Nonadiabatic Alignment of Asymmetric Top Molecules: Field-Free Alignment of Iodobenzene

Péronne, Emmanuel; Poulsen, Mikael D.; Bisgaard, Christer Z.; Stapelfeldt, Henrik; Seideman, Tamar

doi:10.1103/physrevlett.91.043003

Cited by 112 publications

(64 citation statements)

References 20 publications

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“…Quantum mechanically, the two-pulse sequence will enhance the average angular momentum, J 2 , of the molecule [10] and so broaden the J -state composition of the rotational wave packet similar to the effect that happens when the intensity of a single alignment pulse is increased [32]. The larger width of the wave packet in J space, i.e., the larger J 2 , can result in enhanced alignment when the timing of the second pulse is correct.…”

Section: Discussionmentioning

confidence: 99%

Alignment enhancement of molecules embedded in helium nanodroplets by multiple laser pulses

et al. 2015

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We show experimentally that field-free one-dimensional (1D) alignment of 1,4-diiodobenzene molecules embedded in helium nanodroplets, induced by a single, linearly polarized 200-fs laser pulse, can be significantly enhanced by using two or four optimally synchronized laser pulses. The strongest degree of 1D alignment is obtained with four pulses and gives cos 2 θ > 0.60. Besides the immediate implications for molecular frame studies, our results pave the way for more general manipulation of rotational motion of molecules in He droplets.

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Section: Discussionmentioning

confidence: 99%

Alignment enhancement of molecules embedded in helium nanodroplets by multiple laser pulses

et al. 2015

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“…These developments will push the scope of TRPES research to include molecular-frame measurements, photofragment-photoelectron scalar and vector correlations, extreme time scales, and innershell dynamics. For example, the use of shaped, intense nonresonant laser fields to create field-free alignment in polyatomic systems 270,271 will combine with 2D and 3D imaging variants of TRPES to probe molecular-frame dynamics. Further development of the multiply differential photoelectron-photofragment coincidence and coincidence-imaging methods will permit highly detailed investigation of statistical and nonstatistical photoinduced charge and energy flow, an area of fundamental dynamical interest and of interest in applications to the gas-phase photophysics of biomolecules.…”

Section: Discussionmentioning

confidence: 99%

Femtosecond Time-Resolved Photoelectron Spectroscopy

2004

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“…Well developed optimal control technology [11] can be profitably applied to improve the degree of FF3DA and will be an area of future research. This technique is readily scalable to larger molecules, such as aromatic hydrocarbons, for which 1D field-free alignment was achieved [12]. To scale this technique to still larger molecules, it may be necessary to employ longer wavelength laser fields to avoid loworder resonances, ensuring that the Stark interaction with the molecular polarizability is dominant.…”

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confidence: 99%

Field-Free Three-Dimensional Alignment of Polyatomic Molecules

et al. 2006

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We experimentally demonstrate field-free, three-dimensional alignment (FF3DA) of polyatomic asymmetric top molecules. We achieve FF3DA in sulfur dioxide gas using two time-delayed, orthogonally polarized, nonresonant, femtosecond laser pulses. Our method avoids the use of rotational revivals and is therefore more robust to temperature. The alignment is probed using time-delayed coincidence Coulomb explosion imaging. FF3DA will be important for all molecular imaging, dynamics, or spectroscopy experiments for which random alignment leads to a loss of information. DOI: 10.1103/PhysRevLett.97.173001 PACS numbers: 33.15.Bh, 33.55.Be, 33.80.ÿb The random alignment of gas phase molecules generally reduces the information content of a measurement made in the laboratory frame. The situation is analogous to the well-known case of powder, as opposed to crystal, x-ray diffraction. To ameliorate this situation, it is necessary to define the direction of the molecules in the lab frame prior to making a measurement. Polyatomic molecules are generally asymmetric rotors with three distinct axes of rotation. Three-dimensional alignment, i.e., the alignment of all three molecular axes, was achieved in the presence of an aligning laser field [1,2], but this field strongly perturbs the system, distorting the electronic and vibrational structure of the molecule [3] and preventing the measurement of innate molecular properties. Field-free one-dimensional alignment, i.e., alignment of a single molecular axis, was achieved using a short laser pulse [4,5], and by the rapid turn off of an adiabatic strong laser field [6]. In these experiments, maximal alignment is produced after the pulse [4,7] when the molecule is field-free, followed by periodic revivals of the rotational wave packet [4]. The rotational energy level spacings for asymmetric tops are much less regular than for linear and symmetric top molecules. This complicates the rotational wave-packet evolution for asymmetric rotors, reducing alignment at revivals. The degradation of alignment worsens at elevated rotational temperatures due to the incoherent contributions of thermally populated rotational states which can lead to complete obfuscation of the rotational revival structure. This is a challenge for experimentalists since rotational cooling is often compromised in order to produce sufficiently dense molecular beams.Here we report the experimental demonstration of a general, flexible, and robust method for producing fieldfree, three-dimensional alignment (FF3DA) of polyatomic molecules. This method makes use of the prompt alignment occurring just after the laser pulse and is much more robust with respect to temperature effects than is an earlier proposal for FF3DA at rotational revivals [8]. This technique is broadly applicable and we demonstrate it here for the asymmetric top molecule SO 2 .Our method is based upon the use of two time-separated, perpendicularly polarized, nonresonant, femtosecond laser pulses. The first laser pulse produces postpulse 1D alignment of the...

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Nonadiabatic Alignment of Asymmetric Top Molecules: Field-Free Alignment of Iodobenzene

Cited by 112 publications

References 20 publications

Alignment enhancement of molecules embedded in helium nanodroplets by multiple laser pulses

Alignment enhancement of molecules embedded in helium nanodroplets by multiple laser pulses

Femtosecond Time-Resolved Photoelectron Spectroscopy

Field-Free Three-Dimensional Alignment of Polyatomic Molecules

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