Erratum: Direct imaging of rotational wave packet dynamics of diatomic molecules [Phys. Rev. A<b>68</b>, 023406 (2003)]

Dooley, P. W.; Litvinyuk, Igor; Lee, Kevin F.; Rayner, D. M.; Spanner, M.; Villeneuve, D. M.; Corkum, P. B.

doi:10.1103/physreva.74.059906

Cited by 64 publications

(110 citation statements)

References 0 publications

Supporting

Mentioning

106

Contrasting

Order By: Relevance

“…2, and the alignment of the S axis was measured with a pulse linearly polarized along the x axis (probe II). The symmetries of these probe geometries ensures that there can be no probe induced rotation in the plane of the measured angle [9]. For both measurements, probe-only Coulomb explosion data from a randomly oriented gas sample was used to characterize the nonuniform orientation dependence of the ionization efficiency, and any detector defects.…”

Section: Fig 2 (Color Online)mentioning

confidence: 99%

“…The 3D velocity vector of each fragment was measured using a time and position sensitive delay line anode detector in a time-of-flight spectrometer [9]. The detector system employed allowed for coincident detection of ion arrivals.…”

Section: Fig 2 (Color Online)mentioning

confidence: 99%

“…In order to unambiguously demonstrate FF3DA, we employ coincidence Coulomb explosion imaging which determines the complete 3D lab frame orientation of each molecule [9,10]. For each molecule measured, we determine two angles, # O and # S , depicted in Fig.…”

mentioning

confidence: 99%

See 2 more Smart Citations

Field-Free Three-Dimensional Alignment of Polyatomic Molecules

et al. 2006

Self Cite

View full text Add to dashboard Cite

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...

show abstract

Section: Fig 2 (Color Online)mentioning

confidence: 99%

Section: Fig 2 (Color Online)mentioning

confidence: 99%

See 1 more Smart Citation

Field-Free Three-Dimensional Alignment of Polyatomic Molecules

et al. 2006

Self Cite

View full text Add to dashboard Cite

show abstract

“…However, rotational wavepackets have been previously observed in heavy many-electron systems (N 2 [6], O 2 [13,14], CO 2 [15,16], CS 2 [16], I 2 [17] etc. ), where rotations occur with periods on the picosecond time scale.…”

mentioning

confidence: 99%

“…Traditional 'brute force' techniques employing strong DC fields [2,3] have recently yielded to new, more subtle and yet more powerful and versatile techniques using intense laser systems [4,5]. In particular intense femtosecond pulses have been successfully used to align molecules along an axis for application in areas such as the study of fragmentation dynamics [6,7], high harmonic generation [8,9] and the creation of single cycle laser pulses [10]. In this case the alignment of a molecule (or spatial ordering of an ensemble of molecules) evolves temporally following the creation of a rotational wavepacket by a linearly polarized laser pulse of far shorter duration than the natural period of rotation.…”

mentioning

confidence: 99%

Mapping the evolution of optically generated rotational wave packets in a room-temperature ensemble ofD2

et al. 2007

View full text Add to dashboard Cite

A coherent superposition of rotational states in D2 has been excited by nonresonant ultrafast (12 femtosecond) intense (2 × 10 14 Wcm −2 ) 800 nm laser pulses leading to impulsive dynamic alignment. Field-free evolution of this rotational wavepacket has been mapped to high temporal resolution by a time-delayed pulse, initiating rapid double ionization, which is highly sensitive to the angle of orientation of the molecular axis with respect to the polarization direction, θ. The detailed fractional revivals of the neutral D2 wavepacket as a function of θ and evolution time have been observed and modelled theoretically.PACS numbers: 42.50. Hz, 33.80.Gj, 33.80.Wz The importance of being able to enforce spatial order on an initially random ensemble of molecules has been recognized since the discovery of steric effects in chemical reactions [1]. Traditional 'brute force' techniques employing strong DC fields [2,3] have recently yielded to new, more subtle and yet more powerful and versatile techniques using intense laser systems [4,5]. In particular intense femtosecond pulses have been successfully used to align molecules along an axis for application in areas such as the study of fragmentation dynamics [6,7], high harmonic generation [8,9] and the creation of single cycle laser pulses [10]. In this case the alignment of a molecule (or spatial ordering of an ensemble of molecules) evolves temporally following the creation of a rotational wavepacket by a linearly polarized laser pulse of far shorter duration than the natural period of rotation.In this Letter, we report on a detailed ultrafast study of the temporal evolution of such a rotational wavepacket in the neutral deuterium molecule D 2 . The wavepacket is created impulsively by a 12 femtosecond laser pulse, with temporal and angular ordering probed at some later time with a similar pulse that initiates sequential double. Such high resolution measurements represent the state-of-theart in ultrafast molecular physics in the high rotational frequency limit as dictated by this most fundamental and theoretically tractable of molecules.It is known that an intense linearly polarized laser pulse interacting with an ensemble of molecules generates a degree of spatial alignment from a random ensemble [4,5]. The only condition for this phenomenon is that the molecular polarizability is anisotropic. Thus, the induced dipole moment created in the interaction with the electric field of the laser generates a torque that causes the axis of maximum polarizability to librate around the polarization vector of the laser field. Quantum mechanically, the process is described as a sequence of Rabi-type cycles accompanied by the exchange of two quanta of angular momentum between the molecule and the laser field. If the aligning pulse duration is much greater than the rotational period, the system evolves adiabatically to the the so-called pendular states, which dissipate as soon as the laser pulse passes [12]. However, when the pulse duration is much shorter than the rotational perio...

show abstract

Time‐Resolved Photoelectron Spectroscopy of Nonadiabatic Dynamics in Polyatomic Molecules

Stolow

Underwood

2008

Advances in Chemical Physics

166

201

View full text Add to dashboard Cite

Erratum: Direct imaging of rotational wave packet dynamics of diatomic molecules [Phys. Rev. A68, 023406 (2003)]

Abstract: There is a typographical error in the Appendix resulting in a missing factor of 2. Specifically, Eq. ͑A6͒ should read͑A6͒

Cited by 64 publications

References 0 publications

Field-Free Three-Dimensional Alignment of Polyatomic Molecules

Field-Free Three-Dimensional Alignment of Polyatomic Molecules

Mapping the evolution of optically generated rotational wave packets in a room-temperature ensemble ofD2

Time‐Resolved Photoelectron Spectroscopy of Nonadiabatic Dynamics in Polyatomic Molecules

Contact Info

Product

Resources

About