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Chemical and Structural Trends of In...

Oxley, Benjamin Milton.

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Chemical and Structural Trends of Infrared Nonlinear Optical Properties in Alkali Chalcopnictates.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Chemical and Structural Trends of Infrared Nonlinear Optical Properties in Alkali Chalcopnictates./
作者:	Oxley, Benjamin Milton.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2024,
面頁冊數:	381 p.
附註:	Source: Dissertations Abstracts International, Volume: 85-11, Section: B.
Contained By:	Dissertations Abstracts International85-11B.
標題:	Inorganic chemistry. -
電子資源:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31243796
ISBN:	9798382761497

Chemical and Structural Trends of Infrared Nonlinear Optical Properties in Alkali Chalcopnictates.
Oxley, Benjamin Milton.

Chemical and Structural Trends of Infrared Nonlinear Optical Properties in Alkali Chalcopnictates. - Ann Arbor : ProQuest Dissertations & Theses, 2024 - 381 p.

Source: Dissertations Abstracts International, Volume: 85-11, Section: B.

Thesis (Ph.D.)--Northwestern University, 2024.

This item must not be sold to any third party vendors.

This thesis explores chalcopnictates developed for infrared nonlinear optics and how subtle chemical and structural changes can affect nonlinear behavior. These structure-property relationships are critical for developing the next generation of NLO materials and serve to guide synthetic chemists in their search for the next revolutionary material.Anionic substitution was used in LiAsS2-xSex to identify a high-performing material which could overcome the problems of the endmembers LiAsS2 and LiAsSe2. A mixed-anion material was discovered which avoided the extreme moisture sensitivity of the sulfide and the poor growth habits of the selenide. Multiwavelength measurements across five compositions showed chemical trends confirming that nonlinear response grows with atomic polarizability. Additionally, a large single crystal was grown and yielded one of the highest IR NLO responses to date, showing the power of optimization through substitution.The crystal structure of Li4P2S6, previously studied as a Li battery material, was determined through single crystal structure determination for the first time, confirming its noncentrosymmetric space group, P321. The material was found to be 0D, composed of molecular [P2S6] 4- units separated by 4 charge-balancing Li+ atoms. NLO studies found Li4P2S6 to be moderately performing as an SHG material, but high performing as a THG material, due to{A0}the wide bandgap enabling light conversion at wavelengths inaccessible to commercial materials. Additionally, the wide bandgap led to exceptional laser-induced damage threshold.The novel 1D materials RbSbP2S6 and {CE}{ostrok}-RbBiP2S6 were discovered and have many structural similarities, however, RbSbP2S6 is CS and {CE}{ostrok}-RbBiP2S6 is NCS. Additionally, the main difference between {CE}{ostrok}-RbBiP2S6 and its polymorph is the dimensionality, with the {CE}{lstrok}-phase taking a 2D structure. NLO studies were done to determine the effect of dimensionality on the nonlinearity of the RbBiP2S6 polymorphs, as well as the relationship of intensity between SHG and THG between RbSbP2S6 and {CE}{ostrok}-RbBiP2S6. Single crystal studies of {CE}{ostrok}-RbBiP2S6 show that additional symmetry constraints lead to a decreased nonlinearity.Alkali substitution was employed to explore a wide range of novel alkali chalcophosphates, demonstrating the power of chemical substitution and dimensional reduction as synthetic techniques for the discovery of new materials.{A0}

ISBN: 9798382761497Subjects--Topical Terms:

3173556
Inorganic chemistry.
Subjects--Index Terms:

Chalcogenide

Chemical and Structural Trends of Infrared Nonlinear Optical Properties in Alkali Chalcopnictates.
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245 1 0 $a Chemical and Structural Trends of Infrared Nonlinear Optical Properties in Alkali Chalcopnictates.
260 1 $a Ann Arbor : $b ProQuest Dissertations & Theses, $c 2024
300 $a 381 p.
500 $a Source: Dissertations Abstracts International, Volume: 85-11, Section: B.
500 $a Advisor: Kanatzidis, Mercouri G.
502 $a Thesis (Ph.D.)--Northwestern University, 2024.
506 $a This item must not be sold to any third party vendors.
520 $a This thesis explores chalcopnictates developed for infrared nonlinear optics and how subtle chemical and structural changes can affect nonlinear behavior. These structure-property relationships are critical for developing the next generation of NLO materials and serve to guide synthetic chemists in their search for the next revolutionary material.Anionic substitution was used in LiAsS2-xSex to identify a high-performing material which could overcome the problems of the endmembers LiAsS2 and LiAsSe2. A mixed-anion material was discovered which avoided the extreme moisture sensitivity of the sulfide and the poor growth habits of the selenide. Multiwavelength measurements across five compositions showed chemical trends confirming that nonlinear response grows with atomic polarizability. Additionally, a large single crystal was grown and yielded one of the highest IR NLO responses to date, showing the power of optimization through substitution.The crystal structure of Li4P2S6, previously studied as a Li battery material, was determined through single crystal structure determination for the first time, confirming its noncentrosymmetric space group, P321. The material was found to be 0D, composed of molecular [P2S6] 4- units separated by 4 charge-balancing Li+ atoms. NLO studies found Li4P2S6 to be moderately performing as an SHG material, but high performing as a THG material, due to{A0}the wide bandgap enabling light conversion at wavelengths inaccessible to commercial materials. Additionally, the wide bandgap led to exceptional laser-induced damage threshold.The novel 1D materials RbSbP2S6 and {CE}{ostrok}-RbBiP2S6 were discovered and have many structural similarities, however, RbSbP2S6 is CS and {CE}{ostrok}-RbBiP2S6 is NCS. Additionally, the main difference between {CE}{ostrok}-RbBiP2S6 and its polymorph is the dimensionality, with the {CE}{lstrok}-phase taking a 2D structure. NLO studies were done to determine the effect of dimensionality on the nonlinearity of the RbBiP2S6 polymorphs, as well as the relationship of intensity between SHG and THG between RbSbP2S6 and {CE}{ostrok}-RbBiP2S6. Single crystal studies of {CE}{ostrok}-RbBiP2S6 show that additional symmetry constraints lead to a decreased nonlinearity.Alkali substitution was employed to explore a wide range of novel alkali chalcophosphates, demonstrating the power of chemical substitution and dimensional reduction as synthetic techniques for the discovery of new materials.{A0}
590 $a School code: 0163.
650 4 $a Inorganic chemistry. $3 3173556
650 4 $a Materials science. $3 543314
650 4 $a Chemical engineering. $3 560457
653 $a Chalcogenide
653 $a Crystallography
653 $a Infrared nonlinear optics
653 $a Synthesis
653 $a Commercial materials
690 $a 0488
690 $a 0794
690 $a 0542
710 2 $a Northwestern University. $b Chemistry. $3 1030729
773 0 $t Dissertations Abstracts International $g 85-11B.
790 $a 0163
791 $a Ph.D.
792 $a 2024
793 $a English
856 4 0 $u https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31243796