a-multimodal-wide-field-fourier-transform-raman-microscope

A Multimodal Wide-Field Fourier-Transform Raman Microscope

Raman microscopy is a powerful technique to determine the chemical composition of a sample. The main challenge of the state-of-the-art spontaneous Raman ...

We present a transient absorption setup combining broadband detection over the visible-UV range with high temporal resolution (∼20 fs) which is ideally suited to trigger and detect vibrational coherences in different classes of materials. We generate and detect coherent phonons (CPs) in single-layer (1L)-MoS, as a representative semiconducting 1L-transition metal dichalcogenide (TMD), where the confined dynamical interaction between excitons and phonons is unexplored. The coherent oscillatory motion of the out-of-plane A' phonons, triggered by the ultrashort laser pulses, dynamically modulates the excitonic resonances on a time scale of few tens of fs. We observe an enhancement by almost 2 orders of magnitude of the CP amplitude when detected in resonance with the C exciton peak, combined with a resonant enhancement of CP generation efficiency.  calculations of the change in the 1L-MoS band structure induced by the A' phonon displacement confirm a strong coupling with the C exciton. The resonant behavior of the CP amplitude follows the same spectral profile of the calculated Raman susceptibility tensor. These results explain the CP generation process in 1L-TMDs and demonstrate that CP excitation in 1L-MoS can be described as a Raman-like scattering process.

Strongly Coupled Coherent Phonons in Single-Layer MoS.

Spectrally resolved measurements of optical activity, such as circular dichroism (CD) and optical rotatory dispersion (ORD), are powerful tools to study chiroptical properties of (bio)molecular and nanoplasmonic systems. The wider utilization of these techniques, however, has been impeded by the bulky and slow design of conventional spectropolarimeters, which have been limited to a narrowband scanning approach for more than 50 years. In this work, we demonstrate broadband measurements of optical activity by combining a balanced detection scheme with interferometric Fourier-transform spectroscopy. The setup utilizes a linearly polarized light field that creates an orthogonally polarized weak chiral free-induction-decay field, along with a phase-locked achiral transmitted signal, which serves as the local oscillator for heterodyne amplification. By scanning the delay between the two fields with a birefringent common-path interferometer and recording their interferogram with a balanced detector that measures polarization rotation, broadband CD and ORD spectra are retrieved simultaneously with a Fourier transform. Using an incoherent thermal light source, we achieve state-of-the-art sensitivity for CD and ORD across a broad wavelength range in a remarkably simple setup. We further demonstrate the potential of our technique for highly sensitive measurements of glucose concentration and the real-time monitoring of ground-state chemical reactions. The setup also accepts broadband pulses and will be suitable for broadband transient optical activity spectroscopy and broadband optical activity imaging.

Broadband Optical Activity Spectroscopy with Interferometric Fourier-Transform Balanced Detection.

Acoustic vibrations of matter convey fundamental viscoelastic information that can be optically retrieved by hyperfine spectral analysis of the inelastic Brillouin scattered light. Increasing evidence of the central role of the viscoelastic properties in biological processes has stimulated the rise of non-contact Brillouin microscopy, yet this method faces challenges in turbid samples due to overwhelming elastic background light. Here, we introduce a common-path Birefringence-Induced Phase Delay (BIPD) filter to disentangle the polarization states of the Brillouin and Rayleigh signals, enabling the rejection of the background light using a polarizer. We demonstrate a 65 dB extinction ratio in a single optical pass collecting Brillouin spectra in extremely scattering environments and across highly reflective interfaces. We further employ the BIPD filter to image bone tissues from a mouse model of osteopetrosis, highlighting altered biomechanical properties compared to the healthy control. Results herald new opportunities in mechanobiology where turbid biological samples remain poorly characterized.

Article	Year
Strongly Coupled Coherent Phonons in Single-Layer MoS. ACS nano\| PubMed ID: 32233453	2020
Broadband Optical Activity Spectroscopy with Interferometric Fourier-Transform Balanced Detection. ACS photonics\| PubMed ID: 34476287	2021
Birefringence-induced phase delay enables Brillouin mechanical imaging in turbid media. Nature communications\| PubMed ID: 38898004	2024

C. Manzoni

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