---
_id: '12885'
abstract:
- lang: eng
text: 'High-performance semiconductors rely upon precise control of heat and charge
transport. This can be achieved by precisely engineering defects in polycrystalline
solids. There are multiple approaches to preparing such polycrystalline semiconductors,
and the transformation of solution-processed colloidal nanoparticles is appealing
because colloidal nanoparticles combine low cost with structural and compositional
tunability along with rich surface chemistry. However, the multiple processes
from nanoparticle synthesis to the final bulk nanocomposites are very complex.
They involve nanoparticle purification, post-synthetic modifications, and finally
consolidation (thermal treatments and densification). All these properties dictate
the final material’s composition and microstructure, ultimately affecting its
functional properties. This thesis explores the synthesis, surface chemistry and
consolidation of colloidal semiconductor nanoparticles into dense solids. In particular,
the transformations that take place during these processes, and their effect on
the material’s transport properties are evaluated. '
acknowledged_ssus:
- _id: EM-Fac
- _id: NanoFab
alternative_title:
- ISTA Thesis
article_processing_charge: No
author:
- first_name: Mariano
full_name: Calcabrini, Mariano
id: 45D7531A-F248-11E8-B48F-1D18A9856A87
last_name: Calcabrini
orcid: 0000-0003-4566-5877
citation:
ama: 'Calcabrini M. Nanoparticle-based semiconductor solids: From synthesis to consolidation.
2023. doi:10.15479/at:ista:12885'
apa: 'Calcabrini, M. (2023). Nanoparticle-based semiconductor solids: From synthesis
to consolidation. Institute of Science and Technology Austria. https://doi.org/10.15479/at:ista:12885'
chicago: 'Calcabrini, Mariano. “Nanoparticle-Based Semiconductor Solids: From Synthesis
to Consolidation.” Institute of Science and Technology Austria, 2023. https://doi.org/10.15479/at:ista:12885.'
ieee: 'M. Calcabrini, “Nanoparticle-based semiconductor solids: From synthesis to
consolidation,” Institute of Science and Technology Austria, 2023.'
ista: 'Calcabrini M. 2023. Nanoparticle-based semiconductor solids: From synthesis
to consolidation. Institute of Science and Technology Austria.'
mla: 'Calcabrini, Mariano. Nanoparticle-Based Semiconductor Solids: From Synthesis
to Consolidation. Institute of Science and Technology Austria, 2023, doi:10.15479/at:ista:12885.'
short: 'M. Calcabrini, Nanoparticle-Based Semiconductor Solids: From Synthesis to
Consolidation, Institute of Science and Technology Austria, 2023.'
date_created: 2023-05-02T07:58:57Z
date_published: 2023-04-28T00:00:00Z
date_updated: 2023-08-14T07:25:26Z
day: '28'
ddc:
- '546'
- '541'
degree_awarded: PhD
department:
- _id: GradSch
- _id: MaIb
doi: 10.15479/at:ista:12885
ec_funded: 1
file:
- access_level: closed
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content_type: application/vnd.openxmlformats-officedocument.wordprocessingml.document
creator: mcalcabr
date_created: 2023-05-02T07:43:18Z
date_updated: 2023-05-02T07:43:18Z
file_id: '12887'
file_name: Thesis_Calcabrini.docx
file_size: 99627036
relation: source_file
- access_level: open_access
checksum: 2d188b76621086cd384f0b9264b0a576
content_type: application/pdf
creator: mcalcabr
date_created: 2023-05-02T07:42:45Z
date_updated: 2023-05-02T07:42:45Z
file_id: '12888'
file_name: Thesis_Calcabrini_pdfa.pdf
file_size: 8742220
relation: main_file
success: 1
file_date_updated: 2023-05-02T07:43:18Z
has_accepted_license: '1'
language:
- iso: eng
month: '04'
oa: 1
oa_version: Published Version
page: '82'
project:
- _id: 2564DBCA-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '665385'
name: International IST Doctoral Program
publication_identifier:
isbn:
- 978-3-99078-028-2
issn:
- 2663-337X
publication_status: published
publisher: Institute of Science and Technology Austria
related_material:
record:
- id: '10806'
relation: part_of_dissertation
status: public
- id: '10042'
relation: part_of_dissertation
status: public
- id: '12237'
relation: part_of_dissertation
status: public
- id: '9118'
relation: part_of_dissertation
status: public
- id: '10123'
relation: part_of_dissertation
status: public
status: public
supervisor:
- first_name: Maria
full_name: Ibáñez, Maria
id: 43C61214-F248-11E8-B48F-1D18A9856A87
last_name: Ibáñez
orcid: 0000-0001-5013-2843
title: 'Nanoparticle-based semiconductor solids: From synthesis to consolidation'
type: dissertation
user_id: 8b945eb4-e2f2-11eb-945a-df72226e66a9
year: '2023'
...
---
_id: '10042'
abstract:
- lang: eng
text: SnSe has emerged as one of the most promising materials for thermoelectric
energy conversion due to its extraordinary performance in its single-crystal form
and its low-cost constituent elements. However, to achieve an economic impact,
the polycrystalline counterpart needs to replicate the performance of the single
crystal. Herein, we optimize the thermoelectric performance of polycrystalline
SnSe produced by consolidating solution-processed and surface-engineered SnSe
particles. In particular, the SnSe particles are coated with CdSe molecular complexes
that crystallize during the sintering process, forming CdSe nanoparticles. The
presence of CdSe nanoparticles inhibits SnSe grain growth during the consolidation
step due to Zener pinning, yielding a material with a high density of grain boundaries.
Moreover, the resulting SnSe–CdSe nanocomposites present a large number of defects
at different length scales, which significantly reduce the thermal conductivity.
The produced SnSe–CdSe nanocomposites exhibit thermoelectric figures of merit
up to 2.2 at 786 K, which is among the highest reported for solution-processed
SnSe.
acknowledgement: 'This work was financially supported by IST Austria and the Werner
Siemens Foundation. Y.L. acknowledges funding from the European Union’s Horizon
2020 research and innovation program under the Marie Sklodowska-Curie grant agreement
No. 754411. S.L. and M.C. received funding from the European Union’s Horizon 2020
research and innovation program under the Marie Skłodowska-Curie Grant Agreement
No. 665385. J.D. acknowledges funding from the European Union’s Horizon 2020 research
and innovation program under the Marie Sklodowska-Curie grant agreement no. 665919
(P-SPHERE) cofunded by Severo Ochoa Programme. C.C. acknowledges funding from the
FWF “Lise Meitner Fellowship” grant agreement M 2889-N. Y.Y. and O.C.-M. acknowledge
the financial support from DFG within the project SFB 917: Nanoswitches. M.C.S.
received funding from the European Union’s Horizon 2020 research and innovation
programme under the Marie Skłodowska-Curie grant agreement No. 754510 (PROBIST)
and the Severo Ochoa programme. J.D. received funding from the European Union’s
Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie
grant agreement No. 665919 (P-SPHERE) cofunded by Severo Ochoa Programme. The ICN2
is funded by the CERCA Program/Generalitat de Catalunya and by the Severo Ochoa
program of the Spanish Ministry of Economy, Industry, and Competitiveness (MINECO,
grant no. SEV-2017-0706). ICN2 acknowledges funding from Generalitat de Catalunya
2017 SGR 327 and the Spanish MINECO project NANOGEN (PID2020-116093RB-C43). This
project received funding from the European Union’s Horizon 2020 research and innovation
program under grant agreement No. 823717-ESTEEM3. The FIB sample preparation was
conducted in the LMA-INA-Universidad de Zaragoza.'
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Yu
full_name: Liu, Yu
id: 2A70014E-F248-11E8-B48F-1D18A9856A87
last_name: Liu
orcid: 0000-0001-7313-6740
- first_name: Mariano
full_name: Calcabrini, Mariano
id: 45D7531A-F248-11E8-B48F-1D18A9856A87
last_name: Calcabrini
- first_name: Yuan
full_name: Yu, Yuan
last_name: Yu
- first_name: Seungho
full_name: Lee, Seungho
id: BB243B88-D767-11E9-B658-BC13E6697425
last_name: Lee
orcid: 0000-0002-6962-8598
- first_name: Cheng
full_name: Chang, Cheng
id: 9E331C2E-9F27-11E9-AE48-5033E6697425
last_name: Chang
orcid: 0000-0002-9515-4277
- first_name: Jérémy
full_name: David, Jérémy
last_name: David
- first_name: Tanmoy
full_name: Ghosh, Tanmoy
id: a5fc9bc3-feff-11ea-93fe-e8015a3c7e9d
last_name: Ghosh
- first_name: Maria Chiara
full_name: Spadaro, Maria Chiara
last_name: Spadaro
- first_name: Chenyang
full_name: Xie, Chenyang
last_name: Xie
- first_name: Oana
full_name: Cojocaru-Mirédin, Oana
last_name: Cojocaru-Mirédin
- first_name: Jordi
full_name: Arbiol, Jordi
last_name: Arbiol
- first_name: Maria
full_name: Ibáñez, Maria
id: 43C61214-F248-11E8-B48F-1D18A9856A87
last_name: Ibáñez
orcid: 0000-0001-5013-2843
citation:
ama: Liu Y, Calcabrini M, Yu Y, et al. Defect engineering in solution-processed
polycrystalline SnSe leads to high thermoelectric performance. ACS Nano.
2022;16(1):78-88. doi:10.1021/acsnano.1c06720
apa: Liu, Y., Calcabrini, M., Yu, Y., Lee, S., Chang, C., David, J., … Ibáñez, M.
(2022). Defect engineering in solution-processed polycrystalline SnSe leads to
high thermoelectric performance. ACS Nano. American Chemical Society .
https://doi.org/10.1021/acsnano.1c06720
chicago: Liu, Yu, Mariano Calcabrini, Yuan Yu, Seungho Lee, Cheng Chang, Jérémy
David, Tanmoy Ghosh, et al. “Defect Engineering in Solution-Processed Polycrystalline
SnSe Leads to High Thermoelectric Performance.” ACS Nano. American Chemical
Society , 2022. https://doi.org/10.1021/acsnano.1c06720.
ieee: Y. Liu et al., “Defect engineering in solution-processed polycrystalline
SnSe leads to high thermoelectric performance,” ACS Nano, vol. 16, no.
1. American Chemical Society , pp. 78–88, 2022.
ista: Liu Y, Calcabrini M, Yu Y, Lee S, Chang C, David J, Ghosh T, Spadaro MC, Xie
C, Cojocaru-Mirédin O, Arbiol J, Ibáñez M. 2022. Defect engineering in solution-processed
polycrystalline SnSe leads to high thermoelectric performance. ACS Nano. 16(1),
78–88.
mla: Liu, Yu, et al. “Defect Engineering in Solution-Processed Polycrystalline SnSe
Leads to High Thermoelectric Performance.” ACS Nano, vol. 16, no. 1, American
Chemical Society , 2022, pp. 78–88, doi:10.1021/acsnano.1c06720.
short: Y. Liu, M. Calcabrini, Y. Yu, S. Lee, C. Chang, J. David, T. Ghosh, M.C.
Spadaro, C. Xie, O. Cojocaru-Mirédin, J. Arbiol, M. Ibáñez, ACS Nano 16 (2022)
78–88.
date_created: 2021-09-24T07:55:12Z
date_published: 2022-01-25T00:00:00Z
date_updated: 2023-08-02T14:41:05Z
day: '25'
ddc:
- '540'
department:
- _id: MaIb
doi: 10.1021/acsnano.1c06720
ec_funded: 1
external_id:
isi:
- '000767223400008'
pmid:
- '34549956'
file:
- access_level: open_access
checksum: 74f9c1aa5f95c0b992a4328e8e0247b4
content_type: application/pdf
creator: cchlebak
date_created: 2022-03-02T16:17:29Z
date_updated: 2022-03-02T16:17:29Z
file_id: '10808'
file_name: 2022_ACSNano_Liu.pdf
file_size: 9050764
relation: main_file
success: 1
file_date_updated: 2022-03-02T16:17:29Z
has_accepted_license: '1'
intvolume: ' 16'
isi: 1
issue: '1'
keyword:
- tin selenide
- nanocomposite
- grain growth
- Zener pinning
- thermoelectricity
- annealing
- solution processing
language:
- iso: eng
month: '01'
oa: 1
oa_version: Published Version
page: 78-88
pmid: 1
project:
- _id: 260C2330-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '754411'
name: ISTplus - Postdoctoral Fellowships
- _id: 2564DBCA-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '665385'
name: International IST Doctoral Program
- _id: 9B8F7476-BA93-11EA-9121-9846C619BF3A
name: 'HighTE: The Werner Siemens Laboratory for the High Throughput Discovery of
Semiconductors for Waste Heat Recovery'
- _id: 9B8804FC-BA93-11EA-9121-9846C619BF3A
grant_number: M02889
name: Bottom-up Engineering for Thermoelectric Applications
publication: ACS Nano
publication_identifier:
eissn:
- 1936-086X
issn:
- 1936-0851
publication_status: published
publisher: 'American Chemical Society '
quality_controlled: '1'
related_material:
record:
- id: '12885'
relation: dissertation_contains
status: public
scopus_import: '1'
status: public
title: Defect engineering in solution-processed polycrystalline SnSe leads to high
thermoelectric performance
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 16
year: '2022'
...
---
_id: '12237'
abstract:
- lang: eng
text: Thermoelectric technology requires synthesizing complex materials where not
only the crystal structure but also other structural features such as defects,
grain size and orientation, and interfaces must be controlled. To date, conventional
solid-state techniques are unable to provide this level of control. Herein, we
present a synthetic approach in which dense inorganic thermoelectric materials
are produced by the consolidation of well-defined nanoparticle powders. The idea
is that controlling the characteristics of the powder allows the chemical transformations
that take place during consolidation to be guided, ultimately yielding inorganic
solids with targeted features. Different from conventional methods, syntheses
in solution can produce particles with unprecedented control over their size,
shape, crystal structure, composition, and surface chemistry. However, to date,
most works have focused only on the low-cost benefits of this strategy. In this
perspective, we first cover the opportunities that solution processing of the
powder offers, emphasizing the potential structural features that can be controlled
by precisely engineering the inorganic core of the particle, the surface, and
the organization of the particles before consolidation. We then discuss the challenges
of this synthetic approach and more practical matters related to solution processing.
Finally, we suggest some good practices for adequate knowledge transfer and improving
reproducibility among different laboratories.
acknowledgement: This work was financially supported by ISTA and the Werner Siemens
Foundation. M.C. has received funding from the European Union’s Horizon 2020 research
and innovation program under the Marie Skłodowska-Curie Grant Agreement no. 665385.
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Christine
full_name: Fiedler, Christine
id: bd3fceba-dc74-11ea-a0a7-c17f71817366
last_name: Fiedler
- first_name: Tobias
full_name: Kleinhanns, Tobias
id: 8BD9DE16-AB3C-11E9-9C8C-2A03E6697425
last_name: Kleinhanns
- first_name: Maria
full_name: Garcia, Maria
id: 6e5c50b8-97dc-11ed-be98-b0a74c84cae0
last_name: Garcia
- first_name: Seungho
full_name: Lee, Seungho
id: BB243B88-D767-11E9-B658-BC13E6697425
last_name: Lee
orcid: 0000-0002-6962-8598
- first_name: Mariano
full_name: Calcabrini, Mariano
id: 45D7531A-F248-11E8-B48F-1D18A9856A87
last_name: Calcabrini
- first_name: Maria
full_name: Ibáñez, Maria
id: 43C61214-F248-11E8-B48F-1D18A9856A87
last_name: Ibáñez
orcid: 0000-0001-5013-2843
citation:
ama: 'Fiedler C, Kleinhanns T, Garcia M, Lee S, Calcabrini M, Ibáñez M. Solution-processed
inorganic thermoelectric materials: Opportunities and challenges. Chemistry
of Materials. 2022;34(19):8471-8489. doi:10.1021/acs.chemmater.2c01967'
apa: 'Fiedler, C., Kleinhanns, T., Garcia, M., Lee, S., Calcabrini, M., & Ibáñez,
M. (2022). Solution-processed inorganic thermoelectric materials: Opportunities
and challenges. Chemistry of Materials. American Chemical Society. https://doi.org/10.1021/acs.chemmater.2c01967'
chicago: 'Fiedler, Christine, Tobias Kleinhanns, Maria Garcia, Seungho Lee, Mariano
Calcabrini, and Maria Ibáñez. “Solution-Processed Inorganic Thermoelectric Materials:
Opportunities and Challenges.” Chemistry of Materials. American Chemical
Society, 2022. https://doi.org/10.1021/acs.chemmater.2c01967.'
ieee: 'C. Fiedler, T. Kleinhanns, M. Garcia, S. Lee, M. Calcabrini, and M. Ibáñez,
“Solution-processed inorganic thermoelectric materials: Opportunities and challenges,”
Chemistry of Materials, vol. 34, no. 19. American Chemical Society, pp.
8471–8489, 2022.'
ista: 'Fiedler C, Kleinhanns T, Garcia M, Lee S, Calcabrini M, Ibáñez M. 2022. Solution-processed
inorganic thermoelectric materials: Opportunities and challenges. Chemistry of
Materials. 34(19), 8471–8489.'
mla: 'Fiedler, Christine, et al. “Solution-Processed Inorganic Thermoelectric Materials:
Opportunities and Challenges.” Chemistry of Materials, vol. 34, no. 19,
American Chemical Society, 2022, pp. 8471–89, doi:10.1021/acs.chemmater.2c01967.'
short: C. Fiedler, T. Kleinhanns, M. Garcia, S. Lee, M. Calcabrini, M. Ibáñez, Chemistry
of Materials 34 (2022) 8471–8489.
date_created: 2023-01-16T09:51:26Z
date_published: 2022-09-20T00:00:00Z
date_updated: 2023-08-04T09:38:26Z
day: '20'
ddc:
- '540'
department:
- _id: MaIb
doi: 10.1021/acs.chemmater.2c01967
ec_funded: 1
external_id:
isi:
- '000917837600001'
pmid:
- '36248227'
file:
- access_level: open_access
checksum: f7143e44ab510519d1949099c3558532
content_type: application/pdf
creator: dernst
date_created: 2023-01-30T07:35:09Z
date_updated: 2023-01-30T07:35:09Z
file_id: '12434'
file_name: 2022_ChemistryMaterials_Fiedler.pdf
file_size: 10923495
relation: main_file
success: 1
file_date_updated: 2023-01-30T07:35:09Z
has_accepted_license: '1'
intvolume: ' 34'
isi: 1
issue: '19'
keyword:
- Materials Chemistry
- General Chemical Engineering
- General Chemistry
language:
- iso: eng
month: '09'
oa: 1
oa_version: Published Version
page: 8471-8489
pmid: 1
project:
- _id: 2564DBCA-B435-11E9-9278-68D0E5697425
call_identifier: H2020
grant_number: '665385'
name: International IST Doctoral Program
publication: Chemistry of Materials
publication_identifier:
eissn:
- 1520-5002
issn:
- 0897-4756
publication_status: published
publisher: American Chemical Society
quality_controlled: '1'
related_material:
record:
- id: '12885'
relation: dissertation_contains
status: public
scopus_import: '1'
status: public
title: 'Solution-processed inorganic thermoelectric materials: Opportunities and challenges'
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 34
year: '2022'
...
---
_id: '10806'
abstract:
- lang: eng
text: Ligands are a fundamental part of nanocrystals. They control and direct nanocrystal
syntheses and provide colloidal stability. Bound ligands also affect the nanocrystals’
chemical reactivity and electronic structure. Surface chemistry is thus crucial
to understand nanocrystal properties and functionality. Here, we investigate the
synthesis of metal oxide nanocrystals (CeO2-x, ZnO, and NiO) from metal nitrate
precursors, in the presence of oleylamine ligands. Surprisingly, the nanocrystals
are capped exclusively with a fatty acid instead of oleylamine. Analysis of the
reaction mixtures with nuclear magnetic resonance spectroscopy revealed several
reaction byproducts and intermediates that are common to the decomposition of
Ce, Zn, Ni, and Zr nitrate precursors. Our evidence supports the oxidation of
alkylamine and formation of a carboxylic acid, thus unraveling this counterintuitive
surface chemistry.
acknowledgement: 'This work was financially supported by IST Austria and the Werner
Siemens Foundation. M.C. has received funding from the European Union’s Horizon
2020 research and innovation programme under the Marie Skłodowska-Curie Grant Agreement
No. 665385. The work was also financially supported by University of Basel, SNSF
NCCR Molecular Systems Engineering (project number: 182895) and SNSF R’equip (project
number: 189622). J.L. is a Serra Húnter Fellow and is grateful to ICREA Academia
program and MICINN/FEDER RTI2018-093996-B-C31 and GC 2017 SGR 128 projects.'
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Mariano
full_name: Calcabrini, Mariano
id: 45D7531A-F248-11E8-B48F-1D18A9856A87
last_name: Calcabrini
- first_name: Dietger
full_name: Van den Eynden, Dietger
last_name: Van den Eynden
- first_name: Sergi
full_name: Sanchez Ribot, Sergi
id: ddae5a59-f6e0-11ea-865d-d9dc61e77a2a
last_name: Sanchez Ribot
- first_name: Rohan
full_name: Pokratath, Rohan
last_name: Pokratath
- first_name: Jordi
full_name: Llorca, Jordi
last_name: Llorca
- first_name: Jonathan
full_name: De Roo, Jonathan
last_name: De Roo
- first_name: Maria
full_name: Ibáñez, Maria
id: 43C61214-F248-11E8-B48F-1D18A9856A87
last_name: Ibáñez
orcid: 0000-0001-5013-2843
citation:
ama: 'Calcabrini M, Van den Eynden D, Sanchez Ribot S, et al. Ligand conversion
in nanocrystal synthesis: The oxidation of alkylamines to fatty acids by nitrate.
JACS Au. 2021;1(11):1898-1903. doi:10.1021/jacsau.1c00349'
apa: 'Calcabrini, M., Van den Eynden, D., Sanchez Ribot, S., Pokratath, R., Llorca,
J., De Roo, J., & Ibáñez, M. (2021). Ligand conversion in nanocrystal synthesis:
The oxidation of alkylamines to fatty acids by nitrate. JACS Au. American
Chemical Society. https://doi.org/10.1021/jacsau.1c00349'
chicago: 'Calcabrini, Mariano, Dietger Van den Eynden, Sergi Sanchez Ribot, Rohan
Pokratath, Jordi Llorca, Jonathan De Roo, and Maria Ibáñez. “Ligand Conversion
in Nanocrystal Synthesis: The Oxidation of Alkylamines to Fatty Acids by Nitrate.”
JACS Au. American Chemical Society, 2021. https://doi.org/10.1021/jacsau.1c00349.'
ieee: 'M. Calcabrini et al., “Ligand conversion in nanocrystal synthesis:
The oxidation of alkylamines to fatty acids by nitrate,” JACS Au, vol.
1, no. 11. American Chemical Society, pp. 1898–1903, 2021.'
ista: 'Calcabrini M, Van den Eynden D, Sanchez Ribot S, Pokratath R, Llorca J, De
Roo J, Ibáñez M. 2021. Ligand conversion in nanocrystal synthesis: The oxidation
of alkylamines to fatty acids by nitrate. JACS Au. 1(11), 1898–1903.'
mla: 'Calcabrini, Mariano, et al. “Ligand Conversion in Nanocrystal Synthesis: The
Oxidation of Alkylamines to Fatty Acids by Nitrate.” JACS Au, vol. 1, no.
11, American Chemical Society, 2021, pp. 1898–903, doi:10.1021/jacsau.1c00349.'
short: M. Calcabrini, D. Van den Eynden, S. Sanchez Ribot, R. Pokratath, J. Llorca,
J. De Roo, M. Ibáñez, JACS Au 1 (2021) 1898–1903.
date_created: 2022-03-02T15:24:16Z
date_published: 2021-11-22T00:00:00Z
date_updated: 2023-05-05T08:45:36Z
day: '22'
ddc:
- '540'
department:
- _id: MaIb
doi: 10.1021/jacsau.1c00349
ec_funded: 1
file:
- access_level: open_access
checksum: 1c66a35369e911312a359111420318a9
content_type: application/pdf
creator: cchlebak
date_created: 2022-03-02T15:33:18Z
date_updated: 2022-03-02T15:33:18Z
file_id: '10807'
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url: https://doi.org/10.26434/chemrxiv-2021-cn2fr
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relation: dissertation_contains
status: public
status: public
title: 'Ligand conversion in nanocrystal synthesis: The oxidation of alkylamines to
fatty acids by nitrate'
tmp:
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year: '2021'
...
---
_id: '9118'
abstract:
- lang: eng
text: Cesium lead halides have intrinsically unstable crystal lattices and easily
transform within perovskite and nonperovskite structures. In this work, we explore
the conversion of the perovskite CsPbBr3 into Cs4PbBr6 in the presence of PbS
at 450 °C to produce doped nanocrystal-based composites with embedded Cs4PbBr6
nanoprecipitates. We show that PbBr2 is extracted from CsPbBr3 and diffuses into
the PbS lattice with a consequent increase in the concentration of free charge
carriers. This new doping strategy enables the adjustment of the density of charge
carriers between 1019 and 1020 cm–3, and it may serve as a general strategy for
doping other nanocrystal-based semiconductors.
acknowledgement: "M.C. has received funding from the European Union’s Horizon 2020
research and innovation programme under the Marie Skłodowska-Curie Grant Agreement
No. 665385. ICN2\r\nacknowledges funding from Generalitat de Catalunya 2017 SGR
327. ICN2 is supported by the Severo Ochoa program from Spanish MINECO (Grant No.
SEV-2017-0706) and is funded by the CERCA Programme/Generalitat de Catalunya. This
project has received funding from the European Union’s Horizon 2020 research and
innovation programme under grant agreement No 823717 − ESTEEM3. M.V.K. acknowledges
the support by the European Research Council under the Horizon 2020 Framework Program
(ERC Consolidator Grant SCALEHALO\r\nGrant Agreement No. 819740) and by FET-OPEN
project no. 862656 (DROP-IT)."
article_processing_charge: Yes (via OA deal)
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author:
- first_name: Mariano
full_name: Calcabrini, Mariano
id: 45D7531A-F248-11E8-B48F-1D18A9856A87
last_name: Calcabrini
- first_name: Aziz
full_name: Genc, Aziz
last_name: Genc
- first_name: Yu
full_name: Liu, Yu
id: 2A70014E-F248-11E8-B48F-1D18A9856A87
last_name: Liu
orcid: 0000-0001-7313-6740
- first_name: Tobias
full_name: Kleinhanns, Tobias
id: 8BD9DE16-AB3C-11E9-9C8C-2A03E6697425
last_name: Kleinhanns
- first_name: Seungho
full_name: Lee, Seungho
id: BB243B88-D767-11E9-B658-BC13E6697425
last_name: Lee
orcid: 0000-0002-6962-8598
- first_name: Dmitry N.
full_name: Dirin, Dmitry N.
last_name: Dirin
- first_name: Quinten A.
full_name: Akkerman, Quinten A.
last_name: Akkerman
- first_name: Maksym V.
full_name: Kovalenko, Maksym V.
last_name: Kovalenko
- first_name: Jordi
full_name: Arbiol, Jordi
last_name: Arbiol
- first_name: Maria
full_name: Ibáñez, Maria
id: 43C61214-F248-11E8-B48F-1D18A9856A87
last_name: Ibáñez
orcid: 0000-0001-5013-2843
citation:
ama: Calcabrini M, Genc A, Liu Y, et al. Exploiting the lability of metal halide
perovskites for doping semiconductor nanocomposites. ACS Energy Letters.
2021;6(2):581-587. doi:10.1021/acsenergylett.0c02448
apa: Calcabrini, M., Genc, A., Liu, Y., Kleinhanns, T., Lee, S., Dirin, D. N., …
Ibáñez, M. (2021). Exploiting the lability of metal halide perovskites for doping
semiconductor nanocomposites. ACS Energy Letters. American Chemical Society.
https://doi.org/10.1021/acsenergylett.0c02448
chicago: Calcabrini, Mariano, Aziz Genc, Yu Liu, Tobias Kleinhanns, Seungho Lee,
Dmitry N. Dirin, Quinten A. Akkerman, Maksym V. Kovalenko, Jordi Arbiol, and Maria
Ibáñez. “Exploiting the Lability of Metal Halide Perovskites for Doping Semiconductor
Nanocomposites.” ACS Energy Letters. American Chemical Society, 2021. https://doi.org/10.1021/acsenergylett.0c02448.
ieee: M. Calcabrini et al., “Exploiting the lability of metal halide perovskites
for doping semiconductor nanocomposites,” ACS Energy Letters, vol. 6, no.
2. American Chemical Society, pp. 581–587, 2021.
ista: Calcabrini M, Genc A, Liu Y, Kleinhanns T, Lee S, Dirin DN, Akkerman QA, Kovalenko
MV, Arbiol J, Ibáñez M. 2021. Exploiting the lability of metal halide perovskites
for doping semiconductor nanocomposites. ACS Energy Letters. 6(2), 581–587.
mla: Calcabrini, Mariano, et al. “Exploiting the Lability of Metal Halide Perovskites
for Doping Semiconductor Nanocomposites.” ACS Energy Letters, vol. 6, no.
2, American Chemical Society, 2021, pp. 581–87, doi:10.1021/acsenergylett.0c02448.
short: M. Calcabrini, A. Genc, Y. Liu, T. Kleinhanns, S. Lee, D.N. Dirin, Q.A. Akkerman,
M.V. Kovalenko, J. Arbiol, M. Ibáñez, ACS Energy Letters 6 (2021) 581–587.
date_created: 2021-02-14T23:01:14Z
date_published: 2021-01-20T00:00:00Z
date_updated: 2023-08-07T13:46:00Z
day: '20'
ddc:
- '540'
department:
- _id: MaIb
doi: 10.1021/acsenergylett.0c02448
ec_funded: 1
external_id:
isi:
- '000619803400036'
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page: 581-587
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grant_number: '665385'
name: International IST Doctoral Program
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title: Exploiting the lability of metal halide perovskites for doping semiconductor
nanocomposites
tmp:
image: /images/cc_by.png
legal_code_url: https://creativecommons.org/licenses/by/4.0/legalcode
name: Creative Commons Attribution 4.0 International Public License (CC-BY 4.0)
short: CC BY (4.0)
type: journal_article
user_id: 4359f0d1-fa6c-11eb-b949-802e58b17ae8
volume: 6
year: '2021'
...
---
_id: '10123'
abstract:
- lang: eng
text: Solution synthesis of particles emerged as an alternative to prepare thermoelectric
materials with less demanding processing conditions than conventional solid-state
synthetic methods. However, solution synthesis generally involves the presence
of additional molecules or ions belonging to the precursors or added to enable
solubility and/or regulate nucleation and growth. These molecules or ions can
end up in the particles as surface adsorbates and interfere in the material properties.
This work demonstrates that ionic adsorbates, in particular Na⁺ ions, are electrostatically
adsorbed in SnSe particles synthesized in water and play a crucial role not only
in directing the material nano/microstructure but also in determining the transport
properties of the consolidated material. In dense pellets prepared by sintering
SnSe particles, Na remains within the crystal lattice as dopant, in dislocations,
precipitates, and forming grain boundary complexions. These results highlight
the importance of considering all the possible unintentional impurities to establish
proper structure-property relationships and control material properties in solution-processed
thermoelectric materials.
acknowledged_ssus:
- _id: EM-Fac
- _id: NanoFab
acknowledgement: 'Y.L. and M.C. contributed equally to this work. This research was
supported by the Scientific Service Units (SSU) of IST Austria through resources
provided by Electron Microscopy Facility (EMF) and the Nanofabrication Facility
(NNF). This work was financially supported by IST Austria and the Werner Siemens
Foundation. Y.L. acknowledges funding from the European Union''s Horizon 2020 research
and innovation program under the Marie Sklodowska-Curie grant agreement No. 754411.
M.C. has received funding from the European Union''s Horizon 2020 research and innovation
program under the Marie Skłodowska-Curie Grant Agreement No. 665385. Y.Y. and O.C.-M.
acknowledge the financial support from DFG within the project SFB 917: Nanoswitches.
J.L. is a Serra Húnter Fellow and is grateful to ICREA Academia program. C.C. acknowledges
funding from the FWF “Lise Meitner Fellowship” grant agreement M 2889-N.'
article_number: '2106858'
article_processing_charge: Yes (via OA deal)
article_type: original
author:
- first_name: Yu
full_name: Liu, Yu
id: 2A70014E-F248-11E8-B48F-1D18A9856A87
last_name: Liu
orcid: 0000-0001-7313-6740
- first_name: Mariano
full_name: Calcabrini, Mariano
id: 45D7531A-F248-11E8-B48F-1D18A9856A87
last_name: Calcabrini
orcid: 0000-0003-4566-5877
- first_name: Yuan
full_name: Yu, Yuan
last_name: Yu
- first_name: Aziz
full_name: Genç, Aziz
last_name: Genç
- first_name: Cheng
full_name: Chang, Cheng
id: 9E331C2E-9F27-11E9-AE48-5033E6697425
last_name: Chang
orcid: 0000-0002-9515-4277
- first_name: Tommaso
full_name: Costanzo, Tommaso
id: D93824F4-D9BA-11E9-BB12-F207E6697425
last_name: Costanzo
orcid: 0000-0001-9732-3815
- first_name: Tobias
full_name: Kleinhanns, Tobias
id: 8BD9DE16-AB3C-11E9-9C8C-2A03E6697425
last_name: Kleinhanns
- first_name: Seungho
full_name: Lee, Seungho
id: BB243B88-D767-11E9-B658-BC13E6697425
last_name: Lee
orcid: 0000-0002-6962-8598
- first_name: Jordi
full_name: Llorca, Jordi
last_name: Llorca
- first_name: Oana
full_name: Cojocaru‐Mirédin, Oana
last_name: Cojocaru‐Mirédin
- first_name: Maria
full_name: Ibáñez, Maria
id: 43C61214-F248-11E8-B48F-1D18A9856A87
last_name: Ibáñez
orcid: 0000-0001-5013-2843
citation:
ama: 'Liu Y, Calcabrini M, Yu Y, et al. The importance of surface adsorbates in
solution‐processed thermoelectric materials: The case of SnSe. Advanced Materials.
2021;33(52). doi:10.1002/adma.202106858'
apa: 'Liu, Y., Calcabrini, M., Yu, Y., Genç, A., Chang, C., Costanzo, T., … Ibáñez,
M. (2021). The importance of surface adsorbates in solution‐processed thermoelectric
materials: The case of SnSe. Advanced Materials. Wiley. https://doi.org/10.1002/adma.202106858'
chicago: 'Liu, Yu, Mariano Calcabrini, Yuan Yu, Aziz Genç, Cheng Chang, Tommaso
Costanzo, Tobias Kleinhanns, et al. “The Importance of Surface Adsorbates in Solution‐processed
Thermoelectric Materials: The Case of SnSe.” Advanced Materials. Wiley,
2021. https://doi.org/10.1002/adma.202106858.'
ieee: 'Y. Liu et al., “The importance of surface adsorbates in solution‐processed
thermoelectric materials: The case of SnSe,” Advanced Materials, vol. 33,
no. 52. Wiley, 2021.'
ista: 'Liu Y, Calcabrini M, Yu Y, Genç A, Chang C, Costanzo T, Kleinhanns T, Lee
S, Llorca J, Cojocaru‐Mirédin O, Ibáñez M. 2021. The importance of surface adsorbates
in solution‐processed thermoelectric materials: The case of SnSe. Advanced Materials.
33(52), 2106858.'
mla: 'Liu, Yu, et al. “The Importance of Surface Adsorbates in Solution‐processed
Thermoelectric Materials: The Case of SnSe.” Advanced Materials, vol. 33,
no. 52, 2106858, Wiley, 2021, doi:10.1002/adma.202106858.'
short: Y. Liu, M. Calcabrini, Y. Yu, A. Genç, C. Chang, T. Costanzo, T. Kleinhanns,
S. Lee, J. Llorca, O. Cojocaru‐Mirédin, M. Ibáñez, Advanced Materials 33 (2021).
date_created: 2021-10-11T20:07:24Z
date_published: 2021-12-29T00:00:00Z
date_updated: 2023-08-14T07:25:27Z
day: '29'
ddc:
- '620'
department:
- _id: EM-Fac
- _id: MaIb
doi: 10.1002/adma.202106858
ec_funded: 1
external_id:
isi:
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intvolume: ' 33'
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issue: '52'
keyword:
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- mechanics of materials
- general materials science
language:
- iso: eng
month: '12'
oa: 1
oa_version: Published Version
pmid: 1
project:
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call_identifier: H2020
grant_number: '665385'
name: International IST Doctoral Program
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call_identifier: H2020
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publication: Advanced Materials
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title: 'The importance of surface adsorbates in solution‐processed thermoelectric
materials: The case of SnSe'
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...