Inhomogeneous Photosusceptibility of VO_{2} Films at the Nanoscale.

Pump-probe nano-optical experiments were used to study the light-induced insulator to metal transition (IMT) in thin films of vanadium dioxide (VO_{2}), a prototypical correlated electron system. We show that inhomogeneous optical contrast is prompted by spatially uniform photoexcitation, indicating an inhomogeneous photosusceptibility of VO_{2}. We locally characterize temperature and time dependent variations of the photoexcitation threshold necessary to induce the IMT on picosecond timescales with hundred nanometer spatial resolution. We separately measure the critical temperature T_{L}, where the IMT onsets and the local transient electronic nano-optical contrast at the nanoscale. Our data reveal variations in the photosusceptibility of VO_{2} within nanoscopic regions characterized by the same critical temperature T_{L} where metallic domains can first nucleate.

Programmable hyperbolic polaritons in van der Waals semiconductors.

Collective electronic modes or lattice vibrations usually prohibit propagation of electromagnetic radiation through the bulk of common materials over a frequency range associated with these oscillations. However, this textbook tenet does not necessarily apply to layered crystals. Highly anisotropic materials often display nonintuitive optical properties and can permit propagation of subdiffractional waveguide modes, with hyperbolic dispersion, throughout their bulk. Here, we report on the observation of optically induced electronic hyperbolicity in the layered transition metal dichalcogenide tungsten diselenide (WSe2). We used photoexcitation to inject electron-hole pairs in WSe2 and then visualized, by transient nanoimaging, the hyperbolic rays that traveled along conical trajectories inside of the crystal. We establish here the signatures of programmable hyperbolic electrodynamics and assess the role of quantum transitions of excitons within the Rydberg series in the observed polaritonic response.

Ultrafast Enhancement of Ferromagnetic Spin Exchange Induced by Ligand-to-Metal Charge Transfer.

We theoretically predict and experimentally demonstrate a nonthermal pathway to optically enhance superexchange interaction energies in a material based on exciting ligand-to-metal charge-transfer transitions, which introduces lower-order virtual hopping contributions that are absent in the ground state. We demonstrate this effect in the layered ferromagnetic insulator CrSiTe_{3} by exciting Te-to-Cr charge-transfer transitions using ultrashort laser pulses and detecting coherent phonon oscillations that are impulsively generated by superexchange enhancement via magneto-elastic coupling. This mechanism kicks in below the temperature scale where short-range in-plane spin correlations begin to develop and disappears when the excitation energy is tuned away from the charge-transfer resonance, consistent with our predictions.

Nucleation and Growth Bottleneck in the Conductivity Recovery Dynamics of Nickelate Ultrathin Films.

We investigate THz conductivity dynamics in NdNiO3 and EuNiO3 ultrathin films (15 unit cells, u.c., ∼5.7 nm thick) following a photoinduced thermal quench into the metallic state and reveal a clear contrast between first- and second-order dynamics. While in EuNiO3 the conductivity recovers exponentially, in NdNiO3 the recovery is nonexponential and slower than a simple thermal model. Crucially, it is consistent with first-order dynamics and well-described by a 2d Avrami model, with supercooling leading to metastable phase coexistence on the nano- to mesoscopic scale. This novel observation is a fundamentally dynamic manifestation of the first-order character of the insulator-to-metal transition, which the nanoscale thickness of our films and their fast cooling rate enable us to detect. The large transients seen in our films are promising for fast electronic (and magnetic) switching applications.

Multi-messenger nanoprobes of hidden magnetism in a strained manganite.

The ground-state properties of correlated electron systems can be extraordinarily sensitive to external stimuli, offering abundant platforms for functional materials. Using the multi-messenger combination of atomic force microscopy, cryogenic scanning near-field optical microscopy, magnetic force microscopy and ultrafast laser excitation, we demonstrate both 'writing' and 'erasing' of a metastable ferromagnetic metal phase in strained films of La2/3Ca1/3MnO3 (LCMO) with nanometre-resolved finesse. By tracking both optical conductivity and magnetism at the nanoscale, we reveal how strain-coupling underlies the dynamic growth, spontaneous nanotexture and first-order melting transition of this hidden photoinduced metal. Our first-principles calculations reveal that epitaxially engineered Jahn-Teller distortion can stabilize nearly degenerate antiferromagnetic insulator and ferromagnetic metal phases. We propose a Ginzburg-Landau description to rationalize the co-active interplay of strain, lattice distortions and magnetism nano-resolved here in strained LCMO, thus guiding future functional engineering of epitaxial oxides into the regime of phase-programmable materials.

Towards properties on demand in quantum materials.

The past decade has witnessed an explosion in the field of quantum materials, headlined by the predictions and discoveries of novel Landau-symmetry-broken phases in correlated electron systems, topological phases in systems with strong spin-orbit coupling, and ultra-manipulable materials platforms based on two-dimensional van der Waals crystals. Discovering pathways to experimentally realize quantum phases of matter and exert control over their properties is a central goal of modern condensed-matter physics, which holds promise for a new generation of electronic/photonic devices with currently inaccessible and likely unimaginable functionalities. In this Review, we describe emerging strategies for selectively perturbing microscopic interaction parameters, which can be used to transform materials into a desired quantum state. Particular emphasis will be placed on recent successes to tailor electronic interaction parameters through the application of intense fields, impulsive electromagnetic stimulation, and nanostructuring or interface engineering. Together these approaches outline a potential roadmap to an era of quantum phenomena on demand.

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.

Anisotropic electronic state via spontaneous phase separation in strained vanadium dioxide films.

We resolved the enigma of anisotropic electronic transport in strained vanadium dioxide (VO2) films by inquiring into the role that strain plays in the nanoscale phase separation in the vicinity of the insulator-to-metal transition. The root source of the anisotropy was visualized as the formation of a peculiar unidirectional stripe state which accompanies the phase transition. Furthermore, nanoscale infrared spectroscopy unveils distinct facets of electron-lattice interplay at three different stages of the phase transition. These stages include the initial formation of sparse nonpercolating metallic domains without noticeable involvement of the lattice followed by an electron-lattice coupled anisotropic stripe state close to percolation which ultimately evolves into a nearly isotropic rutile metallic phase. Our results provide a unique mesoscopic perspective for the tunable macroscopic phenomena in strained metal oxide films.

Photoinduced phase transitions by time-resolved far-infrared spectroscopy in V2O3.

Using time-resolved far-infrared spectroscopy, we observe multiple routes for photoinduced phase transitions in V(2)O(3). This includes (i) a photothermal antiferromagnetic to paramagnetic transition and (ii) an incipient strain-generated paramagnetic metal to paramagnetic insulator transition, which manifests as coherent oscillations in the far-infrared conductivity. The ∼100 ps conductivity oscillation results from coherent acoustic phonon modulation of the bandwidth W. Our results indicate that poor metals are particularly amenable to coherent strain control of their electronic properties.

Reconfigurable terahertz metamaterials.

We demonstrate reconfigurable anisotropic metamaterials at terahertz frequencies where artificial "atoms" reorient within unit cells in response to an external stimulus. This is accomplished by fabricating planar arrays of split ring resonators on bimaterial cantilevers designed to bend out of plane in response to a thermal stimulus. We observe a marked tunability of the electric and magnetic response as the split ring resonators reorient within their unit cells. Our results demonstrate that adaptive metamaterials offer significant potential to realize novel electromagnetic functionality ranging from thermal detection to reconfigurable cloaks or absorbers.

Morphology effectively controls singlet-triplet exciton relaxation and charge transport in organic semiconductors.

We present a comparative study of ultrafast photoconversion dynamics in tetracene (Tc) and pentacene (Pc) single crystals and Pc films using optical pump-probe spectroscopy. Photoinduced absorption in Tc and Pc crystals is activated and temperature-independent, respectively, demonstrating dominant singlet-triplet exciton fission. In Pc films (as well as C60-doped films) this decay channel is suppressed by electron trapping. These results demonstrate the central role of crystallinity and purity in photogeneration processes and will constrain the design of future photovoltaic devices.

Polarization orientation dependence of the far infrared spectra of oriented single crystals of 1,3,5-trinitro-S-triazine (RDX) using terahertz time-domain spectroscopy.

The far infrared spectra of (100), (010), and (001)-oriented RDX single crystals were measured as the crystal was rotated about the axis perpendicular to the polarization plane of the incident radiation. Absorption measurements were taken at temperatures of both 20 K and 295 K for all rotations using terahertz time-domain spectroscopy. A number of discrete absorptions were found ranging from 10-100 cm(-1) (0.3-3 THz). The absorptions are highly dependent on the orientation of the terahertz polarization with respect to crystallographic axes.

Magnetic exchange interaction between rare-earth and Mn ions in multiferroic hexagonal manganites.

We report a study of magnetic dynamics in multiferroic hexagonal manganite HoMnO3 by far-infrared spectroscopy. The low-temperature magnetic excitation spectrum of HoMnO3 consists of magnetic-dipole transitions of Ho ions within the crystal-field split J = 8 manifold and of the triangular antiferromagnetic resonance of Mn ions. We determine the effective spin Hamiltonian for the Ho ion ground state. The magnetic-field splitting of the Mn antiferromagnetic resonance allows us to measure the magnetic exchange coupling between the rare-earth and Mn ions.

Detection of coherent magnons via ultrafast pump-probe reflectance spectroscopy in multiferroic Ba0.6Sr1.4Zn2Fe12O22.

We report the detection of a magnetic resonance mode in multiferroic Ba0.6Sr1.4Zn2Fe12O22 using time-domain pump-probe reflectance spectroscopy. Magnetic sublattice precession is coherently excited via picosecond thermal modification of the exchange energy. Importantly, this precession is recorded as a change in reflectance caused by the dynamic magnetoelectric effect. Thus, transient reflectance provides a sensitive probe of magnetization dynamics in materials with strong magnetoelectric coupling, such as multiferroics, revealing new possibilities for application in spintronics and ultrafast manipulation of magnetic moments.

Ultrafast carrier dynamics in an InAs/InGaAs quantum dots-in-a-well heterostructure.

Ultrafast differential transmission spectroscopy is used to explore temperature-dependent carrier dynamics in an InAs/InGaAs quantum dots-in-a-well heterostructure. Electron-hole pairs are optically injected into the three dimensional GaAs barriers, after which we monitor carrier relaxation into the two dimensional InGaAs quantum wells and the zero dimensional InAs quantum dots by tuning the probe photon energy. We find that carrier capture and relaxation are dominated by Auger carrier-carrier scattering at low temperatures, with thermal emission playing an increasing role with temperature. Our experiments provide essential insight into carrier relaxation across multiple spatial dimensions.

Coupling between an optical phonon and the Kondo effect.

We explore the ultrafast optical response of Yb14MnSb11, providing further evidence that this compound is the first d-electron, ferromagnetic, underscreened Kondo lattice. These results also provide the first demonstration of coupling between an optical phonon mode and the Kondo effect.

Observation of competing order in a high-Tc superconductor using femtosecond optical pulses.

We present studies of the photoexcited quasiparticle dynamics in Tl(2)Ba(2)Ca(2)Cu(3)O(y) (Tl-2223) using femtosecond optical techniques. Deep into the superconducting state (below 40 K), a dramatic change occurs in the temporal dynamics associated with photoexcited quasiparticles rejoining the condensate. This is suggestive of entry into a coexistence phase which, as our analysis reveals, opens a gap in the density of states (in addition to the superconducting gap), and furthermore, competes with superconductivity resulting in a depression of the superconducting gap.

Enhanced photosusceptibility near Tc for the light-induced insulator-to-metal phase transition in vanadium dioxide.

We use optical-pump terahertz-probe spectroscopy to investigate the near-threshold behavior of the photoinduced insulator-to-metal (IM) transition in vanadium dioxide thin films. Upon approaching Tc a reduction in the fluence required to drive the IM transition is observed, consistent with a softening of the insulating state due to an increasing metallic volume fraction (below the percolation limit). This phase coexistence facilitates the growth of a homogeneous metallic conducting phase following superheating via photoexcitation. A simple dynamic model using Bruggeman effective medium theory describes the observed initial condition sensitivity.

Dynamical electric and magnetic metamaterial response at terahertz frequencies.

Utilizing terahertz time domain spectroscopy, we have characterized the electromagnetic response of a planar array of split ring resonators (SRRs) fabricated upon a high resistivity GaAs substrate. The measured frequency dependent magnetic and electric resonances are in excellent agreement with theory and simulation. For two polarizations, the SRRs yield a negative electric response (epsilon < 0). We demonstrate, for the first time, dynamical control of the electrical response of the SRRs through photoexcitation of free carriers in the substrate. An excited carrier density of approximately 4 x 10(16) cm(-3) is sufficient to short the gap of the SRRs, thereby turning off the electric resonance, demonstrating the potential of such structures as terahertz switches. Because of the universality of metamaterial response over many decades of frequency, these results have implications for other regions of the electromagnetic spectrum.

Dynamic coupling-decoupling crossover in the current-driven vortex state in Tl2Ba2CaCu2O8 probed by the Josephson plasma resonance.

We have used terahertz spectroscopy to measure the Josephson plasma resonance in the superconductor Tl2Ba2CaCu2O8+delta. This allows us to probe the longitudinal ordering of pancake vortices as a function of applied ab-plane current in a 2.5 kG c-axis magnetic field. With increasing current in the low temperature vortex solid phase, we observe a decrease in the interlayer phase coherence consistent with a progressive misalignment of the pancake vortices in neighboring layers. In the high temperature vortex liquid phase, an increase in the longitudinal ordering occurs above a certain threshold current. Our results show evidence of a current-driven coupling-decoupling crossover in the pinned liquid phase.