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In solids, the response of the lattice to photo-excitation is often described by the inertial evolution on an impulsively modified potential energy surface which leads to coherent motion. However, it remains unknown if vibrational coherence is sustained through a phase transition, during which coupling between modes can be strong and may lead to rapid loss of coherence. Here we use coherent phonon spectroscopy to track lattice coherence in the structural phase transition of V$_2$O$_3$. In both the low and high symmetry phases unique coherent phonon modes are generated at low fluence. However, coherence is lost when driving between the low and high symmetry phases. Our results suggest non-inertial dynamics dominate during phase transition due to disorder and multi-mode coupling., Comment: 4 figures and supplementary information

Although ultrafast manipulation of magnetism holds great promise for new physical phenomena and applications, targeting specific states is held back by our limited understanding of how magnetic correlations evolve on ultrafast timescales. Using ultrafast resonant inelastic x-ray scattering we demonstrate that femtosecond laser pulses can excite transient magnons at large wavevectors in gapped antiferromagnets, and that they persist for several picoseconds which is opposite to what is observed in nearly gapless magnets. Our work suggests that materials with isotropic magnetic interactions are preferred to achieve rapid manipulation of magnetism., Comment: 6 pages, 4 figures, not including supplemental material; accepted in PNAS

Many remarkable properties of quantum materials emerge from states with intricate coupling between the charge, spin and orbital degrees of freedom. Ultrafast photo-excitations of these materials hold great promise for understanding and controlling the properties of these states. Here we introduce time-resolved resonant inelastic X-ray scattering (trRIXS) as a means of measuring charge, spin and orbital excitations out of equilibrium. These excitations encode the correlations and interactions that determine the detailed properties of the states generated. After outlining the basic principles and instrumentation of tr-RIXS, we review our first observations of transient antiferromagnetic correlations in quasi-two dimensions in a photo-excited Mott insulator and present possible future routes of this fast-developing technique. The increasing number of X-ray free electron laser facilities not only enables tackling long-standing fundamental scientific problems, but also promises to unleash novel inelastic X-ray scattering spectroscopies, Comment: 14 pages, 5 figures, supplementary information; Accepted in Philosophical Transactions A

Measuring how the magnetic correlations throughout the Brillouin zone evolve in a Mott insulator as charges are introduced dramatically improved our understanding of the pseudogap, non-Fermi liquids and high $T_C$ superconductivity. Recently, photoexcitation has been used to induce similarly exotic states transiently. However, understanding how these states emerge has been limited because of a lack of available probes of magnetic correlations in the time domain, which hinders further investigation of how light can be used to control the properties of solids. Here we implement magnetic resonant inelastic X-ray scattering at a free electron laser, and directly determine the magnetization dynamics after photo-doping the Mott insulator Sr$_2$IrO$_4$. We find that the non-equilibrium state 2~ps after the excitation has strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. The magnetism recovers its two-dimensional (2D) in-plane N\'eel correlations on a timescale of a few ps, while the three-dimensional (3D) long-range magnetic order restores over a far longer, fluence-dependent timescale of a few hundred ps. The dramatic difference in these two timescales, implies that characterizing the dimensionality of magnetic correlations will be vital in our efforts to understand ultrafast magnetic dynamics., Comment: 7 page, 4 figures; to appear in Nature Materials

Optical control of magnetism, of interest for high-speed data processing and storage, has only been demonstrated with near-infrared excitation to date. However, in absorbing materials, such high photon energies can lead to significant dissipation, making switch back times long and miniaturization challenging. In manganites, magnetism is directly coupled to the lattice, as evidenced by the response to external and chemical pressure, or to ferroelectric polarization. Here, femtosecond mid-infrared pulses are used to excite the lattice in La0.5Sr1.5MnO4 and the dynamics of electronic order are measured by femtosecond resonant soft x-ray scattering with an x-ray free electron laser. We observe that magnetic and orbital orders are reduced by excitation of the lattice. This process, which occurs within few picoseconds, is interpreted as relaxation of the complex charge-orbital-spin structure following a displacive exchange quench - a prompt shift in the equilibrium value of the magnetic and orbital order parameters after the lattice has been distorted. A microscopic picture of the underlying unidirectional lattice displacement is proposed, based on nonlinear rectification of the directly-excited vibrational field, as analyzed in the specific lattice symmetry of La0.5Sr1.5MnO4. Control of magnetism through ultrafast lattice excitation has important analogies to the multiferroic effect and may serve as a new paradigm for high-speed optomagnetism., Comment: 10 pages manuscript, 4 figures

Photo-excitation in complex oxides1 transfers charge across semicovalent bonds, drastically perturbing spin and orbital orders2. Light may then be used in compounds like magnetoresistive manganites to control magnetism on nanometre lengthscales and ultrafast timescales. Here, we show how ultrafast resonant soft x-ray diffraction can separately probe the photo-induced dynamics of spin and orbital orders in La0.5Sr1.5MnO4. Ultrafast melting of CE antiferromagnetic spin order is evidenced by the disappearance of a (1/4,1/4,1/2) diffraction peak. On the other hand the (1/4,1/4,0) peak, reflecting orbital order, is only partially reduced. Cluster calculations aid our interpretation by considering different magnetically ordered states accessible after photo-excitation. Nonthermal coupling between light and magnetism emerges as a primary aspect of photo-induced phase transitions in manganites., Comment: 7 pages manuscript, 4 figures

The competition between electron localization and de-localization in Mott insulators underpins the physics of strongly-correlated electron systems. Photo-excitation, which re-distributes charge between sites, can control this many-body process on the ultrafast timescale. To date, time-resolved studies have been performed in solids in which other degrees of freedom, such as lattice, spin, or orbital excitations come into play. However, the underlying quantum dynamics of bare electronic excitations has remained out of reach. Quantum many-body dynamics have only been detected in the controlled environment of optical lattices where the dynamics are slower and lattice excitations are absent. By using nearly-single-cycle near-IR pulses, we have measured coherent electronic excitations in the organic salt ET-F2TCNQ, a prototypical one-dimensional Mott Insulator. After photo-excitation, a new resonance appears on the low-energy side of the Mott gap, which oscillates at 25 THz. Time-dependent simulations of the Mott-Hubbard Hamiltonian reproduce the oscillations, showing that electronic delocalization occurs through quantum interference between bound and ionized holon-doublon pairs., Comment: 4 figures and supplementary information

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