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Terahertz (THz) frequencies remain among the least utilized in the electromagnetic spectrum, largely due to the lack of powerful and compact sources. The invention of THz quantum cascade lasers (QCLs) was a major breakthrough to bridge the so-called ‘THz gap’ between semiconductor electronic and photonic sources. However, their demanding cooling requirement has confined the technology to a laboratory environment. A portable and high-power THz laser system will have a qualitative impact on applications in medical imaging, communications, quality control, security and biochemistry. Here, by adopting a design strategy that achieves a clean three-level system, we have developed THz QCLs (at ~4 THz) with a maximum operating temperature of 250 K. The high operating temperature enables portable THz systems to perform real-time imaging with a room-temperature THz camera, as well as fast spectral measurements with a room-temperature detector.GaAs-based terahertz quantum cascade lasers emitting around 4 THz are demonstrated up to 250 K without a magnetic field. To elevate the operation temperature, carrier leakage channels are reduced by carefully designing the quantum well structures.

Continuously graded parabolic quantum wells with excellent optical performances are used to overcome the low-frequency and thermal limitations of square quantum wells at terahertz frequencies. The formation of microcavity intersubband polaritons at frequencies as low as 1.8 THz is demonstrated, with a sustained ultra-strong coupling regime up to a temperature of 200K. It is additionally shown that the ultra-strong coupling regime is preserved when the active region is embedded in sub-wavelength resonators, with an estimated relative strength \\( = _R / _0 = 0.12\\). This represents an important milestone for future studies of quantum vacuum radiation because such resonators can be optically modulated at ultrafast rates, possibly leading to the generation of non-classical light via the dynamic Casimir effect. Finally, with an effective volume of \\(2.10^-6 _0^3\\), it is estimated that fewer than 3000 electrons per resonator are ultra-strongly coupled to the quantized electromagnetic mode, proving it is also a promising approach to explore few-electron polaritonic systems operating at relatively high temperatures.

We investigate the coupling of a multi-mode metal-insulator-metal cavity to a two-dimensional electron gas (2DEG) in a quantum well in the presence of a strong magnetic field. The TM cavity mode is strongly hybridized with an intersubband transition of the 2DEG, forming a polaritonic mode in the ultrastrong coupling regime, while the TE mode remains an almost purely cavity mode. The magnetoplasmon excitation emerging from the presence of the magnetic field couples with both TM and TE modes, exhibiting different coupling strengths and levels of spatial field inhomogeneity. While the strong homogeneity of the bare TE mode gives rise to the standard anticrossing of strong coupling, the inhomogeneous polaritonic TM mode is shown to activate an observable Coulombic effect in the spectral response, often referred to as non-locality. This experiment demonstrates a cavity-induced modification of the 2DEG response and offers a new route to probing the effect of Coulomb interactions in ultrastrongly coupled systems via reshaping of their cavity mode profiles.

We investigate the coupling of a multi-mode metal-insulator-metal cavity to a two-dimensional electron gas (2DEG) in a quantum well in the presence of a strong magnetic field. The TM cavity mode is strongly hybridized with an intersubband transition of the 2DEG, forming a polaritonic mode in the ultrastrong coupling regime, while the TE mode remains an almost purely cavity mode. The magnetoplasmon excitation emerging from the presence of the magnetic field couples with both TM and TE modes, exhibiting different coupling strengths and levels of spatial field inhomogeneity. While the strong homogeneity of the bare TE mode gives rise to the standard anticrossing of strong coupling, the inhomogeneous polaritonic TM mode is shown to activate an observable Coulombic effect in the spectral response, often referred to as non-locality. This experiment demonstrates a cavity-induced modification of the 2DEG response and offers a new route to probing the effect of Coulomb interactions in ultrastrongly coupled systems via reshaping of their cavity mode profiles.

Continuously graded parabolic quantum wells with excellent optical performances are used to overcome the low-frequency and thermal limitations of square quantum wells at terahertz frequencies. The formation of microcavity intersubband polaritons at frequencies as low as 1.8 THz is demonstrated, with a sustained ultra-strong coupling regime up to a temperature of 200K. It is additionally shown that the ultra-strong coupling regime is preserved when the active region is embedded in sub-wavelength resonators, with an estimated relative strength \\( = _R / _0 = 0.12\\). This represents an important milestone for future studies of quantum vacuum radiation because such resonators can be optically modulated at ultrafast rates, possibly leading to the generation of non-classical light via the dynamic Casimir effect. Finally, with an effective volume of \\(2.10^-6 _0^3\\), it is estimated that fewer than 3000 electrons per resonator are ultra-strongly coupled to the quantized electromagnetic mode, proving it is also a promising approach to explore few-electron polaritonic systems operating at relatively high temperatures.

The ability to build atomically precise structures on surfaces with complete control over both atomic placement and chemical bonding remains a central challenge in nanoscale fabrication. Here, we demonstrate simultaneous spatial and chemical control over the mechanosynthetic fabrication of carbon structures. Using inverted-mode STM, C\\(_2\\) units are donated from surface-deposited molecules to pre-patterned reactive sites on a hydrogen-passivated Si(100) surface. We demonstrate single-site C\\(_2\\) donation, spatially patterned multi-site C\\(_2\\) donation, and the stepwise assembly of polyyne structures through successive C-C bond formation. Together, these results establish controlled mechanosynthetic donation as a foundational capability for programmable atomically precise fabrication.

Enabled by inverted-mode scanning tunneling microscopy (IM-STM) and the use of functionalized molecular tools, we demonstrate positionally-controlled mechanosynthetic addition (donation) of carbon and subtraction (abstraction) of silicon atoms on a model build site: atomically clean and crystalline Si(100). The resulting structures represent the first demonstrations of an emerging ability to manipulate radical chemistry with positional control of specific atoms and moieties in 3D. Furthermore, by comparing the behavior of molecular tools designed for atomic donation versus abstraction, we highlight general principles governing molecular tool design for selective and reliable mechanosynthetic functionality.

Scanning Tunneling Microscopy (STM) enables fabrication of atomically precise structures with unique properties and growing technological potential. However, reproducible manipulation of covalently bonded atoms requires control over the atomic configuration of both sample and probe - a longstanding challenge in STM. Here, we introduce inverted-mode STM, an approach that enables mechanically controlled chemical reactions for atomically precise fabrication. Tailored molecules on a Si(100) surface image the probe apex, and the usual challenge of understanding the probe structure is effectively solved. The molecules can also react with the probe, with the two sides of the tunnel junction acting as reagents positioned with sub-angstrom precision. This allows abstraction or donation of atoms from or to the probe apex. We demonstrate this by using a novel alkynyl-terminated molecule to reproducibly abstract hydrogen atoms from the probe. The approach is expected to extend to other elements and moieties, opening a new avenue for scalable atomically precise fabrication.