Testing flatness of the universe with probes of cosmic distances and growth

When using distance measurements to probe spatial curvature, the geometric degeneracy between curvature and dark energy in the distance-redshift relation typically requires either making strong assumptions about the dark energy evolution or sacrificing precision in a more model-independent approach. Measurements of the redshift evolution of the linear growth of perturbations can break the geometric degeneracy, providing curvature constraints that are both precise and model-independent. Future supernova, CMB, and cluster data have the potential to measure the curvature with an accuracy of sigma(Omega_K)=0.002, without specifying a particular dark energy phenomenology. In combination with distance measurements, the evolution of the growth function at low redshifts provides the strongest curvature constraint if the high-redshift universe is well approximated as being purely matter dominated. However, in the presence of early dark energy or massive neutrinos, the precision in curvature is reduced due to additional degeneracies, and precise normalization of the growth function relative to recombination is important for obtaining accurate constraints. Curvature limits from distances and growth compare favorably to other approaches to curvature estimation proposed in the literature, providing either greater accuracy or greater freedom from dark energy modeling assumptions, and are complementary due to the use of independent data sets. Model-independent estimates of curvature are critical for both testing inflation and obtaining unbiased constraints on dark energy parameters.Comment: 23 pages, 11 figures; submitted to Phys. Rev.

Active Carboxylic Acid-Terminated Alkanethiol Self-Assembled Monolayers on Gold Bead Electrodes for Immobilization of Cytochromes c

It is extremely difficult to immobilize cytochrome c (cyt c) on carboxylic acid-terminated alkanethiol self-assembled monolayers (HOOC-SAM) on gold bead electrodes prepared in a hydrogen flame. We found that simple pretreatment of a HOOC-SAM/gold bead electrode by potential cycling in buffer solution in the range ±300 mV prior to immobilization of the protein facilitated stable cyt c binding to HOOC-SAMs. The stability of cyt c on the HOOC-SAMs is independent of the topology of the gold surface

Scanning Electrochemical Microscopy of DNA Monolayers Modified with Nile Blue

Scanning electrochemical microscopy (SECM) is used to probe long-range charge transport (CT) through DNA monolayers containing the redox-active Nile Blue (NB) intercalator covalently affixed at a specific location in the DNA film. At substrate potentials negative of the formal potential of covalently attached NB, the electrocatalytic reduction of Fe(CN)63− generated at the SECM tip is observed only when NB is located at the DNA/solution interface; for DNA films containing NB in close proximity to the DNA/electrode interface, the electrocatalytic effect is absent. This behavior is consistent with both rapid DNA-mediated CT between the NB intercalator and the gold electrode as well as a rate-limiting electron transfer between NB and the solution phase Fe(CN)63−. The DNA-mediated nature of the catalytic cycle is confirmed through sequence-specific and localized detection of attomoles of TATA-binding protein, a transcription factor that severely distorts DNA upon binding. Importantly, the strategy outlined here is general and allows for the local investigation of the surface characteristics of DNA monolayers both in the absence and in the presence of DNA binding proteins. These experiments highlight the utility of DNA-modified electrodes as versatile platforms for SECM detection schemes that take advantage of CT mediated by the DNA base pair stack

M–M Bond-Stretching Energy Landscapes for M_2(dimen)_(4)^(2+) (M = Rh, Ir; dimen = 1,8-Diisocyanomenthane) Complexes

Isomers of Ir_2(dimen)_(4)^(2+) (dimen = 1,8-diisocyanomenthane) exhibit different Ir–Ir bond distances in a 2:1 MTHF/EtCN solution (MTHF = 2-methyltetrahydrofuran). Variable-temperature absorption data suggest that the isomer with the shorter Ir–Ir distance is favored at room temperature [K = ~8; ΔH° = −0.8 kcal/mol; ΔS° = 1.44 cal mol^(–1) K^(–1)]. We report calculations that shed light on M_2(dimen)_(4)^(2+) (M = Rh, Ir) structural differences: (1) metal–metal interaction favors short distances; (2) ligand deformational-strain energy favors long distances; (3) out-of-plane (A_(2u)) distortion promotes twisting of the ligand backbone at short metal–metal separations. Calculated potential-energy surfaces reveal a double minimum for Ir_2(dimen)_(4)^(2+) (4.1 Å Ir–Ir with 0° twist angle and ~3.6 Å Ir–Ir with ±12° twist angle) but not for the rhodium analogue (4.5 Å Rh–Rh with no twisting). Because both the ligand strain and A_(2u) distortional energy are virtually identical for the two complexes, the strength of the metal–metal interaction is the determining factor. On the basis of the magnitude of this interaction, we obtain the following results: (1) a single-minimum (along the Ir–Ir coordinate), harmonic potential-energy surface for the triplet electronic excited state of Ir_2(dimen)_(4)^(2+) (R_(e,Ir–Ir) = 2.87 Å; F_(Ir–Ir) = 0.99 mdyn Å^(–1)); (2) a single-minimum, anharmonic surface for the ground state of Rh_2(dimen)_(4)^(2+) (R_(e,Rh–Rh) = 3.23 Å; F_(Rh–Rh) = 0.09 mdyn Å^(–1)); (3) a double-minimum (along the Ir–Ir coordinate) surface for the ground state of Ir_2(dimen)_(4)^(2+) (R_(e,Ir–Ir) = 3.23 Å; F_(Ir–Ir) = 0.16 mdyn Å^(–1))

Design and fabrication of highly efficient non-linear optical devices for implementing high-speed optical processing

We present the design and fabrication of micro-cavity semiconductor devices for enhanced Two-Photon-Absorption response, and demonstrate the use of these devices for implementing sensitive autocorrelation measurements on pico-second optical pulses

High-sensitivity two-photon absorption microcavity autocorrelator

A GaAs-AlAs microcavity device has been used as a photodetector in an autocorrelator for measuring the temporal pulsewidth of 1.5-/spl mu/m optical pulses. Enhancement of the two-photon absorption photocurrent due to the microcavity structure results in an autocorrelation (average power times peak power) sensitivity of 9.3/spl times/10/sup -4/ (mW)/sup 2/, which represents two orders of magnitude improvement when compared with conventional autocorrelators

Two-photon absorption in microcavities for optical autocorrelation and sampling

We have designed novel semiconductor microcavity structures for the enhancement of the two-photon absorption (TPA) photocurrent. We report a TPA autocorrelation technique for short optical pulses that uses the microcavity structure instead of a second harmonic generation crystal. Knowledge of these characteristics is important for implementation in applications such as optical switching and sampling in optical time division multiplexed (OTDM) communications systems

DNA-Modified Electrodes Fabricated Using Copper-Free Click Chemistry for Enhanced Protein Detection

A method of DNA monolayer formation has been developed using copper-free click chemistry that yields enhanced surface homogeneity and enables variation in the amount of DNA assembled; extremely low-density DNA monolayers, with as little as 5% of the monolayer being DNA, have been formed. These DNA-modified electrodes (DMEs) were characterized visually, with AFM, and electrochemically, and were found to facilitate DNA-mediated reduction of a distally bound redox probe. These low-density monolayers were found to be more homogeneous than traditional thiol-modified DNA monolayers, with greater helix accessibility through an increased surface area-to-volume ratio. Protein binding efficiency of the transcriptional activator TATA-binding protein (TBP) was also investigated on these surfaces and compared to that on DNA monolayers formed with standard thiol-modified DNA. Our low-density monolayers were found to be extremely sensitive to TBP binding, with a signal decrease in excess of 75% for 150 nM protein. This protein was detectable at 4 nM, on the order of its dissociation constant, with our low-density monolayers. The improved DNA helix accessibility and sensitivity of our low-density DNA monolayers to TBP binding reflects the general utility of this method of DNA monolayer formation for DNA-based electrochemical sensor development