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Shyamsunder Erramilli

Publications and source records attributed to Shyamsunder Erramilli.

At least 19 recordsLinked to original sources

Radio Frequency Field-Induced Enhancement of Detection Sensitivity in Silicon Nanowire Sensors

Sensitive biomarker detection in physiological fluids is often limited by Debye screening, which suppresses electrostatic signals at sensor surfaces. Here we report a sensing approach based on flexoelectric resonance in silicon nanowire field-effect transistors. An applied radiofrequency field induces strain gradients in the nanowires, generating flexoelectric polarization that is amplified at resonant frequencies. This effect enhances the sensitivity of conductance measurements to small surface charge variations associated with biomolecular binding. Using C-reactive protein as a model biomarker, we observe an order-of-magnitude improvement in detection sensitivity compared to conventional operation, with a 62% conductance increase versus 30% without radiofrequency modulation. The high-frequency field also perturbs the electrical double layer, reducing Debye screening in high-ionic-strength environments. These combined effects enable direct biomarker detection without sample dilution. This work establishes flexoelectric resonance as a general strategy for improving nanoscale biosensing performance in physiologically relevant conditions.

cond-mat.mtrl-sci

Widefield pump-probe microscopy with coherent background subtraction by angle-compensated temporal shearing

Pump-probe microscopy enables label-free imaging of structural and chemical features of samples. However, signals in pump-probe microscopy are typically small and often must be measured in the presence of large backgrounds. As a result, achieving measurements with a high signal-to-noise ratio is challenging, particularly when using sensors that are easily saturated, such as CMOS cameras. We present a method for enhancing signal-to-noise ratio while avoiding detector saturation. In this approach, temporally separated (sheared) reference and probe pulses transmit through a sample before and after the arrival of a pump pulse. The probe and reference pulses are then temporally recombined with opposing phases and nearly matched amplitudes, resulting in interferometric background subtraction. This recombining operation is performed by a novel common-path interferometer. Unlike previous techniques for temporal shearing, this interferometer demonstrates negligible phase and group delay dispersion with angle of incidence, allowing convenient widefield imaging. To our knowledge, this is the first common-path interferometer with such a property. We demonstrate the technique by measuring transient absorption signals in gold nanorod films with a signal-to-background ratio enhanced by over 100% and a signal-to-noise ratio enhanced by about 70%.

physics.optics

Energy Relaxation of N$_2$O in Gaseous, Supercritical and Liquid Xenon and SF$_6$

Rotational and vibrational energy relaxation (RER and VER) of N$_2$O embedded in xenon and SF$_6$ environments ranging from the gas phase to the liquid, including the supercritical regime, is studied at a molecular level. Calibrated intermolecular interactions from high-level electronic structure calculations, validated against experiments for the pure solvents were used to carry out classical molecular dynamics simulations corresponding to experimental state points for near-critical isotherms. Computed RER rates in low-density solvent of $k_{\rm rot}^{\rm Xe} = (3.67\pm0.25)\cdot10^{10}$ s$^{-1}$M$^{-1}$ and $k_{\rm rot}^{\rm SF_6} = (1.25\pm0.12)\cdot10^{11}$ s$^{-1}$M$^{-1}$ compare well with rates determined by analysis of 2-dimensional infrared experiments. Simulations find that an isolated binary collision (IBC) description is successful up to solvent concentrations of $\sim 4$ M. For higher densities, including the supercritical regime, the simulations do not correctly describe RER, probably due to neglect of solvent-solute coupling in the analysis of the rotational motion. For VER, the near-quantitative agreement between simulations and pump-probe experiments captures the solvent density-dependent trends.

physics.chem-ph

Molecular-Level Understanding of the Ro-vibrational Spectra of N$_2$O in Gaseous, Supercritical and Liquid SF$_6$ and Xe

The transition between the gas-, supercritical-, and liquid-phase behaviour is a fascinating topic which still lacks molecular-level understanding. Recent ultrafast two-dimensional infrared spectroscopy experiments suggested that the vibrational spectroscopy of N$_2$O embedded in xenon and SF$_6$ as solvents provides an avenue to characterize the transitions between different phases as the concentration (or density) of the solvent increases. The present work demonstrates that classical molecular dynamics simulations together with accurate interaction potentials allows to (semi-)quantitatively describe the transition in rotational vibrational infrared spectra from the P-/R-branch lineshape for the stretch vibrations of N$_2$O at low solvent densities to the Q-branch-like lineshapes at high densities. The results are interpreted within the classical theory of rigid-body rotation in more/less constraining environments at high/low solvent densities or based on phenomenological models for the orientational relaxation of rotational motion. It is concluded that classical MD simulations provide a powerful approach to characterize and interpret the ultrafast motion of solutes in low to high density solvents at a molecular level.

physics.chem-ph

Flatfield Ultrafast Imaging with Single-Shot Non-Synchronous Array Photography

We present a method for acquiring a sequence of time-resolved images in a single shot, called Single-Shot Non-Synchronous Array Photography (SNAP). In SNAP, a pulsed laser beam is split by a diffractive optical element into an array of angled beamlets whose illumination fronts remain perpendicular to the optical axis. Different time delays are imparted to each beamlet by an echelon, enabling them to probe a scene in rapid succession. The beamlets are then imaged onto different regions of a camera by a lenslet array. Because the illumination fronts remain flat (head-on) independently of beamlet angle, the temporal resolution of SNAP is fundamentally limited only by the laser pulse duration, akin to a "global shutter" in conventional imaging. We demonstrate SNAP by capturing the evolution of a laser induced plasma filament for 20 frames at an average rate of 4.2 Tfps.

physics.optics

Resonant Gold Nanoparticles Achieve Plasmon-Enhanced Pan-Microbial Pathogen Inactivation in the Shockwave Regime

Pan-microbial inactivation technologies that do not require high temperatures, reactive chemical compounds, or UV radiation could address gaps in current infection control strategies and provide efficient sterilization of biologics in the biotechnological industry. Here, we demonstrate that femtosecond (fs) laser irradiation of resonant gold nanoparticles (NPs) under conditions that allow for E-field mediated cavitation and shockwave generation achieve an efficient plasmon-enhanced photonic microbial pathogen inactivation. We demonstrate that this NP-enhanced, physical inactivation approach is effective against a diverse group of pathogens, including both enveloped and non-enveloped viruses, and a variety of bacteria and mycoplasma. Photonic inactivation is wavelength-dependent and in the absence of plasmonic enhancement from NPs, negligible levels of microbial inactivation are observed in the near-infrared (NIR) at 800 nm. This changes upon addition of resonant plasmonic NPs, which provide a strong enhancement of inactivation of viral and bacterial contaminants. Importantly, the plasmon-enhanced 800 nm femtosecond (fs)-pulse induced inactivation was selective to pathogens. No measurable damage was observed for antibodies included as representative biologics under identical conditions.

physics.bio-ph

Femtosecond Photonic Viral Inactivation Probed Using Solid-State Nanopores

We report on the detection of inactivation of virus particles using femtosecond laser radiation by measuring the conductance of a solid state nanopore designed for detecting single virus particles. Conventional methods of assaying for viral inactivation based on plaque forming assays require 24-48 hours for bacterial growth. Nanopore conductance measurements provide information on morphological changes at a single virion level. We show that analysis of a time series of nanopore conductance can quantify the detection of inactivation, requiring only a few minutes from collection to analysis. Morphological changes were verified by Dynamic Light Scattering (DLS). Statistical analysis maximizing the information entropy provides a measure of the Log-reduction value. Taken together, our work provides a rapid method for assaying viral inactivation with femtosecond lasers using solid-state nanopores.

physics.bio-ph

Measurement of nonlinear piezoelectric coefficients using a micromechanical resonator

We describe and demonstrate a method by which the nonlinear piezoelectric properties of a piezoelectric material may be measured by detecting the force that it applies on a suspended micromechanical resonator at one of its mechanical resonance frequencies. Resonators are used in countless applications; this method could provide a means for better-characterizing material behaviors within real MEMS devices. Further, special devices can be designed to probe this nonlinear behavior at specific frequencies with enhanced signal sizes. The resonators used for this experiment are actuated using a 1-$μ$m-thick layer of aluminum nitride. When driven at large amplitudes, the piezoelectric layer generates harmonics, which are measurable in the response of the resonator. In this experiment, we measured the second-order piezoelectric coefficient of aluminum nitride to be $-(23.1\pm14.1)\times10^{-22}\ \mathrm{m/V^2}$.

physics.app-ph

Wireless transfer of power by a 35-GHz metamaterial split-ring resonator rectenna

Wireless transfer of power via high frequency microwave radiation using a miniature split ring resonator rectenna is reported. RF power is converted into DC power by integrating a rectification circuit with the split ring resonator. The near-field behavior of the rectenna is investigated with microwave radiation in the frequency range between 20-40 GHz with a maximum power level of 17 dBm. The observed resonance peaks match those predicted by simulation. Polarization studies show the expected maximum in signal when the electric field is polarized along the edge of the split ring resonator with the gap and minimum for perpendicular orientation. The efficiency of the rectenna is on the order of 1% for a frequency of 37.2 GHz. By using a cascading array of 9 split ring resonators the output power was increased by a factor of 20.

physics.ins-det

Perspective: Melanoma diagnosis and monitoring: Sunrise for melanoma therapy but early detection remains in the shade

Melanoma is one of the most dangerous forms of cancer. The five-year survival rate is 98% if it is detected early. However, this rate plummets to 63% for regional disease and 17% when tumors have metastasized, that is, spread to distant sites. Furthermore, the incidence of melanoma has been rising by about 3% per year, whereas the incidence of cancers that are more common is decreasing. A handful of targeted therapies have recently become available that have finally shown real promise for treatment, but for reasons that remain unclear only a fraction of patients respond long term. These drugs often increase survival by only a few months in metastatic patient groups before relapse occurs. More effective treatment may be possible if a diagnosis can be made when the tumor burden is still low. Here, an overview of the current state-of-the-art is provided along with an argument for newer technologies towards early point-of-care diagnosis of melanoma.

q-bio.TO

Field Effect Transistor Nanosensor for Breast Cancer Diagnostics

Silicon nanochannel field effect transistor (FET) biosensors are one of the most promising technologies in the development of highly sensitive and label-free analyte detection for cancer diagnostics. With their exceptional electrical properties and small dimensions, silicon nanochannels are ideally suited for extraordinarily high sensitivity. In fact, the high surface-to-volume ratios of these systems make single molecule detection possible. Further, FET biosensors offer the benefits of high speed, low cost, and high yield manufacturing, without sacrificing the sensitivity typical for traditional optical methods in diagnostics. Top down manufacturing methods leverage advantages in Complementary Metal Oxide Semiconductor (CMOS) technologies, making richly multiplexed sensor arrays a reality. Here, we discuss the fabrication and use of silicon nanochannel FET devices as biosensors for breast cancer diagnosis and monitoring.

q-bio.QM

Detection of the melanoma biomarker TROY using silicon nanowire field-effect transistors

Antibody-functionalized silicon nanowire field-effect transistors have been shown to exhibit excellent analyte detection sensitivity enabling sensing of analyte concentrations at levels not readily accessible by other methods. One example where accurate measurement of small concentrations is necessary is detection of serum biomarkers, such as the recently discovered tumor necrosis factor receptor superfamily member TROY (TNFRSF19), which may serve as a biomarker for melanoma. TROY is normally only present in brain but it is aberrantly expressed in primary and metastatic melanoma cells and shed into the surrounding environment. In this study, we show the detection of different concentrations of TROY in buffer solution using top-down fabricated silicon nanowires. We demonstrate the selectivity of our sensors by comparing the signal with that obtained from bovine serum albumin in buffer solution. Both the signal size and the reaction kinetics serve to distinguish the two signals. Using a fast-mixing two-compartment reaction model, we are able to extract the association and dissociation rate constants for the reaction of TROY with the antibody immobilized on the sensor surface.

q-bio.QM

Pitchfork Bifurcation and Zharov Splitting in Nonlinear Mid-infrared Photothermal Spectroscopy in a liquid crystal using a Quantum Cascade Laser

We report on the mid-infrared nonlinear photothermal spectrum of the neat liquid crystal 4-Octyl-4'-Cyanobiphenyl (8CB) using a tunable Quantum Cascade Laser (QCL). The nonequilibrium steady state characterized by the nonlinear photothermal infrared response undergoes a supercritical pitchfork bifurcation. The bifurcation, observed in heterodyne two-color pump-probe detection, leads to ultrasharp nonlinear infrared spectra similar to those reported in the visible region. A systematic study of the peak splitting as function of absorbed infrared power shows the bifurcation has a critical exponent of 0.5. The surprising observation of an apparently universal critical exponent in a nonequilibrium state is explained using a simple model reminiscent of mean field theory. Apart from the intrinsic interest for nonequilibrium studies, nonlinear photothermal methods lead to a dramatic narrowing of spectral lines, giving rise to a potential new contrast mechanism for the rapidly emerging new field of mid-infrared microspectroscopy using QCLs.

physics.optics

Surface modified silicon nanochannel for urea sensing

Silicon nanowires have been surface functionalized with the enzyme urease for biosensor applications to detect and quantify urea concentration. The device is nanofabricated from a silicon on insulator (SOI) wafer with a top down lithography approach. The differential conductance of silicon nanowires can be tuned for optimum performance using the source drain bias voltage, and is sensitive to urea at low concentration. The experimental results show a linear relationship between surface potential change and urea concentration in the range of 0.1 to 0.68 mM. The sensitivity of our devices shows high reproducibility with time and different measurement conditions. The nanowire urea biosensor offers the possibility of high quality, reusable enzyme sensor array integration with silicon based circuits.

physics.bio-ph

Channel-Width Dependent Enhancement in Nanoscale Field Effect Transistor

We report the observation of channel-width dependent enhancement in nanoscale field effect transistors containing lithographically-patterned silicon nanowires as the conduction channel. These devices behave as conventional metal-oxide-semiconductor field-effect transistors in reverse source drain bias. Reduction of nanowire width below 200 nm leads to dramatic change in the threshold voltage. Due to increased surface-to-volume ratio, these devices show higher transconductance per unit width at smaller width. Our devices with nanoscale channel width demonstrate extreme sensitivity to surface field profile, and therefore can be used as logic elements in computation and as ultrasensitive sensors of surface-charge in chemical and biological species.

cond-mat.other

Nanoscale field effect transistor for biomolecular signal amplification

We report amplification of biomolecular recognition signal in lithographically defined silicon nanochannel devices. The devices are configured as field effect transistors (FET) in the reversed source-drain bias region. The measurement of the differential conductance of the nanowire channels in the FET allows sensitive detection of changes in the surface potential due to biomolecular binding. Narrower silicon channels demonstrate higher sensitivity to binding due to increased surface-to-volume ratio. The operation of the device in the negative source-drain region demonstrates signal amplification. The equivalence between protein binding and change in the surface potential is described.

physics.bio-ph

Silicon-based nanochannel glucose sensor

Silicon nanochannel biological field effect transistors have been developed for glucose detection. The device is nanofabricated from a silicon-on-insulator wafer with a top-down approach and surface functionalized with glucose oxidase. The differential conductance of silicon nanowires, tuned with source-drain bias voltage, is demonstrated to be sensitive to the biocatalyzed oxidation of glucose. The glucose biosensor response is linear in the 0.5-8 mM concentration range with 3-5 min response time. This silicon nanochannel-based glucose biosensor technology offers the possibility of high density, high quality glucose biosensor integration with silicon-based circuitry.

physics.bio-ph

Vibrational Infrared Lifetime of the Anesthetic nitrous oxide gas in solution

The lifetime of the asymmetric fundamental stretching 2218 cm$^{-1}$ vibration of the anesthetic gas nitrous oxide (N$_2$O) dissolved in octanol and olive oil is reported. These solvents are model systems commonly used to assess anesthetic potency. Picosecond time-scale molecular dynamics simulations have suggested that protein dynamics or membrane dynamics play a role in the molecular mechanism of anesthetic action. Ultrafast infrared spectroscopy with 100 fs time resolution is an ideal tool to probe dynamics of anesthetic molecules on such timescales. Pump-probe studies at the peak of the vibrational band yield a lifetime of $55 \pm 1$ ps in olive oil and $52 \pm 1 ps$ in octanol. The similarity of lifetimes suggests that energy relaxation of the anesthetic is determined primarily by the hydrophobic nature of the environment, consistent with models of anesthetic action. The results show that nitrous oxide is a good model system for probing anesthetic-solvent interactions using nonlinear infrared spectroscopy.

physics.bio-ph