4.8 Article

Resolving Molecular Structures with High-Resolution Tip-Enhanced Raman Scattering Images

Journal

ACS NANO
Volume 13, Issue 8, Pages 9342-9351

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b03980

Keywords

tip-enhanced Raman spectroscopy; structural characterization; atomic resolution; near field; plasmonics; TDDFT

Funding

  1. National Science Foundation Center for Chemical Innovation [CHE-1414466]
  2. National Science Foundation [ACI-1548562]

Ask authors/readers for more resources

Vibrational modes of a single molecule can be visualized by tip-enhanced Raman spectroscopy with atomic resolution. However, the exact vibrations associated with these Raman scattering images are still in debate due to the lack of theoretical interpretation. In this work, we systematically study the Raman scattering images of a single Co (II)-tetraphenylporphyrin molecule. The stable structure whose Raman scattering images consistently match experimental results is discovered. Furthermore, we elucidate the effects of near-field localizations and field gradient on the resolution in Raman scattering images. The approach of locally integrated Raman polarizability density employed in this work provides an intuitive explanation of the origin of the experimental Raman scattering images.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.8
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

Article Chemistry, Physical

Doubly resonant sum frequency spectroscopy of mixed photochromic isomers on surfaces reveals conformation-specific vibronic effects

Micah Raab, Jeffrey C. Becca, Jeongyun Heo, Chang-Keun Lim, Alexander Baev, Lasse Jensen, Paras N. Prasad, Luis Velarde

JOURNAL OF CHEMICAL PHYSICS (2019)

Article Chemistry, Physical

Atomistic Characterization of Plasmonic Dimers in the Quantum Size Regime

Pengchong Liu, Dhabih V. Chulhai, Lasse Jensen

JOURNAL OF PHYSICAL CHEMISTRY C (2019)

Review Physics, Applied

Atomistic electrodynamics simulations of plasmonic nanoparticles

Xing Chen, Pengchong Liu, Lasse Jensen

JOURNAL OF PHYSICS D-APPLIED PHYSICS (2019)

Article Multidisciplinary Sciences

High-resolution tip-enhanced Raman scattering probes sub-molecular density changes

Xing Chen, Pengchong Liu, Zhongwei Hu, Lasse Jensen

NATURE COMMUNICATIONS (2019)

Article Chemistry, Physical

Polarizable Frozen Density Embedding with External Orthogonalization

Partha Pratim Pal, Pengchong Liu, Lasse Jensen

JOURNAL OF CHEMICAL THEORY AND COMPUTATION (2019)

Article Chemistry, Applied

Shear-induced unidirectional deposition of bacterial cellulose microfibrils using rising bubble stream cultivation

Inseok Chae, Syed M. Q. Bokhari, Xing Chen, Rui Zu, Ke Liu, Ali Borhan, Venkatraman Gopalan, Jeffrey M. Catchmark, Seong H. Kim

Summary: A method is reported to induce the parallel packing of bacterial cellulose microfibrils by applying unidirectional shear stress during synthesis and deposition. The driving force for alignment is explained with mathematical estimation of the shear stress. Evidence of the parallel alignment of crystalline cellulose I alpha domains was obtained using nonlinear optical spectroscopy techniques.

CARBOHYDRATE POLYMERS (2021)

Article Chemistry, Physical

A discrete interaction model/quantum mechanical method for simulating surface-enhanced Raman spectroscopy in solution

Jeffrey C. Becca, Xing Chen, Lasse Jensen

Summary: In this study, an atomistic electrodynamics-quantum mechanical method was proposed to simulate the role of solvent in SERS, revealing the mechanism behind the solvent-induced enhancement of SERS. By implementing a cut-off based approach, the computational cost was reduced without sacrificing accuracy in describing the local environment of solvent molecules in SERS modeling.

JOURNAL OF CHEMICAL PHYSICS (2021)

Article Multidisciplinary Sciences

Near-infrared-featured broadband CO2 reduction with water to hydrocarbons by surface plasmon

Canyu Hu, Xing Chen, Jingxiang Low, Yaw-Wen Yang, Hao Li, Di Wu, Shuangming Chen, Jianbo Jin, He Li, Huanxin Ju, Chia-Hsin Wang, Zhou Lu, Ran Long, Li Song, Yujie Xiong

Summary: Imitating natural photosynthesis to synthesize hydrocarbon fuels is a viable strategy for solar-to-chemical energy conversion. Utilizing low-energy photons, especially near-infrared photons, has been a challenging aim to improve conversion efficiency. In this study, we report a broadband plasmon-induced CO2 reduction reaction with water, achieving a CH4 production rate of 0.55 mmol g(-1) h(-1) with 100% selectivity to hydrocarbon products under full-spectrum light illumination. The enhanced local electric field plays a crucial role in efficient multiphoton absorption and selective energy transfer, paving the way for low-energy photon utilization.

NATURE COMMUNICATIONS (2023)

Correction Multidisciplinary Sciences

Near-infrared-featured broadband CO2 reduction with water to hydrocarbons by surface plasmon (vol 14, 221, 2023)

Canyu Hu, Xing Chen, Jingxiang Low, Yaw-Wen Yang, Hao Li, Di Wu, Shuangming Chen, Jianbo Jin, He Li, Huanxin Ju, Chia-Hsin Wang, Zhou Lu, Ran Long, Li Song, Yujie Xiong

NATURE COMMUNICATIONS (2023)

Article Nanoscience & Nanotechnology

Bimetallic Synergy in Single-Atom Alloy Nanocatalysts for CO2 Reduction to Ethylene

Na Zhang, Yubing Si, Xing Chen, Xi Wang, Jiannian Yao

Summary: Carbon dioxide reduction is a promising strategy for generating valuable multi-carbon compounds. The single-atom Sc-doped Cu(111) surface shows excellent C2H4 selectivity due to the synergy of distinct adsorption sites. The Sc dopant promotes C-C dimerization via COCO, which is thermodynamically and kinetically favorable. This study provides insight into nanocatalyst design for reaction products with different chemical characters.

ACS APPLIED NANO MATERIALS (2023)

No Data Available