Samuel W. Teitelbaum

Cooperative photoinduced metastable phase control in strained manganite films

A major challenge in condensed-matter physics is active control of quantum phases. Dynamic control with pulsed electromagnetic fields can overcome energetic barriers, enabling access to transient or metastable states that are not thermally accessible. Here we demonstrate strain-engineered tuning of La2/3Ca1/3MnO3 into an emergent charge-ordered insulating phase with extreme photo-susceptibility, where even a single optical pulse can initiate a transition to a long-lived metastable hidden metallic phase. Comprehensive single-shot pulsed excitation measurements demonstrate that the transition is cooperative and ultrafast, requiring a critical absorbed photon density to activate local charge excitations that mediate magnetic-lattice coupling that, in turn, stabilize the metallic phase. These results reveal that strain engineering can tune emergent functionality towards proximal macroscopic states to enable dynamic ultrafast optical phase switching and control.

Dual echelon femtosecond single-shot spectroscopy

We have developed a femtosecond single-shot spectroscopic technique to measure irreversible changes in condensed phase materials in real time. Crossed echelons generate a two-dimensional array of time-delayed pulses with one femtosecond probe pulse. This yields 9 ps of time-resolved data from a single laser shot, filling a gap in currently employed measurement methods. We can now monitor ultrafast irreversible dynamics in solid-state materials or other samples that cannot be flowed or replenished between laser shots, circumventing limitations of conventional pump-probe methods due to sample damage or product buildup. Despite the absence of signal-averaging in the single-shot measurement, an acceptable signal-to-noise level has been achieved via background and reference calibration procedures. Pump-induced changes in relative reflectivity as small as 0.2%-0.5% are demonstrated in semimetals, with both electronic and coherent phonon dynamics revealed by the data. The optical arrangement and the space-to-time conversion and calibration procedures necessary to achieve this level of operation are described. Sources of noise and approaches for dealing with them are discussed.

Extended two-temperature model for ultrafast thermal response of band gap materials upon impulsive optical excitation

Thermal modeling and numerical simulations have been performed to describe the ultrafast thermal response of band gap materials upon optical excitation. A model was established by extending the conventional two-temperature model that is adequate for metals, but not for semiconductors. It considers the time- and space-dependent density of electrons photoexcited to the conduction band and accordingly allows a more accurate description of the transient thermal equilibration between the hot electrons and lattice. Ultrafast thermal behaviors of bismuth, as a model system, were demonstrated using the extended two-temperature model with a view to elucidating the thermal effects of excitation laser pulse fluence, electron diffusivity, electron-hole recombination kinetics, and electron-phonon interactions, focusing on high-density excitation.

Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase

Excursions far from their equilibrium structures can bring crystalline solids through collective transformations including transitions into new phases that may be transient or long-lived. Direct spectroscopic observation of far-from-equilibrium rearrangements provides fundamental mechanistic insight into chemical and structural transformations, and a potential route to practical applications, including ultrafast optical control over material structure and properties. However, in many cases photoinduced transitions are irreversible or only slowly reversible, or the light fluence required exceeds material damage thresholds. This precludes conventional ultrafast spectroscopy in which optical excitation and probe pulses irradiate the sample many times, each measurement providing information about the sample response at just one probe delay time following excitation, with each measurement at a high repetition rate and with the sample fully recovering its initial state in between measurements. Using a single-shot, real-time measurement method, we were able to observe the photoinduced phase transition from the semimetallic, low-symmetry phase of crystalline bismuth into a high-symmetry phase whose existence at high electronic excitation densities was predicted based on earlier measurements at moderate excitation densities below the damage threshold. Our observations indicate that coherent lattice vibrational motion launched upon photoexcitation with an incident fluence above 10 mJ/cm2 in bulk bismuth brings the lattice structure directly into the high-symmetry configuration for tens of picoseconds, after which carrier relaxation and diffusion restore the equilibrium lattice configuration.