Electron-Vibrational Energy Exchange in Nitrogen-Containing Plasma:a Comparison Between an Analytical Approach and a Kinetic Model

This paper investigates the electron-vibrational（e-V）energy exchange in nitrogencontaining plasma,which is very efficient in the case of gas discharge and high speed flow.Based on Harmonic oscillator approximation and the assumption of the e-V relaxation through a continuous series of Boltzmann distributions over the vibrational states,an analytic approach is derived from the proposed scaling relation of e-V transition rates.A full kinetic model is then investigated by numerically solving the state-to-state master equation for all vibrational levels.The analytical approach leads to a Landau-Teller（LT）-type equation for relaxation of vibrational energy,and predicts the relaxation time on the right order of magnitude.By comparison with the kinetic model,the LT-type equation is valid in typical electron temperatures in gas discharge.However,the analytical approach is not capable of describing the vibrational distribution function during the e-V process in which a full kinetic model is required.

Direct Observation of Electron-Vibration Coupling at MXene-Solvent Interface

MXenes,a new family of two-dimensional(2D)materials,have received extensive interest due to their fascinating physicochemical properties,such as outstandinglight-to-heat conversion efficiency.However,the photothermal conversion mechanism of MXenes is still poorly understood.Here,by using femtosecond visible and mid-infrared transient absorption spectroscopy,the electronic energy dissipation dynamics of MXene(Ti_(3)C_(2)T_(x))nanosheets dispersed in various solvents are carefully studied.Our results indicate that the lifetime of photoexcited MXene is strongly dependent on the surrounding environment.Especially,the interfacial electron-vibration coupling between the MXene nanosheets and the adjacent solvent molecules is directly observed following the ultrafast photoexcitation of MXene.It suggests that the interfacial interactions at the MXene-solvent interface play a critical role in the ultrafast energy transport dynamics of MXene,which offers a potentially feasible route for tailoring the light conversion properties of 2D systems.

Coherent Vibrational Dynamics of[Au_(25)(SR)_(18)]^(-) Nanoclusters

Coherent vibrational dynamics can be observed in atomically precise gold nanoclusters using femtosecond time-resolved pump-probe spectroscopy.It can not only reveal the coupling between electrons and vibrations,but also reflect the mechanical and electronic properties of metal nanoclusters,which holds potential applications in biological sensing and mass detection.Here,we investigated the coherent vibrational dynamics of[Au_(25)(SR)_(18)]^(-)nanoclusters by ultrafast spectroscopy and revealed the origins of thesecoherent vibrations by analyzing their frequency,phase and probe wavelength distributions.Strong coherent oscillations with frequency of 40 cm^(-1) and 80 cm^(-1) can be reproduced in the excited state dynamics of[Au_(25)(SR)_(18)]^(-),which should originate from acoustic vibrations of the Au13 metal core.Phase analysis on the oscillations indicates that the 80 cm^(-1) mode should arise from the frequency modulation of the electronic states while the 40 cm^(-1) mode should originate from the amplitude modulation of the dynamic spectrum.Moreover,it is found that the vibration frequencies of[Au_(25)(SR)_(18)]^(-)obtained in pump-probe measurements are independent of the surface ligands so that they are intrinsic properties of the metal core.These results are of great value to understand the electron-vibration coupling of metal nanoclusters.

Observations of abundant structural and electronic phases in potassium-doped single-layer p-quaterphenyl film

Scanning tunneling microscopy/spectroscopy is applied herein to study the pristine and potassium(K)-doped single-layer pquaterphenyl(P4P) films grown on the Au(111) substrate at the molecular level. Abundant complex structural and electronic phases are induced by various K doping. The Fermi-level pinning effect is observed at a low doping level. On the contrary,K3P4P exhibits intriguing versatile phases and properties because charge carriers are effectively doped in. For example, two kinds of molecular vibration modes with energies below 100 meV are observed, indicating a possible strong electron-phonon coupling. The splitting of the lowest unoccupied molecular orbital state in K3P4P illustrates an electronic correlation effect, and its strength varies for four different K3P4P phases with different structures. In addition, the appearance of a Kondo resonance on the molecular vacancy/impurity implies a local molecular magnetic moment. Our results demonstrate that the complex electronic properties of an alkali metal-doped P4P/Au film stem from the existence of many competing interactions, such as electronelectron correlations and electron-vibration coupling, which can be effectively tuned via variable carrier doping and molecular structure. Our work also opens new routes toward engineering novel molecular devices and creating new electronic phases in strongly correlated molecular materials.