Field-free molecular orientation with terahertz few-cycle pulses.

We demonstrate theoretically an efficient field-free orientation in LiH and LiCl driven by available terahertz few-cycle pulses (TFCPs). Exact results by numerically solving the time-dependent Schrodinger equation including the vibrational and rotational degrees of freedom are compared to the rigid-rotor approximation (RRA) as well as to the impulsive approximation (IA), and the effect of rotational-vibrational coupling on the both RRA and IA is examined in detail. We find that the current available TFCPs may overcome the technical limitation of terahertz half-cycle pulse for enhancing the field-free molecular orientation.

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

[2]  D. DeMille,et al.  Preparation and detection of states with simultaneous spin alignment and selectable molecular orientation in PbO , 2008, 0807.4851.

[3]  P. Schmelcher,et al.  Impact of electric fields on highly excited rovibrational states of polar dimers , 2008, 0812.4297.

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

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

[6]  N. Henriksen Molecular alignment and orientation in short pulse laser fields , 1999 .

[7]  Wenhui Hu,et al.  Determination of the phase of terahertz few-cycle laser pulses. , 2009, Optics letters.

[8]  H. Hasegawa,et al.  Decoding the state distribution in a nonadiabatic rotational excitation by a nonresonant intense laser field , 2006 .

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

[10]  G. Meijer,et al.  Laser-induced alignment and orientation of quantum-state-selected large molecules. , 2008, Physical review letters.

[11]  Alec M. Wodtke,et al.  The Stereodynamics of a Gas-Surface Reaction , 1997 .

[12]  U. Buck,et al.  The pseudo-first-order stark effect and the orientation of HXeI molecules , 2003 .

[13]  T. Seideman,et al.  Nonadiabatic Alignment by Intense Pulses. Concepts, Theory, and Directions , 2005 .

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

[15]  S. Langhoff,et al.  Theoretical treatment of the X 1Σ+, A 1Σ+, and B 1Π states of LiH , 1981 .

[16]  Alfred Leitenstorfer,et al.  Phase-locked generation and field-resolved detection of widely tunable terahertz pulses with amplitudes exceeding 100 MV/cm. , 2008, Optics letters.

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

[18]  Zhi‐zhan Xu,et al.  Carrier-envelope phase-dependent transmitted spectra in inversion-asymmetric media with permanent dipole moments , 2009 .

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

[20]  Dominique Sugny,et al.  Field-free molecular orientation by nonresonant and quasiresonant two-color laser pulses , 2008 .

[21]  Chuan-Cun Shu,et al.  Carrier-envelope phase-dependent field-free molecular orientation , 2009 .

[22]  H. Zeng,et al.  Field-free molecular orientation control by two ultrashort dual-color laser pulses , 2010 .

[23]  Laser-assisted control of molecular orientation at high temperatures , 2008 .

[24]  Julien Salomon,et al.  Optimal molecular alignment and orientation through rotational ladder climbing. , 2005, The Journal of chemical physics.

[25]  S. Minemoto,et al.  Field-free molecular orientation by an intense nonresonant two-color laser field with a slow turn on and rapid turn off , 2009 .

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

[27]  W. Heisenberg,et al.  Zur Quantentheorie der Molekeln , 1924 .

[28]  Maxim Sukharev,et al.  Laser field alignment of organic molecules on semiconductor surfaces: toward ultrafast molecular switches. , 2008, Physical review letters.

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

[30]  Hirofumi Sakai,et al.  All-optical molecular orientation. , 2010, Physical review letters.

[31]  L. Serrano-Andrés,et al.  Quantum simulations of toroidal electric ring currents and magnetic fields in linear molecules induced by circularly polarized laser pulses , 2008 .

[32]  M. Vrakking,et al.  Coherent control of molecular orientation , 1997 .

[33]  H. Milchberg,et al.  Single-shot, space- and time-resolved measurement of rotational wavepacket revivals in H(2), D(2), N(2), O(2), and N(2)O. , 2007, Optics express.

[34]  Yasuhiro Ohshima,et al.  Quantum state reconstruction of a rotational wave packet created by a nonresonant intense femtosecond laser field. , 2008, Physical review letters.

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

[36]  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).

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

[38]  I. Averbukh,et al.  Angular focusing, squeezing, and rainbow formation in a strongly driven quantum rotor. , 2001, Physical review letters.

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

[40]  P. Schmelcher,et al.  Electric-field-induced adiabaticity in the rovibrational motion of heteronuclear diatomic molecules , 2005 .

[41]  X. Yi,et al.  Born-Oppenheimer approximation in open systems , 2009, 0905.2741.

[42]  Wenhui Hu,et al.  Enhancement of molecular field-free orientation by utilizing rovibrational excitation , 2009 .

[43]  Hongbing Jiang,et al.  Controlling molecular rotational population by wave-packet interference. , 2009, The Journal of chemical physics.

[44]  T. Kanai,et al.  Quantum interference during high-order harmonic generation from aligned molecules , 2005, Nature.

[45]  M. Vrakking,et al.  Impulsive orientation and alignment of quantum-state-selected NO molecules , 2009 .

[46]  H. Harde,et al.  Coherent transients excited by subpicosecond pulses of terahertz radiation , 1991 .

[47]  S. Minemoto,et al.  Laser-field-free molecular orientation. , 2008, Physical review letters.

[48]  M. Tachiya,et al.  Selective ionization of oriented nonpolar molecules with asymmetric structure by phase-controlled two-color laser fields. , 2006, Physical review letters.

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

[50]  S. Chu,et al.  Multielectron effects on the orientation dependence and photoelectron angular distribution of multiphoton ionization of CO 2 in strong laser fields , 2009 .

[51]  Wenhui Hu,et al.  Stimulated Raman adiabatic passage in molecular electronic states , 2009 .

[52]  I. Bocharova,et al.  Field-free orientation of CO molecules by femtosecond two-color laser fields. , 2009, Physical review letters.

[53]  Yongwei Zhang,et al.  Controlling rotational state distributions using two-pulse stimulated Raman excitation , 2007 .

[54]  Michael Spanner,et al.  Quantum logic approach to wave packet control. , 2003, Physical review letters.

[55]  Zhi‐zhan Xu,et al.  Carrier-envelope phase dependence of few-cycle ultrashort laser pulse propagation in a polar molecule medium. , 2007, Physical review letters.

[56]  L. Serrano-Andrés,et al.  Nonadiabatic orientation, toroidal current, and induced magnetic field in BeO molecules. , 2008, The Journal of chemical physics.

[57]  Raffaele Velotta,et al.  Probing orbital structure of polyatomic molecules by high-order harmonic generation. , 2007 .