Probing molecular dynamics at the nanoscale via an individual paramagnetic center

Understanding the dynamics of molecules adsorbed to surfaces or confined to small volumes is a matter of increasing scientific and technological importance. Here, we demonstrate a pulse protocol using individual paramagnetic nitrogen vacancy (NV) centers in diamond to observe the time evolution of 1H spins from organic molecules located a few nanometers from the diamond surface. The protocol records temporal correlations among the interacting 1H spins, and thus is sensitive to the local system dynamics via its impact on the nuclear spin relaxation and interaction with the NV. We are able to gather information on the nanoscale rotational and translational diffusion dynamics by carefully analyzing the time dependence of the NMR signal. Applying this technique to various liquid and solid samples, we find evidence that liquid samples form a semi-solid layer of 1.5 nm thickness on the surface of diamond, where translational diffusion is suppressed while rotational diffusion remains present. Extensions of the present technique could be adapted to highlight the chemical composition of molecules tethered to the diamond surface or to investigate thermally or chemically activated dynamical processes such as molecular folding

Atom lithography without laser cooling

Using direct-write atom lithography, Fe nanolines are deposited with a pitch of 186 nm, a full width at half maximum (FWHM) of 50 nm, and a height of up to 6 nm. These values are achieved by relying on geometrical collimation of the atomic beam, thus without using laser collimation techniques. This opens the way for applying direct-write atom lithography to a wide variety of elements.Comment: 7 pages, 11 figure

Optical properties of an ensemble of G-centers in silicon

We addressed the carrier dynamics in so-called G-centers in silicon (consisting of substitutional-interstitial carbon pairs interacting with interstitial silicons) obtained via ion implantation into a silicon-on-insulator wafer. For this point defect in silicon emitting in the telecommunication wavelength range, we unravel the recombination dynamics by time-resolved photoluminescence spectroscopy. More specifically, we performed detailed photoluminescence experiments as a function of excitation energy, incident power, irradiation fluence and temperature in order to study the impact of radiative and non-radiative recombination channels on the spectrum, yield and lifetime of G-centers. The sharp line emitting at 969 meV ($\sim$1280 nm) and the broad asymmetric sideband developing at lower energy share the same recombination dynamics as shown by time-resolved experiments performed selectively on each spectral component. This feature accounts for the common origin of the two emission bands which are unambiguously attributed to the zero-phonon line and to the corresponding phonon sideband. In the framework of the Huang-Rhys theory with non-perturbative calculations, we reach an estimation of 1.6$\pm$0.1 \angstrom for the spatial extension of the electronic wave function in the G-center. The radiative recombination time measured at low temperature lies in the 6 ns-range. The estimation of both radiative and non-radiative recombination rates as a function of temperature further demonstrate a constant radiative lifetime. Finally, although G-centers are shallow levels in silicon, we find a value of the Debye-Waller factor comparable to deep levels in wide-bandgap materials. Our results point out the potential of G-centers as a solid-state light source to be integrated into opto-electronic devices within a common silicon platform

Stark shift and field ionization of arsenic donors in 28^{28}Si-SOI structures

We develop an efficient back gate for silicon-on-insulator (SOI) devices operating at cryogenic temperatures, and measure the quadratic hyperfine Stark shift parameter of arsenic donors in isotopically purified $^{28}$Si-SOI layers using such structures. The back gate is implemented using MeV ion implantation through the SOI layer forming a metallic electrode in the handle wafer, enabling large and uniform electric fields up to $\sim$ 2 V/$\mu$m to be applied across the SOI layer. Utilizing this structure we measure the Stark shift parameters of arsenic donors embedded in the $^{28}$Si SOI layer and find a contact hyperfine Stark parameter of $\eta_a=-1.9\pm0.2\times10^{-3} \mu$m$^2$/V$^2$. We also demonstrate electric-field driven dopant ionization in the SOI device layer, measured by electron spin resonance.Comment: 5 pages, 3 figure

Multiple packets of neutral molecules revolving for over a mile

The level of control that one has over neutral molecules in beams dictates their possible applications. Here we experimentally demonstrate that state-selected, neutral molecules can be kept together in a few mm long packet for a distance of over one mile. This is accomplished in a circular arrangement of 40 straight electrostatic hexapoles through which the molecules propagate over 1000 times. Up to 19 packets of molecules have simultaneously been stored in this ring structure. This brings the realization of a molecular low-energy collider within reach

Anharmonic magnetic deformation of self-assembled molecular nanocapsules

High magnetic fields were used to deform spherical nanocapsules, self-assembled from bola-amphiphilic sexithiophene molecules. At low fields the deformation -- measured through linear birefringence -- scales quadratically with the capsule radius and with the magnetic field strength. These data confirm a long standing theoretical prediction (W. Helfrich, Phys. Lett. {\bf 43A}, 409 (1973)), and permits the determination of the bending rigidity of the capsules as (2.6$\pm$0.8)$\times 10^{-21}$ J. At high fields, an enhanced rigidity is found which cannot be explained within the Helfrich model. We propose a complete form of the free energy functional that accounts for this behaviour, and allows discussion of the formation and stability of nanocapsules in solution.Comment: 4 pages, 3 figures, accepted in Phys. Rev. Let

Can Polymer Coils be modeled as "Soft Colloids"?

We map dilute or semi-dilute solutions of non-intersecting polymer chains onto a fluid of ``soft'' particles interacting via a concentration dependent effective pair potential, by inverting the pair distribution function of the centers of mass of the initial polymer chains. A similar inversion is used to derive an effective wall-polymer potential; these potentials are combined to successfully reproduce the calculated exact depletion interaction induced by non-intersecting polymers between two walls. The mapping opens up the possibility of large-scale simulations of polymer solutions in complex geometries.Comment: 4 pages, 3 figures ReVTeX[epsfig,multicol,amssymb] references update