

Abstract

We used a computer controlled LCD to shape the spectrum of a short laser pulse which was then used to excite a shaped atomic wavepacket. We use amplified programmable shaped optical pulses to engineer Rydberg wavefunctions. The method employs a computer-controlled liquid crystal pulse shaper[l]. The wavefunctions, which are nonstationary states, are monitored by observing temporal interference via the optical Ramsey method[2,3].

DOI
10.1364/up.1994.pd.11

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We used a computer controlled LCD to shape the spectrum of a short laser pulse which was then used to excite a shaped atomic wavepacket. We use amplified programmable shaped optical pulses to engineer Rydberg wavefunctions. The method employs a computer-controlled liquid crystal pulse shaper[l]. The wavefunctions, which are nonstationary states, are monitored by observing temporal interference via the optical Ramsey method[2,3].
We have used amplified, programmable, shaped optical pulses to engineer Rydberg wave packets in cesium. Our apparatus employs a computer-controlled liquid-crystal pulse shaper which could control either the phase or the magnitude of the pulse's spectrum. The shaped optical field was analyzed via cross correlation and frequency-resolved optical gating. The wave-packet evolution was analyzed by monitoring temporal interference via the optical Ramsey method to obtain both auto- and cross-interferograms of the engineered wave packet.
The control of atoms and molecules using coherent light fields has been a long-standing goal in chemical physics. This thesis discusses experiments which use a programmable pulse shaper to control the quantum state of electronic wavepackets in Rydberg atoms and electronic and nuclear dynamics in molecular liquids. The shape of Rydberg wavepackets was controlled by using tailored ultrafast pulses to excite a beam of cesium atoms. The quantum state of these atoms was measured using holographic techniques borrowed from optics. The experiments with molecular liquids involved the construction of an automated learning machine. A Genetic Algorithm directed the choice of shaped pulses which interacted with the molecular system inside a learning control loop. Analysis of successful pulse shapes that were found by using the GA yield insight into the systems being controlled.
A longstanding goal in chemical physics has been the control of atoms and molecules using coherent light fields. This paper provides a brief overview of the field and discusses experiments that use a programmable pulse shaper to control the quantum state of electronic wavepackets in Rydberg atoms and electronic and nuclear dynamics in molecular liquids. The shape of Rydberg wavepackets was controlled by using tailored ultrafast pulses to excite a beam of caesium atoms. The quantum state of these atoms was measured using holographic techniques borrowed from optics. The experiments with molecular liquids involved the construction of an automated learning machine. A genetic algorithm directed the choice of shaped pulses which interacted with the molecular system inside a learning control loop. Analysis of successful pulse shapes that were found by using the genetic algorithm yield insight into the systems being controlled.
Atoms in high-lying Rydberg states with large values of the principal quantum number n, n {ge} 300, form a valuable laboratory in which to explore the control and manipulation of quantum states of mesoscopic size using carefully tailored sequences of short electric field pulses whose characteristic times (duration and/or rise/fall times) are less than the classical electron orbital period. Atoms react to such pulse sequences very differently than to short laser or microwave pulses providing the foundation for a number of new approaches to engineering atomic wavefunctions. The remarkable level of control that can be achieved is illustrated with reference to the generation of localized wavepackets in Bohr-like near-circular orbits, and the production of non-dispersive wavepackets under periodic driving and their transport to targeted regions of phase space. The testing of these control schemes, together with their reversibility, through the creation of electric dipole echoes in Stark wavepackets, is also described. New protocols continue to be developed that will allow even tighter control with the promise of new insights into quantum-classical correspondence, information storage in mesoscopic systems, physics in the ultra-fast ultra-intense regime and nonlinear dynamics in driven systems.
Programmable control of individual pulses in a high-repetition-rate (typically MHz) ultrafast pulse train is a long-standing goal for optical arbitrary waveform synthesis. Here, we report a programmable pulse-by-pulse shaper that enables deterministic spectral-temporal control of ultrafast pulses at a repetition rate of ∼\sim∼ 20~MHz. By synchronizing an FPGA-driven electro-optic modulation on the stretched waveform in a temporal 4fff shaping system, the regime writes pulse-index-dependent spectral phase profiles onto individual pulses. We demonstrate three levels of programmable ability: zero-order phase coding that maps pulse-by-pulse phase sequences into double-slit-like spectral-temporal interference; first-order phase programming that produces arbitrary temporal trajectories with deterministic delay; and fractional-order phase engineering that generates programmable temporal breathing. By launching the shaped pulse train into a nonlinear fiber stage, the programmed temporal breathing is converted into one spectral breathing. We further construct a phase-level-dependent regime map of nonlinear spectral breathing, revealing transitions from weak single-envelope breathing to multi-peak spectral splitting and strongly breathing merged-spectrum dynamics, in agreement with numerical simulations. This pulse-by-pulse spectral-temporal synthesis platform establishes pulse index as a programmable degree of freedom for ultrafast pulse shaping and provides a route toward real-time and pulse resolved optical arbitary waveform synthesis.