Ultrafast Structural Phase Transition Driven by Photoinduced Melting of Charge and Orbital Order

Beaud, P.; Johnson, S. L.; Vorobeva, Ekaterina; Staub, U.; Souza, R. A. de; Milne, Christopher J.; Jia, Q. X.; Ingold, G.

doi:10.1103/physrevlett.103.155702

Cited by 117 publications

(106 citation statements)

References 25 publications

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“…According to Raman spectroscopy by Amelitchev and co-workers the 2 THz coherent oscillation corresponds to an A g mode, that strongly depends on the A-cation mass and is accordingly attributed to vibrations of Pr/Ca atoms. [48,49] Clearly, introducing disorder into the CO state via long living hot polaron states can induce structural rearrangements, which trigger coherent motion of the Mn, O, and the Pr/Ca atoms. The strong change of the amplitude of the THz oscillations at T CO (Figure 5d) is a consequence of this effect.…”

Section: Discussionmentioning

confidence: 99%

Evolution of Hot Polaron States with a Nanosecond Lifetime in a Manganite Perovskite

Raiser

Mildner

Ifland

et al. 2017

Advanced Energy Materials

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Understanding and controlling the relaxation process of optically excited charge carriers in solids with strong correlations is of great interest in the quest for new strategies to exploit solar energy. Usually, optically excited electrons in a solid thermalize rapidly on a femtosecond to picosecond timescale due to interactions with other electrons and phonons. New mechanisms to slow down thermalization will thus be of great significance for efficient light energy conversion, e.g., in photovoltaic devices. Ultrafast optical pump–probe experiments in the manganite Pr0.65Ca0.35MnO3, a photovoltaic, thermoelectric, and electrocatalytic material with strong polaronic correlations, reveal an ultraslow recombination dynamics on a nanosecond‐time scale. The nature of long living excitations is further elucidated by photovoltaic measurements, showing the presence of photodiffusion of excited electron–hole polaron pairs. Theoretical considerations suggest that the excited charge carriers are trapped in a hot polaron state. Escape from this state is possible via a slow dipole‐forbidden recombination process or via rare thermal fluctuations toward a conical intersection followed by a radiation‐less decay. The strong correlation between the excited polaron and the octahedral dynamics of its environment appears to be substantial for stabilizing the hot polaron.

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Section: Discussionmentioning

confidence: 99%

Evolution of Hot Polaron States with a Nanosecond Lifetime in a Manganite Perovskite

Raiser

Mildner

Ifland

et al. 2017

Advanced Energy Materials

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“…Resonant phonon excitation minimizes both electron and lattice heating: two detrimental effects that are difficult to avoid under non-discriminative pumping of materials with convenient near-IR or visible lasers. Apart from inducing metallicity, phononic excitation has been employed to melt orbital order 116 and trigger strong effective magnetic fields 117 . A particularly intriguing series of experiments has reported on phononically driven enhancement of superconducting correlations both in the cuprates and in K 3 C 60 (refs 103,118).…”

Section: Phononic Controls Of Quantum Materialsmentioning

confidence: 99%

Towards properties on demand in quantum materials

2017

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Q uantum materials are on the ascent. This term embodies a vast portfolio of compounds and phenomena where ramifications of quantum mechanics are demonstrably real. Quantum materials are in the vanguard of contemporary physics in part because these systems afford an exceptional venue to uncover the many roles of symmetry, topology, dimensionality and strong correlations in macroscopic observables. Here we set out to explore the ways and means of creating new states of matter in quantum materials and manipulating their phases via external stimuli. Practical control of these properties is a precondition for exploiting quantum advantages in new photonic, electronic and energy technologies, a task of significant societal impact 1 . We will primarily focus on the following classes of quantum materials: transition metal oxides, Fe-and Cu-based high-T c superconductors, van der Waals semiconductors, topological insulators and Weyl semimetals, and, finally, graphene.The properties of quantum materials are anomalously sensitive to external stimuli. In these systems, interactions associated with spin, charge, lattice and orbital degrees of freedom are commonly on par with the electronic kinetic energy. A rather fragile balance between coexisting and competing ground states can be readily shifted via external stimuli, leading to a raft of quantum phases and transitions between them 2,3 . Furthermore, certain classes of driven quantum states (Fig. 1a and Box 1) are explicit products of coherent interaction between light and matter 4-6 . Alternatively, the properties of quantum materials can be pre-programmed by directly manipulating the electronic wavefunction and the attendant Berry phase that give rise to the anomalous velocity of electrons in a solid [7][8][9] . These complementary avenues of controls mean that investigations no longer need to be reduced to merely observing (in contrast, for example, to astrophysics). Instead, it is now feasible to attain, in a predictable fashion, 'properties on demand' by steering a quantum material towards a desirable ground, metastable or transient state. 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 th...

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“…At thermodynamic equilibrium, the corresponding many-body interactions lead to rich phase diagrams as a function of temperature, pressure or doping. Such compounds also display fascinating out-of-equilibrium physics, in the form of ultra-fast symmetry changes known as photoinduced phase transitions [4][5][6], and occurrence of new, transient states [6][7][8].Charge density wave (CDW) states are broken symmetry states of metals arising from electron-phonon interactions. They are characterized by a periodic modulation of both atomic positions and electron density.…”

mentioning

confidence: 99%

Ultrafast Formation of a Charge Density Wave State in 1T−TaS2 : Observation at Nanometer Scales Using Time-Resolved X-Ray Diffraction

et al. 2017

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Femtosecond time-resolved X-ray diffraction is used to study a photo-induced phase transition between two charge density wave (CDW) states in 1T-TaS2, namely the nearly commensurate (NC) and the incommensurate (I) CDW states. Structural modulations associated with the NC-CDW order are found to disappear within 400 fs. The photo-induced I-CDW phase then develops through a nucleation/growth process which ends 100 ps after laser excitation. We demonstrate that the newly formed I-CDW phase is fragmented into several nanometric domains that are growing through a coarsening process. The coarsening dynamics is found to follow the universal Lifshitz-Allen-Cahn growth law, which describes the ordering kinetics in systems exhibiting a non-conservative order parameter.Among strongly correlated electron systems, superconductors and materials exhibiting metal-insulator transitions are usually characterized by strong electronelectron and electron-phonon couplings [1][2][3]. At thermodynamic equilibrium, the corresponding many-body interactions lead to rich phase diagrams as a function of temperature, pressure or doping. Such compounds also display fascinating out-of-equilibrium physics, in the form of ultra-fast symmetry changes known as photoinduced phase transitions [4][5][6], and occurrence of new, transient states [6][7][8].Charge density wave (CDW) states are broken symmetry states of metals arising from electron-phonon interactions. They are characterized by a periodic modulation of both atomic positions and electron density. The metal-to-CDW phase transition is characterized by the growth of a complex-valued order parameter p = A exp iΦ , which reflects both the amplitude A and the phase Φ of the periodic modulation [3]. A number of photo-induced phase transitions that have been achieved in CDW compounds correspond to a suppression of the CDW order, i.e. a transition between a CDW state and a metallic state free of any structural modulation [5,[9][10][11][12][13][14][15]. Among those, the photo-induced suppression of the CDW state in blue bronze was shown to involve a coherent motion of atoms along the normal coordinates of the CDW amplitude mode [5]. In this case, the amplitude mode allows continuous variations of the modulus of the order parameter |p|, the metallic state corresponding to |p|=0. In the present work, we focus on the photo-induced phase transition between the nearly commensurate (NC) and the incommensurate (I) CDW states in 1T-TaS 2 , which exhibit two distinct order parameters. When thermallyinduced, this first-order phase transition involves a discontinuous change of atomic positions, and a coexistence of NC and I phase domains over a 3 K range [16,17]. It is thus expected that the photo-induced I phase appears through non-coherent atomic motions, by a nucleation/growth process. We report that the photo-induced NC → I phase is completed within 100 ps after laser excitation. At this 100 ps delay, the photo-induced I-CDW phase is found divided into domains with a typical size of 150Å. Its ordering kinet...

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Ultrafast Structural Phase Transition Driven by Photoinduced Melting of Charge and Orbital Order

Cited by 117 publications

References 25 publications

Evolution of Hot Polaron States with a Nanosecond Lifetime in a Manganite Perovskite

Evolution of Hot Polaron States with a Nanosecond Lifetime in a Manganite Perovskite

Towards properties on demand in quantum materials

Ultrafast Formation of a Charge Density Wave State in 1T−TaS2 : Observation at Nanometer Scales Using Time-Resolved X-Ray Diffraction

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