Probing the Interatomic Potential of Solids by Strong-Field Nonlinear Phononics

Femtosecond optical pulses at mid-infrared frequencies have opened up the nonlinear control of lattice vibrations in solids. So far, all applications have relied on second order phonon nonlinearities, which are dominant at field strengths near 1 MVcm-1. In this regime, nonlinear phononics can transiently change the average lattice structure, and with it the functionality of a material. Here, we achieve an order-of-magnitude increase in field strength, and explore higher-order lattice nonlinearities. We drive up to five phonon harmonics of the A1 mode in LiNbO3. Phase-sensitive measurements of atomic trajectories in this regime are used to experimentally reconstruct the interatomic potential and to benchmark ab-initio calculations for this material. Tomography of the Free Energy surface by high-order nonlinear phononics will impact many aspects of materials research, including the study of classical and quantum phase transitions

Disentangling the Electronic and Lattice Contributions to the Dielectric Response of Photoexcited Bismuth

Elucidating the interplay between nuclear and electronic degrees of freedom that govern the complex dielectric behavior of materials under intense photoexcitation is essential for tailoring optical properties on demand. However, conventional transient reflectivity experiments have been unable to differentiate between real and imaginary components of the dielectric response, omitting crucial electron-lattice interactions. Utilizing thin film interference we unambiguously determined the photoinduced change in complex dielectric function in the Peierls semimetal bismuth and examined its dependence on the excitation density and nuclear motion of the A$_{1g}$ phonon. Our modeled transient reflectivity data reveals a progressive broadening and redshift of Lorentz oscillators with increasing excitation density and underscores the importance of both, electronic and nuclear coordinates in the renormalization of interband transitions.Comment: Manuscript (6 pages) plus supplemental material (6 pages

Picosecond electric-field-induced threshold switching in phase-change materials

Many chalcogenide glasses undergo a breakdown in electronic resistance above a critical field strength. Known as threshold switching, this mechanism enables field-induced crystallization in emerging phase-change memory. Purely electronic as well as crystal nucleation assisted models have been employed to explain the electronic breakdown. Here, picosecond electric pulses are used to excite amorphous Ag$_4$In$_3$Sb$_{67}$Te$_{26}$. Field-dependent reversible changes in conductivity and pulse-driven crystallization are observed. The present results show that threshold switching can take place within the electric pulse on sub-picosecond time-scales - faster than crystals can nucleate. This supports purely electronic models of threshold switching and reveals potential applications as an ultrafast electronic switch.Comment: 6 pages manuscript with 3 figures and 8 pages supplementary materia

Direct Observation of Collective Modes of the Charge Density Wave in the Kagome Metal CsV3_3Sb5_5

A new group of kagome metals AV$_3$Sb$_5$ (A = K, Rb, Cs) exhibit a variety of intertwined unconventional electronic phases, which emerge from a puzzling charge density wave phase. Understanding of this parent charge order phase is crucial for deciphering the entire phase diagram. However, the mechanism of the charge density wave is still controversial, and its primary source of fluctuations - the collective modes - have not been experimentally observed. Here, we use ultrashort laser pulses to melt the charge order in CsV$_3$Sb$_5$ and record the resulting dynamics using femtosecond angle-resolved photoemission. We resolve the melting time of the charge order and directly observe its amplitude mode, imposing a fundamental limit for the fastest possible lattice rearrangement time. These observations together with ab-initio calculations provide clear evidence for a structural rather than electronic mechanism of the charge density wave. Our findings pave the way for better understanding of the unconventional phases hosted on the kagome lattice.Comment: 17 pages, 4 figure

Nonlinear coupled magnonics: Terahertz field-driven magnon upconversion

Tailored light excitation and nonlinear control of lattice vibrations have emerged as powerful strategies to manipulate the properties of quantum materials out of equilibrium. Generalizing the exploitation of coherent phonon-phonon interactions to nonlinear couplings among other types of collective modes would open unprecedented opportunities in the design of novel dynamic functionalities in solids. For example, the collective excitations of magnetic order - magnons - can efficiently transfer information via spin current flow, and their coherent and nonlinear control would provide an attractive route to achieve faster signal processing for next-generation information technologies. Here, we discover that intense terahertz (THz) fields can initiate processes of magnon upconversion via coherent magnon-magnon interactions - a phenomenon that opens the paradigm of nonlinear coupled magnonics. By using a suite of advanced spectroscopic tools, including a newly demonstrated two-dimensional (2D) THz polarimetry technique enabled by single-shot detection, we unveil the unidirectional nature of coupling between distinct magnon modes of a canted antiferromagnet. Calculations of spin dynamics further suggest that this coupling is a universal feature of antiferromagnets with canted magnetic moments. These results demonstrate a route to inducing desirable energy transfer pathways between coherent magnons in solids and pave the way for a new era in the development of magnonic signal processing devices

Rehabilitation outcome following war-related below-knee amputation in Kosovo: observational retrospective study

Glass-forming materials are employed in information storage technologies making use of the transition between a disordered (amorphous) and an ordered (crystalline) state. With increasing temperature, the crystal growth velocity of these phase-change materials becomes so fast that prior studies have not been able to resolve these crystallization dynamics. However, crystallization is the time-limiting factor in the write speed of phase-change memory devices. Here, for the first time, we quantify crystal growth velocities up to the melting point using the relaxation of photoexcited carriers as an ultrafast heating mechanism. During repetitive femtosecond optical excitation, each pulse enables dynamical evolution for tens of picoseconds before the intermediate atomic structure is frozen-in as the sample rapidly cools. We apply this technique to $Ag_{4}In_{3}Sb_{67}Te_{26}$ (AIST) and compare the dynamics of as-deposited and application-relevant melt-quenched glass. Both glasses retain their different kinetics even in the supercooled liquid state, thereby revealing differences in their kinetic fragilities. This approach enables the characterization of application-relevant properties of phase-change materials up to the melting temperature, which has not been possible before