Surface Optical Phonon Research Articles

Polaron effect on the bandgap modulation in monolayer transition metal dichalcogenides

We theoretically study the bandgap modulation in monolayer transition metal dichalcogenides (TMDs) originating from the carrier-optical phonon coupling in the Fröhlich polaron model, in which both of the surface optical phonons modes induced by the polar substrate and the intrinsic longitudinal optical phonons modes have been taken into account. We find that the modulated magnitude of the bandgap is in the range of 100–500 meV by altering different polar substrates and tuning the internal distance between TMDs and polar substrate. The large tunability of the bandgap not only provides a possible explanation for the experimental measurements regarding the dielectric environmental sensitivity of the bandgap, but also holds promise for potential applications in optoelectronics and photovoltaics.

Self-energy effect and Coulomb potential modulation of the exciton in monolayer MoS2 on polar substrate

We theoretically investigate the correction of exciton binding energy in monolayer MoS2 resulting from the exciton couples with surface optical (SO) phonons induced by polar substrate. The total correction of binding energy can be divided into the self-energy effect and modification of Coulomb potential using the unitary transformation method. We find that both the self-energy and Coulomb potential vary from tens of meV to several hundreds of meV depending on the cut-off wave vector of SO phonon modes, polarizability of substrate materials and internal distance between the monolayer MoS2 and polar substrate. An effective Coulomb potential is obtained by combining the modified term into the Coulomb potential. This potentially could be widely used in various two-dimensional materials. Our theoretical results not only propose the ways to externally control the exciton binding energy in experiment, but also enrich the understanding of the exciton properties in the dielectric environment.

High-Velocity Saturation in Graphene Encapsulated by Hexagonal Boron Nitride.

We measure drift velocity in monolayer graphene encapsulated by hexagonal boron nitride (hBN), probing its dependence on carrier density and temperature. Due to the high mobility (>5 × 104 cm2/V/s) of our samples, the drift velocity begins to saturate at low electric fields (∼0.1 V/μm) at room temperature. Comparing results to a canonical drift velocity model, we extract room-temperature electron saturation velocities ranging from 6 × 107 cm/s at a low carrier density of 8 × 1011 cm-2 to 2.7 × 107 cm/s at a higher density of 4.4 × 1012 cm-2. Such drift velocities are much higher than those in silicon (∼107 cm/s) and in graphene on SiO2, likely due to reduced carrier scattering with surface optical phonons whose energy in hBN (>100 meV) is higher than that in other substrates.

Plasmons in graphene nanoribbons

We calculate the dielectric function and plasmonic response of armchair (aGNRs) and zigzag (zGNRs) graphene nanoribbons using the self-consistent-field approach within the Markovian master equation formalism (SCF-MMEF). We accurately account for electron scattering with phonons, ionized impurities, and line-edge roughness and show that electron scattering with surface optical phonons is much more prominent in GNRs than in graphene. We calculate the loss function, plasmon dispersion, and the plasmon propagation length in supported GNRs. Midinfrared plasmons in supported (3N+2)-aGNRs can propagate as far as several microns at room temperature, with 4--5-nm-wide ribbons having the longest propagation length. In other types of aGNRs and in zGNRs, the plasmon propagation length seldom exceeds 100 nm. Plasmon propagation lengths are much longer on nonpolar (e.g., diamondlike carbon) than on polar substrates (e.g., ${\mathrm{SiO}}_{2}$ or hBN), where electrons scatter strongly with surface optical phonons. We also show that the aGNR plasmon density is nearly uniform across the ribbon, while in zGNRs, because of the highly localized edge states, plasmons of different spin polarization are accumulated near the opposite edges.

Magneto-optical transport properties of monolayer MoS2 on polar substrates

We theoretically study the magneto-optical transport properties of monolayer molybdenum disulfide (${\mathrm{MoS}}_{2}$) on polar substrates in the presence of a perpendicular magnetic field. The magneto-optical absorption coefficient (MOAC) is investigated as a function of the incident photon energy when carriers are scattered by three different types of phonons: the intrinsic ${\mathrm{MoS}}_{2}$ acoustic, optical phonons, and the surface optical (SO) phonons induced by polar substrates. Among the substrates considered, the largest magnitude of MOAC and full-width at half maximum (FWHM) are observed for a ${\mathrm{SiO}}_{2}$ substrate over the entire temperature and magnetic field range considered due to its strongest electron-SO phonon scattering, while an h-BN substrate displays the lowest one. The piezoelectric (PE) coupling to the transverse (TA) phonon is shown to dominate the MOAC and FWHM due to intrinsic acoustic phonon scattering. Meanwhile, these properties for intrinsic optical phonons are dominated by zero-order deformation potential (DP) couplings and the Fr\"ohlich interaction. The dependence of the MOAC and FWHM on temperature, magnetic field, and the effective ${\mathrm{MoS}}_{2}$-substrate distance is also examined. The present results for monolayer ${\mathrm{MoS}}_{2}$ are compared with those in conventional two-dimensional systems as well as in graphene. Our results show that SO phonons play a crucial role at high temperature depending on the substrates and have a non-negligible effect on the magneto-optical transport properties of monolayer ${\mathrm{MoS}}_{2}$, which could be further experimentally and theoretically investigated in the future.

Surface optical phonon modes in hexagonal shaped Al0.97Ga0.03N nanostructures

Raman modes of plasma assisted molecular beam epitaxy grown, c-plane oriented and hexagonal shaped cylindrical Al0.97Ga0.03N nanostructures are reported. Apart from the group theoretically allowed optical phonons at zone center (wave vector, q = 0), two additional phonon modes around 763 and 846 cm−1 are observed in between the reported values of longitudinal optical (LO q=0) and transverse optical (TO q=0) phonon modes. The observed phonon mode frequencies are matched with the simulated dispersion curve for the surface optical (SO) phonon modes and subsequently assigned as SO(A 1) and SO(E 1) with A 1 and E 1 symmetries, respectively. A change in the dielectric constant of the surrounding medium using CCl4 is demonstrated to show a significant red shift of the additional modes with respect to those in air, and they show good agreement with the calculated SO phonon frequencies. The origin of SO phonon modes are attributed to the relaxation of Raman selection rules away from the Brillouin zone centre because of the presence of periodic surface modulations of sharp edges at the corners of well-faceted Al0.97Ga0.03N hexagonal crystallites in the sample. An appropriate quantification is also made in this regard to find out the Fourier component of the surface potential responsible for activating the SO mode.

Influence of exciton-phonons coupling on the exciton binding energy in monolayer transition metal dichalcogenides

We theoretically investigate the correction of exciton binding energy arising from the exciton-optical phonon coupling in monolayer transition metal dichalcogenides (TMDs) using the linear operator and Lee-Low-Pines unitary transformation methods. We take into account not only the exciton coupling with intrinsic longitudinal optical phonon modes but also the surface optical phonon modes induced by polar substrates supporting monolayer TMDs. We find that the exciton binding energies are corrected on a large scale due to these exciton-optical phonon couplings. We discuss the dependences of exciton binding energy on the cut-off wave vector of optical phonon modes, the polarization strength of substrate materials, and the distance between polar substrates and TMDs. These results provide potential explanations for the divergence of the exciton binding energy between the experiment and theory in TMDs.

Antiproliferative effects on human lung cell lines A549 activity of cadmium selenide nanoparticles extracted from cytotoxic effects: Investigation of bio-electronic application

Cadmium selenide (CdSe) nanoparticles make necessary to acquire more information against the cytotoxic effects on human lung epithelial cells A549 potential adverse to health effects. More biological studies highlighted their cytotoxic potential like pulmonary or respiratory diseases were focused on toxicity nanoparticles mechanisms are involved. The aim of our research, is the comparison of cytotoxicity effect between cells-particle interactions, viability test, membrane integrity and oxidative stress were investigated. XRD showed a strong peak associated with (111) plane of hexagonal CdSe suggesting formation of highly orientated nanoparticles. The longitudinal optical phonon shifted slightly due to strain whereas strong low-energy shoulder shift can be explained within a model for surface optical phonons. Photocatalytic activity of CdSe nanoparticles were investigated by exploiting photocatalytic degradation of Rhodamine B (RhB). The typical UV–vis absorption spectra of RhB solution at different time intervals it can be clearly seen that the relative intensity of the absorption peak corresponding to RhB, with the catalyst for different concentration time intervals (0mM, 2mM, 5mM & 10mM) of the prepared CdSe nanoparticles. After completion of 5mM % the dye was completely degraded and the absorption spectra act as a photocatalyst. CdSe nanoparticles exhibits antibacterial activity over a broad range of bacterial species and in particular against P. vulgaris where it out competes four other commonly used S. aureus, E.coli, P. vulgaris and E. hermannii, well as testing four different appropriate concentration from the results showed a significant gain in viable cell numbers of all four bacteria species, with 5mM and 10mM being the most effective and 2mM being the worst, where it provided only a slight improvement from the control in detail.

Enhanced performance in graphene RF transistors via advanced process integration

The state-of-the-art performance of a graphene radio-frequency (RF) field-effect transistor (FET) made of chemical vapor deposition (CVD) graphene is presented. The record high cut-off frequency as high as 380 GHz using CVD graphene was attributed to the implementation of advanced process integration. On the one hand, interface engineering has become critical in two-dimensional (2D) electronics since the charge transport of a 2D electron system like graphene is highly affected by the interface. The interface engineering was made for both the top and bottom of the graphene surface by implementing a non-polar material (1, 3, 5-trimethyl-1, 3, 5-trivinyl cyclotrisiloxane). In contrast to conventional polar materials, such as SiO2, the non-polar materials significantly reduce the surface optical phonon scattering in the graphene channel, leading to the enhanced RF performance of graphene FET. On the other hand, micro-scaled holes over the multilayer graphene and self-aligned structure also become a critical factor in minimizing the parasitic resistance that is inversely proportional to RF performance. As the growth technique of CVD graphene greatly advances, the advanced process integration scheme could bring graphene electronics one step further towards practical application.

Surface optical phonon propagation in defect modulated nanowires

Planar defects, such as stacking faults and twins, are the most common defects in III–V semiconductor nanowires. Here we report on the effect of surface perturbation caused by twin planes on surface optical (SO) phonon modes. Self-catalyzed GaAs nanowires with varying planar defect density were grown by molecular beam epitaxy and investigated by Raman spectroscopy and transmission electron microscopy (TEM). SO phonon peaks have been detected, and the corresponding spatial period along the nanowire axis were measured to be 1.47 μm (±0.47 μm) and 446 nm (±35 nm) for wires with twin densities of about 0.6 (±0.2) and 2.2 (±0.18) per micron. For the wires with extremely high density of twins, no SO phonon peaks were detected. TEM analysis of the wires reveal that the average distance between the defects are in good agreement with the SO phonon spatial period determined by Raman spectroscopy.

Nitride Dielectric Environments to Suppress Surface Optical Phonon Dominated Scattering in High‐Performance Multilayer MoS2 FETs

The ultrathin channel in 2D semiconductors, although playing host to several interesting properties, also renders strong interactions (scattering) of charge carriers with the surrounding medium. The over‐arching dominance of surface (interfacial) optical phonons in 2D charge transport and engineering ideal nitride‐based dielectric environments for large performance gains is reported. Charge transport in MoS2 field effect transistors (FETs) fabricated on three conventional substrates, SiO2, Al2O3, and HfO2, is contrasted with a newly introduced, CMOS‐compatible nitride‐based dielectric: aluminum nitride (AlN) by employing semi‐classical models which account for charged impurity, surface optical phonon, and intrinsic phonon scattering. Unlike previous reports focused on charge impurity scattering, this work presents a new paradigm of utilizing high optical phonon energies intrinsic to “stiff” nitride bonds. This results in substantially lower surface optical phonon scattering in 2D FETs which directly influences peak field effect (FE) mobility, high field mobility degradation, and temperature‐dependent mobility. Leveraging on these insights, high‐performance sulfur‐passivated MoS2 FETs with an optimum all‐nitride environment (hexagonal boron nitride/MoS2/AlN) are demonstrated with FE mobility up to 72.8 cm2 V−1 s−1. This work is envisioned to address important issues in design of dielectric environments for a host of applications based on 2D materials.

Effect of epoxy exposure on the electronic properties of graphene

The effect of epoxy exposure and its curing agent (trimethyl-1, 6-hexanediamine), widely used for the biocompatible packaging of graphene-based devices, on the electrical characteristics of a graphene field effect transistor is investigated in this work. Upon 5 min of the epoxy curing agent exposure, the Dirac point shifted from 60 to 13 V, while for 15 min of the epoxy curing agent exposure, the Dirac point changed more than 130 V, from 63 to −68 V, completely changing the doping of graphene from strong p-type to strong n-type due to the electron donating nature of the adsorbed molecules. Additionally, due to exposure, the hole mobility was found to reduce from 1243 to 401 cm2 V−1 s−1, indicating the strong impact of ionized impurity scattering. The temperature-dependent Hall measurement of single layer graphene before and after the epoxy curing agent exposure also exhibited a change in the dominant scattering mechanism from surface optical phonon scattering to Coulomb scattering near room temperature due to epoxy exposure. Reduction of initial p-type doping in chemical vapor deposited (CVD) graphene after epoxy exposure is also confirmed by Raman spectroscopy. We found that the Dirac point recovered very slowly upon storage of the epoxy (or curing agent) exposed devices, changing by only ~11 V after 4 months without significant change in carrier mobility.

Raman spectroscopy based measurements of carrier concentration in n-type GaN nanowires grown by plasma-assisted molecular beam epitaxy

The carrier concentration in as-grown ensembles of n-type GaN nanowires was determined by Raman spectroscopy of the coupled longitudinal phonon–plasmon (LPP+) mode and modeling of the carrier concentration dependence of the LPP+ frequency. The Raman measurements and analyses enabled estimation of the carrier concentration in single-nanowire devices fabricated from the as-grown ensembles. The nanowires were grown by plasma-assisted molecular beam epitaxy in either of the two growth systems. Twelve samples were examined, of which 11 samples were Si-doped and one was undoped. The Raman-measured carrier concentrations in the Si-doped samples ranged from (5.28 ± 1.19) × 1016 cm−3 to (6.16 ± 0.35) × 1017 cm−3. For a subset of samples grown with varying Si cell temperature, from 1125 °C to 1175 °C, the carrier concentration was found to be an Arrhenius function of Si cell temperature, with activation energy of 6.281±0.011 eV. Co-illumination by an above band gap UV laser (325 nm, excitation intensity = 0.7 W/cm2 or 4.5 W/cm2) induced small increases in carrier concentration, relative to illumination by the Raman excitation laser alone (633 nm, excitation intensity ≈100 kW/cm2). The lowest Si-doped sample showed the largest increase in carrier concentration, (6.3 ± 4.8) × 1015 cm−3 with UV excitation intensity of 0.7 W/cm2. These results imply that, even in the absence of UV illumination, surface depletion does not have a significant effect on the Raman carrier concentration measurements. Immersion in a high-dielectric-constant oil (ε = 2.24) caused downshifts of similar magnitude in the LPP+ frequencies of undoped and doped nanowires. This result implies that the LPP+ mode has bulk plasmon rather than surface plasmon character, because immersion in a high-dielectric-constant medium is predicted to cause a large decrease in the surface plasmon frequency, which would induce a larger LPP+ downshift in doped than undoped nanowires. A surface optical (SO) phonon peak was observed in each sample in air at ≈96.4% of the LPP+ frequency. The SO frequency decreased to ≈93.1% of the LPP+ frequency upon oil immersion, as predicted by a simple dielectric model.

Magneto-optical transitions in monolayer molybdenum disulphide on polar substrates

Within the frame of the Huang–Rhys's lattice relaxation model, we theoretically studied the effects of lattice relaxation due to the electrons (holes)-surface optical (SO) phonons coupling on the magneto-optical (MO) transitions in monolayer molybdenum disulphide on three different types of polar substrates. The lattice relaxation resulted in the peak position shifting and the linewidths broadening in MO transitions. The dependences of MO transitions on the magnetic field, temperature and polarization strength of substrates have been discussed in detail. The obtained results may provide a possible method to measure the coupling strength between the electrons (holes) and SO phonons in MO experiments.

Polaron effect on the optical rectification in spherical quantum dots with electric field**Project supported by the National Natural Science Foundation of China (Grant No. 11364028), the Major Projects of the Natural Science Foundation of Inner Mongolia Autonomous Region, China (Grant No. 2013ZD02), and the Project of “Prairie Excellent” Engineering in Inner Mongolia Autonomous Region, China.

The polaron effect on the optical rectification in spherical quantum dots with a shallow hydrogenic impurity in the presence of electric field is theoretically investigated by taking into account the interactions of the electrons with both confined and surface optical phonons. Besides, the interaction between impurity and phonons is also considered. Numerical calculations are presented for typical Zn1−xCdxSe/ZnSe material. It is found that the polaronic effect or electric field leads to the redshifted resonant peaks of the optical rectification coefficients. It is also found that the peak values of the optical rectification coefficients with the polaronic effect are larger than without the polaronic effect, especially for smaller Cd concentrations or stronger electric field.

Raman study of surface optical phonons in hydrothermally obtained ZnO(Mn) nanoparticles

Nanocrystalline samples of ZnO(Mn) were synthesized by hydrothermal method. The morphology of the samples was studied by HRTEM and SEM. X-ray diffraction was used to determine composition of the samples (ZnO and ZnMn2O4) and the mean crystalline size (from 16 to 99 nm). In this paper we report the experimental spectra of Raman scattering (from 100 to 1600 cm−1) with surface optical phonons (SOP) in range of 497–538 cm−1 as well as formation of new phases MnO, Mn3O4 and ZnMnO3. The phonon of registered phase's exhibit effects connected to phase concentration, while the SOP phonon mode exhibit significant confinement effect.

Origin of additional broad peaks in Raman spectra from thin germanium-rich silicon–germanium films

Additional broad peaks in Raman spectra from thin Ge-rich SiGe films were examined in detail. The broad peak on the low-wavenumber side of first-order optical phonon was also present for pure Ge, which indicates that the localized mode is not the reason for the broad peaks. Furthermore, other factors, e.g., strain, defect, phonon confinement effect, Fano effect, and fluorescence from oil, were excluded from the origin of the broad peaks. We assigned the broad peaks to surface optical phonon modes. The dependence of this surface mode on Ge concentration in Ge-rich SiGe was also investigated and the behavior was discussed.

Analytical band Monte Carlo analysis of electron transport in silicene

An analytical band Monte Carlo (AMC) with linear energy band dispersion has been developed to study the electron transport in suspended silicene and silicene on aluminium oxide (Al2O3) substrate. We have calibrated our model against the full band Monte Carlo (FMC) results by matching the velocity-field curve. Using this model, we discover that the collective effects of charge impurity scattering and surface optical phonon scattering can degrade the electron mobility down to about 400 cm2 V−1 s−1 and thereafter it is less sensitive to the changes of charge impurity in the substrate and surface optical phonon. We also found that further reduction of mobility to ∼100 cm2 V−1 s−1 as experimentally demonstrated by Tao et al (2015 Nat. Nanotechnol. 10 227) can only be explained by the renormalization of Fermi velocity due to interaction with Al2O3 substrate.

Robust Phonon-Plasmon Coupling in Quasifreestanding Graphene on Silicon Carbide.

Using inelastic electron scattering in combination with dielectric theory simulations on differently prepared graphene layers on silicon carbide, we demonstrate that the coupling between the 2D plasmon of graphene and the surface optical phonon of the substrate cannot be quenched by modification of the interface via intercalation. The intercalation rather provides additional modes like, e.g., the silicon-hydrogen stretch mode in the case of hydrogen intercalation or the silicon-oxygen vibrations for water intercalation that couple to the 2D plasmons of graphene. Furthermore, in the case of bilayer graphene with broken inversion symmetry due to charge imbalance between the layers, we observe a similar coupling of the 2D plasmon to an internal infrared-active mode, the LO phonon mode. The coupling of graphene plasmons to vibrational modes of the substrate surface and internal infrared active modes is envisioned to provide an excellent tool for tailoring the plasmon band structure of monolayer and bilayer graphene for plasmonic devices such as plasmon filters or plasmonic waveguides. The rigidity of the effect furthermore suggests that it may be of importance for other 2D materials as well.

Temperature dependent carrier mobility in graphene: Effect of Pd nanoparticle functionalization and hydrogenation

The two dimensional nature of graphene, with charge carriers confined within one atomic layer thickness, causes its electrical, optical, and sensing properties to be strongly influenced by the surrounding media and functionalization layers. In this study, the effect of catalytically active Pd nanoparticle (NP) functionalization and subsequent hydrogenation on the hall mobility and carrier density of chemical vapor deposition synthesized graphene has been investigated as a function of temperature. Prior to functionalization, the mobility decreased monotonically as the temperature was reduced from 298 to 10 K, indicating coulomb scattering as the dominant scattering mechanism as expected for bilayer graphene. Similar decreasing trend with temperature was also observed after 2 nm Pd deposition, however, hydrogenation of the Pd NP led to significant enhancement in mobility from ∼2250 to 3840 cm2/V s at room temperature, which further monotonically increased to 5280 cm2/V s at 10 K. We attribute this contrasting trend in temperature dependent mobility to a switch in the dominant scattering mechanism from coulomb to surface optical (SO) phonon scattering due to higher dielectric constant and polar nature of PdHx formed upon hydrogenation of the Pd NPs.