Related papers: Orientation Dynamics of Asymmetric Rotors Using Ra…
We experimentally study the optical- and terahertz- induced rotational dynamics of asymmetric molecules in the gas phase. Terahertz and optical fields are identified as two distinct control handles over asymmetric molecules, as they couple…
Intense single-cycle THz pulses resonantly interacting with molecular rotations are shown to induce significant field-free orientation under ambient conditions. We calculate and measure the angular distribution associated with THz-driven…
Significant molecular orientation can be achieved by time-symmetric single-cycle pulses of zero area, in the THz region. We show that in spite of the existence of a combined time-space symmetry operation, not only large peak instantaneous…
Ultrafast two-dimensional spectroscopy utilizes correlated multiple light-matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum. Its extension to the terahertz regime of the…
We show clear experimental evidence of co-operative terahertz (THz) dynamics observed below 3 THz (~100 cm-1), for a low-symmetry Zr-based metal-organic framework (MOF) structure, termed MIL-140A [ZrO(O2C-C6H4-CO2)]. Utilizing a combination…
We investigate the persistent orientation of asymmetric-top molecules induced by time-delayed THz pulses that are either collinearly or cross polarized. Our theoretical and numerical results demonstrate that the orthogonal configuration…
We present a combined analytical and numerical investigation to show how an optimal control field can be designed to generate maximum field-free orientation of molecules for three populated rotational states. Based on a model involving pure…
Control of molecular rotations by laser fields is an active area of research focusing on the alignment/orientation of otherwise isotropic molecular samples. Oriented molecules are useful in many applications, such as molecular orbital…
A new and efficient method for orientation echo spectroscopy is presented and realized experimentally. The excitation scheme utilizes concerted rotational excitations by both ultrashort terahertz and near-IR pulses and its all-optical…
We propose and computationally study a method for simultaneously orienting the angular momentum of asymmetric top molecules along: 1) a laboratory-fixed direction; 2) the molecular intermediate moment of inertia axis; 3) the laser field…
The control of ultrafast molecular rotational motion has benefited from the development of innovative techniques in strong-field laser physics. Here, we theoretically demonstrate a novel type of coherent control by inducing rotation of an…
We present a theoretical study of the shaping of the time-evolution of field-free orientation of linear molecules. We show the extend to which the degree of orientation can be steered along a desired periodic time-dependent signal. The…
We present a theoretical study of the impact of an electrostatic field combined with nonresonant linearly polarized laser pulses on the rotational dynamics of a thermal ensemble of linear molecules. We solve the time-dependent Schr\"odinger…
The decay of field-free rotational dynamics is experimentally studied in two complementary methods: laser-induced molecular alignment and terahertz-field-induced molecular orientation. Comparison between the decay rates of different…
An important goal in molecular physics and chemistry today is to obtain structure-dependent information about molecular function to obtain a deeper understanding into chemical reactions. However, until now, asymmetric tops, which comprise…
We investigate to which extend a THz laser pulse can be used to produce field-free molecular orientation at high temperature. We consider laser pulses that can be implemented with the state of the art technology and we show that the…
Because of their central importance in chemistry and biology, water molecules have been the subject of decades of intense spectroscopic investigations. Rotational spectroscopy of water vapor has yielded detailed information about the…
High energy single- to few-cycle terahertz pulses enable the exploration of the frontier of science, such as electron acceleration, strong-field physics, and spectroscopy. One important method of generating such terahertz pulses is to use…
We computationally demonstrate a new method for coherently controlling the rotation-axis direction in asymmetric top molecules with an optical centrifuge. Appropriately chosen electric-field strengths and the centrifuge's acceleration rate…
We present a computational study of the rotational molecular dynamics of bromotrifluoromethane (CF3Br) molecules in gas phase. The rotation is manipulated with an offresonant, 800nm laser. The molecules are treated as rigid rotors.…