Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals

Burak Guzelturk, Benjamin L. Cotts, Dipti Jasrasaria, John P. Philbin, David A. Hanifi, Brent A. Koscher, Arunima D. Balan, Ethan Curling, Marc Zajac, Suji Park, Nuri Yazdani, Clara Nyby, Vladislav Kamysbayev, Stefan Fischer, Zach Nett, Xiaozhe Shen, Michael E. Kozina, Ming Fu Lin, Alexander H. Reid, Stephen P. WeathersbyRichard D. Schaller, Vanessa Wood, Xijie Wang, Jennifer A. Dionne, Dmitri V. Talapin, A. Paul Alivisatos, Alberto Salleo, Eran Rabani, Aaron M. Lindenberg

פרסום מחקרי: פרסום בכתב עתמאמרביקורת עמיתים

תקציר

Nonradiative processes limit optoelectronic functionality of nanocrystals and curb their device performance. Nevertheless, the dynamic structural origins of nonradiative relaxations in such materials are not understood. Here, femtosecond electron diffraction measurements corroborated by atomistic simulations uncover transient lattice deformations accompanying radiationless electronic processes in colloidal semiconductor nanocrystals. Investigation of the excitation energy dependence in a core/shell system shows that hot carriers created by a photon energy considerably larger than the bandgap induce structural distortions at nanocrystal surfaces on few picosecond timescales associated with the localization of trapped holes. On the other hand, carriers created by a photon energy close to the bandgap of the core in the same system result in transient lattice heating that occurs on a much longer 200 picosecond timescale, dominated by an Auger heating mechanism. Elucidation of the structural deformations associated with the surface trapping of hot holes provides atomic-scale insights into the mechanisms deteriorating optoelectronic performance and a pathway towards minimizing these losses in nanocrystal devices.

שפה מקוריתאנגלית
מספר המאמר1860
כתב עתNature Communications
כרך12
מספר גיליון1
מזהי עצם דיגיטלי (DOIs)
סטטוס פרסוםפורסם - 1 דצמ׳ 2021

ASJC Scopus subject areas

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