Ab initio molecular dynamics with the multipolar interaction for near-field photoexcitation
Project/Area Number |
17K14428
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Research Category |
Grant-in-Aid for Young Scientists (B)
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Allocation Type | Multi-year Fund |
Research Field |
Physical chemistry
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Research Institution | Hokkaido University |
Principal Investigator |
Iwasa Takeshi 北海道大学, 理学研究院, 助教 (80596685)
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Project Period (FY) |
2017-04-01 – 2020-03-31
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Project Status |
Completed (Fiscal Year 2019)
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Budget Amount *help |
¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000)
Fiscal Year 2019: ¥650,000 (Direct Cost: ¥500,000、Indirect Cost: ¥150,000)
Fiscal Year 2018: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000)
Fiscal Year 2017: ¥2,730,000 (Direct Cost: ¥2,100,000、Indirect Cost: ¥630,000)
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Keywords | 近接場光 / 多重極ハミルトニアン / Ehrenfest分子動力学 / 近接場光励起 / 第一原理分子動力学 / 時間依存密度汎関数理論 / 近接場光学 / 理論化学 / 物理化学 / 化学物理 |
Outline of Final Research Achievements |
Near field, a highly localized non-uniform light field around a surface, can excite a molecule to dipole-forbidden excited states and can induce unexpected photo chemical reactions. To understand the interactions between the near-field and molecule, a theoretical method beyond the widely used dipole approximation is required. We have developed a theory starting from the original form of the Hamiltonian before the dipole-approximation. The theory is applied to an Ehrenfest molecular dynamics. In addition, we studied structural and electronic properties and relaxation pathways in dipole-forbidden excited states of pure and adsorbed molecules relevant to the near-field excitations. Near-field vibrational excitations including near-field IR and Raman spectroscopic experiments have also been studied by means of an integrated computational chemistry and computational electrodynamics technique. In the future, a diabatic method for near-field photochemistry will be developed.
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Academic Significance and Societal Importance of the Research Achievements |
近接場光は伝搬光にはない局在性という特徴を持ち、双極子近似を超えた光学応答や、伝搬光とは異なる光化学反応も報告されている。また伝搬光は回折限界があるため、その空間分解能は波長の半分程度に制限されるが、近接場光ではこのような制限がなくなる。最近は特に走査型プローブ顕微鏡と組み合わせた実験も出てきており、単分子の分子内振動イメージングなどの原子レベルの分解能を持った分光や、単分子の光化学反応の誘起と解析も可能になってきている。近接場光と分子の相互作用から出てくる新しい科学を理解・開拓していくためには、双極子近似を超えた理論化学に基づいた本手法が必要であり、今後も更に発展させていく。
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Report
(4 results)
Research Products
(32 results)
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[Journal Article] Structural and Electronic Properties, Isomerization, and NO Dissociation Reactions on Au, Ag, Cu Clusters2019
Author(s)
Yusuke KONDO, Rina TAKAHARA, Hirono MOHRI, Makito TAKAGI, Satoshi MAEDA, Takeshi IWASA, Tetsuya TAKETSUGU
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Journal Title
Journal of Computer Chemistry, Japan
Volume: 18
Issue: 1
Pages: 64-69
DOI
NAID
ISSN
1347-1767, 1347-3824
Related Report
Peer Reviewed
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[Journal Article] Spiral Eu(III) coordination polymers with circularly polarized luminescence2018
Author(s)
Yasuchika Hasegawa, Yui Miura, Yuichi Kitagawa, Satoshi Wada, Takayuki Nakanishi, Koji Fushimi, Tomohiro Seki, Hajime Ito, Takeshi Iwasa, Tetsuya Taketsugu, Masayuki Gon, Kazuo Tanaka, Yoshiki Chujo, Shingo Hattori, Masanobu Karasawa and Kazuyuki Ishii
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Journal Title
Chemical Communications
Volume: 54
Issue: 76
Pages: 10695-10697
DOI
NAID
Related Report
Peer Reviewed
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[Journal Article] Optical readout of hydrogen storage in films of Au and Pd2017
Author(s)
Yoshiaki Nishijima, Shogo Shimizu, Keisuke Kurihara, Yoshikazu Hashimoto, Hajime Takahashi, Armandas Balcytis, Gediminas Seniutinas, Shinji Okazaki, Jurga Juodkazyte, Takeshi Iwasa, Tetsuya Taketsugu, Yoriko Tominaga, and Saulius Juodkazis
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Journal Title
Optics Express
Volume: 25
Issue: 20
Pages: 24081-24092
DOI
Related Report
Peer Reviewed / Open Access / Int'l Joint Research
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