arXiv subjects

N. Clark

Publications and source records attributed to N. Clark.

4 recordsLinked to original sources

arXiv2026

The JWST Proto-PAH project. Computational modeling of the emission carriers

The infrared spectra of many carbon-rich post-asymptotic giant branch stars are dominated by emission features from aromatic and aliphatic hydrocarbons, but the chemical structure of the carriers remains unidentified. Class D sources show unusual emission profiles with strong aliphatic emission, providing a stringent test of carrier candidates. Here we investigate whether hydrogenated carbonaceous molecular particles can be the carriers of these features. Rather than assuming candidate geometries we generate the initial structures using ab initio molecular dynamics simulations and optimize them using density functional theory. We then compare the computed emission spectra to JWST NIRSpec and MIRI/MRS observations of Class D sources. The structures providing the best agreements contain sizeable domains with defect-bearing aromatics and hydrogenated-aromatics connected by aliphatic bridges, in contrast to the "arophatic" cluster model of isolated two- to three-ring aromatics connected by aliphatic and olefinic bridges. As a representative example, we discuss in detail the molecular particle C130H96 (radius of 5.5 A) and compare its computed spectrum to the JWST spectra of IRAS 05110-6616, a Class D2 source with apparent shifts of the aromatic C-H out-of-plane bands. The calculated spectra are in qualitative agreement with the observed 3 micron profile, the aliphatic C-H bending bands, the broad 8 micron feature, the 11-14 micron C-H out-of-plane region, and the bands at 16 and 21 microns. We hypothesize that UV photo-driven fragmentation of such molecular particles releases aromatics linked by aliphatics, followed by the formation of polycyclic aromatic hydrocarbons and fullerenes as these objects evolve into planetary nebulae.

astro-ph.GA↗

arXiv2026

The JWST Proto-PAH project: Aromatic backbones with extensive aliphatic substitution account for both the aromatic and aliphatic emission

We find that the aromatic and aliphatic emission bands in four carbon-rich post-asymptotic giant branch stars with class D emission arise from a single carrier population: extensive aliphatic decoration of an aromatic skeleton, i.e. molecules with a coherent aromatic backbone and an unusually high aliphatic content. This conclusion is based on JWST NIRSpec and MIRI/MRS spectroscopy, covering 2.88-28.7um. The aliphatic 3.4um feature is stronger than the aromatic 3.3um feature, reversing the ratio seen in sources with typical polycyclic aromatic hydrocarbon (PAH) emission. If the aromatic emission arose from nominal PAHs, the 3.3um feature - unavailable in previous observations - together with the mid-infrared aromatic features, would constrain them to be large (greater than about carbon atoms), compact, and at least partially ionized. These properties predict a strong 8.6um feature. However, the 8.6um feature is weak or absent in all four sources, ruling out PAHs as the source of the aromatic emission. Instead, the emission must arise from the same carriers as the aliphatic emission. The position of the 6.9um feature and the broadened 11-14um out-of-plane emission independently support this. The CH2 and CH3 feature strengths vary across the sample, with the class D2 sources showing higher CH3 content. These carriers are far more aliphatic than the PAHs of planetary nebulae and the interstellar medium. However, they retain the aromatic skeleton that produces their aromatic features.

astro-ph.GA↗

arXiv2026

Electron-phonon coupling across the TMD/hBN van der Waals interface

Many-body interactions can couple electronic states in one layer with collective excitations in the adjacent layer, providing a route to tailor properties of heterostructures. However, detecting and quantifying interlayer many-body interactions proved a major challenge. Here, we demonstrate that quasiparticles in monolayer transition metal dichalcogenides (TMDs) are dressed by a remote cloud of phonons in the adjacent hexagonal boron nitride slab. Using angle resolved photoemission, we identify replica bands in the TMDs which are a clear fingerprint of long-range electron-phonon interaction. We develop a modified Fröhlich model that shows semi-quantitative agreement with the experimental spectral functions. Our analysis shows that remote electron-phonon coupling is a generic property of interfaces with hBN. This has implications for electron mobilities in 2D materials, for superconductivity and possibly for moiré correlated phases.

cond-mat.mtrl-sci↗

arXiv2019

Enhanced superconductivity in few-layer TaS$_2$ due to healing by oxygenation

When approaching the atomically thin limit, defects and disorder play an increasingly important role in the properties of two-dimensional materials. Superconductivity is generally thought to be vulnerable to these effects, but here we demonstrate the contrary in the case of oxygenation of ultrathin tantalum disulfide (TaS$_2$). Our first-principles calculations show that incorporation of oxygen into the TaS$_2$ crystal lattice is energetically favourable and effectively heals sulfur vacancies typically present in these crystals, thus restoring the carrier density to the intrinsic value of TaS$_2$. Strikingly, this leads to a strong enhancement of the electron-phonon coupling, by up to 80% in the highly-oxygenated limit. Using transport measurements on fresh and aged (oxygenated) few-layer TaS$_2$, we found a marked increase of the superconducting critical temperature ($T_{\mathrm{c}}$) upon aging, in agreement with our theory, while concurrent electron microscopy and electron-energy loss spectroscopy confirmed the presence of sulfur vacancies in freshly prepared TaS$_2$ and incorporation of oxygen into the crystal lattice with time. Our work thus reveals the mechanism by which certain atomic-scale defects can be beneficial to superconductivity and opens a new route to engineer $T_{\mathrm{c}}$ in ultrathin materials.

cond-mat.supr-con↗