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We propose a nonlinear-optics-based nanosensor to detect malachite green (MG) contaminants on semiconductor interfaces such as silicon (Si). Applying the simplified bond hyperpolarizability model (SBHM), we simplified the second-harmonic generation (SHG) analysis of an MG-Si(111) surface and were able to validate our model by reproducing experimental rotational anisotropy (RA) SHG experiments. For the first time, density functional theory (DFT) calculations using ultrasoft pseudopotentials were implemented to obtain the molecular configuration and bond vector orientation required by the SBHM to investigate and predict the second-harmonic generation contribution for an MG-Si 001 surface. We show that the SBHM model significantly reduces the number of independent components in the nonlinear tensor of the MG-Si(111) interface, opening up the possibility for real-time and non-destructive contaminant detection at the nanoscale. In addition, we derive an explicit formula for the SHG far field, demonstrating its applicability for various input polarization angles. Finally, an RASHG signal can be enhanced through a simulated photonic crystal cavity up to 4000 times for more sensitivity of detection. Our work can stimulate more exploration using nonlinear optical methods to detect and analyze surface-bound contaminants, which is beneficial for environmental monitoring, especially for mitigating pollution from textile dyes, and underscores the role of nonlinear optics in real-time ambient-condition applications.

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.

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 × 10 14 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.

Topological domain walls in dual-gated gapped bilayer graphene host edge states that are gate-tunable and valley polarized. Here we predict that plasmonic collective modes can propagate along these topological domain walls even at zero bulk density and possess a markedly different character from that of bulk plasmons. Strikingly, domain wall plasmons are extremely long-lived with plasmon lifetimes that can be orders of magnitude larger than the transport scattering time in the bulk at low temperatures. Importantly, long domain wall plasmon lifetimes persist even at room temperature with values up to a few picoseconds. Domain wall plasmons possess a rich phenomenology including plasmon oscillation over a wide range of frequencies (up to the mid-infrared), tunable subwavelength electromagnetic confinement lengths, as well as a valley polarization for forward/backward propagating modes. Its unusual features render them as a new tool for realizing low-dissipation plasmonics that transcend the restrictions of the bulk.

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.

In this article, we overview our recent theoretical works on electronic and optical properties of carbon nanotubes by going from the background to the perspectives. Electronic Raman spectra of metallic carbon nanotubes give a new picture of Raman processes. Thermoelectricity of semiconducting nanotubes gives a general concept of the confinement effect on the thermoelectric power factor. Selective excitation of only a single phonon mode is proposed by the pulsed train technique of coherent phonon spectroscopy. Occurrence of both two and four fold degeneracy in the carbon nanotube quantum dot is explained by difference group velocities and the intra/inter valley scattering near the hexagonal corner of the Brillouin zone.

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.

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.