
- Advanced Photonics
- Vol. 6, Issue 1, 016006 (2024)
Abstract
1 Introduction
Spectroscopy is the essential tool to investigate the structures of atoms and molecules, which has outstandingly contributed to atomic and molecular physics, analytical chemistry, and molecular biology. It also gained enormous significance in the fields of optical sensing, environmental study, and medical diagnostics. High spectral resolution is required in Doppler-free spectroscopy, high-Q cavity characterization, and precise sensing. Broadband spectroscopy with calibrated frequency is vital for investigations of multiple samples and interrogations of multiplexed sensors.
Spectrometers, widely implemented in spectroscopic measurement, are facilitated by using speckle patterns.1,2 The speckle pattern generated in disordered media is unique at each wavelength to reconstruct the input spectrum. Random reflection, scattering, and interference generate speckle patterns during the propagation of light in multimode fiber,3
The OFC,19,20 invented from the femtosecond pulse laser for optical metrology, has significantly promoted precision spectroscopy by building a link between optical frequency and radio frequency (RF). The equidistant coherent lines of OFC are also powerful tools to measure broadband spectra in direct comb spectroscopy, and line resolving can be performed using virtually imaged phase array,21 scanning Fabry–Perot (F–P) cavity,22 Fourier transform spectrometer,23 heterodyne interferometer,24 and dual-comb spectrometer.25 Advanced comb-based spectroscopy, such as dual-comb spectroscopy, can exploit the frequency resolution, frequency accuracy, and broad bandwidth of OFC.26 The resolution of comb-based spectroscopy is generally equal to the comb repetition rate. Although interleaved frequencies can be sampled by shifting the comb in principle, shifting two mutually coherent comb sources locked to atom clock at fine steps may only be performed in an advanced metrology laboratory.27 Spectroscopic techniques have developed together with the new demonstrations of comb sources in the last decade with different repetition frequencies at more wavelength regions.28
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EOFC can be generated by overdriving modulators using a high-voltage signal for high-order sidebands with a limited number of comb lines.30,31 Recent demonstrations using tailored waveforms in electro-optic modulation could cost-effectively generate more comb lines. Tailored waveforms are designed by inverse Fourier transformation of equidistant frequency components, including pseudo-random bit sequence,24,32 frequency chirp,33,34 pulse,35 or chirped pulse,36,37 generated from arbitrary waveform generator, programmable pulse generator, step recovery diode,38 and direct digital synthesizer.39 The repetition rate, depending on repetitive period, easily reaches megahertz, kilohertz or even sub-kilohertz levels.39 For these ultrafine EOFCs, the bandwidths, approximately proportional to repetition rate, are much more limited within electronics bandwidth. Although source lasers provide agility of center wavelength, due to pm precision of laser tuning, the measurement bandwidth of femtometer-resolution EOFC is hardly broadened.40 Extending the measurement bandwidth of ultrafine EOFC is attractive in precise spectroscopy and high-sensitivity sensing.
Here, a broadband speckle generated from whispering-gallery-mode (WGM) resonator breaks the bandwidth limitation of sub-femtometer-resolution EOFC to reach the tunable range of the source laser by linking its center frequency to an optical reference. High-resolution spectrum of sample and accurately determined frequency of each comb line are simultaneously obtained in sub-millisecond measurement time. Spectroscopic measurements of a fiber F–P cavity with 0.8 fm resolution and HCN gas cell with 40 nm bandwidth are, respectively, demonstrated with a fiber laser and an external cavity diode laser (ECDL). Our work leverages the advantages of speckle-based wavemeter and ultrafine EOFC to achieve ultrahigh-resolution spectroscopy with calibrated frequency over a broad bandwidth.
2 Principles and Methods
Long optical path length and random features are expected for speckle-based spectrometer or wavemeter. Among existing structures, WGM resonators have an exceptionally high Q-factor and easily excited multiple modes, which may simultaneously realize high resolution and miniaturization. The WGM barcodes, composed of multiple WGM resonances, are unique at different temperatures and were first proposed for temperature sensing.41 The WGM barcodes (or WGM speckle patterns) are also unique at each optical frequency (or wavelength), since depths, spacings, linewidths, and resonant wavelengths of WGM resonances are different. Here, a wavelength or optical frequency determination scheme based on WGM barcodes is proposed, which benefits from the crowded WGMs instead of trying to obtain a series of clean single-mode resonances. As shown in Fig. 1, the relative optical frequency of an unknown CW laser can be determined by comparing its individual WGM speckle with a prerecorded reference speckle, due to the relationship between WGM speckle and optical frequency. An ultrastable laser with known frequency
Figure 1.Speckle-based spectroscopy with an EOFC. Reference WGM speckle, excited from a microrod resonator attached with a tapered fiber, is unique to be a “ruler” to determine the calibrated frequency of probe laser for electro-optic comb generation. The measurement bandwidth of narrowband ultrafine electro-optic comb is unlocked to the range of tunable probe laser while its center frequency is determined. An ultrastable laser for frequency calibration also eliminates external perturbation-induced shift of speckle. Ultrahigh-resolution spectroscopy with far extended bandwidth can be performed.
An EOFC with arbitrarily selected repetition frequency can be generated from the CW laser. Especially, without physical restriction of cavity length, sub-femtometer-interval comb lines (less than 125 kHz at telecommunication wavelength) are feasible to record ultrahigh resolution spectra of the samples. Accordingly, the bandwidth of such an EOFC is only tens of picometers, due to the universal limitation of the number of comb lines in EOFC generation. Even so, a tunable seed laser can offer the frequency agility (
The WGM resonator in our experiment is a fused silica microrod with a diameter of 1.5 mm fabricated by using
A specific experimental setup is shown in Fig. 2. The ultrastable laser is a fiber laser locked to an ultrastable vacuum F–P cavity (provided by Stable Laser Systems) by using Pound–Drever–Hall locking technique. The finesse of cavity is up to 400 k. The nominal daily frequency drift is
Figure 2.The experimental setup of the speckle-based spectroscopy with an EOFC. AWG, arbitrary waveform generator; EOM, electro-optic modulator; SSBM, single-sideband modulator; WGM, whispering-gallery-mode; PD, photodetector; BPD, balanced photodetector.
The reference speckle and individual speckle are obtained by an RF-driven swept laser configuration. A linearly frequency swept RF signal with a sweep range of 8 GHz is applied on the single-sideband modulator (SSBM). The modulated laser, passing through the WGM resonator, is detected by a photodetector (PD) with 120 MHz bandwidth. The power fluctuation, caused by modulator frequency response, is eliminated by introducing a branch without a resonator. Only a tunable laser is utilized to prerecord the reference speckle by tuning its center frequency with a step of about 5 GHz (or 40 pm). The spectra of adjacent acquisitions have an overlapping region for stitching. The stitching points are calculated by using a cross-correlation algorithm. The overall reference speckle in 10 THz bandwidth can be obtained, which is limited by the operation window of the modulators and tunable range of source laser. The tunable laser and the ultrastable laser are used together to obtain measurement speckle for frequency determination. The cross-correlation curve calculated by comparing the measurement speckle and the reference speckle provides two distinguished peaks, representing the frequencies of tunable laser and ultrastable laser, respectively, while the measurement speckle is the superposition of each individual WGM speckle. Therefore, the calibrated frequency of the tunable laser can be derived from the relative peak locations. The calibrated readout prevents the linear drift of WGM speckle introduced by surrounding perturbation.
Another partial output of the tunable laser is modulated by using an electro-optic modulator (EOM) for EOFC generation. The modulator is driven by a tailored waveform designed by inverse Fourier transformation of multiple frequency components with parabolic phase relation (See Fig. S1 in the Supplementary Material). The driven signal in the frequency domain already looks like an “electrical comb.” The repetitive period is freely selected, 10 or
The spectra of the comb are obtained by Fourier transformation in digital processing. The spectra of samples are recorded by the ultrafine comb lines and demodulated after being compared with spectra of a branch without a sample. The tunable laser is not tuned during the measurement. The acquisition of WGM speckle and comb spectrum can be realized within
3 Results
3.1 High Resolution of the System
A fiber laser serves as the tunable laser in the demonstration of high-resolution measurement. The laser provides
Figure 3.Frequency determination for a fiber laser with a resolution of 100 kHz in 120 GHz bandwidth. (a) The speckle was recorded in 0.8 ms, corresponding to a frequency range of 8 GHz. (b) A zoom-in figure of (a) in 0.05 ms. (c) Cross-correlation result between the measurement speckle and the reference speckle over a bandwidth of 120 GHz. (d) and (e) are zoom-in correlation peaks of the reference laser and the fiber laser. The frequency of the tunable laser is determined to be 193.4046926 THz. The FWHMs of two peaks are both about 41 MHz. (f) Frequency readouts of the fiber laser with frequency modulation. (g) Fourier transformation of frequency readouts. The amplitude and frequency of the modulation are 100 kHz and 250 Hz, respectively. The sampling rate of the frequency readout is 1.25 kHz.
The resolution of frequency determination is evaluated by measuring a frequency-modulated fiber laser. Another AOM is introduced to modulate the center frequency of the probe laser. The readouts of the relative frequency obtained from the WGM speckles are shown in Fig. 3(f). The sinusoidal frequency modulation with an amplitude of 100 kHz is well demodulated. The refresh rate of the frequency determination is 1.25 kHz. The Fourier transformation shown in Fig. 3(g) reveals the modulation frequency at 250 Hz with an SNR of 261.
3.2 Spectroscopic Measurement of a High-Q F–P Cavity
The EOFC with 100 kHz line spacing and 2.5 GHz bandwidth is generated using a tailored waveform and an electro-optic modulator. The reflectance spectrum of an ultrahigh Q-factor fiber cavity composed of two fiber Bragg gratings is measured. The reflection band is about 60 GHz. The frequency shift introduced by AOM is 80.025 MHz, with a remainder of a quarter of repetition rate, to fold comb lines within RF detection bandwidth. The interferograms [see Fig. S2(a) in the Supplementary Material] in 1 ms recording time are Fourier-transformed to obtain the RF spectrum [see Fig. S2(b) in the Supplementary Material]. The optical spectrum, unfolded from the RF spectrum, is shown in Fig. 4(a) in linear scale. About 25,000 comb lines covering a bandwidth of 2.5 GHz are resolved. The center frequency in the optical domain is determined by the WGM speckle of the source laser in 0.8 ms. The measurement speed depends on the readout rate of frequency determination up to 1 kHz. The 25 kHz refresh rate of heterodyne interferometer could enable time-resolved measurement. A zoom-in figure in 2.5 MHz bandwidth is shown in Fig. 4(b), in which the linewidth of the comb line is Fourier-transform-limited to be 1 kHz. The line spacing is 100 kHz, corresponding to the resolution of spectroscopy. One resonance of the fiber cavity is represented in Fig. 4(b). The demodulated reflection spectrum is the maxima of comb lines in Fig. 4(a) dividing these in the reference branch without a sample. The ratio calculation is for eliminating the unflatness caused by the frequency response of devices.
Figure 4.Spectroscopic measurement of the reflection spectrum of a fiber F–P cavity. (a) Resolved spectrum of the EOFC in linear scale with a bandwidth of 2.5 GHz by Fourier transformation of data in 1 ms recording time. (b) Zoom-in figure of (a) in the box with resolved comb lines and one recorded resonance. The line spacing, corresponding to the spectral resolution, is 100 kHz. (c) The reflectance spectrum of a fiber F–P cavity in 117 GHz bandwidth. The spectrum is composed of 47 acquisitions by changing the center frequency of the tunable laser. Each acquisition contains 25,000 resolved comb lines with 100 kHz resolution over 2.5 GHz bandwidth. Two acquisitions with adjacent center frequencies are drawn in red and blue. (d) Zoom-in figure of (c) for an overlapped region in 0.8 GHz. The free spectral range of the fiber cavity is measured to be 105.6 MHz. (e) Zoom-in figure of a fiber cavity resonance. The linewidth of the resonance is 250 kHz, corresponding to a
The spectroscopy with extended bandwidth is performed by adjusting the center frequency of the fiber laser with temperature tuning. At each center wavelength, one acquisition is performed for spectroscopic measurement, and wavelength determination in 1 ms recording time. Each acquisition resolves 25,000 comb lines. All the reflectance spectra in the 117 GHz bandwidth are obtained from a sequence of 47 acquisitions, as shown in Fig. 4(c). The red curve is obtained from Fig. 4(a), and the blue curve is another adjacent channel. Totally
3.3 Broad Bandwidth of the System
The broad bandwidth of the system is performed by using an ECDL as the tunable probe laser. The tunable range of the laser is up to 9.5 THz or 76 nm. The wavelength tuning can be performed manually from the front panel, or by using a programmable software. A LabView-based program automatically controls the laser at sequentially selected wavelengths for reference speckle recording, frequency determination, and spectroscopic measurement. The nominal linewidth of ECDL is about 100 kHz. However, the free-running frequency stability in milliseconds is measured to be
Figure 5.Frequency determination for the external cavity laser diode with a resolution of 1 MHz in 9.5 THz bandwidth. (a) Cross-correlation result between the measurement speckle and reference speckle over a bandwidth of 9.5 THz. (b) Zoom-in correlation peak of the ECDL. The frequency is determined to be 190.164017 THz. (c) Zoom-in correlation peak of the reference laser. The FWHMs of two peaks are 31 and 54 MHz, respectively. (d) Frequency readouts of the ECDL with frequency modulation. (e) Fourier transformation of (d). The amplitude and frequency of the modulation are 1 MHz and 2.5 kHz, respectively. The low-frequency region is the frequency noise of the ECDL. The averaged frequency error of ECDL in 1 ms (recording time for following spectroscopy experiment) is 0.48 MHz. The sampling rate of frequency determination is 12.5 kHz.
To evaluate the resolution, frequency modulation with an amplitude of 1 MHz is also introduced by using AOM. The frequency readouts are shown in Fig. 5(d). The measurement rate of the frequency determination is increased to 12.5 kHz. The Fourier transformation reveals the frequency modulation with an amplitude of 1 MHz and a frequency of 2.5 kHz, as shown in Fig. 5(e). Intrinsic frequency noises of the ECDL in the low-frequency region with about 1-MHz amplitudes are also observed. Therefore, the readouts in Fig. 5(d) are the superposition of artificial frequency modulation and the frequency noise of the laser.
3.4 Spectroscopic Measurement of HCN Gas
An EOFC with 2.35-GHz bandwidth and 1-MHz repetition rate is generated to measure the transmission spectrum of a
Figure 6.Spectroscopic measurement of the transmission spectrum of HCN gas cell with 1 MHz resolution. (a) The reference database and (b) the measurement result of HCN transmittance spectrum in 4.74 THz bandwidth (corresponding to 38 nm) with a resolution of 1 MHz. The result is composed of 1890 acquisitions. Each acquisition contains 2350 resolved comb lines with a line spacing of 1 MHz in 1 ms recording time. (c) Residual error between (a) and (b). The standard deviation is 0.0069, corresponding to an SNR of 144.
Each acquisition at a wavelength contains 2350 comb lines with a resolution of 1 MHz. Totally,
4 Long-Term Stability
Although the WGM resonator is affected by surrounding temperature and vibration and looks easy to be disturbed, our system shows remarkable robustness in long-term measurement. The microrod resonator and tapered fiber are attached by using ultraviolet-curing adhesive. Adhesion prevents moderate change of coupling states. No transmitted power fluctuation is observed. The nonlinear response of input power can be ignored for a steady optical power. Other disturbing effects can be categorized into two aspects. One introduces linear frequency shift into the WGM speckle and measurement offset error. Another one distorts the WGM speckle and decreases the cross-correlation coefficient, including the change of linewidth, depth, and the nonlinear frequency shift. The main reason for the former disturbing effect is system linear response of environmental temperature change, which makes the WGM speckle shift in the frequency domain. The distortion of the WGM speckle in the latter aspect is typically caused by change of coupling state, polarization, and nonlinear environmental perturbation. The effect of these perturbations is ultimately reflected in the changes in free spectral range and the Q-factor of the WGM speckle. Since the frequency shift of resonance is real-time-calibrated by using a stable reference laser in the experiment, measurement offset error caused by the linear frequency shift can be real-time-eliminated in experiments. However, the distortion of WGM speckle cannot be eliminated. We experimentally monitor the stability of the proposed WGM resonator-based system in 10 h. The change of peak position in the cross-correlation curve indicates measurement offset error caused by the WGM speckle shift, and its coefficient represents the degree of WGM speckle distortion. The evolution of a selected resonance in reference speckle circled in Fig. 7(b) is shown in Fig. 7(a). Its center frequency shift is calibrated by a stable laser. The frequency bias for calibration is within
Figure 7.Long-term stability of WGM resonance and WGM-based wavemeter in 10 h. (a) Linewidth, depth, and center frequency evolution of the WGM resonance circled in (b). (b) A portion of WGM speckle. (c) Frequency bias obtained from the readout of stable laser for calibration. (d) Cross-correlation coefficients, which are always >0.64. (e) and (f) Cross-correlation peaks pointed by arrows in (d).
We further perform a simulation to quantitatively analyze the effects of the Q-factor and free spectral range. The simulated result is shown in Fig. 8 (see Fig. S9 in the Supplementary Material for specific simulated speckles). According to our fabrication and measurement, the initial situation of the cavity is on the top-left corner (Q-factor =
Figure 8.Cross-correlation coefficient versus the change of
5 Discussion
Optical path length in a speckle-based spectrometer or wavemeter is longer than in conventional spectrum analyzers. WGM resonators have an exceptionally high Q-factor compared to existing structures, which makes high resolution and miniaturization possible. The WGM resonator in our demonstration with sub-femtometer resolution in wavemeter or possibly sub-pm resolution in spectrometer is attractive with a millimeter-scale footprint. Considering inverse relationship between correlation peak FWHM, linking to frequency resolution, and resonator Q-factor is found in our simulation (see Fig. S6 in the Supplementary Material), higher resolution may be realized with a billion Q-factor WGM resonator.42 In addition, integrated WGM resonators on chip,43,44 together with recently developed integrated thin-film lithium niobate and electro-optic comb source,45,46 show the potential of a fully integrated system with a smaller footprint.
The operation bandwidths of our demonstration and most EOFC demonstrations are at the telecommunication band. In fact, electro-optic modulators working on almost all near-infrared band are commercially available, supporting the EOFC generation from 800 nm34 to
It is instructive to compare the performance of the proposed system with existing various spectroscopic measurement approaches, as shown in Fig. 9, which shows resolution, bandwidth, and measurement speed of selected representative spectroscopic methods. The proposed method combining EOFC and WGM speckle provides 8 fm spectral resolution with 80 nm bandwidth, comparable to interleaved fs-comb-based DCS. Remarkably, another demonstration of 0.8 fm resolution by the proposed scheme outperforms existing methods in bandwidth. Moreover, compared with other spectroscopic methods, the proposed system shows fine stability, a fast refresh rate, low complexity, and much cost-effectiveness (see detailed discussion in the Supplementary Material).
Figure 9.Performance metric chart of various spectroscopic methods – EOFC, dual-comb spectroscopy, reconstructive spectrometers – using resolution and bandwidth constraints.
6 Conclusion
Here, spectroscopic measurement is experimentally demonstrated with a combination of ultrafine EOFC and speckle pattern. The combination fully exploits the high resolution and broad bandwidth property of the speckle-based wavemeter and breaks through the bandwidth limitation of the ultrafine EOFC. Few-gigahertz electronics and telecommunication components are predominantly used in the proposed scheme. The compact and cost-effective system with high resolution and broad bandwidth will be a prospective way toward precise investigation in biochemical sensing and physics.
Bingxin Xu is currently a postdoctoral researcher at Max-Planck Institute of Quantum Optics, Germany. He received his PhD in electronics engineering from Shanghai Jiao Tong University in 2021. His research interests are dual-comb spectroscopy, electro-optic frequency comb, optical sampling, and reconstructive spectrometer.
Yangyang Wan received his PhD from Shanghai Jiao Tong University, Shanghai, China, in 2023. He received his BS degree from Huazhong University of Science and Technology, Wuhan, China. He is currently a postdoctoral researcher at the Center for Intelligent Photonics, Shanghai Jiao Tong University, Shanghai, China. His research interests include spectrum measurement, distributed optical fiber sensing, and machine learning.
Xinyu Fan received his BS and MS degrees in applied physics from Shanghai Jiao Tong University in 2000 and 2003, respectively, and his PhD in electrical engineering from the University of Tokyo in 2006. He joined NTT Access Network Service Systems Laboratories in 2006, where he researched on optical reflectometry and optical measurement. Since 2012, he has been in the Department of Electronic Engineering, Shanghai Jiao Tong University, where he is currently a professor. His research interests include distributed fiber-optic sensing, dual-comb spectroscopy, and optical precision measurement technology.
Zuyuan He received his BS and MS degrees in electronic engineering from Shanghai Jiao Tong University in 1984 and 1987, respectively, and his PhD in optoelectronics from the University of Tokyo in 1999. He joined Nanjing University of Science and Technology as a research associate in 1987, and became a lecturer in 1990. From 1995, he was a research fellow and later a research associate at the University of Tokyo. In 2001, he joined CIENA Corporation as a lead engineer. He returned to the University of Tokyo as a lecturer in 2003, and became an associate professor in 2005, and a full professor in 2010. He is currently a chair professor and the director of the State Key Laboratory of Advanced Optical Communication Systems and Networks, Shanghai Jiao Tong University. His current research interests include optical fiber sensors, specialty optical fibers, and optical inter-connection.
References
[13] B. Redding et al. Evanescently coupled multimode spiral spectrometer. Optica, 3, 956-962(2016).
[16] Y. Kwak et al. A pearl spectrometer. Nano Lett., 21, 921-930(2020).
[17] Q. Cen et al. Microtaper leaky-mode spectrometer with picometer resolution. eLight, 3, 9(2023).
[19] T. Udem, R. Holzwarth, T. W. Hänsch. Optical frequency metrology. Nature, 416, 233-237(2002).
[20] S. A. Diddams. The evolving optical frequency comb. J. Opt. Soc. Am. B, 27, B51-B62(2010).
[25] I. Coddington, N. Newbury, W. Swann. Dual-comb spectroscopy. Optica, 3, 414-426(2016).
[27] S. A. Meek et al. Doppler-free Fourier transform spectroscopy. Opt. Lett., 43, 162-165(2018).
[35] G. Millot et al. Frequency-agile dual-comb spectroscopy. Nat. Photonics, 10, 27-30(2016).
[42] A. Shitikov et al. Billion
[48] B. Xu, T. W. Hänsch, N. Picqué. Near-ultraviolet dual-comb spectroscopy with photon-counting, SM1D–4(2022).

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