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1.
ACS Nano ; 2020 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-32584026

RESUMO

Quasi-two-dimensional (2D) semiconductor nanoplatelets manifest strong quantum confinement with exceptional optical characteristics of narrow photoluminescence peaks with energies tunable by thickness with monolayer precision. We employed scanning tunneling spectroscopy (STS) in conjunction with optical measurements to probe the thickness-dependent band gap and density of excited states in a series of CdSe nanoplatelets. The tunneling spectra, measured in the double-barrier tunnel junction configuration, reveal the effect of quantum confinement on the band gap taking place mainly through a blue-shift of the conduction band edge, along with a signature of 2D electronic structure intermixed with finite lateral-size and/or defects effects. The STS fundamental band gaps are larger than the optical gaps as expected from the contributions of exciton binding in the absorption, as confirmed by theoretical calculations. The calculations also point to strong valence band mixing between the light- and split-off hole levels. Strikingly, the energy difference between the heavy-hole and light-hole levels in the tunneling spectra are significantly larger than the corresponding values extracted from the absorption spectra. Possible explanations for this, including an interplay of nanoplatelet charging, dielectric confinement, and difference in exciton binding energy for light and heavy holes, are analyzed and discussed.

2.
Nano Lett ; 19(8): 5167-5175, 2019 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-31361954

RESUMO

Hybrid ferromagnetic/superconducting systems are well-known for hosting intriguing phenomena such as emergent triplet superconductivity at their interfaces and the appearance of in-gap, spin-polarized Yu-Shiba-Rusinov (YSR) states bound to magnetic impurities on a superconducting surface. In this work we demonstrate that similar phenomena can be induced on a surface of a conventional superconductor by chemisorbing nonmagnetic chiral molecules. Conductance spectra measured on NbSe2 flakes over which chiral α-helix polyalanine molecules were adsorbed exhibit, in some cases, in-gap states nearly symmetrically positioned around zero bias that shift with magnetic field, akin to YSR states, as corroborated by theoretical simulations. Other samples show evidence for a collective phenomenon of hybridized YSR-like states giving rise to unconventional, possibly triplet superconductivity, manifested in the conductance spectra by the appearance of a zero bias conductance that diminishes, but does not split, with magnetic field. The transition between these two scenarios appears to be governed by the density of adsorbed molecules.

3.
Sci Adv ; 5(4): eaav5532, 2019 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-31032414

RESUMO

A long-term goal for superconductors is to increase the superconducting transition temperature, T C. In cuprates, T C depends strongly on the out-of-plane Cu-apical oxygen distance and the in-plane Cu-O distance, but there has been little attention paid to tuning them independently. Here, in simply grown, self-assembled, vertically aligned nanocomposite thin films of La2CuO4+δ + LaCuO3, by strongly increasing out-of-plane distances without reducing in-plane distances (three-dimensional strain engineering), we achieve superconductivity up to 50 K in the vertical interface regions, spaced ~50 nm apart. No additional process to supply excess oxygen, e.g., by ozone or high-pressure oxygen annealing, was required, as is normally the case for plain La2CuO4+δ films. Our proof-of-concept work represents an entirely new approach to increasing T C in cuprates or other superconductors.

4.
Phys Chem Chem Phys ; 20(37): 24444-24452, 2018 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-30221290

RESUMO

In-gap states in solar cell absorbers that are recombination centers determine the cell's photovoltaic performance. Using scanning tunneling spectroscopy (STS), temperature-dependent photoconductivity and steady-state photocarrier-grating measurements we probed, directly and indirectly, the energies of such states, both at the surface and in the bulk of two similar, but different halide perovskites, the single cation MAPbI3 (here MAPI) and the mixed cation halide perovskite, FA0.79MA0.16Cs0.05Pb(I0.83Br0.17)3 (here MCHP). We found a correlation between the energy distribution of the in-gap states, as determined by STS measurements, and their manifestation in the photo-transport parameters of the MCHP absorbers. In particular, our results suggest that the in-gap recombination centers in the MCHP are shallower than those of MAPI. This can be one explanation for the better photovoltaic efficiency of the former.

5.
Philos Trans A Math Phys Eng Sci ; 376(2125)2018 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-29941620

RESUMO

Zero-energy Andreev bound states, which manifest themselves in the tunnelling spectra as zero-bias conductance peaks (ZBCPs), are abundant at interfaces between superconductors and other materials and on the nodal surface of high-temperature superconductors. In this review, we focus on the information such excitations can provide on the properties of superconductor systems. First, a general introduction to the physics of Andreev bound states in superconductor/normal metal interfaces is given with a particular emphasis on why they appear at zero energy in d-wave superconductors. Then, specific spectroscopic tunnelling studies of thin films, bilayers and junctions are described, focusing on the corresponding ZBCP features. Scanning tunnelling spectroscopy (STS) studies show that the ZBCPs on the c-axis YBa2Cu3O7-δ (YBCO) films are correlated with the surface morphology and appear only in proximity to (110) facets. STS on c-axis La1.88Sr0.12CuO4 (LSCO) films exhibiting the 1/8 anomaly shows spatially modulated peaks near zero bias associated with the anti-phase ordering of the d-wave order parameter predicted at this doping level. ZBCPs were also found in micrometre-size edge junctions of YBCO/SrRuO3/YBCO, where SrRuO3 is ferromagnetic. Here, the results are consistent with a crossed Andreev reflection effect (CARE) at the narrow domain walls of the SrRuO3 ZBCPs measured in STS studies of manganite/cuprate bilayers could not be attributed to CARE because the manganite's domain wall is much larger than the coherence length in YBCO, and instead are attributed to proximity-induced triplet-pairing superconductivity with non-conventional symmetry. And finally, ZBCPs found in junctions of non-intentionally doped topological insulator films of Bi2Se3 and the s-wave superconductor NbN are attributed to proximity-induced px + ipy triplet order parameter in the topological material.This article is part of the theme issue 'Andreev bound states'.

6.
Nanotechnology ; 29(35): 355705, 2018 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-29862985

RESUMO

Developing new methods, other than size and shape, for controlling the optoelectronic properties of semiconductor nanocrystals is a highly desired target. Here we demonstrate that the photoluminescence (PL) of silicon nanocrystals (SiNCs) can be tuned in the range 685-800 nm solely via surface functionalization with alkynyl(aryl) (phenylacetylene, 2-ethynylnaphthalene, 2-ethynyl-5-hexylthiophene) surface groups. Scanning tunneling microscopy/spectroscopy on single nanocrystals revealed the formation of new in-gap states adjacent to the conduction band edge of the functionalized SiNCs. PL red-shifts were attributed to emission through these in-gap states, which reduce the effective band gap for the electron-hole recombination process. The observed in-gap states can be associated with new interface states formed via (-Si-C≡C-) bonds in combination with conjugated molecules as indicated by ab initio calculations. In contrast to alkynyl(aryl)s, the formation of in-gap states and shifts in PL maximum of the SiNCs were not observed with aryl (phenyl, naphthalene, 2-hexylthiophene) and alkynyl (1-dodecyne) surface groups. These outcomes show that surface functionalization with alkynyl(aryl) molecules is a valuable tool to control the electronic structure and optical properties of SiNCs via tuneable interface states, which may enhance the performance of SiNCs in semiconductor devices.

7.
Nanoscale ; 9(45): 17884-17892, 2017 Nov 23.
Artigo em Inglês | MEDLINE | ID: mdl-29120002

RESUMO

The electrical and optical properties of semiconductor nanocrystals (NCs) can be controlled, in addition to size and shape, by doping. However, such a process is not trivial in NCs due to the high formation energy of dopants there. Nevertheless, it has been shown theoretically that in the case of B and P (acceptor/donor) codoped Si-NCs the formation energy is reduced relative to that of single type doping. Previous comprehensive measurements on ensembles of such codoped Si-NCs have pointed to the presence of donor and acceptor states within the energy gap. However, such a conjecture has not been directly verified previously. Following that, we investigate here the electronic properties of B and P codoped Si-NCs via Scanning Tunneling Spectroscopy. We monitored the quantum confinement effect in this system, for which the energy gap changed from ∼1.4 eV to ∼1.8 eV with the decrease of NC diameter from 8.5 to 3.5 nm. Importantly, all spectra showed two in-gap band-states, one close to the conduction band edge and the other to the valence band edge, which we attribute to the P and B dopant levels, respectively. The energy separation between these dopants states decrease monotonically with increasing NC diameter, in parallel to the decrease of the conduction-to-valence bands separation. A fundamental quantity that is derived directly for these Si-NCs is the intrinsic like position of the Fermi energy, a non-trivial result that is very relevant for understanding the system. Following the above results we suggest an explanation for the character and the origin of the dopants bands.

8.
Nano Lett ; 17(5): 2934-2939, 2017 05 10.
Artigo em Inglês | MEDLINE | ID: mdl-28406304

RESUMO

Control over the vortex potential at the nanoscale in a superconductor is a subject of great interest for both fundamental and technological reasons. Many methods for achieving artificial pinning centers have been demonstrated, for example, with magnetic nanostructures or engineered imperfections, yielding many intriguing effects. However, these pinning mechanisms do not offer dynamic control over the strength of the patterned vortex potential because they involve static nanostructures created in or near the superconductor. Dynamic control has been achieved with scanning probe methods on the single vortex level but these are difficult so scale up. Here, we show that by applying controllable nanopatterned current injection, the superconductor can be locally driven out of equilibrium, creating an artificial vortex potential that can be tuned by the magnitude of the injected current, yielding a unique vortex channeling effect.

9.
J Phys Chem Lett ; 7(24): 5219-5226, 2016 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-27973905

RESUMO

Photovoltaic solar cells operate under steady-state conditions that are established during the charge carrier excitation and recombination. However, to date no model of the steady-state recombination scenario in halide perovskites has been proposed. In this Letter we present such a model that is based on a single type of recombination center, which is deduced from our measurements of the illumination intensity dependence of the photoconductivity and the ambipolar diffusion length in those materials. The relation between the present results and those from time-resolved measurements, such as photoluminescence that are commonly reported in the literature, is discussed.

10.
Angew Chem Int Ed Engl ; 55(26): 7393-7, 2016 06 20.
Artigo em Inglês | MEDLINE | ID: mdl-27144670

RESUMO

Hybrid functional materials (HFMs) comprised of semiconductor nanoparticles and conjugated polymers offer the potential of synergetic photophysical properties. We have developed HFMs based upon silicon nanocrystals (SiNCs) and the conductive polymer poly(3-hexylthiophene) (SiNC@P3HT) by applying surface-initiated Kumada catalyst transfer polycondensation (SI-KCTP). One unique characteristic of the developed SiNC@P3HT is the formation of a direct covalent bonding between SiNCs and P3HT. The presented method for obtaining direct interfacial attachment, which is not accessible using other methods, may allow for the development of materials with efficient electronic communication at the donor-acceptor interfaces. Systematic characterization provides evidence of a core-shell structure, enhanced interfacial electron and/or energy transfer between the P3HT and SiNC components, as well as formation of a type-II heterostructure.

11.
Nanoscale ; 8(15): 7849-53, 2016 Apr 21.
Artigo em Inglês | MEDLINE | ID: mdl-27020915

RESUMO

Optoelectronic properties of Si nanocrystals (SiNCs) were studied by combining scanning tunneling spectroscopy (STS) and optical measurements. The photoluminescence (PL) of phenylacetylene functionalized SiNCs red shifts relative to hexyl- and phenyl-capped counterparts, whereas the absorption spectra and the band gaps extracted from STS are similar for all surface groups. However, an in-gap state near the conduction band edge was detected by STS only for the phenylacetylene terminated SiNCs, which can account for the PL shift via relaxation across this state.

12.
Chemphyschem ; 17(5): 675-80, 2016 Mar 03.
Artigo em Inglês | MEDLINE | ID: mdl-26541934

RESUMO

The level structure of copper sulfide nanocrystals of different sizes was investigated by correlating scanning tunneling spectroscopy and cyclic voltammetry data in relation to sensing applications. Upon oxidation of Cu2 S nanocrystals in the low-chalcocite phase, correlated changes are detected by both methods. The cyclic voltammetry oxidation peak of Cu(1+) down shifts, while in-gap states, adjacent to the valence-band edge, appeared in the tunneling spectra. These changes are attributed to Cu vacancy formation leading to a Cu depleted phase of the nanocrystals. The relevance of the oxidation to the use of copper sulfide nanocrystals in hydrogen peroxide sensing was also addressed, showing that upon oxidation the sensitivity vanishes. These findings bare significance to the use of copper sulfide nanocrystals in glucose sensing applications.

13.
J Phys Chem Lett ; 6(17): 3396-402, 2015 Sep 03.
Artigo em Inglês | MEDLINE | ID: mdl-26275992

RESUMO

To address the yet open question regarding the nature of quantum confinement in Ge nanocrystals (Ge NCs) we employed scanning tunneling spectroscopy to monitor the electronic structure of individual isolated Ge NCs as a function of their size. The (single-particle) band gaps extracted from the tunneling spectra increase monotonically with decreasing nanocrystal size, irrespective of the capping ligands, manifesting the effect of quantum confinement. Band-gap widening of ∼1 eV with respect to the bulk value was observed for Ge-NCs 3 nm in diameter. The picture emerging from comparison with theoretical calculations and other experimental results is discussed.


Assuntos
Geranium/química , Nanopartículas/química , Teoria Quântica
14.
Phys Rev Lett ; 111(3): 037401, 2013 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-23909359

RESUMO

Infrared absorption measurements of amorphous and crystalline nanoparticles of GeTe reveal a localized surface plasmon resonance (LSPR) mode in the crystalline phase that is absent in the amorphous phase. The LSPR mode emerges upon crystallization of amorphous nanoparticles. The contrasting plasmonic properties are elucidated with scanning tunneling spectroscopy measurements indicating a Burstein-Moss shift of the band gap in the crystalline phase and a finite density of electronic states throughout the band gap in the amorphous phase that limits the effective free carrier density.

15.
Nanotechnology ; 23(50): 505710, 2012 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-23196692

RESUMO

Hybrid inorganic nanoparticles, comprising a semiconducting Cu(2)S quantum-dot (QD) core encapsulated by a metallic Ru cage-like shell, and each of their individual components, are studied via scanning tunneling spectroscopy. Bare Cu(2)S QDs show nearly identical semiconducting-like I-V characteristics while the empty Ru cages exhibit single electron tunneling effects-the Coulomb blockade and staircase. Surprisingly, in some cases negative differential conductance features, with periodicity that correlates to the Coulomb staircase, were observed. The tunneling spectra measured on the hybrid QDs varies greatly along a single particle, manifesting synergetic electrical properties that originate from this unique semiconducting-metallic interface.

16.
Phys Rev Lett ; 108(10): 107004, 2012 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-22463444

RESUMO

The superconducting critical temperature, T(C), of thin Nb films is significantly modified when gold nanoparticles (NPs) are chemically linked to the Nb film, with a consistent enhancement when using 3 nm long disilane linker molecules. The T(C) increases by up to 10% for certain linker length and NP size. No change is observed when the nanoparticles are physisorbed with nonlinking molecules. Electron tunneling spectra acquired on the linked NPs below T(C) typically exhibit zero-bias peaks. We attribute these results to a pairing mechanism coupling electrons in the Nb and the NPs, mediated by the organic linkers.

17.
Phys Rev Lett ; 108(7): 076603, 2012 Feb 17.
Artigo em Inglês | MEDLINE | ID: mdl-22401233

RESUMO

We investigated the electronic properties around grain boundaries of polycrystalline Cu(In(1-x),Ga(x)Se(2)) films as a function of Ga content, using scanning tunneling spectroscopy. Spectra acquired on samples with low Ga content (x=0 and 0.33) reveal downward band bending with respect to adjacent p-type grains, suggesting type inversion at the surface of grain boundaries. Such a behavior was not observed for samples with high Ga contents. These results are consistent with our atomic force microscopy data and may shed light on the origin of the x-dependent efficiency for polycrystalline Cu(In(1-x),Ga(x)Se(2))-based solar cells.

18.
ACS Nano ; 6(1): 176-82, 2012 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-22136306

RESUMO

We utilize single-molecule spectroscopy combined with time-correlated single-photon counting to probe the electron transfer (ET) rates from various types of semiconductor hetero-nanocrystals, having either type-I or type-II band alignment, to single-walled carbon nanotubes. A significantly larger ET rate was observed for type-II ZnSe/CdS dot-in-rod nanostructures as compared to type-I spherical CdSe/ZnS core/shell quantum dots and to CdSe/CdS dot-in-rod structures. Furthermore, such rapid ET dynamics can compete with both Auger and radiative recombination processes, with significance for effective photovoltaic operation.


Assuntos
Nanoestruturas/química , Nanoestruturas/ultraestrutura , Semicondutores , Titânio/química , Condutividade Elétrica , Transporte de Elétrons , Desenho de Equipamento , Análise de Falha de Equipamento , Teste de Materiais
19.
Science ; 332(6025): 77-81, 2011 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-21454783

RESUMO

Doping of semiconductors by impurity atoms enabled their widespread technological application in microelectronics and optoelectronics. However, doping has proven elusive for strongly confined colloidal semiconductor nanocrystals because of the synthetic challenge of how to introduce single impurities, as well as a lack of fundamental understanding of this heavily doped limit under strong quantum confinement. We developed a method to dope semiconductor nanocrystals with metal impurities, enabling control of the band gap and Fermi energy. A combination of optical measurements, scanning tunneling spectroscopy, and theory revealed the emergence of a confined impurity band and band-tailing. Our method yields n- and p-doped semiconductor nanocrystals, which have potential applications in solar cells, thin-film transistors, and optoelectronic devices.

20.
Nano Lett ; 10(7): 2416-20, 2010 Jul 14.
Artigo em Inglês | MEDLINE | ID: mdl-20507148

RESUMO

Electrical current measurements through individually wired colloidal CdSe nanorods exhibit pronounced multistability. This current switching is analogous to the widely observed fluorescence intermittency in similar systems and may be associated with surface charge dynamics. Such association is quantitatively established for the case when the current is bistable, where the probability of the sojourn time t at the high or low current state follows an exponential dependence. Remarkably, this behavior can be modeled by charging dynamics of a single surface trap, whose position could be estimated from the intermittent current-voltage characteristics. The methodology presented here provides a unique route for charge dynamic sensing at the nanoscale, where the nanorod senses its own surface charge.

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