Controlling Atomic Line Shapes

Lin, C. D.; Chu, Wei-Chun

doi:10.1126/science.1238396

Cited by 21 publications

(17 citation statements)

References 5 publications

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“…is complex from the aspect of Autler-Townes splitting, it manifests clearly an asymmetric lineshape with the changes of t, similar to the Fano profile resulting from the interference of the transition to the bound state embedded in the continuum [32,34,[52][53][54]. As was recently approved, the laser control allows us to manipulate the interference and as the results of changing the lineshape of the transient absorption spectra from the Lorentz to Fano profile [31,55,56]. In the present case of CO, the final bound state F , with a large shift of the PEC equilibrium from the ground state and core-excited state and a shallow PEC with the vibrational frequency much smaller than the bandwidth of the control pulse, can be considered as a quasicontinuum, similar to the molecular dissociative continuum, where the Fano profile for the populations dynamics was observed earlier [57].…”

Section: Numerical Resultsmentioning

confidence: 99%

Nonlinear resonant Auger spectroscopy in CO using an x-ray pump-control scheme

2016

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In the present paper we propose nonlinear femtosecond x-ray pump-probe spectroscopy to study the vibrational dynamics of a core-excited molecular state and discuss numerical results in CO. A femtosecond pump resonantly excites the carbon core-excited 1s-1π * state of the CO molecule. A second strong probe (control) pulse is applied at variable delay and is resonantly coupled to a valence excited state of the molecule. The strong nonlinear coupling of the control pulse induces Rabi flopping between the two electronic states. During this process, a vibrational wave packet in the core-excited state is created, which can be effectively manipulated by changing the time delay between pump and control pulses. We present an analysis of the resonant Auger electron spectrum and the transient absorption or emission spectrum on the pump transition and discuss their information content for reconstruction of the vibrational wave packet.

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Section: Numerical Resultsmentioning

confidence: 99%

Nonlinear resonant Auger spectroscopy in CO using an x-ray pump-control scheme

2016

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“…Here, we demonstrate a new scheme for ATAS combining the measurement of time-resolved quantum dynamics with the characterization of the few-cycle driving laser pulse in one single experiment. Our method is based on extracting the time-delay-dependent phase shift [11,[13][14][15] imprinted on a resonance, which is excited by XUV light and dressed by the femtosecond laser pulse that is to be characterized. From this phase shift, we are able to directly obtain the laser pulse duration, as well as its time dependent intensity.…”

Section: Fig 1 Dipole Control Model (A)mentioning

confidence: 99%

In situ characterization of few-cycle laser pulses in transient absorption spectroscopy

Blättermann¹,

Ott²,

Kaldun³

et al. 2015

Opt. Lett.

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Fig. 1. Dipole control model. (a)Perturbations to the field-free evolution of the dipole response (dashed blue) are treated as instantaneous modifications of the amplitude and phase expressed by the complex factor A. The perturbed decay (dark purple, light purple) is shown for two time-delays ( 1 , 2 ) leading to very different spectral line shapes (inset). (b) Treatment of a ponderomotive shift in the dipole control model. Instead of a continuously modified dipole phase ( ) , the effect of the dressing field is approximated by a single phase step at time , the peak of the intense laser pulse envelope. Since the temporal profile of the dressing laser pulse intensity is mapped onto ( ) via Eq. (4), it is possible to determine both the pulse duration and intensity.In situ characterization of few-cycle laser pulses in transient absorption spectroscopy Attosecond transient absorption spectroscopy has thus far been lacking the capability to simultaneously characterize the intense laser pulses at work within a time-resolved quantum-dynamics experiment. However, precise knowledge of these pulses is key to extracting quantitative information in strong-field highly nonlinear light-matter interactions. Here, we introduce and experimentally demonstrate an ultrafast metrology tool based on the time-delay-dependent phase shift imprinted on a strong-field driven resonance. Since we analyze the signature of the laser pulse interacting with the absorbing spectroscopy target, the laser pulse duration and intensity are determined in situ. As we also show, this approach allows for the quantification of time-dependent bound-state dynamics in one and the same experiment. In the future, such experimental data will facilitate more precise tests of strong-field dynamics theories.In the transformative field of ultrafast light-matter interaction, characterization of strong-field laser pulses is crucial in order to draw quantitative conclusions from measurement results. Based on the detection of photoelectrons, the attosecond streaking technique provides insight into the system's underlying quantum dynamics on the natural electronic time scale, combined with a powerful characterization of the used strong-field laser pulses [1][2][3]. Being capable of resolving bound-state quantum dynamics, the all-optical method of attosecond transient absorption spectroscopy (ATAS) [4][5][6][7][8][9][10][11][12] is an important complement to photoelectron-based methods. In addition to being sensitive to bound-bound transitions, ATAS allows targets to be studied all the way from a natural -weak-field -environment up to the strong-field regime. Using attosecond pulsed extreme-ultraviolet (XUV) light together with (typically) femtosecond nearinfrared (NIR) pulses in a pump-probe scheme, dynamical processes leave their fingerprints in the spectrum of the transmitted XUV light. Yet unlike streaking, up to now ATAS lacks the possibility for in-situ characterization of the femtosecond NIR laser pulse, which drives and controls the underlying electron dynamics. ...

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“…The current representative result confirms that the replacement reaction can be triggered between Mn 3 O 4 and Co 2+ , resulting in hollow Co 3 O 4 nanocages. 22 …”

Section: Introductionmentioning

confidence: 99%

Galvanic replacement synthesis of Ag_xAu_1−x@CeO₂ (0 ≤ x ≤ 1) core@shell nanospheres with greatly enhanced catalytic performance

Liu

Feng

2015

Chem. Sci.

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Controlling Atomic Line Shapes

Abstract: Intense infrared lasers can be used to control the spectral line shapes of atoms, with implications for spectroscopy and quantum dynamical processes. [Also see Report by Ott et al. ]

Cited by 21 publications

References 5 publications

Nonlinear resonant Auger spectroscopy in CO using an x-ray pump-control scheme

Nonlinear resonant Auger spectroscopy in CO using an x-ray pump-control scheme

In situ characterization of few-cycle laser pulses in transient absorption spectroscopy

Galvanic replacement synthesis of Ag_xAu_1−x@CeO₂ (0 ≤ x ≤ 1) core@shell nanospheres with greatly enhanced catalytic performance

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Controlling Atomic Line Shapes

Abstract: Intense infrared lasers can be used to control the spectral line shapes of atoms, with implications for spectroscopy and quantum dynamical processes. [Also see Report by Ott et al. ]

Cited by 21 publications

References 5 publications

Nonlinear resonant Auger spectroscopy in CO using an x-ray pump-control scheme

Nonlinear resonant Auger spectroscopy in CO using an x-ray pump-control scheme

In situ characterization of few-cycle laser pulses in transient absorption spectroscopy

Galvanic replacement synthesis of AgxAu1−x@CeO2 (0 ≤ x ≤ 1) core@shell nanospheres with greatly enhanced catalytic performance

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Galvanic replacement synthesis of Ag_xAu_1−x@CeO₂ (0 ≤ x ≤ 1) core@shell nanospheres with greatly enhanced catalytic performance