SearcharxivSearch

arXiv · 1808.06493

Attosecond state-resolved carrier motion in quantum materials probed by soft X-ray XANES

Abstract

Recent developments in attosecond technology led to tabletop X-ray spectroscopy in the soft X-ray range, thus uniting the element- and state-specificity of core-level x-ray absorption spectroscopy with the time resolution to follow electronic dynamics in real time. We describe recent work in attosecond technology and investigations into materials such as Si, SiO2, GaN, Al2O3, Ti, TiO2, enabled by the convergence of these two capabilities. We showcase the state-of-the-art on isolated attosecond soft x-ray pulses for x-ray absorption near edge spectroscopy (XANES) to observe the 3d-state dynamics of the semi-metal TiS2 with attosecond resolution at the Ti L-edge (460 eV). We describe how the element- and state-specificity at the transition metal L-edge of the quantum material allows to unambiguously identify how and where the optical field influences charge carriers. This precision elucidates that the Ti:3d conduction band states are efficiently photo-doped to a density of 1.9 x 10^21 cm^-3 and that the light-field induces coherent motion of intra-band carriers across 38% of the first Brillouin zone. Lastly, we describe the prospects with such unambiguous real-time observation of carrier dynamics in specific bonding or anti-bonding states and speculate that such capability will bring unprecedented opportunities towards an engineered approach for designer materials with pre-defined properties and efficiency. Examples are composites of semiconductors and insulators like Si, Ge, SiO2, GaN, BN, quantum materials like graphene, TMDCs, or high-Tc superconductors like NbN or LaBaCuO. Exiting are prospects to scrutinize canonical questions in multi-body physics such as whether the electrons or lattice trigger phase transitions.

Explore related subjects

Keep this discovery

BibTeXRIS

Barbara Buades, Antonio Picon, Emma Berger, Iker Leon, Nicola Di Palo, Seth L. Cousin, Caterina Cocchi, Eric Pellegrin, Javier Herrero Martin, Samuel Mañas-Valero, Eugenio Coronado, Thomas Danz, Claudia Draxl, Mitsuharu Uemoto, Kazuhiro Yabana, Martin Schultze, Simon Wall, Michael Zürch, Jens Biegert. 2018-08-20. Attosecond state-resolved carrier motion in quantum materials probed by soft X-ray XANES. https://doi.org/10.1063/5.0020649

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related papers

Measuring chiral phonons

Chiral phonons are quantized vibrations where the atomic motion in a solid breaks improper rotation symmetries. In many cases, chiral phonons possess angular momenta and are therefore selective to circularly polarized light. Both fundamental and applied research efforts on chiral phonons have been gaining increasing attention owing to their importance in a variety of fields including spintronics, spin-selective chemical reactions, thermal transport, quantum information processing and biosensing, where the bi-directional spin-lattice coupling enabled by chiral phonons can be harnessed in new ways, and potentially lead to new functionalities. Thus far, the studies of chiral phonons across diverse materials platforms have evolved largely independently within these fields, but the experimental techniques are often interrelated. In this perspective, we present a detailed description, as well as advantages and disadvantages of the current approaches for experimentally measuring chiral phonons in chiral and achiral materials. We conclude with a discussion of new methods for measuring chiral phonons. Ultimately, this work seeks to offer an experimental guide for systematically investigating the properties of chiral phonons in various materials systems and applications.

cond-mat.mtrl-sci

A model of grain growth in UN integrating molecular dynamics, phase-field modeling, and uncertainty quantification

Grain growth kinetics and grain-boundary (GB) properties in uranium mononitride (UN) are investigated through an integrated multiscale framework combining molecular dynamics (MD), phase-field modeling, and surrogate-assisted uncertainty quantification. MD simulations yield GB energies for 27 symmetric tilt boundaries from 0--2000~K, which are consistent with available DFT values. The average GB energy is nearly temperature-independent below 1000~K and increases at higher temperatures. A mechanistic pore-drag model applied to the only available grain growth dataset for actinide nitrides yields a mobility reduction factor of $s \approx 0.93$--$0.99$, statistically indistinguishable from unity, confirming that pore drag is negligible under the experimental conditions. The intrinsic GB mobility is therefore extracted directly from the effective mobility, yielding $M_0 = 2.05\times10^{-15}$~m$^4$/(J$\cdot$s) and $Q_M = 0.89$~eV. Phase-field simulations conducted from 1500--2000~K confirm normal curvature-driven grain growth, with grain size distributions converging to the Hillert-like form. A surrogate-assisted global sensitivity analysis---combining principal component analysis, Gaussian process regression, and Sobol decomposition---reveals that the mobility prefactor $M_0$ dominates output variance at all times, followed by the activation energy $Q_M$, while the GB energy $\gamma$ contributes minimally. These results establish the first quantitative grain growth framework for UN and identify the reduction of uncertainty in $M_0$ and $Q_M$ as the highest-priority target for future experimental efforts.

cond-mat.mtrl-sci

Silicon Solar Cell Design for >30% Efficiency via Singlet Fission

Singlet fission (SF) materials convert high-energy photons into multiple charge carriers, providing a route to exceed the efficiency limits of single-junction silicon solar cells without many of the complexities of multi-junction tandem designs. Following the first demonstration of an SF-enhanced silicon solar cell in 2025, there is a need to understand how SF materials can be effectively integrated into high-efficiency industrial silicon devices and translated from proof of concept to a manufacturable technology. Using coupled optical and electrical simulations, we assess the efficiency potential of several industrially relevant silicon cell architectures combined with SF materials. Interdigitated back-contact (IBC) cells offer the greatest potential for improvement due to unrestricted front-surface access and can achieve efficiencies exceeding 33%. However, performance is highly sensitive to front-surface passivation quality. Appropriate silicon design, particularly controlled surface doping and fixed interfacial charge, can mitigate recombination losses and relax passivation requirements for ultra-thin exciton-transfer layers.

cond-mat.mtrl-sci