Strong-field two-photon transition by phase shaping (original) (raw)
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Strong-field two-photon absorption in atomic cesium: an analytical control approach
Optics Express, 2009
We have considered an analytical control of two-photon absorption process of atoms in the strong-field interaction regime. The experiment was performed on gaseous cesium atoms strongly interacting with a shaped laser-pulse from a femtosecond laser amplifier and a programmable pulse-shaper. When this shaped laser-pulse transfers the atomic population from the 6s ground state to the 8s excited state, we have found that both positively-and negatively-chirped laser pulses, compared with a Gaussian pulse, enhance this excitation in the strong-field regime of laser-atom interaction. This unusual phenomena is explained because the temporal shape of the laser intensity compensates the effect of dynamic Stark shift for the two-photon resonant condition to be optimally maintained. We provide analytic calculations using the strong-field phase matching, which show good agreement with the experiment.
Journal of Physics B: Atomic, Molecular and Optical Physics, 2008
Coherent control of femtosecond two-photon absorption in the intermediate-field regime is analyzed in detail in the powerful frequency domain using an extended 4 th-order perturbative description. The corresponding absorption is coherently induced by the weak-field non-resonant two-photon transitions as well as by four-photon transitions involving three absorbed photons and one emitted photons. The interferences between these two groups of transitions lead to a difference between the intermediate-field and weak-field absorption dynamics. The corresponding interference nature (constructive or destructive) strongly depends on the detuning direction of the pulse spectrum from half the two-photon transition frequency. The model system of the study is atomic sodium, for which both experimental and theoretical results are obtained. The detailed understanding obtained here serves as a basis for coherent control with rationally-shaped femtosecond pulses in a regime of sizable absorption yields.
Strong-field quantum control of 2 + 1 photon absorption of atomic sodium
Optics express, 2011
We demonstrate ultrafast coherent control of multiphoton absorption in a dynamically shifted energy level structure. In a three-level system that models optical interactions with sodium atoms, we control the quantum interference of sequential 2 + 1 photons and direct three-photon transitions. Dynamic change in energy levels predicts an enormous enhancement of |7p>-state excitation in the strong-field regime by a negatively chirped pulse. In addition, the |4s>-state excitation is enhanced symmetrically by nonzero linear chirp rates given as a function of laser peak intensity and laser detuning. Experiments performed by ultrafast shaped-pulse excitation of ground-state atomic sodium verifies the various strong-field contributions to |3s>-|7p> and |3s>-|4s> transitions. The result suggests that for systems of molecular level understanding adiabatic control approach with analytically shaped pulses becomes a more direct control than feedback-loop black-box approaches.
Physical Review A, 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 in 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.
Two-Photon Coherent Atomic Absorption of Multiple Laser Beams
2006
Physical processes on two-photon coherent atomic absorption of multiple laser beams were discussed about thirty years ago [M. C. Li, Bull. Am. Phys. Soc. 20, 654 (1975)]. These processes can be divided into two distinct groups. In the first group, laser beams are from a single source, and in the second group laser beams are from two different sources [M. C. Li, Phys. Rev. A 22 (1980) 1323]. Several experiments in the first group were carried out and have led to the 2005 Nobel Prize in physics. The second group is more interesting. Beside atoms are in random motion, two photons are from different sources. Classically, it is impossible for atoms to transit coherently in the absorption process, but quantum mechanically, such a transition is possible and that is one of the spooky phenomena in quantum mechanic. To assure the coherent transition, each photon as absorbed by the atom must have two possible paths of choices. If one photon has the choice and other one is not, then the atomic transitions cannot be coherent. Around1990, there were very active experimental pursuits on such a spooky phenomenon of two photons emitted from crystal parametric down conversion. The present talk will review various spooky phenomena associated with two-photon coherent atomic absorption. Hope that the talk will stimulate the interest on the long neglected experimental front on two-photon coherent atomic absorption from two different laser sources.
Quantum focusing and coherent control of nonresonant two-photon absorption in frequency domain
Optics Letters, 2014
We theoretically investigate the nonresonant two-photon absorption (TPA) process in a two-level atom induced by a weak chirped pulse in the frequency domain. According to the extremum condition of the two-photon transition probability (TPTP) at the transition center frequency, we propose a Fresnel-inspired pulse tailoring scheme for TPA that is significantly different from that of Broers et al. [Phys. Rev. A 46, 2749 (1992)]. Using this scheme, the TPTP can be focused or eliminated completely by constructively or destructively modulating various pathways of the quantum interference. Our results are a significant improvement on those obtained by Broers et al. and will have potential applications in selective two-photon microscopy and spectroscopy.
Coherent Control of Single-Photon Absorption and Reemission in a Two-Level Atomic Ensemble
Physical Review Letters, 2012
We demonstrate coherent control of single-photon absorption and reemission in a two-level cold atomic ensemble. This is achieved by interfering the incident single-photon wave packet with the emission (or scattering) wave. For a photon with an exponential growth waveform with a time constant equal to the excited-state lifetime, we observe that the single-photon emission probability during the absorption can be suppressed due to the perfect destructive interference. After the incident photon waveform is switched off, the absorbed photon is then reemitted to the same spatial mode as that of the incident photon with an efficiency of 20%. For a photon with an exponential decay waveform with the same time constant, both the absorption and reemission occur within the waveform duration. Our experimental results suggest that the absorption and emission of a single photon in a two-level atomic ensemble may possibly be manipulated by shaping its waveform in the time domain.
Coherent phase control of resonance-mediated(2+1)three-photon absorption
Physical Review A, 2007
Femtosecond coherent phase control of resonance mediated ͑2+1͒ 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 ϳ300% of the absorption induced by the transform-limited pulse. It is achieved by phase manipulating intraand intergroup interferences involving two groups of three-photon excitation pathways: ͑i͒ on resonance and ͑ii͒ near resonance with the intermediate resonance state accessed by nonresonant two-photon transition.
Strong-field spatiotemporal ultrafast coherent control in three-level atoms
Physical Review A, 2010
Simple analytical approaches for implementing strong field coherent control schemes are often elusive due to the complexity of the interaction between the intense excitation field and the system of interest. Here, we demonstrate control over multiphoton excitation in a three-level resonant system using simple, analytically derived ultrafast pulse shapes. We utilize a two-dimensional spatiotemporal control technique, in which temporal focusing produces a spatially dependent quadratic spectral phase, while a second, arbitrary phase parameter is scanned using a pulse shaper. In the current work, we demonstrate weak-to-strong field excitation of 85 Rb, with a π phase step and the quadratic phase as the chosen control parameters. The intricate dependence of the multilevel dynamics on these parameters is exhibited by mapping the data onto a two-dimensional control landscape. Further insight is gained by simulating the complete landscape using a dressed-state, time-domain model, in which the influence of individual shaping parameters can be extracted using both exact and asymptotic time-domain representations of the dressed-state energies.
Journal of Physics B-atomic Molecular and Optical Physics, 2008
Coherent control of resonant and non-resonant two-photon absorption processes was examined using a spatio-temporal pulse-shaping technique. By utilizing a combination of temporal focusing and femtosecond pulse-shaping techniques, we spatially control multiphoton absorption processes in a completely deterministic manner. Distinctive symmetry properties emerge through two-dimensional mapping of spatio-temporal data. These symmetries break down in the transition to strong fields, revealing details of strong-field effects such as power broadenings and dynamic Stark shifts. We also present demonstrations of chirp-dependent population transfer in atomic rubidium, as well as the spatial separation of resonant and non-resonant excitation pathways in atomic caesium.