We have measured the optically injected excess carrier lifetime in silicon using photoexcited muon spin spectroscopy. Positive muons implanted deep in a wafer can interact with the excess carriers and directly probe the bulk carrier lifetime whilst minimizing the effect from surface recombination. The method is based on the relaxation rate of muon spin asymmetry, which depends on the excess carrier concentration. The underlying microscopic mechanism has been understood by simulating the fourstate muonium model in Si under illumination. We apply the technique to different injection levels and temperatures, and demonstrate its ability for injection-and temperature-dependent lifetime spectroscopy.Excess carrier lifetime in semiconductors is an extremely sensitive probe of recombination active defect density N t [1,2]. In the case of silicon, a lifetime spectroscopy can probe N t as low as 10 10 cm −3 , corresponding to the carrier lifetime in the order of 10 ms. Therefore the lifetime measurements have been utilized to test a quality of Si wafers in various areas, and especially appreciated in photovoltaic applications where the carrier lifetime is a key parameter for the excess carriers to successfully diffuse across the p-n junction in solar cells. The microchip industries have also found its use as a cleanliness monitor in the chip manufacturing processes. It is now widely accepted that there are three main mechanisms that cause the electron-hole pair (EHP) recombination in semiconductors: 1) Shockley-Read-Hall (SRH) recombination (characterized by its lifetime τ SRH ), 2) Auger recombination (τ Auger ), and 3) radiative recombination (τ rad ) [1,2]. The bulk recombination lifetime τ bulk is then given by a relation,Among those mechanisms, the SRH recombination is a multiphonon process mediated by deep-level defect centers, and dominates τ bulk in low-level carrier injections, whilst the Auger recombination plays a key role in highlevel injections. The radiative recombination is usually negligible in bulk Si due to the indirect band structure. Although τ SRH gives a good indication of the N t level, it alone cannot determine N t explicitly -it is always necessary to assume the defect type, which is characterized by its energy level and capture cross section for electrons and holes. To measure the carrier lifetime, there are several traditional and novel methods, such as the photoconductance decay (PCD) and photoluminescence decay measurements. Induction-coupled PCD and its varieties are becoming more popular by virtue of their contactless and non-destructive measurement [1,2,6]. These techniques measure, by their nature, the effective lifetime of injected carriers, given by 1/τ ef f = 1/τ bulk + 1/τ S . The second term represents a contribution from the surface lifetime τ S which strongly depends on how the wafer surface has been conditioned. It is therefore necessary to extract τ bulk by 1) treating the surface to make τ S asymptote either 0 (e.g. sandblasting) or ∞ (e.g. passivation), or 2) measuring the same ...