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Register a new userDisentangling the role of laser coupling in directional breaking of molecules
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The directional control of molecular dissociation with the laser electric field waveform is a paradigm and was demonstrated for a variety of molecules. In most cases, the directional control occurs via a dissociative ionization pathway. The role of laser-induced coupling of electronic states in the dissociating ion versus selective ionization of oriented neutral molecules, however, could not be distinguished for even small heteronuclear molecules such as CO. Here, we introduce a technique, using elliptically polarized pump and linearly polarized two-color probe pulses that unambiguously distinguishes the roles of laser-induced state coupling and selective ionization. The measured photoelectron momentum distributions governed by the light polarizations allow us to coincidently identify the ionization and dissociation from the pump and probe pulses. Directional dissociation of CO+ as a function of the relative phase of the linearly polarized two-color pulse is observed for both parallel and orthogonally oriented molecules. We find that the laser-induced coupling of various electronic states of CO+ plays an important role for the observed directional bond breaking, which is verified by quantum calculations.
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Gauge invariance was discovered in the development of classical electromagnetism and was required when the latter was formulated in terms of the scalar and vector potentials. It is now considered to be a fundamental principle of nature, stating that different forms of these potentials yield the same physical description: they describe the same electromagnetic field as long as they are related to each other by gauge transformations. Gauge invariance can also be included into the quantum description of matter interacting with an electromagnetic field by assuming that the wave function transforms under a given local unitary transformation. The result of this procedure is a quantum theory describing the coupling of electrons, nuclei and photons. Therefore, it is a very important concept: it is used in almost every fields of physics and it has been generalized to describe electroweak and strong interactions in the standard model of particles. A review of quantum mechanical gauge invariance and general unitary transformations is presented for atoms and molecules in interaction with intense short laser pulses, spanning the perturbative to highly nonlinear nonperturbative interaction regimes. Various unitary transformations for single spinless particle Time Dependent Schrodinger Equations, TDSE, are shown to correspond to different time-dependent Hamiltonians and wave functions. Accuracy of approximation methods involved in solutions of TDSEs such as perturbation theory and popular numerical methods depend on gauge or representation choices which can be more convenient due to faster convergence criteria. We focus on three main representations: length and velocity gauges, in addition to the acceleration form which is not a gauge, to describe perturbative and nonperturbative radiative interactions. Numerical schemes for solving TDSEs in different representations are also discussed.
We present an analysis of two experimental approaches to controlling the directionality of molecular rotation with ultrashort laser pulses. The two methods are based on the molecular interaction with either a pair of pulses (a double kick scheme) or a longer pulse sequence (a chiral pulse train scheme). In both cases, rotational control is achieved by varying the polarization of and the time delay between the consecutive laser pulses. Using the technique of polarization sensitive resonance-enhanced multi-photon ionization, we show that both methods produce significant rotational directionality. We demonstrate that increasing the number of excitation pulses supplements the ability to control the sense of molecular rotation with quantum state selectivity, i.e. predominant excitation of a single rotational state. We also demonstrate the ability of both techniques to generate counter-rotation of molecular nuclear spin isomers (here, ortho- and para-nitrogen) and molecular isotopologues (here, 14N_2 and 15N_2).
We establish a generalized picture of the phase-sensitivity of laser-induced directional bond-breaking using the H$_2$ molecule as the example. We show that the well-known proton ejection anisotropy measured with few-cycle pulses arises as an amplitude-modulation of an intrinsic anisotropy that is sensitive to the laser phase at the ionization time and determined by the molecules electronic structure. Our work furthermore reveals a strong electron-proton correlation that may open up a new approach to experimentally accessing the laser-sub-cycle intramolecular electron dynamics also in large molecules.
We report a phenomenon of self-sweeping in a bi-directional ring thulium-doped fiber laser, for the first time. The laser is spontaneously sweeping in both directions at a rate up to 0.2 nm/s with 15 nm sweeping range in 1.95 {mu}m wavelength region. The laser output is switchable between two different working modes: periodical spontaneous laser line sweeping with generation of microsecond pulses in time domain; or static central wavelength with amplitude modulated temporally.
Enhancement cavities where a beam of large size (several millimeters) can resonate have several applications, in particular in atomic physics. However, reaching large beam waists in a compact geometry (less than a meter long) typically brings the resonator close to the degeneracy limit. Here we experimentally study a degenerate optical cavity, 44-cm long and consisting of two flat mirrors placed in the focal planes of a lens, in a regime of intermediate finesse ($sim 150$). We study the impact of the longitudinal misalignement on the optical gain, for different input beam waists up to 5.6~mm, and find data consistent with the prediction of a model based on ABCD propagation of Gaussian beams. We reach an optical gain of 26 for a waist of 1.4~mm, which can have an impact on several applications, in particular atom interferometry. We numerically investigate the optical gain reduction for large beam waists using the angular spectrum method to consider the effects of optical aberrations, which play an important role in such a degenerate cavity. Our calculations quantitatively reproduce the experimental data and will provide a key tool for designing enhancement cavities close to the degeneracy limit. As an illustration, we discuss the application of this resonator geometry to the enhancement of laser beams with top-hat intensity profiles.
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