First-principles perspective on full-spectrum infrared photodetectors from doping an excitonic insulator

Innovations in imaging technology involves finding strategies and materials suitable for detection applications over the entire infrared range. Herein, we propose a new design concept based on the unique feature of an excitonic insulator, namely, negative exciton transition energy ($E_t$). We demonstrate this concept using first-principles $GW$-BSE calculations on one-dimensional organometallic wire (CrBz)$_\infty$. The pristine (CrBz)$_\infty$ exhibits an excitonic instability due to a negative $E_t$ for the lowest exciton. Substitutional doping can continuously tune the $E_t$ from $\sim$0 to $\sim$0.6 eV, which shows the ability of photon detection from terahertz to near-infrared. This type of detectors have advantages of outstanding wavelength selectivity, reduced thermal disturbance and elevated working temperature. Our work not only adds another member in the family of rare one-dimensional excitonic insulators, but also opens a new avenue for the development of high-performance infrared photodetectors in the future.