No. 18
纳米尺度量子传感器的固态激光制冷Solid-state laser refrigeration of nanoscale quantum sensors
将纳米金刚石与金纳米晶体经范德华作用贴附于陶瓷激光制冷衬底,结合德拜–瓦勒因子测温与氮空位色心光探测磁共振,证明衬底制冷可使金刚石温度比稳态低25±3 K,并使表面增强拉曼传感中金纳米晶的光热升温减少8.8±2.7 K。
在纳米尺度量子传感器的光激发过程中,光热加热始终是一项主要挑战[C. Bradac, S. F. Lim, H. C. Chang, I. Aharonovich, Adv. Opt. Mater. 8, 2000183 (2020)]。在低激光功率下,传感器受热会引起量子电子跃迁能量的热漂移;在高激光功率下,传感器因热致相变(包括熔化)而退化。在此,我们提出一种通用方法,通过固态激光制冷传感器的底层衬底来缓解纳米尺度量子传感器的光热加热。实验中,纳米金刚石和金纳米晶体分别通过范德华相互作用贴附在陶瓷激光制冷衬底上。结合德拜–瓦勒因子测温与氮空位中心的光探测磁共振谱,我们证明衬底的固态激光制冷可使贴附的纳米金刚石负载温度比稳态工作温度低25 ± 3 K。在罗丹明6G分子的表面增强拉曼光谱传感中,利用斯托克斯/反斯托克斯拉曼光谱证明,等离激元金纳米晶体的光热加热降低了8.8 ± 2.7 K。这些结果表明,固态激光冷却或可为多种纳米尺度量子资源提供快速反馈控制冷却的实验可能。
Abstract (English)
Photothermal heating remains a major challenge during the optical excitation of nanoscale quantum sensors [C. Bradac, S. F. Lim, H. C. Chang, I. Aharonovich, Adv. Opt. Mater. 8 , 2000183 (2020)]. At low laser powers, heating of the sensor leads to the thermal drift of quantum electronic transition energies. At high laser powers, sensors degrade due to thermally induced phase transitions, including melting. Here, we report a general approach for mitigating the photothermal heating of nanoscale quantum sensors through solid-state laser refrigeration of the sensors’ underlying substrate. Experimentally, both nanodiamonds and gold nanocrystals are attached separately to a ceramic laser-cooling substrate through van der Waals interaction. A combination of Debye–Waller factor thermometry and optically detected magnetic resonance spectroscopy of nitrogen vacancy centers is used to demonstrate that solid-state laser refrigeration of the substrate can reduce the temperature of attached nanodiamond payloads by 25 ± 3 K below steady-state operating temperatures. Stokes/anti-Stokes Raman spectroscopy is used to demonstrate reduced photothermal heating of plasmonic gold nanocrystals by 8.8 ± 2.7 K during surface-enhanced Raman spectroscopy sensing of rhodamine-6G molecules. These results suggest that solid-state laser cooling could open up experimental possibilities for rapid feedback-controlled cooling of a wide range of nanoscale quantum resources.
Zhaojie Feng, Anupum Pant, Robert G. Felsted, Alexander B. Bard, Xiaojing Xia, Siamak Dadras, Kamran Shayan, Danika R. Luntz-Martin, Donald Mannikko, Lars Forberger, Alexey Soldatenko, Ilia M. Pavlovetc, Stefan Stoll, Masaru Kuno, A. Nickolas Vamivakas, Peter J. Pauzauskie
PNAS 123 (2026)
10.1073/pnas.2534326123