VO2 is one of the most studied vanadium oxides because it undergoes a reversible metal-insulator transition (MIT) upon heating with a critical temperature of around 340 K. One of the most overlooked aspects of VO2 is the band’s anisotropy in the metallic phase when the Fermi level is crossed by two bands: π* and d||. They are oriented perpendicularly in one respect to the other, hence generating anisotropy. One of the parameters tuning MIT properties is the unbalance of the electron population of π* and d|| bands that arise from their different energy position with respect to the Fermi level. In systems with reduced dimensionality, the electron population disproportion is different with respect to the bulk leading to a different anisotropy. Investigating such a system with a band-selective spectroscopic tool is mandatory. In this manuscript, we show the results of the investigation of a single crystalline 8 nm VO2/TiO2(101) film. We report on the effectiveness of linearly polarized resonant photoemission (ResPES) as a band-selective technique probing the intrinsic anisotropy of VO2.
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J. Phys. Chem. C, 126, 27, 11174–11181, (2022)
Lifetime of Photogenerated Positive Charges in Hybrid Cerium Oxide-Based Materials from Space and Mirror Charge Effects in Time-Resolved Photoemission Spectroscopy
J.S. Pelli Cresi, E. Spurio, L. Di Mario, P. O’Keeffe, S. Turchini, S. Benedetti, G.M. Pierantozzi, A. De Vita, R. Cucini, D. Catone, and P. Luches
Space and mirror charge effects in time-resolved photoemission spectroscopy can be modeled to obtain relevant information on the recombination dynamics of charge carriers. We successfully extracted from these phenomena the reneutralization characteristic time of positive charges generated by photoexcitation in CeO2-based films. For the above-band-gap excitation, a large fraction of positive carriers with a lifetime that exceeds 100 ps are generated. Otherwise, the sub-band-gap excitation induces the formation of a significantly smaller fraction of charges with lifetimes of tens of picoseconds, ascribed to the excitation of defect sites or to multiphoton absorption. When the oxide is combined with Ag nanoparticles, the sub-band-gap excitation of localized surface plasmon resonances leads to reneutralization times longer than 300 ps. This was interpreted by considering the electronic unbalance at the surface of the nanoparticles generated by the injection of electrons, via localized surface plasmon resonance (LSPR) decay, into CeO2. This study represents an example of how to exploit the space charge effect in gaining access to the surface carrier dynamics in CeO2 within the picosecond range of time, which is fundamental to describe the photocatalytic processes.
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Phys. Rev. Materials, 5, 104403, (2021)
Identification of hidden orbital contributions in the La0.65Sr0.35MnO3 valence band
F. Offi, K. Yamauchi, S. Picozzi, V. Lollobrigida, A. Verna, C. Schlueter, T.-L. Lee, A. Regoutz, D. J. Payne, A. Petrov, G. Vinai, G. M. Pierantozzi, T. Pincelli, G. Panaccione, and F. Borgatti
Hybridization of electronic states and orbital symmetry in transition metal oxides are generally considered key ingredients in the description of both their electronic and magnetic properties. In the prototypical case of La0.65Sr0.35MnO3 (LSMO), a landmark system for spintronics applications, a description based solely on Mn 3d and O 2p electronic states is reductive. We thus analyzed elemental and orbital distributions in the LSMO valence band through a comparison between density functional theory calculations and experimental photoelectron spectra in a photon energy range from soft to hard x rays. We reveal a number of hidden contributions, arising specifically from La 5p, Mn 4s, and O 2s orbitals, considered negligible in previous analyses; our results demonstrate that all these contributions are significant for a correct description of the valence band of LSMO and of transition metal oxides in general.
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Small, 17, 2100050, (2021)
Quantitative Ultrafast Electron-Temperature Dynamics in Photo-Excited Au Nanoparticles
M. Sygletou, S. Benedetti, M. Ferrera, G.M. Pierantozzi, R. Cucini, G. Della Valle, P. Carrara, A. De Vita, A. di Bona, P. Torelli, D. Catone, Gi. Panaccione, M. Canepa, F. Bisio
The femtosecond evolution of the electronic temperature of laser-excited gold nanoparticles is measured, by means of ultrafast time-resolved photoemission spectroscopy induced by extreme-ultraviolet radiation pulses. The temperature of the electron gas is deduced by recording and fitting high-resolution photo emission spectra around the Fermi edge of gold nanoparticles providing a direct, unambiguous picture of the ultrafast electron-gas dynamics. These results will be instrumental to the refinement of existing models of femtosecond processes in laterally-confined and bulk condensed-matter systems, and for understanding more deeply the role of hot electrons in technological applications.
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J. Vac. Sci. Technol. B, 37, 061209, (2019)
Transparent conductive oxide-based architectures for the electrical modulation of the optical response: A spectroscopic ellipsometry study
M. Sygletou, F. Bisio, S. Benedetti, P. Torelli, A. di Bona, A. Petrov, and M. Canepa
Transparent conductive oxides are a class of materials that combine high optical transparency with high electrical conductivity. This property makes them uniquely appealing as transparent conductive electrodes in solar cells and interesting for optoelectronic and infrared-plasmonic applications. One of the new challenges that researchers and engineers are facing is merging optical and electrical control in a single device for developing next-generation photovoltaic, optoelectronic devices and energy-efficient solid-state lighting. In this work, the authors investigated the possible variations in the dielectric properties of aluminum-doped ZnO (AZO) upon gating by means of spectroscopic ellipsometry (SE). The authors investigated the electrical-bias-dependent optical response of thin AZO films fabricated by magnetron sputtering within a parallel-plane capacitor configuration. The authors address the possibility to control their optical and electric performances by applying bias, monitoring the effect of charge injection/depletion in the AZO layer by means of in operando SE versus applied gate voltage.
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OSA Technical Digest, paper EW2B.5, (2018)
A Novel High Order Harmonic Source for Time- and Angle-Resolved Photoemission Experiments
P. Miotti, F. Cilento, R. Cucini, A. De Luisa, A. Fondacaro, F. Frassetto, D. Kopić, D. Payne, A. Sterzi, T. Pincelli, G. Panaccione, F. Parmigiani, G. Rossi, and L. Poletto
The design and characterization of a HHG source conceived for Time and Angle Resolved PhotoElectron Spectroscopy (TR-ARPES) experiments are presented. The harmonics are selected through a grating monochromator with an innovative design able to provide XUV radiation for two distinct TR-ARPES setups.
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Chemical Physics Letters, 683. 135, (2017)
Time resolved resonant photoemission study of energy level alignment at donor/acceptor interfaces
R. Costantini, T. Pincelli, A. Cossaro, A. Verdini, A. Goldoni, S. Cichoň, M. Caputo, M.Pedio, G. Panaccione, M.G. Silly, F. Sirotti, A. Morgante, M. Dell'Angela
The knowledge of the picosecond dynamics of the energy level alignment between donor and acceptor materials in organic photovoltaic devices under working conditions is a challenge for fundamental material research. We measured by means of time-resolved Resonant X-ray Photoemission Spectroscopy (RPES) the energy level alignment in ZnPc/C60 films. We employed 800 nm femtosecond laser pulses to pump the system simulating sunlight excitation and X-rays from the synchrotron as a probe. We measured changes in the valence bands due to pump induced modifications of the interface dipole. Our measurements prove the feasibility of time-resolved RPES with high repetition rate sources.
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