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1.
J Phys Chem Lett ; 13(5): 1241-1248, 2022 Feb 10.
Artigo em Inglês | MEDLINE | ID: mdl-35089044

RESUMO

In anisotropic two-dimensional materials, complex values of Raman tensors are necessary to explain the abnormal linearly polarized Raman spectra. In this work, we measured the helicity-changing Raman spectra of few-layer black phosphorus (BP) excited by circularly polarized light. We observed that the polarized Raman intensities of the Ag modes show a deflection angle that depends on the sample orientation, thickness, and laser excitation energy. To understand the deflection, we calculated the resonant Raman spectra by first-principles calculations, which give complex Raman tensors as a function of laser excitation energy. In particular, the phase difference between the elements of the complex Raman tensor is relevant to the deflection angle. The calculated results of monolayer BP reproduce the experimental helicity-resolved Raman spectra of few-layer BP satisfactorily.

2.
Phys Chem Chem Phys ; 23(32): 17271-17278, 2021 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-34355711

RESUMO

Conservation of spin and orbital angular momenta of circularly-polarized vortex light is discussed for Raman spectra of two-dimensional materials. We first show the selection rule for optical absorption of two-dimensional materials as a function of the spin and orbital angular momentum of incident vortex light. In the case of two-dimensional materials, the Raman tensor for the incident vortex light does not change the symmetry of the phonon mode. Furthermore, the Raman active modes are classified by either "helicity-changing" or "helicity-conserved" Raman modes, in which the scattered photon of circularly polarized light either changes or does not change the helicity of the light, respectively. We show tables of selection rules for the Raman active modes of two-dimensional materials with 2, 3, 4, and 6 rotational symmetry for vortex light.

3.
Nano Lett ; 21(11): 4809-4815, 2021 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-34048260

RESUMO

The strength of interlayer coupling critically affects the physical properties of 2D materials such as black phosphorus (BP), where the electronic structure depends sensitively on layer thickness. Rigid-layer vibrations reflect directly the interlayer coupling strength in 2D van der Waals solids, but measurement of these characteristic frequencies is made difficult by sample instability and small Raman scattering cross sections in atomically thin elemental crystals. Here, we overcome these challenges in BP by performing resonance-enhanced low-frequency Raman scattering under an argon-protective environment. Interlayer breathing modes for atomically thin BP were previously unobservable under conventional (nonresonant) excitation but became strongly enhanced when the excitation energy matched the sub-band electronic transitions of few-layer BP, down to bilayer thicknesses. The measured out-of-plane interlayer force constant was found to be 10.1 × 1019 N/m3 in BP, which is comparable to graphene. Accurate characterization of the interlayer coupling strength lays the foundation for future exploration of BP twisted structures and heterostructures.

4.
J Phys Condens Matter ; 33(18)2021 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-33706295

RESUMO

Optical absorption with retardation effect is discussed for two-dimensional (2D) metal. The absorption is given by the induced Joule heat in the metal and it is proportional to Re(σ)/|ɛ|2in whichσandɛdenote conductivity and dielectric function, respectively. Here, we investigate the effective impedance in both retarded and non-retarded regions of surface plasmon by discussing the response of the current density to the electric fields. The absorption formula Re(σ)/|ɛ|2is compared with the formula Re(σ/ɛ) that is commonly used for the absorption in carbon nanotube. We show that Re(σ/ɛ) is equal to Re(σ)/|ɛ|2only in the non-retarded region. The physical reason for Re(σ/ɛ) ≠ Re(σ)/|ɛ|2in the retarded region is that the induced current density is not out-of-phase with the induced electric field, which is explained by the effective impedance for both regions. The opposite response of the current to the induced electric field distinguishes the retarded and non-retarded regions. The calculated optical absorption spectra by Re(σ)/|ɛ|2reproduce the absorption spectra by solving the Maxwell equation as a function of the angular frequency of light or incident angle relative to the 2D surface, which makes Re(σ)/|ɛ|2a general representation of absorption.

5.
Sci Rep ; 10(1): 15282, 2020 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-32943656

RESUMO

The temperature-dependent ([Formula: see text]) optical constants of monolayer [Formula: see text], [Formula: see text], [Formula: see text], and [Formula: see text] were investigated through spectroscopic ellipsometry over the spectral range of 0.73-6.42 eV. At room temperature, the spectra of refractive index exhibited several anomalous dispersion features below 800 nm and approached a constant value of 3.5-4.0 in the near-infrared frequency range. With a decrease in temperature, the refractive indices decreased monotonically in the near-infrared region due to the temperature-dependent optical band gap. The thermo-optic coefficients at room temperature had values from [Formula: see text] to [Formula: see text] for monolayer transition metal dichalcogenides at a wavelength of 1200 nm below the optical band gap. The optical band gap increased with a decrease in temperature due to the suppression of electron-phonon interactions. On the basis of first-principles calculations, the observed optical excitations at 4.5 K were appropriately assigned. These results provide basic information for the technological development of monolayer transition metal dichalcogenides-based photonic devices at various temperatures.

6.
ACS Nano ; 14(8): 10527-10535, 2020 Aug 25.
Artigo em Inglês | MEDLINE | ID: mdl-32790282

RESUMO

We propose a technique of Raman spectroscopy to characterize the excitonic nature and to evaluate the relative contribution of the two kinds of electron/exciton-phonon interactions that are observed in two-dimensional transition-metal dichalcogenides (TMDCs). In the TMDCs, the electron/exciton-phonon interactions mainly originate from the deformation potential (DP) or the Fröhlich interaction (FI) which give the mutually different Raman tensors. Using a circularly polarized light, the relative proportion of the DP and the FI can be defined by the ratio of helicity-polarized intensity that is observed by MoS2. By this analysis, we show that the excitonic FI interaction gradually increases with decreasing temperature, contributes equally to DP at ∼230 K, and dominates at lower temperatures. The excitonic effect in the Raman spectra is confirmed by modulating the dielectric environment for the exciton and by changing the laser power.

7.
J Phys Condens Matter ; 32(42): 425301, 2020 Jun 16.
Artigo em Inglês | MEDLINE | ID: mdl-32544896

RESUMO

A step-like conductance as a function of the Fermi energy is theoretically predicted for a junction made of silicene, in which the energy gap in the junction can be controlled by a perpendicular electric field. When the electric field is applied at the central area of the junction, the transmission probability of an electron becomes partially suppressed and the calculated conductance behaves a step-like function of the Fermi energy. Origins of the step-like conductance are (1) formation of a standing-wave of electron, (2) changing number of transport channels and (3) a rotation of out-of-plane pseudospin of the electron in silicene. We analytically show that the transmission probability of the electron through the junction depends on the direction of the pseudospin, in which the large rotation results in a vanishing conductance. When we switch-off the electric field, on the other hand, the pseudospin does not change the direction, which gives a finite conductance. Thus a switching device can be realized in the silicene pseudospin junction.

8.
ACS Nano ; 14(1): 1055-1069, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31825586

RESUMO

A flat energy dispersion of electrons at the Fermi level of a material leads to instabilities in the electronic system and can drive phase transitions. Here we show that the flat band in graphene can be achieved by sandwiching a graphene monolayer by two cesium (Cs) layers. We investigate the flat band by a combination of angle-resolved photoemission spectroscopy experiment and the calculations. Our work highlights that charge transfer, zone folding of graphene bands, and the covalent bonding between C and Cs atoms are the origin of the flat energy band formation. Analysis of the Stoner criterion for the flat band suggests the presence of a ferromagnetic instability. The presented approach is an alternative route for obtaining flat band materials to twisting bilayer graphene which yields thermodynamically stable flat band materials in large areas.

9.
J Phys Condens Matter ; 31(26): 265701, 2019 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-30909176

RESUMO

We theoretically investigate the optical transition of an electron in graphene that is excited by near-field around a conical Au tip. The interaction between the near-field and the electron is calculated by tight-binding method. In the case of near-field, the wavevector of the electron changes by the optical absorption from the valence band to the conduction band. We show that the change of the wavevector is inversely proportional to the localization width of the near-field, which is given as a function of the distance between the tip and graphene. We calculate the near-field absorption probability as a function of k in the Brillouin zone.

10.
Nano Lett ; 18(9): 6045-6056, 2018 09 12.
Artigo em Inglês | MEDLINE | ID: mdl-30157652

RESUMO

We employ ultra-high vacuum (UHV) Raman spectroscopy in tandem with angle-resolved photoemission (ARPES) to investigate the doping-dependent Raman spectrum of epitaxial graphene on Ir(111). The evolution of Raman spectra from pristine to heavily Cs doped graphene up to a carrier concentration of 4.4 × 1014 cm-2 is investigated. At this doping, graphene is at the onset of the Lifshitz transition and renormalization effects reduce the electronic bandwidth. The optical transition at the saddle point in the Brillouin zone then becomes experimentally accessible by ultraviolet (UV) light excitation, which achieves resonance Raman conditions in close vicinity to the van Hove singularity in the joint density of states. The position of the Raman G band of fully doped graphene/Ir(111) shifts down by ∼60 cm-1. The G band asymmetry of Cs doped epitaxial graphene assumes an unusual strong Fano asymmetry opposite to that of the G band of doped graphene on insulators. Our calculations can fully explain these observations by substrate dependent quantum interference effects in the scattering pathways for vibrational and electronic Raman scattering.

11.
Sci Rep ; 8(1): 11398, 2018 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-30061708

RESUMO

Raman scattering measurements of monolayer WS2 are reported as a function of the laser excitation energies from the near-infrared (1.58 eV) to the deep-ultraviolet (4.82 eV). In particular, we observed several strong Raman peaks in the range of 700∼850 cm-1 with the deep-ultraviolet laser lights (4.66 eV and 4.82 eV). Using the first-principles calculations, these peaks and other weak peaks were appropriately assigned by the double resonance Raman scattering spectra of phonons around the M and K points in the hexagonal Brillouin zone. The relative intensity of the first-order [Formula: see text] to A1g peak changes dramatically with the 1.58 eV and 2.33 eV laser excitations, while the comparable relative intensity was observed for other laser energies. The disappearance of the [Formula: see text] peak with the 1.58 eV laser light comes from the fact that valley polarization of the laser light surpasses the [Formula: see text] mode since the [Formula: see text] mode is the helicity-exchange Raman mode. On the other hand, the disappearance of the A1g peak with the 2.33 eV laser light might be due to the strain effect on the electron-phonon matrix element.

12.
RSC Adv ; 8(58): 33391-33397, 2018 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-35548164

RESUMO

Structural defects, including point defects, dislocation and planar defects, significantly affect the physical and chemical properties of low-dimensional materials, such as layered compounds. In particular, inversion domain boundary is an intrinsic defect surrounded by a 60° grain boundary, which significantly influences electronic transport properties. We study atomic structures of the inversion domain grain boundaries (IDBs) in layered transition metal dichalcogenides (MoSe2 and MoS2) obtained by an exfoliation method, based on the aberration-corrected scanning transmission electron microscopy observation and density functional theory (DFT) calculation. The atomic-scale observation shows that the grain boundaries consist of two different types of 4-fold ring point shared and 8-fold ring edge shared chains. The results of DFT calculations indicate that the inversion domain grain boundary behaves as a metallic one-dimensional chain embedded in the semiconducting MoSe2 matrix with the occurrence of a new state within the band gap.

13.
J Phys Condens Matter ; 29(45): 455303, 2017 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-28809756

RESUMO

The optical properties of a multilayer system with arbitrary N layers of dielectric media are investigated. Each layer is one of two dielectric media, with a thickness one-quarter the wavelength of light in that medium, corresponding to a central frequency f 0. Using the transfer matrix method, the transmittance T is calculated for all possible 2 N sequences for small N. Unexpectedly, it is found that instead of 2 N different values of T at f 0 (T 0), there are only [Formula: see text] discrete values of T 0, for even N, and (N + 1) for odd N. We explain this high degeneracy in T 0 values by finding symmetry operations on the sequences that do not change T 0. Analytical formulae were derived for the T 0 values and their degeneracies as functions of N and an integer parameter for each sequence we call 'charge'. Additionally, the bandwidth at f 0 and filter response of the transmission spectra are investigated, revealing asymptotic behavior at large N.

14.
J Am Chem Soc ; 139(25): 8396-8399, 2017 06 28.
Artigo em Inglês | MEDLINE | ID: mdl-28541698

RESUMO

In this work, by combining transmission electron microscopy and polarized Raman spectroscopy for the 1T' MoTe2 flakes with different thicknesses, we found that the polarization dependence of Raman intensity is given as a function of excitation laser wavelength, phonon symmetry, and phonon frequency, but has weak dependence on the flake thickness from few-layer to multilayer. In addition, the frequency of Raman peaks and the relative Raman intensity are sensitive to flake thickness, which manifests Raman spectroscopy as an effective probe for thickness of 1T' MoTe2. Our work demonstrates that polarized Raman spectroscopy is a powerful and nondestructive method to quickly identify the crystal structure and thickness of 1T' MoTe2 simultaneously, which opens up opportunities for the in situ probe of anisotropic properties and broad applications of this novel material.

15.
J Phys Condens Matter ; 29(5): 055302, 2017 Feb 08.
Artigo em Inglês | MEDLINE | ID: mdl-27941224

RESUMO

The pulse-train technique within ultrafast pump-probe spectroscopy is theoretically investigated to excite a specific coherent phonon mode while suppressing the other phonon modes generated in single-wall carbon nanotubes (SWNTs). In particular, we focus on the selectivity of the radial breathing mode (RBM) and the G-band for a given SWNT. We find that if the repetition period of the pulse train matches with the integer multiple of the RBM phonon period, the RBM amplitude can be maintained while the amplitudes of the other modes are suppressed. As for the G-band, when we apply a repetition period of a half-integer multiple of the RBM period, the RBM can be suppressed because of destructive interference, while the G-band still survives. It is also possible to keep the G-band and suppress the RBM by applying a repetition period that matches with the integer multiple of the G-band phonon period. However, in this case we have to use a large number of laser pulses having a property of "magic ratio" of the G-band and RBM periods.

16.
Nat Commun ; 7: 12899, 2016 10 05.
Artigo em Inglês | MEDLINE | ID: mdl-27703139

RESUMO

Experimental band structure analyses of single-walled carbon nanotubes have not yet been reported, to the best of our knowledge, except for a limited number of reports using scanning tunnelling spectroscopy. Here we demonstrate the experimental determination of the excitonic band structures of single-chirality single-walled carbon nanotubes using their circular dichroism spectra. In this analysis, we use gel column chromatography combining overloading selective adsorption with stepwise elution to separate 12 different single-chirality enantiomers. Our samples show higher circular dichroism intensities than the highest values reported in previous works, indicating their high enantiomeric purity. Excitonic band structure analysis is performed by assigning all observed Eii and Eij optical transitions in the circular dichroism spectra. The results reproduce the asymmetric structures of the valence and conduction bands predicted by density functional theory. Finally, we demonstrate that an extended empirical formula can estimate Eij optical transition energies for any (n,m) species.

17.
ACS Nano ; 10(9): 8964-72, 2016 09 27.
Artigo em Inglês | MEDLINE | ID: mdl-27529802

RESUMO

Layered gallium telluride (GaTe) has attracted much attention recently, due to its extremely high photoresponsivity, short response time, and promising thermoelectric performance. Different from most commonly studied two-dimensional (2D) materials, GaTe has in-plane anisotropy and a low symmetry with the C2h(3) space group. Investigating the in-plane optical anisotropy, including the electron-photon and electron-phonon interactions of GaTe is essential in realizing its applications in optoelectronics and thermoelectrics. In this work, the anisotropic light-matter interactions in the low-symmetry material GaTe are studied using anisotropic optical extinction and Raman spectroscopies as probes. Our polarized optical extinction spectroscopy reveals the weak anisotropy in optical extinction spectra for visible light of multilayer GaTe. Polarized Raman spectroscopy proves to be sensitive to the crystalline orientation of GaTe, and shows the intricate dependences of Raman anisotropy on flake thickness, photon and phonon energies. Such intricate dependences can be explained by theoretical analyses employing first-principles calculations and group theory. These studies are a crucial step toward the applications of GaTe especially in optoelectronics and thermoelectrics, and provide a general methodology for the study of the anisotropy of light-matter interactions in 2D layered materials with in-plane anisotropy.

18.
Phys Rev Lett ; 117(3): 036602, 2016 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-27472126

RESUMO

We theoretically investigate the interplay between the confinement length L and the thermal de Broglie wavelength Λ to optimize the thermoelectric power factor of semiconducting materials. An analytical formula for the power factor is derived based on the one-band model assuming nondegenerate semiconductors to describe quantum effects on the power factor of the low-dimensional semiconductors. The power factor is enhanced for one- and two-dimensional semiconductors when L is smaller than Λ of the semiconductors. In this case, the low-dimensional semiconductors having L smaller than their Λ will give a better thermoelectric performance compared to their bulk counterpart. On the other hand, when L is larger than Λ, bulk semiconductors may give a higher power factor compared to the lower dimensional ones.

20.
Nano Lett ; 16(4): 2260-7, 2016 Apr 13.
Artigo em Inglês | MEDLINE | ID: mdl-26963685

RESUMO

Orthorhombic black phosphorus (BP) and other layered materials, such as gallium telluride (GaTe) and tin selenide (SnSe), stand out among two-dimensional (2D) materials owing to their anisotropic in-plane structure. This anisotropy adds a new dimension to the properties of 2D materials and stimulates the development of angle-resolved photonics and electronics. However, understanding the effect of anisotropy has remained unsatisfactory to date, as shown by a number of inconsistencies in the recent literature. We use angle-resolved absorption and Raman spectroscopies to investigate the role of anisotropy on the electron-photon and electron-phonon interactions in BP. We highlight, both experimentally and theoretically, a nontrivial dependence between anisotropy and flake thickness and photon and phonon energies. We show that once understood, the anisotropic optical absorption appears to be a reliable and simple way to identify the crystalline orientation of BP, which cannot be determined from Raman spectroscopy without the explicit consideration of excitation wavelength and flake thickness, as commonly used previously.

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