Ultrafast Melting Research Articles

Infrared-induced ultrafast melting of nanostructured platinum films probed by an x-ray free-electron laser

Infrared-induced ultrafast melting of nanostructured platinum films probed by an x-ray free-electron laser

Interplay of thermal and nonthermal effects in x-ray-induced ultrafast melting

Interplay of thermal and nonthermal effects in x-ray-induced ultrafast melting

Structural pathways for ultrafast melting of optically excited thin polycrystalline Palladium films

Due to its extremely short timescale, the non-equilibrium melting of metals is exceptionally difficult to probe experimentally. The knowledge of melting mechanisms is thus based mainly on the results of theoretical predictions. This work reports on the investigation of ultrafast melting of thin polycrystalline Pd films studied by optical laser pump – X-ray free-electron laser probe experiments and molecular-dynamics simulations. By acquiring X-ray diffraction snapshots with sub-picosecond resolution, we capture the sample's atomic structure during its transition from the crystalline to the liquid state. Bridging the timescales of experiments and simulations allows us to formulate a realistic microscopic picture of the crystal-liquid transition. According to the experimental data, the melting process gradually accelerates with the increasing density of deposited energy. The molecular dynamics simulations reveal that the transition mechanism progressively varies from heterogeneous, initiated inside the material at structurally disordered grain boundaries, to homogenous, proceeding catastrophically in the crystal volume on a picosecond timescale comparable to that of electron-phonon coupling. We demonstrate that the existing models of strongly non-equilibrium melting, developed for systems with relatively weak electron-phonon coupling, remain valid even for ultrafast heating rates achieved in femtosecond laser-excited Pd. Furthermore, we highlight the role of pre-existing and transiently generated crystal defects in the transition to the liquid state.

Theoretical Studies of Anisotropic Melting of Ice Induced by Ultrafast Nonthermal Heating.

Water and ice are routinely studied with X-rays to reveal their diverse structures and anomalous properties. We employ a hybrid collisional-radiative/molecular-dynamics method to explore how femtosecond X-ray pulses interact with hexagonal ice. We find that ice makes a phase transition into a crystalline plasma where its initial structure is maintained up to tens of femtoseconds. The ultrafast melting process occurs anisotropically, where different geometric configurations of the structure melt on different time scales. The transient state and anisotropic melting of crystals can be captured by X-ray diffraction, which impacts any study of crystalline structures probed by femtosecond X-ray lasers.

Inverted nucleation for photoinduced nonequilibrium melting.

Ultrafast photoinduced melting provides an essential platform for studying nonequilibrium phase transitions by linking the kinetics of electron dynamics to ionic motions. Knowledge of dynamic balance in their energetics is essential to understanding how the ionic reaction is influenced by femtosecond photoexcited electrons with notable time lag depending on reaction mechanisms. Here, by directly imaging fluctuating density distributions and evaluating the ionic pressure and Gibbs free energy from two-temperature molecular dynamics that verified experimental results, we uncovered that transient ionic pressure, triggered by photoexcited electrons, controls the overall melting kinetics. In particular, ultrafast nonequilibrium melting can be described by the reverse nucleation process with voids as nucleation seeds. The strongly driven solid-to-liquid transition of metallic gold is successfully explained by void nucleation facilitated by photoexcited electron-initiated ionic pressure, establishing a solid knowledge base for understanding ultrafast nonequilibrium kinetics.

Atomistic-Continuum Study of an Ultrafast Melting Process Controlled by a Femtosecond Laser-Pulse Train.

In femtosecond laser fabrication, the laser-pulse train shows great promise in improving processing efficiency, quality, and precision. This research investigates the influence of pulse number, pulse interval, and pulse energy ratio on the lateral and longitudinal ultrafast melting process using an experiment and the molecular dynamics coupling two-temperature model (MD-TTM model), which incorporates temperature-dependent thermophysical parameters. The comparison of experimental and simulation results under single and double pulses proves the reliability of the MD-TTM model and indicates that as the pulse number increases, the melting threshold at the edge region of the laser spot decreases, resulting in a larger diameter of the melting region in the 2D lateral melting results. Using the same model, the lateral melting results of five pulses are simulated. Moreover, the longitudinal melting results are also predicted, and an increasing pulse number leads to a greater early-stage melting depth in the melting process. In the case of double femtosecond laser pulses, the pulse interval and pulse energy ratio also affect the early-stage melting depth, with the best enhancement observed with a 2 ps interval and a 3:7 energy ratio. However, pulse number, pulse energy ratio, and pulse interval do not affect the final melting depth with the same total energies. The findings mean that the phenomena of melting region can be flexibly manipulated through the laser-pulse train, which is expected to be applied to improve the structural precision and boundary quality.

Observing femtosecond orbital dynamics in ultrafast Ge melting with time-resolved resonant X-ray scattering.

Photoinduced nonequilibrium phase transitions have stimulated interest in the dynamic interactions between electrons and crystalline ions, which have long been overlooked within the Born-Oppenheimer approximation. Ultrafast melting before lattice thermalization prompted researchers to revisit this issue to understand ultrafast photoinduced weakening of the crystal bonding. However, the absence of direct evidence demonstrating the role of orbital dynamics in lattice disorder leaves it elusive. By performing time-resolved resonant X-ray scattering with an X-ray free-electron laser, we directly monitored the ultrafast dynamics of bonding orbitals of Ge to drive photoinduced melting. Increased photoexcitation of bonding electrons amplifies the orbital disturbance to expedite the lattice disorder approaching the sub-picosecond scale of the nonthermal regime. The lattice disorder time shows strong nonlinear dependence on the laser fluence with a crossover behavior from thermal-driven to nonthermal-dominant kinetics, which is also verified by ab initio and two-temperature molecular dynamics simulations. This study elucidates the impact of bonding orbitals on lattice stability with a unifying interpretation on photoinduced melting.

Ultrafast melting of charge-density wave fluctuations at room temperature in 1T-TiSe2 monitored under non-equilibrium conditions

We investigate the ultrafast lattice dynamics in 1T-TiSe2 using femtosecond reflection pump–probe and pump–pump–probe techniques at room temperature. The time-domain signals and Fourier-transformed spectra show the A1g phonon mode at 5.9 THz. Moreover, we observe an additional mode at ≈ 3 THz, corresponding to the charge-density wave (CDW) amplitude mode (AM), which is generally visible below Tc≈200 K. We argue that the emergence of the CDW amplitude mode at room temperature can be a consequence of fluctuations of order parameters based on the additional experiment using the pump–pump–probe technique, which exhibited suppression of the AM signal within the ultrafast timescale of ∼0.5 ps.

Two-temperature model for ultrafast melting of Au-based bimetallic films interacting with single-pulse femtosecond laser: Theoretical study of damage threshold

Ultrashort-pulse laser excitation and associated thermal damage of single-layer metallic films have been extensively studied both theoretically as well as experimentally. However, study of ultrafast heat transfer mechanism in bimetallic films, a topic of immense current interest for designing next-generation optical components with better thermal resilience, is limited to a low fluence regime. Moreover, available results for damage threshold (DT) of bimetallic films have several ambiguities. The current work is an attempt towards development of comprehensive theory for the DT of Au-based bimetallic films, analyzing its dependence on associated physical parameters and bridging the gap in existing literature. This has been achieved by developing fully implicit two-temperature model-based Python code. Excellent agreement of the predicted temperature profiles with recently reported [E. L. Gurevich, Y. Levy, S. V. Gurevich, and N. M. Bulgakova, Phys. Rev. B 95, 054305 (2017)] femtosecond laser irradiated Au film validates the code. Subsequently, the code is utilized to investigate the influence of different metallic substrates, $M$ ($M$ = Ni, Cr, Cu) on ultrafast melting damage of $\mathrm{Au}\text{/}M$ films excited by single-pulse femtosecond laser. Simulations carried out for increasing Au layer thickness revealed a nonmonotonic variation of DT for all substrates. This study also brought out an important observation that for every substrate metal, there exists an optimum Au thickness for maximizing the incipient and the complete melting threshold. Maximum achievable enhancement for $\mathrm{Au}\text{/}M$ films over pure Au are found to be 30%, 22%, and 14% with Cu, Ni, and Cr substrates, respectively. The observed distinction in maximum DT among three different $\mathrm{Au}\text{/}M$ targets is explained by developing appropriate thermophysical models. Finally, an empirical function is proposed here for expressing nonmonotonic variation of two-layer DTs. Very good agreement between the substrate-specific peak positions predicted by the proposed function and effective electron diffusion length arising from thermophysical analysis makes the modeling robust and applicable for a wide range of laser wavelengths as well as arbitrary combinations of bimetallic films.

Numerical insight into heat transfer in surface melting and ablation subject to femtosecond laser processing aluminum

In the present work, the heat transfer in surface melting and ablation subject to femtosecond laser processing aluminum is investigated by a proposed algorithm concentrating on the energy consumed by latent heat of melting. The electron temperature-dependent material optical and thermophysical properties are employed in solving the two-temperature model (TTM). The evolutions of electron temperature and ion temperature pave a spatiotemporal way for evaluating the surface melting and ablation. The validation of proposed model is carried out by comparing the numerically calculated ablation depth with the experimentally measured ablation depth. The fraction of liquid by taking the latent heat of melting into account is put forward to describe the surface melting. A mushy zone characterizing the surface melting is identified. The electron-ion coupled heat transfer is found to trigger the rapid expansion of the mushy zone and melting depth in ultrafast surface melting. The energy consumed by latent heat of melting accounts for the delay of melting initiation moment and smaller melting depth, but it is inappreciable to ablation. Moreover, the energy loss through thermal radiation is numerically proved to have a neglectable impact on surface melting and ablation.

Ultrafast Energy Transfer Process in Confined Gold Nanospheres Revealed by Femtosecond X-ray Imaging and Diffraction.

Femtosecond laser pulses drive nonequilibrium phase transitions via reaction paths hidden in thermal equilibrium. This stimulates interest to understand photoinduced ultrafast melting processes, which remains incomplete due to challenges in resolving accompanied kinetics at the relevant space-time resolution. Here, by newly establishing a multiplexing femtosecond X-ray probe, we have successfully revealed ultrafast energy transfer processes in confined Au nanospheres. Real-time images of electron density distributions with the corresponding lattice structures elucidate that the energy transfer begins with subpicosecond melting at the specimen boundary earlier than the lattice thermalization, and proceeds by forming voids. Two temperature molecular dynamics simulations uncovered the presence of both heterogeneous melting with the melting front propagation from surface and grain boundaries and homogeneous melting with random melting seeds and nanoscale voids. Supported by experimental and theoretical results, we provide a comprehensive atomic-scale picture that accounts for the ultrafast laser-induced melting and evaporation kinetics.

Single-shot selective femtosecond and picosecond infrared laser crystallization of an amorphous Ge/Si multilayer stack

Pulsed laser crystallization is an efficient annealing technique to obtain polycrystalline silicon or germanium films on non-refractory substrates. This is important for creating “flexible electronics” and can also be used to fabricate thin-film solar cells. In this work, near- and mid-infrared femtosecond and picosecond laser pulses were used to crystallize a Ge/Si multilayer stack consisting of alternating amorphous thin films of silicon and germanium. The use of infrared radiation at wavelengths of 1030 and 1500 nm with photon energies lower than the optical absorption edge in amorphous silicon allowed obtaining selective crystallization of germanium layers with a single laser shot. The phase composition of the irradiated stack was investigated by the Raman scattering technique. Several non-ablative regimes of ultrashort-pulse laser crystallization were found, from partial crystallization of germanium without intermixing the Ge/Si layers to complete intermixing of the layers with formation of GexSi1-x solid alloys. The roles of single- and two-photon absorption, thermal and non-thermal (ultrafast) melting processes, and laser-induced stresses in selective pico- and femtosecond laser annealing are discussed. It is concluded that, due to a mismatch of the thermal expansion coefficients between the adjacent stack layers, efficient explosive solid-phase crystallization of the Ge layers is possible at relatively low temperatures, well below the melting point.

Ultrafast Melting of Superconductivity in an Iron-Based Superconductor

Optical pumping of an ``unconventional'' iron-chalcogenide superconductor leads to a metastable state in which superconductivity disappears on very fast timescales, possibly due to magnetic correlations triggered by the pumping.

The seeds and homogeneous nucleation of photoinduced nonthermal melting in semiconductors due to self-amplified local dynamic instability.

Laser-induced nonthermal melting in semiconductors has been studied over the past four decades, but the underlying mechanism is still under debate. Here, by using an advanced real-time time-dependent density functional theory simulation, we reveal that the photoexcitation-induced ultrafast nonthermal melting in silicon occurs via homogeneous nucleation with random seeds originating from a self-amplified local dynamic instability. Because of this local dynamic instability, any initial small random thermal displacements of atoms can be amplified by a charge transfer of photoexcited carriers, which, in turn, creates a local self-trapping center for the excited carriers and yields the random nucleation seeds. Because a sufficient amount of photoexcited hot carriers must be cooled down to band edges before participating in the self-amplification of local lattice distortions, the time needed for hot carrier cooling is the response for the longer melting time scales at shorter laser wavelengths. This finding provides fresh insights into photoinduced ultrafast nonthermal melting.

Ultrafast atomic view of laser-induced melting and breathing motion of metallic liquid clusters with MeV ultrafast electron diffraction

Under the irradiation of an ultrafast intense laser, solid materials can be driven into nonequilibrium states undergoing an ultrafast solid-liquid phase transition. Understanding such nonequilibrium states is essential for scientific research and industrial applications because they exist in various processes including laser fusion and laser machining yet challenging in the sense that high resolution and single-shot capability are required for the measurements. Herein, an ultrafast diffraction technique with megaelectron-volt (MeV) electrons is used to resolve the atomic pathway over the entire laser-induced ultrafast melting process, from the initial loss of long-range order and the formation of high-density liquid to the progressive evolution of short-range order and relaxation into the metastable low-density liquid state. High-resolution measurements using electron pulse compression and a time-stamping technique reveal a coherent breathing motion of polyhedral clusters in transient liquid aluminum during the ultrafast melting process, as indicated by the oscillation of the interatomic distance between the center atom and atoms in the nearest-neighbor shell. Furthermore, contraction of interatomic distance was observed in a superheated liquid state with temperatures up to 6,000 K. The results provide an atomic view of melting accompanied with internal pressure relaxation and are critical for understanding the structures and properties of matter under extreme conditions.

Multi-mode excitation drives disorder during the ultrafast melting of a C4-symmetry-broken phase

Spontaneous C4-symmetry breaking phases are ubiquitous in layered quantum materials, and often compete with other phases such as superconductivity. Preferential suppression of the symmetry broken phases by light has been used to explain non-equilibrium light induced superconductivity, metallicity, and the creation of metastable states. Key to understanding how these phases emerge is understanding how C4 symmetry is restored. A leading approach is based on time-dependent Ginzburg-Landau theory, which explains the coherence response seen in many systems. However, we show that, for the case of the single layered manganite La0.5Sr1.5MnO4, the theory fails. Instead, we find an ultrafast inhomogeneous disordering transition in which the mean-field order parameter no longer reflects the atomic-scale state of the system. Our results suggest that disorder may be common to light-induced phase transitions, and methods beyond the mean-field are necessary for understanding and manipulating photoinduced phases.

Selective ultrashort laser annealing of amorphous Ge/Si multilayer stacks

We report on single-short laser crystallization of Ge/Si multilayer stacks consisting of alternating amorphous nanosized films of silicon and germanium using near- and mid-infrared femtosecond and picosecond laser pulses. The phase composition of the irradiated stacks was investigated by the Raman scattering technique. Several non-ablative regimes of crystallization were found, from partial crystallization of germanium without intermixing the Ge/Si layers to complete intermixing of the layers with formation of GexSi1-x solid alloys. The roles of one- and two-photon absorption, thermal and non-thermal (ultrafast) melting processes, and laser-induced stresses in selective pico- and femtosecond laser annealing are analysed based on theoretical estimations and comparison with experimental data. It is concluded that, due to a mismatch of the thermal expansion coefficients between the adjacent stack layers, efficient explosive solid-phase crystallization of the Ge layers is possible at relatively low temperatures, well below the melting point. The possibility of ultrafast non-thermal phase transition in germanium in the studied regimes is also discussed.

Femtosecond optical breakdown in silicon

We investigate photo-ionization, energy deposition, plasma formation and the ultrafast optical breakdown in crystalline silicon irradiated by intense near-infrared laser pulses with duration τ≤ 100 fs. The occurrence of high-intensity breakdown was established by the sudden increase of the absorbed laser energy inside the bulk, which corresponds to threshold energy fluence Φth> 1 J/cm2. The optical breakdown is accompanied by severe spectral broadening of the transmitted pulse. For the studied irradiation conditions, we find that the threshold fluence increases linearly with the increase of the pulse duration, while the corresponding laser intensity threshold decreases. The effect of the high plasma density on the stability of diamond lattice is also examined. For near threshold fluences, when about 5 % of valence electrons are promoted into the conduction band, the Si–Si bonds are softened and large Fermi degeneracy pressure arises (with pressure up to 100 kbar). The mechanical instability of the diamond lattice suggests that the large number of electron–hole pairs leads directly to ultrafast melting of the crystal structure.

Real-space observation of surface structuring induced by ultra-fast-laser illumination far below the melting threshold

Intense short laser pulses are an intriguing tool for tailoring surface properties via ultra-fast melting of the surface layer of an irradiated target. Despite extensive studies on the interaction of femto-second laser interaction with matter, the initial steps of the morphological changes are not yet fully understood. Here, we reveal that substantial surface structure changes occur at energy densities far below the melting threshold. By using low-temperature scanning tunneling microscopy we resolve atomic-scale changes, i.e. the creation of nanosized adatom and vacancy clusters. The two cluster types have distinct non-linear fluence-dependencies. A theoretical analysis reveals their creation and motion to be non-thermal in nature. The formation of these atomistic changes, individually resolved here for the first time, recast our understanding of how surfaces respond to low-intensity ultra-short laser illumination. A visualization and control of the initial morphological changes upon laser illumination are not only of fundamental interest, but pave the way for the designing material properties through surface structuring.

Ultrafast creation and melting of nonequilibrium excitonic condensates in bulk WSe2

We study the screened dynamics of the nonequilibrium excitonic consensate forming in a bulk WSe$_{2}$ when illuminated by coherent light resonant with the lowest-energy exciton. Intervalley scattering causes electron migration from the optically populated K valley to the conduction band minimum at $\Sigma$. Due to the electron-hole unbalance at the K point a plasma of quasi-free holes develops, which efficiently screens the interaction of the remaining excitons. We show that this plasma screening causes an ultrafast melting of the nonequilibrium consensate and that during melting coherent excitons and quasi-free electron-hole pairs coexist. The time-resolved spectral function does exhibit a conduction and excitonic sidebands of opposite convexity and relative spectral weight that changes in time. Both the dependence of the time-dependent conduction density on the laser intensity and the time-resolved spectral function agree with recent experiments.