TY - JOUR
T1 - Fiber Vector Light-Field-Based Tip-Enhanced Raman Spectroscopy
AU - Meng, Chao
AU - Xie, Zhonglin
AU - Lu, Fanfan
AU - Jiang, Shenlong
AU - Xu, Lei
AU - Zhang, Wending
AU - Luo, Yi
AU - Mei, Ting
N1 - Publisher Copyright:
© 2025 American Chemical Society.
PY - 2025/2/12
Y1 - 2025/2/12
N2 - Tip-enhanced Raman spectroscopy (TERS) has been extensively employed to investigate the light-matter interaction at the nanoscale. However, the current TERS strategies lack the ability to excite the low-background inhomogeneous electromagnetic field with significant enhancement of electric field, electric field gradient, and optomagnetic field, simultaneously. To overcome this, we developed a fiber vector light-field-based TERS strategy aimed at exploring the multipole Raman scattering processes of molecules. By modulating the excitation power, we have observed for the first time the Stark effect associated with Raman-forbidden transitions, revealing a strong electric-field gradient and optomagnetic effect within the plasmon cavity. Furthermore, by manipulating the plasmon tip to minimize the nanogap, we demonstrate that splitting occurs in the dipole Raman spectrum, indicating that the plasmon cavity enters a strong coupling regime. This fiber vector light-field-based TERS approach offers a unique opportunity to investigate weak matter responses with potential applications in single-molecule spectroscopy, sensors, and catalysis monitoring.
AB - Tip-enhanced Raman spectroscopy (TERS) has been extensively employed to investigate the light-matter interaction at the nanoscale. However, the current TERS strategies lack the ability to excite the low-background inhomogeneous electromagnetic field with significant enhancement of electric field, electric field gradient, and optomagnetic field, simultaneously. To overcome this, we developed a fiber vector light-field-based TERS strategy aimed at exploring the multipole Raman scattering processes of molecules. By modulating the excitation power, we have observed for the first time the Stark effect associated with Raman-forbidden transitions, revealing a strong electric-field gradient and optomagnetic effect within the plasmon cavity. Furthermore, by manipulating the plasmon tip to minimize the nanogap, we demonstrate that splitting occurs in the dipole Raman spectrum, indicating that the plasmon cavity enters a strong coupling regime. This fiber vector light-field-based TERS approach offers a unique opportunity to investigate weak matter responses with potential applications in single-molecule spectroscopy, sensors, and catalysis monitoring.
KW - Raman forbidden transitions
KW - Stark effect
KW - fiber vector light field
KW - tip-enhanced Raman scattering
UR - http://www.scopus.com/inward/record.url?scp=85217838343&partnerID=8YFLogxK
U2 - 10.1021/acs.nanolett.4c04379
DO - 10.1021/acs.nanolett.4c04379
M3 - 文章
AN - SCOPUS:85217838343
SN - 1530-6984
VL - 25
SP - 2112
EP - 2117
JO - Nano Letters
JF - Nano Letters
IS - 6
ER -