skip to main content


Title: Mono- and bilayer smectic liquid crystal ordering in dense solutions of “gapped” DNA duplexes

Although its mesomorphic properties have been studied for many years, only recently has the molecule of life begun to reveal the true range of its rich liquid crystalline behavior. End-to-end interactions between concentrated, ultrashort DNA duplexes—driving the self-assembly of aggregates that organize into liquid crystal phases—and the incorporation of flexible single-stranded “gaps” in otherwise fully paired duplexes—producing clear evidence of an elementary lamellar (smectic-A) phase in DNA solutions—are two exciting developments that have opened avenues for discovery. Here, we report on a wider investigation of the nature and temperature dependence of smectic ordering in concentrated solutions of various “gapped” DNA (GDNA) constructs. We examine symmetric GDNA constructs consisting of two 48-base pair duplex segments bridged by a single-stranded sequence of 2 to 20 thymine bases. Two distinct smectic layer structures are observed for DNA concentration in the range230to280mg/mL. One exhibits an interlayer periodicity comparable with two-duplex lengths (“bilayer” structure), and the other has a period similar to a single-duplex length (“monolayer” structure). The bilayer structure is observed for gap length ≳10 bases and melts into the cholesteric phase at a temperature between 30 °C and 35 °C. The monolayer structure predominates for gap length ≲10 bases and persists to>40°C. We discuss models for the two layer structures and mechanisms for their stability. We also report results for asymmetric gapped constructs and for constructs with terminal overhangs, which further support the model layer structures.

 
more » « less
Award ID(s):
2005212
NSF-PAR ID:
10217803
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
Proceedings of the National Academy of Sciences
Date Published:
Journal Name:
Proceedings of the National Academy of Sciences
Volume:
118
Issue:
12
ISSN:
0027-8424
Page Range / eLocation ID:
Article No. e2019996118
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    The sensitivity of urban canopy air temperature (Ta) to anthropogenic heat flux (QAH) is known to vary with space and time, but the key factors controlling such spatiotemporal variabilities remain elusive. To quantify the contributions of different physical processes to the magnitude and variability ofΔTa/ΔQAH(whereΔrepresents a change), we develop a forcing-feedback framework based on the energy budget of air within the urban canopy layer and apply it to diagnosingΔTa/ΔQAHsimulated by the Community Land Model Urban over the contiguous United States (CONUS). In summer, the medianΔTa/ΔQAHis around 0.01K W m21over the CONUS. Besides the direct effect ofQAHonTa, there are important feedbacks through changes in the surface temperature, the atmosphere–canopy air heat conductance (ca), and the surface–canopy air heat conductance. The positive and negative feedbacks nearly cancel each other out andΔTa/ΔQAHis mostly controlled by the direct effect in summer. In winter,ΔTa/ΔQAHbecomes stronger, with the median value increased by about 20% due to weakened negative feedback associated withca. The spatial and temporal (both seasonal and diurnal) variability ofΔTa/ΔQAHas well as the nonlinear response ofΔTatoΔQAHare strongly related to the variability ofca, highlighting the importance of correctly parameterizing convective heat transfer in urban canopy models.

     
    more » « less
  2. Abstract

    Broken symmetries in topological condensed matter systems have implications for the spectrum of Fermionic excitations confined on surfaces or topological defects. The Fermionic spectrum of confined (quasi-2D)3He-A consists of branches of chiral edge states. The negative energy states are related to the ground-state angular momentum,Lz=(N/2), forN/2Cooper pairs. The power law suppression of the angular momentum,Lz(T)(N/2)[123(πT/Δ)2]for0TTc, in the fully gapped 2D chiral A-phase reflects the thermal excitation of the chiral edge Fermions. We discuss the effects of wave function overlap, and hybridization between edge states confined near opposing edge boundaries on the edge currents, ground-state angular momentum and ground-state order parameter of superfluid3He thin films. Under strong lateral confinement, the chiral A phase undergoes a sequence of phase transitions, first to a pair density wave (PDW) phase with broken translational symmetry atDc216ξ0. The PDW phase is described by a periodic array of chiral domains with alternating chirality, separated by domain walls. The period of PDW phase diverges as the confinement lengthDDc2. The PDW phase breaks time-reversal symmetry, translation invariance, but is invariant under the combination of time-reversal and translation by a one-half period of the PDW. The mass current distribution of the PDW phase reflects this combined symmetry, and originates from the spectra of edge Fermions and the chiral branches bound to the domain walls. Under sufficiently strong confinement a second-order transition occurs to the non-chiral ‘polar phase’ atDc19ξ0, in which a single p-wave orbital state of Cooper pairs is aligned along the channel.

     
    more » « less
  3. Abstract

    The interplay between charge transfer and electronic disorder in transition-metal dichalcogenide multilayers gives rise to superconductive coupling driven by proximity enhancement, tunneling and superconducting fluctuations, of a yet unwieldy variety. Artificial spacer layers introduced with atomic precision change the density of states by charge transfer. Here, we tune the superconductive coupling betweenNbSe2monolayers from proximity-enhanced to tunneling-dominated. We correlate normal and superconducting properties inSnSe1+δmNbSe21tailored multilayers with varying SnSe layer thickness (m=115). From high-field magnetotransport the critical fields yield Ginzburg–Landau coherence lengths with an increase of140%cross-plane (m=19), trending towards two-dimensional superconductivity form>9. We show cross-overs between three regimes: metallic with proximity-enhanced coupling (m=14), disordered-metallic with intermediate coupling (m=59) and insulating with Josephson tunneling (m>9). Our results demonstrate that stacking metal mono- and dichalcogenides allows to convert a metal/superconductor into an insulator/superconductor system, prospecting the control of two-dimensional superconductivity in embedded layers.

     
    more » « less
  4. Abstract

    The formation and evolution of post-solitons has been discussed for quite some time both analytically and through the use of particle-in-cell (PIC) codes. It is however only recently that they have been directly observed in laser-plasma experiments. Relativistic electromagnetic (EM) solitons are localised structures that can occur in collisionless plasmas. They consist of a low-frequency EM wave trapped in a low electron number-density cavity surrounded by a shell with a higher electron number-density. Here we describe the results of an experiment in which a 100 TW Ti:sapphire laser (30 fs, 800 nm) irradiates a0.03gcm3TMPTA foam target with a focused intensityIl=9.5×1017Wcm2. A third harmonic (λprobe266nm) probe is employed to diagnose plasma motion for 25 ps after the main pulse interaction via Doppler-Spectroscopy. Both radiation-hydrodynamics and 2D PIC simulations are performed to aid in the interpretation of the experimental results. We show that the rapid motion of the probe critical-surface observed in the experiment might be a signature of post-soliton wall motion.

     
    more » « less
  5. The negatively charged silicon monovacancyVSiin 4H silicon carbide (SiC) is a spin-active point defect that has the potential to act as a qubit in solid-state quantum information applications. Photonic crystal cavities (PCCs) can augment the optical emission of theVSi, yet fine-tuning the defect–cavity interaction remains challenging. We report on two postfabrication processes that result in enhancement of theV1optical emission from our PCCs, an indication of improved coupling between the cavity and ensemble of silicon vacancies. Below-bandgap irradiation at 785-nm and 532-nm wavelengths carried out at times ranging from a few minutes to several hours results in stable enhancement of emission, believed to result from changing the relative ratio ofVSi0(“dark state”) toVSi(“bright state”). The much faster change effected by 532-nm irradiation may result from cooperative charge-state conversion due to proximal defects. Thermal annealing at 100 °C, carried out over 20 min, also results in emission enhancements and may be explained by the relatively low-activation energy diffusion of carbon interstitialsCi, subsequently recombining with other defects to create additionalVSis. These PCC-enabled experiments reveal insights into defect modifications and interactions within a controlled, designated volume and indicate pathways to improved defect–cavity interactions.

     
    more » « less