TY - JOUR
T1 - Dopant-Assisted Matrix Stabilization Enables Thermoelectric Performance Enhancement in n-Type Quantum Dot Films.
AU - Nugraha, Mohamad Insan
AU - Sun, Bin
AU - Kim, Hyunho
AU - El Labban, Abdulrahman
AU - Desai, Saheena
AU - Chaturvedi, Neha
AU - Hou, Yi
AU - García de Arquer, F Pelayo
AU - Alshareef, Husam N.
AU - Sargent, E.
AU - Baran, Derya
N1 - KAUST Repository Item: Exported on 2021-04-20
Acknowledged KAUST grant number(s): CRG2018-3737.
Acknowledgements: The authors would like to acknowledge Nimer Wehbe at KAUST Core Labs for supporting XPS measurements in this work. Research in this publication was supported by the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under Award no. OSRCRG2018-3737.
PY - 2021/4/15
Y1 - 2021/4/15
N2 - Efficient thermoelectric generators require further progress in developing n-type semiconductors that combine low thermal conductivity with high electrical conductivity. By embedding colloidal quantum dots (CQDs) in a metal halide matrix (QDMH), the metal halide matrix can enhance phonon scattering, thus suppressing thermal transport; however, simultaneously achieving high electrical conductivity in such systems has previously been limited by the deleterious impact of a large density of interfaces on charge transport. Therefore, new strategies are needed to improve charge carrier transport without sacrificing matrix-enabled low thermal transport. Here, we report the use of chemical doping in the solution state to improve electron transport while maintaining low thermal transport in QDMH films. By incorporating cesium carbonate (Cs2CO3) salts as a dopant prior to matrix formation, we find that the dopant stabilizes the matrix in colloidal inks and enables efficient n-type doping in QDMH films. As a result, this strategy leads to an enhanced n-type thermoelectric behavior in solution-processed QDMH films near room temperature, with a thermal conductivity of 0.25 W m–1 K–1—significantly lower than in prior films based on organic-ligand-cross-linked CQD films (>0.6 W m–1 K–1) and spark-plasma-sintered CQD systems (>1 W m–1 K–1). This study provides a pathway to developing efficient n-type thermoelectric materials with low thermal conductivity using single-step deposition and low-temperature processing.
AB - Efficient thermoelectric generators require further progress in developing n-type semiconductors that combine low thermal conductivity with high electrical conductivity. By embedding colloidal quantum dots (CQDs) in a metal halide matrix (QDMH), the metal halide matrix can enhance phonon scattering, thus suppressing thermal transport; however, simultaneously achieving high electrical conductivity in such systems has previously been limited by the deleterious impact of a large density of interfaces on charge transport. Therefore, new strategies are needed to improve charge carrier transport without sacrificing matrix-enabled low thermal transport. Here, we report the use of chemical doping in the solution state to improve electron transport while maintaining low thermal transport in QDMH films. By incorporating cesium carbonate (Cs2CO3) salts as a dopant prior to matrix formation, we find that the dopant stabilizes the matrix in colloidal inks and enables efficient n-type doping in QDMH films. As a result, this strategy leads to an enhanced n-type thermoelectric behavior in solution-processed QDMH films near room temperature, with a thermal conductivity of 0.25 W m–1 K–1—significantly lower than in prior films based on organic-ligand-cross-linked CQD films (>0.6 W m–1 K–1) and spark-plasma-sintered CQD systems (>1 W m–1 K–1). This study provides a pathway to developing efficient n-type thermoelectric materials with low thermal conductivity using single-step deposition and low-temperature processing.
UR - http://hdl.handle.net/10754/668824
UR - https://pubs.acs.org/doi/10.1021/acsami.1c01886
U2 - 10.1021/acsami.1c01886
DO - 10.1021/acsami.1c01886
M3 - Article
C2 - 33856780
SN - 1944-8244
JO - ACS Applied Materials & Interfaces
JF - ACS Applied Materials & Interfaces
ER -