Publications by authors named "Robert Carley"

8 Publications

  • Page 1 of 1

Observation of fluctuation-mediated picosecond nucleation of a topological phase.

Nat Mater 2021 Jan 5;20(1):30-37. Epub 2020 Oct 5.

European XFEL, Schenefeld, Germany.

Topological states of matter exhibit fascinating physics combined with an intrinsic stability. A key challenge is the fast creation of topological phases, which requires massive reorientation of charge or spin degrees of freedom. Here we report the picosecond emergence of an extended topological phase that comprises many magnetic skyrmions. The nucleation of this phase, followed in real time via single-shot soft X-ray scattering after infrared laser excitation, is mediated by a transient topological fluctuation state. This state is enabled by the presence of a time-reversal symmetry-breaking perpendicular magnetic field and exists for less than 300 ps. Atomistic simulations indicate that the fluctuation state largely reduces the topological energy barrier and thereby enables the observed rapid and homogeneous nucleation of the skyrmion phase. These observations provide fundamental insights into the nature of topological phase transitions, and suggest a path towards ultrafast topological switching in a wide variety of materials through intermediate fluctuating states.
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http://dx.doi.org/10.1038/s41563-020-00807-1DOI Listing
January 2021

Coverage- and temperature-controlled isomerization of an imine derivative on Au(111).

J Am Chem Soc 2013 Mar 8;135(11):4273-81. Epub 2013 Mar 8.

Fachbereich Physik, Freie Universität Berlin, Arnimallee 14, 14195 Berlin, Germany.

The isomerization behavior of photochromic molecular switches is strongly influenced by adsorption on metal surfaces. For (E)-3,5-di-tert-butyl-N-(3,5-di-tert-butylbenzylidene)aniline (abbreviated as TBI for tetra-tert-butyl imine), it is found that a layer adsorbed on Au(111) can undergo an isomerization from the trans to the cis and back to the trans configuration when continuously increasing the sample temperature and accordingly decreasing the sample coverage. The conformation and adsorption geometry of TBI are determined from near-edge X-ray absorption fine structure measurements in agreement with density functional theory calculations taking into account the van der Waals interaction between adsorbate and metal surface. The coverage- and temperature-controlled conformational transitions are reversible and are driven by the higher packing density of the less stable cis-isomer in combination with the low thermal activation barrier of the trans- to cis-isomerization typical for imine derivatives. This unexpected scenario is corroborated by thermal desorption and vibrational spectroscopy as well as scanning tunneling microscopy.
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http://dx.doi.org/10.1021/ja309330eDOI Listing
March 2013

Femtosecond laser excitation drives ferromagnetic gadolinium out of magnetic equilibrium.

Phys Rev Lett 2012 Aug 31;109(5):057401. Epub 2012 Jul 31.

Max-Born-Institut, Berlin, Germany.

The temporal evolution of the exchange-split Δ(2)-like Σ valence bands of the 4f-ferromagnet gadolinium after femtosecond laser excitation has been studied using angle-resolved photoelectron spectroscopy based on high-order harmonic generation. The ultrafast drop of the exchange splitting reflects the magnetic response seen in femtosecond magnetic dichroism experiments. However, while the minority valence band reacts immediately, the response of the majority counterpart is delayed by 1 picosecond and is only half as fast. These findings demonstrate that laser excitation drives the valence band structure out of magnetic equilibrium.
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http://dx.doi.org/10.1103/PhysRevLett.109.057401DOI Listing
August 2012

Mixed self-assembled monolayers of azobenzene photoswitches with trifluoromethyl and cyano end groups.

J Phys Condens Matter 2012 Oct 11;24(39):394015. Epub 2012 Sep 11.

Freie Universität Berlin, Fachbereich Physik, Arnimallee 14, 14195 Berlin, Germany.

Mixed self-assembled monolayers (SAMs) of alkanethiolates carrying azobenzene chromophores with either a trifluoromethyl or a cyano substituent have been studied. High-resolution x-ray photoelectron spectroscopy proves that the ratio of adsorbed molecules can be arbitrarily adjusted via the molar fractions in solution. As a function of these molar fractions core level shifts are observed which are attributed to local work-function changes. By simulating the electric dipole field distribution, the continuous core level shifts are ascribed to a homogeneous mixture of molecules with different end groups adsorbed on adjacent lattice sites. Near-edge x-ray absorption fine structure measurements reveal formation of well-ordered SAMs. Despite the difference in dipole moment of the end groups, the molecular tilt and twist angles are identical for both single-component SAMs and a 1:1 mixed SAM.
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http://dx.doi.org/10.1088/0953-8984/24/39/394015DOI Listing
October 2012

On the electronic and geometrical structure of the trans- and cis-isomer of tetra-tert-butyl-azobenzene on Au(111).

Phys Chem Chem Phys 2010 May 23;12(17):4488-97. Epub 2010 Mar 23.

Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie, Max-Born-Str. 2A, 12489 Berlin, Germany.

Near edge X-ray absorption fine structure and X-ray photoelectron spectroscopy have been employed to follow the reversible trans to cis isomerization of tetra-tert-butyl-azobenzene (TBA) adsorbed on Au(111). For one monolayer the molecules adopt an adsorption geometry characteristic of the trans-TBA isomer. The azo-bridge (N = N) is aligned nearly parallel to the surface and the phenyl rings exhibit a planar orientation with a small tilt angle
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http://dx.doi.org/10.1039/b924409cDOI Listing
May 2010

Structure and excitonic coupling in self-assembled monolayers of azobenzene-functionalized alkanethiols.

J Am Chem Soc 2010 Feb;132(6):1831-8

Max-Born-Institut, Max-Born-Str. 2A, 12489 Berlin, Germany.

Optical properties and the geometric structure of self-assembled monolayers of azobenzene-functionalized alkanethiols have been investigated by UV/visible and near edge X-ray absorption fine structure spectroscopy in combination with density-functional theory. By attaching a trifluoro-methyl end group to the chromophore both the molecular tilt and twist angle of the azobenzene moiety are accessible. Based on this detailed structural analysis the energetic shifts observed in optical reflection spectroscopy can be qualitatively described within an extended dipole model. This substantiates sizable excitonic coupling among the azobenzene chromophores as an important mechanism that hinders trans to cis isomerization in densely packed self-assembled monolayers.
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http://dx.doi.org/10.1021/ja903636qDOI Listing
February 2010

Effects of geographical location and land use on atmospheric deposition of nitrogen in the State of Connecticut.

Environ Pollut 2003 ;124(3):437-48

Department of Natural Resources Management and Engineering, University of Connecticut, Storrs, CT 06269-4087, USA.

A network of eight monitoring stations was established to study the atmospheric nitrogen concentration and deposition in the State of Connecticut. The stations were classified into urban, rural, coastal and inland categories to represent the geographical location and land use characteristics surrounding the monitoring sites. Nitrogen species including nitrate, ammonium, nitric acid vapor and organic nitrogen in the air and precipitation were collected, analyzed and used to infer nitrogen concentrations and dry and wet deposition flux densities for the sampling period from 1997 through 1999, with independently collected meteorological data. Statistical analyses were conducted to evaluate the spatial variations of atmospheric concentration and deposition fluxes of total nitrogen in Connecticut. A slightly higher atmospheric concentration of total nitrogen was observed along the Connecticut coastline of Long Island Sound compared to inland areas, while the differences of nitrogen deposition fluxes were insignificant between coastal and inland sites. The land use characteristics surrounding the monitoring sites had profound effects on the atmospheric nitrogen concentration and dry deposition flux. The ambient nitrogen concentration over the four urban sites was averaged 38.9% higher than that over the rural sites, resulting a 58.0% higher dry deposition flux in these sites compared to their rural counterparts. The local industrial activities and traffic emissions of nitrogen at urban areas had significant effects on the spatial distribution of atmospheric nitrogen concentration and dry deposition flux in the State. Wet and total deposition fluxes appeared to be invariant between the monitoring sites, except for high flux densities measured at Old Greenwich, a monitoring station near to and downwind of the New York and New Jersey industrial complexes.
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http://dx.doi.org/10.1016/s0269-7491(03)00043-5DOI Listing
September 2003

Atmospheric mercury monitoring survey in Beijing, China.

Chemosphere 2002 Jul;48(1):97-107

The Environmental Research Institute, University of Connecticut, Storrs 06269-3210, USA.

With the aid of one industrial, two urban, two suburban, and two rural sampling locations, diurnal patterns of total gaseous mercury (TGM) were monitored in January, February and September of 1998 in Beijing, China. Monitoring was conducted in six (two urban, two suburban, one rural and the industrial sites) of the seven sampling sites during January and February (winter) and in four (two urban, one rural, and the industrial sites) of the sampling locations during September (summer) of 1998. In the three suburban sampling stations, mean TGM concentrations during the winter sampling period were 8.6, 10.7, and 6.2 ng/m3, respectively. In the two urban sampling locations mean TGM concentrations during winter and summer sampling periods were 24.7, 8.3, 10, and 12.7 ng/m3, respectively. In the suburban-industrial and the two rural sampling locations, mean mercury concentrations ranged from 3.1-5.3 ng/m3 in winter to 4.1-7.7 ng/m3 in summer sampling periods. In the Tiananmen Square (urban), and Shijingshan (suburban) sampling locations the mean TGM concentrations during the summer sampling period were higher than winter concentrations, which may have been caused by evaporation of soil-bound mercury in warm periods. Continuous meteorological data were available at one of the suburban sites, which allowed the observation of mercury concentration variations associated with some weather parameters. It was found that there was a moderate negative correlation between the wind speed and the TGM concentration at this suburban sampling location. It was also found that during the sampling period at the same site, the quantity of TGM transported to or from the sampling site was mainly influenced by the duration and frequency of wind occurrence from certain directions.
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http://dx.doi.org/10.1016/s0045-6535(02)00026-7DOI Listing
July 2002
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