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Phys Rev Lett ; 123(21): 213001, 2019 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-31809166


We report the observation of the radiative decay of singly charged noble gas ground-state ions embedded in heterogeneous van der Waals clusters. Electron-photon coincidence spectroscopy and dispersed photon spectroscopy are applied to identify the radiative charge transfer from Kr atoms to a Ne_{2}^{+} dimer, which forms after single valence photoionization of Ne atoms at the surface of a NeKr cluster. This mechanism might be a fundamental decay process of ionized systems in an environment.

J Phys Chem A ; 123(16): 3551-3557, 2019 Apr 25.
Artigo em Inglês | MEDLINE | ID: mdl-30943036


Action spectroscopy using photon excitation in the VUV range (photon energy 4.5-9 eV) was performed on protonated uracil (UraH+) and uridine (UrdH+). The precursor ions with m/ z 113 and m/ z 245, respectively, were produced by an electrospray ionization source and accumulated inside a quadrupole ion trap mass spectrometer. After irradiation with tunable synchrotron radiation, product ion mass spectra were obtained. Fragment yields as a function of excitation energy show several maxima that can be attributed to the photoexcitation into different electronic states. For uracil, vertically excited states were calculated using the equation-of-motion coupled cluster approach and compared to the observed maxima. This allows to establish correlations between electronic states and the resulting fragment masses and can thus help to disentangle the complex de-excitation and fragmentation pathways of nucleic acid building blocks. Photofragmentation of the nucleoside uridine shows a significantly lower variety of fragments, indicating stabilization of the nucleobase by the attached sugar.

J Phys Chem Lett ; 10(5): 1078-1082, 2019 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-30779875


Energy and charge transfer processes play an important role in many fundamental reactions in chemistry, biochemistry, and even technology. If an entity that is part of a larger system is photoexcited, its energy will dissipate, for example, by rearrangement of electron density in a large molecule or by photon emission (fluorescence). Here, we report the experimental observation of free electrons from a heterogeneous van der Waals cluster, in which some sites act as electron emitters receiving their energy efficiently from other "antenna" sites that are resonantly excited in the UV range. By complementing electron spectroscopy with fluorescence detection, we can directly observe that electron emission via this mechanism completely quenches fluorescence once the channel opens. We suggest this mechanism to be important for both quenching of fluorescence as well as resonantly enhancing free electron production in a variety of systems.

Molecules ; 23(7)2018 06 26.
Artigo em Inglês | MEDLINE | ID: mdl-29949868


Dichroism in angle-resolved spectra of circularly polarized fluorescence from freely-rotating CO molecules was studied experimentally and theoretically. For this purpose, carbon monoxide in the gas phase was exposed to circularly polarized soft X-ray synchrotron radiation. The photon energy was tuned across the C 1s→π* resonant excitation, which decayed via the participator Auger transition into the CO⁺ A ²Π state. The dichroic parameter ß1 of the subsequent CO⁺ (A ²Π → X ²Σ⁺) visible fluorescence was measured by photon-induced fluorescence spectroscopy. Present experimental results are explained with the ab initio electronic structure and dynamics calculations performed by the single center method. Our results confirm the possibility to perform partial wave analysis of the emitted photoelectrons in closed-shell molecules.

Monóxido de Carbono/química , Dicroísmo Circular , Modelos Teóricos , Espectrometria de Fluorescência
Materials (Basel) ; 11(6)2018 May 23.
Artigo em Inglês | MEDLINE | ID: mdl-29789512


The detection of a single photon is the most sensitive method for sensing of photon emission. A common technique for single photon detection uses microchannel plate arrays combined with photocathodes and position sensitive anodes. Here, we report on the combination of such detectors with grating diffraction spectrometers, constituting a low-noise wavelength resolving photon spectroscopy apparatus with versatile applicability. We recapitulate the operation principle of such detectors and present the details of the experimental set-up, which we use to investigate fundamental mechanisms in atomic and molecular systems after excitation with tuneable synchrotron radiation. Extensions for time and polarization resolved measurements are described and examples of recent applications in current research are given.

J Phys Chem B ; 121(10): 2326-2330, 2017 03 16.
Artigo em Inglês | MEDLINE | ID: mdl-28187257


Despite its importance, the structure and dynamics of liquid water are still poorly understood in many apsects. Here, we report on the observation of optical fluorescence upon soft X-ray irradiation of liquid water. Detection of spectrally resolved fluorescence was achieved by a combination of the liquid microjet technique and fluorescence spectroscopy. We observe a genuine liquid-phase fluorescence manifested by a broad emission band in the 170-340 nm (4-7 eV) photon wavelength range. In addition, another narrower emission near 300 nm can be assigned to the fluorescence of OH (A state) in the gas phase, the emitting species being formed by Auger electrons escaping from liquid water. We argue that the newly observed broad-band emission of liquid water is relevant in search of extraterrestrial life, and we also envision the observed electron-ejection mechanism to find application for exploring solutes at liquid-vapor interfaces.