X‑Ray-Induced Modification of the Photophysical Properties of MAPbBr3 Single Crystals

Methylammonium lead tribromide (MAPbBr3) perovskite single crystals demonstrate to be excellent direct X-ray and gamma-ray detectors with outstanding sensitivity and low limit of detection. Despite this, thorough studies on the photophysical effects of exposure to high doses of ionizing radiation on...

Full description

Saved in:
Bibliographic Details
Published inACS applied materials & interfaces Vol. 13; no. 49; pp. 58301 - 58308
Main Authors Armaroli, Giovanni, Ferlauto, Laura, Lédée, Ferdinand, Lini, Matilde, Ciavatti, Andrea, Kovtun, Alessandro, Borgatti, Francesco, Calabrese, Gabriele, Milita, Silvia, Fraboni, Beatrice, Cavalcoli, Daniela
Format Journal Article
LanguageEnglish
Published American Chemical Society 15.12.2021
Subjects
Online AccessGet full text

Cover

Loading…
Abstract Methylammonium lead tribromide (MAPbBr3) perovskite single crystals demonstrate to be excellent direct X-ray and gamma-ray detectors with outstanding sensitivity and low limit of detection. Despite this, thorough studies on the photophysical effects of exposure to high doses of ionizing radiation on this material are still lacking. In this work, we present our findings regarding the effects of controlled X-ray irradiation on the optoelectronic properties of MAPbBr3 single crystals. Irradiation is carried out in air with an imaging X-ray tube, simulating real-life application in a medical facility. By means of surface photovoltage spectroscopy, we find that X-ray exposure quenches free excitons in the material and introduces new bound excitonic species. Despite this drastic effect, the crystals recover after 1 week of storage in dark and low humidity conditions. By means of X-ray photoelectron spectroscopy, we find that the origin of the new bound excitonic species is the formation of bromine vacancies, leading to local changes in the dielectric response of the material. The recovery effect is attributed to vacancy filling by atmospheric oxygen and water.
AbstractList Methylammonium lead tribromide (MAPbBr 3 ) perovskite single crystals demonstrate to be excellent direct X-ray and gamma-ray detectors with outstanding sensitivity and low limit of detection. Despite this, thorough studies on the photophysical effects of exposure to high doses of ionizing radiation on this material are still lacking. In this work, we present our findings regarding the effects of controlled X-ray irradiation on the optoelectronic properties of MAPbBr 3 single crystals. Irradiation is carried out in air with an imaging X-ray tube, simulating real-life application in a medical facility. By means of surface photovoltage spectroscopy, we find that X-ray exposure quenches free excitons in the material and introduces new bound excitonic species. Despite this drastic effect, the crystals recover after 1 week of storage in dark and low humidity conditions. By means of X-ray photoelectron spectroscopy, we find that the origin of the new bound excitonic species is the formation of bromine vacancies, leading to local changes in the dielectric response of the material. The recovery effect is attributed to vacancy filling by atmospheric oxygen and water.
Methylammonium lead tribromide (MAPbBr3) perovskite single crystals demonstrate to be excellent direct X-ray and gamma-ray detectors with outstanding sensitivity and low limit of detection. Despite this, thorough studies on the photophysical effects of exposure to high doses of ionizing radiation on this material are still lacking. In this work, we present our findings regarding the effects of controlled X-ray irradiation on the optoelectronic properties of MAPbBr3 single crystals. Irradiation is carried out in air with an imaging X-ray tube, simulating real-life application in a medical facility. By means of surface photovoltage spectroscopy, we find that X-ray exposure quenches free excitons in the material and introduces new bound excitonic species. Despite this drastic effect, the crystals recover after 1 week of storage in dark and low humidity conditions. By means of X-ray photoelectron spectroscopy, we find that the origin of the new bound excitonic species is the formation of bromine vacancies, leading to local changes in the dielectric response of the material. The recovery effect is attributed to vacancy filling by atmospheric oxygen and water.
Methylammonium lead tribromide (MAPbBr₃) perovskite single crystals demonstrate to be excellent direct X-ray and gamma-ray detectors with outstanding sensitivity and low limit of detection. Despite this, thorough studies on the photophysical effects of exposure to high doses of ionizing radiation on this material are still lacking. In this work, we present our findings regarding the effects of controlled X-ray irradiation on the optoelectronic properties of MAPbBr₃ single crystals. Irradiation is carried out in air with an imaging X-ray tube, simulating real-life application in a medical facility. By means of surface photovoltage spectroscopy, we find that X-ray exposure quenches free excitons in the material and introduces new bound excitonic species. Despite this drastic effect, the crystals recover after 1 week of storage in dark and low humidity conditions. By means of X-ray photoelectron spectroscopy, we find that the origin of the new bound excitonic species is the formation of bromine vacancies, leading to local changes in the dielectric response of the material. The recovery effect is attributed to vacancy filling by atmospheric oxygen and water.
Methylammonium lead tribromide (MAPbBr3) perovskite single crystals demonstrate to be excellent direct X-ray and gamma-ray detectors with outstanding sensitivity and low limit of detection. Despite this, thorough studies on the photophysical effects of exposure to high doses of ionizing radiation on this material are still lacking. In this work, we present our findings regarding the effects of controlled X-ray irradiation on the optoelectronic properties of MAPbBr3 single crystals. Irradiation is carried out in air with an imaging X-ray tube, simulating real-life application in a medical facility. By means of surface photovoltage spectroscopy, we find that X-ray exposure quenches free excitons in the material and introduces new bound excitonic species. Despite this drastic effect, the crystals recover after 1 week of storage in dark and low humidity conditions. By means of X-ray photoelectron spectroscopy, we find that the origin of the new bound excitonic species is the formation of bromine vacancies, leading to local changes in the dielectric response of the material. The recovery effect is attributed to vacancy filling by atmospheric oxygen and water.Methylammonium lead tribromide (MAPbBr3) perovskite single crystals demonstrate to be excellent direct X-ray and gamma-ray detectors with outstanding sensitivity and low limit of detection. Despite this, thorough studies on the photophysical effects of exposure to high doses of ionizing radiation on this material are still lacking. In this work, we present our findings regarding the effects of controlled X-ray irradiation on the optoelectronic properties of MAPbBr3 single crystals. Irradiation is carried out in air with an imaging X-ray tube, simulating real-life application in a medical facility. By means of surface photovoltage spectroscopy, we find that X-ray exposure quenches free excitons in the material and introduces new bound excitonic species. Despite this drastic effect, the crystals recover after 1 week of storage in dark and low humidity conditions. By means of X-ray photoelectron spectroscopy, we find that the origin of the new bound excitonic species is the formation of bromine vacancies, leading to local changes in the dielectric response of the material. The recovery effect is attributed to vacancy filling by atmospheric oxygen and water.
Author Lini, Matilde
Armaroli, Giovanni
Ferlauto, Laura
Lédée, Ferdinand
Fraboni, Beatrice
Ciavatti, Andrea
Borgatti, Francesco
Kovtun, Alessandro
Cavalcoli, Daniela
Milita, Silvia
Calabrese, Gabriele
AuthorAffiliation Department of Physics and Astronomy
Institute of Organic Synthesis and Photoreactivity(CNR-ISOF)
Interdepartmental Center for Industrial Research of the University of Bologna (CIRI-MAM)
Institute for Microelectronics and Microsystems (CNR-IMM)
AuthorAffiliation_xml – name: Institute of Organic Synthesis and Photoreactivity(CNR-ISOF)
– name: Institute for Microelectronics and Microsystems (CNR-IMM)
– name: Department of Physics and Astronomy
– name: Interdepartmental Center for Industrial Research of the University of Bologna (CIRI-MAM)
Author_xml – sequence: 1
  givenname: Giovanni
  orcidid: 0000-0002-0458-7027
  surname: Armaroli
  fullname: Armaroli, Giovanni
  organization: Department of Physics and Astronomy
– sequence: 2
  givenname: Laura
  orcidid: 0000-0003-2131-6795
  surname: Ferlauto
  fullname: Ferlauto, Laura
  email: laura.ferlauto@unibo.it
  organization: Interdepartmental Center for Industrial Research of the University of Bologna (CIRI-MAM)
– sequence: 3
  givenname: Ferdinand
  orcidid: 0000-0001-9949-0529
  surname: Lédée
  fullname: Lédée, Ferdinand
  organization: Interdepartmental Center for Industrial Research of the University of Bologna (CIRI-MAM)
– sequence: 4
  givenname: Matilde
  orcidid: 0000-0001-8970-5012
  surname: Lini
  fullname: Lini, Matilde
  organization: Department of Physics and Astronomy
– sequence: 5
  givenname: Andrea
  orcidid: 0000-0002-7877-7739
  surname: Ciavatti
  fullname: Ciavatti, Andrea
  organization: Department of Physics and Astronomy
– sequence: 6
  givenname: Alessandro
  orcidid: 0000-0002-7614-7100
  surname: Kovtun
  fullname: Kovtun, Alessandro
  organization: Institute of Organic Synthesis and Photoreactivity(CNR-ISOF)
– sequence: 7
  givenname: Francesco
  orcidid: 0000-0003-4659-4329
  surname: Borgatti
  fullname: Borgatti, Francesco
– sequence: 8
  givenname: Gabriele
  orcidid: 0000-0002-5869-4688
  surname: Calabrese
  fullname: Calabrese, Gabriele
  organization: Institute for Microelectronics and Microsystems (CNR-IMM)
– sequence: 9
  givenname: Silvia
  orcidid: 0000-0002-9612-2541
  surname: Milita
  fullname: Milita, Silvia
  organization: Institute for Microelectronics and Microsystems (CNR-IMM)
– sequence: 10
  givenname: Beatrice
  orcidid: 0000-0002-4875-3816
  surname: Fraboni
  fullname: Fraboni, Beatrice
  organization: Department of Physics and Astronomy
– sequence: 11
  givenname: Daniela
  orcidid: 0000-0002-2417-1248
  surname: Cavalcoli
  fullname: Cavalcoli, Daniela
  email: daniela.cavalcoli@unibo.it
  organization: Department of Physics and Astronomy
BookMark eNqNkctKAzEUhoMoatWt61mKMDX3ZjaCFm-gWLygu5AmmTZlJhmTGaE7X8FX9EkcaRHcyVn8h3N-fjjnG4BNH7wF4BDBIYIYnSidVO2GSCMOR3gD7KKC0lxghjd_e0p3wCClBYScYMi2wQ6hgiGO2S54ef36-HxQy_zGm05bk90F40qnVeuCz0KZtXObTeahDc18mfp5lU1iaGxsnU0_-7uzyfQ8kuzR-Vlls3FcplZVaR9slb3Yg7XugefLi6fxdX57f3UzPrvNFRaoza3SJRaaI2qpJqUgGBuhhBC0gFoYCO2IaDYlULCCEEwMV9P-CKOJGXHNKNkDp6vcppvW1mjr26gq2URXq7iUQTn5d-PdXM7CuxR8JApB-oCjdUAMb51Nraxd0raqlLehSxJzwhnqi_7DChmHuCCitx6vrD0fuQhd9P0TJILyB5pcQZNraOQbXPOMkQ
ContentType Journal Article
Copyright 2021 The Authors. Published by American Chemical Society
2021 The Authors. Published by American Chemical Society 2021 The Authors
Copyright_xml – notice: 2021 The Authors. Published by American Chemical Society
– notice: 2021 The Authors. Published by American Chemical Society 2021 The Authors
DBID 7X8
7S9
L.6
5PM
DOI 10.1021/acsami.1c16072
DatabaseName MEDLINE - Academic
AGRICOLA
AGRICOLA - Academic
PubMed Central (Full Participant titles)
DatabaseTitle MEDLINE - Academic
AGRICOLA
AGRICOLA - Academic
DatabaseTitleList

AGRICOLA
MEDLINE - Academic
DeliveryMethod fulltext_linktorsrc
Discipline Engineering
EISSN 1944-8252
EndPage 58308
ExternalDocumentID PMC8678983
c809286711
GrantInformation_xml – fundername: ;
  grantid: I38D18000150009
GroupedDBID -
23M
4.4
53G
55A
5GY
5VS
7~N
AABXI
ABFRP
ABMVS
ABUCX
ACGFS
ACS
AEESW
AENEX
AFEFF
AHGAQ
ALMA_UNASSIGNED_HOLDINGS
AQSVZ
EBS
ED
F5P
GGK
GNL
IH9
JG
K2
P2P
RNS
ROL
UI2
VF5
VG9
W1F
XKZ
---
.K2
5ZA
6J9
7X8
AAHBH
ABBLG
ABJNI
ABLBI
ABQRX
ADHLV
BAANH
CUPRZ
ED~
JG~
7S9
L.6
5PM
ID FETCH-LOGICAL-a281t-eacf28c614e4c3f8322d8a888490c8d00e73c5b308593323d6ab632dc3d76c543
IEDL.DBID ACS
ISSN 1944-8244
1944-8252
IngestDate Thu Aug 21 14:14:27 EDT 2025
Thu Jul 10 18:58:01 EDT 2025
Fri Jul 11 06:54:48 EDT 2025
Fri Dec 17 03:11:36 EST 2021
IsDoiOpenAccess true
IsOpenAccess true
IsPeerReviewed true
IsScholarly true
Issue 49
Keywords methylammonium lead bromide
excitons
surface photovoltage spectroscopy
hybrid lead halide perovskites
ionizing radiation
X-ray photoelectron spectroscopy
Language English
License Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
LinkModel DirectLink
MergedId FETCHMERGED-LOGICAL-a281t-eacf28c614e4c3f8322d8a888490c8d00e73c5b308593323d6ab632dc3d76c543
Notes ObjectType-Article-1
SourceType-Scholarly Journals-1
ObjectType-Feature-2
content type line 23
ORCID 0000-0002-0458-7027
0000-0002-7614-7100
0000-0002-2417-1248
0000-0001-9949-0529
0000-0002-5869-4688
0000-0001-8970-5012
0000-0003-2131-6795
0000-0002-7877-7739
0000-0002-4875-3816
0000-0003-4659-4329
0000-0002-9612-2541
OpenAccessLink https://pubmed.ncbi.nlm.nih.gov/PMC8678983
PMID 34851625
PQID 2605602938
PQPubID 23479
PageCount 8
ParticipantIDs pubmedcentral_primary_oai_pubmedcentral_nih_gov_8678983
proquest_miscellaneous_2636515154
proquest_miscellaneous_2605602938
acs_journals_10_1021_acsami_1c16072
PublicationCentury 2000
PublicationDate 2021-12-15
PublicationDateYYYYMMDD 2021-12-15
PublicationDate_xml – month: 12
  year: 2021
  text: 2021-12-15
  day: 15
PublicationDecade 2020
PublicationTitle ACS applied materials & interfaces
PublicationTitleAlternate ACS Appl. Mater. Interfaces
PublicationYear 2021
Publisher American Chemical Society
Publisher_xml – name: American Chemical Society
SSID ssj0063205
Score 2.4557655
Snippet Methylammonium lead tribromide (MAPbBr3) perovskite single crystals demonstrate to be excellent direct X-ray and gamma-ray detectors with outstanding...
Methylammonium lead tribromide (MAPbBr₃) perovskite single crystals demonstrate to be excellent direct X-ray and gamma-ray detectors with outstanding...
Methylammonium lead tribromide (MAPbBr 3 ) perovskite single crystals demonstrate to be excellent direct X-ray and gamma-ray detectors with outstanding...
SourceID pubmedcentral
proquest
acs
SourceType Open Access Repository
Aggregation Database
Publisher
StartPage 58301
SubjectTerms air
Biological and Medical Applications of Materials and Interfaces
bromine
detection limit
humidity
irradiation
lead
medical facilities
oxygen
X-radiation
X-ray photoelectron spectroscopy
Title X‑Ray-Induced Modification of the Photophysical Properties of MAPbBr3 Single Crystals
URI http://dx.doi.org/10.1021/acsami.1c16072
https://www.proquest.com/docview/2605602938
https://www.proquest.com/docview/2636515154
https://pubmed.ncbi.nlm.nih.gov/PMC8678983
Volume 13
hasFullText 1
inHoldings 1
isFullTextHit
isPrint
link http://utb.summon.serialssolutions.com/2.0.0/link/0/eLvHCXMwjZ1LSwMxEMeD6EUPvsX6IqLX1G6ym6bHWixFqBRrsbclr1JRdqXbHvTkV_Ar-kmc2W3RWlDP2Q1hJsn8kwy_IeQcRIZAjAyTyisGEcow4waC6ZrUkVY20HmxifaNbPXC637U_7rv-PmCz4MLbTMshRNYRKHBZrvCJaxgFEGN7mzPlYLnyYpwIg-Zgog1wzMu_I9ByGZzcnI-GfJbdGluFKijLIcSYlLJY3kyNmX7uohs_HPgm2R9KjFpvZgTW2TJJ9tk7Rt4cIfc9z_e3m_1C8PKHdY72k4d5gzlbqLpgIIspJ1hitSBwo-0g7f2I8SvYnu73jGXI0G70N2Tp43RC6jMp2yX9JpXd40Wm5ZYYJqrYMxg2x1wZSFG-9CKAS5vpzScisNaxSpXqfiqsJERORZNcOGkNmBsZ4WrShuFYo8sJ2ni9wl1GtSaCq00hofSiloAWs9EWnNjQJTZEjkDi8TTJZLF-es3D-LCTPHUTCVyOvNMDBMdXy904tNJFuPBS1ZAnajfvhFY2h1kYYlU59waPxfwjhhx2vMtycMwx2oriNs1JQ7-Nc5DssoxuyXgLIiOyPJ4NPHHIE_G5iSfmZ9sD-Ic
linkProvider American Chemical Society
linkToHtml http://utb.summon.serialssolutions.com/2.0.0/link/0/eLvHCXMwlV1LbxMxEB5V5QAceJQiwtNVe3WbtXcd5xgiqgBNFfWh5mb5FRVR7aJscggn_gJ_sb-kM04CSZGqcl3vWqOZsefzzvgbgD0EGZJoZLjSUXOMUI67MJLctpUtrPaZTc0m-seqd55_GRbDDThY3oVBIWqcqU5J_L_sAtkBPqOOOJknRjTccx8gEhHk0p3u6XLrVVKkmkU8mOdcY-BasjT-8z3FIl-vocr1msiVIHP4FAZ_xEu1Jd_3pxO373_eYm78D_mfwZMF4GSduYc8h41YbsHjFRrCF3AxvP71-8TOOPXx8DGwfhWogigZjVUjhiCRDS4r4iCYW5UN6B_-mMhYabzfGbiPY8lOcbqryLrjGWLOq3obzg8_nXV7fNFwgVuhswnHTXgktMeIHXMvR7TYg7Z4Rs7bTa9Dsxlb0hdOJpI0KWRQ1qHOg5ehpXyRy5ewWVZlfAUsWMRuOvfKOZErL9sZIj9XWCucQ4jmG7CLGjGLBVOblAsXmZmrySzU1ICdpYEMuj3lMmwZq2lt6BimmohV9F3vSGr0jiCxAa0165ofcyoPQ-Ta6yPlt8tEsq0xire1fH0vOT_Aw95Z_8gcfT7--gYeCap7yQTPirewORlP4zsELhP3PjnrDfFw6n0
linkToPdf http://utb.summon.serialssolutions.com/2.0.0/link/0/eLvHCXMwlV1LTxsxELYqkKr2AJS2ani0RnA1zdq7jnMMoRF9BEU81Nwsv1ZUoN0omxzCib_AX-SXMONsEGmlqr2udy3vzNjz2TP-hpADABkCaWSYVEEx8FCWWZ8LZtrSZEa5xMRiE_1TeXKZfhtmw_oeN96FgUFU0FMVg_g4q0c-rxkGks_wHKviJA5Z0WDdXcWYHZp1p3u-WH6l4DFvETbnKVPgvBZMjX98j_7IVUvIcjkv8pmj6a2Ti6chxvyS68PpxB6629_YG__zHzbIWg08aWduKW_Ii1BsktfP6Ajfkp_Dh7v7MzNjWM_DBU_7pcdMoqg8WuYUwCIdXJXIRTDXLh3gWf4YSVmxvd8Z2KOxoOfQ3U2g3fEMsOdN9Y5c9r5cdE9YXXiBGa6SCYPFOOfKgecOqRM5TnqvDOyV03bTKd9shpZwmRWRLE1w4aWxIHfvhG9Jl6XiPVkpyiJ8INQbwHAqddJankon2gkgQJsZw60FqOYaZB8kouuJU-kYE-eJnotJ12JqkL2FkjSYP8Y0TBHKaaVxOyabgFnU394RWPAdwGKDtJY0rEdzSg-NJNvLLcWvq0i2rcCbt5XY-qdxfiIvB8c9_ePr6fdt8opj-kvCWZLtkJXJeBp2Ab9M7Mdor4-Gh-0A
openUrl ctx_ver=Z39.88-2004&ctx_enc=info%3Aofi%2Fenc%3AUTF-8&rfr_id=info%3Asid%2Fsummon.serialssolutions.com&rft_val_fmt=info%3Aofi%2Ffmt%3Akev%3Amtx%3Ajournal&rft.genre=article&rft.atitle=X%E2%80%91Ray-Induced+Modification+of+the+Photophysical+Properties+of+MAPbBr3+Single+Crystals&rft.jtitle=ACS+applied+materials+%26+interfaces&rft.au=Armaroli%2C+Giovanni&rft.au=Ferlauto%2C+Laura&rft.au=Le%CC%81de%CC%81e%2C+Ferdinand&rft.au=Lini%2C+Matilde&rft.date=2021-12-15&rft.pub=American+Chemical+Society&rft.issn=1944-8244&rft.eissn=1944-8252&rft.volume=13&rft.issue=49&rft.spage=58301&rft.epage=58308&rft_id=info:doi/10.1021%2Facsami.1c16072&rft.externalDocID=c809286711
thumbnail_l http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/lc.gif&issn=1944-8244&client=summon
thumbnail_m http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/mc.gif&issn=1944-8244&client=summon
thumbnail_s http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/sc.gif&issn=1944-8244&client=summon