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1.
J Phys Chem A ; 2020 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-32463669

RESUMO

Electronic excitations in the valence shell of Ne clusters were studied by fluorescence spectroscopy. The measured fluorescence excitation functions contain information about the nature and number of excitonic states and the mean cluster size of the produced size distribution. Mean cluster sizes were determined by comparing surface and bulk contributions using a multidimensional fitting algorithm, with good agreement to commonly used scaling laws. The influence of different size distributions, which were not considered in previous investigations on homogeneous noble gas cluster jets, are implemented into the proposed model. The present work is the first approach using fluorescence spectroscopy for the determination of the mean size of Ne cluster jets created by supersonic expansion.

2.
Phys Rev Lett ; 124(4): 047203, 2020 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-32058758

RESUMO

We show that it is possible to engineer magnetic multidomain configurations without domain walls in a prototypical rare-earth-transition-metal ferrimagnet using keV He^{+} ion bombardment. We additionally show that these patterns display a particularly stable magnetic configuration due to a deep minimum in the energy of the system caused by flux closure and a corresponding reduction of the magnetostatic energy without an increase in energy by exchange and anisotropy terms across the walls. This occurs because light-ion bombardment affects an element's relative contribution to the properties of the ferrimagnet differently. Therefore, it is possible to control the relative contribution from each magnetic subsystem. The selection of material and the use of light-ion bombardment allow us to engineer domain patterns in continuous magnetic films, which open a way to fabricate them in a much smaller scale than currently possible. Our Letter emphasizes that the right criterion to determine the presence or absence of a domain wall is whether there is a rotation of the spin for each sublattice and that changes of the direction of effective magnetization alone do not constitute an appropriate criterion.

3.
Soft Matter ; 16(6): 1594-1598, 2020 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-31956884

RESUMO

Single and double paramagnetic colloidal particles are placed above a magnetic square pattern and are driven with an external magnetic field processing around a high symmetry direction of the pattern. The external magnetic field and that of the pattern confine the colloids into lanes parallel to a lattice vector of the pattern. The precession of the external field causes traveling minima of the magnetic potential along the direction of the lanes. At sufficiently high frequencies of modulation, only the doublets respond to the external field and move in direction of the traveling minima along the lanes, while the single colloids cannot follow and remain static. We show how the doublets can induce a coordinated motion of the single colloids building colloidal trains made of a chain of several single colloids transported by doublets.

4.
Phys Rev Lett ; 123(21): 213001, 2019 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-31809166

RESUMO

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.

5.
J Phys Chem A ; 123(16): 3551-3557, 2019 Apr 25.
Artigo em Inglês | MEDLINE | ID: mdl-30943036

RESUMO

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.

6.
J Phys Chem Lett ; 10(5): 1078-1082, 2019 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-30779875

RESUMO

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.

7.
Soft Matter ; 15(7): 1539-1550, 2019 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-30608507

RESUMO

Edge currents of paramagnetic colloidal particles propagate at the edge between two topologically equivalent magnetic lattices of different lattice constant when the system is driven with periodic modulation loops of an external magnetic field. The number of topologically protected particle edge transport modes is not determined by a bulk-boundary correspondence. Instead, we find a rich variety of edge transport modes that depend on the symmetry of both the edge and the modulation loop. The edge transport can be ratchet-like or adiabatic, time or non-time reversal symmetric. The topological nature of the edge transport is classified by a set of winding numbers around bulk fence points extended by winding numbers around edge specific bifurcation points that cannot be deduced from the two bulk lattices.

8.
Beilstein J Nanotechnol ; 9: 2968-2979, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30591845

RESUMO

Background: The application of superparamagnetic particles as biomolecular transporters in microfluidic systems for lab-on-a-chip applications crucially depends on the ability to control their motion. One approach for magnetic-particle motion control is the superposition of static magnetic stray field landscapes (MFLs) with dynamically varying external fields. These MFLs may emerge from magnetic domains engineered both in shape and in their local anisotropies. Motion control of smaller beads does necessarily need smaller magnetic patterns, i.e., MFLs varying on smaller lateral scales. The achievable size limit of engineered magnetic domains depends on the magnetic patterning method and on the magnetic anisotropies of the material system. Smallest patterns are expected to be in the range of the domain wall width of the particular material system. To explore these limits a patterning technology is needed with a spatial resolution significantly smaller than the domain wall width. Results: We demonstrate the application of a helium ion microscope with a beam diameter of 8 nm as a mask-less method for local domain patterning of magnetic thin-film systems. For a prototypical in-plane exchange-bias system the domain wall width has been investigated as a function of the angle between unidirectional anisotropy and domain wall. By shrinking the domain size of periodic domain stripes, we analyzed the influence of domain wall overlap on the domain stability. Finally, by changing the geometry of artificial two-dimensional domains, the influence of domain wall overlap and domain wall geometry on the ultimate domain size in the chosen system was analyzed. Conclusion: The application of a helium ion microscope for magnetic patterning has been shown. It allowed for exploring the fundamental limits of domain engineering in an in-plane exchange-bias thin film as a prototypical system. For two-dimensional domains the limit depends on the domain geometry. The relative orientation between domain wall and anisotropy axes is a crucial parameter and therefore influences the achievable minimum domain size dramatically.

10.
Nanomaterials (Basel) ; 8(10)2018 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-30308934

RESUMO

Here, we systematically investigated the influence of ion bombardment with different fluences on the strength and direction of the exchange bias coupling in Au/Co/NiO systems with perpendicular magnetic anisotropy of the Co layer. We found that the direction of the exchange bias coupling can be reversed as a result of ion bombardment performed in an external magnetic field which is in the opposite direction to the magnetic field applied during film deposition. Moreover, the strength of the exchange bias coupling can be tailored by varying the ion fluence. These results show behaviors similar to the results found for systems of ferromagnetic layers with in-plane anisotropy. Our experimental work, supported by a two-energy-level model, demonstrates that exchange bias coupling can be tuned in a layered system with perpendicular magnetic anisotropy using ion bombardment.

11.
Biomicrofluidics ; 12(4): 044117, 2018 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-30174776

RESUMO

Colloidal magnetophoretic lensing of water suspended micrometer-sized superparamagnetic beads (SPBs) above a topographically patterned magnetic thin film system with perpendicular magnetic anisotropy is demonstrated. The magnetic pattern consisting of concentric annuli of micron-sized widths has been superimposed with a rotating external magnetic field, and it is shown that the trajectories of the SPBs above this structure are similar to light rays in an optical focusing lens. SPB trajectories converge towards the central region and have divergent trajectories while passing the center. The experimental findings are corroborated by a quantitative model for the SPB trajectories. The magnetophoretic lensing effect leads to a high SPB concentration in the center of the pattern and may be useful for applications where SPBs have to approach each other in a controlled way.

12.
Molecules ; 23(7)2018 06 26.
Artigo em Inglês | MEDLINE | ID: mdl-29949868

RESUMO

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.


Assuntos
Monóxido de Carbono/química , Dicroísmo Circular , Modelos Teóricos , Espectrometria de Fluorescência
13.
Materials (Basel) ; 11(6)2018 May 23.
Artigo em Inglês | MEDLINE | ID: mdl-29789512

RESUMO

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.

14.
Soft Matter ; 13(29): 5044-5075, 2017 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-28703235

RESUMO

The topologically protected transport of colloidal particles on top of periodic magnetic patterns is studied experimentally, theoretically, and with computer simulations. To uncover the interplay between topology and symmetry we use patterns of all possible two dimensional magnetic point group symmetries with equal lengths lattice vectors. Transport of colloids is achieved by modulating the potential with external, homogeneous but time dependent magnetic fields. The modulation loops can be classified into topologically distinct classes. All loops falling into the same class cause motion in the same direction, making the transport robust against internal and external perturbations. We show that the lattice symmetry has a profound influence on the transport modes, the accessibility of transport networks, and the individual transport directions of paramagnetic and diamagnetic colloidal particles. We show how the transport of colloidal particles above a two fold symmetric stripe pattern changes from universal adiabatic transport at large elevations via a topologically protected ratchet motion at intermediate elevations toward a non-transport regime at low elevations. Transport above four-fold symmetric patterns is closely related to the two-fold symmetric case. The three-fold symmetric case however consists of a whole family of patterns that continuously vary with a phase variable. We show how this family can be divided into two topologically distinct classes supporting different transport modes and being protected by proper and improper six fold symmetries. We discuss and experimentally demonstrate the topological transition between both classes. All three-fold symmetric patterns support independent transport directions of paramagnetic and diamagnetic particles. The similarities and the differences in the lattice symmetry protected transport of classical over-damped colloidal particles versus the topologically protected transport in quantum mechanical systems are emphasized.

15.
J Phys Chem Lett ; 8(13): 2780-2786, 2017 Jul 06.
Artigo em Inglês | MEDLINE | ID: mdl-28582620

RESUMO

Most large molecules are chiral in their structure: they exist as two enantiomers, which are mirror images of each other. Whereas the rovibronic sublevels of two enantiomers are almost identical (neglecting a minuscular effect of the weak interaction), it turns out that the photoelectric effect is sensitive to the absolute configuration of the ionized enantiomer. Indeed, photoionization of randomly oriented enantiomers by left or right circularly polarized light results in a slightly different electron flux parallel or antiparallel with respect to the photon propagation direction-an effect termed photoelectron circular dichroism (PECD). Our comprehensive study demonstrates that the origin of PECD can be found in the molecular frame electron emission pattern connecting PECD to other fundamental photophysical effects such as the circular dichroism in angular distributions (CDAD). Accordingly, distinct spatial orientations of a chiral molecule enhance the PECD by a factor of about 10.

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

RESUMO

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.

17.
J Phys Condens Matter ; 29(12): 125801, 2017 Mar 29.
Artigo em Inglês | MEDLINE | ID: mdl-28106005

RESUMO

The magnetic modification of exchange bias materials by 'ion bombardment induced magnetic patterning' has been established more than a decade ago. To understand these experimental findings several theoretical models were introduced. Few investigations, however, did focus on magnetic property modifications caused by effects of ion bombardment in the ferromagnetic layer. In the present study, the structural changes occurring under ion bombardment were investigated by Monte-Carlo simulations and in experiments. A strong reduction of the saturation magnetization scaling linearly with increasing ion doses is observed and our findings suggest that it is correlated to the swelling of the layer material based on helium implantation and vacancy creation.

18.
Langmuir ; 32(41): 10491-10496, 2016 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-27661087

RESUMO

It is shown that the self-assembly of diamagnetic molecule submonolayers on a surface can be influenced by magnetic stray field landscapes emerging from artificially fabricated magnetic domains and domain walls. The directed local chemisorption of diamagnetic subphthalocyaninatoboron molecules in relation to the artificially created domain pattern is proved by a combination of surface analytical methods: ToF-SIMS, X-PEEM, and NEXAFS imaging. Thereby, a new method to influence self-assembly processes and to produce patterned submonolayers is presented.

19.
ACS Nano ; 10(9): 8491-8, 2016 09 27.
Artigo em Inglês | MEDLINE | ID: mdl-27529182

RESUMO

We realized a deterministic transport system for superparamagnetic microbeads through micrometer-sized tubes acting as channels. Beads are moved stepwise in a paternoster-like manner through the tube and back on top of it by weak magnetic field pulses without changing the field pulse polarity and taking advantage of the magnetic stray field emerging from the tubular structures. The microtubes are engineered by rolling up exchange bias layer systems, magnetically patterned into parallel stripe magnetic domains. In this way, the tubes possess distinct azimuthally aligned magnetic domain patterns. This transport mechanism features high step velocities and remote control of not only the direction and trajectory but also the velocity of the transport without the need of fuel or catalytic material. Therefore, this approach has the potential to impact several fields of 3D applications in biotechnology, including particle transport related phenomena in lab-on-a-chip and lab-in-a-tube devices.

20.
Phys Chem Chem Phys ; 17(48): 32574-5, 2015 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-26597710

RESUMO

Correction for 'Size and shape dependent photoluminescence and excited state decay rates of diamondoids' by Robert Richter et al., Phys. Chem. Chem. Phys., 2014, 16, 3070-3076.

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