Thermal Resolution Research Articles

Engineering Visible to Near-Infrared Luminescence through a Selective Doping Strategy for High-Performance Temperature Sensing.

Luminescence nanothermometers have garnered considerable attention due to their noncontact measurement, high spatial resolution, and rapid response. However, many nanothermometers employing single-mode measurement encounter challenges regarding their relative sensitivity. Herein, a unique class of tunable upconversion (UC) and downshifting (DS) luminescence covering the visible to near-infrared range (400-1700 nm) is reported, characterized by the superior Tm3+, Ho3+, and Er3+ emissions induced by efficient energy transfer. The outstanding negative thermal expansion characteristic of ScF3 nanocrystals has been found to guide excitation energy toward the relevant emitting states in the Yb3+-Ho3+-Tm3+-codoped system, consequently resulting in remarkable near-infrared III (NIR-III) luminescence at ∼1625 nm (Tm3+:3F4 → 3H6 transition), which in turn presents numerous opportunities for designing multimode ratiometric luminescence thermometry. Furthermore, by facilitating phonon-assisted energy transfer in Er3+-Ho3+-codoped systems, the luminescence intensity ratio (LIR) of 4I13/2 of Er3+ and 5I6 of Ho3+ in ScF3:Yb3+/Ho3+/Er3+ exhibits a strong temperature dependence, enabling NIR-II/III luminescence thermometry with superior thermal sensitivity and resolution (Sr = 0.78% K-1, δT = 0.64 K). These findings not only underscore the distinctive and ubiquitous attributes of lanthanide ion-doped nanomaterials but also hold significant implications for crafting luminescence thermometers with unparalleled sensitivity.

Temperature-Dependent Luminescence of Nd3+-Doped Carbon Nanodots for Nanothermometry.

Noncontact optical nanothermometers operating within the biological transparency windows are required to study temperature-sensitive biological phenomena at the nanoscale. Nanoparticles containing rare-earth ions such as Nd3+ have been reported to be efficient luminescence-based ratiometric thermometers, however often limited by poor water solubility and concentration-related quenching effects. Herein, we introduce a new type of nanothermometer, obtained by employing low-dimensional carbon nanodots (CNDs) as matrices to host Nd3+ ions (NdCNDs). By means of a one-pot procedure, small (∼7-12 nm), water-soluble nanoparticles were obtained, with high (15 wt %) Nd3+ loading. This stable metal-CND system features temperature-dependent photoluminescence in the second biological window (BW II) upon irradiation at 808 nm, thereby allowing accurate and reversible (heating/cooling) temperature measurements with good sensitivity and thermal resolution. The system possesses remarkable biocompatibility in vitro and promising performance at a high penetration depth in tissue models.

A Methodology for Robust Multislice Ptychography.

While multislice electron ptychography can provide thermal vibration limited resolution and structural information in 3D, it relies on properly selecting many intertwined acquisition and computational parameters. Here, we outline a methodology for selecting acquisition parameters to enable robust ptychographic reconstructions. We develop two physically informed metrics, areal oversampling and Ronchigram magnification, to describe the selection of these parameters in multislice ptychography. Through simulations, we comprehensively evaluate the validity of these two metrics over a broad range of conditions and show that they accurately guide reconstruction success. Further, we validate these conclusions with experimental ptychographic data and demonstrate close agreement between trends in simulated and experimental data. Using these metrics, we achieve experimental multislice reconstructions at a scan step of 2.1Å/px, enabling large field-of-view, data-efficient reconstructions. These experimental design principles enable the routine and robust use of multislice ptychography for 3D characterization of materials at the atomic scale.

Metoda pomiaru minimalnej rozróżnialnej różnicy temperatury w funkcji powiększenia i rozogniskowania kamery termowizyjnej

Temperature measurement of allergic skin reactions requires meeting certain criteria regarding temperature resolution between small areas. The usual criterion of temperature resolution is NETD. However, this metric does not take into account the limitations of the spatial resolution of the optical system or the detector. In this paper, a model is presented that allows for selection of camera parameters based on the required spatial thermal resolution and size of the object being imaged. The method has been implemented and compared to results obtained in commercial software and has been applied to evaluate spatial thermal resolution of a prototype objective designed for the LWIR band.

Doping-mediated thermal control of phase transition for supersensitive ratiometric luminescence thermometry

Intelligent luminescent materials, characterized by optical switching in response to thermal stimulation, are highly attractive for cutting-edge temperature sensing technologies. However, the exploration of sensitive and reliable thermometric materials remains challenging. Herein, we establish a phase-transition-driven thermometric model that relies on the reversible transition between the monoclinic (β) and tetragonal (α) phase of LiYO2:Dy3+ crystals under controlled thermal stimulations. Accordingly, the ratiometric emissions from hypersensitive electric diploe transitions (4F9/2 → 6H13/2) drastically varied across the phase-transition temperature range, rendering remarkable thermal sensitivity and resolution (Sr-max = 35.24% K−1, δTmin = 0.009 K). We further demonstrate the extended control of phase-transition temperature and thermal hysteresis by a partial substitution approach. These findings highlight an endogenic approach to constructing customized luminescence thermometers via local crystal-field engineering, which raises new possibilities for practical sensing applications.

Dual-modal optical temperature sensing based on Sb3+/Mn2+ co-doped Cs2NaYCl6 double perovskites

Optical temperature sensing based on luminescence intensity ratio shows significant potential in achieving accurate temperature detection. In this work, Sb3+/Mn2+ co-doped Cs2NaYCl6 double perovskites were synthesised via a hydrothermal method. Introducing Sb3+ ions to the host significantly enhances the radiative recombination of self-trapped excitons (STEs), resulting in a broad blue emission. The co-doping of Mn2+ ions to the composition leads to a tunable dual-emission in the spectra, originating from the energy transfer between the STEs and Mn2+ ions. The dependence of the dual-emission on temperature is employed for optical temperature sensing. The maximum relative sensitivity, optimal thermal resolution, and optimal thermal repeatability are determined as 1.40 % K−1, 0.002 K and 99.3% at 250 K, respectively. The results indicate that the synthesised Cs2NaYCl6: Sb3+/Mn2+ double perovskites are promising candidates for high-sensitivity optical thermometers.

A complex case of thermal maturity assessment in a terrigenous sedimentary system: The Northwestern Black Sea basin

An integrated approach combining fluorescence spectrometry, pyrolysis geochemistry, and dispersed organic matter (DOM) maceral analysis has been used to determine the thermal maturity of Oligocene source rocks in two neighboring offshore wells within the complex deep-sea system of the Northwestern Black Sea. The samples contain predominantly immature Type II kerogen, including a mixture of marine liptinite (alginite, liptodetrinite), degraded liptinite, primary vitrinite, and reworked vitrinitic macerals. The occurrence of several vitrinite reflectance (VRo) populations in the samples is attributed to a high influx of reworked vitrinite transported to the marine basin from multiple terrestrial sources with diverse degrees of degradation. The presence of multiple VRo populations complicates the application of VRo for determining the thermal maturity of the organic matter. Further, the VRo measurements on the primary vitrinite population show only a subtle increasing trend with depth. A significantly improved thermal maturity resolution was obtained using the red to green quotient (R/G). R/G was measured on the autochthonous unicellular Tasmanites-type alginite under UV-excitation. In contrast to VRo the results show a significant correlation between increasing R/G values with increasing depth. This indicates that the R/G quotient is a better maturity proxy for the studied low maturity marine system with a large influx of sediments. The beginning of the downward declining trend in the temporal variation of liptinite is regarded as the onset of catagenesis. This occurs at a burial depth of 2.5 km and a R/G value of 0.50, corresponding to a VRo equivalent (VRo Eq) of 0.44%. At a burial depth of 3.2 km and a R/G value of 0.57 (VRo Eq = 0.57%), the onset of the oil window is marked by an increase in the amount of solid bitumen (initial oil solid bitumen). The observed alterations in maceral composition with burial depth align with the thermal maturity of the wells. However, the data suggest that the thermal evolution of the organic matter is out of sync with the surrounding formation temperature, possibly due to rapid burial induced by a high sedimentation rate.

Ultrasound-switchable fluorescence thermometry with dual detection channels using temperature-sensitive liposomes.

Temperature measurements in biological tissues play a crucial role in studying metabolic activities. In this study, we introduce a noninvasive thermometry technique based on two-color ultrasound-switchable fluorescence (USF). This innovative method allows for a local temperature mapping within a microtube filled with temperature-sensitive liposomes as nano imaging agents. By measuring the temperature-dependent fluorescence emission of the liposomes using a spectrometer, we identify four characteristic temperatures. The local background temperature can be estimated by analyzing the corresponding appearance time of these four characteristic temperatures in the dynamic USF signals captured by a camera-based USF system with two detection channels. Simultaneous measurements with an infrared (IR) camera showed a 0.38°C ± 0.27°C difference between USF thermometry and IR thermography in a physiological temperature range of 36.48°C-40.14°C. This shows that the two-color USF thermometry technique is a reliable, noninvasive tool with excellent spatial and thermal resolution.

Water-dispersed bismuth-doped strontium pyrovanadate phosphor particles with sub-degree celsius thermal resolution

The lifetime and emission of water-dispersed Sr2V2O7:Bi3+ exhibit strong thermal quenching around ambient temperatures. The high-temperature sensitivity and microsecond lifetime of this material make it suitable for temperature imaging applications.

System multi-scale analysis of temperature control for spaceborne electronic devices

<sec>To improve the simulation resolution and accuracy in thermal analysis of spaceborne electronic devices and the temperature control performance of passive thermal control devices, a system multi-scale model is established, thereby obtaining the temperature field and heat flux of electronic devices inside the satellite on different scales as illustrated in the below figure. The temperature fluctuation mechanism inside the satellite is analyzed on different physical scales. The thermal analysis resolution of spaceborne electronic equipment is improved, and a method to reduce the power fluctuation of spaceborne equipment is proposed based on the results of system multi-scale thermal analysis.</sec><sec>The results indicate that the accuracy deviation between the multi-scale model of the system and the actual model is less than 9%. However, the system multi-scale model saves 99.67% of the mesh generation time, which greatly improves the computation efficiency. The system multi-scale model can capture the thermal information about device-level chip microstructures at a lower computational cost. The system-level model can evaluate the temperature control and insulation performance of passive thermal control materials on a macroscale. The temperature fluctuation amplitude of the platform compartment is 7.95 K, while the temperature fluctuation amplitude of the load compartment decreases to 2.43 K after the temperature of the composite phase change insulation material has been controlled, which is 69.43% lower than that of the platform compartment. Compared with traditional vacuum insulation panels, the composite phase change materials are very superior in controlling the temperature of the chamber and suppressing temperature fluctuations. The temperature fluctuation signal after being insulated by the composite phase change insulation materials shows a characteristic of shifting to the high-frequency domain. After selecting the cabins that require key insulation and temperature control through multiple regression analysis, a simplified model at device level is employed to obtain temperature fields under different thermal control device layouts as a training dataset. A neural network genetic algorithm is used to predict the optimal installation position of passive thermal control device on the device scale and a thermal control layout scheme is obtained, which reduces the maximum temperature fluctuation of the device by 2.74 K. If the temperature uniformity coefficient is taken as the optimization goal, the temperature of each device on PCB board can be reduced to 14.39% of the average temperature of all devices through optimizations.</sec>

Joint Use of a Low Thermal Resolution Thermal Camera and an RGB Camera for Respiration Measurement

Joint Use of a Low Thermal Resolution Thermal Camera and an RGB Camera for Respiration Measurement

Advanced temperature sensing with Er3+/Yb3+ co-doped Ba2GdV3O11 phosphors through upconversion luminescence.

Optical thermometry is a non-contact temperature sensing technique with widespread applications. It offers precise measurements without physical contact, making it ideal for situations where contact-based methods are impractical. However, improving the accuracy of optical thermometry remains an ongoing challenge. Herein, enhancing the thermometric properties of luminescent thermometers through novel materials or strategies is crucial for developing more precise sensors. Hence, the present study focuses on the application of four-mode luminescence thermometric techniques in sol-gel synthesized Er3+/Yb3+ co-doped Ba2GdV3O11 phosphors for optical temperature sensing in the temperature range of 298-573 K. The upconversion (UC) luminescence is achieved under excitations of 980 nm or 1550 nm, resulting in bright yellow-green emission in the visible spectral range. Temperature sensing is realized by exploiting the UC emissions of 4S3/2, 2H11/2 and 4F7/2 bands, which represent intensity ratios of thermally coupled levels (TCELs) and non-thermally coupled levels (NTCELs) of Er3+/Yb3+, along with the emission lifetimes at 4S3/2. The relative sensitivity (Sr) values for TCELs exhibit a gradual decrease with rising temperature, reaching a maximum of 1.1% K-1 for 980 nm excitation and 0.86% K-1 for 1550 nm excitation at 298 K. Conversely, for NTCELs, the highest Sr value observed is 0.9% K-1 at 298 K for 1550 nm excitation. Moreover, the emission lifetimes at 4S3/2 yield notably high Sr values of up to 5.0% μs K-1 (at 425 K). Furthermore, the studied phosphors have a sub-degree thermal resolution, making them excellent materials for accurate temperature sensing. Overall, this study provides a promising new direction for the development of more precise and reliable optical thermometry techniques, which could have important implications for a range of scientific and industrial optical temperature sensing applications.

A novel ultrahigh-sensitive optical thermometer based on inverse thermal responses of Nd3+ and Yb3+ emissions in BaGd2(MoO4)4 phosphor

Nowadays, lots of efforts have been vested on the exploitation of novel luminescent thermometric materials to achieve remote temperature readout with ultra-high sensitivity and sub-degree resolution. Herein, the BaGd2(MoO4)4: Yb3+, Nd3+ phosphors were successfully prepared via a solid-state reaction method, and their concentration/temperature-dependent luminescence behaviors were investigated systematically. Upon 980 nm excitation, the photoluminescence (PL) spectra consisted of three emission bands centered at 754 nm, 805 nm and 872 nm from Nd3+, together with an emission band peaked at 1008 nm from Yb3+. As the temperature elevated, the Yb3+: 2F5/2 → 2F7/2 emission weakened sharply, whereas the promoted phonon-assisted energy transfer process from Yb3+ to Nd3+ and excited-state absorption process of Nd3+ led to an intense thermal enhancement of the Nd3+: 4Fj → 4I9/2 (j = 7/2, 5/2, 3/2) transitions. Moreover, the thermally enhancing factor was found to depend on the Nd3+ concentration. By utilizing the luminescence intensity ratio (LIR) technique, the temperature sensing behaviors based on thermally coupled levels (Nd3+: 4Fj, j = 7/2, 5/2, 3/2) and non-thermally coupled levels (Nd3+: 4Fj and Yb3+: 2F5/2) were studied at the different doping concentrations. When the temperature sensing was based on LIR between Nd3+: 4F3/2 → 2I9/2 and Yb3+: 2F5/2 → 2F7/2 transitions, the BaGd2(MoO4)4: 3 mol%Nd3+, 15 mol%Yb3+ sample displayed excellent thermal sensitivity (2.28–8.42 %K−1) and temperature resolution (0.1–0.22 K) at temperatures ranging from 298 K to 573 K, which were superior to those of many other reported luminescence materials. The present work might give a new input for developing near-infrared (NIR) luminescence materials with desirable temperature sensing performances.

Boltzmann thermometer with broadband emission in Mn4+-Doped β-Ga2O3 crystals

The luminescence properties of Mn4+-doped β-Ga2O3 are strongly affected by the surrounding crystal field within the [MnO6] octahedral site, which is substitute for GaⅡ site, as determined through the first-principles calculations. The crystal field strength parameters Dq, B, and C are computed, and the Tanabe-Sugano diagram is redrawn for C/B = 6.7. The temperature dependence of the optical spectra is thoroughly examined, revealing the thermal quenching mechanisms involving the thermal activation energy of 2Eg and 4T2g, which are 378 ± 26 cm−1 and 3527 ± 25 cm−1, respectively. In order to further investigate the temperature sensing characteristics, the absolute (Sa) and relative (Sr) sensitivities are obtained. At 303 K, the Sr is determined to be 0.72 %K−1, while Sa is estimated to be in the range of 10−2 (below 0.05 K-1) for the Mn4+ doped β-Ga2O3 thermometers. The thermal resolution δT is demonstrated to be below 0.1 K, surpassing that of traditional Nd3+ and Er3+-doped thermometers. Moreover, a linear relationship between the energy separation ΔE of the thermally coupled 2Eg-4T2g energy levels and the crystal field strength Dq is observed in numerous materials. With this consideration, the nature of the thermometer, along with its Sa and Sr, can be roughly predicted and designed for various operational conditions.

Thermoelectric Nanofluidics Probing Thermal Heterogeneity inside Single Cells.

Accurate temperature measurement in one living cell is of great significance for understanding biological functions and regulation. Here, a nanopipet electric thermometer (NET) is established for real-time intracellular temperature measurement. Based on the temperature-controlled ion migration, the temperature change in solution results in altered ion mobilities and ion distributions, which can be converted to the thermoelectric responses of NET in a galvanostatic configuration. The exponential relationship between the voltage and the temperature promises highly sensitive thermoelectric responses up to 11.1 mV K-1, which is over an order of magnitude higher than previous thermoelectric thermometry. Moreover, the NET exhibits superior thermal resolution of 25 mK and spatiotemporal resolution of 100 nm and 0.9 ms as well as excellent stability and reproducibility. Benefiting from these unique features, both thermal fluctuations in steady-state cells and heat generation and dissipation upon drug administration can be successfully monitored, which are hardly achieved by current methods. By using NET, thermal heterogeneities of single cancer cells during immunotherapy were reported first in this work, in which the increased intracellular temperature was demonstrated to be associated with the survival benefit and resistance of cancer cells in immunotherapy. This work not only provides a reliable method for microscopic temperature monitoring but also gains new insights to elucidate the mechanism of immune evasion and therapeutic resistance.

Thermally boosted upconversion luminescence and high-performance thermometry in ScF3:Yb3+/Tm3+ nanorods with negative thermal expansion

Luminescence nanothermometers featuring high spatial resolution and thermal resolution have aroused extensive interest in biological and nanomedical fields. However, the challenge of thermal quenching in upconversion (UC) nanocrystals hampers achieving elevated relative temperature sensitivity (Sr). In this study, the quasi cubic nanorods of ScF3:Yb3+/Tm3+ with negative thermal expansion were prepared, and thermally boosted luminescence was found to derive from the phonon-assisted energy transfer, resulting in the emission band of 3F2,3 → 3H6 of Tm3+ ions enhanced monotonously. While the emission bands of (1G4)1D2→3F4 of Tm3+ ions first increased slightly and then decreased seriously because of the competition between phonon-assisted and cross-relaxation (CR) processes. Relying on this high-contrast thermal dependent feature, the maximum relative sensitivity of 1.60% K−1 at 523 K was achieved in the proposed luminescence intensity ratio (LIR) thermometry. These findings would open a new avenue for designing thermally boosted upconversion nanocrystals and reliable optical thermometers by using Tm3+ activated luminescent materials.

Structural Confinement Induced Near‐Unity Quantum Yield for Single‐Band Ratiometric Thermometry

AbstractLuminescence quenching at high dopant concentration and temperature typically limits the brightness of luminescence materials, which remains a major obstacle in diverse technological applications, especially in the field of luminescence thermometry. In this work, a unique class of non‐concentration quenching double‐tungstate phosphors is reported that feature the near‐unity quantum yield of Tb3+ and Eu3+ emissions induced by the structural confinement effect. Mechanistic studies affirm that the activator ions can be isolated in NaYW2O8 crystal to confine the absorbed photon energy, leading to a relatively high quenching concentration of various lanthanide activators. By facilitating interionic cross‐relaxation at heavy dopant concentration, a remarkable thermal enhancement of Tb3+ emissions over 20‐fold upon the excitation of excited‐state absorption is recorded. In contrast, thermally quenched emissions are detected under the excitation of ground‐state absorption. This excitation wavelength‐dependent thermal behavior of Tb3+ emissions is harnessed for single‐band ratiometric thermometry, registering superior thermal sensitivity and resolution (Sr = 4.01% K−1, δT = 0.1 K). The advances in combating concentration and thermal quenching of luminescence materials provide exciting opportunities for flexible thermometry in real‐world sensing scenarios.

Self-calibrated multi-mode optical thermometry in up-converting phosphor Cs2NaErCl6: Yb3+

With the development of temperature measurement technology, people put forward higher requirements for the accuracy and precision of temperature measurement. However, most of the current luminescent thermometers use a single optical signal for temperature detection, which has a certain range of temperature insensitivity, resulting in inaccurate temperature measurement. Here, an all-inorganic rare-earth halide double perovskite Cs2NaErCl6: Yb3+ (CNEC: Yb3+) phosphor was synthesized, which not only expressed triple-mode thermometric properties based on thermally coupled levels (TCLs), non-thermally coupled levels (N-TCLs) and lifetime (FL), but also capable of providing self-referencing and high-sensitivity temperature measurements under excitation at 980 nm. Benefiting from the low phonon energy of the matrix, high doping concentration and the excellent internal up-conversion quantum efficiency (UCQY) about 6.52% of optimal composition CNEC: 40%Yb3+, all modes exhibit superior sensitivities, reversibility and thermal resolution under 980 nm irradiation. In addition, a flexible thin film thermometer composed of CNEC: 40%Yb3+ was prepared to realized multi-mode thermal monitoring of local hot spots of electronic components. The excellent three-mode temperature measurement results indicated that CNEC: Yb3+ phosphors have great potential in temperature sensing.

The incorporation of xenon at point defects and bubbles in uranium mononitride

Uranium mononitride (UN) has been proposed as an accident tolerant fuel for nuclear fission reactors and offers enhanced performance during accident scenarios relative to the current fuel, uranium dioxide. However, its performance in reactor is significantly less well understood than for the oxide. Therefore, this work explores incorporation of Xe into UN using density functional theory to understand the early stages of fission gas evolution. These results are used to derive a new potential for Xe in UN, which is then employed to simulate the growth of xenon bubbles in spherical voids of various sizes at 300 K and 1200 K. At sufficiently high gas densities, the xenon was found to mainly crystallise in an fcc arrangement. Loop punching was observed at 10.2 GPa and above for larger bubbles of 4.8 nm radius, significantly so for higher temperatures. This work suggests that no Xe undergoes thermal resolution at temperatures up to 1200 K and that the UN lattice prefers to undergo deformation instead.

Structural, luminescence and thermometric properties of LaVO4:Ln3+ nanopowders (Ln = Dy and Sm)

Lanthanide-doped materials have been intensively studied for optical thermometry due to their unique luminescence properties. However, the engineering of high-resolution multimode nanopowders for high-sensitivity thermometry is still a big challenge. Here, we study the structural and luminescence properties of Dy3+- and Sm3+-doped LaVO4 concentration series to find the suitable candidates for possible application as a temperature sensor. The synthesized nanocrystalline phosphors have successfully demonstrated multimode thermal sensing in the wide temperature range based on the temperature-induced red shift of the charge transfer band. The proposed sensing strategies were compared in terms of thermal sensitivity and temperature resolution. The best thermometric performances of Sr = 2.07 % K−1 and ΔT = 0.2 K at room temperature were found for LaVO4:Sm3+ 2 at% sample. The studies testify that Ln3+-doped LaVO4 materials are promising in multimode high-sensitivity optical thermometry.