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A decade-spanning high-resolution asynchronous optical sampling terahertz time-domain and frequency comb

Jacob T Good¹, Daniel B Holland¹, Ian A Finneran¹

¹Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, USA.

The Review of Scientific Instruments

|November 2, 2015

Summary

We developed a new TeraHertz Time-Domain Spectroscopy instrument using asynchronous optical sampling for high-resolution, decade-spanning measurements. This advanced tool enables precise gas-phase spectroscopy with tunable resolution, advancing THz region research.

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Area of Science:

Spectroscopy
Quantum Optics
Molecular Physics

Background:

Terahertz (THz) spectroscopy is crucial for analyzing molecular properties.
Existing THz-TDS instruments face limitations in resolution and tuning range.
High-resolution spectroscopic tools are needed for detailed gas-phase analysis.

Purpose of the Study:

To design and demonstrate a high-resolution, decade-spanning THz Time-Domain Spectroscopy (THz-TDS) instrument.
To achieve tunable spectral resolution from 80 MHz down to sub-MHz.
To enable new capabilities in gas-phase spectroscopy within the THz region.

Main Methods:

Utilized dual mode-locked femtosecond Ti:Sapphire oscillators with offset-locked repetition rates (100 Hz difference) via a Phase-Locked Loop (PLL).
Implemented a 12.5 ns time delay scan window with 15.6 fs resolution.
Synchronized pump oscillator to a Rb frequency standard for milliHertz (mHz) stability.

Main Results:

Achieved a 50 dB signal-to-noise ratio with 70 min of data acquisition.
Measured water vapor and acetonitrile absorption lines with high accuracy (sub-MHz deviation).
Demonstrated THz frequency comb spectroscopy (THz-FCS) with 5 MHz tooth width, achieving Doppler-limited precision.

Conclusions:

The developed ASOPS-based THz-TDS instrument offers unprecedented decade-spanning, tunable resolution.
This technology heralds a new generation of advanced gas-phase spectroscopic tools in the THz region.
The system's stability and precision open new avenues for molecular spectroscopy research.