From 0e81e212ce788f088b19209cbe1b4fd7c046c08b Mon Sep 17 00:00:00 2001 From: Davide Grilli Date: Thu, 15 Oct 2026 09:16:04 +0200 Subject: [PATCH] Riscrive risultati e conclusioni del riassunto con sezioni esplicite e nuove figure Co-Authored-By: Claude Sonnet 5.5 --- riassunto/TEMP.docx | Bin 432731 -> 622625 bytes .../immagini/fig-film-bottle-brush-uv.png | Bin 0 -> 171919 bytes riassunto/riassunto_tesi.md | 20 ++++++++++++++---- 3 files changed, 16 insertions(+), 4 deletions(-) create mode 100644 riassunto/immagini/fig-film-bottle-brush-uv.png diff --git a/riassunto/TEMP.docx b/riassunto/TEMP.docx index 26e38259c6660b7948585cc7aefe2bdb9a403443..94b53de3cf06785f18c645e801d5ad4c6592033c 100644 GIT binary patch delta 211729 zcmV(?K-a(9v>Ks+CJRtY0|XQR000O8^|1>x0s-~2KLQZ}0rj&{1EK)|^|SN@rU8HT zNl#r9AeSzrO8@}c>;V7~0001YZ*pWWWN%}2ZDnqBE_iKh?Y&Kp+gi35I)A@{aB$;t zAXV|3RGn+5B}zJWclo&5c6Yz~ULG10MX7e1BGn{S{dlgpW-+#QEM&4@Shp7Z3gvsT{ 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I valori GPC risultano sottostimati rispetto ai teorici: la GPC separa per volume idrodinamico, relativo a standard di polistirene lineare, e un polimero altamente ramificato assume in soluzione una conformazione compatta. I dati confermano indirettamente una struttura ramificata altamente impaccata, con polidispersità (PD) contenuta (1,2-1,5); **3.3c** si discosta dall'andamento generale, forse per l'ingombro sterico. Rispetto al peso molecolare da 1H-NMR, la GPC concorda per bassa densità di grafting e sottostima all'aumentare delle catene laterali. La DSC mostra per tutti i bottle brush transizioni dominate dal PCL (temperatura di fusione 55-60 °C, di cristallizzazione 25-35 °C). Tabella 2 - Pesi molecolari dei bottle brush da GPC e da 1H-NMR @@ -91,15 +93,23 @@ Tabella 2 - Pesi molecolari dei bottle brush da GPC e da 1H-NMR | **3.2c** | 19200 | 24400 | 1,3 | 35500 | | **3.3c** | 14500 | 19500 | 1,3 | 41300 | -In soluzione di THF i massimi di assorbimento dei bottle brush cadono tra 544 e 554 nm, quelli di emissione tra 557 e 564 nm e gli Stokes shift tra 8 e 14 nm, senza andamento lineare con il peso molecolare del PCL: l'ingombro sterico non perturba livelli energetici e transizioni del core DPP, che conserva l'assetto planare. +In soluzione di THF i massimi di assorbimento dei bottle brush cadono tra 544 e 554 nm, quelli di emissione tra 557 e 564 nm e gli Stokes shift tra 8 e 14 nm, senza andamento lineare con il peso molecolare del PCL: l'ingombro sterico non perturba livelli energetici e transizioni del core DPP, che conserva l'assetto planare. Il basso Stokes shift indica una geometria rigida, mentre i domini flessibili di PCL allontanano le catene principali. -Allo stato solido, studiato sul campione **3.2b** *(Figura 9)*, il quadro cambia. In soluzione il massimo di assorbimento è a circa 550 nm e l'emissione, stretta e strutturata, a circa 560-565 nm. Allo stato solido l'assorbimento si allarga e si sposta a 570-580 nm, per la planarizzazione dello scheletro; l'emissione è molto allargata, con massimo a circa 650-660 nm e Stokes shift di circa 80-90 nm, segno di forte aggregazione: l'energia migra verso siti a energia minore, creati dalla vicinanza dei piani coniugati, e l'emissione parte da stati aggregati o specie eccimeriche, come descritto dall'accoppiamento eccitonico di Kasha per gli aggregati H e J.9,10 Nonostante ciò, il bottle brush mantiene un'apprezzabile emissione nel rosso, in accordo con il ruolo del PCL come spaziatore sterico; l'effetto dipende dalla lunghezza delle catene laterali: nei film quelle più lunghe preservano un'intensa emissione, con le più corte la fluorescenza si spegne, come nei lineari. +Allo stato solido, studiato sul campione **3.2b** *(Figura 9)*, il quadro cambia. In soluzione il massimo di assorbimento è a circa 550 nm e l'emissione, stretta e strutturata, a circa 560-565 nm. Allo stato solido l'assorbimento si allarga e si sposta a 570-580 nm, per la planarizzazione dello scheletro; l'emissione è molto allargata, con massimo a circa 650-660 nm e Stokes shift di circa 80-90 nm, segno di forte aggregazione: l'energia migra verso siti a energia minore, creati dalla vicinanza dei piani coniugati, e l'emissione parte da stati aggregati o specie eccimeriche, come descritto dall'accoppiamento eccitonico di Kasha per gli aggregati H e J.9,10 Nonostante ciò, il bottle brush mantiene un'apprezzabile emissione nel rosso, in accordo con il ruolo del PCL come spaziatore sterico. L'effetto dipende dalla lunghezza delle catene laterali *(Figura 10)*: nei film quelle più lunghe preservano un'intensa emissione, con le più corte (3 kDa) l'ingombro non basta e la fluorescenza si spegne, come nei copolimeri lineari DPP-3HT. ![](immagini/fig6-uv-em-3.2b.jpg) Figura 9 - spettri UV-Vis (in nero) ed emissione (in rosso) del polimero **3.2b** in soluzione (linea continua) e allo stato solido (linea tratteggiata) -Resta da verificare che il design non comprometta le proprietà elettroniche. La ciclovoltammetria mostra per i polimeri un trasferimento di carica irreversibile di tipo elettrochimico-chimico, per l'elevata reattività di cationi e anioni radicali all'interfaccia elettrodica. Dagli onset di ossidazione e riduzione, calibrati sul ferrocene (−4,8 eV), si ricavano i livelli HOMO e LUMO (orbitali molecolari occupato più alto e non occupato più basso) e il band gap *(Tabella 3)*. Nei copolimeri lineari il band gap cresce con la frazione reale di DPP, da 0,97 a 1,37 eV, con andamento che tende a un plateau, soprattutto per lo spostamento del potenziale di riduzione verso valori più negativi: il DPP riduce la lunghezza di coniugazione effettiva, per cui il rapporto tra i monomeri controlla il band gap. Il DPP, forte porzione elettron-attrattrice, stabilizza inoltre il LUMO e rende favorevole l'iniezione di elettroni, a differenza del poli(3-esiltiofene) (P3HT). I bottle brush mantengono l'elettroattività dello scheletro (i processi redox avvengono a carico del core DPP-3HT, mentre i rami alifatici fungono da matrice dielettrica) e, per l'ingombro dei rami di PCL sulla coplanarità locale, hanno band gap tra 0,929 e 1,521 eV: l'ingegnerizzazione con PCL non compromette le potenzialità optoelettroniche. +![](immagini/fig-film-bottle-brush-uv.png) + +Figura 10 - film solidi dei bottle brush (BB) e dei copolimeri lineari DPP-3HT sotto lampada Kessil (456 nm); le sigle in figura indicano rapporto DPP:3HT di partenza e massa delle catene laterali + +Resta da verificare che il design non comprometta le proprietà elettroniche. La ciclovoltammetria mostra per i polimeri un trasferimento di carica irreversibile di tipo elettrochimico-chimico, per l'elevata reattività di cationi e anioni radicali all'interfaccia elettrodica. Dagli onset di ossidazione e riduzione, calibrati sul ferrocene (−4,8 eV), si ricavano i livelli HOMO e LUMO (orbitali molecolari occupato più alto e non occupato più basso) e il band gap *(Tabella 3)*. Per il monomero **2** il band gap è 2,01 eV (HOMO −5,357 eV, LUMO −3,347 eV); nei copolimeri lineari scende a 0,97-1,37 eV e cresce con la frazione reale di DPP *(Figura 11)*, con andamento che tende a un plateau, soprattutto per lo spostamento del potenziale di riduzione verso valori più negativi: il DPP riduce la lunghezza di coniugazione effettiva, per cui il rapporto tra i monomeri controlla il band gap. Il DPP, forte porzione elettron-attrattrice, stabilizza inoltre il LUMO e rende favorevole l'iniezione di elettroni, a differenza del poli(3-esiltiofene) (P3HT). I bottle brush mantengono l'elettroattività dello scheletro (i processi redox avvengono a carico del core DPP-3HT, mentre i rami alifatici fungono da matrice dielettrica) e, per l'ingombro dei rami di PCL sulla coplanarità locale, hanno band gap tra 0,929 e 1,521 eV: l'ingegnerizzazione con PCL non compromette le potenzialità optoelettroniche. + +![](immagini/fig7-bandgap-vs-dpp.jpg) + +Figura 11 - correlazione tra band gap elettrochimico e frazione reale di DPP nei copolimeri lineari Tabella 3 - Livelli HOMO, LUMO e band gap elettrochimici dei copolimeri lineari e dei bottle brush @@ -115,7 +125,9 @@ Tabella 3 - Livelli HOMO, LUMO e band gap elettrochimici dei copolimeri lineari | **3.2c** | -4,69 | -3,27 | 1,42 | | **3.3c** | -4,48 | -3,55 | 0,93 | -In conclusione, i risultati confermano la validità del design proposto: l'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati con catene laterali di PCL combina proprietà elettrochimiche modulabili e capacità emissiva allo stato solido. Il nucleo DPP conserva in soluzione le proprietà ottiche e, allo stato solido, il bottle brush **3.2b** mantiene un'apprezzabile emissione nel rosso. I limiti sono l'integrazione di DPP non superiore al 35%, l'esclusione di **3a** dall'innesto, la sottostima dei pesi molecolari da GPC e le discrepanze di **3.3c**. La prospettiva è l'impiego di questi materiali come strato elettro-luminescente in OLED. +**Conclusioni** + +I risultati confermano la validità del design proposto: l'approccio ortogonale basato su scheletri semiconduttori DPP-3HT modificati con catene laterali di PCL combina proprietà elettrochimiche modulabili e capacità emissiva allo stato solido. Rispetto alla domanda iniziale, l'architettura bottle brush attenua l'ACQ, perché i film lineari non emettono mentre i bottle brush con catene sufficientemente lunghe emettono nel rosso, e preserva l'integrità elettrochimica del nucleo DPP; l'emissione allo stato solido resta però allargata e spostata verso il rosso rispetto alla soluzione, per l'aggregazione residua. Il nucleo DPP conserva in soluzione le proprietà ottiche. I limiti sono l'integrazione di DPP non superiore al 35%, l'esclusione di **3a** dall'innesto per la scarsa efficienza della sua sintesi, la sottostima dei pesi molecolari da GPC, le discrepanze di **3.3c** e l'assenza di rese quantiche allo stato solido. La prospettiva è l'impiego di questi materiali come strato elettro-luminescente in diodi organici a emissione di luce (OLED). **Bibliografia** 1. Ostroverkhova, O. Organic Optoelectronic Materials: Mechanisms and Applications. *Chem. Rev.* **2016**, *116*, 13279-13412. https://doi.org/10.1021/acs.chemrev.6b00127