Searcharxiv⌕ Search

arXiv subjects

Johannes Floß

Publications and source records attributed to Johannes Floß.

12 recordsLinked to original sources

Observation of persistent orientation of chiral molecules by laser field with twisted polarization

Molecular chirality is an omnipresent phenomenon of fundamental significance in physics, chemistry and biology. For this reason, search for novel techniques for enantioselective control, detection and separation of chiral molecules is of particular importance. It has been recently predicted that laser fields with twisted polarization may induce persistent enantioselective field-free orientation of chiral molecules. Here we report the first experimental observation of this phenomenon using propylene oxide molecules ($\mathrm{CH_{3}CHCH_{2}O}$, or PPO) spun by an optical centrifuge - a laser pulse, whose linear polarization undergoes an accelerated rotation around its propagation direction. We show that PPO molecules remain oriented on a time scale exceeding the duration of the centrifuge pulse by several orders of magnitude. The demonstrated long-time field-free enantioselective orientation opens new avenues for optical manipulation, discrimination, and, potentially, separation of molecular enantiomers.

physics.chem-ph↗

Laser induced persistent orientation of chiral molecules

We show, both classically and quantum mechanically, enantioselective orientation of gas phase chiral molecules excited by laser fields with twisted polarization. Counterintuitively, the induced orientation, whose direction is laser controllable, does not disappear after the excitation, but stays approximately constant long after the end of the laser pulses, behavior unique to chiral systems. We computationally demonstrate this long-lasting orientation using propylene oxide molecules (${\rm CH_{3}CHCH_{2}O}$, or PPO) as an example, and consider two kinds of fields with twisted polarization: a pair of delayed cross-polarized pulses, and an optical centrifuge. This novel chiral effect opens new avenues for detecting molecular chirality, measuring enantiomeric excess and separating enantiomers with the help of inhomogeneous external fields.

physics.chem-ph↗

Coherent Control of Penning and Associative Ionization: Insights from Symmetries

Coherent control of reactive atomic and molecular collision processes remains elusive experimentally due to quantum interference-based requirements. Here, with insights from symmetry conditions, a viable method for controlling Penning and Associative ionization in atomic collisions is proposed. Computational applications to He$^*({}^3\text{S})$-Li(${^2\text{S}}$) and Ne$^*{}(^3\text{P}_2$)-Ar($^1\text{S}_0$) show extensive control over the ionization processes under experimentally feasible conditions.

quant-ph↗

Dimensionality and integrals of motion of the Trappist-1 planetary system

The number of isolating integrals of motion of the Trappist-1 system - a late M-dwarf orbited by seven Earth-sized planets - was determined numerically, using an adapted version of the correlation dimension method. It was found that over the investigated time-scales of up to 20 000 years the number of isolating integrals of motion is the same as one would find for a system of seven non-interacting planets - despite the fact that the planets in the Trappist-1 system are strongly interacting. Considering perturbed versions of the Trappist-1 system shows that the system may occupy an atypical part of phase-space with high stability. These findings are consistent with earlier studies.

astro-ph.EP↗

Laser-induced molecular alignment in the presence of chaotic rotational dynamics

Coherent control of chaotic molecular systems, using laser-assisted alignment of sulphur dioxide (SO$_2$) molecules in the presence of a static electric field as an example, is considered. Conditions for which the classical version of this system is chaotic are established, and the quantum and classical analogs are shown to be in very good correspondence. It is found that the chaos present in the classical system does not impede the alignment, neither in the classical nor the quantum system. Using the results of numerical calculations, we suggest that laser-assisted alignment is stable against rotational chaos for all asymmetric top molecules.

physics.chem-ph↗

Edge states of periodically kicked quantum rotors

We present a quantum localization phenomenon that exists in periodically kicked 3D rotors, but is absent in the commonly studied 2D ones: edge localization. We show that under the condition of a fractional quantum resonance there are states of the kicked rotor that are strongly localized near the edge of the angular momentum space at $J=0$. These states are analogs of surface states in crystalline solids, and they significantly affect resonant excitation of molecular rotation by laser pulse trains.

quant-ph↗

Observation of Bloch oscillations in molecular rotation

The periodically kicked quantum rotor is known for non-classical effects such as quantum localisation in angular momentum space or quantum resonances in rotational excitation. These phenomena have been studied in diverse systems mimicking the kicked rotor, such as cold atoms in optical lattices, or coupled photonic structures. Recently, it was predicted that several solid state quantum localisation phenomena - Anderson localisation, Bloch oscillations, and Tamm-Shockley surface states - may manifest themselves in the rotational dynamics of laser-kicked molecules. Here, we report the first observation of rotational Bloch oscillations in a gas of nitrogen molecules kicked by a periodic train of femtosecond laser pulses. A controllable detuning from the quantum resonance creates an effective accelerating potential in angular momentum space, inducing Bloch-like oscillations of the rotational excitation. These oscillations are measured via the temporal modulation of the refractive index of the gas. Our results introduce room-temperature laser-kicked molecules as a new laboratory for studies of localisation phenomena in quantum transport.

quant-ph↗

A theoretical study of the dynamics of paramagnetic superrotors in external magnetic fields

We present a detailed theoretical study of oxygen molecules in high rotational states (molecular superrotors) interacting with an external magnetic field. The system shows rich dynamics, ranging from a spin-selective splitting of the angular distribution over molecular alignment to an inversion of the rotational direction. We find that the observed magneto-rotational effects are due to a spin-mediated precession of the orbital angular momentum around the magnetic field. Analytical expressions for the precession frequency in the limits of weak and strong magnetic fields are derived and used to support the proposed mechanism. In addition, we provide the procedure for a numerical treatment of oxygen superrotors in an external magnetic field.

physics.chem-ph↗

Anderson wall and Bloch oscillations in molecular rotation

We describe a universal behavior of linear molecules excited by a periodic train of short laser pulses under quantum resonance conditions. In a rigid rotor the resonance causes an unlimited ballistic growth of the angular momentum. We show that the centrifugal distortion of rotating molecules eventually halts the growth, by causing Anderson localization beyond a critical value of the angular momentum -- the Anderson wall. Its position solely depends on the molecular rotational constants and lies in the range of a few tens of hbar. Below the wall, rotational excitation oscillates with the number of pulses due to a mechanism similar to Bloch oscillations in crystalline solids. We suggest optical experiments capable of observing the rotational Anderson wall and Bloch oscillations at near-ambient conditions with the help of existing laser technology.

quant-ph↗

Anderson localisation in laser kicked molecules

The paper explores the prospects of observing the phenomenon of dynamical Anderson localisation via non-resonant Raman-type rotational excitation of molecules by periodic trains of short laser pulses. We define conditions for such an experiment, and show that current femtosecond technology used for non-adiabatic laser alignment of linear molecules is sufficient for this task. Several observables which can serve as indicator for Anderson localisation are suggested for measurement, and the influence of experimental limitations imposed by laser intensity noise, finite pulse duration, limited number of pulses in a train, and thermal effects is analysed.

quant-ph↗

Molecular spinning by a chiral train of short laser pulses

We provide a detailed theoretical analysis of molecular rotational excitation by a chiral pulse train -- a sequence of linearly polarised pulses with the polarisation direction rotating from pulse to pulse by a controllable angle. Molecular rotation with a preferential rotational sense (clockwise or counter-clockwise) can be excited by this scheme. We show that the directionality of the rotation is caused by quantum interference of different excitation pathways. The chiral pulse train is capable of selective excitation of molecular isotopologues and nuclear spin isomers in a mixture. We demonstrate this using 14N2 and 15N2 as examples for isotopologues, and para- and ortho-nitrogen as examples for nuclear spin isomers.

quant-ph↗

Quantum resonance, Anderson localisation and selective manipulations in molecular mixtures by ultrashort laser pulses

We demonstrate that the current laser technology used for field-free molecular alignment via a cascade of Raman rotational transitions allows for observing long-discussed non-linear quantum phenomena in the dynamics of the periodically kicked rotor. This includes the scaling of the absorbed energy near the conditions of quantum resonance and Anderson-like localisation in the angular momentum. Based on these findings, we suggest a novel approach to tunable selective rotational excitation and alignment in a molecular mixture, using trains of short laser pulses. We demonstrate the efficiency of this approach by applying it to a mixture of two nitrogen isotopologues (14N2 and 15N2), and show that strong selectivity is possible even at room temperature.

quant-ph↗