The non-equilibrium control of emergent phenomena in solids is an important research frontier, encompassing effects like the optical enhancement of superconductivity 1 . Recently, nonlinear excitation 2 , 3 of certain phonons in bilayer cuprates was shown to induce superconducting-like optical properties at temperatures far above T c 4,5,6 . This effect was accompanied by the disruption of competing charge-density-wave correlations 7,8 , which explained some but not all of the experimental results. Here, we report a similar phenomenon in a very different compound. By exciting metallic K 3 C 60 with mid-infrared optical pulses, we induce a large increase in carrier mobility, accompanied by the opening of a gap in the optical conductivity. Strikingly, these sameReprints and permissions information is available online at www.nature.com/reprints.Users may view, print, copy, and download text and data-mine the content in such documents, for the purposes of academic research, subject always to the full Conditions of use:http://www.nature.com/authors/editorial_policies/license.html#termsCorrespondence and request for materials should be addressed to An.C. (andrea.cavalleri@mpsd.mpg.de). Author Contributions

The optical properties of graphene are made unique by the linear band structure and the vanishing density of states at the Dirac point. It has been proposed that even in the absence of a bandgap, a relaxation bottleneck at the Dirac point may allow for population inversion and lasing at arbitrarily long wavelengths. Furthermore, efficient carrier multiplication by impact ionization has been discussed in the context of light harvesting applications. However, all of these effects are difficult to test quantitatively by measuring the transient optical properties alone, as these only indirectly reflect the energy- and momentum-dependent carrier distributions. Here, we use time- and angle-resolved photoemission spectroscopy with femtosecond extreme-ultraviolet pulses to directly probe the non-equilibrium response of Dirac electrons near the K-point of the Brillouin zone. In lightly hole-doped epitaxial graphene samples, we explore excitation in the mid- and near-infrared, both below and above the minimum photon energy for direct interband transitions. Whereas excitation in the mid-infrared results only in heating of the equilibrium carrier distribution, interband excitations give rise to population inversion, suggesting that terahertz lasing may be possible. However, in neither excitation regime do we find any indication of carrier multiplication, questioning the applicability of graphene for light harvesting.

A central mystery in high-temperature superconductivity is the origin of the so-called strange metal (i.e., the anomalous conductor from which superconductivity emerges at low temperature). Measuring the dynamic charge response of the copper oxides, [Formula: see text], would directly reveal the collective properties of the strange metal, but it has never been possible to measure this quantity with millielectronvolt resolution. Here, we present a measurement of [Formula: see text] for a cuprate, optimally doped BiSrCaCuO ( = 91 K), using momentum-resolved inelastic electron scattering. In the medium energy range 0.1-2 eV relevant to the strange metal, the spectra are dominated by a featureless, temperature- and momentum-independent continuum persisting to the electronvolt energy scale. This continuum displays a simple power-law form, exhibiting behavior at low energy and/ behavior at high energy. Measurements of an overdoped crystal ( = 50 K) showed the emergence of a gap-like feature at low temperature, indicating deviation from power law form outside the strange-metal regime. Our study suggests the strange metal exhibits a new type of charge dynamics in which excitations are local to such a degree that space and time axes are decoupled.

We report on ultrafast optical experiments in which femtosecond midinfrared radiation is used to excite the lattice of complex oxide heterostructures. By tuning the excitation energy to a vibrational mode of the substrate, a long-lived five-order-of-magnitude increase of the electrical conductivity of NdNiO(3) epitaxial thin films is observed as a structural distortion propagates across the interface. Vibrational excitation, extended here to a wide class of heterostructures and interfaces, may be conducive to new strategies for electronic phase control at THz repetition rates.

One of the most fundamental properties of an interacting electron system is its frequency-and wave-vector-dependent density response function, χ(q, ω). The imaginary part, χ (q, ω), defines the fundamental bosonic charge excitations of the system, exhibiting peaks wherever collective modes are present. χ quantifies the electronic compressibility of a material, its response to external fields, its ability to screen charge, and its tendency to form charge density waves. Unfortunately, there has never been a fully momentum-resolved means to measure χ(q, ω) at the meV energy scale relevant to modern electronic materials. Here, we demonstrate a way to measure χ with quantitative momentum resolution by applying alignment techniques from x-ray and neutron scattering to surface high-resolution electron energy-loss spectroscopy (HR-EELS). This approach, which we refer to here as "M-EELS", allows direct measurement of χ (q, ω) with meV resolution while controlling the momentum with an accuracy better than a percent of a typical Brillouin zone. We apply this technique to finite-q excitations in the optimally-doped high temperature superconductor, Bi 2 Sr 2 CaCu 2 O 8+x (Bi2212), which exhibits several phonons potentially relevant to dispersion anomalies observed in ARPES and STM experiments. Our study defines a path to studying the long-sought collective charge modes in quantum materials at the meV scale and with full momentum control.

Optical excitation at terahertz frequencies has emerged as an effective means to dynamically manipulate complex materials. In the molecular solid K3C60, short mid-infrared pulses transform the high-temperature metal into a non-equilibrium state with the optical properties of a superconductor. Here we tune this effect with hydrostatic pressure and find that the superconducting-like features gradually disappear at around 0.3 GPa. Reduction with pressure underscores the similarity with the equilibrium superconducting phase of K3C60, in which a larger electronic bandwidth induced by pressure is also detrimental for pairing. Crucially, our observation excludes alternative interpretations based on a high-mobility metallic phase. The pressure dependence also suggests that transient, incipient superconductivity occurs far above the 150 K hypothesised previously, and rather extends all the way to room temperature.

Abstract:We use midinfrared pulses with stable carrier-envelope phase offset to drive molecular vibrations in the charge transfer salt ET-F2TCNQ, a prototypical one-dimensional Mott insulator. We find that the Mott gap, which is probed resonantly with 10 fs laser pulses, oscillates with the pump field. This observation reveals that molecular excitations can coherently perturb the electronic on-site interactions (Hubbard U) by changing the local orbital wave function. The gap oscillates at twice the frequency of the vibrational mode, indicating that the molecular distortions couple quadratically to the local charge density.

A normal metal exhibits a valence plasmon, which is a sound wave in its conduction electron density. The mysterious strange metal is characterized by non-Boltzmann transport and violates most fundamental Fermi liquid scaling laws. A fundamental question is: Do strange metals have plasmons? Using momentum-resolved inelastic electron scattering (M-EELS) we recently showed that, rather than a plasmon, optimally-doped Bi2.1Sr1.9Ca1.0Cu2.0O8+x (Bi-2212) exhibits a featureless, temperature-independent continuum with a power-law form over most energy and momentum scales [M. Mitrano, PNAS 115, 5392-5396 (2018)]. Here, we show that this continuum is present throughout the fan-shaped, strange metal region of the phase diagram. Outside this region, dramatic changes in spectral weight are observed: In underdoped samples, spectral weight up to 0.5 eV is enhanced at low temperature, biasing the system towards a charge order instability. The situation is reversed in the overdoped case, where spectral weight is strongly suppressed at low temperature, increasing quasiparticle coherence in this regime. Optimal doping corresponds to the boundary between these two opposite behaviors at which the response is temperature-independent. Our study suggests that plasmons do not exist as well-defined excitations in Bi-2212, and that a featureless continuum is a defining property of the strange metal, which is connected to a peculiar crossover where the spectral weight change undergoes a sign reversal. arXiv:1903.04038v2 [cond-mat.str-el]