arXiv subjects

Britta Redlich

Publications and source records attributed to Britta Redlich.

8 recordsLinked to original sources

arXiv2026

First detection of C2H+ in the interstellar medium

Despite the detection of nearly 350 molecules in the interstellar medium, almost half of which are carbon chains, the pathways that build molecular complexity remain poorly understood. Observed abundances of carbon-chain and aromatic species are difficult to reconcile with existing top-down or bottom-up formation scenarios, due in part to limited observational constraints and incomplete theoretical understanding. In particular, small intermediary ions, key drivers of ion-molecule reactions capable of seeding larger hydrocarbons and aromatic rings, could provide critical support for the bottom-up formation scenario. Constraining the abundance and chemistry of these ions is therefore essential to test whether bottom-up growth can operate efficiently under interstellar conditions. Here, we report the first detection of the small hydrocarbon cation ethynylium, C2H+, toward the Orion Bar, based on observations with the APEX 12m sub-mm telescope of its lowest-lying J=3-2 rotational transition near 211GHz, which exhibits a unique spectroscopic fingerprint through resolved Lambda-doubling and hyperfine splitting components, as recently measured in the laboratory. Meudon PDR models successfully reproduce these values, placing C2H+ formation at the outer edges of PDR fronts. Our results link C2H+ production to CH+ and CH3+ within a network of ion-molecule reactions driven by vibrationally excited H2, a scenario now further supported by recent detections of these species in PDRs like the Orion Bar with JWST observations. The importance of C2H+ lies in its role as a key intermediate: it produces C2H2+ and subsequently C2H3+, effectively channelling small C2 building blocks toward larger hydrocarbons and facilitating bottom-up growth at the PDR surface. Targeted searches for C2H+ in other regions promise to provide a potentially decisive probe of ion-driven bottom-up chemistry in the ISM.

astro-ph.GA↗

arXiv2026

High-resolution ro-vibrational and rotational spectroscopy of the open-shell, linear CCH$^+$ ion ($^3\Pi$)

In this work, we report on the high-resolution infrared spectrum of CCH$^+$ ($^3\Pi$) recorded in the range $3066-3184$~cm$^{-1}$ by means of leak-out spectroscopy. This spectral range covers the fundamental of the CH stretching mode and a highly excited bending vibrational mode. Based on this data (385 ro-vibrational lines), accurate spectroscopic descriptions of the ground and the two vibrationally excited states of CCH$^+$ were obtained. Besides the band origins, spin-orbit coupling constants, rotational constants, centrifugal distortion constants and $\Lambda$-doubling constants for the ground and excited vibrational states have been derived. This effective Hamiltonian analysis allowed a search for pure rotational lines of CCH$^+$ in its electronic and vibrational ground state using a two-color millimeterwave - infrared scheme. We observed all rotational transitions from $J^{\prime\prime} = 2$ up to $J^{\prime\prime} = 6$ within the $\Omega = 2$ lowest energy fine structure component with resolved hyperfine splittings. This data has already guided the first detection of CCH$^+$ in space toward the Orion Bar photo-dissociation region, and has the potential to support further astronomical searches for CCH$^+$ either through radio or infrared spectroscopy, for example with the James Webb Space Telescope.

physics.chem-ph↗

arXiv2026

Experimental proof of strong $\Pi$-$\Sigma$ mixing in the Renner-Teller and Pseudo-Jahn-Teller affected CCH$^+$ ($^3\Pi$) ion

The ethynyl radical cation, CCH$^+$ ($^3\Pi$), offers a unique system for fundamental spectroscopic studies of non-adiabatic effects due to its open-shell linear structure and the presence of a low-lying $^3\Sigma^-$ state, which induces notable perturbations in the (ro-)vibrational spectrum. To probe these effects, we recorded the broadband vibrational spectrum of CCH$^+$ from 350-3450 cm$^{-1}$ using leak-out spectroscopy. The spectrum reveals a complex splitting pattern in the CCH bending mode, attributed to Renner-Teller and pseudo-Jahn-Teller coupling effects between the $^3 \Pi$ and $^3 \Sigma^-$ electronic states. A three-state diabatic model, validated here against high-resolution IR data of the CH stretching mode, facilitated assignments within the broadband infrared (IR) spectrum, including an additional $\Pi$ vibronic feature observed in the aforementioned high-resolution spectrum. Our results highlight a pronounced sensitivity of the splitting pattern to the $\Pi$-$\Sigma$ energy gap, with couplings so large that even the zero-point vibrational motion of the bending vibration is sufficient to disrupt the vibronic structure of this ion. This compact ion, with strong coupling effects and high-quality spectroscopic data, serves as an exemplary system for evaluating non-adiabatic models.

physics.chem-ph↗

arXiv2026

Sub-wavelength mid-infrared imaging of locally driven photocurrents using diamond campanile probes

Precise and high efficiency concentration of mid-infrared (mid-IR) light into sub wavelength volumes is essential for probing low-energy excitations and achieving strong field enhancements, which can be hindered by absorption losses and coupling inefficiencies at long wavelengths. Here, we introduce an innovative diamond-based metal-insulator-metal campanile probe that adiabatically compresses free-space mid infrared light (10 \mum) into \approx 1 \mum domains. Integrated into a scanning photovoltage microscope, the probe enables sub-wavelength mapping of locally driven photocurrents in graphene, resolving polarization dependent and contact-sensitive responses at energies down to \approx 0.1 eV. Experiments reveal a photocurrent signal density enhancement of 10^3 and coupling efficiencies approaching 80%, in agreement with numerical simulations. Operation of the probe with quantum cascade and free electron lasers demonstrates a robust, spectrally tunable platform for high-resolution exploration of low-energy carrier dynamics in atomically thin materials, opening opportunities for mid-IR optoelectronics and quantum photonics.

cond-mat.mes-hall↗

arXiv2022

Energy transfer and restructuring in amorphous solid water upon consecutive irradiation

Interstellar and cometary ices play an important role in the formation of planetary systems around young stars. Their main constituent is amorphous solid water (ASW). Although ASW is widely studied, vibrational energy dissipation and structural changes due to vibrational excitation are less well understood. The hydrogen-bonding network is likely a crucial component in this. Here we present experimental results on hydrogen-bonding changes in ASW induced by the intense, nearly monochromatic mid-IR free-electron laser (FEL) radiation of the FELIX-2 beamline at the HFML-FELIX facility at the Radboud University in Nijmegen, the Netherlands. Structural changes in ASW are monitored by reflection-absorption infrared spectroscopy and depend on the irradiation history of the ice. The experiments show that FEL irradiation can induce changes in the local neighborhood of the excited molecules due to energy transfer. Molecular Dynamics simulations confirm this picture: vibrationally excited molecules can reorient for a more optimal tetrahedral surrounding without breaking existing hydrogen bonds. The vibrational energy can transfer through the hydrogen-bonding network to water molecules that have the same vibrational frequency. We hence expect a reduced energy dissipation in amorphous material with respect to crystalline material due to the inhomogeneity in vibrational frequencies as well as the presence of specific hydrogen-bonding defect sites which can also hamper the energy transfer.

astro-ph.GA↗

arXiv2022

Infrared free-electron laser irradiation of carbon dioxide ice

Interstellar ice grains are believed to play a key role in the formation of many of the simple and complex organic species detected in space. However, many fundamental questions on the physicochemical processes linked to the formation and survival of species in ice grains remain unanswered. Field work at large-scale facilities such as free-electron lasers (FELs) can aid the investigation of the composition and morphology of ice grains by providing novel tools to the laboratory astrophysics community. We combined the high tunability, wide infrared spectral range and intensity of the FEL beam line FELIX-2 at the HFML-FELIX Laboratory in the Netherlands with the characteristics of the ultrahigh vacuum LISA end station to perform wavelength-dependent mid-IR irradiation experiments of space-relevant pure carbon dioxide (CO2) ice at 20 K. We used the intense monochromatic radiation of FELIX to inject vibrational energy at selected frequencies into the CO2 ice to study ice restructuring effects in situ by Fourier Transform Reflection-Absorption Infrared (FT-RAIR) spectroscopy. This work improves our understanding of how vibrational energy introduced by external triggers such as photons, electrons, cosmic rays, and thermal heating coming from a nascent protostar or field stars is dissipated in an interstellar icy dust grain in space. Moreover, it adds to the current literature debate concerning the amorphous and polycrystalline structure of CO2 ice observed upon deposition at low temperatures, showing that, under our experimental conditions, CO2 ice presents amorphous characteristics when deposited at 20 K and is unambiguously crystalline if deposited at 75 K.

astro-ph.GA↗

arXiv2021

Infrared action spectroscopy of doubly charged PAHs and their contribution to the aromatic infrared bands

The so-called aromatic infrared bands are attributed to emission of polycyclic aromatic hydrocarbons. The observed variations toward different regions in space are believed to be caused by contributions of different classes of PAH molecules, i.e. with respect to their size, structure, and charge state. Laboratory spectra of members of these classes are needed to compare them to observations and to benchmark quantum-chemically computed spectra of these species. In this paper we present the experimental infrared spectra of three different PAH dications, naphthalene$^{2+}$, anthracene$^{2+}$, and phenanthrene$^{2+}$, in the vibrational fingerprint region 500-1700~cm$^{-1}$. The dications were produced by electron impact ionization of the vapors with 70 eV electrons, and they remained stable against dissociation and Coulomb explosion. The vibrational spectra were obtained by IR predissociation of the PAH$^{2+}$ complexed with neon in a 22-pole cryogenic ion trap setup coupled to a free-electron infrared laser at the Free-Electron Lasers for Infrared eXperiments (FELIX) Laboratory. We performed anharmonic density-functional theory calculations for both singly and doubly charged states of the three molecules. The experimental band positions showed excellent agreement with the calculated band positions of the singlet electronic ground state for all three doubly charged species, indicating its higher stability over the triplet state. The presence of several strong combination bands and additional weaker features in the recorded spectra, especially in the 10-15~$μ$m region of the mid-IR spectrum, required anharmonic calculations to understand their effects on the total integrated intensity for the different charge states. These measurements, in tandem with theoretical calculations, will help in the identification of this specific class of doubly-charged PAHs as carriers of AIBs.

astro-ph.GA↗

arXiv2013

Probing of electromagnetic fields on atomic scale by photoelectric phenomena in graphene

We report on the observation of the reststrahl band assisted photocurrents in epitaxial graphene on SiC excited by infrared radiation. The peculiar spectral dependence for frequencies lying within the reststrahl band of the SiC substrate provides a direct and noninvasive way to probe the electric field magnitude at atomic distances from the material's surface. Furthermore our results reveal that nonlinear optical and optoelectronic phenomena in 2D crystals and other atomic scale structures can be giantly enhanced by a proper combination of the spectral range and substrate material.

cond-mat.mes-hall↗