arXiv subjects

Henning Sirringhaus

Publications and source records attributed to Henning Sirringhaus.

26 records · Page 2Linked to original sources

arXiv2020

Tuning Spin Current Injection at Ferromagnet/Non-Magnet Interfaces by Molecular Design

There is a growing interest in utilizing the distinctive material properties of organic semiconductors for spintronic applications. Here, we explore injection of pure spin current from Permalloy into a small molecule system based on dinaphtho[2,3-b:2,3-f]thieno[3,2-b]thiophene (DNTT) at ferromagnetic resonance. The unique tunability of organic materials by molecular design allows us to study the impact of interfacial properties on the spin injection efficiency systematically. We show that both, spin injection efficiency at the interface as well as the spin diffusion length can be tuned sensitively by the interfacial molecular structure and side chain substitution of the molecule.

physics.app-ph↗

arXiv2019

Fragment Graphical Variational AutoEncoding for Screening Molecules with Small Data

In the majority of molecular optimization tasks, predictive machine learning (ML) models are limited due to the unavailability and cost of generating big experimental datasets on the specific task. To circumvent this limitation, ML models are trained on big theoretical datasets or experimental indicators of molecular suitability that are either publicly available or inexpensive to acquire. These approaches produce a set of candidate molecules which have to be ranked using limited experimental data or expert knowledge. Under the assumption that structure is related to functionality, here we use a molecular fragment-based graphical autoencoder to generate unique structural fingerprints to efficiently search through the candidate set. We demonstrate that fragment-based graphical autoencoding reduces the error in predicting physical characteristics such as the solubility and partition coefficient in the small data regime compared to other extended circular fingerprints and string based approaches. We further demonstrate that this approach is capable of providing insight into real world molecular optimization problems, such as searching for stabilization additives in organic semiconductors by accurately predicting 92% of test molecules given 69 training examples. This task is a model example of black box molecular optimization as there is minimal theoretical and experimental knowledge to accurately predict the suitability of the additives.

physics.data-an↗

arXiv2019

Chasing the killer phonon mode for the rational design of low disorder, high mobility molecular semiconductors

Molecular vibrations play a critical role in the charge transport properties of weakly van der Waals bonded organic semiconductors. To understand which specific phonon modes contribute most strongly to the electron-phonon coupling and ensuing thermal energetic disorder in some of the most widely studied high mobility molecular semiconductors, state-of-the-art quantum mechanical simulations of the vibrational modes and the ensuing electron phonon coupling constants are combined with experimental measurements of the low-frequency vibrations using inelastic neutron scattering and terahertz time-domain spectroscopy. In this way, the long-axis sliding motion is identified as a killer phonon mode, which in some molecules contributes more than 80% to the total thermal disorder. Based on this insight, a way to rationalize mobility trends between different materials and derive important molecular design guidelines for new high mobility molecular semiconductors is suggested.

cond-mat.mtrl-sci↗

arXiv2018

Low-dimensional quantum magnetism in Cu(NCS)$_2$: A molecular framework material

Low-dimensional magnetic materials with spin-$\frac{1}{2}$ moments can host a range of exotic magnetic phenomena due to the intrinsic importance of quantum fluctuations to their behavior. Here, we report the structure, magnetic structure and magnetic properties of copper(II) thiocyanate, Cu(NCS)$_2$, a one-dimensional coordination polymer which displays low-dimensional quantum magnetism. Magnetic susceptibility, electron paramagnetic resonance (EPR) spectroscopy, $^{13}$C magic-angle spinning nuclear magnetic resonance (MASNMR) spectroscopy, and density functional theory (DFT) investigations indicate that Cu(NCS)$_2$ behaves as a two-dimensional array of weakly coupled antiferromagnetic spin chains ($J_2 = 133(1)$ K, $α= J_1/J_2 = 0.08$). Powder neutron-diffraction measurements confirm that Cu(NCS)$_2$ orders as a commensurate antiferromagnet below $T_\mathrm{N} = 12$ K, with a strongly reduced ordered moment (0.3 $μ_\mathrm{B}$) due to quantum fluctuations.

cond-mat.str-el↗

arXiv2017

Molecular Tuning of the Magnetic Response in Organic Semiconductors

The tunability of high-mobility organic semi-conductors (OSCs) holds great promise for molecular spintronics. In this study, we show this extreme variability - and therefore potential tunability - of the molecular gyromagnetic coupling ("g-") tensor with respect to the geometric and electronic structure in a much studied class of OSCs. Composed of a structural theme of phenyl- and chalcogenophene (group XVI element containing, five-membered) rings and alkyl functional groups, this class forms the basis of several intensely studied high-mobility polymers and molecular OSCs. We show how in this class the g-tensor shifts, $Δg$, are determined by the effective molecular spin-orbit coupling (SOC), defined by the overlap of the atomic spin-density and the heavy atoms in the polymers. We explain the dramatic variations in SOC with molecular geometry, chemical composition, functionalization, and charge life-time using a first-principles theoretical model based on atomic spin populations. Our approach gives a guide to tuning the magnetic response of these OSCs by chemical synthesis.

cond-mat.mtrl-sci↗

arXiv2017

Tuning the effective spin-orbit coupling in molecular semiconductors

The control of spins and spin to charge conversion in organics requires understanding the molecular spin-orbit coupling (SOC), and a means to tune its strength. However, quantifying SOC strengths indirectly through spin relaxation effects has proven diffi- cult due to competing relaxation mechanisms. Here we present a systematic study of the g-tensor shift in molecular semiconductors and link it directly to the SOC strength in a series of high mobility molecular semiconductors with strong potential for future devices. The results demonstrate a rich variability of the molecular g-shifts with the effective SOC, depending on subtle aspects of molecular composition and structure. We correlate the above g -shifts to spin-lattice relaxation times over four orders of magnitude, from 200 μs to 0.15 μs, for isolated molecules in solution and relate our findings for isolated molecules in solution to the spin relaxation mechanisms that are likely to be relevant in solid state systems.

cond-mat.mtrl-sci↗

arXiv2015

Spin-current emission governed by nonlinear spin dynamics

Coupling between conduction electrons and localized magnetization is responsible for a variety of phenomena in spintronic devices. This coupling enables to generate spin currents from dynamical magnetization. Due to the nonlinearity of magnetization dynamics, the spin-current emission through the dynamical spin-exchange coupling offers a route for nonlinear generation of spin currents. Here, we demonstrate spin-current emission governed by nonlinear magnetization dynamics in a metal/magnetic insulator bilayer. The spin-current emission from the magnetic insulator is probed by the inverse spin Hall effect, which demonstrates nontrivial temperature and excitation power dependences of the voltage generation. The experimental results reveal that nonlinear magnetization dynamics and enhanced spin-current emission due to magnon scatterings are triggered by decreasing temperature. This result illustrates the crucial role of the nonlinear magnon interactions in the spin-current emission driven by dynamical magnetization, or nonequilibrium magnons, from magnetic insulators.

cond-mat.mes-hall↗

arXiv2014

Simultaneous Extraction of Charge Density Dependent Mobility and Variable Contact Resistance from Thin Film Transistors

A model for the extraction of the charge density dependent mobility and variable contact resistance in thin film transistors is proposed by performing a full derivation of the current-voltage characteristics both in the linear and saturation regime of operation. The calculated values are validated against the ones obtained from direct experimental methods. This approach allows unambiguous determination of both contact and channel resistance from the analysis of the current voltage characteristics of a single device, with no a-priori assumption on the two parameters. It solves the inconsistencies in the commonly accepted mobility extraction methods and provides new possibilities for the analysis of the injection and transport processes in semiconducting materials.

cond-mat.mes-hall↗