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Excited-state vibrational dynamics in molecules can be studied by an electronically off-resonant Raman process induced by a probe pulse with variable delay with respect to an actinic pulse. We establish the connection between several…

Chemical Physics · Physics 2013-09-27 Konstantin E. Dorfman , Benjamin P. Fingerhut , Shaul Mukamel

We propose a method for achieving highly efficient transfer between the vibrational states in a diatomic molecule. The process is mediated by strong laser pulses and can be understood in terms of light-induced potentials. In addition to…

Quantum Physics · Physics 2009-11-06 M. Rodriguez , K. -A. Suominen , B. M. Garraway

We report on the excitation of single molecules via narrow zero-phonon transitions using short laser pulses. By monitoring the Stokes-shifted fluorescence, we studied the excited state population as a function of the delay time, laser…

Quantum Physics · Physics 2009-01-30 Ilja Gerhardt , Gert Wrigge , Gert Zumofen , Jaesuk Hwang , Alois Renn , Vahid Sandoghdar

Ultrafast lasers ($< 500$ fs) have enabled laser-matter interactions at intensities exceeding $10^{18} \rm{Wcm}^{-2}$ with only millijoules of laser energy. However, as pulse durations become shorter, larger spectral bandwidths are…

Laser cooling of large, complex molecules is a long-standing goal, instrumental for enabling new quantum technology and precision measurements. A primary consideration for the feasibility of laser cooling, which determines the efficiency…

We consider the use of pulse-shaped broadband femtosecond lasers to optically cool rotational and vibrational degrees of freedom of molecules. Since this approach relies on cooling rotational and vibrational quanta by exciting an electronic…

Atomic Physics · Physics 2017-09-13 Chien-Yu Lien , Scott R. Williams , Brian Odom

A coherent control scheme for the population distribution in the vibrational states of nonpolar molecules is proposed. Our theoretical analysis and results of numerical simulations for the interaction of the hydrogen molecular ion in its…

Quantum Physics · Physics 2011-02-17 A. Picón , J. Biegert , A. Jaron-Becker , A. Becker

Atomic excitation to excited states in strong laser field is the key to high-order harmonic generation below ionization threshold, yet remains unclear mainly due to the lack of proper detection methods. We propose a frequency-resolved…

Atomic Physics · Physics 2018-12-17 Long Xu , Hui Dong , Libin Fu

Laser cooling and trapping of atoms and atomic ions has led to numerous advances including the observation of exotic phases of matter, development of exquisite sensors and state-of-the-art atomic clocks. The same level of control in…

Determining the vibrational structure of a molecule is central to fundamental applications in several areas, from atmospheric science to catalysis, fuel combustion modeling, biochemical imaging, and astrochemistry. However, when significant…

Quantum Physics · Physics 2021-12-22 Nicolas P. D. Sawaya , Francesco Paesani , Daniel P. Tabor

We investigate the prospects of creating broad rotational wave packets by means of molecular interaction with long sequences of intense femtosecond pulses. Using state-resolved rotational Raman spectroscopy of oxygen, subject to a sequence…

Quantum Physics · Physics 2016-01-27 M. Bitter , V. Milner

We propose a scheme to generate superpositions of coherent states for the vibrational motion of a laser cooled trapped-ion. It is based on the interaction with a standing wave making use of the counter-rotating terms, i.e. not applying the…

Quantum Physics · Physics 2013-03-13 S. Mancini , H. Moya-Cessa , P. Tombesi

We investigate the dynamics of molecular photoexcitation by unchirped femtosecond laser pulses using RbCs as a model system. This study is motivated by a goal of optimizing a two-color scheme of transferring vibrationally-excited ultracold…

Atomic Physics · Physics 2015-06-04 B. E. Londono , A. Derevianko , J. E. Mahecha , A. Crubellier , E. Luc-Koenig

Analytical formulas for the excitation energies as well as for the electric quadrupole reduced transition probabilities in the ground, beta and gamma bands were derived within the coherent state model for the near vibrational and well…

Nuclear Theory · Physics 2015-05-30 A. A. Raduta , R. Budaca , Amand Faessler

The possibility of achieving highly selective excitation of low metastable states of hydrogen and helium atoms by using short laser pulses with reasonable parameters is demonstrated theoretically. Interactions of atoms with the laser field…

Atomic Physics · Physics 2007-05-23 A. D. Kondorskiy , L. P. Presnyakov , Yu. Ralchenko

Vibrational-excitation cross sections of ground electronic state of carbon dioxide molecule by electron-impact through the CO2-(2\Pi) shape resonance is considered in the separation of the normal modes approximation. Resonance curves and…

Chemical Physics · Physics 2016-11-01 V. Laporta , J. Tennyson , R. Celiberto

Understanding and controlling the electronic as well as ro-vibrational motion and, thus, the entire chemical dynamics in molecules is the ultimate goal of ultrafast laser and imaging science. In photochemistry, laser-induced dissociation…

This paper describes a method to do ab initio molecular dynamics in electronically excited systems within the random phase approximation (RPA). Using a dynamical variational treatment of the RPA frequency, which corresponds to the…

Condensed Matter · Physics 2009-10-31 Eric R. Bittner , D. S. Kosov

A recombination reaction model for high-temperature chemical kinetics is derived from ab initio simulations data. A kinetic recombination rate model is derived using a recently developed ab initio state-specific dissociation model and the…

Chemical Physics · Physics 2020-09-15 Narendra Singh , Thomas Schwartzentruber

A method is proposed for preparing any pure and a wide class of mixed quantum states in the decoherence-free ground-state subspace of a degenerate multilevel lambda system. The scheme is a combination of optical pumping and a series of…

Quantum Physics · Physics 2009-11-10 Attila Karpati , Zsolt Kis , Peter Adam