Remarkable Second Harmonic Generation Response in (C5H6NO)+(CH3SO3)−: Unraveling the Role of Hydrogen Bond in Thermal Driven Nonlinear Optical Switch

Heat‐activated second harmonic generation (SHG) switching materials are gaining interest for their ability to switch between SHG on and off states, offering potential in optoelectronic applications. The novel nonlinear optical (NLO) switch, (C5H6NO)+(CH3SO3)− (4‐hydroxypyridinium methylsulfonate, 4H...

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Published inAngewandte Chemie International Edition Vol. 63; no. 38; pp. e202408551 - n/a
Main Authors Zhang, Zi‐Peng, Liu, Xin, Wang, Rui‐Xi, Zhao, Shuang, He, Wen‐Jie, Chen, Hong‐Yu, Deng, Xue‐Bin, Wu, Li‐Ming, Zhou, Zhengyang, Chen, Ling
Format Journal Article
LanguageEnglish
Published Germany Wiley Subscription Services, Inc 16.09.2024
EditionInternational ed. in English
Subjects
4-hydroxypyridinium
Birefringence
Density functional theory
group rotation
Hydrogen bonding
Hydrogen bonds
Laser damage
NLO switch
Nonlinear optics
Optical switching
Optoelectronics
organic–inorganic hybrid
partial hydrogen bonds breaking
Room temperature
Second harmonic generation
Yield point
NLO switch
organic−inorganic hybrid
group rotation
partial hydrogen bonds breaking
4-hydroxypyridinum
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Abstract Heat‐activated second harmonic generation (SHG) switching materials are gaining interest for their ability to switch between SHG on and off states, offering potential in optoelectronic applications. The novel nonlinear optical (NLO) switch, (C5H6NO)+(CH3SO3)− (4‐hydroxypyridinium methylsulfonate, 4HPMS), is a near‐room‐temperature thermal driven material with a strong SHG response (3.3 × KDP), making it one of the most potent heat‐stimulated NLO switches. It offers excellent contrast of 13 and a high laser‐induced damage threshold (2.5 × KDP), with reversibility > 5 cycles. At 73 °C, 4HPMS transitions from the noncentrosymmetric Pna21 room temperature phase (RTP) to the centrosymmetric P21/c phase, caused by the rotation of the (C5H6NO)+ and (CH3SO3)− due to partially thermal breaking of intermolecular hydrogen bonds. The reverse phase change exhibits a large 50 °C thermal hysteresis. Density functional theory (DFT) calculations show that (C5H6NO)+ primarily dictates both the SHG coefficient (dij) and birefringence (▵n(Zeiss) = 0.216 vs ▵n(cal.) = 0.202 at 546 nm; Δn(Immersion) = 0.210 vs ▵n(cal.) = 0.198 at 589.3 nm), while the band gap (Eg) is influenced synergistically by (C5H6NO)+ and (CH3SO3)−. Additionally, 4HPMS‐RTP also exhibits mechanochromism upon grinding as well as an aggregation‐enhanced emission in a mixture of acetone and water. We report a novel material (C5H6NO)+(CH3SO3)− (4HPMS), exhibiting the strongest second harmonic generation (SHG) intensity among all heat‐stimulated nonlinear optical (NLO) switches. We unravel an unprecedently easier breaking of the shorter hydrogen bond and a rare large thermal hysteresis of 50 °C during the reversible structural phase transition.
AbstractList Heat-activated second harmonic generation (SHG) switching materials are gaining interest for their ability to switch between SHG on and off states, offering potential in optoelectronic applications. The novel nonlinear optical (NLO) switch, (C5H6NO)+(CH3SO3)- (4-hydroxypyridinium methylsulfonate, 4HPMS), is a near-room-temperature thermal driven material with a strong SHG response (3.3 × KDP), making it one of the most potent heat-stimulated NLO switches. It offers excellent contrast of 13 and a high laser-induced damage threshold (2.5 × KDP), with reversibility > 5 cycles. At 73 °C, 4HPMS transitions from the noncentrosymmetric Pna21 room temperature phase (RTP) to the centrosymmetric P21/c phase, caused by the rotation of the (C5H6NO)+ and (CH3SO3)- due to partially thermal breaking of intermolecular hydrogen bonds. The reverse phase change exhibits a large 50 °C thermal hysteresis. Density functional theory (DFT) calculations show that (C5H6NO)+ primarily dictates both the SHG coefficient (dij) and birefringence (∆n(Zeiss) = 0.216 vs ∆n(cal.) = 0.202 at 546 nm; Δn(Immersion) = 0.210 vs ∆n(cal.) = 0.198 at 589.3 nm), while the band gap (Eg) is influenced synergistically by (C5H6NO)+ and (CH3SO3)-. Additionally, 4HPMS-RTP also exhibits mechanochromism upon grinding as well as an aggregation-enhanced emission in a mixture of acetone and water.
Heat‐activated second harmonic generation (SHG) switching materials are gaining interest for their ability to switch between SHG on and off states, offering potential in optoelectronic applications. The novel nonlinear optical (NLO) switch, (C5H6NO)+(CH3SO3)− (4‐hydroxypyridinium methylsulfonate, 4HPMS), is a near‐room‐temperature thermal driven material with a strong SHG response (3.3 × KDP), making it one of the most potent heat‐stimulated NLO switches. It offers excellent contrast of 13 and a high laser‐induced damage threshold (2.5 × KDP), with reversibility > 5 cycles. At 73 °C, 4HPMS transitions from the noncentrosymmetric Pna21 room temperature phase (RTP) to the centrosymmetric P21/c phase, caused by the rotation of the (C5H6NO)+ and (CH3SO3)− due to partially thermal breaking of intermolecular hydrogen bonds. The reverse phase change exhibits a large 50 °C thermal hysteresis. Density functional theory (DFT) calculations show that (C5H6NO)+ primarily dictates both the SHG coefficient (dij) and birefringence (▵n(Zeiss) = 0.216 vs ▵n(cal.) = 0.202 at 546 nm; Δn(Immersion) = 0.210 vs ▵n(cal.) = 0.198 at 589.3 nm), while the band gap (Eg) is influenced synergistically by (C5H6NO)+ and (CH3SO3)−. Additionally, 4HPMS‐RTP also exhibits mechanochromism upon grinding as well as an aggregation‐enhanced emission in a mixture of acetone and water.
Heat-activated second harmonic generation (SHG) switching materials are gaining interest for their ability to switch between SHG on and off states, offering potential in optoelectronic applications. The novel nonlinear optical (NLO) switch, (C5H6NO)+(CH3SO3)- (4-hydroxypyridinium methylsulfonate, 4HPMS), is a near-room-temperature thermal driven material with a strong SHG response (3.3 × KDP), making it one of the most potent heat-stimulated NLO switches. It offers excellent contrast of 13 and a high laser-induced damage threshold (2.5 × KDP), with reversibility > 5 cycles. At 73 °C, 4HPMS transitions from the noncentrosymmetric Pna21 room temperature phase (RTP) to the centrosymmetric P21/c phase, caused by the rotation of the (C5H6NO)+ and (CH3SO3)- due to partially thermal breaking of intermolecular hydrogen bonds. The reverse phase change exhibits a large 50 °C thermal hysteresis. Density functional theory (DFT) calculations show that (C5H6NO)+ primarily dictates both the SHG coefficient (dij) and birefringence (▵n(Zeiss) = 0.216 vs ▵n(cal.) = 0.202 at 546 nm; Δn(Immersion) = 0.210 vs ▵n(cal.) = 0.198 at 589.3 nm), while the band gap (Eg) is influenced synergistically by (C5H6NO)+ and (CH3SO3)-. Additionally, 4HPMS-RTP also exhibits mechanochromism upon grinding as well as an aggregation-enhanced emission in a mixture of acetone and water.Heat-activated second harmonic generation (SHG) switching materials are gaining interest for their ability to switch between SHG on and off states, offering potential in optoelectronic applications. The novel nonlinear optical (NLO) switch, (C5H6NO)+(CH3SO3)- (4-hydroxypyridinium methylsulfonate, 4HPMS), is a near-room-temperature thermal driven material with a strong SHG response (3.3 × KDP), making it one of the most potent heat-stimulated NLO switches. It offers excellent contrast of 13 and a high laser-induced damage threshold (2.5 × KDP), with reversibility > 5 cycles. At 73 °C, 4HPMS transitions from the noncentrosymmetric Pna21 room temperature phase (RTP) to the centrosymmetric P21/c phase, caused by the rotation of the (C5H6NO)+ and (CH3SO3)- due to partially thermal breaking of intermolecular hydrogen bonds. The reverse phase change exhibits a large 50 °C thermal hysteresis. Density functional theory (DFT) calculations show that (C5H6NO)+ primarily dictates both the SHG coefficient (dij) and birefringence (▵n(Zeiss) = 0.216 vs ▵n(cal.) = 0.202 at 546 nm; Δn(Immersion) = 0.210 vs ▵n(cal.) = 0.198 at 589.3 nm), while the band gap (Eg) is influenced synergistically by (C5H6NO)+ and (CH3SO3)-. Additionally, 4HPMS-RTP also exhibits mechanochromism upon grinding as well as an aggregation-enhanced emission in a mixture of acetone and water.
Heat‐activated second harmonic generation (SHG) switching materials are gaining interest for their ability to switch between SHG on and off states, offering potential in optoelectronic applications. The novel nonlinear optical (NLO) switch, (C5H6NO)+(CH3SO3)− (4‐hydroxypyridinium methylsulfonate, 4HPMS), is a near‐room‐temperature thermal driven material with a strong SHG response (3.3 × KDP), making it one of the most potent heat‐stimulated NLO switches. It offers excellent contrast of 13 and a high laser‐induced damage threshold (2.5 × KDP), with reversibility > 5 cycles. At 73 °C, 4HPMS transitions from the noncentrosymmetric Pna21 room temperature phase (RTP) to the centrosymmetric P21/c phase, caused by the rotation of the (C5H6NO)+ and (CH3SO3)− due to partially thermal breaking of intermolecular hydrogen bonds. The reverse phase change exhibits a large 50 °C thermal hysteresis. Density functional theory (DFT) calculations show that (C5H6NO)+ primarily dictates both the SHG coefficient (dij) and birefringence (▵n(Zeiss) = 0.216 vs ▵n(cal.) = 0.202 at 546 nm; Δn(Immersion) = 0.210 vs ▵n(cal.) = 0.198 at 589.3 nm), while the band gap (Eg) is influenced synergistically by (C5H6NO)+ and (CH3SO3)−. Additionally, 4HPMS‐RTP also exhibits mechanochromism upon grinding as well as an aggregation‐enhanced emission in a mixture of acetone and water. We report a novel material (C5H6NO)+(CH3SO3)− (4HPMS), exhibiting the strongest second harmonic generation (SHG) intensity among all heat‐stimulated nonlinear optical (NLO) switches. We unravel an unprecedently easier breaking of the shorter hydrogen bond and a rare large thermal hysteresis of 50 °C during the reversible structural phase transition.
Heat‐activated second harmonic generation (SHG) switching materials are gaining interest for their ability to switch between SHG on and off states, offering potential in optoelectronic applications. The novel nonlinear optical (NLO) switch, (C 5 H 6 NO) + (CH 3 SO 3 ) − (4‐hydroxypyridinium methylsulfonate, 4HPMS), is a near‐room‐temperature thermal driven material with a strong SHG response (3.3 × KDP), making it one of the most potent heat‐stimulated NLO switches. It offers excellent contrast of 13 and a high laser‐induced damage threshold (2.5 × KDP), with reversibility > 5 cycles. At 73 °C, 4HPMS transitions from the noncentrosymmetric Pna 2 1 room temperature phase (RTP) to the centrosymmetric P 2 1 / c phase, caused by the rotation of the (C 5 H 6 NO) + and (CH 3 SO 3 ) − due to partially thermal breaking of intermolecular hydrogen bonds. The reverse phase change exhibits a large 50 °C thermal hysteresis. Density functional theory (DFT) calculations show that (C 5 H 6 NO) + primarily dictates both the SHG coefficient ( d ij ) and birefringence (▵ n (Zeiss) = 0.216 vs ▵ n (cal.) = 0.202 at 546 nm; Δ n (Immersion) = 0.210 vs ▵ n (cal.) = 0.198 at 589.3 nm), while the band gap ( E g ) is influenced synergistically by (C 5 H 6 NO) + and (CH 3 SO 3 ) − . Additionally, 4HPMS‐RTP also exhibits mechanochromism upon grinding as well as an aggregation‐enhanced emission in a mixture of acetone and water.
Author Zhao, Shuang
Wu, Li‐Ming
Liu, Xin
He, Wen‐Jie
Zhou, Zhengyang
Zhang, Zi‐Peng
Wang, Rui‐Xi
Chen, Hong‐Yu
Deng, Xue‐Bin
Chen, Ling
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  givenname: Zi‐Peng
  surname: Zhang
  fullname: Zhang, Zi‐Peng
  organization: Beijing Normal University
– sequence: 2
  givenname: Xin
  surname: Liu
  fullname: Liu, Xin
  organization: Beijing Normal University
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  givenname: Rui‐Xi
  surname: Wang
  fullname: Wang, Rui‐Xi
  organization: Beijing Normal University
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  givenname: Shuang
  surname: Zhao
  fullname: Zhao, Shuang
  organization: Beijing Normal University
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  fullname: He, Wen‐Jie
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  orcidid: 0000-0002-3693-4193
  surname: Chen
  fullname: Chen, Ling
  email: chenl@bnu.edu.cn
  organization: Beijing Normal University
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Keywords NLO switch
organic−inorganic hybrid
group rotation
partial hydrogen bonds breaking
4-hydroxypyridinum
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Snippet Heat‐activated second harmonic generation (SHG) switching materials are gaining interest for their ability to switch between SHG on and off states, offering...
Heat-activated second harmonic generation (SHG) switching materials are gaining interest for their ability to switch between SHG on and off states, offering...
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SubjectTerms 4-hydroxypyridinium
Birefringence
Density functional theory
group rotation
Hydrogen bonding
Hydrogen bonds
Laser damage
NLO switch
Nonlinear optics
Optical switching
Optoelectronics
organic–inorganic hybrid
partial hydrogen bonds breaking
Room temperature
Second harmonic generation
Yield point
Title Remarkable Second Harmonic Generation Response in (C5H6NO)+(CH3SO3)−: Unraveling the Role of Hydrogen Bond in Thermal Driven Nonlinear Optical Switch
URI https://onlinelibrary.wiley.com/doi/abs/10.1002%2Fanie.202408551
https://www.ncbi.nlm.nih.gov/pubmed/38858167
https://www.proquest.com/docview/3109844557
https://www.proquest.com/docview/3066793096
Volume 63
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