Hole Burning Research Articles

Modeling of fluence-dependent hole-burned spectra and hole-growth kinetics using multiple two-level system model.

Numerical formalism is presented that perfectly describes resonant low-temperature hole-burned spectra (including zero-phonon holes, ZPHs) and spectral hole-growth dynamics of Al-phthalocyanine tetrasulphonate embedded in hyperquenched glassy water films over more than seven orders of fluence magnitude (0.4 µJ/cm2-5.9 J/cm2). Frequency changes during spectral hole-burning (HB) are traditionally explained with the help of a single extrinsic two-level-system (TLSext) associated with impurity molecules. The new multiple two-level system (n-TLSext) models and data analysis presented in this work show that each chromophore in an amorphous medium can couple with multiple independent TLSext, which maintain perfect photo-memory, allowing a full return of the photoproduct to the initial ("preburn") state. Modeling reveals that the experimentally observed narrow photoproduct peak at higher energies, in close vicinity of the zero-phonon hole (ZPH), reflects a dynamical feature of the HB process populating so-called "terminal" states (states that do not interact with laser excitation). Within the n-TLSext model, each chromophore possesses multiple possibilities to create a photoproduct when in interaction with the burning laser, i.e., chromophores can interact with burning laser-light multiple times until reaching the terminal states. Due to phonon-assisted absorption, terminal states are typically at higher energies than the ZPH, in agreement with the hole burned spectra reported for many molecules embedded in various amorphous solids. However, many HB systems reveal both blue- (high-energy) and red-shifted (low-energy) antiholes (i.e., photoproducts). We suggest that future modeling of resonant holes in various proteins using our n-TLSext model will provide more insight on the complexity of the protein energy landscape.

An 8-channel narrow linewidth multi-wavelength laser hybrid integrated by photonic wire bonding structures for DWDM systems

An 8-channel monolithically integrated narrow linewidth multi-wavelength laser array (NL-MLA) combined with the commercial 8 × 1 planar lightwave circuit (PLC) coupler by the photonic wire bonding (PWB) technique is demonstrated in this paper. A distributed feedback (DFB) laser with the high-reflection and anti-reflection coatings (HR-AR) and the tapered asymmetric corrugation-pitch-modulated (TACPM) grating structure is proposed. The TACPM grating is achieved by the reconstruction equivalent chirp (REC) technique, which is low-cost and of high wavelength accuracy. According to the numerical simulation results, under the unavoidable impact of the facet phase of the HR end, the TACPM DFB laser suppresses the longitudinal spatial hole burning (LSHB) effect significantly, while having better single-mode performance and control of wavelength compared with the conventional HR-AR DFB laser. An 8-channel HR-AR TACPM DFB NL-MLA is fabricated with the 0.8 nm wavelength spacing design. The hybrid integration between the 8-channel NL-MLA and the PLC chip is achieved using the PWB technique. Both good single-mode performance and accurate wavelength interval of 0.8 nm can be obtained when all channels work simultaneously. The laser linewidth is below 273.8 kHz with good uniformity, and the relative intensity noise is under −159.6 dB/Hz for each channel.

Toward liquid cell quantum sensing: Ytterbium complexes with ultranarrow absorption.

The energetic disorder induced by fluctuating liquid environments acts in opposition to the precise control required for coherence-based sensing. Overcoming fluctuations requires a protected quantum subspace that only weakly interacts with the local environment. We report a ytterbium complex that exhibited an ultranarrow absorption linewidth in solution at room temperature with a full width at half maximum of 0.625 milli-electron volts. Using spectral hole burning, we measured an even narrower linewidth of 410 pico-electron volts at 77 kelvin. Narrow linewidths allowed low-field magnetic circular dichroism at room temperature, used to sense Earth-scale magnetic fields. These results demonstrated that ligand protection in lanthanide complexes could substantially diminish electronic state fluctuations. We have termed this system an "atomlike molecular sensor" (ALMS) and proposed approaches to improve its performance.

Spectral Hole-Burning Studies of a Mononuclear Eu(III) Complex Reveal Narrow Optical Linewidths of the 5D0→7F0 Transition and Seconds Long Nuclear Spin Lifetimes.

Coordination complexes of rare-earth ions (REI) show optical transitions with narrow linewidths enabling the creation of coherent light-matter interfaces for quantum information processing (QIP) applications. Among the REI-based complexes, Eu(III) complexes showing the 5D0→7F0 transition are of interest for QIP applications due to the narrow linewidths associated with the transition. Herein, we report on the synthesis, structure, and optical properties of a novel Eu(III) complex and its Gd(III) analogue composed of 2,9-bis(pyrazol-1-yl)-1,10-phenanthroline (dpphen) and three nitrate (NO3) ligands. The Eu(III) complex-[Eu(dpphen)(NO3)3]-showed sensitized metal-centred emission (5D0→7FJ; J=0,1,2,3, 4, 5, or 6) in the visible region, upon irradiation of the ligand-centred band at 369 nm, with the 5D0→7F0 transition centred at 580.9 nm. Spectral hole-burning (SHB) studies of the complex with stoichiometric Eu(III) concentration revealed a narrow homogeneous linewidth (Γh) of 1.55 MHz corresponding to a 0.205 μs long optical coherence lifetime (T2opt). Remarkably, long nuclear spin lifetimes (T1spin) of up to 41 s have been observed for the complex. The narrow optical linewidths and long T1spin lifetimes obtained for the Eu(III) complex showcase the utility of Eu(III) complexes as tuneable, following molecular engineering principles, coherent light-matter interfaces for QIP applications.

Conformation-Selective Ultraviolet-Ultraviolet Hole Burning Spectra of Ubiquitin Ions in a Cryogenic Ion Trap.

Understanding the structural variations of conformational isomers in proteins is crucial for elucidating protein folding mechanisms. Here, we present a novel method for obtaining conformation-selective ultraviolet (UV)-UV hole burning (HB) spectra of ubiquitin ions ((Ubi+zH)+z, z = 7-10) produced via electrospray ionization. Our approach involves binding multiple N2 molecules to ubiquitin ions ((Ubi+zH)+z(N2)m, m = 1-55) within a cryogenic ion trap. Upon exposure to UV irradiation, efficient fragmentation of (Ubi+zH)+z(N2)m occurs, primarily yielding bare (Ubi+zH)+z ions as fragments. The significant mass difference between the parent and fragment ions facilitates the acquisition of UV-UV HB spectra, which reveal the presence of at least two distinct conformers. Molecular dynamics simulations suggest that these conformers correspond to A-state structures, differing only in the interactions of a tyrosine residue with neighboring residues. Our findings underscore UV-UV HB spectroscopy of protein ions as a powerful tool for exploring diverse protein isomers.

Cavity-enhanced narrowband spectral filters using rare-earth ions doped in thin-film lithium niobate

On-chip optical filters are fundamental components in optical signal processing. While rare-earth ion-doped crystals offer ultra-narrow optical filtering via spectral hole burning, their applications have primarily been limited to those using bulk crystals, restricting their utility. In this work, we demonstrate cavity-enhanced spectral filtering based on rare-earth ions in an integrated nonlinear optical platform. We incorporate rare-earth ions into high quality-factor ring resonators patterned in thin-film lithium niobate. By spectral hole burning at 4 K in a critically coupled resonance mode, we achieve bandpass filters ranging from 7 MHz linewidth, with 13.0 dB of extinction, to 24 MHz linewidth, with 20.4 dB of extinction. By reducing the temperature to 100 mK to eliminate phonon broadening, we achieve an even narrower linewidth of 681 kHz, which is comparable to the narrowest filter linewidth demonstrated in an integrated photonic device, while only requiring a small device footprint. Moreover, the cavity enables reconfigurable filtering by varying the cavity coupling rate. For instance, as opposed to the bandpass filter, we demonstrate a bandstop filter utilizing an under-coupled ring resonator. Such versatile integrated spectral filters with high extinction ratio and narrow linewidth could serve as fundamental components for optical signal processing and optical memories on-a-chip.

Impact of Grating Duty-Cycle Randomness on DFB Laser Performance

The duty-cycle randomness (DCR) of the Bragg grating of the distributed feedback (DFB) lasers introduced by the fabrication process is inevitable, even with state-of-the-art technologies such as electron beam lithography and dry or wet etching.This work investigates the impact of grating DCR on DFB laser performance through numerical simulations. The result reveals that such randomness causes a reduction in the side mode suppression ratio (SMSR), and deteriorates the noise characteristics, i.e., broadens the linewidth and increases the relative intensity noise (RIN). With the grating DCR, the effective grating coupling coefficient decreases as evidenced by the reduced Bragg stopband width. However, the longitudinal spatial hole burning (LSHB) effect in the DFB lasers can somewhat be diminished by the grating DCR. The seriousness of these effects depends on different grating structures and their coupling strengths. Our simulation shows that a degradation of 17 dB can be brought to the SMSR of the uniform grating DFB lasers with their duty cycles taking a deviation of ±25% in a uniformly distributed random fashion. It also broadens the linewidth of the quarter-wavelength phase-shifted DFB lasers by more than 2.5 folds. The impact of this effect on the RIN is moderate—less than 2%. All the performance deteriorations can partially be attributed to the effective reduction in the grating coupling coefficient of around 20% by such a DCR.

High-power and narrow-linewidth nanosecond pulsed intracavity crystalline Raman laser operating at 1.7 µm

We report on a high-power and narrow-linewidth nanosecond pulsed intracavity crystalline Raman laser at 1.7 µm. Driven by an acousto-optically Q-switched 1314 nm two-crystal Nd:YLF laser, the highly efficient cascaded YVO4 Raman laser at 1715nm was obtained within the well-designed L-shaped resonator. Thanks to the absence of spatial hole burning in the stimulated Raman scattering process, significant spectral purification of second-Stokes radiation was observed by incorporating a fused silica etalon in the high-Q fundamental cavity. Under the repetition rate of 4 kHz, the highest average output power for single longitudinal mode operation was up to 2.2 W with the aid of precision vibration isolation and precision temperature controlling, corresponding to the pulse duration of ∼2.8 ns and the spectral linewidth of ∼330 MHz. Further increasing the launched pump power, the second-Stokes laser tended toward be always multimode, and the maximum average output power amounted to 4.8 W with the peak power of ∼0.8 MW and the spectral linewidth of ∼0.08 nm. The second-Stokes emission was near diffraction limited with M2 < 1.4 across the whole pump power range.

Tunable superluminal propagation at spectral hole-burning regions in magneto-optical atomic medium

In the context of spectral hole-burning, normal dispersion with subluminal propagation is usually observed in the spectral hole-burning depth region. However, anomalous dispersion can occur in the continuous absorption peak region, which leads to superluminal light propagation. In this paper, we report an unusual behavior of dispersion at discontinued absorption kink regions. We demonstrate both normal dispersion at the kink absorption region and anomalous dispersion at the spectral hole-burning depth region. The unusual dispersion leads to a positive group index in the absorption kink region and a negative group index in the spectral hole-burning depth region. The spectral hole-burning is due to variation of magnetization rather than the molecular distribution. The outcomes of our work offer promising applications in communication technologies and storage devices.

Theoretical model of passive mode-locking in terahertz quantum cascade lasers with distributed saturable absorbers

Abstract In research and engineering, short laser pulses are fundamental for metrology and communication. The generation of pulses by passive mode-locking is especially desirable due to the compact setup dimensions, without the need for active modulation requiring dedicated external circuitry. However, well-established models do not cover regular self-pulsing in gain media that recover faster than the cavity round trip time. For quantum cascade lasers (QCLs), this marked a significant limitation in their operation, as they exhibit picosecond gain dynamics associated with intersubband transitions. We present a model that gives detailed insights into the pulse dynamics of the first passively mode-locked QCL that was recently demonstrated. The presence of an incoherent saturable absorber, exemplarily realized by multilayer graphene distributed along the cavity, drives the laser into a pulsed state by exhibiting a similarly fast recovery time as the gain medium. This previously unstudied state of laser operation reveals a remarkable response of the gain medium on unevenly distributed intracavity intensity. We show that in presence of strong spatial hole burning in the laser gain medium, the pulse stabilizes itself by suppressing counter-propagating light and getting shortened again at the cavity facets. Finally, we study the robustness of passive mode-locking with respect to the saturable absorber properties and identify strategies for generating even shorter pulses. The obtained results may also have implications for other nanostructured mode-locked laser sources, for example, based on quantum dots.

Subtomographic imaging of a polarisation sensitive phase pattern localised in phase space

A transparent polarisation-sensitive phase pattern changes the phase of transmitted light without absorption, whereas this change of phase depends on the polarisation of incident light. A position-localised polarisation-dependent phase pattern is imprinted onto the phase-space of atoms by using atomic state dependent velocity-selective hole burning. A phase-space localised pattern is a higher dimensional generalisation of patterns localised in the position-space. Such a pattern cannot be imaged with a lens. The imprinted pattern is localised in a unique three-dimensional subspace of the six-dimensional phase-space of atoms. The phase-space localised pattern transforms the polarisation of light transmitting through it. This pattern is tomographically imaged at room temperature by measuring the intensity of the transmitted imaging laser beam of variable frequency with a camera after its polarisation analysis. Two sub-tomographs of the imprinted phase-space localised pattern are constructed. This paper presents a concept and experiment of imprinting and imaging of a polarisation-sensitive phase pattern localised in the phase-space.

Optimization of Dual-Wavelength linear cavity Erbium-Doped fiber laser based on pairs of fiber Bragg gratings

There are few reports in the field of linear cavity dual-wavelength fiber lasers about the laser output characteristics when 3-dB fiber loop mirror (FLM) and Fiber Bragg grating (FBG) are used as full reflective mirrors, respectively. Additionally, there is scarce research on further tuning of the FBG parameters (reflectivity and center wavelength interval) to study dual-wavelength fiber lasers. In this paper, we compare the performances of dual-wavelength lasing outputs between the 3-dB FLM-FBG cavity and the FBG-only cavity in a linear-cavity erbium-doped fiber laser (EDFL) based on the polarization hole burning effect. The results show that the optical signal-to-noise ratios (OSNRs) of the dual-wavelength lasing outputs with the FBG-only cavity are approximately 4 ∼ 5 dB higher than those with the 3-dB FLM-FBG cavity. Furthermore, the lasing output performances based on the FBG-only cavity are compared when the reflectivities of the output-mirror FBGs are the same or different. It is observed that the dual-wavelength laser with the same output reflectivity leads to higher OSNR, slope efficiency, and stability. Moreover, by varying the center wavelength interval of pairs of FBGs in the FBG-only cavity to values of 4 nm, 8 nm, and 12 nm respectively. It is shown that wider intervals result in higher OSNRs but lower laser slope efficiency. Finally, we demonstrate a dual- wavelength linear cavity EDFL operating at room temperature with two lasing wavelengths of 1550 nm and 1562 nm. The laser results in OSNRs around 50.62 dB and 50.93 dB; center wavelength variations of less than 0.030 nm and 0.035 nm; output power fluctuations of less than 0.061 mW and 0.059 mW, respectively.

Effects of Different Levels of Physical Damage Combined with Fungal Induction on Agarwood Formation

As wild Aquilaria sinensis resources are exhausted and protected, China has established a huge number of plantations of Aquilaria trees and developed artificial induction techniques. However, the current output and quality of artificial induction technology have not yet met the expected results. It has been found that high-oil-containing agarwood may contain particular fungal stains associated with agarwood production. To enhance the quality of agarwood, we recovered and characterized three highly active fungi from high-oil-containing agarwood and inoculated them onto A. sinensis trees using two traditional physical methods. The results showed that fungi extracted from high-oil-containing agarwood can effectively increase the yield and quality of agarwood. During the agarwood formation process, parenchyma cells, xylem rays, and axial parenchyma cells in the xylem gradually undergo apoptosis, thereby promoting the expansion of the color range of agarwood. Nine months after the treatment, the alcohol-soluble extract content in agarwood reached the standard specified in the Chinese Pharmacopoeia (10%), and the proportions of sesquiterpenes and chromones in each treatment were 55.82%, 58.31%, 62.65%, 70.97%, and 13.71%, respectively. These results indicate that fungal induction has a positive impact on the quality of agarwood. In addition, compared to drilling and fungus combined induction, “burning holes and fungi” combined induction demonstrates better results and can further improve the yield and quality of agarwood.

Contributions to the optical linewidth of shallow donor-bound excitonic transition in ZnO

Neutral shallow donors in zinc oxide (ZnO) are spin qubits with optical access via the donor-bound exciton. This spin–photon interface enables applications in quantum networking, memories, and transduction. Essential optical parameters which impact the spin–photon interface include radiative lifetime, optical inhomogeneous and homogeneous linewidth, and optical depth. We study the donor-bound exciton optical linewidth properties of Al, Ga, and In donors in single-crystal ZnO. The ensemble photoluminescence linewidth ranges from 4 to 11 GHz, less than two orders of magnitude larger than the expected lifetime-limited linewidth. The ensemble linewidth remains narrow in absorption through samples with an estimated optical depth up to several hundred. The primary thermal relaxation mechanism is identified and found to have a negligible contribution to the total linewidth at 2 K. We find that inhomogeneous broadening due to the disordered isotopic environment in natural ZnO is significant, contributing 2 GHz. Two-laser spectral hole burning measurements indicate that the dominant mechanism, however, is homogeneous. Despite this broadening, the high homogeneity, large optical depth, and potential for isotope purification indicate that the optical properties of the ZnO donor-bound exciton are promising for a wide range of quantum technologies, and motivate a need to improve the isotope and chemical purity of ZnO for quantum technologies.

Controlled multiple spectral hole burning via a tripod-type atomic medium

In limit of saturation spectroscopy, we theoretically study the spectral hole burning (SHB) in the absorption spectrum of a probe field through a tripod atomic system. The response function for the probe field is calculated in a Doppler-broadened medium. Burning of spectral holes is observed only for the counter propagation of either one or both the coupling fields in the medium. The SHB is not observed below some critical temperature which is a condition for the electromagnetically induced transparency (EIT) in the medium. The most interesting and significant feature is that the Doppler broadening acts as a decoherence effect in case of EIT, however, the Doppler broadening acts inversely in case of SHB and consequently the burning effect enhances. The SHB is further enhanced and controlled by classes of the average velocity of atoms. The classes of high average atomic velocity in the medium increase the number of spectral hole burns (HBs). The widths of HBs can be controlled by the intensity of the driving fields. A single HB can be switched to multiple HBs in a well-controlled manner using different classes of high average atomic velocity. The various switchable holes can be burned in a desired position of the absorption spectrum which in turn simultaneously slow down multiple probe fields. The phenomenon of SHB may be useful in the construction of multichannel optical switching and storage devices.

The tautomer-specific excited state dynamics of 2,6-diaminopurine using resonance-enhanced multiphoton ionization and quantum chemical calculations.

2,6-Diaminopurine (2,6-dAP) is an alternative nucleobase that potentially played a role in prebiotic chemistry. We studied its excited state dynamics in the gas phase by REMPI, IR-UV hole burning, and ps pump-probe spectroscopy and performed quantum chemical calculations at the SCS-ADC(2) level of theory to interpret the experimental results. We found the 9H tautomer to have a small barrier to ultrafast relaxation via puckering of its 6-membered ring. The 7H tautomer has a larger barrier to reach a conical intersection and also has a sizable triplet yield. These results are discussed relative to other purines, for which 9H tautomerization appears to be more photostable than 7H and homosubstituted purines appear to be less photostable than heterosubstituted or singly substituted purines.

Anti-phase pulsation of counter-propagating dissipative solitons in a bidirectional fiber laser

Due to its unique geometric structure, the bidirectional ultrafast fiber laser is an excellent light source for dual-comb applications. However, sharing the same gain between the counter-propagating solitons also gives rise to complex dynamics. Herein, we report the anti-phase pulsation of counter-propagating dissipative solitons in a bidirectional fiber laser. The in-phase and anti-phase soliton pulsation can be manipulated by adjusting the intracavity birefringence. The periodic modulation of polarization-dependent gain (PDG) caused by polarization hole burning (PHB) in the gain fiber can be responsible for anti-phase pulsation of bidirectional dissipative solitons. These findings offer new, to the best of our knowledge, insights into the complex dynamics of solitons in dissipative optical systems and performance improvement of bidirectional ultrafast fiber lasers.

Anti-correlation phenomena in quantum cascade laser frequency combs

In quantum cascade laser frequency combs, the intensity distribution of the optical spectrum can be split into two well-separated lobes of longitudinal modes that, even when far apart, have a common phase relation and preserve equal frequency separation. The temporal dynamics of two lasers emitting at 4.4 and 8.1 µm operating in this bilobed regime are here investigated. The laser intensity shows a peculiar temporal behavior associated with the spectral features whereby, every half a round-trip, the total emitted power switches from one lobe to the other, with a perfect temporal anti-correlation. The anti-correlation between the lobes is also observed in the intensity noise figure of the emission. This coherent phenomenon arises from gain nonlinearities induced by spatial hole burning and the extremely fast gain dynamics typical of quantum cascade lasers.

Spatial Microwave Field Frequency Measurement through Two‐Level Resonance of Nitrogen‐Vacancy Color Center in Diamond

This article presents a frequency measurement method for spatial microwave signals with solid‐state atom resonance, performing measurements based on the burnt hole in spectrum with two microwave fields acting on nitrogen vacancies (NVs) simultaneously. The population on |0⟩ of the NV color center in the ground state affected by the resonance of two microwave fields with similar frequencies responds excellently to external microwave frequencies, and a phenomenon named hole burning occurs. The full width at half maximum (FWHM) of the resonant peak at the hole is 18.9 kHz. When microwaves of different frequencies are applied, the resonant peak precisely follows the signal frequency in the experiment. Subsequently, the resonant peak is processed using the differential method to obtain a frequency measurement error on the order of 100 Hz. The spatial resolution of this method is within the millimeter scale. This study can provide technical support for applications in microwave frequency measurement and spatial mapping with quantum precision measurement.

Exploring the spatial hole burning effect on the mode-locking characteristics of self-mode-locked Nd:YVO4 lasers

The spatial hole burning (SHB) effect on the mode-locking characteristics of Nd:YVO4 self-mode-locked (SML) lasers are investigated. By varying the cavity length, pump power, and crystal temperature, we manipulate the SHB effect on the longitudinal mode distributions and the temporal waveforms of the SML lasers. The experimental results indicate that, at a pump power of 3395 mW and a cavity length of 23 mm, the SHB effect is minimal, the temporal waveform remains stable and the longitudinal mode spacing equals the fundamental longitudinal mode interval (FLMI). As increasing the cavity length to 75 mm, the experimental longitudinal mode spacing becomes 1 to 5 times the FLMI and the temporal waveforms are then multi-pulse mode-locked state, indicating an aggravation in the SHB effect of the SML laser. With the cavity length of 23 mm, as the pump power increases from 3.4 W to 9.7 W, the SHB effect on the mode-locking characteristics gradually also aggravates. The laser gradually changes from the fundamental mode-locked state to the spaced mode-locked state. By adjusting the crystal temperature from 25 °C to 35 °C, the aggravated SHB effect caused by the increase in pump power is counteracted.