Development of ultrahigh-precision coherent control and its applications

Abstract

Coherent control is based on optical manipulation of the amplitudes and phases of wave functions. It is expected to be a key technique to develop novel quantum technologies such as bond-selective chemistry and quantum computing, and to better understand the quantum worldview founded on wave-particle duality. We have developed high-precision coherent control by imprinting optical amplitudes and phases of ultrashort laser pulses on the quantum amplitudes and phases of molecular wave functions. The history and perspective of coherent control and our recent achievements are described.

Numerical Tests of a Fixed Vibrational Basis/Gaussian Bath Theory for Small Molecule Dynamics in Low-Temperature Media

“…The behavior of small molecules in low-temperature solid crystals, including electronic and vibrational dynamics − as well as chemical reactions, − is affected in fundamental ways by interactions with the environment; these interactions can also generate coherent nonequilibrium environmental states that are not swamped by thermal agitation. , Electronic and vibrational excitation-induced dynamics in systems of this kind are being studied by myriad time-resolved nonlinear optical techniques. An interpretation of the resultant spectroscopic signals in terms of the underlying quantum mechanical motion is of keen interest in its own right, for the possible demonstration of coherent control, − and for potential quantum-information applications. In addition, several key features of small-molecule chromophores embedded in cryogenic noble gas hosts may enable their comprehensive simulation with computationally efficient first-principles approaches that provide a rigorous quantum mechanical description of a small number of directly excited intramolecular degrees of freedom along with a well-defined, albeit approximate, treatment of the indirectly triggered semiclassical dynamics of the surrounding medium.…”