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21.
We report on the free diffusion of single molecule near an interface studied using fluorescence correlation spectroscopy.
In particular, we show that the chemical nature of the substrate may modify the free diffusion of a widely used molecule (rhodamine
6G), thus inducing unexpected effects in fluorescence correlation spectroscopy measurements. Our results show a strong influence,
up to a few micrometer from the interface, of the surface polarity. This effect is assessed through the relative weight of
the two dimensions diffusion process observed close to the surface. Our results are discussed in terms of competition between
surface-solvent, solvent-molecule and molecule-surface specific interactions. 相似文献
22.
Dr. Carlos Sánchez-Sánchez Dr. Thomas Dienel Dr. Adrien Nicolaï Dr. Neerav Kharche Dr. Liangbo Liang Colin Daniels Prof. Vincent Meunier Dr. Junzhi Liu Prof. Xinliang Feng Prof. Klaus Müllen Dr. Juan Ramón Sánchez-Valencia Dr. Oliver Gröning Dr. Pascal Ruffieux Prof. Roman Fasel 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(52):12074-12082
A bottom up method for the synthesis of unique tetracene-based nanoribbons, which incorporate cyclobutadiene moieties as linkers between the acene segments, is reported. These structures were achieved through the formal [2+2] cycloaddition reaction of ortho-functionalized tetracene precursor monomers. The formation mechanism and the electronic and magnetic properties of these nanoribbons were comprehensively studied by means of a multitechnique approach. Ultra-high vacuum scanning tunneling microscopy showed the occurrence of metal-coordinated nanostructures at room temperature and their evolution into nanoribbons through formal [2+2] cycloaddition at 475 K. Frequency-shift non-contact atomic force microscopy images clearly proved the presence of bridging cyclobutadiene moieties upon covalent coupling of activated tetracene molecules. Insight into the electronic and vibrational properties of the so-formed ribbons was obtained by scanning tunneling microscopy, Raman spectroscopy, and theoretical calculations. Magnetic properties were addressed from a computational point of view, allowing us to propose promising candidates to magnetic acene-based ribbons incorporating four-membered rings. The reported findings will increase the understanding and availability of new graphene-based nanoribbons with high potential in future spintronics. 相似文献
23.
Pascal Tournier 《电子设计技术》2005,12(12):74-74,115
手机等便携式电子产品正集成越来越多的多媒体功能,这引起了人们对增加立体声功能的极大兴趣。单声道结构用于声音放大及和弦铃声,在某些情况下可用作免提扬声器。虽然功能已足够,但这并非是令人满意的高质量音乐播放解决方案。 相似文献
24.
Jalal Ghilane Olivier Fontaine Pascal Martin Jean-Christophe Lacroix Hyacinthe Randriamahazaka 《Electrochemistry communications》2008,10(8):1205-1209
The electrochemical reduction of noble metal electrodes in the presence of redox ionic liquid, 1-ferrocenylethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, [FcEMIM][TFSI], was investigated by cyclic voltammetry. Our experiments suggest the formation of metal with negative oxidation states, in the cases of platinum and gold electrodes [Mn−, FcEMIM+]. By analogy with the previous work, the formation of these phases is concomitant with the insertion of the supporting electrolyte; which correspond in our experimental condition to the redox cation of the ionic liquid. As an exciting result, the electrochemical investigations of the reduced electrode in electrolytic solution, containing solvent and supporting electrolyte, evidence the presence of the ferrocene groups at the electrode surface. Moreover, the reduced electrode exhibits the presence of the ferrocene even after, contact with air, after ultrasound, and after physical polishing, highlighting the large stability of this organo-metallic phases formed in this media. The AFM investigations demonstrate the morphological change of the platinum surface after the reduction process. Finally, our works bring a formal electrochemical proof of the presence of the ionic liquid cation inside the electrode material after the cathodic treatment in this media. 相似文献
25.
Gadolinium chelate coated gold nanoparticles as contrast agents for both X-ray computed tomography and magnetic resonance imaging 总被引:1,自引:0,他引:1
Alric C Taleb J Le Duc G Mandon C Billotey C Le Meur-Herland A Brochard T Vocanson F Janier M Perriat P Roux S Tillement O 《Journal of the American Chemical Society》2008,130(18):5908-5915
Functionalized gold nanoparticles were applied as contrast agents for both in vivo X-ray and magnetic resonance imaging. These particles were obtained by encapsulating gold cores within a multilayered organic shell which is composed of gadolinium chelates bound to each other through disulfide bonds. The contrast enhancement in MRI stems from the presence of gadolinium ions which are entrapped in the organic shell, whereas the gold core provides a strong X-ray absorption. This study revealed that these particles suited for dual modality imaging freely circulate in the blood vessels without undesirable accumulation in the lungs, spleen, and liver. 相似文献
26.
Pirali O Van-Oanh NT Parneix P Vervloet M Bréchignac P 《Physical chemistry chemical physics : PCCP》2006,8(32):3707-3714
Both experimental and theoretical spectroscopic studies on small gas phase polycyclic aromatic hydrocarbons in the far-infrared spectral region are reported. The experimental set-up based on thermal emission and Fourier transform far infrared analysis led to the detection of relatively broad vibrational bands, unresolved in rotation, representative of each molecule. Detailed theoretical investigations were performed, including both ab initio calculations and spectral simulations. For the majority of the samples, this study provides the first detection of the vibrational modes associated with the skeleton motions. 相似文献
27.
Shikhova E Danilov EO Kinayyigit S Pomestchenko IE Tregubov AD Camerel F Retailleau P Ziessel R Castellano FN 《Inorganic chemistry》2007,46(8):3038-3048
A comprehensive photophysical study is presented which compares the ground- and excited-state properties of four platinum(II) terpyridyl acetylide compounds of the general formula [Pt(tBu3tpy)(CCR)]+, where tBu3tpy is 4,4',4' '-tri-tert-butyl-2,2':6',2' '-terpyridine and R is an alkyl or aryl group. [Ru(tBu3tpy)3]2+ and the pivotal synthetic precursor [Pt(tBu3tpy)Cl]+ were also investigated in the current work. The latter two complexes possess short excited-state lifetimes and were investigated using ultrafast spectrometry while the other four compounds were evaluated using conventional nanosecond transient-absorption spectroscopy. The original intention of this study was to comprehend the nature of the impressive excited-state absorptions that emanate from this class of transition-metal chromophores. Transient-absorbance-difference spectra across the series contain the same salient features, which are modulated only slightly in wavelength and markedly in intensity as a function of the appended acetylide ligand. More intense absorption transients are observed in the arylacetylide structures relative to those bearing an alkylacetylide, consistent with transitions coupled to the pi system of the ancillary ligand. Reductive spectroelectrochemical measurements successfully generated the electronic spectrum of the tBu3tpy radical anion in all six complexes at room temperature. These measurements confirm that electronic absorptions associated with the tBu3tpy radical anion simply do not account for the intense optical transitions observed in the excited state of the Pt(II) chromophores. Transient-trapping experiments using the spectroscopically silent reductive quencher DABCO clearly demonstrate the loss of most transient-absorption features in the acetylide complexes throughout the UV, visible, and near-IR regions following bimolecular excited-state electron transfer, suggesting that these features are strongly tied to the photogenerated hole which is delocalized across the Pt center and the ancillary acetylide ligand. 相似文献
28.
Emi Evangelio Dr. Marie‐Laure Bonnet Dr. Miquel Cabañas Dr. Motohiro Nakano Dr. Jean‐Pascal Sutter Dr. Andrea Dei Prof. Vincent Robert Dr. Daniel Ruiz‐Molina Dr. 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(22):6666-6677
The different thermally induced intermolecular electron transfer (IET) processes that can take place in the series of complexes [M(Cat‐N‐BQ)(Cat‐N‐SQ)]/[M(Cat‐N‐BQ)2], for which M=Co ( 2 ), Fe ( 3 ) and Ni( 4 ), and Cat‐N‐BQ and Cat‐N‐SQ denote the mononegative (Cat‐N‐BQ?) or dinegative (Cat‐N‐SQ2?) radical forms of the tridentate Schiff‐base ligand 3,5‐di‐tert‐butyl‐1,2‐quinone‐1‐(2‐hydroxy‐3,5‐di‐tert‐butylphenyl)imine, have been studied by variable‐temperature UV/Vis and NMR spectroscopies. Depending on the metal ion, rather different behaviors are observed. Complex 2 has been found to be one of the few examples so far reported to exhibit the coexistence of two thermally induced electron transfer processes, ligand‐to‐metal (IETLM) and ligand‐to‐ligand (IETLL). IETLL was only found to take place in complex 3 , and no IET was observed for complex 4 . Such experimental studies have been combined with ab initio wavefunction‐based CASSCF/CASPT2 calculations. Such a strategy allows one to solicit selectively the speculated orbitals and to access the ground states and excited‐spin states, as well as charge‐transfer states giving additional information on the different IET processes. 相似文献
29.
Popeney CS Setaro A Mutihac RC Bluemmel P Trappmann B Vonneman J Reich S Haag R 《Chemphyschem》2012,13(1):203-211
A series of nonionic amphiphiles derived from polyglycerol dendrons were studied for their ability to solubilize and isolate single-walled carbon nanotubes. The amphiphiles possessed differently sized polar head groups, hydrophobic tail units, and various aromatic and non-aromatic groups between the head and tail groups. Absorbance analysis revealed that amphiphiles with anchor groups derived from pyrene were far inferior to those that possessed simple linear aliphatic tail groups. Absorbance and near-infrared fluorescence analyses revealed a weak dependence on the dendron size of the head group, but a strong positive trend in suspended nanotube density and fluorescence intensity for amphiphiles with longer tail units. Variations in the moieties linking the head and tail groups led to a range of effects on the suspensions, with linkers imparting flexibility and a bent shape that gave improved performance overall. This was illustrated most dramatically by a pair of benzamide-containing amphiphiles, the para isomer of which showed evidence in the fluorescence data of increased nanotube aggregate formation when compared with the meta isomer. In addition, statistical AFM was used to illustrate more directly the microscopic differences between amphiphiles that were effective at nanotube bundle disruption and those that were not. 相似文献
30.
Phenyliodine(III) bis(trifluoroacetate) (PIFA) in conjunction with a Lewis acid promotes C-C coupling of Bodipy monomers leading to mixtures of various oligomers. When a single position is blocked with an iodo or phenyl group, formation of the dimer is favored. These dimers display two successive oxidation and two reduction waves separated on average by 260 and 130 mV, respectively, corresponding to each Bodipy subunit. 相似文献