Partial laser treatment is introduced to carbon‐based microfibers to generate excellent photon sensing capability without bias. This treatment brings about a Seebeck coefficient distribution along the sample's length, out of which a photovoltage with no external bias is generated and sensed. Using a line‐shaped laser spot, carbon microfiber (CMF), graphene microfiber (GMF), and graphene aerogel fiber (GAF) are investigated for their response to µm‐scale photon irradiation. A higher sensitivity for the incident photon is found for the GAF with no position sensitivity. More Seebeck coefficient variation is also observed for the GAF considering the amount of laser power used for the laser treatment. A weaker Seebeck coefficient spatial variation is observed for the GMF compared with the GAF. However, its photovoltage shows an abrupt magnitude change from the laser‐treated region to the non‐treated one. Despite the low spatial variation of the Seebeck coefficient for the CMF, it features an excellent and accurate position‐sensitive photoresponse with polarization change over a distance of ≈100 µm. Such unique capability prompts novel applications in using partially annealed CMF for sensing the position of optical beams at the microscale.
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Abstract Free, publicly-accessible full text available September 17, 2024 -
Abstract This work reports the dynamic behaviors of graphene aerogel (GA) microfibers during and after continuous wave (CW) laser photoreduction. The reduction results in one‐order of magnitude increase in the electrical conductivity. The experimental results reveal the exact mechanisms of photoreduction as it occurs: immediate photochemical removal of oxygen functional groups causing a sharp decrease in electrical resistance and subsequent laser heating that facilitates thermal rearrangement of GO sheets towards more graphene‐like domains. X‐ray and Raman spectroscopy analysis confirm that photoreduction removes virtually all oxygen and nitrogen containing functional groups. Interestingly, a dynamic period immediately following the end of laser exposure shows a slow, gradual increase in electrical resistance, suggesting that a proportion of the electrical conductivity enhancement from photoreduction is not permanent. A two‐part experiment monitoring the resistance changes in real‐time before and after photoreduction is conducted to investigate this critical period. The thermal diffusivity evolution of the microfiber is tracked and shows an improvement of 277 % after all photoreduction experiments. A strong linear coherency between thermal diffusivity and electrical conductivity is also uncovered. This is the first known work to explore both the dynamic electrical and thermal evolution of a GO‐based aerogel during and after photoreduction.
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Abstract This work explores the 2D interfacial energy transport between monolayer WSe2and SiO2while considering the thermal nonequilibrium between optical and acoustic phonons caused by photoexcitation. Recent modeling and experimental work have shown substantial temperature differences between optical and acoustic phonons (Δ
T OA) in various nanostructures upon laser irradiation. Generally, characterizations of interfacial thermal resistance (R ′′tc) at the nanoscale are difficult and depend on Raman‐probed temperature measurements, which only reveal optical phonon temperature information. Here it is shown that ΔT OAfor supported monolayer WSe2can be as high as 48% of the total temperature rise revealed by optothermal Raman methods—a significant proportion that can introduce sizeable error toR ′′tcmeasurements if not properly considered. A frequency energy transport state‐resolved Raman technique (FET‐Raman) along with a 3D finite volume modeling of 2D material laser heating is used to extract the true interfacial thermal resistanceR ′′tc(determined by acoustic phonon transport). Additionally, a novel ET‐Raman technique is developed to determine the energy coupling factorG between optical and acoustic phonons (on the order of 1015W m−3K−1). This work demonstrates the need for special consideration of thermal nonequilibriums during laser–matter interactions at the nanoscale. -
Abstract Raman spectroscopy has been widely used to measure thermophysical properties of 2D materials. The local intense photon heating induces strong thermal nonequilibrium between optical and acoustic phonons. Both first principle calculations and recent indirect Raman measurements prove this phenomenon. To date, no direct measurement of the thermal nonequilibrium between optical and acoustic phonons has been reported. Here, this physical phenomenon is directly characterized for the first time through a novel approach combining both electrothermal and optothermal techniques. While the optical phonon temperature is determined from Raman wavenumber, the acoustic phonon temperature is precisely determined using high‐precision thermal conductivity and laser power absorption that are measured with negligible nonequilibrium among energy carriers. For graphene paper, the energy coupling factor between in‐plane optical and overall acoustic phonons is found at (1.59–3.10) × 1015W m−3K−1, agreeing well with the quantum mechanical modeling result of 4.1 × 1015W m−3K−1. Under ≈1 µm diameter laser heating, the optical phonon temperature rise is over 80% higher than that of the acoustic phonons. This observation points out the importance of subtracting optical–acoustic phonon thermal nonequilibrium in Raman‐based thermal characterization.
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Abstract Laser-assisted manufacturing (LAM) is a technique that performs machining of materials using a laser heating process. During the process, temperatures can rise above over 2000 °C. As a result, it is crucial to explore the thermal behavior of materials under such high temperatures to understand the physics behind LAM and provide feedback for manufacturing optimization. Raman spectroscopy, which is widely used for structure characterization, can provide a novel way to measure temperature during LAM. In this review, we discuss the mechanism of Raman-based temperature probing, its calibration, and sources of uncertainty/error, and how to control them. We critically review the Raman-based temperature measurement considering the spatial resolution under near-field optical heating and surface structure-induced asymmetries. As another critical aspect of Raman-based temperature measurement, temporal resolution is also reviewed to cover various ways of realizing ultrafast thermal probing. We conclude with a detailed outlook on Raman-based temperature probing in LAM and issues that need special attention.
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Abstract Under photon excitation, 2D materials experience cascading energy transfer from electrons to optical phonons (OPs) and acoustic phonons (APs). Despite few modeling works, it remains a long‐history open problem to distinguish the OP and AP temperatures, not to mention characterizing their energy coupling factor (
G ). Here, the temperatures of longitudinal/transverse optical (LO/TO) phonons, flexural optical (ZO) phonons, and APs are distinguished by constructing steady and nanosecond (ns) interphonon branch energy transport states and simultaneously probing them using nanosecond energy transport state‐resolved Raman spectroscopy. ΔT OP −APis measured to take more than 30% of the Raman‐probed temperature rise. A breakthrough is made on measuring the intrinsic in‐plane thermal conductivity of suspended nm MoS2and MoSe2by completely excluding the interphonon cascading energy transfer effect, rewriting the Raman‐based thermal conductivity measurement of 2D materials.G OP↔APfor MoS2, MoSe2, and graphene paper (GP) are characterized. For MoS2and MoSe2,G OP↔APis in the order of 1015and 1014W m−3K−1andG ZO↔APis much smaller thanG LO/TO↔AP. Under ns laser excitation,G OP↔APis significantly increased, probably due to the reduced phonon scattering time by the significantly increased hot carrier population. For GP,G LO/TO↔APis 0.549 × 1016W m−3K−1, agreeing well with the value of 0.41 × 1016W m−3K−1by first‐principles modeling. -
Free, publicly-accessible full text available October 1, 2024
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Free, publicly-accessible full text available September 1, 2024
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The temperature coefficient of resistivity (θT) of carbon-based materials is a critical property that directly determines their electrical response upon thermal impulses. It could have metal- (positive) or semiconductor-like (negative) behavior, depending on the combined temperature dependence of electron density and electron scattering. Its distribution in space is very difficult to measure and is rarely studied. Here, for the first time, we report that carbon-based micro/nanoscale structures have a strong non-uniform spatial distribution of θT. This distribution is probed by measuring the transient electro-thermal response of the material under extremely localized step laser heating and scanning, which magnifies the local θT effect in the measured transient voltage evolution. For carbon microfibers (CMFs), after electrical current annealing, θT varies from negative to positive from the sample end to the center with a magnitude change of >130% over <1 mm. This θT sign change is confirmed by directly testing smaller segments from different regions of an annealed CMF. For micro-thick carbon nanotube bundles, θT is found to have a relative change of >125% within a length of ∼2 mm, uncovering strong metallic to semiconductive behavior change in space. Our θT scanning technique can be readily extended to nm-thick samples with μm scanning resolution to explore the distribution of θT and provide a deep insight into the local electron conduction.
Free, publicly-accessible full text available August 28, 2024 -
Free, publicly-accessible full text available June 3, 2024