RESUMEN

Functionalizing surfaces with self-assembled monolayers (SAMs) allows to efficiently bind bioreceptors, for instance, by bio-orthogonal click reactions, which is useful in biosensor fabrication. Control of the bioreceptor concentration on the surface can be achieved by coating an SAM mixture consisting of a functional SAM, which binds the bioreceptor, and a nonfunctional SAM for dilution. In this work, a novel vapor-based coating approach for the preparation of mixed SAM coatings is presented. Sequential evaporation of the SAM precursors, i.e., fluoroalkyl and azidoalkyl silanes, by heating under reduced pressure leads to the formation of a two-dimensional siloxane monolayer network on silicon oxide. The presence of both SAMs in the mixed coatings is confirmed by Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. As verified by atomic force microscopy, the morphologies of the coatings and the uncoated silicon oxide substrates are similar, indicating a conformal coating. Functionality of the SAM mixture is demonstrated by a reaction with a fluorescent dye, illustrating its potential application in biosensors.

RESUMEN

The ability to apply force and torque directly to micro- and nanoscale particles in optical traps has a wide range of applications. While full control of both force and torque in three dimensions has been realized using top-down fabrication of rod-shaped particles composed of birefringent crystalline materials, widespread usage of such particles is limited as the optical constants of the predominant birefringent materials (quartz SiO2 and rutile TiO2) preclude coverage of the full application space of optical trapping. Here, we show that multilayer metamaterial nanoparticles provide access to a wide range of optical constants that can be specifically tuned for each application. Selecting the material pair Nb2O5/SiO2 from the library of amorphous dielectrics as our metamaterial, we show that its refractive index and birefringence can be designed by adapting the ratio of layer thicknesses. Using a robust top-down fabrication process, we show that uniformly sized, free-floating Nb2O5/SiO2 particles with high birefringence at moderate refractive index are obtained at high yield. Using an optical torque wrench, we show that these particles function as joint force and torque transducers while maintaining excellent stability in aqueous solutions and can be controllably optimized for particular physical characteristics such as maximal torque transfer or rapid response time. We expect that such customizable birefringent metamaterial nanoparticles whose properties surpass those of conventional crystalline particles will provide a means to unleash the full potential of optical trapping applications.

RESUMEN

Optical trapping of (sub)micron-sized particles is broadly employed in nanoscience and engineering. The materials commonly employed for these particles, however, have physical properties that limit the transfer of linear or angular momentum (or both). This reduces the magnitude of forces and torques, and the spatiotemporal resolution, achievable in linear and angular traps. Here, we overcome these limitations through the use of single-crystal rutile TiO2, which has an exceptionally large optical birefringence, a high index of refraction, good chemical stability, and is amenable to geometric control at the nanoscale. We show that rutile TiO2 nanocylinders form powerful joint force and torque transducers in aqueous environments by using only moderate laser powers to apply nN·nm torques at kHz rotational frequencies to tightly trapped particles. In doing so, we demonstrate how rutile TiO2 nanocylinders outperform other materials and offer unprecedented opportunities to expand the control of optical force and torque at the nanoscale.

RESUMEN

Single-molecule manipulation techniques have provided unprecedented insights into the structure, function, interactions, and mechanical properties of biological macromolecules. Recently, the single-molecule toolbox has been expanded by techniques that enable measurements of rotation and torque, such as the optical torque wrench (OTW) and several different implementations of magnetic (torque) tweezers. Although systematic analyses of the position and force precision of single-molecule techniques have attracted considerable attention, their angle and torque precision have been treated in much less detail. Here, we propose Allan deviation as a tool to systematically quantitate angle and torque precision in single-molecule measurements. We apply the Allan variance method to experimental data from our implementations of (electro)magnetic torque tweezers and an OTW and find that both approaches can achieve a torque precision better than 1 pN · nm. The OTW, capable of measuring torque on (sub)millisecond timescales, provides the best torque precision for measurement times ≲10 s, after which drift becomes a limiting factor. For longer measurement times, magnetic torque tweezers with their superior stability provide the best torque precision. Use of the Allan deviation enables critical assessments of the torque precision as a function of measurement time across different measurement modalities and provides a tool to optimize measurement protocols for a given instrument and application.

Asunto(s)

RESUMEN

Titanium dioxide (TiO2) is a key component of diverse optical and electronic applications that exploit its exceptional material properties. In particular, the use of TiO2 in its single-crystalline phase can offer substantial advantages over its amorphous and polycrystalline phases for existing and yet-to-be-developed applications. However, the implementation of single-crystal TiO2 has been hampered by challenges in its fabrication and subsequent surface functionalization. Here, we introduce a novel top-down approach that allows for batch fabrication of uniform high-aspect-ratio single-crystal TiO2 nanostructures with targeted sidewall profiles. We complement our fabrication approach with a functionalization strategy that achieves dense, uniform, and area-selective coating with a variety of biomolecules. This allows us to fabricate single-crystal rutile TiO2 nanocylinders tethered with individual DNA molecules for use as force- and torque-transducers in an optical torque wrench. These developments provide the means for increased exploitation of the superior material properties of single-crystal TiO2 at the nanoscale.