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Quantum control using the nonresonant dynamic Stark effect

Benjamin Sussman

Published Jan 1, 2007• 0 citations
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Nonperturbative quantum control schemes in the intermediate field strength (nonionizing) regime are investigated. We restrict the matter-field interaction to the nonresonant dynamic Stark effect (NRDSE) as induced by infrared laser fields, which we argue is a new and general tool for quantum control of atomic and molecular dynamics. For the case of Raman coupled matter states, an effective Hamiltionian may be constructed, and quantum control via NRDSE may be thought of as reversibly modifying the effective Hamiltonian during system propagation, thus leading to control over dynamic processes. As an illustration, the creation of field-free ``switched'' wave packets through the adiabatic turn on and sudden turn off of the NRDSE is considered and experimentally demonstrated. Wave packets generated through the switched NRDSE interaction may be very different in form and content than wave packets generated via resonant transitions with Gaussian optical pulses. In order to provide an example, we discuss the specific case of rotational wave packet dynamics where the NRDSE manifests itself as molecular axis alignment. This technique is applied to the creation of field-free molecular axis alignment using an intense switched $1.064\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$ laser pulse. This switched laser pulse was generated via a plasma shuttering technique, giving a pulse with a rise time of $150\phantom{\rule{0.3em}{0ex}}\mathrm{ps}$ and a fall time of $170\phantom{\rule{0.3em}{0ex}}\mathrm{fs}$. The temporal evolution of the molecular axis alignment is probed via the optical Kerr effect. Field-free alignment via the switched NRDSE is demonstrated for both linear ($\mathrm{C}{\mathrm{O}}_{2}$, $\mathrm{C}{\mathrm{S}}_{2}$) and symmetric top (1,2-propadiene) polyatomic molecules.

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The application of nonresonant lasers to quantum systems can modify energy levels in a general way. This approach, using the nonresonant dynamic Stark effect, is an effective mechanism for modifying chemical dynamics. These molecular techniques have analogous implementations in quantum technologies. Applications include controlling vacuum fluctuations to create molecular alignment and broadband light sources, photonic catalysis, quantum memories in atomic vapours, and photonics in bulk diamond phonons. The links between these different applications are investigated.

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Nonperturbative quantum control schemes in the intermediate field strength (nonionizing) regime are investigated. We restrict the matter-field interaction to the nonresonant dynamic Stark effect (NRDSE) as induced by infrared laser fields, which we argue is a new and general tool for quantum control of atomic and molecular dynamics. For the case of Raman coupled matter states, an effective Hamiltionian may be constructed, and quantum control via NRDSE may be thought of as reversibly modifying the effective Hamiltonian during system propagation, thus leading to control over dynamic processes. As an illustration, the creation of field-free ``switched'' wave packets through the adiabatic turn on and sudden turn off of the NRDSE is considered and experimentally demonstrated. Wave packets generated through the switched NRDSE interaction may be very different in form and content than wave packets generated via resonant transitions with Gaussian optical pulses. In order to provide an example, we discuss the specific case of rotational wave packet dynamics where the NRDSE manifests itself as molecular axis alignment. This technique is applied to the creation of field-free molecular axis alignment using an intense switched $1.064\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$ laser pulse. This switched laser pulse was generated via a plasma shuttering technique, giving a pulse with a rise time of 150ps150\phantom{\rule{0.3em}{0ex}}\mathrm{ps}150ps and a fall time of 170fs170\phantom{\rule{0.3em}{0ex}}\mathrm{fs}170fs. The temporal evolution of the molecular axis alignment is probed via the optical Kerr effect. Field-free alignment via the switched NRDSE is demonstrated for both linear (CO2\mathrm{C}{\mathrm{O}}_{2}CO2​, CS2\mathrm{C}{\mathrm{S}}_{2}CS2​) and symmetric top (1,2-propadiene) polyatomic molecules.
The application of nonresonant lasers to quantum systems can modify energy levels in a general way. This approach, using the nonresonant dynamic Stark effect, is an effective mechanism for modifying chemical dynamics. These molecular techniques have analogous implementations in quantum technologies. Applications include controlling vacuum fluctuations to create molecular alignment and broadband light sources, photonic catalysis, quantum memories in atomic vapours, and photonics in bulk diamond phonons. The links between these different applications are investigated.