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1.
Chem Sci ; 15(19): 7170-7177, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38756816

ABSTRACT

Modern technology demands miniaturization of electronic components to build small, light, and portable devices. Hence, discovery and synthesis of new non-toxic, low cost, ultra-thin ferroelectric materials having potential applications in various electronic and optoelectronic devices are of paramount importance. However, achieving room-temperature ferroelectricity in two dimensional (2D) ultra-thin systems remains a major challenge as conventional three-dimensional ferroelectric materials lose their ferroelectricity when the thickness is brought down below a critical value owing to the depolarization field. Herein, we report room-temperature ferroelectricity in ultra-thin single-crystalline 2D nanosheets of Bi2O2S synthesized by a simple, rapid, and scalable solution-based soft chemistry method. The ferroelectric ground state of Bi2O2S nanosheets is confirmed by temperature-dependent dielectric measurements as well as piezoelectric force microscopy and spectroscopy. High resolution transmission electron microscopy analysis and density functional theory-based calculations suggest that the ferroelectricity in Bi2O2S nanosheets arises due to the local distortion of Bi2O2 layers, which destroys the local inversion symmetry of Bi2O2S.

2.
Sci Rep ; 11(1): 21030, 2021 Oct 26.
Article in English | MEDLINE | ID: mdl-34702967

ABSTRACT

Superconducting crystals with a lack of inversion symmetry can potentially host unconventional pairing. However, till today, no direct conclusive experimental evidence of such unconventional order parameters in non-centrosymmetric superconductors has been reported. In this paper, through direct measurement of the superconducting energy gap by scanning tunnelling spectroscopy, we report the existence of both s-wave (singlet) and p-wave (triplet) pairing symmetries in non-centrosymmetric Ru[Formula: see text]B[Formula: see text]. Our temperature and magnetic field-dependent studies also indicate that the relative amplitudes of the singlet and triplet components change differently with temperature.

3.
Sci Rep ; 11(1): 17190, 2021 Aug 25.
Article in English | MEDLINE | ID: mdl-34433850

ABSTRACT

A remarkable decrease in the lattice thermal conductivity and enhancement of thermoelectric figure of merit were recently observed in rock-salt cubic SnTe, when doped with germanium (Ge). Primarily, based on theoretical analysis, the decrease in lattice thermal conductivity was attributed to local ferroelectric fluctuations induced softening of the optical phonons which may strongly scatter the heat carrying acoustic phonons. Although the previous structural analysis indicated that the local ferroelectric transition temperature would be near room temperature in [Formula: see text], a direct evidence of local ferroelectricity remained elusive. Here we report a direct evidence of local nanoscale ferroelectric domains and their switching in [Formula: see text] using piezoeresponse force microscopy(PFM) and switching spectroscopy over a range of temperatures near the room temperature. From temperature dependent (250-300 K) synchrotron X-ray pair distribution function (PDF) analysis, we show the presence of local off-centering distortion of Ge along the rhombohedral direction in global cubic [Formula: see text]. The length scale of the [Formula: see text] off-centering is 0.25-0.10 Å near the room temperatures (250-300 K). This local emphatic behaviour of cation is the cause for the observed local ferroelectric instability, thereby low lattice thermal conductivity in [Formula: see text].

4.
J Phys Condens Matter ; 33(25)2021 May 21.
Article in English | MEDLINE | ID: mdl-33857934

ABSTRACT

Novel electronic systems displaying exotic physical properties can be derived from complex topological materials through chemical doping. MoTe2, the candidate type-II Weyl semimetal shows dramatically enhanced superconductivity up to 4.1 K upon Re doping in Mo sites. Based on bulk transport and local scanning tunnelling microscopy here we show that Re doping also leads to the emergence of a possible charge density wave phase in Re0.2Mo0.8Te2. In addition, the tunnellingI-Vcharacteristics display non-linearity and hysteresis which is commensurate with a hysteresis observed in the change in tip-height (z) as a function of applied voltageV. The observations indicate an electric field induced hysteretic switching consistent with piezoelectricity and possible ferroelectricity.

5.
Angew Chem Int Ed Engl ; 60(18): 10350-10358, 2021 Apr 26.
Article in English | MEDLINE | ID: mdl-33619797

ABSTRACT

Orthorhombic GeSe is a promising thermoelectric material. However, large band gap and strong covalent bonding result in a low thermoelectric figure of merit, zT≈0.2. Here, we demonstrate a maximum zT≈1.35 at 627 K in p-type polycrystalline rhombohedral (GeSe)0.9 (AgBiTe2 )0.1 , which is the highest value reported among GeSe based materials. The rhombohedral phase is stable in ambient conditions for x=0.8-0.29 in (GeSe)1-x (AgBiTe2 )x . The structural transformation accompanies change from covalent bonding in orthorhombic GeSe to metavalent bonding in rhombohedral (GeSe)1-x (AgBiTe2 )x . (GeSe)0.9 (AgBiTe2 )0.1 has closely lying primary and secondary valence bands (within 0.25-0.30 eV), which results in high power factor 12.8 µW cm-1 K-2 at 627 K. It also exhibits intrinsically low lattice thermal conductivity (0.38 Wm-1 K-1 at 578 K). Theoretical phonon dispersion calculations reveal vicinity of a ferroelectric instability, with large anomalous Born effective charges and high optical dielectric constant, which, in concurrence with high effective coordination number, low band gap and moderate electrical conductivity, corroborate metavalent bonding in (GeSe)0.9 (AgBiTe2 )0.1 . We confirmed the presence of low energy phonon modes and local ferroelectric domains using heat capacity measurement (3-30 K) and switching spectroscopy in piezoresponse force microscopy, respectively.

6.
Sci Rep ; 11(1): 4090, 2021 Feb 18.
Article in English | MEDLINE | ID: mdl-33603100

ABSTRACT

The superconducting systems emerging from topological insulators upon metal ion intercalation or application of high pressure are ideal for investigation of possible topological superconductivity. In this context, Sr-intercalated Bi[Formula: see text]Se[Formula: see text] is specially interesting because it displays pressure induced re-entrant superconductivity where the high pressure phase shows almost two times higher [Formula: see text] than the ambient superconducting phase ( [Formula: see text] K). Interestingly, unlike the ambient phase, the pressure-induced superconducting phase shows strong indication of unconventional superconductivity. However, since the pressure-induced phase remains inaccessible to spectroscopic techniques, the detailed study of the phase remained an unattained goal. Here we show that the high-pressure phase can be realized under a mesoscopic point contact, where transport spectroscopy can be used to probe the spectroscopic properties of the pressure-induced phase. We find that the point contact junctions on the high-pressure phase show unusual response to magnetic field supporting the possibility of unconventional superconductivity.

7.
J Phys Condens Matter ; 32(31): 315701, 2020 Feb 25.
Article in English | MEDLINE | ID: mdl-32097894

ABSTRACT

Recently RuB2 was shown to be a possible two-gap, type-I superconductor. Temperature dependent heat capacity measurements revealed a two-gap superconducting ground state, while magnetic field dependent magnetization measurements indicated surprizing type-I superconductivity with a very low experimental critical field (H c) ∼120 Oe. In this paper, we report direct spectroscopic evidence of two superconducting energy gaps in RuB2. We have measured scanning tunnelling spectra exhibiting signature of two gaps on different grains of polycrystalline RuB2, possibly originating from multiple bands. Analysis of the temperature dependent tunnelling spectra revealed that the gaps from different bands evolve differently with temperature before disappearing simultaneously at a single T c. Interestingly, our experiments also reveal that the gaps in quasiparticle density of states survive up to magnetic fields much higher than the bulk H c and they evolve smoothly with field, unlike what is expected for a type-I superconductor, indicating the existence of a 'mixed state'.

8.
J Phys Condens Matter ; 32(12): 125701, 2020 Mar 20.
Article in English | MEDLINE | ID: mdl-31756726

ABSTRACT

Though the superconducting phase of the type-II Dirac semimetal PdTe2 was shown to be conventional in nature, the phase continued to be interesting in terms of its magnetic properties. While certain experiments indicated an unexpected type-I superconducting phase, other experiments revealed formation of vortices under the application of magnetic fields. Recently, scanning tunneling spectroscopy (STS) experiments revealed the existence of a mixed phase where type-I and type-II behaviours coexist. Here, based on our temperature and magnetic field dependent STS experiments on Cu-intercalated PdTe2, we show that as the critical temperature of the superconducting phase goes up from 1.7 K to 2.4 K on Cu-intercalation, the mixed phase disappears and the system becomes homogeneously type-II. This may be attributed to an averaging effect caused by quasiparticle exchange between type-I and type-II domains mediated by the Cu atoms and to decreased coherence length due to increased disorder.

9.
Nano Lett ; 19(8): 5703-5709, 2019 Aug 14.
Article in English | MEDLINE | ID: mdl-31347854

ABSTRACT

Ultrathin ferroelectric semiconductors with high charge carrier mobility are much coveted systems for the advancement of various electronic and optoelectronic devices. However, in traditional oxide ferroelectric insulators, the ferroelectric transition temperature decreases drastically with decreasing material thickness and ceases to exist below certain critical thickness owing to depolarizing fields. Herein, we show the emergence of an ordered ferroelectric ground state in ultrathin (∼2 nm) single crystalline nanosheets of Bi2O2Se at room temperature. Free-standing ferroelectric nanosheets, in which oppositely charged alternating layers are self-assembled together by electrostatic interactions, are synthesized by a simple, rapid, and scalable wet chemical procedure at room temperature. The existence of ferroelectricity in Bi2O2Se nanosheets is confirmed by dielectric measurements and piezoresponse force spectroscopy. The spontaneous orthorhombic distortion in the ultrathin nanosheets breaks the local inversion symmetry, thereby resulting in ferroelectricity. The local structural distortion and the formation of spontaneous dipole moment were directly probed by atomic resolution scanning transmission electron microscopy and density functional theory calculations.

10.
ACS Appl Mater Interfaces ; 11(12): 11749-11754, 2019 Mar 27.
Article in English | MEDLINE | ID: mdl-30807098

ABSTRACT

A differentiator is an electronic component used to accomplish mathematical operations of calculus functions of differentiation for shaping different waveforms. Differentiators are used in numerous areas of electronics, including electronic analog computers, wave-shaping circuits, and frequency modulators. Conventional differentiators are fabricated using active operational amplifiers or using passive resistor-capacitor combinations. Here, we report that a single Cu2S-CdS heterostructure acts as a differentiator for performing numerical functions of input waveform conversion into different shapes. When a rectangular wave signal is applied through the tip of a conductive atomic force microscope, a spikelike wave signal is obtained from the Cu2S-CdS heterostructure. The Cu2S-CdS differentiator is able to convert a sine wave signal into a cosine wave signal and a triangular wave signal into a square wave signal similar to the classical differentiators. The finding of a nanoscale differentiator at extremely small length scales may have profound applications in different domains of electronics.

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