Searcharxiv⌕ Search

arXiv subjects

Can B. Uzundal

Publications and source records attributed to Can B. Uzundal.

4 recordsLinked to original sources

Moiré Phonons and Emergent Exciton-Phonon Coupling in a Moiré Heterobilayer

Moiré superlattices have emerged as a new platform for engineering electronic and optical properties in van der Waals heterostructures, enabling control over correlated and excitonic phenomena. Yet the impact of moiré superlattices on exciton-phonon coupling remains largely unexplored. Here we demonstrate emergent, layer-selective coupling between moiré phonons and moiré excitons in angle-aligned WS2/WSe2 heterobilayers. Using a broadband terahertz phonon transducer, we coherently launch moiré phonons that resonantly perturb the excitonic states. We show that the exciton-phonon coupling is intrinsically modified by the moiré superlattice in a layer-selective manner. A driven oscillator model captures the dynamics, revealing three moiré phonon resonances with distinct coupling to the moiré excitons. First principles calculations show that many moiré phonon modes can arise with distinct strongly hybridized in-plane and out-of-plane vibrations in the moiré unit cells. The calculations further identify the three experimentally observed moiré phonons and their emergent characteristic coupling to the moiré excitons.

cond-mat.mtrl-sci↗

Signatures of multi-band effects in high-harmonic generation in monolayer MoS$_2$

High-harmonic generation (HHG) in solids has been touted as a way to probe ultrafast dynamics and crystal symmetries in condensed matter systems. Here, we investigate the polarization properties of high-order harmonics generated in monolayer MoS$_2$, as a function of crystal orientation relative to the mid-infrared laser field polarization. At several different laser wavelengths we experimentally observe a prominent angular shift of the parallel-polarized odd harmonics for energies above approximately 3.5 eV, and our calculations indicate that this shift originates in subtle differences in the recombination dipole strengths involving multiple conduction bands. This observation is material specific and is in addition to the angular dependence imposed by the dynamical symmetry properties of the crystal interacting with the laser field, and may pave the way for probing the vectorial character of multi-band recombination dipoles.

cond-mat.mtrl-sci↗

Polarization-Resolved Extreme Ultraviolet Second Harmonic Generation from LiNbO$_3$

Second harmonic generation (SHG) spectroscopy ubiquitously enables the investigation of surface chemistry, interfacial chemistry as well as symmetry properties in solids. Polarization-resolved SHG spectroscopy in the visible to infrared regime is regularly used to investigate electronic and magnetic orders through their angular anisotropies within the crystal structure. However, the increasing complexity of novel materials and emerging phenomena hamper the interpretation of experiments solely based on the investigation of hybridized valence states. Here, polarization-resolved SHG in the extreme ultraviolet (XUV-SHG) is demonstrated for the first time, enabling element-resolved angular anisotropy investigations. In non-centrosymmetric LiNbO$_3$, elemental contributions by lithium and niobium are clearly distinguished by energy dependent XUV-SHG measurements. This element-resolved and symmetry-sensitive experiment suggests that the displacement of Li ions in LiNbO$_3$, which is known to lead to ferroelectricity, is accompanied by distortions to the Nb ion environment that breaks the inversion symmetry of the NbO$_{6}$ octahedron as well. Our simulations show that the measured second harmonic spectrum is consistent with Li ion displacements from the centrosymmetric position by $\sim$0.5 Angstrom while the Nb-O bonds are elongated/contracted by displacements of the O atoms by $\sim$0.1 Angstrom. In addition, the polarization-resolved measurement of XUV-SHG shows excellent agreement with numerical predictions based on dipole-induced SHG commonly used in the optical wavelengths. This constitutes the first verification of the dipole-based SHG model in the XUV regime. The findings of this work pave the way for future angle and time-resolved XUV-SHG studies with elemental specificity in condensed matter systems.

cond-mat.mtrl-sci↗

Ångström-resolved Interfacial Structure in Organic-Inorganic Junctions

Charge transport processes at interfaces which are governed by complex interfacial electronic structure play a crucial role in catalytic reactions, energy storage, photovoltaics, and many biological processes. Here, the first soft X-ray second harmonic generation (SXR-SHG) interfacial spectrum of a buried interface (boron/Parylene-N) is reported. SXR-SHG shows distinct spectral features that are not observed in X-ray absorption spectra, demonstrating its extraordinary interfacial sensitivity. Comparison to electronic structure calculations indicates a boron-organic separation distance of 1.9 Å, wherein changes as small as 0.1 Å result in easily detectable SXR-SHG spectral shifts (ca. 100s of meV). As SXR-SHG is inherently ultrafast and sensitive to individual atomic layers, it creates the possibility to study a variety of interfacial processes, e.g. catalysis, with ultrafast time resolution and bond specificity.

cond-mat.mtrl-sci↗