Laser Field Alignment of Organic Molecules on Semiconductor Surfaces: Toward Ultrafast Molecular Switches

Reuter, Matthew G.; Sukharev, Maxim; Seideman, Tamar

doi:10.1103/physrevlett.101.208303

Cited by 66 publications

(65 citation statements)

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“…Manipulating the molecular rotational degrees of freedom in gas phase by means of laser fields remains a very attractive topic in quantum control [1,2] with a wide range of applications in photochemistry extending from chemical reactivity [3,4] to nanoscale design [5,6], stereochemistry [7], surface processing [5,8], catalysis [9], and attosecond molecular dynamics [10]. Such phenomena play also a role in quantum computing [11] and high-order harmonic generation [12,13,14,15].…”

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confidence: 99%

Observation of the field-free orientation of a symmetric-top molecule by terahertz laser pulses at high temperature

et al. 2016

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We investigate experimentally and numerically the field-free orientation of the symmetric top molecule of methyl-iodide at high temperature using a terahertz radiation generated by a plasma induced by a two-color laser beam. The degree of orientation is measured from the free-induction decay emitted by the sample. The observed experimental signal is reproduced with a good accuracy by numerical simulations.

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Section: Introductionmentioning

confidence: 99%

Observation of the field-free orientation of a symmetric-top molecule by terahertz laser pulses at high temperature

et al. 2016

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“…The torsional motion of nonrigid quantum objects [7,31] or surface adsorbed molecules [29,32,33] is governed by a 2π -periodic potential about the torsional or dihedral angle [34]. Variations in the relative alignment of the two moieties will lead to variations in, e. g., the current through a molecular switch [31,35].…”

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Strongly driven quantum pendulum of the carbonyl sulfide molecule

et al. 2014

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We demonstrate and analyze a strongly driven quantum pendulum in the angular motion of state-selected and laser-aligned carbonyl sulfide molecules. Raman couplings during the rising edge of a 50-ps laser pulse create a wave packet of pendular states, which propagates in the confining potential formed by the polarizability interaction between the molecule and the laser field. This wave-packet dynamics manifests itself as pronounced oscillations in the degree of alignment with a laser-intensity-dependent period. Pendular states, directional superpositions of field-free rotational states, are created by the anisotropic interaction between an isolated molecule and a strong electric field [1][2][3][4]. In a classical sense, this corresponds to the free rotation of the molecule changing into a restricted angular motion, where a molecular axis librates about the field direction. In the case of a strong static electric field the pendular states result from the interaction with the permanent dipole moment. This was exploited, for instance, for the simplification of spectroscopic signatures of large molecular clusters [5]. In the case of a nonresonant laser field the pendular states are formed due to the interaction with the molecular polarizability. This interaction constitutes the basis for laser-induced alignment [3,4], the confinement of molecular axes to laboratory-fixed axes defined by the polarization of the alignment field. Notably, in the limit where the laser field is turned on slowly compared to the inherent rotational period(s) of the molecule, the initial field-free rotational states are converted into the corresponding pendular states. This process is called adiabatic alignment [4] and it has found widespread use in molecular sciences [6][7][8][9][10][11]. The pendular states persist for as long as the laser field is turned on and the molecules return to their initial field-free rotational states upon turning off the laser field, provided this occurs slowly compared to the rotational period(s), τ rot .Pendular states were investigated through frequencyresolved spectroscopy [12,13] and by photodissociation or Coulomb explosion imaging [4,14]. The former approach probes the field-induced changes of the rotational energy levels, thus the pendular state energies, while the latter approach probes the way the molecules are confined in space, i. e., the orientational character of the pendular states. So far these studies were all performed in the adiabatic limit where the classical signature of the pendular states, i. e., the librational motion of a molecular axis about the field direction, cannot be observed directly. To observe this motion it would * jochen.kuepper@cfel.de; http://desy.cfel.de/cid/cmi be necessary to create a coherent superposition of pendular states.Here, we demonstrate that such pendular motion can be induced through the use of a laser pulse with a duration τ laser ∼ τ rot in between the common limits of adiabatic (τ laser τ rot ) and impulsive (τ laser τ rot ) alignment. The intermediate regim...

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“…Within the additive model, only the component α (2,2) depends on ρ, while α (0,0) and α (2,0) are considered to be constant, minimizing the field-induced rotational-torsional coupling, c.f. Eq.…”

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confidence: 99%

“…in terms of the elements of the Wigner D-matrices D J m,k [21] and the symmetry-adapted, molecule-fixed components of the polarizability tensor [18] α (0,0) , α (2,0) and α (2,2) . For molecules with feasible torsion, the latter depend on the torsion angle ρ, resulting in a second, fieldinduced type of rotational-torsional coupling.…”

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confidence: 99%

“…Among the variety of applications of torsional control that have fueled this interest are the control of energy transfer [1], charge transport [2] and chemical reactions [3], the enhancement of transient absorption spectroscopy [4] and the design of molecular rotors [5][6][7]. A relatively recent approach to manipulating the conformation of molecules in the electronic ground state involves the application of a moderately intense, non-resonant laser field to generate a broad torsional wavepacket that is correspondingly localized in the conjugated angle space.…”

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confidence: 99%

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Laser-Controlled Torsions: Four-Dimensional Theory and the Validity of Reduced Dimensionality Models

2017

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Laser Field Alignment of Organic Molecules on Semiconductor Surfaces: Toward Ultrafast Molecular Switches

Cited by 66 publications

References 20 publications

Observation of the field-free orientation of a symmetric-top molecule by terahertz laser pulses at high temperature

Observation of the field-free orientation of a symmetric-top molecule by terahertz laser pulses at high temperature

Strongly driven quantum pendulum of the carbonyl sulfide molecule

Laser-Controlled Torsions: Four-Dimensional Theory and the Validity of Reduced Dimensionality Models

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