This thesis completes my work as doctoral student of the Scuola di Dottorato in Fisica, Astrofisica e Fisica Applicata at the Università degli Studi di Milano that has been carried out, starting in November 2014, mostly at the Laboratorio TASC of IOM-CNR in the premises of the Elettra - Sincrotrone Trieste and FERMI@Elettra infrastructures, in the framework of the NFFA and APE-beamline facilites, as well as by accessing international large scale infrastructures and laboratories. The activity has addressed the development of experimental methodologies and novel instrumentation oriented to the study of the dynamical properties of highly correlated materials after high energy excitation. The science programme has been carried out by exploiting ultrafast femtosecond probes from the optical regime (Ti-Sa lasers, fibre laser oscillators) to the extreme UV-soft X rays at FERMI, to the picosecond hard X-rays from the SPring-8 and Diamond synchrotron radiation source. The sample synthesis of correlated oxides and its characterization has been performed within the NFFA facility and APE-group collaboration in Trieste as well as the design and construction of the all new laser High Harmonic Generation beam line NFFA-SPRINT and its end station for time resolved vectorial electron spin polarimetry. This report concentrates on the main scientific concern of my work that has been the relaxation of external perturbations in a correlated electron material both in the time and space domain. I have employed Photoelectron Spectroscopy (PES) mostly in the Hard X-ray regime (HAXPES), pushing the boundaries of its application to achieve a coherent perspective. The material I have mainly focused on is La0.67Sr0.33MnO3 (LSMO), of high interest for spintronics. This system is prototypical, yielding the highest simplicity in the class of transition metal oxides. In the spatial investigation, I have controlled with high precision the PES probing depth and I have observed the evolution of one spectral feature. I have identified it as probe of electronic hybridization and long-range ordering. I have studied LSMO films of 40 nm in three substrate-induced strain states (1% tensile in-plane, relaxed, 1% compressive in-plane) and a 18 nm film of (Ga,Mn)As (GMA), a well-studied diluted magnetic semiconductor. I have found that the electronic properties to be modified at significant distances from the surface, 4 nm for LSMO and 1.2 nm for GMA, while strain had no detectable effects. In the temporal study, I have employed HAXPES in pump-probe mode (TR-HAXPES) to observe the evolution of the electronic structure after intense optical excitation. A detailed dynamical characterization with optical techniques has allowed me to identify the characteristic time of the collapse of long-range magnetic order to be significantly longer than the one of elemental transition metals. I have ascribed this effect to the half-metallic character of LSMO. With TR-HAXPES I have observed that the whole electronic band-structure evolution is bottlenecked by the slow response of the magnetization, proceeding on hundreds of picoseconds timescales. Finally, I have described the techniques and the instrumentation that can be used to push these investigations to shorter spatial and temporal scales. This has been realized in the form of the NFFA-SPRINT laboratory, a facility open to users, which I participated in designing and developing.

PROBING ELECTRON CORRELATION DYNAMICS: A MULTI-TECHNIQUE STUDY APPLIED TO THE HALF-METALLIC OXIDE LA1-XSRXMNO3 / T. Pincelli ; supervisor: G. Rossi ; co-supervisor: G. Panccione ; coordinatore: M. Bersanelli. DIPARTIMENTO DI FISICA, 2017 Dec 19. 30. ciclo, Anno Accademico 2017. [10.13130/pincelli-tommaso_phd2017-12-19].

PROBING ELECTRON CORRELATION DYNAMICS: A MULTI-TECHNIQUE STUDY APPLIED TO THE HALF-METALLIC OXIDE LA1-XSRXMNO3

T. Pincelli
2017

Abstract

This thesis completes my work as doctoral student of the Scuola di Dottorato in Fisica, Astrofisica e Fisica Applicata at the Università degli Studi di Milano that has been carried out, starting in November 2014, mostly at the Laboratorio TASC of IOM-CNR in the premises of the Elettra - Sincrotrone Trieste and FERMI@Elettra infrastructures, in the framework of the NFFA and APE-beamline facilites, as well as by accessing international large scale infrastructures and laboratories. The activity has addressed the development of experimental methodologies and novel instrumentation oriented to the study of the dynamical properties of highly correlated materials after high energy excitation. The science programme has been carried out by exploiting ultrafast femtosecond probes from the optical regime (Ti-Sa lasers, fibre laser oscillators) to the extreme UV-soft X rays at FERMI, to the picosecond hard X-rays from the SPring-8 and Diamond synchrotron radiation source. The sample synthesis of correlated oxides and its characterization has been performed within the NFFA facility and APE-group collaboration in Trieste as well as the design and construction of the all new laser High Harmonic Generation beam line NFFA-SPRINT and its end station for time resolved vectorial electron spin polarimetry. This report concentrates on the main scientific concern of my work that has been the relaxation of external perturbations in a correlated electron material both in the time and space domain. I have employed Photoelectron Spectroscopy (PES) mostly in the Hard X-ray regime (HAXPES), pushing the boundaries of its application to achieve a coherent perspective. The material I have mainly focused on is La0.67Sr0.33MnO3 (LSMO), of high interest for spintronics. This system is prototypical, yielding the highest simplicity in the class of transition metal oxides. In the spatial investigation, I have controlled with high precision the PES probing depth and I have observed the evolution of one spectral feature. I have identified it as probe of electronic hybridization and long-range ordering. I have studied LSMO films of 40 nm in three substrate-induced strain states (1% tensile in-plane, relaxed, 1% compressive in-plane) and a 18 nm film of (Ga,Mn)As (GMA), a well-studied diluted magnetic semiconductor. I have found that the electronic properties to be modified at significant distances from the surface, 4 nm for LSMO and 1.2 nm for GMA, while strain had no detectable effects. In the temporal study, I have employed HAXPES in pump-probe mode (TR-HAXPES) to observe the evolution of the electronic structure after intense optical excitation. A detailed dynamical characterization with optical techniques has allowed me to identify the characteristic time of the collapse of long-range magnetic order to be significantly longer than the one of elemental transition metals. I have ascribed this effect to the half-metallic character of LSMO. With TR-HAXPES I have observed that the whole electronic band-structure evolution is bottlenecked by the slow response of the magnetization, proceeding on hundreds of picoseconds timescales. Finally, I have described the techniques and the instrumentation that can be used to push these investigations to shorter spatial and temporal scales. This has been realized in the form of the NFFA-SPRINT laboratory, a facility open to users, which I participated in designing and developing.
19-dic-2017
Settore FIS/03 - Fisica della Materia
hard X-ray photoelectron spectroscopy; photoelectron spectroscopy; spin-resolved; dichroism in photoemission; transition metal oxides; condensed matter; spintronics; manganite; half-metallic; pump-probe; time-resolved; magneto-optical Kerr effect; HAXPES; MOKE; LSMO; GMA; TR-MOKE; high harmonics generation; HHG
hdl:2434/517361
hdl:2434/478170
hdl:2434/384281
ROSSI, GIORGIO
ROSSI, GIORGIO
BERSANELLI, MARCO RINALDO FEDELE
Doctoral Thesis
PROBING ELECTRON CORRELATION DYNAMICS: A MULTI-TECHNIQUE STUDY APPLIED TO THE HALF-METALLIC OXIDE LA1-XSRXMNO3 / T. Pincelli ; supervisor: G. Rossi ; co-supervisor: G. Panccione ; coordinatore: M. Bersanelli. DIPARTIMENTO DI FISICA, 2017 Dec 19. 30. ciclo, Anno Accademico 2017. [10.13130/pincelli-tommaso_phd2017-12-19].
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