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Margola, Tommaso (2015) Polymer/fullerene OPV materials investigated by unconvenctional EPR techniques. [Tesi di dottorato]

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Abstract (inglese)

Organic Photovoltaics (OPV)s has gained lot of interest in the last decades thanks to its improved characteristics with respect to inorganic photovoltaic such as, flexibility, easy production processes, cheaper costs etc. Even though power conversion efficiency (PCE) is quite lower than silicon based solar cells, there've been quite an improvement of organic cells characteristics and a 12% PCE was registered. Among all the possible
features that are responsible for a better efficiency (morphology, energy levels set-up, method of deposition etc), this work focused on the photophysical processes of solid state blends based on conjugated polymer/fullerene studied by EPR spectroscopy.
Electron Paramagnetic Resonance is a useful tool in organic blends investigation thanks to its great sensitivity towards most of the photo-generated species. Distribution of states inside the band gap (or mobility edge) was studied by LMEPR which is able to detect an apparent lifetime that has been used as comparison parameter between different blends in order to find the degree of mobility of polarons after CT states dissociation. Data were supplied by LEPR measurement as a function of wavelength of excitation. LEPR intensity was found not to follow the absorption band profile and maximum LEPR intensity was found to be red-shifted. In the end we compare the possibility of relaxed and hot charge transfer states formation and the global apparent lifetime by LMEPR. P3HT/PC61BM thin film by spin-coating showed an orientation
dependent LEPR signal outlining a macroscopic order of polymeric phase. Simulation allowed to determine the parameter of order which is attributed only to polymeric phase. The effect of Diiodooctane (DIO) on PTB7/PC61BM and PTB7/PC71BM blends on bulk and thin films. LEPR spectra showed that DIO completely shut down the fullerene signals while TREPR spectra displayed, for thin film samples with DIO, oriented
recombination triplets for PTB7 and ISC oriented triplets for both fullerenes.
Simulation allows to determine the degree of order of about = 0.87 for PTB7 and = 0.93 for fullerenes. In the end we found PTB7 has dipolar axis as preferential orientation axis, PC61BM the dipolar axis and PC71BM a in plane axis.

Abstract (italiano)

Il fotovoltaico organico (OPVS) ha guadagnato molto interesse nelle ultime decadi grazie ad alcune caratteristiche migliori rispetto al fotovoltaico inorganico come flessibilità, facilità di produzione e costi inferiori. Anche se l'efficienza di conversione è ancora molto inferiore rispetto alle celle solari basate su silicio, l'intensa ricerca ha portato ad un netto miglioramento delle performance fino all'ottenimento del 12% di
efficienza. Tra tutte le possibili caratteristiche responsabili di una migliore efficienza (morfologia, energetica del sistema, metodo di deposizione ecc), questo lavoro di tesi si concentra sui processi fotofisici di miscele, in stato solido, di polimeri coniugati e fullereni, studiati attraverso spettroscopia EPR. La Risonanza Paramagnetica Elettronica rappresenta uno strumento molto potente nello studio delle miscele organiche grazie alla grande sensibilità che questa tecnica possiede nei confronti della
maggioranza delle specie foto-generate che si formano durante il processo
fotovoltaico. La distribuzione degli stati energetici all'interno del band gap (o mobility edge) è stata studiata attraverso misure LMEPR, da cui si è in grado di rilevare il tempo di vita apparente delle specie. Questo può essere usato come parametro di paragone tra campioni differenti per individuare qualitativamente il grado di mobilità dei polaroni dopo la dissociazione degli stati CT. Queste osservazioni sono state
confermate da misure LEPR in funzione delle lunghezza d'onda di eccitazione in cui l'intensità degli spettri ha mostrato un red-shift rispetto alla banda di assorbimento . Si è quindi confrontato il grado di generazione di polaroni, per dissociazione da stati CT rilassati e hot, con i tempi di vita apparenti ottenuti dalle misure LMEPR.
Spettri LEPR di film sottili di P3HT/Pc61BM, depositati per spin-coating, hanno mostrato un segnale dipendente dall'orientazione del campione. Le simulazioni degli spettri hanno permesso di calcolare il parametro d'ordine che identifica un ordine macroscopico assegnato unicamente al polimero.
In ultima è stato studiato l'effetto del Diiodoottano (DIO) come additivo in film sottili e di bulk per miscele di PTB7/PC61BM e PTB7/PC71BM. Gli spettri LEPR mostrano che il 1 Abstract is written in double language: Italian and English 4 DIO porta ad una scomparsa del segnale di entrambi i fullereni, mentre gli spettri TREPR, nel caso di film sottili in presenza di DIO, mostrano segnali di tripletto dipendendi dall'orientazione del campione per entrambe le fasi. In particolare per il PTB7 è stato individuato un tripletto di ricombinazione mentre per i fullereni un tripletto di ISC.

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Tipo di EPrint:Tesi di dottorato
Relatore:Toffoletti, Antonio
Dottorato (corsi e scuole):Ciclo 27 > scuole 27 > SCIENZE MOLECOLARI > SCIENZE CHIMICHE
Data di deposito della tesi:29 Gennaio 2015
Anno di Pubblicazione:29 Gennaio 2015
Parole chiave (italiano / inglese):EPR, LEPR, TREPR, OPV, polymer, fullerene
Settori scientifico-disciplinari MIUR:Area 03 - Scienze chimiche > CHIM/02 Chimica fisica
Struttura di riferimento:Dipartimenti > Dipartimento di Scienze Chimiche
Codice ID:7705
Depositato il:01 Dic 2015 13:09
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