TY - JOUR
T1 - Low-threshold laser medium utilizing semiconductor nanoshell quantum dots
AU - Porotnikov, Dmitry
AU - Diroll, Benjamin T.
AU - Harankahage, Dulanjan
AU - Obloy, Laura
AU - Yang, Mingrui
AU - Cassidy, James
AU - Ellison, Cole
AU - Miller, Emily
AU - Rogers, Spencer
AU - Tarnovsky, Alexander N.
AU - Schaller, Richard D.
AU - Zamkov, Mikhail
N1 - Funding Information:
This work was supported by the Award DE-SC0016872 (MZ) funded by the U.S. Department of Energy, Office of Science. JC was supported in part by NSF Award DMR-1710063. The authors acknowledge the financial support of the University of Michigan College of Engineering and NSF grant #DMR-9871177, and technical support from the Michigan Center for Materials Characterization. This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. A. N. T. acknowledges NSF awards CHE-0923360 and CHE-1626420.
Publisher Copyright:
© The Royal Society of Chemistry.
PY - 2020/9/7
Y1 - 2020/9/7
N2 - Colloidal semiconductor nanocrystals (NCs) represent a promising class of nanomaterials for lasing applications. Currently, one of the key challenges facing the development of high-performance NC optical gain media lies in enhancing the lifetime of biexciton populations. This usually requires the employment of charge-delocalizing particle architectures, such as core/shell NCs, nanorods, and nanoplatelets. Here, we report on a two-dimensional nanoshell quantum dot (QD) morphology that enables a strong delocalization of photoinduced charges, leading to enhanced biexciton lifetimes and low lasing thresholds. A unique combination of a large exciton volume and a smoothed potential gradient across interfaces of the reported CdSbulk/CdSe/CdSshell (core/shell/shell) nanoshell QDs results in strong suppression of Auger processes, which was manifested in this work though the observation of stable amplified stimulated emission (ASE) at low pump fluences. An extensive charge delocalization in nanoshell QDs was confirmed by transient absorption measurements, showing that the presence of a bulk-size core in CdSbulk/CdSe/CdSshell QDs reduces exciton-exciton interactions. Overall, present findings demonstrate unique advantages of the nanoshell QD architecture as a promising optical gain medium in solid-state lighting and lasing applications.
AB - Colloidal semiconductor nanocrystals (NCs) represent a promising class of nanomaterials for lasing applications. Currently, one of the key challenges facing the development of high-performance NC optical gain media lies in enhancing the lifetime of biexciton populations. This usually requires the employment of charge-delocalizing particle architectures, such as core/shell NCs, nanorods, and nanoplatelets. Here, we report on a two-dimensional nanoshell quantum dot (QD) morphology that enables a strong delocalization of photoinduced charges, leading to enhanced biexciton lifetimes and low lasing thresholds. A unique combination of a large exciton volume and a smoothed potential gradient across interfaces of the reported CdSbulk/CdSe/CdSshell (core/shell/shell) nanoshell QDs results in strong suppression of Auger processes, which was manifested in this work though the observation of stable amplified stimulated emission (ASE) at low pump fluences. An extensive charge delocalization in nanoshell QDs was confirmed by transient absorption measurements, showing that the presence of a bulk-size core in CdSbulk/CdSe/CdSshell QDs reduces exciton-exciton interactions. Overall, present findings demonstrate unique advantages of the nanoshell QD architecture as a promising optical gain medium in solid-state lighting and lasing applications.
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U2 - 10.1039/d0nr03582c
DO - 10.1039/d0nr03582c
M3 - Article
C2 - 32797122
AN - SCOPUS:85090080298
SN - 2040-3364
VL - 12
SP - 17426
EP - 17436
JO - Nanoscale
JF - Nanoscale
IS - 33
ER -