Coherent Phonon Assisted Ultrafast Order-Parameter Reversal and Hidden Metallic State in Ta_{2}NiSe_{5}.

The nonequilibrium dynamics during photoinduced insulator-to-metal transition (IMT) in the excitonic insulator (EI) candidate Ta_{2}NiSe_{5} have been investigated, which reproduce the timescale and spectral features of the ultrafast switch and reveal intricate many-body interactions involving multidegrees of freedom. The key role of lattice order parameter (OP) reversal, occurring on a timescale comparable to that of purely electronic processes (<100  fs), is identified. This reversal is enabled by the anharmonic interactions between EI-OP-coupled phonons and the conventional coherent phonons, leading to a modified potential energy landscape and a high-frequency mode up-conversion.

Coherent ultrafast photoemission from a single quantized state of a one-dimensional emitter.

Femtosecond laser-driven photoemission source provides an unprecedented femtosecond-resolved electron probe not only for atomic-scale ultrafast characterization but also for free-electron radiation sources. However, for conventional metallic electron source, intense lasers may induce a considerable broadening of emitting energy level, which results in large energy spread (>600 milli-electron volts) and thus limits the spatiotemporal resolution of electron probe. Here, we demonstrate the coherent ultrafast photoemission from a single quantized energy level of a carbon nanotube.

Giant acceleration of polaron transport by ultrafast laser-induced coherent phonons.

Polaron formation is ubiquitous in polarized materials, but severely hampers carrier transport for which effective controlling methods are urgently needed. Here, we show that laser-controlled coherent phonon excitation enables orders of magnitude enhancement of carrier mobility via accelerating polaron transport in a prototypical material, lithium peroxide (LiO). The selective excitation of specific phonon modes, whose vibrational pattern directly overlap with the polaronic lattice deformation, can remarkably reduce the energy barrier for polaron hopping.

Super-resolved time-frequency measurements of coupled phonon dynamics in a 2D quantum material.

Methods to probe and understand the dynamic response of materials following impulsive excitation are important for many fields, from materials and energy sciences to chemical and neuroscience. To design more efficient nano, energy, and quantum devices, new methods are needed to uncover the dominant excitations and reaction pathways. In this work, we implement a newly-developed superlet transform-a super-resolution time-frequency analytical method-to analyze and extract phonon dynamics in a laser-excited two-dimensional (2D) quantum material.

Traversing Double-Well Potential Energy Surfaces: Photoinduced Concurrent Intralayer and Interlayer Structural Transitions in XTe (X = Mo, W).

The microscopic arrangement of atoms and molecules is the determining factor in how materials behave and perform; , the structure determines the property, a traditional paradigm in materials science. Photoexcitation-driven manipulation of the crystal structure and associated electronic properties in quantum materials provides opportunities for the exploration of exotic physics and practical applications; however, a generalized mechanism for such symmetry engineering is absent. Here, by ultrafast electron diffraction, structure factor calculation, and TDDFT-MD simulations, we report the photoinduced concurrent intralayer and interlayer structural transitions in the Td and 1T' phases of XTe (X = Mo, W).

Calibrating Out-of-Equilibrium Electron-Phonon Couplings in Photoexcited MoS.

Nonequilibrium electron-phonon coupling (EPC) serves as a dominant interaction in a multitude of transient processes, including photoinduced phase transitions, coherent phonon generation, and possible light-induced superconductivity. Here we use monolayer MoS as a prototype to investigate the variation in electron-phonon couplings under laser excitation, on the basis of real-time time-dependent density functional theory simulations. Phonon softening, anisotropic modification of the deformation potential, and enhancement of EPC are observed, which are attributed to the reduced electronic screening and modulated potential energy surfaces by photoexcitation.

Creation of a novel inverted charge density wave state.

Charge density wave (CDW) order is an emergent quantum phase that is characterized by periodic lattice distortion and charge density modulation, often present near superconducting transitions. Here, we uncover a novel inverted CDW state by using a femtosecond laser to coherently reverse the star-of-David lattice distortion in 1-TaSe. We track the signature of this novel CDW state using time- and angle-resolved photoemission spectroscopy and the time-dependent density functional theory to validate that it is associated with a unique lattice and charge arrangement never before realized.

Optical Control of Multistage Phase Transition via Phonon Coupling in MoTe_{2}.

The temporal characters of laser-driven phase transition from 2H to 1T^{'} has been investigated in the prototype MoTe_{2} monolayer. This process is found to be induced by fundamental electron-phonon interactions, with an unexpected phonon excitation and coupling pathway closely related to the nonequilibrium relaxation of photoexcited electrons. The order-to-order phase transformation is dissected into three substages, involving energy and momentum scattering processes from optical (A_{1}^{'} and E^{'}) to acoustic phonon modes [LA(M)] in subpicosecond timescale.

Indirect to Direct Charge Transfer Transition in Plasmon-Enabled CO Photoreduction.

Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon-enhanced photoelectronic processes such as photocatalysis, optical sensing and spectroscopic analysis. However, it is often challenging to identify specific dominant mechanisms for a given process because of the complex pathways and ultrafast interactive dynamics of the photoelectrons. Here, using CO reduction as an example, the underlying mechanisms of plasmon-driven catalysis at the single-molecule level using time-dependent density functional theory calculations is clearly probed.

Manipulating Weyl quasiparticles by orbital-selective photoexcitation in WTe.

Optical control of structural and electronic properties of Weyl semimetals allows development of switchable and dissipationless topological devices at the ultrafast scale. An unexpected orbital-selective photoexcitation in type-II Weyl material WTe is reported under linearly polarized light (LPL), inducing striking transitions among several topologically-distinct phases mediated by effective electron-phonon couplings. The symmetry features of atomic orbitals comprising the Weyl bands result in asymmetric electronic transitions near the Weyl points, and in turn a switchable interlayer shear motion with respect to linear light polarization, when a near-infrared laser pulse is applied.

Phase Transition Photodetection in Charge Density Wave Tantalum Disulfide.

The charge density wave (CDW) phase is a macroscopic quantum state with periodic charge density modulation accompanied by periodic lattice distortion in low-dimensional metals. External fields, such as an electric field and optical excitation, can trigger the transitions among different CDW states, leaving an under-explored mechanism and attracting great interest toward optoelectronic applications. Here, we explore a photoinduced phase transition in 1T-TaS under an electrical field.

Ultrafast charge ordering by self-amplified exciton-phonon dynamics in TiSe.

The origin of charge density waves (CDWs) in TiSe[Formula: see text] has long been debated, mainly due to the difficulties in identifying the timescales of the excitonic pairing and electron-phonon coupling (EPC). Without a time-resolved and microscopic mechanism, one has to assume simultaneous appearance of CDW and periodic lattice distortions (PLD). Here, we accomplish a complete separation of ultrafast exciton and PLD dynamics and unravel their interplay in our real-time time-dependent density functional theory simulations.

Extreme nonlinear strong-field photoemission from carbon nanotubes.

Strong-field photoemission produces attosecond (10 s) electron pulses that are synchronized to the waveform of the incident light. This nonlinear photoemission lies at the heart of current attosecond technologies. Here we report a new nonlinear photoemission behaviour-the nonlinearity in strong-field regime sharply increases (approaching 40th power-law scaling), making use of sub-nanometric carbon nanotubes and 800 nm pulses.

Photoexcitation Induced Quantum Dynamics of Charge Density Wave and Emergence of a Collective Mode in 1-TaS.

Photoexcitation is a powerful means in distinguishing different interactions and manipulating the states of matter, especially in charge density wave (CDW) materials. The CDW state of 1-TaS has been widely studied experimentally mainly because of its intriguing laser-induced ultrafast responses of electronic and lattice subsystems. However, the microscopic atomic dynamics and underlying electronic mechanism upon photoexcitation remain unclear.

Coexistence of Different Charge-Transfer Mechanisms in the Hot-Carrier Dynamics of Hybrid Plasmonic Nanomaterials.

Hot-carrier dynamics at the interfaces of semiconductors and nanoclusters is of significant importance for photovoltaic and photocatalytic applications. Plasmon-driven charge separation processes are considered to be only dependent on the type of donor-acceptor interactions, that is, the conventional hot-electron-transfer mechanism for van der Waals interactions and the plasmon-induced interfacial charge-transfer transition mechanism for chemical bonds. Here, we demonstrate that the two mechanisms can coexist in a nanoparticle-semiconductor hybrid nanomaterial, both leading to faster transfer than carrier relaxation.

Momentum-resolved TDDFT algorithm in atomic basis for real time tracking of electronic excitation.

Ultrafast electronic dynamics in solids lies at the core of modern condensed matter and materials physics. To build up a practical method for studying solids under photoexcitation, we develop a momentum-resolved real-time time dependent density functional theory (rt-TDDFT) algorithm using numerical atomic basis, together with the implementation of both the length and vector gauge of the electromagnetic field. When applied to simulate elementary excitations in two-dimensional materials such as graphene, different excitation modes, only distinguishable in momentum space, are observed.

Plasmon-induced nonlinear response of silver atomic chains.

Nonlinear response of a linear silver atomic chain upon ultrafast laser excitation has been studied in real time using the time-dependent density functional theory. We observe the presence of nonlinear responses up to the fifth order in tunneling current, which is ascribed to the excitation of high-energy electrons generated by Landau damping of plasmons. The nonlinear effect is enhanced after adsorption of polar molecules such as water due to the enhanced damping rates during plasmon decay.

Plasmon-driven sub-picosecond breathing of metal nanoparticles.

We present the first real-time atomistic simulation on the quantum dynamics of icosahedral silver nanoparticles under strong laser pulses, using time dependent density functional theory (TDDFT) molecular dynamics. We identify the emergence of sub-picosecond breathing-like radial oscillations starting immediately after laser pulse excitation, with increasing amplitude as the field intensity increases. The ultrafast dynamic response of nanoparticles to laser excitation points to a new mechanism other than equilibrium electron-phonon scattering previously assumed, which takes a much longer timescale.

Facile and straightforward synthesis of superparamagnetic reduced graphene oxide-Fe3O4 hybrid composite by a solvothermal reaction.

A superparamagnetic reduced graphene oxide-Fe(3)O(4) hybrid composite (rGO-Fe(3)O(4)) was prepared via a facile and straightforward method through the solvothermal reaction of iron (III) acetylacetonate (Fe(acac)(3)) and graphene oxide (GO) in ethylenediamine (EDA) and water. By this method, chemical reduction of GO as well as the formation of Fe(3)O(4) nanoparticles (NPs) can be achieved in one step. The Fe(3)O(4) NPs are firmly deposited on the surfaces of rGO, avoiding their reassembly to graphite.