TY - JOUR
T1 - Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals
AU - Guzelturk, Burak
AU - Cotts, Benjamin L.
AU - Jasrasaria, Dipti
AU - Philbin, John P.
AU - Hanifi, David A.
AU - Koscher, Brent A.
AU - Balan, Arunima D.
AU - Curling, Ethan
AU - Zajac, Marc
AU - Park, Suji
AU - Yazdani, Nuri
AU - Nyby, Clara
AU - Kamysbayev, Vladislav
AU - Fischer, Stefan
AU - Nett, Zach
AU - Shen, Xiaozhe
AU - Kozina, Michael E.
AU - Lin, Ming Fu
AU - Reid, Alexander H.
AU - Weathersby, Stephen P.
AU - Schaller, Richard D.
AU - Wood, Vanessa
AU - Wang, Xijie
AU - Dionne, Jennifer A.
AU - Talapin, Dmitri V.
AU - Alivisatos, A. Paul
AU - Salleo, Alberto
AU - Rabani, Eran
AU - Lindenberg, Aaron M.
N1 - Publisher Copyright:
© 2021, This is a U.S. government work and not under copyright protection in the U.S.; foreign copyright protection may apply.
PY - 2021/12/1
Y1 - 2021/12/1
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85103404155&partnerID=8YFLogxK
U2 - 10.1038/s41467-021-22116-0
DO - 10.1038/s41467-021-22116-0
M3 - ???researchoutput.researchoutputtypes.contributiontojournal.article???
C2 - 33767138
AN - SCOPUS:85103404155
SN - 2041-1723
VL - 12
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 1860
ER -