Nonadiabatic Alignment by Intense Pulses. Concepts, Theory, and Directions

We review the theory of intense laser alignment of molecules and present a survey of the many recent developments in this rapidly evolving field. Starting with a qualitative discussion that emphasizes the physical mechanism responsible for laser alignment, we proceed with a detailed exposition of the underlying theory, focusing on aspects that have not been presented in the past. Application of the theory in several pedagogical illustrations is then followed by a review of the recent experimental and theoretical advances in the field. We conclude with a discussion of new directions, future opportunities, and areas where we expect intense laser alignment to play a role in the future. Throughout we emphasize the recent evolution of the method of nonadiabatic alignment from isolated diatomic molecules to complex media.

[1]  P. Corkum,et al.  Deflection of Neutral Molecules using the Nonresonant Dipole Force , 1997 .

[2]  M M Murnane,et al.  Phase-matching conditions for nonlinear frequency conversion by use of aligned molecular gases. , 2003, Optics letters.

[3]  Dudley R. Herschbach,et al.  Polarization of Molecules Induced by Intense Nonresonant Laser Fields , 1995 .

[4]  T. Seideman.  Time-resolved photoelectron angular distributions as a means of studying polyatomic nonadiabatic dynamics , 2000 .

[5]  Sang‐Hee Shim,et al.  Molecular lens applied to benzene and carbon disulfide molecular beams , 2001 .

[6]  T. Seideman,et al.  Photomanipulation of external molecular modes: A time-dependent self-consistent-field approach , 1999 .

[7]  Giovanni Granucci,et al.  Alignment of molecules in pulsed resonant laser fields. , 2004, The Journal of chemical physics.

[8]  Takayuki Suzuki,et al.  Controlling the orientation of polar molecules with combined electrostatic and pulsed, nonresonant laser fields. , 2003 .

[9]  T. Seideman.  On the dynamics of rotationally broad, spatially aligned wave packets , 2001 .

[10]  R. W. Robinett.  Quantum wave packet revivals , 2004 .

[11]  Kevin F. Lee,et al.  Direct imaging of rotational wave-packet dynamics of diatomic molecules , 2003 .

[12]  B. Friedrich.  Slowing of supersonically cooled atoms and molecules by time-varying nonresonant induced dipole forces , 2000 .

[13]  G. Herzberg,et al.  Molecular Spectra and Molecular Structure , 1992 .

[14]  R. Bemish,et al.  Photodissociation of molecules oriented by dc electric fields: Determining photofragment angular distributions , 1994 .

[15]  André D. Bandrauk,et al.  LASER-INDUCED ALIGNMENT DYNAMICS OF HCN : ROLES OF THE PERMANENT DIPOLE MOMENT AND THE POLARIZABILITY , 1999 .

[16]  O. Faucher,et al.  Orientation of polar molecules by laser induced adiabatic passage. , 2002, Physical review letters.

[17]  A. Matos-Abiague.  Sustainable orientation of polar molecules induced by half-cycle pulses (7 pages) , 2003 .

[18]  T. Seideman.  Rotational excitation and molecular alignment in intense laser fields , 1995 .

[19]  Y. Ohshima,et al.  Pendular-limit representation of energy levels and spectra of symmetric- and asymmetric-top molecules , 2004 .

[20]  R. Gilmore,et al.  Coherent states: Theory and some Applications , 1990 .

[21]  Friedrich,et al.  Alignment and trapping of molecules in intense laser fields. , 1995, Physical review letters.

[22]  G Gerber,et al.  Quantum control by ultrafast polarization shaping. , 2004, Physical review letters.

[23]  M. Machholm,et al.  Field-free orientation of molecules. , 2001, Physical review letters.

[24]  H. Loesch,et al.  Brute force in reactive scattering: steric effects in the reaction potassium + iodine chloride .fwdarw. potassium iodide + chlorine atom, potassium chloride + iodine atom at Etr = 3.03 eV , 1993 .

[25]  T. Kanai,et al.  Numerical simulations of molecular orientation using strong, nonresonant, two-color laser fields , 2001, Technical Digest. CLEO/Pacific Rim 2001. 4th Pacific Rim Conference on Lasers and Electro-Optics (Cat. No.01TH8557).

[26]  M Spanner,et al.  Forced molecular rotation in an optical centrifuge. , 2000, Physical review letters.

[27]  Fernando Pirani,et al.  Orienting and aligning molecules for stereochemistry and photodynamics. , 2005, Physical chemistry chemical physics : PCCP.

[28]  G. S. Ezra,et al.  Quantum monodromy for diatomic molecules in combined electrostatic and pulsed nonresonant laser fields , 2004 .

[29]  H. Rabitz,et al.  Enhanced molecular alignment by short laser pulses , 2004 .

[30]  T. Seideman,et al.  Nonadiabatic alignment of asymmetric top molecules: field-free alignment of iodobenzene. , 2003, Physical review letters.

[31]  P. Pershan,et al.  Theoretical Discussion of the Inverse Faraday Effect, Raman Scattering, and Related Phenomena , 1966 .

[32]  D. Herschbach,et al.  Spatial orientation of molecules in strong electric fields and evidence for pendular states , 1991, Nature.

[33]  T. Seideman,et al.  Nonadiabatic laser-induced alignment of iodobenzene molecules , 2004 .

[34]  N. Schwentner,et al.  A potential energy surface and a trajectory study of photodynamics and strong-field alignment of ClF molecule in rare gas (Ar,Kr) solids , 2004 .

[35]  Takayuki Suzuki,et al.  Observation of molecular orientation by the combination of electrostatic and nonresonant, pulsed laser fields , 2003 .

[36]  Adel Ben Haj Yedder,et al.  Evolutionary algorithms for the optimal laser control of molecular orientation , 2003 .

[37]  O. Faucher,et al.  Nonintrusive monitoring and quantitative analysis of strong laser-field-induced impulsive alignment , 2004 .

[38]  M. Murnane,et al.  Phase modulation of ultrashort light pulses using molecular rotational wave packets. , 2001, Physical review letters.

[39]  P. Schmelcher,et al.  Rovibrational spectra of diatomic molecules in strong electric fields: The adiabatic regime , 2004 .

[40]  D. Herschbach,et al.  Manipulating Molecules via Combined Static and Laser Fields , 1999 .

[41]  Henrik Stapelfeldt,et al.  Colloquium: Aligning molecules with strong laser pulses , 2003 .

[42]  H. Ohmura,et al.  Quantum control of molecular orientation by two-color laser fields. , 2004, The Journal of chemical physics.

[43]  Harmonic generation by molecules in intense laser and magnetic fields: Orientation effects , 2004 .

[44]  Hald,et al.  Three dimensional alignment of molecules using elliptically polarized laser fields , 2000, Physical review letters.

[45]  M. Janssen,et al.  Directional Dynamics in the Photodissociation of Oriented Molecules , 2004, Science.

[46]  P. Corkum,et al.  Disentangling molecular alignment and enhanced ionization in intense laser fields , 1999 .

[47]  H. Chung,et al.  Separation of a benzene and nitric oxide mixture by a molecule prism , 2003 .

[48]  T. Seideman.  The analysis of magnetic-state-selected angular distributions: A quantum mechanical form and an asymptotic approximation , 1996 .

[49]  T. Seideman.  New means of spatially manipulating molecules with light , 1999 .

[50]  B. Schmidt,et al.  Intense-field alignment of molecules confined in octahedral fields. , 2005, Physical review letters.

[51]  Michael Spanner,et al.  Coherent control of rotational wave-packet dynamics via fractional revivals. , 2004, Physical review letters.

[52]  André D. Bandrauk,et al.  Two-frequency IR laser orientation of polar molecules. Numerical simulations for HCN , 1999 .

[53]  O. Faucher,et al.  Controlling ground-state rotational dynamics of molecules by shaped femtosecond laser pulses , 2004 .

[54]  T. Seideman.  Time-resolved photoelectron angular distributions as a probe of coupled polyatomic dynamics , 2001 .

[55]  Kevin F. Lee,et al.  Two-pulse alignment of molecules , 2004 .

[56]  H. Loesch,et al.  Steric effects and vector correlations in reactions of K atoms with brute force oriented aromatic molecules , 1999 .

[57]  M. Castillejo,et al.  Role of orbital symmetry in high-order harmonic generation from aligned molecules , 2004 .

[58]  K. Miyazaki,et al.  Observation of Revival Structure in Femtosecond-Laser-Induced Alignment of N2 with High-Order Harmonic Generation , 2004 .

[59]  T. Seideman,et al.  Intense laser alignment in dissipative media as a route to solvent dynamics. , 2005, Physical review letters.

[60]  G Gerber,et al.  Femtosecond polarization pulse shaping. , 2001, Optics letters.

[61]  P Marquetand,et al.  Molecular orientation via a dynamically induced pulse-train: wave packet dynamics of NaI in a static electric field. , 2004, The Journal of chemical physics.

[62]  J. Levesque,et al.  Tomographic imaging of molecular orbitals , 2004, Nature.

[63]  V. Matylitsky,et al.  Rotational recurrences in thermal ensembles of nonrigid molecules , 2003 .

[64]  P. Corkum,et al.  OPTICAL DEFLECTION OF MOLECULES , 1998 .

[65]  P. Felker.  Rotational coherence spectroscopy: studies of the geometries of large gas-phase species by picosecond time-domain methods , 1992 .

[66]  H. Stapelfeldt,et al.  Controlling the Branching Ratio of Photodissociation Using Aligned Molecules , 1999 .

[67]  Takayuki Suzuki,et al.  Nontrivial polarization shaping of femtosecond pulses by reference to the results of dual-channel spectral interferometry. , 2004, Applied optics.

[68]  I. Averbukh,et al.  Semiclassical catastrophes and cumulative angular squeezing of a kicked quantum rotor , 2003, quant-ph/0306146.

[69]  O. Faucher,et al.  Postpulse molecular alignment measured by a weak field polarization technique. , 2003, Physical review letters.

[70]  M. Child.  Classical aspects of Raman excited rotational revivals , 2003 .

[71]  D. Sugny,et al.  Time-dependent unitary perturbation theory for intense laser-driven molecular orientation , 2004 .

[72]  M. Spanner,et al.  Switched wave packets: a route to nonperturbative quantum control. , 2003, Physical review letters.

[73]  S. Minemoto,et al.  Polarizability anisotropies of rare gas van der Waals dimers studied by laser-induced molecular alignment , 2003 .

[74]  H. Stapelfeldt,et al.  Observation of enhanced field-free molecular alignment by two laser pulses. , 2004, Physical review letters.

[75]  S. Wallentowitz,et al.  Quantum decoherence in the rotation of small molecules , 2004, quant-ph/0401158.

[76]  K. Hoki,et al.  Selective preparation of enantiomers from a racemate by laser pulses: model simulation for oriented atropisomers with coupled rotations and torsions , 2001 .

[77]  M. Castillejo,et al.  High-Order Harmonic Generation in Aligned Molecules , 2001 .

[78]  T. Seideman.  Time-resolved photoelectron angular distributions: concepts, applications, and directions. , 2002, Annual review of physical chemistry.

[79]  Kevin F. Lee,et al.  Phase control of rotational wave packets and quantum information. , 2004, Physical review letters.

[80]  T. Seideman.  Shaping molecular beams with intense light , 1997 .

[81]  Cho,et al.  Molecular lens of the nonresonant dipole force , 2000, Physical review letters.

[82]  B. Friedrich,et al.  Time-dependent alignment and orientation of molecules in combined electrostatic and pulsed nonresonant laser fields. , 2001, Physical review letters.

[83]  D. Sugny,et al.  Reaching optimally oriented molecular states by laser kicks (4 pages) , 2004 .

[84]  A. Pines,et al.  Two-dimensional NMR correlations of liquid crystals using switched angle spinning. , 2002, Journal of magnetic resonance.

[85]  Arne Keller,et al.  Orienting molecules using half-cycle pulses , 2001 .

[86]  T. Seideman.  MANIPULATING EXTERNAL DEGREES OF FREEDOM WITH INTENSE LIGHT : LASER FOCUSING AND TRAPPING OF MOLECULES , 1997 .

[87]  C. Riehn.  High-resolution pump probe rotational coherence spectroscopy rotational constants and structure of ground and electronically excited states of large molecular systems , 2002 .

[88]  Takayuki Suzuki,et al.  Orientation of polar molecules with combined electrostatic and pulsed, nonresonant laser fields , 2003, Physical review letters.

[89]  H. Loesch,et al.  Brute force in molecular reaction dynamics: A novel technique for measuring steric effects , 1990 .

[90]  T. Seideman.  Molecular optics in an intense laser field: A route to nanoscale material design , 1997 .

[91]  Paul B. Corkum,et al.  Optical Centrifuge for Molecules , 1999 .

[92]  J. Ohkubo,et al.  Molecular alignment in a liquid induced by a nonresonant laser field: Molecular dynamics simulation. , 2004, The Journal of chemical physics.

[93]  T. Seideman,et al.  Nanolithography using molecular optics , 2003 .

[94]  Miller Re,et al.  Spectroscopy of pendular states: The use of molecular complexes in achieving orientation. , 1992 .

[95]  T. Seideman,et al.  Nonadiabatic alignment of asymmetric top molecules: rotational revivals. , 2004, The Journal of chemical physics.

[96]  J. Berakdar,et al.  Controlling the orientation of polar molecules by half-cycle pulses , 2003 .

[97]  A. R. Edmonds.  Angular Momentum in Quantum Mechanics , 1957 .

[98]  M. Vrakking,et al.  Experimental observation of revival structures in picosecond laser-induced alignment of I2. , 2001, Physical review letters.

[99]  U. Buck,et al.  Photodissociation of oriented HXeI molecules in the gas phase , 2001 .

[100]  T. Seideman.  Revival Structure of Aligned Rotational Wave Packets , 1999 .

[101]  V. Matylitsky,et al.  Rotational coherence spectroscopy of jet-cooled molecules by femtosecond degenerate four-wave mixing: non-rigid symmetric and asymmetric tops , 2003 .