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Modular DNA origami-based electrochemical detection of DNA and proteins
Authors:
Byoung-jin Jeon,
Matteo M. Guareschi,
Jaimie M. Stewart,
Emily Wu,
Ashwin Gopinath,
Netzahualcóyotl Arroyo-Currás,
Philippe Dauphin-Ducharme,
Kevin W. Plaxco,
Philip S. Lukeman,
Paul W. K. Rothemund
Abstract:
The diversity and heterogeneity of biomarkers has made the development of general methods for single-step quantification of analytes difficult. For individual biomarkers, electrochemical methods that detect a conformational change in an affinity binder upon analyte binding have shown promise. However, because the conformational change must operate within a nanometer-scale working distance, an enti…
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The diversity and heterogeneity of biomarkers has made the development of general methods for single-step quantification of analytes difficult. For individual biomarkers, electrochemical methods that detect a conformational change in an affinity binder upon analyte binding have shown promise. However, because the conformational change must operate within a nanometer-scale working distance, an entirely new sensor, with a unique conformational change, must be developed for each analyte. Here, we demonstrate a modular electrochemical biosensor, built from DNA origami, which is easily adapted to diverse molecules by merely replacing its analyte binding domains. Instead of relying on a unique nanometer-scale movement of a single redox reporter, all sensor variants rely on the same 100-nanometer scale conformational change, which brings dozens of reporters close enough to a gold electrode surface that a signal can be measured via square wave voltammetry, a standard electrochemical technique. To validate our sensor's mechanism, we used single-stranded DNA as an analyte, and optimized the number of redox reporters and various linker lengths. Adaptation of the sensor to streptavidin and PDGF-BB analytes was achieved by simply adding biotin or anti-PDGF aptamers to appropriate DNA linkers. Geometrically-optimized streptavidin sensors exhibited signal gain and limit of detection markedly better than comparable reagentless electrochemical sensors. After use, the same sensors could be regenerated under mild conditions: performance was largely maintained over four cycles of DNA strand displacement and rehybridization. By leveraging the modularity of DNA nanostructures, our work provides a straightforward route to the single-step quantification of arbitrary nucleic acids and proteins.
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Submitted 28 August, 2024; v1 submitted 11 December, 2023;
originally announced December 2023.
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Scaling of Hybrid QDs-Graphene Photodetectors to Subwavelength Dimension
Authors:
Gökhan Kara,
Patrik Rohner,
Erfu Wu,
Dmitry N. Dirin,
Roman Furrer,
Dimos Poulikakos,
Maksym V. Kovalenko,
Michel Calame,
Ivan Shorubalko
Abstract:
Emerging colloidal quantum dot (cQD) photodetectors currently challenge established state-of-the-art infrared photodetectors in response speed, spectral tunability, simplicity of solution processable fabrication, and integration onto curved or flexible substrates. Hybrid phototransistors based on 2D materials and cQDs, in particular, are promising due to their inherent photogain enabling direct ph…
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Emerging colloidal quantum dot (cQD) photodetectors currently challenge established state-of-the-art infrared photodetectors in response speed, spectral tunability, simplicity of solution processable fabrication, and integration onto curved or flexible substrates. Hybrid phototransistors based on 2D materials and cQDs, in particular, are promising due to their inherent photogain enabling direct photosignal enhancement. The photogain is sensitive to both, measurement conditions and photodetector geometry. This makes the cross-comparison of devices reported in the literature rather involved. Here, the effect of device length L and width W scaling to subwavelength dimensions (sizes down to 500 nm) on the photoresponse of graphene-PbS cQD phototransistors was experimentally investigated. Photogain and responsivity were found to scale with 1/LW, whereas the photocurrent and specific detectivity were independent of geometrical parameters. The measurements were performed at scaled bias voltage conditions for comparable currents. Contact effects were found to limit the photoresponse for devices with L < 3 μm. The relation of gate voltage, bias current, light intensity, and frequency on the photoresponse was investigated in detail, and a photogating efficiency to assess the cQD-graphene interface is presented. In particular, the specific detectivity values in the range between 10^8 to 10^9 Jones (wavelength of 1550 nm, frequency 6 Hz, room temperature) were found to be limited by the charge transfer across the photoactive interface.
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Submitted 8 December, 2023;
originally announced December 2023.
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Synthetic control of structure and conduction properties in Na-Y-Zr-Cl solid electrolytes
Authors:
Elias Sebti,
Ji Qi,
Peter M. Richardson,
Phillip Ridley,
Erik A. Wu,
Swastika Banerjee,
Raynald Giovine,
Ashley Cronk,
So-Yeon Ham,
Ying Shirley Meng,
Shyue Ping Ong,
Raphaële J. Clément
Abstract:
In the development of low cost, sustainable, and energy-dense batteries, chloride-based compounds are promising catholyte materials for solid-state batteries owing to their high Na-ion conductivities and oxidative stabilities. The ability to further improve Na-ion conduction, however, requires an understanding of the impact of long-range and local structural features on transport in these systems.…
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In the development of low cost, sustainable, and energy-dense batteries, chloride-based compounds are promising catholyte materials for solid-state batteries owing to their high Na-ion conductivities and oxidative stabilities. The ability to further improve Na-ion conduction, however, requires an understanding of the impact of long-range and local structural features on transport in these systems. In this study, we leverage different synthesis methods to control polymorphism and cation disorder in Na-Y-Zr-Cl solid electrolytes and interrogate the impact on Na-ion conduction. We demonstrate the existence of a more conductive P2$_1$/n polymorph of Na$_2$ZrCl$_6$ formed upon ball milling. In Na$_3$YCl$_6$, the R$\bar{3}$ polymorph is shown to be more conductive than its P2$_1$/n counterpart owing to the presence of intrinsic vacancies and disorder on the Y sublattice. Transition metal ordering in the Na$_{2.25}$Y$_{0.25}$Zr$_{0.75}$Cl$_6$ composition strongly impacts Na-ion transport, where a greater mixing of Y$^{3+}$ and Zr$^{4+}$ on the transition metal sublattice facilitates ion migration through partial activation of Cl rotations at relevant temperatures. Overall, Na-ion transport sensitively depends on the phases and transition metal distributions stabilized during synthesis. These results are likely generalizable to other halide compositions and indicate that achieving control over the synthetic protocol and resultant structure is key in the pursuit of improved catholytes for high voltage solid-state sodium-ion batteries.
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Submitted 16 August, 2022;
originally announced August 2022.
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The Rendering from the Periodic System of the Elements on the stability, elastic, and electronic properties of M2AC phases
Authors:
Erxiao Wu,
Yiming Zhang,
Mian Li,
Youbing Li,
Kan Luo,
Shiyu Du,
Qing Huang
Abstract:
MAX phases are nanolaminated ternary materials that combine metallic and ceramic properties. Currently, the A-site elements replacement in traditional ones by later transition-metals opens a door to explore new types of MAX phases. In this work, we performed a systematic first-principle study to explore trends in stability, electronic structure and mechanical properties of 288 compositions of M2AX…
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MAX phases are nanolaminated ternary materials that combine metallic and ceramic properties. Currently, the A-site elements replacement in traditional ones by later transition-metals opens a door to explore new types of MAX phases. In this work, we performed a systematic first-principle study to explore trends in stability, electronic structure and mechanical properties of 288 compositions of M2AX phases (M=Ti, V, Cr, Zr, Nb, Mo, Hf, Ta, W; A=Al, Si, P, S, Ga, Ge, As, Se, In, Sn, Sb, Te, Tl, Pb, Bi, Mn, Fe, Co, Ni, Cu, Zn, Tc, Ru, Rh, Pd, Ag, Cd, Os, Ir, Pt, Au, Hg; X=C). Such a dataset, combined with the rigid-band model been applied to most transition metal carbides, shows us the fundamental trends in bonding mechanisms and mechanical properties of MAX phases endowed with the periodic arrangements of M/A-site elements. It worth noting, in particular, the M-A d-d interactions of MAX phases uniquely contribute to the elastic constant C33.
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Submitted 23 November, 2021;
originally announced November 2021.
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Synthesis and thermal expansion of chalcogenide MAX phase Hf2SeC
Authors:
Xudong Wang,
Ke Chen,
Erxiao Wu,
Yiming Zhang,
Haoming Ding,
Nianxiang Qiu,
Yujie Song,
Shiyu Du,
Zhifang Chai,
Qing Huang
Abstract:
Thermal expansion of MAX phases along different directions tended to be different because of the anisotropy of hexagonal crystals. Herein, a new Hf2SeC phase was synthesized and confirmed to be relatively isotropic, whose coefficients of thermal expansion (CTEs) were determined to be 9.73 μK-1 and 10.18 μK-1 along a and c directions. The strong M-S bond endowed Hf2SC and Zr2SC lower CTEs than Hf2S…
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Thermal expansion of MAX phases along different directions tended to be different because of the anisotropy of hexagonal crystals. Herein, a new Hf2SeC phase was synthesized and confirmed to be relatively isotropic, whose coefficients of thermal expansion (CTEs) were determined to be 9.73 μK-1 and 10.18 μK-1 along a and c directions. The strong M-S bond endowed Hf2SC and Zr2SC lower CTEs than Hf2SeC and Zr2SeC. A good relationship between the thermal expansion anisotropy and the ratio of elastic stiffness constant c11 and c33 was established. This straightforward approximation could be used to roughly predict the thermal expansion anisotropy of MAX phases.
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Submitted 16 November, 2021;
originally announced November 2021.
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Carbon Free High Loading Silicon Anodes Enabled by Sulfide Solid Electrolytes for Robust All Solid-State Batteries
Authors:
Darren H. S. Tan,
Yu-Ting Chen,
Hedi Yang,
Wurigumula Bao,
Bhagath Sreenarayanan,
Jean-Marie Doux,
Weikang Li,
Bingyu Lu,
So-Yeon Ham,
Baharak Sayahpour,
Jonathan Scharf,
Erik A. Wu,
Grayson Deysher,
Hyea Eun Han,
Hoe Jin Hah,
Hyeri Jeong,
Zheng Chen,
Ying Shirley Meng
Abstract:
The development of silicon anodes to replace conventional graphite in efforts to increase energy densities of lithium-ion batteries has been largely impeded by poor interfacial stability against liquid electrolytes. Here, stable operation of 99.9 weight% micro-Si (uSi) anode is enabled by utilizing the interface passivating properties of sulfide based solid-electrolytes. Bulk to surface characteri…
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The development of silicon anodes to replace conventional graphite in efforts to increase energy densities of lithium-ion batteries has been largely impeded by poor interfacial stability against liquid electrolytes. Here, stable operation of 99.9 weight% micro-Si (uSi) anode is enabled by utilizing the interface passivating properties of sulfide based solid-electrolytes. Bulk to surface characterization, as well as quantification of interfacial components showed that such an approach eliminates continuous interfacial growth and irreversible lithium losses. In uSi || layered-oxide full cells, high current densities at room temperature (5 mA cm 2), wide operating temperature (-20°C to 80°C) and high loadings (>11 mAh cm-2) were demonstrated for both charge and discharge operations. The promising battery performance can be attributed to both the desirable interfacial property between uSi and sulfide electrolytes, as well as the unique chemo-mechanical behavior of the Li-Si alloys.
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Submitted 6 March, 2021;
originally announced March 2021.
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Stack Pressure Considerations for Room Temperature All-Solid-State Lithium Metal Batteries
Authors:
Jean-Marie Doux,
Han Nguyen,
Darren H. S. Tan,
Abhik Banerjee,
Xuefeng Wang,
Erik A. Wu,
Chiho Jo,
Hedi Yang,
Ying Shirley Meng
Abstract:
All-solid-state batteries are expected to enable batteries with high energy density with the use of lithium metal anodes. Although solid electrolytes are believed to be mechanically strong enough to prevent lithium dendrites from propagating, various reports today still show cell failure due to lithium dendritic growth at room temperature. While cell parameters such as current density, electrolyte…
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All-solid-state batteries are expected to enable batteries with high energy density with the use of lithium metal anodes. Although solid electrolytes are believed to be mechanically strong enough to prevent lithium dendrites from propagating, various reports today still show cell failure due to lithium dendritic growth at room temperature. While cell parameters such as current density, electrolyte porosity and interfacial properties have been investigated, mechanical properties of lithium metal and the role of applied stack pressure on the shorting behavior is still poorly understood. Here, we investigated failure mechanisms of lithium metal in all-solid-state batteries as a function of stack pressure, and conducted in situ characterization of the interfacial and morphological properties of the buried lithium in solid electrolytes. We found that a low stack pressure of 5 MPa allows reliable plating and stripping in a lithium symmetric cell for more than 1000 hours, and a Li | Li6PS5Cl | LiNi0.80Co0.15Al0.05O2 full cell, plating more than 4 um of lithium per charge, is able to cycle over 200 cycles at room temperature. These results suggest the possibility of enabling the lithium metal anode in all-solid-state batteries at reasonable stack pressures.
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Submitted 3 December, 2019; v1 submitted 4 October, 2019;
originally announced October 2019.
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Chirp control of directional current in monolayer graphene by intense few-cycle laser
Authors:
Erheng Wu,
Qiang Zhan,
Zhanshan Wang,
Chaojin Zhang,
Chengpu Liu
Abstract:
The residual current density in monolayer graphene driven by an intense few-cycle chirped laser pulse is investigated via numerical solution of the time-dependent Schrödinger equation. It is found that the residual current is sensitive to the initial chirp rate, and the defined asymmetry degree for current along the different polarization direction versus chirp rate follows a simple sinusoidal fun…
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The residual current density in monolayer graphene driven by an intense few-cycle chirped laser pulse is investigated via numerical solution of the time-dependent Schrödinger equation. It is found that the residual current is sensitive to the initial chirp rate, and the defined asymmetry degree for current along the different polarization direction versus chirp rate follows a simple sinusoidal function. The underlying physical mechanism is the chirp-dependent Landau-Zener-Stückelberg interference. The chirp control of currents provides a novel convenient tool in the petaHertz switching of two-dimensional materials based optoelectronic devices on the sub-femtosecond timescale.
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Submitted 28 May, 2019;
originally announced May 2019.
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Simultaneous Onset of Condensation of Molecules and Atoms in an Attractive Fermi Gas of Atoms
Authors:
Fuxiang Han,
Minghao Lei,
E Wu
Abstract:
The self-consistent equations for the order parameters of Bose-Einstein condensation (BEC) of molecules and Bardeen-Cooper-Schrieffer (BCS) condensation of atoms in a Fermi gas of atoms with an attractive two-body interaction between atoms have been derived within the Hartree-Fock-Bogoliubov approximation from the path integral representation of the grand partition function. We have found that t…
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The self-consistent equations for the order parameters of Bose-Einstein condensation (BEC) of molecules and Bardeen-Cooper-Schrieffer (BCS) condensation of atoms in a Fermi gas of atoms with an attractive two-body interaction between atoms have been derived within the Hartree-Fock-Bogoliubov approximation from the path integral representation of the grand partition function. We have found that the order parameters for BEC and BCS are proportional to each other, which implies that BEC and BCS onsets simultaneously. We have also found that the common critical temperature of BEC and BCS increases as the average number of molecules increases and that the atom-molecule coupling enhances the common critical temperature.
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Submitted 11 October, 2005;
originally announced October 2005.
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Absence of BCS Condensation of Atoms in a Repulsive Fermi Gas of Atoms
Authors:
Fuxiang Han,
Hailing Li,
Minghao Lei,
E Wu
Abstract:
Possible Bose-Einstein condensation of molecules and Bardeen-Cooper-Schrieffer (BCS) condensation of Cooper pairs of atoms in an ultracold Fermi gas of atoms with a repulsive two-body interaction are studied by using the path integral representation of the grand partition function. From the self-consistent equations obtained in the present work for the order parameters, we have found that BCS co…
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Possible Bose-Einstein condensation of molecules and Bardeen-Cooper-Schrieffer (BCS) condensation of Cooper pairs of atoms in an ultracold Fermi gas of atoms with a repulsive two-body interaction are studied by using the path integral representation of the grand partition function. From the self-consistent equations obtained in the present work for the order parameters, we have found that BCS condensation of atoms can't occur in such a Fermi gas of atoms and that the condensate observed experimentally is composed of condensed molecules or possibly of preformed Cooper pairs. To substantiate our conclusions from the self-consistent equations for the order parameters, the effective atom-atom interaction mediated through molecules has also been computed with the Foldy-Wouthuysen transformation and has been found to be repulsive, which implies a net repulsive two-body interaction between atoms and hence the absence of BCS condensation of atoms.
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Submitted 11 October, 2005;
originally announced October 2005.
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Single-photon emission in the near infrared from diamond colour centre
Authors:
E Wu,
V. Jacques,
F. Treussart,
H. Zeng,
P. Grangier,
J. -F. Roch
Abstract:
Optically active colour centres based on Nickel-Nitrogen impurities are observed in natural diamond under continuous-wave excitation. The spectral analysis shows that the single emitters have a narrow-band emission in the near infrared, around 780 nm, which is almost entirely concentrated in the zero phonon line even at room temperature. The colour centre excited-state lifetime is as short as 2…
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Optically active colour centres based on Nickel-Nitrogen impurities are observed in natural diamond under continuous-wave excitation. The spectral analysis shows that the single emitters have a narrow-band emission in the near infrared, around 780 nm, which is almost entirely concentrated in the zero phonon line even at room temperature. The colour centre excited-state lifetime is as short as 2 ns, and the photoluminescence is linear polarized. These striking features pave the way to the realization of a triggered single photon source based on this colour centre emission well suited for open-air single-photon Quantum Key Distribution operating in day-light conditions.
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Submitted 20 September, 2005;
originally announced September 2005.
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Photoluminescence of single colour defects in 50 nm diamond nanocrystals
Authors:
F. Treussart,
V. Jacques,
E. Wu,
T. Gacoin,
P. Grangier,
J. -F. Roch
Abstract:
We used optical confocal microscopy to study optical properties of diamond 50 nm nanocrystals first irradiated with an electron beam, then dispersed as a colloidal solution and finally deposited on a silica slide. At room temperature, under CW laser excitation at a wavelength of 514.5 nm we observed perfectly photostable single Nitrogen-Vacancy (NV) colour defects embedded in the nanocrystals. F…
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We used optical confocal microscopy to study optical properties of diamond 50 nm nanocrystals first irradiated with an electron beam, then dispersed as a colloidal solution and finally deposited on a silica slide. At room temperature, under CW laser excitation at a wavelength of 514.5 nm we observed perfectly photostable single Nitrogen-Vacancy (NV) colour defects embedded in the nanocrystals. From the zero-phonon line around 575 nm in the spectrum of emitted light, we infer a neutral NV0 type of defect. Such nanoparticle with intrinsic fluorescence are highly promising for applications in biology where long-term emitting fluorescent bio-compatible nanoprobes are still missing.
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Submitted 20 September, 2005;
originally announced September 2005.
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Using bond-length dependent transferable force constants to predict vibrational entropies in Au-Cu, Au-Pd, and Cu-Pd alloys
Authors:
Eric J. Wu,
Gerbrand Ceder,
Axel van de Walle
Abstract:
A model is tested to rapidly evaluate the vibrational properties of alloys with site disorder. It is shown that length-dependent transferable force constants exist, and can be used to accurately predict the vibrational entropy of substitutionally ordered and disordered structures in Au-Cu, Au-Pd, and Cu-Pd. For each relevant force constant, a length- dependent function is determined and fitted t…
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A model is tested to rapidly evaluate the vibrational properties of alloys with site disorder. It is shown that length-dependent transferable force constants exist, and can be used to accurately predict the vibrational entropy of substitutionally ordered and disordered structures in Au-Cu, Au-Pd, and Cu-Pd. For each relevant force constant, a length- dependent function is determined and fitted to force constants obtained from first-principles pseudopotential calculations. We show that these transferable force constants can accurately predict vibrational entropies of L1$_{2}$-ordered and disordered phases in Cu$_{3}$Au, Au$_{3}$Pd, Pd$_{3}$Au, Cu$_{3}$Pd, and Pd$_{3}$Au. In addition, we calculate the vibrational entropy difference between L1$_{2}$-ordered and disordered phases of Au$_{3}$Cu and Cu$_{3}$Pt.
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Submitted 5 February, 2003;
originally announced February 2003.