Yi-Da Hsieh

Spectrally interleaved, comb-mode-resolved spectroscopy using swept dual terahertz combs

Optical frequency combs are innovative tools for broadband spectroscopy because a series of comb modes can serve as frequency markers that are traceable to a microwave frequency standard. However, a mode distribution that is too discrete limits the spectral sampling interval to the mode frequency spacing even though individual mode linewidth is sufficiently narrow. Here, using a combination of a spectral interleaving and dual-comb spectroscopy in the terahertz (THz) region, we achieved a spectral sampling interval equal to the mode linewidth rather than the mode spacing. The spectrally interleaved THz comb was realized by sweeping the laser repetition frequency and interleaving additional frequency marks. In low-pressure gas spectroscopy, we achieved an improved spectral sampling density of 2.5 MHz and enhanced spectral accuracy of 8.39 × 10−7 in the THz region. The proposed method is a powerful tool for simultaneously achieving high resolution, high accuracy, and broad spectral coverage in THz spectroscopy.We demonstrated combination of gapless terahertz (THz) comb with dual-comb spectroscopy, namely gapless dual-THz-comb spectroscopy, to achieve the spectral resolution equal to width of the THz comb tooth. The gapless THz comb was realized by interpolating frequency gaps between the comb teeth with sweeping of a laser mode-locked frequency. The demonstration of low-pressure gas spectroscopy with gapless dual-THz-comb spectroscopy clearly indicated that the spectral resolution was decreased down to 2.5-MHz width of the comb tooth and the spectral accuracy was enhanced to 10-6 within the spectral range of 1THz. The proposed method will be a powerful tool to simultaneously achieve high resolution, high accuracy, and broad spectral coverage in THz spectroscopy.

Terahertz Comb Spectroscopy Traceable to Microwave Frequency Standard

The fine-structured spectrum of a terahertz (THz) frequency comb has been observed using asynchronous-optical-sampling THz time-domain spectroscopy with an extended time window covering multiple THz pulses. Fourier transformation of 10 consecutive THz pulses enables us to obtain the spectrum of THz comb mode having a linewidth of 25 MHz at intervals of 250 MHz. Further expansion of time window up to 100 consecutive THz pulses reduces the linewidth of THz comb mode down to 2.5 MHz while conserving interval of 250 MHz. The observed THz comb mode can be used as a precise and accurate frequency marker for broadband THz spectroscopy because it is phase-locked to a microwave frequency standard by laser control. The spectroscopy of pharmaceutical tablets and low-pressure molecular gas is used to demonstrate the utility of this approach, indicating a spectral resolution of 250 MHz. The proposed method enables frequency calibration of the THz spectrometer based on a microwave frequency standard.

Enhancement of spectral resolution and accuracy in asynchronous-optical-sampling terahertz time-domain spectroscopy for low-pressure gas-phase analysis

The spectral resolution and accuracy of asynchronous-optical-sampling terahertz time-domain spectroscopy (ASOPS-THz-TDS) were evaluated by examining low-pressure gas-phase samples. Use of dual 56-MHz, erbium (Er)-doped, mode-locked femtosecond fiber lasers enhanced the spectral resolution to as low as 50.5 MHz and the spectral accuracy to as low as 6.2 × 10(-6). The results indicate that ASOPS-THz-TDS has the potential to achieve high spectral resolution, high spectral accuracy, and wide spectral coverage at the same time. ASOPS-THz-TDS will open a new door to gas-phase spectroscopy of multiple chemical species in the field of atmospheric gas analysis.

Adaptive sampling dual terahertz comb spectroscopy using dual free-running femtosecond lasers.

Terahertz (THz) dual comb spectroscopy (DCS) is a promising method for high-accuracy, high-resolution, broadband THz spectroscopy because the mode-resolved THz comb spectrum includes both broadband THz radiation and narrow-line CW-THz radiation characteristics. In addition, all frequency modes of a THz comb can be phase-locked to a microwave frequency standard, providing excellent traceability. However, the need for stabilization of dual femtosecond lasers has often hindered its wide use. To overcome this limitation, here we have demonstrated adaptive-sampling THz-DCS, allowing the use of free-running femtosecond lasers. To correct the fluctuation of the time and frequency scales caused by the laser timing jitter, an adaptive sampling clock is generated by dual THz-comb-referenced spectrum analysers and is used for a timing clock signal in a data acquisition board. The results not only indicated the successful implementation of THz-DCS with free-running lasers but also showed that this configuration outperforms standard THz-DCS with stabilized lasers due to the slight jitter remained in the stabilized lasers.

Dynamic terahertz spectroscopy of gas molecules mixed with unwanted aerosol under atmospheric pressure using fibre-based asynchronous-optical-sampling terahertz time-domain spectroscopy

Terahertz (THz) spectroscopy is a promising method for analysing polar gas molecules mixed with unwanted aerosols due to its ability to obtain spectral fingerprints of rotational transition and immunity to aerosol scattering. In this article, dynamic THz spectroscopy of acetonitrile (CH3CN) gas was performed in the presence of smoke under the atmospheric pressure using a fibre-based, asynchronous-optical-sampling THz time-domain spectrometer. To match THz spectral signatures of gas molecules at atmospheric pressure, the spectral resolution was optimized to 1 GHz with a measurement rate of 1 Hz. The spectral overlapping of closely packed absorption lines significantly boosted the detection limit to 200 ppm when considering all the spectral contributions of the numerous absorption lines from 0.2 THz to 1 THz. Temporal changes of the CH3CN gas concentration were monitored under the smoky condition at the atmospheric pressure during volatilization of CH3CN droplets and the following diffusion of the volatilized CH3CN gas without the influence of scattering or absorption by the smoke. This system will be a powerful tool for real-time monitoring of target gases in practical applications of gas analysis in the atmospheric pressure, such as combustion processes or fire accident.

Super-resolution discrete Fourier transform spectroscopy beyond time-window size limitation using precisely periodic pulsed radiation

Fourier transform spectroscopy (FTS) has been widely used in a variety of fields in research, industry, and medicine due to its high signal-to-noise ratio, simultaneous acquisition of signals in a broad spectrum, and versatility for different radiation sources. Further improvement of the spectroscopic performance will widen its scope of applications. Here, we demonstrate improved spectral resolution by overcoming the time window limitation using discrete Fourier transform spectroscopy (dFTS) with precisely periodic pulsed terahertz (THz) radiation. Since infinitesimal resolution can be achieved at periodically discrete frequencies when the time window size is exactly matched to the repetition period T, a combination of THz-dFTS with a spectral interleaving technique achieves a spectral resolution only limited by the spectral interleaving interval. Linewidths narrower than 1/(50T) are fully resolved allowing the attribution of rotational-transition absorption lines of low-pressure molecular gases within a 1.25 MHz band. The proposed method represents a powerful tool to improve spectrometer performance and accelerate the practical use of various types of FTS.

Real-time absolute frequency measurement of continuous-wave terahertz radiation based on dual terahertz combs of photocarriers with different frequency spacings.

Real-time measurement of the absolute frequency of continuous-wave terahertz (CW-THz) radiation is required for characterization and frequency calibration of practical CW-THz sources. We proposed a method for real-time monitoring of the absolute frequency of CW-THz radiation involving temporally parallel, i.e., simultaneous, measurement of two pairs of beat frequencies and laser repetition frequencies based on dual THz combs of photocarriers (PC-THz combs) with different frequency spacings. To demonstrate the method, THz-comb-referenced spectrum analyzers were constructed with a dual configuration based on dual femtosecond lasers. Regardless of the presence or absence of frequency control in the PC-THz combs, a frequency precision of 10(-11) was achieved at a measurement rate of 100 Hz. Furthermore, large fluctuation of the CW-THz frequencies, crossing several modes of the PC-THz combs, was correctly monitored in real time. The proposed method will be a powerful tool for the research and development of practical CW-THz sources, and other applications.

Near-infrared broadband dual-frequency-comb spectroscopy with a resolution beyond the Fourier limit determined by the observation time window

We performed broadband dual-frequency-comb spectroscopy in the near-infrared region with a much higher resolution than the Fourier limit by using discrete Fourier transforms and spectral interleaving. We observed the resonant spectrum of a Fabry-Perot cavity over a spectral range of 187 to 218 THz using this technique, and measured its free spectral ranges and finesses. The recorded spectrum includes cavity resonance lines with widths of about 2 MHz, which is much narrower than the resolution of 48 MHz determined by the observation time window.

Dual-comb spectroscopic ellipsometry

Spectroscopic ellipsometry is a means of investigating optical and dielectric material responses. Conventional spectroscopic ellipsometry is subject to trade-offs between spectral accuracy, resolution, and measurement time. Polarization modulation has afforded poor performance because of its sensitivity to mechanical vibrational noise, thermal instability, and polarization-wavelength dependency. We combine spectroscopic ellipsometry with dual-comb spectroscopy, namely, dual-comb spectroscopic ellipsometry. Dual-comb spectroscopic ellipsometry (DCSE). DCSE directly and simultaneously obtains the ellipsometric parameters of the amplitude ratio and phase difference between s-polarized and p-polarized light signals with ultra-high spectral resolution and no polarization modulation, beyond the conventional limit. Ellipsometric evaluation without polarization modulation also enhances the stability and robustness of the system. In this study, we construct a polarization-modulation-free DCSE system with a spectral resolution of up to 1.2 × 10−5 nm throughout the spectral range of 1514–1595 nm and achieved an accuracy of 38.4 nm and a precision of 3.3 nm in the measurement of thin-film samples.Spectroscopic ellipsometry is an established technique to characterize the optical properties of a material. Here, Minamikawa et al. combine the method with dual-comb spectroscopy, which allows them to obtain ellipsometric parameters including the phase difference between s-polarized and p-polarized light.

Frequency-swept asynchronous-optical-sampling terahertz time-domain spectroscopy

We proposed frequency-swept asynchronous-optical-sampling terahertz time-domain spectroscopy to further improve the spectral resolution. The spectral resolution achieved here was 2.2 MHz, which is two orders of magnitude smaller than the mode-locked frequency.