arXiv subjects

Lanhai He

Publications and source records attributed to Lanhai He.

10 recordsLinked to original sources

arXiv2024

A versatile and transportable endstation for controlled molecule experiments

We report on a new versatile transportable endstation for controlled molecule (eCOMO) experiments providing a combination of molecular beam purification by electrostatic deflection and simultaneous ion and electron detection using velocity-map imaging (VMI). The $b$-type electrostatic deflector provides spatial dispersion of species based on their effective-dipole-moment-to-mass ratio. This enables selective investigation of molecular rotational quantum states, conformers, and molecular clusters. Furthermore, the double-sided VMI spectrometer equipped with two high-temporal-resolution event-driven Timepix3 cameras provides detection of all generated ions independently of their mass-over-charge ratio and electrons. To demonstrate the potential of this novel apparatus, we present experimental results from our investigation of carbonyl sulfide (OCS) after ionization. Specifically, we provide the characterization of the molecular beam, electrostatic deflector, and electron- and ion-VMI spectrometer. The eCOMO endstation delivers a platform for ultrafast dynamics studies using a wide range of light sources from table-top lasers to free-electron-laser and synchrotron-radiation facilities. This makes it suitable for research activities spanning from atomic, molecular, and cluster physics, over energy science and chemistry, to structural biology.

physics.chem-ph↗

arXiv2024

Specific versus Nonspecific Solvent Interactions of a Biomolecule in Water

Solvent interactions, particularly hydration, are vital in chemical and biochemical systems. Model systems unveil microscopic details of such interactions. We uncover a specific hydrogen-bonding motif of the biomolecular building block indole (C$_8$H$_7$N), tryptophan's chromophore, in water: a strong localized $\text{N-H}\cdots\text{OH}_2$ hydrogen bond, alongside unstructured solvent interactions. This insight is revealed from a combined experimental and theoretical analysis of indole's electronic structure in aqueous solution. We have recorded the complete X-ray photoemission and Auger spectrum of aqueous-phase indole, quantitatively explaining all peaks through \emph{ab initio} modeling. The efficient and accurate technique for modeling valence and core photoemission spectra involves the maximum-overlap method and the non-equilibrium polarizable-continuum model. A two-hole electron-population analysis quantitatively describes the Auger spectra. Core-electron binding energies for nitrogen and carbon highlight the specific interaction with a hydrogen-bonded water molecule at the N-H group and otherwise nonspecific solvent interactions.

physics.chem-ph↗

arXiv2024

Controlled molecule injector for cold, dense, and pure molecular beams at the European x-ray free-electron laser

A permanently available molecular-beam injection setup for controlled molecules (COMO) was installed and commissioned at the small quantum systems (SQS) instrument at the European x-ray free-electron laser (EuXFEL). A $b$-type electrostatic deflector allows for pure state-, size-, and isomer-selected samples of polar molecules and clusters. The source provides a rotationally cold ($T\approx1$~K) and dense ($ρ\approx10^8$~cm$^{-3}$) molecular beam with pulse durations up to 100~\us generated by a new version of the Even-Lavie valve. Here, a performance overview of the COMO setup is presented along with characterization experiments performed both, with an optical laser at the Center for Free-Electron-Laser Science and with x-rays at EuXFEL under burst-mode operation. COMO was designed to be attached to different instruments at the EuXFEL, in particular at the small quantum systems (SQS) and single particles, clusters, and biomolecules (SPB) instruments. This advanced controlled-molecules injection setup enables XFEL studies using highly defined samples with soft and hard x-ray FEL radiation for applications ranging from atomic, molecular, and cluster physics to elementary processes in chemistry and biology.

physics.chem-ph↗

arXiv2024

Water is a radiation protection agent for ionised pyrrole

Radiation-induced damage of biological matter is an ubiquitous problem in nature. The influence of the hydration environment is widely discussed, but its exact role remains elusive. Utilising well defined solvated-molecule aggregates, we experimentally observed a hydrogen-bonded water molecule acting as a radiation protection agent for ionised pyrrole, a prototypical aromatic biomolecule. Pure samples of pyrrole and pyrrole(H$_2$O) were outer-valence ionised and the subsequent damage and relaxation processes were studied. Bare pyrrole ions fragmented through the breaking of C-C or N-C covalent bonds. However, for pyrrole(H$_2$O)$^+$, we observed a strong protection of the pyrrole ring through the dissociative release of neutral water or by transferring an electron or proton across the hydrogen bond. Overall, a single water molecule strongly reduces the fragmentation probability and thus the persistent radiation damage of singly-ionised pyrrole.

physics.chem-ph↗

arXiv2022

The Kinetic Energy of PAH Dication and Trication Dissociation Determined by Recoil-Frame Covariance Map Imaging

We investigated the dissociation of dications and trications of three polycyclic aromatic hydrocarbons (PAHs), fluorene, phenanthrene, and pyrene. PAHs are a family of molecules ubiquitous in space and involved in much of the chemistry of the interstellar medium. In our experiments, ions are formed by interaction with 30.3 nm extreme ultraviolet (XUV) photons, and their velocity map images are recorded using a PImMS2 multi-mass imaging sensor. Application of recoil-frame covariance analysis allows the total kinetic energy release (TKER) associated with multiple fragmentation channels to be determined to high precision, ranging 1.94-2.60 eV and 2.95-5.29 eV for the dications and trications, respectively. Experimental measurements are supported by Born-Oppenheimer molecular dynamics (BOMD) simulations.

physics.chem-ph↗

arXiv2021

New source for tuning the effective Rabi frequency discovered in multiphoton ionization

The Autler-Townes effect due to near resonance transition between 4s-4p states in potassium atoms is mapped out in the photo-electron-momentum distribution and manifests itself as a splitting in the photo-electron kinetic energy spectra. The energy splitting fits well with the calculated Rabi frequency at low laser intensities and shows clear deviation at laser intensities above 1.5x10^11 W/cm^2. An effective Rabi frequency formulae including the ionization process explains the observed results. Our results reveal the possibility to tune the effective coupling strength with the cost of the number of level-populations.

physics.atom-ph↗

arXiv2021

Single-shot MHz velocity-map-imaging using two Timepix3 cameras

We demonstrate the application of event-driven Timepix3-based detectors in combination with a double-sided velocity-map-imaging spectrometer to record the full 3D momentum of charged particles at the free-electron-laser facility FLASH. We measured the XUV induced fragmentation of $\text{N}_2$ using 250 kHz FLASH bursts with sub-pixel spatial resolution and up to 1.7~ns temporal resolution for photoelectrons. To further demonstrate the capabilities of this camera at even higher repetition rates we measured single-shot images of He($1s$) photoelectrons for bursts with a repetition rate of 1 MHz. Overall, with the Timepix3 camera we overcome limitations of standard-camera technology for advanced-imaging experiments with requirements on high event-rates and high spatio-temporal resolution.

physics.ins-det↗

arXiv2020

Spatial Separation of the Conformers of Methyl Vinyl Ketone

Methyl vinyl ketone (C$_4$H$_6$O) is a volatile, labile organic compound of importance in atmospheric chemistry. We prepared a molecular beam of methyl vinyl ketone with a rotational temperature of 1.2(2)~K and demonstrated the spatial separation of the \emph{s-cis} and \emph{s-trans} conformers of methyl vinyl ketone using the electrostatic deflector. The resulting sample density was $1.5(2)\times10^{8}~\text{cm}^{-3}$ for the direct beam in the laser ionization region. These conformer-selected methyl vinyl ketone samples are well suited for conformer-specific chemical reactivity studies such as in Diels-Alder cycloaddition reactions.

physics.chem-ph↗

arXiv2020

Spatial separation of 2-propanol monomer and its ionization-fragmentation pathways

The spatial separation of 2-propanol monomer from its clusters in a molecular beam by an electrostatic deflector was demonstrated. Samples of 2-propanol monomer with a purity of 90 % and a beam density of $7\times10^6~\text{cm}^{-3}$ were obtained. These samples were utilized to study the femtosecond-laser-induced strong-field multi-photon ionization and fragmentation of 2-propanol using non-resonant 800 nm light with peak intensities of $3-7\times10^{13}~W/cm^{2}$.

physics.chem-ph↗

arXiv2019

Pure Molecular Beam of Water Dimer

Spatial separation of water dimer from water monomer and larger water-clusters through the electric deflector is presented. A beam of water dimer with $93~\%$ purity and a rotational temperature of $1.5~$K was obtained. Following strong-field ionization using a $35~$fs laser pulse with a wavelength centered around $800~$nm and a peak intensity of $10^{14}~\text{W}/\text{cm}^2$ we observed proton transfer and $46~\%$ of the ionized water dimer broke apart into a hydronium ion $\text{H}_3\text{O}^+$ and neutral OH.

physics.atm-clus↗