32 research outputs found
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.Comment: 22 pages, 4 figure
Carrier confinement and bond softening in photoexcited bismuth films
Femtosecond pump-probe spectroscopy of bismuth thin films has revealed strong dependencies of reflectivity and phonon frequency on film thickness in the range of 25−40 nm. The reflectivity variations are ascribed to distinct electronic structures originating from strongly varying electronic temperatures and proximity of the film thickness to the optical penetration depth of visible light. The phonon frequency is redshifted by an amount that increases with decreasing film thickness under the same excitation fluence, indicating carrier density-dependent bond softening that increases due to suppressed diffusion of carriers away from the photoexcited region in thin films. The results have significant implications for nonthermal melting of bismuth as well as lattice heating due to inelastic electron-phonon scattering.United States. Office of Naval Research (Grant N00014-12-1-0530)National Science Foundation (U.S.) (Grant CHE-1111557
The persistence of memory in ionic conduction probed by nonlinear optics
Predicting practical rates of transport in condensed phases enables the rational design of materials, devices and processes. This is especially critical to developing low-carbon energy technologies such as rechargeable batteries1,2,3. For ionic conduction, the collective mechanisms4,5, variation of conductivity with timescales6,7,8 and confinement9,10, and ambiguity in the phononic origin of translation11,12, call for a direct probe of the fundamental steps of ionic diffusion: ion hops. However, such hops are rare-event large-amplitude translations, and are challenging to excite and detect. Here we use single-cycle terahertz pumps to impulsively trigger ionic hopping in battery solid electrolytes. This is visualized by an induced transient birefringence, enabling direct probing of anisotropy in ionic hopping on the picosecond timescale. The relaxation of the transient signal measures the decay of orientational memory, and the production of entropy in diffusion. We extend experimental results using in silico transient birefringence to identify vibrational attempt frequencies for ion hopping. Using nonlinear optical methods, we probe ion transport at its fastest limit, distinguish correlated conduction mechanisms from a true random walk at the atomic scale, and demonstrate the connection between activated transport and the thermodynamics of information
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
Myeloid-specific Asxl2 deletion limits diet-induced obesity by regulating energy expenditure
We previously established that global deletion of the enhancer of trithorax and polycomb (ETP) gene, Asxl2, prevents weight gain. Because proinflammatory macrophages recruited to adipose tissue are central to the metabolic complications of obesity, we explored the role of ASXL2 in myeloid lineage cells. Unexpectedly, mice without Asxl2 only in myeloid cells (Asxl2ΔLysM) were completely resistant to diet-induced weight gain and metabolically normal despite increased food intake, comparable activity, and equivalent fecal fat. Asxl2ΔLysM mice resisted HFD-induced adipose tissue macrophage infiltration and inflammatory cytokine gene expression. Energy expenditure and brown adipose tissue metabolism in Asxl2ΔLysM mice were protected from the suppressive effects of HFD, a phenomenon associated with relatively increased catecholamines likely due to their suppressed degradation by macrophages. White adipose tissue of HFD-fed Asxl2ΔLysM mice also exhibited none of the pathological remodeling extant in their control counterparts. Suppression of macrophage Asxl2 expression, via nanoparticle-based siRNA delivery, prevented HFD-induced obesity. Thus, ASXL2 controlled the response of macrophages to dietary factors to regulate metabolic homeostasis, suggesting modulation of the cells\u27 inflammatory phenotype may impact obesity and its complications
Ultrafast measurements of mode-specific deformation potentials of BiTe and BiSe
Quantifying electron-phonon interactions for the surface states of
topological materials can provide key insights into surface-state transport,
topological superconductivity, and potentially how to manipulate the surface
state using a structural degree of freedom. We perform time-resolved x-ray
diffraction (XRD) and angle-resolved photoemission (ARPES) measurements on
BiTe and BiSe, following the excitation of coherent A
optical phonons. We extract and compare the deformation potentials coupling the
surface electronic states to local A-like displacements in these two
materials using the experimentally determined atomic displacements from XRD and
electron band shifts from ARPES.We find the coupling in BiTe and
BiSe to be similar and in general in agreement with expectations from
density functional theory. We establish a methodology that quantifies the
mode-specific electron-phonon coupling experimentally, allowing detailed
comparison to theory. Our results shed light on fundamental processes in
topological insulators involving electron-phonon coupling
Measurements of nonequilibrium interatomic forces using time-domain x-ray scattering
We demonstrate an experimental approach to determining the excited-state interatomic forces using femtosecond x-ray pulses from an x-ray free-electron laser. We determine experimentally the excited-state interatomic forces that connect photoexcited carriers to the nonequilibrium lattice dynamics in the prototypical Peierls-distorted material, bismuth. The forces are obtained by a constrained least-squares fit of a pairwise interatomic force model to the excited-state phonon dispersion relation as measured by the time- and momentum-resolved x-ray diffuse scattering. We find that photoexcited carriers weaken predominantly the nearest-neighbor forces, which drives the measured softening of the transverse acoustic modes throughout the Brillouin zone as well as the zone-center A1g optical mode. This demonstrates a bond-selective approach to measuring electron-phonon coupling relevant to a broad range of photoinduced phase transitions and transient light-driven states in quantum materials
Direct measurement of anharmonic decay channels of a coherent phonon
We report channel-resolved measurements of the anharmonic coupling of the coherent A1g phonon in photoexcited bismuth to pairs of high wave vector acoustic phonons. The decay of a coherent phonon can be understood as a parametric resonance process whereby the atomic displacement periodically modulates the frequency of a broad continuum of modes. This coupling drives temporal oscillations in the phonon mean-square displacements at the A1g frequency that are observed across the Brillouin zone by femtosecond x-ray diffuse scattering. We extract anharmonic coupling constants between the A1g and several representative decay channels that are within an order of magnitude of density functional perturbation theory calculations